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| 1.
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Murahashi, Tsuyoshi ; Kizu, Ryoichi ; Kakimoto, Hitoshi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Diesel-engine exhaust and airborne particulates were collected in downtown and suburban areas and five mutagenic nitroarenes (2-nitrofluoranthene (NF), 1-, 2- and 4-nitropyrenes (NPs) and 6-nitrochrysene (NC) in benzene-ethanol extracts
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were determined by high-performance liquid chromatography with chemiluminescence detection. 1- and 4-NPs and 6-NC were found in diesel-engine exhaust particulates, however, 2-NF and 2-NP were not detected. On the other hand, all five nitroarenes were found in airborne particulates. Diurnal concentration patterns of 4-NP and 6-NC in the downtown area were similar to the pattern of 1-NP, but the patterns of 2-NF and 2-NP were different from the pattern of 1-NP. These results strongly suggested that 2-NF and 2-NP are formed in the atmosphere. Of the five nitroarenes, 2-NF had the largest suburban / downtown concentration ratio. 2- and 4-NPs and 6-NC all showed larger ratios than did 1-NP. These results showed that 2-NF and 2-NP were formed in the atmosphere, but that the secondary formation of 4-NP and 6-NC were not known. Taking mutagenic activity and the atmospheric concentration into consideration, the mutagenic contribution of 2-NF was estimated to be comparable with that of 1-NP in the downtown area, and more than that of 1-NP in the suburban area. This result suggested that the mutagenic contribution of the minor nitroarenes formed in urban air might not be negligible.
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| 2.
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Tang, Ning ; Sato, Kousuke ; Tokuda, Takahiro ; Tatematsu, Michiya ; Hama, Hirotaka ; Suematsu, Chikako ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Airborne particulates were collected at a background site (Wajima Air Monitoring Station; WAMS) on the Noto Peninsula, J
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apan from January 2006 to December 2007. 1-, 2-nitropyrenes (1-, 2-NPs) and 2-nitrofluoranthene (2-NFR), in the particulates were determined with a sensitive HPLC method with chemiluminescence detection. The average concentrations were higher in winter than in summer. A meteorological analysis indicated that the air samples collected in winter were transported mainly from Northeast China over the Japan Sea. Both the concentration ratios of 2-NFR to 1-NP and 1-NP to pyrene were similar to those in Shenyang in Northeast China which located along the air transportation route to WAMS, but not in Kanazawa which near WAMS. These results strongly suggest that most of the atmospheric 1-, 2-NPs and 2-NFR at WAMS in winter were long range transported from Northeast China. © 2014 Elsevier Ltd. All rights reserved.
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| 3.
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Tamura, Masayoshi ; Mochizuki, Naoki ; Nagatomi, Yasushi ; Harayama, Koichi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Three compounds, hypothesized as fumonisin A1 (FA1), fumonisin A2 (FA2), and fumonisin A3 (FA3), were detected in a corn
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sample contaminated with mycotoxins by high-resolution liquid chromatography-Orbitrap mass spectrometry (LC-Orbitrap MS). One of them has been identified as FA1 synthesized by the acetylation of fumonisin B1 (FB1), and established a method for its quantification. Herein, we identified the two remaining compounds as FA2 and FA3, which were acetylated fumonisin B2 (FB2) and fumonisin B3 (FB3), respectively. Moreover, we examined a method for the simultaneous analysis of FA1, FA2, FA3, FB1, FB2, and FB 3. The corn samples were prepared by extraction using a QuEChERS kit and purification using a multifunctional cartridge. The linearity, recovery, repeatability, limit of detection, and limit of quantification of the method were >0.99, 82.9%–104.6%, 3.7%–9.5%, 0.02–0.60 μg/kg, and 0.05–1.98 μg/kg, respectively. The simultaneous analysis of the six fumonisins revealed that FA1, FA2, and FA3 were present in all corn samples contaminated with FB1, FB2, and FB 3. The results suggested that corn marketed for consumption can be considered as being contaminated with both the fumonisin B-series and with fumonisin A-series. This report presents the first identification and quantification of FA1, FA2, and FA3 in corn samples. © 2015 by the authors; licensee MDPI, Basel, Switzerland.
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| 4.
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Tanaka, Hiroki ; Sugita-Kounishi, Yuka ; Takino, Masahiko ; Tanaka, Toshitsugu ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />By adopting a rapid and sensitive method for simultaneous detection of nivalenol (NIV), deoxynivalen
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ol (DON), fusarenon-X (FX), 3-acetyl deoxinivalenol (3ADON), HT-2 toxin (HT-2), T-2 toxin (T-2) and zearalenone (ZEN), the natural occurrence of these mycotoxins in biscuits made of wheat (201 samples) in Japan was surveyed. Samples were analyzed by LC/MS with atmospheric pressure photo ionization (APPI). Further confirmation was performed by liquid chromatography/time of flight mass spectrometry (LC/TOFMS). The average contamination of each Fusarium mycotoxin was 3.1, 23, 0.7, 0.1 and 4.2 ng/g for NIV, DON, HT-2, T-2 and ZEN, respectively. Multiple toxins were observed in 120 samples while FX and 3ADON were not detected. The incidence of these toxins was 41% for NIV, 98% for DON, 19% for HT-2, 11% for T-2 and 2% for ZEN. There were no significant differences in the concentration and incidence between conventional biscuits made of wheat and biscuits made of wheat for infants. This is the first report concerning the presence of NIV, DON, HT-2, T-2 and ZEN in biscuits in Japan. © 2010 The Pharmaceutical Society of Japan.
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| 5.
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Motoyama, Yumi ; Bekki, Kanae ; Chung, Sang Woon ; Tang, Ning ; Kameda, Takayuki ; Toriba, Akira ; Taguchi, Keiko ; Hayakawa, Kazuichi
概要:
The effect of four ortho-quinoid polycyclic aromatic hydrocarbons (PAHs) and seven para-quinoid PAHs on the viability of
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A549 cells were examined. The ortho-quinoid PAHs [1,2-naphthoquinone (1,2-NQ), 9,10-phenanthrenquinone (9,10-PQ), 5,6-chrysenequinone (5,6-CQ), and benzo[c]phenanthrene-5,6-quinone (B[c]P-5,6-Q)] overproduced hydrogen peroxide (H2O2) without being consumed themselves. These ortho-quinoid had strong cytotoxic effects except for 1,2-NQ, since of its tendency to covalently bind to thiol groups. The cytotoxicity appears to be due to the overproduction of H 2O2 by ortho-quinoid PAHs in a redox cycle coupled with the consumption of thiol group. In contrast, the para-quinoid PAHs were not as strong cytotoxic and did not produce H2O2. ©2009 The Pharmaceutical Society of Japan.
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| 6.
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Suzuki, Nobuo ; Maruyama, Yusuke ; Nakano, Masaki ; Hattori, Atsuhiko ; Honda, Masato ; Shimasaki, Yohei ; Sekiguchi, Toshio ; Mishima, Hiroyuki ; Wada, Shigehito ; Srivastav, Ajai K. ; Hayakawa, Kazuichi ; Oshima, Yuji
概要:
We recently demonstrated that prostaglandin E2 PG¿ increases osteoclastic activity and induces bone resorption in both i
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n vitro and in vivo experiments using goldfish. In the fish reproductive period, the plasma calcium (Ca) level in female teleosts increases remarkably to make vitellogenin, which is a major component of egg protein and a Ca-binding protein. In this period, however, there is no reported relationship between PGE2 and Ca metabolism in fish. To clarify the Ca metabolism in fish reproduction, we examined plasma PGE2 and Ca levels and measured tartrate-resistant acid phosphatase (TRAP) activities as an indicator of osteoclastic activity in goldfish. Plasma PGE2 levels in the reproductive stage significantly increased as compared with those in non-reproductive stages. Also, both plasma Ca and TRAP increased in the reproductive stage. Significant positive correlations were recognized between plasma Ca and the gonad somatic index (r=0.81, p<0.001), plasma Ca and plasma PGE2 levels (r=0.635, p<0.05), and plasma Ca and plasma TRAP activities (r=0.584, p<0.05) from the analysis using samples of both reproductive and nonreproductive stages. Taking these data into consideration, we suggested that PGE, acts on osteoclasts and increases plasma Ca as a result of osteoclastic bone resorption, and we concluded that PGE, is an important hormone in Ca metabolism during fish reproduction.
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| 7.
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Kameda, Takayuki ; Akiyama, Ayuko ; Yoshita, Morio ; Tachikawa, Chihiro ; Toriba, Akira ; Tang, Ning ; Hayakawa, Kazuichi
概要:
The mutagenicities and endocrine-disrupting activities of two isomers of mononitrated 1-hydroxypyrene [1-hydroxy-x-nitro
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pyrenes (1-OH-x-NPs); x = 2 and 5], which are not only photoreaction products of 1-nitropyrene (1-NP) but also constituent of ambient airborne particles, were evaluated for the first time using the Ames plate incorporation assay and the yeast two-hybrid assay, respectively. The mutagenicity of 1-OH-5-NP was weakly positive in the absence of rat liver S9, but was enhanced up to 3-fold with the metabolic activation by S9. On the contrary, 1-OH-2-NPdid not exhibit significant mutagenicity in the presence or absence of S9. 1-OH-5-NP showed weak estrogenic activity, but 1-OH-2-NP did not show any estrogenic activity. The concentration of 1-OH-5-NP that gave 10% of activity of 1.0 × 10-6M 17ß- estradiol (E2) was 5.4 × 10-7M. 1-OH-5-NP exhibited stronger antiestrogenic and antiandrogenic activities than 1-OH-2-NP. 1-OH-5-NP at a concentration of 1.0 × 10-6M inhibited 71 and 90%of ß-galactosidase activity induced by 1.0 × 10-9Mof E2 and 1.0 × 10-8M of 5a-dihydrotestosterone (DHT), respectively. On the other hand, 1.0 × 10-6M of 1-OH-2-NP inhibited 16 and 43% of ß-galactosidase activity induced by 1.0 × 10-9M of E2 and 1.0 × 10-8M of DHT, respectively. These findings point out the need for determining the environmental sources and distribution of 1-OH-2-NP and 1-OH-5-NP as well as the other hydroxynitropyrene isomers. © 2011 The Pharmaceutical Society of Japan.
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| 8.
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Hosozumi, Chiemi ; Toriba, Akira ; Chuesaard, Thanyarat ; Kameda, Takayuki ; Tang, Ning ; Hayakawa, Kazuichi
概要:
Urinary 8-hydroxy-2'-deoxyguanosine (8-OHdG) is a widely used noninvasive biomarker of oxidative stress. A selective, se
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nsitive and rapid method for determining 8-OHdG in human urine was developed using hydrophilic interaction chromatography-tandem mass spectrometry (HILIC-MS/MS) with electrospray ionization. 8-OHdG and isotopically labeled 8-OHdG (internal standard) were separated on a HILIC column with a mobile phase of 10. mM ammonium acetate: acetonitrile (1:9, v/v) within 10. min and detected by using a positive electrospray ionization interface under the selected reaction monitoring mode. The detection limits of 8-OHdG (corresponding to a signal-to-noise ratio of 3) for the HILIC-MS/MS system and the conventional method using a reversed-phase column with MS/MS were 1.0 and 26.0. fmol/injection, respectively. The proposed method makes it possible to monitor the basal level of urinary 8-OHdG from non-exposed healthy subjects and can be used for large-scale human studies. © 2012 Elsevier B.V.
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| 9.
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Tamura, Masayoshi ; Mochizuki, Naoki ; Nagatomi, Yasushi ; Harayama, Koichi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
A high-resolution liquid chromatography-Orbitrap mass spectrometry (LC-Orbitrap MS) method was developed for simultaneou
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s determination of 20 Fusarium toxins (nivalenol, fusarenon-X, deoxynivalenol, 3-acetyl deoxynivalenol, 15-acetyl deoxynivalenol, HT-2 toxin, T-2 toxin, neosolaniol, diacetoxyscirpenol, fumonisin B1, fumonisin B2, fumonisin B3, fumonisin A1, fumonisin A2, fumonisin A3, zearalenone, α-zearalenol, β-zearalenol, α-zearalanol, and β-zearalanol) in cereals. The separation of 20 Fusarium toxins with good peak shapes was achieved using a pentafluorophenyl column, and Orbitrap MS was able to detect accurately from cereal matrix components within ±0.77 ppm. The samples were prepared using a QuEChERS kit for extraction and a multifunctional cartridge for purification. The linearity, repeatability, and recovery of the method were >0.9964, 0.8%–14.7%, and 71%–106%, respectively. Using this method, an analysis of 34 commercially available cereals detected the presence of deoxynivalenol, 15-acetyl deoxynivalenol, fumonisin B1, fumonisin B2, fumonisin B3, fumonisn A1, fumonisin A2, fumonisin A3, and zearalenone in corn samples with high concentration and frequency. Trichothecenes was detected from wheat samples with high frequency; in particular, the concentration of deoxynivalenol was high. Conversely, α-zearalenol, β-zearalenol, α-zearalanol, and β-zearalanol were not detected in any of the samples. © 2015 by the authors; licensee MDPI, Basel, Switzerland.
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| 10.
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Hayakawa, Kazuichi ; Onoda, Yu ; Tachikawa, Chihiro ; Hosoi, Shinzo ; Yoshita, Morio ; Chung, Sang Woon ; Kizu, Ryoichi ; Toriba, Akira ; Kameda, Takayuki ; Tang, Ning
概要:
Estrogenic/antiestrogenic activities of 14 polycyclic aromatic hydrocarbons (PAHs) and 63 monohydroxylated PAHs (OHPAHs)
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having 2 to 6 rings were evaluated by yeast two-hybrid assay expressing human estrogen receptor α. Relative effective potencies of estrogenic and antiestrogenic activities were calculated as the inverse values of the relative concentration of the test compound that gave the same activities of E2 and 4-hydroxytamoxifen, respectively. PAHs did not show any estrogenic/antiestrogenic activity, but several OHPAHs having 3 to 5 rings showed activities. Especially, OHPAHs having 4 rings such as 3-, 4- and 10-hydroxybenz[a]anthracenes (3-, 4- and 10-OHBaAs) and 2-hydroxychrysene (2-OHCh) showed strongly estrogenic activity. Several other OHPAHs having 4 rings such as 2- and 3-hydroxybenzo[c]phenanthrenes (2-, 3- OHBcPhs), 2-OHBaA and 3-OHCh showed strongly antiestrogenic activity. The length-to-breadth (L/B) ratios of the rectangular van der Walls planes surrounding the ring molecules of estrogenic OHPAHs were in the narrow range from 1.599 to 1.734. The distances between the oxygen atom of the phenol group and farthest hydrogen atom (O-H distance) of the estrogenic OHPAHs ranged from 10.825 A° to 11.738 A°. The L/B ratios and O-H distances of antiestrogenic OHPAHs were in the wider ranges from 1.277 to 1.734 and from 8.47 A° to 11.681 A°, respectively. The partial charges (atomic unit) of the phenol group of both estrogenic and antiestrogenic OHPAHs were in the range from 0.250 atmic unit (au) to 0.253 au. The similarity of these values to those of E2 and diethylstilbestrol suggested that the compositions of estrogenic OHPAHs were similar to them and that the compositional conditions of estrogenic OHPAHs were much smaller than those of antiestrogenic OHPAHs. These results raise the possibility of predicting the estrogenic/antiestrogenic activities of OHPAHs from their structural characteristics, although using only the above three parameters might not be enough for accurate estimations.
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| 11.
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Higashi, Tomomi ; Kambayashi, Yasuhiro ; Ohkura, Noriyuki ; Fujimura, Masaki ; Nakai, Satoshi ; Honda, Yasushi ; Saijoh, Kiyofumi ; Hayakawa, Kazuichi ; Kobayashi, Fumihisa ; Michigami, Yoshimasa ; Olando, Anyenda Enoch ; Hitomi, Yoshiaki ; Nakamura, Hiroyuki
概要:
Asian dust, known as kosa in Japanese, is a major public health concern. In this panel study, we evaluated the effects o
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f exposure to kosa on daily cough occurrence. The study subjects were 86 patients being treated for asthma, cough variant asthma, or atopic cough in Kanazawa University Hospital from January 2011 to June 2011. Daily mean concentrations of kosa and spherical particles were obtained from light detection and ranging (LIDAR) measurements, and were categorized from Grade 1 (0μg/m3) to 5 (over 100μg/m3). The association between kosa and cough was analyzed by logistic regression with a generalized estimating equation. Kosa effects on cough were seen for all Grades with potential time lag effect. Particularly at Lag 0 (the day of exposure), a dose-response relationship was observed: the odds ratios for Grades 2, 3, 4, and 5 above the referent (Grade 1) were 1.111 (95% confidence interval (CI): 0.995-1.239), 1.171 (95% CI: 1.006-1.363), 1.357 (95% CI: 1.029-1.788), and 1.414 (95% CI: 0.983-2.036), respectively. Among the patients without asthma, the association was higher: the odds ratios for Grades 2, 3, 4 and 5 were 1.223 (95% CI: 0.999-1.497), 1.309 (95% CI: 0.987-1.737), 1.738 (95% CI: 1.029-2.935) and 2.403 (95% CI: 1.158-4.985), respectively. These associations remained after adjusting for the concentration of spherical particles or particulate matter with an aerodynamic diameter of less than 2.5μm (PM2.5). Our findings demonstrate that kosa is an environmental factor which induces cough in a dose-response relationship. © 2014 Elsevier Ltd.
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| 12.
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Morisaki, Hiroshi ; Nakamura, Shiho ; Tang, Ning ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Benzo[c]fluorene (BcFE) concentrations in benzene/ethanol extracts of airborne particulates were determined by high-perf
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ormance liquid chromatography (HPLC) with fluorescence detection. HPLC conditions were as follows: columns, two ZORBAX Eclipse PAH (4.6 i.d. × 250 mm, 3.5 μm) and one Inertsil ODS-P (4.6 i.d. × 250 mm, 5 μm) in series; mobile phase, acetonitrile–water (98:2, v/v), 0.3 mL/min; detection wavelengths, excitation 309 nm, emission 354 nm. Particulate-phase BcFE concentrations in the atmosphere varied seasonally (winter > summer). The concentrations were 11000 ± 6100 pg m−3 (winter) and 40 ± 12 pg m−3 (summer) in Beijing, China, and 13 ± 5.0 pg m−3 (winter) and 2.7 ± 0.52 pg m−3 (summer), in Kanazawa, Japan. In both cities, the particulate-phase BcFE concentration in the atmosphere was lower than that of benzo[a]pyrene (BaP) by a factor of 0.03 – 0.43. However, the mutagenic contribution of particulate-phase BcFE in the atmosphere in winter calculated from the mutagenicity relative potency factor was greater than that of BaP.
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| 13.
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Hayakawa, Kazuichi
概要:
Airborne particulate matter (PM) has been collected at four cities in Japan starting in the late 1990s, at five or more
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major cities in China, Korea and Russia starting in 2001 and at the Noto Peninsula starting in 2004. Nine polycyclic aromatic hydrocarbons (PAHs) and eleven nitropolycyclic aromatic hydrocarbons (NPAHs) were determined by HPLC with fluorescence and chemiluminescence detections, respectively. Annual concentrations of PAHs and NPAHs were in the order, China>Russia≫Korea=Japan, with seasonal change (winter>summer). During the observation period, concentrations of PAHs and NPAHs in Japanese cities significantly decreased but the increases in the PAH concentration were observed in Chinese and Russian cities. Concentrations of PAHs and NPAHs were higher in the Northern China than those in the Southern China. At the Noto peninsula, which is in the main path of winter northwest winds and a year-round jet stream that blow from the Asian continent to Japan, the concentrations were high in winter and low in summer every year. A cluster analysis and back trajectory analysis indicated that PAHs and NPAHs were long-range transported from Northeastern China, where coal burning systems such as coal-heating boilers are considered to be the major contributors of PAHs and NPAHs. A dramatic change in atmospheric concentrations of PAHs and NPAHs in East Asia suggests the rapid and large change of PM2.5 pollution in East Asia. Considering the adverse health effects of PM2.5, continuous monitoring of atmospheric PAHs and NPAHs is necessary in this area.
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| 14.
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Tang, Ning ; Taga, Rina ; Hattori, Tetsuyuki ; Tamura, Kenji ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
A method using high-performance liquid chromatography with chemiluminescence detection was developed for analyzing mutagenic nitrobenzanthrone (NBA) isomers in airborne particulates. The method was a modification of our previously
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described method for analyzing nitropolycyclic aromatic hydrocarbons (NPAHs). The pretreatment and reducing conditions for 1-, 2-, 3- and 10-NBAs were the same as those for NPAHs. In order to separate these NBA isomers, we used a polymeric-type ODS column (Cosmosil 5C-18MS); a mixture of 40% acetonitrile and 60% 10 mM imidazole-HClO4 buffer was employed as the mobile phase at a flow rate of 1 mL/min. The isomers of 1-, 2-, 3- and 10-NBA were determined in chemiluminescence with linear calibration graphs from 0.1 to 4 pmol, from 200 to 4000 pmol, from 1 to 50 pmol and from 10 to 400 pmol, respectively. The detection limits (S/N = 3) of 1-, 2-, 3- and 10-NBA isomers were 0.02 pmol, 35 pmol, 0.3 pmol and 3 pmol, respectively. The method was used to analyze airborne particulates at a heavy traffic site in Kanazawa. 2- and 3-NBAs were detected in the extracts of the particulates, while 1-NBA and 10-NBA were not detected. The atmospheric concentrations of 2- and 3-NBAs were 1.83 pmol/m3 and 24.7 fmol/m3, respectively.
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| 15.
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Morisaki, Hiroshi ; Nakamura, Shiho ; Tang, Ning ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Benzo[c]fluorene (BcFE) concentrations in benzene/ethanol extracts of airborne particulates were determined by high-perf
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ormance liquid chromatography (HPLC) with fluorescence detection. HPLC conditions were as follows: columns, two ZORBAX Eclipse PAH (4.6 i.d. × 250 mm, 3.5 μm) and one Inertsil ODS-P (4.6 i.d. × 250 mm, 5 μm) in series; mobile phase, acetonitrile–water (98:2, v/v), 0.3 mL/min; detection wavelengths, excitation 309 nm, emission 354 nm. Particulate-phase BcFE concentrations in the atmosphere varied seasonally (winter > summer). The concentrations were 11000 ± 6100 pg m−3 (winter) and 40 ± 12 pg m−3 (summer) in Beijing, China, and 13 ± 5.0 pg m−3 (winter) and 2.7 ± 0.52 pg m−3 (summer), in Kanazawa, Japan. In both cities, the particulate-phase BcFE concentration in the atmosphere was lower than that of benzo[a]pyrene (BaP) by a factor of 0.03 – 0.43. However, the mutagenic contribution of particulate-phase BcFE in the atmosphere in winter calculated from the mutagenicity relative potency factor was greater than that of BaP.
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| 16.
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Higashi, Tomomi ; Ohkura, Noriyuki ; Fujimura, Masaki ; Nakai, Satoshi ; Honda, Yasushi ; Saijoh, Kiyofumi ; Hayakawa, Kazuichi ; Kobayashi, Fumihisa ; Michigami, Yoshimasa ; Olando, Anyenda Enoch ; Hitomi, Yoshiaki ; Nakamura, Hiroyuki ; 東, 朋美 ; 大倉, 徳幸 ; 藤村, 政樹 ; 西條, 淸史 ; 早川, 和一 ; 小林, 史彦 ; 道上, 義正 ; 人見, 嘉哲 ; 中村, 裕之
概要:
金沢大学医薬保健研究域医学系<br />Asian dust, known as kosa in Japanese, is a major public health concern. In this panel study, we eva
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luated the effects of exposure to kosa on daily cough occurrence. The study subjects were 86 patients being treated for asthma, cough variant asthma, or atopic cough in Kanazawa University Hospital from January 2011 to June 2011. Daily mean concentrations of kosa and spherical particles were obtained from light detection and ranging (LIDAR) measurements, and were categorized from Grade 1 (0 μg/m3) to 5 (over 100 μg/m3). The association between kosa and cough was analyzed by logistic regression with a generalized estimating equation. Kosa effects on cough were seen for all Grades with potential time lag effect. Particularly at Lag 0 (the day of exposure), a dose-response relationship was observed: the odds ratios for Grades 2, 3, 4, and 5 above the referent (Grade 1) were 1.111 (95% confidence interval (CI): 0.995-1.239), 1.171 (95% CI: 1.006-1.363), 1.357 (95% CI: 1.029-1.788), and 1.414 (95% CI: 0.983-2.036), respectively. Among the patients without asthma, the association was higher: the odds ratios for Grades 2, 3, 4 and 5 were 1.223 (95% CI: 0.999-1.497), 1.309 (95% CI: 0.987-1.737), 1.738 (95% CI: 1.029-2.935) and 2.403 (95% CI: 1.158-4.985), respectively. These associations remained after adjusting for the concentration of spherical particles or particulate matter with an aerodynamic diameter of less than 2.5 μm (PM2.5). Our findings demonstrate that kosa is an environmental factor which induces cough in a dose-response relationship. © 2014 Elsevier B.V.<br />Embargo Period 12 months
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| 17.
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Imaizumi, Noriko ; Hayakawa, Kazuichi ; Okubo, Noboru ; Miyazaki, Motoichi
概要:
A selective, sensitive and accurate determination of sulfite was proposed by high performance liquid chromatography (HPL
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C). The sulfite was converted quantitatively to an adduct by reacting with a triphenylmethane dye, malachite green (MG). The formation of adduct was complete, and the adduct was stable at the experimental conditions. Then, the adduct was submitted to HPLC. The working curve for sulfite was linear in the range from 2.0×10-12 mol upto 1.2×10-9 mol.
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| 18.
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Tang, Ning ; Tabata, Masahiro ; Mishukov, Vasiliy F. ; Sergineko, Valentine ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
Airborne particulates were collected simultaneously at Vladivostok, Kanazawa and Toyama. 1,3-, 1,6-, 1,8-Dinitropyrenes (DNPs), 1-, 2-, 4-nitropyrenes (NPs), 2-nitrofluorene and 6-nitrochrysene in the particulates were analyzed by HPLC
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with chemiluminescence detection. All compounds were detected not only in Kanazawa but also in Vladivostok and Toyama. Moreover, five unknown peaks which might be nitropolycyclic aromatic hydrocarbons were detected only in chromatograms of Vladivostok. The [DNPs]/[1-NP] ratios at all stations were near the value found in diesel-exhaust particulates, suggesting that one of the main contributors of these compounds was diesel-engine vehicles not only in Kanazawa and Toyama but also in Vladivostok. However, the difference in traffic volume at two stations in Vladivostok did not have a significant effect on the concentrations of DNPs and NPs in contrast to two stations in Kanazawa. These results suggested sources other than diesel-engine vehicles also contributing to DNPs and NPs in Vladivostok. Seasonal variations similar to those in Kanazawa were observed in Vladivostok and Toyama. As in Kanazawa, the [2-NP]/[1-NP] ratio in Vladivostok was larger at the lighter traffic station than that at heavier traffic station. This suggested that, as in Kanazawa, 2-NP was formed in the atmosphere in Vladivostok.
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| 19.
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Chung, Sang Woon ; Chung, Hae Young ; Toriba, Akira ; Hayakawa, Kazuichi
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金沢大学大学院自然科学研究科<br />場所：東京大学弥生講堂，共催：文部科学省２１世紀COE「環日本海域の環境計測と長期・短期変動予測」，大気環境学会
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| 20.
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Tang, Ning ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
An automatic HPLC system for analyzing nitropolycyclic aromatic hydrocarbons (NPAHs, nitroarenes) in airborne particulates was previously described (Anal. Chim. Acta, 2001, 445, 20). Some problems with this system were that it
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generated a peak originating from an ascorbic acid solution that elutes at a retention time close to that of 1,6-dinitropyrene (DNP), and that it was able to analyze only 1,3-, 1,6-, 1,8-DNPs and 1-nitropyrene (1-NP). Here, we describe an improved system that effectively removes the interfering peak by introducing an ODS column just after the pump for the ascorbic acid solution, and which is capable of analyzing several additional compounds (2-, 4-NPs, 2-nitrofluorene, 6-nitrochrysene, 7-nitrobenz[a]anthracene, 3-nitroperylene and 6-nitrobenzo[a]pyrene etc.). The improved sensitivities were achieved by concentrating the compounds in a benzene-ethanol extract from airborne particulates, by increasing the loading time of the sample solution from 20 to 38 min, and by increasing the flow rate of an ascorbic acid solution from 1.3 to 1.8 mL/min.
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| 21.
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Yachiguchi, Koji ; Matsumoto, Noriko ; Haga, Yuki ; Suzuki, Motoharu ; Matsumura, Chisato ; Tsurukawa, Masahiro ; Okuno, Toshihiro ; Nakano, Takeshi ; Kawabe, Kimi ; Kitamura, Kei-ichiro ; Toriba, Akira ; Hayakawa, Kazuichi ; Chowdhury, Vishwajit S. ; Endo, Masato ; Chiba, Atsuhiko ; Sekiguchi, Toshio ; Nakano, Masaki ; Tabuchi, Yoshiaki ; Kondo, Takashi ; Wada, Shigehito ; Mishima, Hiroyuki ; Hattori, Atsuhiko ; Suzuki, Nobuo
概要:
To analyze the effect of polychlorinated biphenyl (PCB) 118 on fish bone metabolism, we examined osteoclastic and osteob
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lastic activities, as well as plasma calcium levels, in the scales of PCB (118)-injected goldfish. In addition, effect of PCB (118) on osteoclasts and osteoblasts was investigated in vitro. Immature goldfish, in which the endogenous effects of sex steroids are negligible, were used. PCB (118) was solubilized in dimethyl sulfoxide at a concentration of 10 ppm. At 1 and 2 days after PCB (118) injection (100 ng/g body weight), both osteoclastic and osteoblastic activities, and plasma calcium levels were measured. In an in vitro study, then, both osteoclastic and osteoblastic activities as well as each marker mRNA expression were examined. At 2 days, scale osteoclastic activity in PCB (118)-injected goldfish increased significantly, while osteoblastic activity did not change significantly. Corresponding to osteoclastic activity, plasma calcium levels increased significantly at 2 days after PCB (118) administration. Osteoclastic activation also occurred in the marker enzyme activities and mRNA expressions in vitro. Thus, we conclude that PCB (118) disrupts bone metabolism in goldfish both in vivo and in vitro experiments. © 2012 The Author(s).
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| 22.
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論文
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Yano, Sachiko ; Kitamura, Kei-ichiro ; Satoh, Yusuke ; Nakano, Masaki ; Hattori, Atsuhiko ; Sekiguchi, Toshio ; Ikegame, Mika ; Nakashima, Hiroshi ; Omori, Katsunori ; Hayakawa, Kazuichi ; Chiba, Atsuhiko ; Sasayama, Yuichi ; Ejiri, Sadakazu ; Mikuni-Takagaki, Yuko ; Mishima, Hiroyuki ; Funahashi, Hisayuki ; Sakamoto, Tatsuya ; Suzuki, Nobuo
概要:
Fish scales are a form of calcified tissue similar to that found in human bone. In medaka scales, we detected both osteo
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blasts and osteoclasts and subsequently developed a new scale assay system. Using this system, we analyzed the osteoblastic and osteoclastic responses under 2-, 3-, and 4-gravity (G) loading by both centrifugation and vibration. After loading for 10 min, the scales from centrifugal and vibration loading were incubated for 6 and 24 hrs, respectively, after which the osteoblastic and osteoclastic activities were measured. Osteoblastic activity significantly increased under 2- to 4-G loading by both centrifugation and vibration. In contrast, we found that osteoclastic activity significantly decreased under 2- and 3-G loading in response to both centrifugation and vibration. Under 4-G loading, osteoclastic activity also decreased on centrifugation, but significantly increased under 4-G loading by vibration, concomitant with markedly increased osteoblastic activity. Expression of the receptor activator of the NF-αB ligand (RANKL), an activation factor of osteoclasts expressed in osteoblasts, increased significantly under 4-G loading by vibration but was unchanged by centrifugal loading. A protein sequence similar to osteoprotegerin (OPG), which is known as an osteoclastogenesis inhibitory factor, was found in medaka using our sequence analysis. The ratio of RANKL/OPG-like mRNAs in the vibration-loaded scales was significantly higher than that in the control scales, although there was no difference between centrifugal loaded scales and the control scales. Accordingly, medaka scales provide a useful model by which to analyze bone metabolism in response to physical strain. © 2013 Zoological Society of Japan.
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| 23.
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論文
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Yachiguchi, Koji ; Matsumoto, Noriko ; Haga, Yuki ; Suzuki, Motoharu ; Matsumura, Chisato ; Tsurukawa, Masahiro ; Okuno, Toshihiro ; Nakano, Takeshi ; Kawabe, Kimi ; Kitamura, Kei-ichiro ; Toriba, Akira ; Hayakawa, Kazuichi ; Chowdhury, Vishwajit S. ; Endo, Masato ; Chiba, Atsuhiko ; Sekiguchi, Toshio ; Nakano, Masaki ; Tabuchi, Yoshiaki ; Kondo, Takashi ; Wada, Shigehito ; Mishima, Hiroyuki ; Hattori, Atsuhiko ; Suzuki, Nobuo
概要:
To analyze the effect of polychlorinated biphenyl (PCB) 118 on fish bone metabolism, we examined osteoclastic and osteob
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lastic activities, as well as plasma calcium levels, in the scales of PCB (118)-injected goldfish. In addition, effect of PCB (118) on osteoclasts and osteoblasts was investigated in vitro. Immature goldfish, in which the endogenous effects of sex steroids are negligible, were used. PCB (118) was solubilized in dimethyl sulfoxide at a concentration of 10 ppm. At 1 and 2 days after PCB (118) injection (100 ng/g body weight), both osteoclastic and osteoblastic activities, and plasma calcium levels were measured. In an in vitro study, then, both osteoclastic and osteoblastic activities as well as each marker mRNA expression were examined. At 2 days, scale osteoclastic activity in PCB (118)-injected goldfish increased significantly, while osteoblastic activity did not change significantly. Corresponding to osteoclastic activity, plasma calcium levels increased significantly at 2 days after PCB (118) administration. Osteoclastic activation also occurred in the marker enzyme activities and mRNA expressions in vitro. Thus, we conclude that PCB (118) disrupts bone metabolism in goldfish both in vivo and in vitro experiments. © 2012 The Author(s).
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| 24.
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論文
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Chung, Sang Woon ; Chung, Hae Young ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />場所：金沢大学自然科学研究科図書館棟1階，講演会場：図書館棟1階 大会議室，ポスター会場：図書館棟1階12会議室,主催・共催：文部科学省２１世紀COE「環日本海域の環境計測と長期・短期変動予測」， 大
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気環境学会， 金沢大学工学部
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| 25.
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論文
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Akutsu, Kazuhiko ; Takatori, S. ; Nozawa, S. ; Yoshiike, M. ; Nakazawa, H. ; Hayakawa, Kazuichi ; Makino, T. ; Iwamoto, T.
概要:
Polybrominated diphenyl ethers (PBDEs) are widely used flame retardants; currently, they are identified as ubiquitous en
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vironmental contaminants. Several studies indicate that PBDEs might affect male fertility. We present the results of a pilot study on the relationship between human serum PBDEs and sperm quality. The PBDE levels in Japan are comparable to those found in European countries. Strong inverse correlations were observed between the serum concentration of 2,2′,4,4′,5,5′-hexabromodiphenyl ether and sperm concentration (r = -0.841, p = 0.002) and testis size (r = -0.764, p = 0.01). Extensive studies on the relationship between PBDEs and sperm quality are required. © 2008 Springer Science+Business Media, LLC.
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| 26.
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論文
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Hayakawa, Kazuichi ; Nakamura, Seiji ; Inaki, Kotoe ; Miyazaki, Motoichi
概要:
Carboxylesters, carboxylic and inorganic anions were determined separately by photometric ion chromatography with an enz
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yme immobilized column. In the system, a carboxylesterase immobilized column (4.6mm i.d.×10mm), which converted carboxylesters to carboxylic anions completely, was set between a sample injector and an analytical column. The other chromatographic conditions were as follows: an anion exchanger-type separation column (4.6mm i.d.×250mm); phthalate-N-2-hydroxyethylpiperazine-N′-2-ethanesulfonic acid e uent (pH 6.5); an oven of temperature 40°C; a flow rate of 1.0ml/min; 280-nm UV detection; and an injection volume of 20μl. Calibration curves for ethyl esters of acetate, propionate, butyrate and isova erate were linear with the range 5×10-10mol to 1×10-7mol according to the peak-height method; their detection limits were 10-10 mol levels. The present method was applied for the determination of carboxylesters in practical samples.
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| 27.
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論文
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Hayakawa, Kazuichi ; Kitamura, Ryuichi ; Butoh, Mizuka ; Imaizumi, Noriko ; Miyazaki, Motoichi
概要:
A high performance liquid chromatographic (HPLC) method with chemiluminescence (CL) detection was developed for the sens
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itive determination of 1, 3-diaminopyrene (1, 3-DAP), 1, 6-DAP, 1, 8-DAP and 1-aminopyrene (1-AP). The HPLC conditions were as follows: column, Cosmosil 5C18 (4.6mm i.d.×250mm); mobile phase, 10mM imidazole- perchloric acid buffer(pH 7.6)-acetonitrile (1:1, v/v); CL reagent, 0.02mM bis(2, 4, 6-trichlorophenyl)oxalate (TCPO) and 15mM hydrogen peroxide in acetonitrile. The oxidative degradation of DAPS and AP in the presence of metals was prevented by adding ascorbic acid to sample solutions. The calibration curves were straight over 2 orders of magnitude for all analytes, and their detection limits (as S/N was 3) were in the sub-fmol range. Dinitro- and nitropyrenes in sooty emissions of diesel- and gasoline-engine cars could be determined by this HPLC after reductive conversion into DAPs and AP, respectively, by refluxing the samples in the presence of sodium hydrosulfide.
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| 28.
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論文
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Suzuki, Nobuo ; Sekiguchi, Toshio ; Satake, Honoo ; Kato, Kanoko ; Nishiyama, Yudai ; Takahashi, Hideya ; Dankse, Janine A. ; Martin, T. John ; Hattori, Atsuhiko ; Nakano, Masaki ; Kakikawa, Makiko ; Yamada, Sotoshi ; Ogoshi, Maho ; Hyodo, Susumu ; Yamaguchi, Yoko ; Chowdhur, Vishwajit S. ; Hayakawa, Kazuichi ; Funahashi, Hisayuki ; Sakamoto, Tatsuya ; Sasayama, Yuichi
概要:
In cartilaginous fish, two cDNAs encoding calcitonin-family receptors were isolated for the first time from the stingray
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brain. The open reading frame of one receptor cDNA coded a 525-amino acid protein. The amino acid identity of this receptor to human calcitonin-receptor-like receptor (CRLR) is 64.5%, frog CRLR is 64.7%, and flounder CRLR is 61.2% and this was higher than to human calcitonin receptor (CTR) (46.1%), frog CTR (54.7%), and flounder CTR (48.9%). We strongly suggested that this receptor is a ray CRLR based on phylogenetic analysis. In case of the second receptor, amino acid identity among CRLRs (human 50.5%, frog 50.7%, flounder 48.0%) and CTRs (human 43.2%, frog 49.1%, flounder 41.8%) was similar. From phylogenetic analysis of both CRLRs and CTRs, we believe that this receptor is ray CTR. The expression of ray CRLR mRNA was predominantly detected in the nervous system (brain) and vascular system (atrium, ventricle, and gill), which reflects the similar localization of CGRP in the nervous and vascular systems as mammals. It was observed that the second receptor was expressed in several tissues, namely cartilage, brain, pituitary gland, gill, atrium, ventricle, pancreas, spleen, liver, gall bladder, intestine, rectal gland, kidney, testis and ovary. This localization pattern was very similar to flounder CTR. Both receptor mRNAs were strongly expressed in the gill. This suggests that the calcitonin-family members are involved in the osmoregulation of stingray as this fish is known to be euryhaline. When a stingray was transferred to diluted seawater (20% seawater), the expression of both receptors significantly decreased in the gill. Similar results were obtained in the kidney of the stingray. Thus, our cloning and isolation of both receptors in the stingray will be helpful for elucidation of their physiological role(s) such as osmoregulation including calcium metabolism of cartilaginous fish. © 2012 Elsevier B.V.
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| 29.
論文 |
論文
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Chung, Sang Woon ; Chung, Hae Young ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />場所：金沢大学自然科学研究科図書館棟1階，講演会場：図書館棟1階 大会議室，ポスター会場：図書館棟1階12会議室,主催・共催：文部科学省２１世紀COE「環日本海域の環境計測と長期・短期変動予測」， 大
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気環境学会， 金沢大学工学部
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| 30.
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論文
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Kakimoto, Kensaku ; Toriba, Akira ; Ohno, Takanori ; Ueno, Mariko ; Kameda, Takayuki ; Tang, Ning ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />To evaluate human exposure to polycyclic aromatic hydrocarbons (PAHs), we developed a rapid, simple
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and sensitive method for determining 1-hydroxypyrene-glucuronide (1-OHP-G) in human urine. To improve precision, a deuterated glucuronide was used as an internal standard. The method requires only 1 mL of urine. The urine was treated with a mixed-mode anion-exchange and reversed-phase solid-phase extraction cartridge (Oasis MAX). The analytes were analyzed with a C18 reversed-phase column with a gradient elution, followed by tandem mass spectrometry with electrospray ionization in negative ion mode. The detection limit of 1-OHP-G (corresponding to a signal-to-noise ratio of 3) was 0.13 fmol/injection. Urinary concentrations of 1-OHP-G determined by this method were strongly correlated (r2 = 0.961) with concentrations of 1-hydroxypyrene by conventional HPLC with fluorescence detection. © 2008 Elsevier B.V. All rights reserved.
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| 31.
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論文
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Hayakawa, Kazuichi ; Nakamura, Akio ; Terai, Noriko ; Kizu, Ryoichi ; Ando, Kyoko
概要:
Diesel exhaust particulates were extracted with benzene-ethanol (3 : 1, v/v) and separated into five fractions by silica-gel column chromatography. Direct-acting mutagenic activity was assayed by the Ames test using the Salmonella typhimurium
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YG1024 strain. The total activity of five fractions was about four times greater than that of the crude extract, suggesting that the activities in the fractions were suppressed in the crude extract. Strong activity was observed in fraction 4 which was eluted with dichloromethane (61.5% of the total activity) and fraction 5 which was eluted with ethanol (35.3%). Nitropolycyclic aromatic hydrocarbons (NPAHs) were determined by high-performance liquid chromatography with chemiluminescence detection. They were found mainly in fraction 4, although one NPAH was in fraction 3 which was eluted with n-hexane-dichloromethane (3 : 1, v/v). Based on these results, 53.1% of the activity in fraction 4 was attributed to NPAHs. The contribution of 1-nitropyrene and 1, 3-, 1, 6- and 1, 8-dinitropyrenes was great and that of the other NPAHs was small. The mutagenic compound in fraction 5 was not identified. Fractions 1 and 2, which were eluted with n-hexane, and fraction 3 suppressed the activity of fraction 4. Polycyclic aromatic hydrocarbons in fractions 2 and 3 were considered as possible suppressors of NPAHs.
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| 32.
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論文
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Araki, Yuki ; Tang, Ning ; Ohno, Michihiro ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
We developed a sampler for collecting atmospheric polycyclic aromatic hydrocarbons (PAHs) and nitropolycyclic aromatic hydrocarbons (NPAHs) by attaching a glass column packed with XAD-4 resin to the gas sampling port of a
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high-volume air sampler equipped with a filter. When the upper and bottom layers of the column were packed with 64 g and 32 g of XAD-4 resin, respectively, all PAHs and NPAHs in the gas phase were quantitatively collected in the XAD-4 resin column without any break through, while PAHs and NPAHs in the particle phase were collected on the filter. We collected air samples at suburban and downtown Kanazawa by using the proposed sampler. It was found that about 95% of 2-3 ring PAHs and more than 99% of 2-ring NPAHs existed chiefly in the gas phase, that 4-ring PAHs such as fluoranthene (FR) and pyrene (Pyr) and 3-ring NPAHs were in both the gas and particle phases and that the other PAHs and NPAHs having 4-rings or more except for FR and Pyr were almost completely in the particle phase. Our data also indicated that the adsorption of NPAHs to the particle phase in the atmosphere is controlled by the same mechanism as that of PAHs.
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| 33.
論文 |
論文
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Ohno, Takanori ; Toriba, Akira ; Kameda, Takayuki ; Tang, Ning ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />To measure the actual exposure of a person to 1-nitropyrene (1-NP) in airborne particulate matter, i
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t is considered more accurate to collect air samples with a portable air sampler than to sample at a fixed location. However, because the portable samplers can sample only small volumes, a sensitive method is needed to analyze the compounds that are collected on a filter. Here we describe a high-performance liquid chromatographic (HPLC) method with fluorescence detection that is sensitive and precise enough for use with portable air samplers. The developed column-switching system successfully removed the interfering substances in the samples with only a simple pretreatment. To improve the precision of the measurement, deuterated 1-NP was used as an internal standard, and it eluted immediately prior to 1-NP with sufficient resolution (Rs, 1.50). The detection limit was 0.32 fmol/injection, and the calibration range was from 2 to 100 fmol. The proposed method was applied to determining 1-NP in fine airborne particulate matter (PM2.5) at two sites with low pollution levels. 1-NP was detected in all samples at concentrations in the low fmol/m3 range. The proposed method has enough sensitivity and precision to determine 1-NP in the limited air volume of the portable sampler. © 2009 Elsevier B.V. All rights reserved.
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| 34.
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論文
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Kameda, Takayuki ; Akiyama, Ayuko ; Toriba, Akira ; Tachikawa, Chihiro ; Yoshita, Morio ; Tang, Ning ; Hayakawa, Kazuichi
概要:
Endocrine disrupting activities of three isomers of monohydroxylated 1-nitropyrene (1-NP) [3-, 6-, and 8-hydroxy-1-nitro
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pyrenes (OHNPs)] were evaluated for the first time by yeast two-hybrid assay. OHNPs, which are not only metabolites of 1-NP but are also found in airborne particles, did not exhibit androgenic activity but exhibited estrogenic, antiestrogenic, and antiandrogenic activities. 6-OHNP showed the strongest estrogenic activity among the three OHNP isomers examined in this study. Concentrations of the OHNP isomers that gave 10% of activity of 1.0 × 10-6 M 17β-estradiol (E2) were as follows: 3-OHNP, 6.0 × 10 -7 M; 6-OHNP, 6.0 × 10-8 M; 8-OHNP, 9.0 × 10-7 M. On the contrary, 8-OHNP exhibited the strongest antiestrogenic and antiandrogenic activities of the three isomers. 1.0 × 10-6 M of 8-OHNP inhibited 32 and 90% of β-galactosidase activity induced by 1.0 × 10-9 M of E2 and 1.0 × 10-8 M of 5α-dihydrotestosterone (DHT), respectively. These findings point out the necessity for detailed investigation of environmental sources and distributions of OHNPs as well as the parent 1-NP.
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| 35.
論文 |
論文
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Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />Project Number 14404021, Peport of Research Project ; Grant-in-Aid for Scientific Research(B)(2), fr
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om April 2002 to March 2006, Edited by Muramoto,Ken-ichiro<br />Kamata, Naoto<br />Kawanishi, Takuya<br />Kubo, Mamoru<br />Liu, Jiyuan<br />Lee, Kyu-Sung , 人工衛星データ活用のための東アジアの植生調査、課題番号14404021, 平成14年度～平成17年度科学研究費補助金, 基盤研究（B)(2)研究成果報告書, 研究代表者：村本, 健一郎, 金沢大学自然科学研究科教授
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| 36.
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論文
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小村, 和久 ; 稲垣, 美幸 ; 西川, 方敏 ; 中西, 孝 ; 早川, 和一 ; 唐, 寧 ; 楊, 小陽 ; 飯田, 孝夫 ; 森泉, 純 ; Komura, Kazuhisa ; Inagaki, Miyuki ; Nishikawa, Katatoshi ; Hayakawa, Kazuichi ; Tang, Ning ; Yang, Xiaoyang ; Iida, Takao ; Moriizumi, Jyun
概要:
金沢大学環日本海域環境研究センター<br />Variations of radiation levels before and after the Noto Hanto Earthquake in 2007 have been analy
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zed from the point of view of environmental radioactivity. The 210Pb activities in the airborne particles are collected from Nishi-Futamata in Wajima, are analyzed. The Radon activity at Hegura Island located 50km North of Wajima, and the spatial gamma rays at Nishi-Futamata are measured since April 21, 2007. Abnormal increase of 210Pb activity started 3 weeks before the earthquake are found, suggesting the maximum value just before the earthquake, because it decrease to normal level after 2 weeks. Increase of radon level was not observed at Hegura Island, however, increase of radiation level at Nishi-Futamata area continued for 6 weeks after the earthquake, and settled to normal level in middle of May 2007.<br />環境放射能の観点から能登半島地震発生前後の放射能関連のデータの解析を試みた.解析したのは,輪島市西二又地区で採取した大気浮遊塵中の210Pb,輪島沖50kmに位置する舳倉島のラドン濃度,地震発生後の4月21日から西二又地区で連続測定を実施した空間γ線レベルの3項目である.その結果,地震発生約3週間前から大気浮遊塵試料のラドンの娘核種210Pbの濃度が増加し,地震直前にピークに達した後に低下に転じ,約2週間後にほぼ平常値に回復していたことが分かった.舳倉島のラドンには地震の影響は見られなかったが,西二又における空間γ線レベルはラドンに由来すると考えれる高い値が約6週間後も続き5月中頃に平常値に戻ったことが明らかになった.
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| 37.
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論文
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Hayakawa, Kazuichi ; Miyoshi, Yasuko ; Kurimoto, Hiroaki ; Matzushima, Yuko ; Takayama, Nariaki ; Tanaka, Seishi ; Miyazaki, Motoichi ; 早川, 和一 ; 三好, 裕子 ; 栗本, 博昭 ; 松島, 優子 ; 高山, 成明 ; 田中, 星司 ; 宮崎, 元一
概要:
金沢大学理工研究域自然システム学系<br />A HPLC determination method for methamphetamine (MA) and its metabolites in the urine samples of
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abusers has been developed. MA, amphetamine (AP), norephedrine (NE), p-hydroxymethamphetamine (pOHMA), p-hydoroxyamphetamine (pOHAP) and an internal standard, namely β-phenylethylamine (PEA) were derivatized with dansyl chloride. They were separated on a reversed phase column with gradient elution using an acetonitrile/tetrahydrofuran/imidazole buffer mobile phase and chemilumigenically determined using bis(2, 4, 6-trichlorophenyl)-oxalate/hydrogen peroxide as post column reagents. The lower determination limits were as low as 1×10-14-3×10-14mol. AP, NE, pOHAP and PEA were derivatized with naphthalene-2, 3-dicarboxaldehyde, and were separated on a reversed phase column using an acetonitrile/imidazole buffer mobile phase and chemilumigenically determined. The lower determination limits were 3×10-16-1.5×10-15mol. Enzymatic hydrolysis of glucuronides of pOHMA (pOHMAG) and pOHAP (pOHAPG) allowed them to be determined as pOHMA and pOHAP, respectively. After adjusting the pH of the urine samples to 10.5 and adding PEA, all metabolites except glucuronides were extracted quantitatively into chloroform-isopropanol (3 : 1). Utilizing the two methods, MA and all metabolites were determined in urine samples of MA abusers. The tendency, in order of decreasing concentration was : [MA]>[A]>[pOHMAG]>[pOHMA]>[NE]>[pOHAPG]>[pOHAP]. Although ephedrine (EP) was detected in several samples, it was not considered to be a metabolite of MA but rather a component derived from cough medicine.
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| 38.
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論文
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Bekki, Kanae ; Takigami, Hidetaka ; Suzuki, Go ; Tang, Ning ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />金沢大学自然科学研究科<br />Several polycyclic aromatic hydrocarbons and nitrated polycyclic aromatic hydrocarb
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ons (PAHs/NPAHs) such as benzo[a]pyrene and 1-nitropyrene are mutagens and/or carcinogens. These compounds secondarily generate PAH hydroxides, ketones, and quinones through atmospheric and metabolic reactions. The health effects of these compounds is now an important social concern. For example, lung cancer, bronchitis, whistling and so on. In this work, we evaluated toxicities of 25 PAH derivatives (hydroxides, ketones and quinones) in terms of aryl hydrocarbon receptor (AhR) binding and thyroid hormone-related endpoints using three in vitro bioassays: dioxinresponsive chemical-activated luciferase gene expression (DR-CALUX), thyroid receptor β chemical-activated luciferase gene expression (TRβ-CALUX), and competitive human transthyretin-binding (TTR-binding) assays. Eleven of the 25 PAH derivatives had AhR agonist activity, six had AhR antagonist activity and seven had TRpotentiation activity in the TR-CALUX. Furthermore, PAH quinones and hydroxides had strong TTR-binding activity. 3,4-Dihydrobenz[a]anthracen-1(2 H)-one had the strongest agonist activity (EC20: 0.4μM) as determined by DR-CALUX. PAH ketones showed stronger activity than the control and significant difference by statistical analysis. Benzo[c]phenanthrene-[1,4]-quinone was the most TTR-active compound (IC50: 2.5μM). Both PAH ketones and quinones, which have functional groups with low polarity, had significant activities in all tested assays. These in vitro results suggest that PAH derivatives might have various toxic activities in animals. For estimating the health effects and accessing the environmental risks of PAHs, further studies on the toxicity mechanisms are necessary. ©2009 The Pharmaceutical Society of Japan.
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| 39.
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論文
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Suzuki, Nobuo ; Hayakawa, Kazuichi ; Kameda, Takayuki ; Toriba, Akira ; Tang, Ning ; Tabata, Makoto J. ; Takada, Koji ; Wada, Shigehito ; Omori, Katsunori ; Srivastav, Ajai K. ; Mishima, Hiroyuki ; Hattori, Atsuhiko
概要:
金沢大学環日本海域環境研究センター生物多様性研究部門<br />AAims: We previously demonstrated that monohydroxylated polycyclic aromatic hydrocarbons
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(OHPAHs) bound to a human estrogen receptor (ER) by a yeast two-hybrid assay, but polycyclic aromatic hydrocarbons did not have a binding activity. Therefore, the direct effect of 3-hydroxybenz[a]anthracene (3-OHBaA) and 4-hydroxybenz[a]anthracene (4-OHBaA) on osteoclasts and osteoblasts in teleosts was examined. As a negative control, 1-hydroxypyrene (1-OHPy), which has no binding activity to human ER, was used. Main methods: The effect of OHPAHs on osteoclasts and osteoblasts was examined by an assay system using teleost scale as each marker: tartrate-resistant acid phosphatase for osteoclasts and alkaline phosphatase for osteoblasts. Changes in cathepsin K (an osteoclastic marker) and insulin-like growth factor-I (IGF-I) (an osteoblastic marker) mRNA expressions in 4-OHBaA-treated goldfish scales were examined by using a reverse transcription-polymerase chain reaction. Key findings: In both goldfish (a freshwater teleost) and wrasse (a marine teleost), the osteoclastic activity in the scales was significantly suppressed by 3-OHBaA and 4-OHBaA, although 1-OHPy did not affect the osteoclastic activity. In reference to osteoblasts, the osteoblastic activity decreased with both 3-OHBaA and 4-OHBaA and did not change with the 1-OHPy treatment. However, 17β-estradiol (E2) significantly increased both the osteoclastic and osteoblastic activities in the scales of both goldfish and wrasse. The mRNA expressions of both cathepsin K and IGF-I decreased in the 4-OHBaA-treated scales but increased in the E2-treated scales. Significance: The current data are the first to demonstrate that 3-OHBaA and 4-OHBaA inhibited both osteoclasts and osteoblasts and disrupted the bone metabolism in teleosts. © 2009 Elsevier Inc. All rights reserved.
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| 40.
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論文
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Suzuki, Nobuo ; Hayakawa, Kazuichi ; Kameda, Takayuki ; Toriba, Akira ; Tang, Ning ; Tabata, Makoto J. ; Takada, Koji ; Wada, Shigehito ; Omori, Katsunori K. ; Srivastav, Ajai ; Mishima, Hiroyuki ; Hattori, Atsuhiko
概要:
金沢大学環日本海域環境研究センター生物多様性研究部門<br />Aims: We previously demonstrated that monohydroxylated polycyclic aromatic hydrocarbons
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(OHPAHs) bound to a human estrogen receptor (ER) by a yeast two-hybrid assay, but polycyclic aromatic hydrocarbons did not have a binding activity. Therefore, the direct effect of 3-hydroxybenz[a]anthracene (3-OHBaA) and 4-hydroxybenz[a]anthracene (4-OHBaA) on osteoclasts and osteoblasts in teleosts was examined. As a negative control, 1-hydroxypyrene (1-OHPy), which has no binding activity to human ER, was used. Main methods: The effect of OHPAHs on osteoclasts and osteoblasts was examined by an assay system using teleost scale as each marker: tartrate-resistant acid phosphatase for osteoclasts and alkaline phosphatase for osteoblasts. Changes in cathepsin K (an osteoclastic marker) and insulin-like growth factor-I (IGF-I) (an osteoblastic marker) mRNA expressions in 4-OHBaA-treated goldfish scales were examined by using a reverse transcription-polymerase chain reaction. Key findings: In both goldfish (a freshwater teleost) and wrasse (a marine teleost), the osteoclastic activity in the scales was significantly suppressed by 3-OHBaA and 4-OHBaA, although 1-OHPy did not affect the osteoclastic activity. In reference to osteoblasts, the osteoblastic activity decreased with both 3-OHBaA and 4-OHBaA and did not change with the 1-OHPy treatment. However, 17β-estradiol (E2) significantly increased both the osteoclastic and osteoblastic activities in the scales of both goldfish and wrasse. The mRNA expressions of both cathepsin K and IGF-I decreased in the 4-OHBaA-treated scales but increased in the E2-treated scales. Significance: The current data are the first to demonstrate that 3-OHBaA and 4-OHBaA inhibited both osteoclasts and osteoblasts and disrupted the bone metabolism in teleosts. © 2009 Elsevier Inc. All rights reserved.
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| 41.
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論文
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早川, 和一 ; Hayakawa, Kazuichi
概要:
1.ニトロアレーン分析法の改良:既報の化学発光検出HPLCによるトロアレーン分析システムにニトロアレーン分離用ODSカラム,亜鉛還元カラム,高圧流路切り替えバルブ等を導入することにより,極微量ニトロアレーンの分析システムを完成した.これによ
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り,数mg以下の大気粉じん中の2-ニトロフルオランテン(2-NF),2-ニトロピレン(2-NP),4-NP,6-ニトロクリセン(6-NC)等を定量可能とした.2.ディーゼル粉塵抽出物の直接変異原性におけるニトロアレーンの寄与:ディーゼル粉塵のbenzen-ethanol(3:1)抽出物をシリカゲルカラムクロマトグラフィー(n-hexane,dichloromethane,methanolの混合溶媒)で5分画した.Ames試験による直接変異原性(S.typhimuriumYG1024株)は高極性溶媒(dichloromethane-methanol及びmethanol)の2分画に集中し,ニトロアレーンはこのうちの前者に集中した.直接変異原性におけるニトロアレーン(8種)の寄与率はこの分画で50%余り,全分画合計の約1/3に達し,大きいことが明らかになった.3.札幌,東京,金沢の大気環境比較:金沢市,東京都,札幌市の大気中DNP及び1-NP濃度は札幌≧東京>金沢の純に低くなったが,都心は都市による差は小さかった.3都市の中では,札幌が1,3-,1,6-,1,8-ジニトロピレン(DNP)濃度に対する1-NP濃度の比が最も大きく,その理由の一つとして,ディーゼル車の保有台数の割合が高いことが考えられた.濃度推移は日内変動(昼高夜低)及び季節変動(夏低冬高)を呈したが,都市により程度に差があった.4.大気中のニトロアレーンの分解と二次生成:金沢市内の都心と郊外の大気中ニトロアレーンの比較により,DNP及び1-NPは大気輸送中に分解し,その主要因が太陽による光分解であることがわかった.また、2-NFと2-NPはディーゼル粉塵には検出されず郊外ほど存在比が大きくなることより,大気中で二次生成することが推定された.<br />(1) We introduced another separation column (ODS), a zinc reducer column and a switching valve into the nitroarene analyzer, a HPLC equipped with a chemiluminescence detector, to determine trace levels of nitroarenes.(2) Benzene-ethanol extracts from diesel exhaust particulates were separated into 5 fractions on a silica-gel column with mixtures of n-hexane, dichloromethane and methanol. The strong direct-acting mutagenicities were observed in the dichloromethane-methanol and methanol fractions in the Ames test using the S.typhimurium YG1024 strain and nitroarenes were mainly in the former fraction of the two. The mutagenic contribution of nitroarenes were 1/3 of the all fractions. The large contribution of nitroarenes to the mutagenicity of urban air suggests that the monitoring of nitroarenes is very important for assessing the risk of air pollutants.(3) Concentrations of 1,3-, 1,6- and 1,8-dinitropyrenes (DNPs) and 1-nitropyrene (NP) in urban air were in the following decreasing order, Sapporo>Tokyo>Kanazawa. However, the concentrations in downtown areas of the three cities were at similar levels. The relative concentration of DNPs to that of 1-NP was the highest in Sapporo. As a reason, the large ration of diesel-engine vehicles was considered. Their concentrations showed diurnal and seasonal variations.(4) The relative concentrations of DNPs and 1-NP to polycyclic aromatic hydrocarbons were lower in the suburban areas than in the downtown areas, suggesting that DNPs and 1-NP degradated in the presence of sun light during the transportation. On the other hand, the fact that both 2-nitrofluoranthene (NF) and 2-NP were not detected in diesel exhaust particulates but detected in airborne particulates suggested that these two compounds were formed in air.<br />研究課題/領域番号:08672472, 研究期間(年度):1996–1997<br />出典：「未規制大気汚染物質ニトロアレーンの動態解析とその軽減に関する基礎研究」研究成果報告書 課題番号08672472(KAKEN：科学研究費助成事業データベース（国立情報学研究所）) 本文データは著者版報告書より作成
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| 42.
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論文
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Koyama, Kazuo ; Hirao, Takashi ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
The quality of starch-containing foods may be significantly impaired by contamination with very small amounts of α-amyla
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se, which can enzymatically hydrolyze the starch and cause viscosity loss. Thus, for quality control, it is necessary to have an analytical method that can measure low amylase activity. We developed a sensitive analytical method for measuring the activity of α-amylase (from Bacillus subtilis) in starch-containing foods. The method consists of six steps: (1) crude extraction of α-amylase by centrifugation and filtration; (2) α-amylase purification by desalting and anion-exchange chromatography; (3) reaction of the purified amylase with boron-dipyrromethene (BODIPY)-labeled substrate, which releases a fluorescent fragment upon digestion of the substrate, thus avoiding interference from starch derivatives in the sample; (4) stopping the reaction with acetonitrile; (5) reversed-phase solid-phase extraction of the fluorescent substrate to remove contaminating dye and impurities; and (6) separation and measurement of BODIPY fluorescence by HPLC. The proposed method could quantify α-amylase activities as low as 10mU/mL, which is enough to reduce the viscosity of starch-containing foods. © 2012 John Wiley & Sons, Ltd.
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| 43.
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論文
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Tang, Ning ; Yoda, Yoshiko ; Otani, Naruhito ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi ; Shima, Masayuki
概要:
Twenty-one data sets composed of readings collected by atmospheric ozone monitors worn by individuals on their clothing
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and installed outside their home or office were collected using Ogawa passive ozone samplers in southeastern Hyogo prefecture, Japan from September 12 to 13, 2011. The concentrations of personal and outdoor ozone ranged from not detectable to 23.2 ppb and from 4.7 to 38.3 ppb, respectively. The mean concentration of personal exposure to ozone was 3.7 ppb and was significantly lower than that of outdoor ozone (18.5 ppb). This suggests that the concentrations of outdoor ozone affect personal ozone exposure. However, in this study, we found no correlation between the concentrations of personal ozone and the total time spent outdoors or the time of day the individual was outside. In contrast, the mean concentrations of outdoor ozone were similar to those of ozone measured at the 12 nearest Ambient Monitoring Stations (AMSs). However, when the AMS was situated near a main road, the regional ozone levels were underestimated.
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| 44.
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Nishimura, Masayuki ; Hayashi, Morimasa ; Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
The selective effect of triethylenetetramine (Trien) on the retention behavior of sulfate in ion chromatography was stud
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ied. When Trien was added to an eluant as a counter ion, retention of sulfate was selectively shortened, while retention times of monovalent anions did not change. The cause for this phenomenon was the complexation of sulfate and Trien in an eluant. The stability constants of divalent sulfate-trivalent Trien and -tetravalent Trien complexes were estimated to be 936 and 4213 (40°C), respectively. As a practical application of this phenomenon, weakly retained monovalent species can be very well separated from both water dip and other species without prolonging the interval of injections.
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| 45.
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論文
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Chen, Chingtan ; Hayakawa, Kazuichi ; Imanari, Toshio ; Tamura, Zenzo
概要:
An analytical method of 5-chloro-7-iodo-8-quinolinol (Clioquinol or Chinoform) (CF) conjugates was established by high p
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erformance liquid chromatography. The chromatographic conditions were as follows : column, SAX (50 cm×2 mm i.d.) ; mobile phase, I (0.02M borate buffer-0.1M KCl, pH9.5), II (0.02M borate buffer-0.5M NaClO4, pH 9.5) ; gradient, 0→25% (II/I+II) at 3%/min ; column pressure, 500 psi ; flow rate, 1 ml/min ; detector, ultraviolet-detector at 254 mμ. Urine samples of a man administered CF were injected directly to the column, and the major metabolite, CF glucuronide was determined, while very small amounts of CF sulfate was detected.
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| 46.
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論文
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Hayakawa, Kazuichi ; Bekki, Kanae ; Yoshita, Morio ; Tachikawa, Chihiro ; Kameda, Takayuki ; Tang, Ning ; Toriba, Akira ; Hosoi, Shinzo
概要:
Estrogenic and antiestrogenic activities of 19 quinoid polycyclic aromatic hydrocarbons (PAHQs) and 9 ketone PAHs were e
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valuated by the yeast two-hybrid assay using yeast cells expressing estrogen receptor-α (ERα). Binding affinity of PAHQs to ERα was assayed by the polarized fluorescence method using FluormoneTM ES2. Ten PAHQs having 3-5 rings showed antiestrogenic activities. The most strongly antiestrogenic PAHQs were 1,4-chrysenequinone and 5,6-chrysenequinone. On the other hand, benzo[a]pyrene-3,6-quinone showed the strongest estrogenic activity. However, the other compounds tested did not show so strong estrogenic/antiestrogenic activities. Binding affinity to ER was required but not sufficient for estrogenic/antiestrogenic activities of PAHQs. The length-to-breadth ratios of the rectangular planes surrounding the ring molecules and the distances between the oxygen atom of the carbonyl group and farthest hydrogen atom of estrogenic/antiestrogenic PAHQs were in narrow ranges, suggesting a structure-activity relationship. As interactions between active PAHQ and ER, hydrogen bonding between carbonyl groups and amino acid residues and van der Waals forces were considered.
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| 47.
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論文
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Hirose, Toshiharu ; Morito, Keiko ; Kizu, Ryoichi ; Toriba, Akira ; Hayakawa, Kazuichi ; Ogawa, Sumito ; Inoue, Satoshi ; Muramatsu, Masami ; Masamune, Yukito
概要:
Benzo[a]pyrene (BaP), a major environmental pollutant, is metabolized in vivo and produces many hydroxy derivatives. The
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estrogenic/antiestrogenic activities of twelve monohydroxy derivatives of BaP (1- through 12-OH species) were investigated using competition binding to human estrogen receptor (hER)α and hERβ, and the gene expression assay of the yeast two-hybrid system. BaP and 5-OH BaP did not bind to either hER. The other monohydroxy derivatives bound to both hERs. These compounds bound more strongly to hERβ than to hERα. Using the yeast two-hybrid assay system, 1-, 2-, 3-, and 9-OH BaP induced β-galactosidase with hERβ but not with hERα. This suggested that these compounds were estrogenic. In the presence of 10-9 M 17 β-estradiol, 8-OH BaP inhibited the induction of β-galactosidase. Because 8-OH BaP did not affect cell growth, it appeared to be an antiestrogen. The present study shows that most of the monohydroxy derivatives of BaP bind to estrogen receptors (ERs), and several of them have estrogenic or antiestrogenic activity.
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| 48.
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Sasaki, Hideki ; Yonekubo, Jun ; Hayakawa, Kazuichi
概要:
Current on-line solid-phase extraction methods combined with HPLC for shortening the clean-up operation are not suitable
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for simultaneously detecting compounds that have a wide variety of hydrophobicities. To solve these problems, we designed a new on-line sample preparation system. The system consists of an eluting pump, a mixing TEE connector, a 10-port 2-position valve and a solid-phase extraction precolumn. The eluate from the precolumn is diluted with a weak solvent from the HPLC at the TEE connection to load low hydrophobic compounds onto the analytical column. The proposed on-line sample preparation system was successfully applied to the simultaneous analysis of 21 pesticides in river water using LC/TOF-MS. In this method, the recoveries from river water samples were 67 to 126% (mean 83%), the reproducibility (CV%) was in the range from 1.1 to 11% (mean 5.6%), the calibration curve was linear in the range from 1 ppb to 500 ppb (r > 0.999) and the detection limits (S/N = 3) were in the range from 0.0034 ppb (daimuron) to 3.3 ppb (oxine-copper). 2006 © The Japan Society for Analytical Chemistry.
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| 49.
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論文
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Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />Proceeding : International Symposium of Kanazawa University 21st-Century COE Program Vol.2(2004),Sch
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edule: February 29(SUN)-March 3(WED), Venue: 29 FEB, Ishikawa Life-Long Learning Center(Former Prefectural Government Building) / 1-3 MAR Kanazawa Art Hall, Organized by: Kanazawa University 21st-Century COE Program / Ishikawa International Cooperation Research Centre / United Nations University-Institute of Advanced Studies, Supported by: Ishikawa Prefectural Government / City of Kanazawa, Eds : Hayakawa, Kazuichi / Kizu, Ryoichi / Kamata, Naoki
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| 50.
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論文
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Chetiyanukornkul, Thaneeya ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
金沢大学大学院自然科学研究科<br />Proceeding : International Symposium of Kanazawa University 21st-Century COE Program Vol.2(2004),Sch
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edule: February 29(SUN)-March 3(WED), Venue: 29 FEB, Ishikawa Life-Long Learning Center(Former Prefectural Government Building) / 1-3 MAR Kanazawa Art Hall, Organized by: Kanazawa University 21st-Century COE Program / Ishikawa International Cooperation Research Centre / United Nations University-Institute of Advanced Studies, Supported by: Ishikawa Prefectural Government / City of Kanazawa, Eds : Hayakawa, Kazuichi / Kizu, Ryoichi / Kamata, Naoki
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| 51.
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論文
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Tamura, Kenji ; Shima, Masayuki ; Tang, Ning ; Hayakawa, Kazuichi ; Sun, Guifan
概要:
国立環境研究所<br />千葉大学<br />金沢大学大学院自然科学研究科<br />China Medical University<br />Proceeding : International Symposium of Kanazaw
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a University 21st-Century COE Program Vol.2(2004),Schedule: February 29(SUN)-March 3(WED), Venue: 29 FEB, Ishikawa Life-Long Learning Center(Former Prefectural Government Building) / 1-3 MAR Kanazawa Art Hall, Organized by: Kanazawa University 21st-Century COE Program / Ishikawa International Cooperation Research Centre / United Nations University-Institute of Advanced Studies, Supported by: Ishikawa Prefectural Government / City of Kanazawa, Eds : Hayakawa, Kazuichi / Kizu, Ryoichi / Kamata, Naoki
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| 52.
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論文
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Okamura, Kazumasa ; Kizu, Ryoichi ; Hayakawa, Kazuichi ; Toriba, Akira
概要:
金沢大学大学院自然科学研究科<br />Proceeding : International Symposium of Kanazawa University 21st-Century COE Program Vol.2(2004),Sch
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edule: February 29(SUN)-March 3(WED), Venue: 29 FEB, Ishikawa Life-Long Learning Center(Former Prefectural Government Building) / 1-3 MAR Kanazawa Art Hall, Organized by: Kanazawa University 21st-Century COE Program / Ishikawa International Cooperation Research Centre / United Nations University-Institute of Advanced Studies, Supported by: Ishikawa Prefectural Government / City of Kanazawa, Eds : Hayakawa, Kazuichi / Kizu, Ryoichi / Kamata, Naoki
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| 53.
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論文
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Kakimoto, Hitoshi ; Oka, Hideo ; Harada, Yumiko ; Ushijima, Shigeru ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi
概要:
Dioxins are present as impurities in agrochemicals applied to the soil. To examine the possibility that dioxins end up in the atmosphere, we compare the homologue composition and some characteristic isomer distributions of
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polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) in air and soil samples collected at sites in Ishikawa Prefecture, Japan. Tetrachloro dibenzo-p-dioxin (TeCDD) was the most abundant PCDD homologue in the air samples, while octachloro dibenzo-p-dioxin (OCDD) was the most abundant PCDD homologue in the soil samples. However, at several site, the most predominant homologue in the soil sample was not OCDD but TeCDD. The mean ratio of TeCDDs to PCDDs in the air samples was significantly smaller in winter than in other seasons, but no such seasonal variation was observed in the distribution of PCDF homologues. The abundance of PCDF homologues was inversely related to the number of chlorine substitutions in the air samples. The contribution of each toxic isomer (2,3,7,8-chlorine-substituted) to the total toxicity equivalency quantity (TEQ) in the air samples tended to be intermediate between their contributions to the TEQs in the soil and cinder samples. This result suggested that the air samples were influenced by both soil/dust suspension and combustion. In order to clarify the contributions of agrochemicals to dioxins in the air, we focused on the ratios of several characteristic isomers that are indicators of agrochemicals (chloronitrophen: CNP and pentachlorophenol: PCP) to their homologues. Significant decreases in the ratios of the isomers to their homologues in the air samples were observed only in winter, probably as a result of suppression of dust suspension by the snow cover. Therefore, the contribution of combustion to the dioxin concentration in the air was thought to be relatively large in winter.
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| 54.
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Tang, Ning ; Hakamata, Mariko ; Sato, Kousuke ; Okada, Yumi ; Yang, Xiaoyang ; Tatematsu, Michiya ; Toriba, Akira ; Kameda, Takayuki ; Hayakawa, Kazuichi
概要:
Total suspended particulates were collected at a Japanese remote background site (Noto Air Monitoring Station; NAMS) on
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the Noto Peninsula from September 2004 to June 2014. Nine polycyclic aromatic hydrocarbons (PAHs) in the particulates (fluoranthene, pyrene, benz[a]anthracene, chrysene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[a]pyrene, benzo[ghi]perylene and indeno[1,2,3-cd]pyrene) were determined by HPLC with fluorescence detection. The mean total concentrations of the nine PAHs in the cold season (November to May for the years 2004-2014) was 670 pg m-3 (range 37-4100 pg m-3). The mean total concentration in the warm season (June to October for the same period) was 170 pg m-3 (range 31-960 pg m-3). The atmospheric PAH level at NAMS decreased in recent years, although no significant change was found in the warm season. An analysis of meteorological conditions showed that the atmospheric PAHs at NAMS were long range transported from Northeast China in the cold seasons and were contributed to by Japanese domestic sources in the warm seasons. Lower concentration ratios of reactive PAHs to their isomers at NAMS also supported these results. Activities associated with the Beijing Olympic and Paralympic Games in 2008 and reconstruction after the 2007 Noto Hanto earthquake may have contributed to the yearly variations of atmospheric PAH levels at NAMS during the period 2007-2009. Source control measures implemented by the Chinese and Japanese governments appear to have been effective in decreasing the atmospheric PAH levels at NAMS in recent years. © 2015 Elsevier Ltd.<br />Embargo Period 24 months
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| 55.
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論文
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Kizu, Ryoichi ; Ikeda, Tomoko ; Hayakawa, Kazuichi ; Miyazaki, Motoichi
概要:
Metal-catalyzed hydrolyses of clioquinol-glucuronide (CG) and clioquinol-sulfate (CS) in the rabbit body were studied following intravenous injection of Cu (II)- or Fe (III)-gluconic acid complex system 6h after the oral administration of
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clioquinol (C). Molar fractions of C, CG and CS remained nearly constant through 24 h after administration of C at doses of 90-300mg/kg weight in rabbits which were not injected with Cu (II) or Fe (III). Therefore, molar fractions of C, CG and CS after the injection of Cu (II) or Fe (III) were monitored to clarify the metabolic changes of C. In rabbits injected with 2.5mg of Cu (II)/kg weight, C rapidly increased and CG and CS decreased after the injection of Cu (II). In rabbits injected with 20 mg of Fe (III)/kg weight, C and CS slowly increased and CG decreased until 18h after the injection of Fe (III). The patterns of the changes in molar fractions of C, CG and CS are consistent with the catalytic features of Cu (II) and Fe (III) seen in previous studies, and therefore, the changes in molar fractions of C, CG and CS observed in this study were considered to have been brought about as a result of metalcatalyzed hydrolyses of CG and CS or metal-catalyzed hydrolysis of CG in the rabbit body.
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| 56.
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論文
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Yamada, Maromu ; Nakamura, Kaya ; Kameda, Takayuki ; Kobayashi, Fumihisa ; Matsuki, Atsushi ; Tsuiki, Hisanaga ; Higaki, Seigo ; Iwasaka, Yasunobu ; Hayakawa, Kazuichi
概要:
Polycyclic aromatic hydrocarbons (PAHs) are known as carcinogenic and/or mutagenic substances, and are present at high c
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oncentration in polluted environments. It has recently been reported that spore-forming bacteria (e.g., Bacillus spp.) can be transported long distances alive in the atmosphere, which raises the possibility that some of the transported bacteria could have adverse effects on human health. There is thus a need for filters that can remove gaseous PAHs from the air that people breathe and that can inhibit bacterial growth on the filters. We focused on metallophthalocyanine derivatives (M-Pc) which are known to adsorb PAHs as well as to inhibit the growth of bacteria as a potential filtering agent. In this study, we developed different types of M-Pc-supported rayon fibers by changing central metals, functional groups, concentrations of M-Pc and rayon types, and evaluated their removal effects by measuring adsorption rates of 3- and 4-ring PAHs with a HPLC and growth curves of Bacillus sp. with a spectrophotometer. The results showed that both the effects depended on functional groups and concentrations of M-Pc, and rayon types. The most effective combination was observed in Fe-Pc with sulfo group supported on cationized rayon fiber at the concentration of 2 to 3.3 wt%. Central metal species of M-Pc were influenced only on the antibacterial properties. This fiber would be applicable to filtering agents and textiles.
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| 57.
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論文
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Tang, Ning ; Suzuki, Genki ; Morisaki, Hiroshi ; Tokuda, Takahiro ; Yang, Xiaoyang ; Zhao, Lixia ; Lin, Jinming ; Kameda, Takayuki ; Toriba, Akira ; Hayakawa, Kazuichi
概要:
Airborne particulates were collected at an urban site (site 1) from 2004 to 2010 and at a suburban site (site 2) in 2010
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in Beijing. Nine polycyclic aromatic hydrocarbons (PAHs) and five nitropolycyclic aromatic hydrocarbons (NPAHs) in the airborne particulates were determined by HPLC with fluorescence and chemiluminescence detection, respectively. The concentrations of PAHs and NPAHs were higher in heating season than in non-heating season at the two sites. Both the concentrations of PAHs and NPAHs decreased in the non-heating season but only the concentrations of NPAHs decreased in heating season at site 1, from 2004 to 2010. These findings suggest that source control measures implemented by the city of Beijing helped to reduce air pollution in Beijing. The concentrations of PAHs increased at site 1 in 2010, possibly because of the transport of emissions from windward other areas, such as Shanxi province. Several diagnostic ratios of PAHs and NPAHs showed that the different sources contributed to Beijing's air pollution, although coal combustion was the main source in the heating season and vehicle emission was the main source in the non-heating season. An analysis of physical parameters at Beijing showed that high wind speed can remove atmospheric PAHs and NPAHs in the heating season and that high relative humidity can remove them in the non-heating season. © 2017 Elsevier Ltd<br />Embargo Period 12 months
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| 58.
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Tang, Ning ; Taga, Rina ; Hattori, Tetsuyuki ; Toriba, Akira ; Kizu, Ryoichi ; Hayakawa, Kazuichi ; Tamura, Kenji ; Kakimoto, Hitoshi
概要:
金沢大学大学院自然科学研究科<br />国立環境研究所<br />石川県保健環境センター<br />Proceeding : International Symposium of Kanazawa University 21st-Centu
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ry COE Program Vol.2(2004),Schedule: February 29(SUN)-March 3(WED), Venue: 29 FEB, Ishikawa Life-Long Learning Center(Former Prefectural Government Building) / 1-3 MAR Kanazawa Art Hall, Organized by: Kanazawa University 21st-Century COE Program / Ishikawa International Cooperation Research Centre / United Nations University-Institute of Advanced Studies, Supported by: Ishikawa Prefectural Government / City of Kanazawa, Eds : Hayakawa, Kazuichi / Kizu, Ryoichi / Kamata, Naoki
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| 59.
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早川, 和一 ; Hayakawa, Kazuichi
概要:
(1)大気粉じんから変異原物質を抽出するために使用されている様々な有機溶媒の中から,ニトロアレーン分析法とAmes法の併用に最適な抽出溶媒の検索をおこなった.1,3-, 1,6-, 1,8-ジニトロピレン(DNP),1-ニトロピレン(NP)
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及び直接変異原性物質の抽出効率はベンゼン-エタノール(3:1),アセトニトリル,エタノール,メタノールの順で高く,毒性を考慮するとこれらの中ではエタノールが最も適していると考えられた. (2)基本ニトロアレーン分析計では試料の前処理として必要な還元操作を,分析システムに亜鉛を充填した還元用カラムを導入することにより省略した.また,分離度を向上させるため,試料を還元後,最も還元成績体の濃度が高い部分をスイッチングバルブでハードカッティングして,分析カラムに導入した.これによって簡単な前処理のみで大気粉じん中の1,3-, 1,6-, 1,8-DNP及び1-NPが定量可能となった. (3)ニトロアレーン分析法の前処理操作では直接変異原性ニトロアレーンと同時に間接変異原性多環芳香族炭化水素(PAH)も定量化に抽出される.この試料をニトロアレーン分析計とPAH分析のための蛍光検出HPLCシステムをスイッチングバルブで併合したシステムに適用することで,両者の同時分析が可能となった.その結果,上記の4種ニトロアレーンに加えて8種PAHも1時間以内に定量可能となった. (4)大気中で2次生成することが知られている2-, 4-NP,2-ニトロフルオランテン,6-ニトロクリセンと1-NPを同時に分析するため,基本ニトロアレーン分析システムに妨害物質を除去するための精製用ODSカラム,還元を自動化する亜鉛充填カラムと分離・検出を改善する濃縮用ODSカラムを導入した.本法によって測定した金沢市市街地大気中の上記化合物濃度は10^<-12>-10^<-16>molm^<-3>の範囲にあった.<br />(1) Both the nitroarene analyzer and the Ames test are necessary in the study on mutagenic nitroarenes. For the simultaneous use of these two methods, several solvent systems were tested to extract 1,3-dinitropyrene (1,3-DNP), 1,6-DNP,1,8-DNP and 1-nitropyrene (1-NP) as well as directacting mutagenic activity from airborne particulates. Benzene-ethanol, acetonitrile, ethanol and methanol gave the high efficiencies. Considering toxicities, ethanol seemed to be the best solvent.(2) Although the nitroarene analyzer determined trace levels of 1,3-, 1,6-and 1,8-DNPs and 1-NP in extracts from a few mg of airborne particulates, the reduction of nitroarenes to corresponding aminoarenes was required before injection. To remove this tedious treatment, a reducer column packed with zinc/glass beads was on-line introduced into the system. Considering the better resolution of aminoarenes, both the reducer column and a switching valve equipped with a heart-cutting loop were introduced just before the ODS separation column. This system could determine the above four compounds in extracts from airborne particulatates without pre-column reduction.(3) In the method, not only nitroarenes but also polycyclic aromatic hydrocarbons (PAHs) were quantitatively extracted from airborne partculates. To determine them simultaneously, both the nitroarene analyzer and a conventional high-performance liquid chromatograph with a fluorescence detector were combined using a switching valve. After the reduced sample solution was injected, four nitroarenes and eight PAHs were separately determined in the two different lines in 1h with high sensitivities.(4) Several mutagenic nitroarenes such as 2-, 4-NPs, 2-nitrofluoranthene and 6-nitrochrycene were formed in air in the presence of NOx. To determine these compounds, a reducer column packed with zinc/glass beads and two ODS columns, one for the clean-up and the other for the concentration, were introduced into the nitroarene analyzer. By the system, the above four compounds were detected in air. The fact that their ratios to 1,3-, 1,6-, 1,8-DNPs and 1-NP in rural air were larger than those in urban air suggested the formation of those compounds during the transportation. However, their mutagenic contributions were not large.<br />研究課題/領域番号:06557121, 研究期間(年度):1994–1995<br />出典：「ニトロアレーン分析計の試作」研究成果報告書 課題番号06557121(KAKEN：科学研究費助成事業データベース（国立情報学研究所）) 本文データは著者版報告書より作成
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| 60.
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早川, 和一 ; Hayakawa, Kazuichi
概要:
1.イオンクロマトグラフィ-(IC)の保持・溶出機構解析:溶離剤成分と試料成分の挙動解析から選択的ピ-ク増感・抑制の理論を提案し、微量リン酸の分析に応用した。Hooverモデルに基づく関係式に新しく溶離剤間分離係数を導入し、二塩基酸溶離液系
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でも試料成分と溶離静成分の挙動が理論的に推定できるようにした。2.自動前処理IC:カラムスイッチング法の導入により、陰イオン分析を妨害するアルカリ土類金属のオンライン除去ICを開発した。このシステムは、生活雑排水中のリン酸分析を妨害する成分のオンライン除去にも有効であった。また、電気伝導度検出ICで報告されている自動濃縮分析システムを吸光度検出ICについて考案した。このシステムは、極地氷床コアや雨水等の希薄環境試料の分析に有効であった。3.吸光度検出IC用機能性溶離剤:配位子交換吸光度検出IC理論に基づく光学異性有機酸の分析法を開発した。本法で前処理なしに清涼飲水中の添加リンゴ酸の分析ができた。4.炭酸のIC:大気中の二酸化炭素の妨害を除去して微量炭酸が分析できる窒素通気ーイオン排除クロマトグラフィ-を開発した。これにより雨水中の炭酸が数種の低級有機酸と同時分析できた。5.偏光吸光度検出法:吸光度検出セルの前後に二枚の偏光子を設置すると、吸光度変化量はセル内に存在する光学活性物質の濃度に比例するという偏光吸光度検出理論を提案した。本法は紫外・可視吸収がなく光学活性がある糖などの分析に適用でき、その検出感度も優れていた。6.化学発光検出HPLCによるニトロピレン類の超高感度分析法:オンライン電気化学還元ー化学発光検出HPLC及びオフライン化学還元ー化学発光検出HPLCによるニトロピレン類の超高感度分析法を開発した。これらの方法で、ニトロピレン類の主要排出源の一つと言われているディ-ゼル及びガソリン自動車排ガス中のジニトロピレンが分析できた。<br />(1) Theoretical studies on the retention and peak formation mechanism in ion chromatography (IC) : Following on from our previous work, a new theory "selective peak enhancement and suppression of conductivity detection IC" was evaluated. This theory was effectively used in the determination of trace level orthophosphate in sewage samples. Ion exchange chromatographic behavior of polyvalent eluent systems was evaluated theoretically by introducing a new parameter "the intereluent separation factor" in equations for Hoover's model.(2) Functional eluents for photometric detection IC : Both[Cu(en)_2SO_4 and[Cu(trien)]SO_4 were effective eluents for the sensitive determination of cations. Using a Na_2[Cu(edta)]- Na_2H_2 edta eluent, not only anions but also metal ions were deterifined as metal-edta anion chelates by photometric detection IC. These methods were effectively used in the determination of cations and anions in environmental water samples. Malic acid enantiomers were separately d etermined by photometric detection IC using a copper - tartaric acid complex eluent, based on a ligand-exchange formation mechanism. Malic acid, an apple juice additive, was determined by this method.(3) Determination of carbonate-carbon : Interfering atmospheric carbon dioxide dissolved in eluents was removed effectively by nitrogen purging. Using this equipment, trace level carbonate carbon as low as 10^<-6> M could be determined by photomeric detection IC as well as ion exclusion chromatography (conductivity detection). Carbonate-carbon in rain water was determined by this method.(4) Polarized photometric detection : When two polarizers were set on both sides of the flow sell of an absorbance detector, the intensity of natural light transmitted through the polarizers and the flow cell was changed according to the optically active compounds if passed through. The change in absorbance was in proportion to the concentration of the compound. Nonchromophoric optically active compounds such as sugars were sensitively determined using photometric detection HPLC without any derivatization.(5) Automatic pretreatment/HPLC system : The combination of column-switching system and a heart-cutting technique effectively removed interfering compounds in IC. This system was used to determine anions in river and rain water samples by photometric detection IC and orthophosphate in sewage samples by conductivity detection IC.(6) Determination of nitopyrenes by HPLC with chemiluminescence detection : A method of determining nitro-, nitroso- and aminopyrenes has been developed using HPLC with chemiluminescence detection after on-line electrochemical reduction. Determination method of 1, 3-, 1, 6-, 1, 8-dinitropyrenes and 1-nitropyrene has also been developed using HPLC with chemiluminescence detection after off-line chemical reduction. Utilizing these methods, dinitropyrenes and nitropyrene were determined in diesel- and gasoline-engine exhaust particulates.<br />研究課題/領域番号:02670975, 研究期間(年度):1990–1991<br />出典：「新しい吸光度検出方式高速液体クロマトグラフィーの応用研究: 環境汚染分析法の開発」研究成果報告書 課題番号02670975(KAKEN：科学研究費助成事業データベース（国立情報学研究所）) 本文データは著者版報告書より作成
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| 61.
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佐川, 岳人 ; 西, 香菜子 ; 納富, 美穂 ; 平岡, 龍之 ; 塚本, 和巳 ; 早川, 和一 ; Sagawa, Takehito ; Nishi, Kanako ; Notomi, Miho ; Hiraoka, Tatsuyuki ; Tsukamoto, Kazumi ; Hayakawa, Kazuichi
概要:
金沢大学理工研究域自然システム学系<br />生スィートバジルを乾燥する際に引き起こされる香りの変化を，香気成分バランスやスィートバジルの組織構造とそのレオロジー特性について，比較解析を行う事で，生スィートバジルの香りを維持する為に必要とさ
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れる因子の探索を行った．スィートバジルの香気寄与成分として特定したシネオール，リナロール，オイゲノール，オクタナール，1-オクタノール，(E)-2-ヘキセナール，(Z)-3-ヘキセノールの7種類の香気成分は官能評価の特徴を説明する因子となると考えられる．その中でも，生スィートバジルの香りを特徴づける因子としては，微量成分バランスが大きな役割を果たし，ハーブ自体には (E)-2ヘキセナールや (Z)-3-ヘキセノールが存在するが，それがハーブティーに溶出されずオクタナールが高い比率で溶出されることが重要であった．そのような性質を持つ組織構造は，葉内部の細胞壁の形状が乾燥工程を経ても維持されており，その状態は貯蔵弾性率の測定でも比較説明が可能であることが明らかになった．これらの結果により，ハーブの組織構造とハーブティーとして溶出される香気成分バランスに密接な関係がある可能性が示唆された．但し，今回確認された (E)-2-ヘキセナールや (Z)-3-ヘキセノールはみどりの香りと称される物質の1つである．これらの物質は植物中のリノレン酸や配糖体を前駆体として酵素が関与し発現するものであり12)，食品加工時に発生することも知られている14）～16) ．今後は配糖体量の変化と酵素の関係についても検討を行い，組織構造変化の香りに対する影響をより明確にしてゆく必要があると考える．しかしながら，細胞壁の損傷が少ない状態であった真空乾燥スィートバジルが生特有の香りを保持していたという事実から，乾燥工程を経ることで喫食時に感じる香りの違いは，単純な香気成分の増減という因子だけではなく，組織構造変化という因子からも説明できる可能性が示唆された．乾燥ハーブの香りに対する品質評価を行う上で，乾燥ハーブからハーブティーに抽出されてゆく香気成分のバランス変化や内部組織構造変化の比較といった多面的なアプローチは，今後の有効な評価手法の1つとなることが期待できる．<br />A quality evaluation method for dried herbs was studied with sweet basil leaves (fresh, air-dried, freeze-dried and vacuum-dried sweet basil leaves) as herbal teas, involving hot-water extraction. Sensory evaluation revealed that the flavor of herbal tea with vacuum-dried sweet basil leaves was similar to that with fresh leaves. Seven odor-active compounds (cineole, linalool, eugenol, octanal, 1-octanol, (E)-2-hexenal and (Z)-3-hexenol) from herbal teas were identified by capillary gas chromatographic-mass spectrometry and olfactometry analysis, and it was considered that three compounds (octanal, (E)-2-hexenal and (Z)-3-hexenol) were key compounds for describing the results of sensory evaluation. The structure of dried sweet basil leaves with water-absorption and fresh leaves was observed by differential interference contact microscopy, and their rheological characteristics were measured for storage modulus. As a result, the characteristics of vacuum-dried sweet basil were similar to those of fresh basil. These results suggest that investigation of the aroma using hot-water extraction, tissue structure and rheological characteristics could be effective approaches to qualitatively evaluate dried herbs.
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| 62.
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早川, 和一 ; Hayakawa, Kazuichi
概要:
ディーゼル排出粉塵(DEPE)及びその構成成分の一つである多環芳香族炭化水素(PAH)類の内分泌攪乱作用について,昨年度はエストロゲン様/抗エストロゲン活性を明らかにした.今年度はDEPE及びPAHのアンドロゲン様活性/抗アンドロゲン活性に
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ついて検討した。DEPEをヒトPC3/AR培養細胞を用いたルシフェラーゼレポーターアッセイに適用した結果,アンドロゲン様活性は認められなかったが,抗アンドロゲン活性が観察された。DEPEに含まれるいくつかの4,5環PAHは,強い抗アンドロゲン活性を示した。また,DEPE及び4,5環PAHはいずれも,ヒトのアリルヒドロカーボンレセプター(AhR)のアゴニストであった。以上の結果から,DEPEは抗アンドロゲン活性を示し,その一部はDEPEに含まれるPAHに由来することがわかった。更に,酵母two-hybrid法を用いた結果,DEPE及びいくつかのニトロ多環芳香族炭化水素が抗アンドロゲン活性を示した。次に,分析対象のモノヒドロキシ多環芳香族炭化水素(OHPAH)の数を増加させるために,逆相HPLC/蛍光検出法の条件を改良した。また,ヒト尿試料に適用可能とするために,OHPAHの抱合体も加水分解してOHPAHと合わせて定量する前処理方法を開発した。その結果,喫煙者は非喫煙者に比較して尿中2-ヒドロキシフルオレン濃度が有為に高く,1-ヒドロキシピレンより有効な喫煙指標となることがわかった。また,2〜4環の複数のOHPAHを同時分析した結果,タイ人は日本人に比較して尿中の各種OHPAH濃度が高く,室内で使用する薪燃料由来の煙の影響が大きいと推定された。このように,開発したOHPAH分析法は,ガス状及び粒子状のいずれのPAHの代謝物も分析対象としており,異なる多様なPAH発生源にも対応できることから,ヒトのPAH個人曝露量評価法として有用なことがわかった。<br />Last year, both estrogenic and antiestrogenic actions of diesel exhaust particulate(DEPE) and polycyclic aromatic hydrocarbon(PAH), which was one of the constituent of DEPE, were clarified. This year, both androgenic and antiandrogenic activities of DEPE and PAH were examined. By applying DEPE to the luciferase reporter gene assay in human PC3/AR culture cells, DEPE did not show androgenic activity but antiestrogenic activity. Several PAHs having 4 or 5 rings, which are included in DEPE, showed strong antiandrogenic activity. Both DEPE and PAHs having 4 or 5 rings, were also agonists of human allyl hydrocarbon receptor(AhR). These results suggested that DEPE showed antiandrogenic activity and that a part of this activity was derived from PAHs which were included in DEPE. In addition, several nitropolycyclic aromatic hydrocarbons showed aniandorgenic activity in the yeast two-hybrid assay. Next, to increase the number of monohydroxy polycyelic aromatic hydrocarbons(OHPAH) as analytes, conditions of our HPLC/fluorimetric detection method were modified. And, to anayze both urinary OHPAHs and their conjugates, the pretreatment method including hydrolysis of the conjugates was developed. As the result, the urinary concentration of 2-hydroxyfluorene in smokers' urine samples was higher than that in nonsmokers', and it was proven that 2-hydroxyfluorene was a more effective biomarker for smoking than 1-hydroxypyrene. Urinary OHPAH concentrations of Thai subjects were higher than those of Japanese. As a possible reason for this, the smoke of the firewood fuel used in the indoor of Thai house was considered.<br />研究課題/領域番号:14370728, 研究期間(年度):2002–2003<br />出典：「多環芳香族炭化水素とその代謝物の内分泌撹乱作用とその測定法に関する研究」研究成果報告書 課題番号14370728 (KAKEN：科学研究費助成事業データベース（国立情報学研究所）) 本文データは著者版報告書より作成
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| 63.
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鳥羽, 陽 ; 笠原, 千栄子 ; 戸次, 加奈江 ; 佐溝, 将之 ; 唐, 寧 ; 早川, 和一 ; Toriba, Akira ; Kasahara, Chieko ; Bekki, Kanae ; Samizo, Masayuki ; Ning, Tang ; Hayakawa, Kazuichi
概要:
金沢大学理工研究域自然システム学系<br />大気中の粒子状物質（PM）中の水酸化多環芳香族炭化水素（OHPAH）を定量することを目的とするGC/MSによる分析法を開発した．母核の環数が2〜4環のOHPAH 10種を分析対象とし，トリメチル
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シリル（TMS）誘導体化したうえで検出し，3種類の重水素化，または安定同位体標識化OHPAHを内部標準物質として用いてPM試料の定量に適用した．OHPAHのTMS誘導体の選択イオン検出（SIM）における検出限界（S/N＝3）は，12〜930 fgの範囲で，すべての分析対象物質について10.5分で分離・検出することができた．都市大気標準粉じんや金沢で捕集したPM試料はジクロロメタンで抽出したのち，シリカゲル固相により精製しTMS誘導体化して定量した．金沢で捕集したPM試料中の8種のOHPAHを定量することに成功し，それらの濃度範囲は，20〜4100 fg m−3であり，3-hydroxyfluorantheneのPM中濃度の報告は本研究が初めてである．確立した分析法は，大気粉じん中のOHPAHを定量する際の分析法の選択肢の一つとして有用である．<br />A GC/MS method was developed for the quantification of hydroxylated polycyclic aromatic hydrocarbons (OHPAHs) in airborne particulate matter (PM). Ten OHPAHs having 2 - 4 rings were detected after trimethylsilyl (TMS) derivatization, and the derivatives in PM samples were quantified with three kinds of deuterated or stable isotope labeled OHPAHs as internal standards. The detection limits (S/N = 3) of the derivatives of OHPAHs in the selected ion monitoring (SIM) mode ranged from 12 to 930 fg and all analytes were separated and detected within 10.5 min. A commercially available urban PM sample and PM samples collected in Kanazawa were extracted with dichloromethane, and then the extracts were purified with silica gel solid phase and derivatized OHPAHs in the extracts were quantified. We successfully quantified 8 OHPAHs in PM samples collected in Kanazawa, and their concentrations were in the range of 20 - 4100 fg m−3 and the levels of 3-hydroxyfluoranthene were reported for the first time. This method should be useful as an optional analytical method to quantify OHPAHs in PM samples.
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| 64.
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早川, 和一 ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />13億人を超える人口を擁し,産業経済が急速に発展する中国は,エネルギー消費量も急増し,今や世界一の石炭消費国になった。その一方で,大量の石炭消費に伴う排煙による都市の大気環境問題が深刻化している。化石
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燃料の不完全燃料に伴って発生する代表的な有害化学物質の一つに多環芳香族炭化水素(PAH)及びそのニトロ誘導体(NPAH)がある。これらは強い発がん性/変異原性/内分泌かく乱性を有するので,ヒトの健康,とりわけ大気汚染濃度が著しく高い中国国民の健康に及ぼす影響が懸念されている。また,中国で大量に大気中に放出されたPAH, NPAHは,黄砂や硫黄酸化物等と同様に日本海を越え,わが国まで長距離輸送されてくることが推定された。昨年度は,中国東北地方の代表的都市である瀋陽市について,季節毎に2週間ずつ大気粉塵を捕集し,含まれるPAH, NPAHをそれぞれHPLC-蛍光検出法,HPLC-化学発光検出法で測定し,過去の測定結果を併せて汚染濃度と主要発生源の推移を解析した。本年度は,冬季偏西風の風下に位置する能登半島先端に在る金沢大学輪島大気観測ステーションで大気粉塵を通年連続捕集し,含まれるPAH, NPAHを同様の方法で分析した。気象条件と合わせて解析した結果,瀋陽市の大気中PAH, NPAH濃度は金沢市及び能登半島における濃度よりはるかに高いこと,瀋陽市を含む中国東北地方の主要発生源が冬季は石炭燃焼システムであり,夏季は自動車と石炭燃焼システムの両方であること,さらに後方流跡線解析法を用いて,冬季に中国東北地方で発生した高濃度PAH, NPAHがわが国の能登半島まで長距離輸送されていることを初めて証明した。<br />研究課題/領域番号:21120503, 研究期間(年度):2009 – 2010
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後藤, 純雄 ; 峯木, 茂 ; 杉田, 和俊 ; 遠藤, 治 ; 村山, 留美子 ; 内山, 巌雄 ; 田中, 基裕 ; 早川, 和一 ; Goto, Sumio ; Mineki, Shigeru ; Sugita, Kazutoshi ; Endo, Osamu ; Murayama, Rumiko ; Uchiyama, Iwao ; Tanaka, Motohiro ; Hayakawa, Kazuichi
概要:
金沢大学理工研究域自然システム学系<br />ナホトカ号から流出し日本海沿岸に漂着した重油の汚染状況を把握するための調査研究の一環として, 平成9年1月16日に採取した漂着重油, ナホトカ号船首部分の重油および市販C重油中に含まれる多環芳香
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族炭化水素 (PAH) の分析及び抽出物の変異原性を測定した。その結果, 漂着重油のベンゾ (a) ピレン (BaP) 含有量は1984年に採取された東京都市部の土砂51試料の平均値の約1/4であることやその変異原比活性は同土砂の約4倍であることなどを認めた。<br />As a part of research studies on the pollution at heavy-oil coated parts of the Sea of Japan coastline, resulting from the wrecked Russian tanker Nakhodka on Jan. 2, the following experiments were performed using three heavy oil samples. Polycyclic aromatic hydrocarbons (PAH) were analyzed by HPLC in the heavy oil that washed ashore, which was collected at Mikuni-cho in Fukui Prefecture on Jan. 16, 1997, heavy oil in the oil compartment of the bow of the tanker, and commercial heavy oil (class C) .Mutagenicities of the extracts of these oil samples were also measured. The amount of benzo (a) pyrene (BaP) contained in the heavy oil that washed ashore was about a quarter of the average in 51 soil extracted samples, which were collected at an urban area in Tokyo in 1984, and mutagenicity of the extract from the oil was about 4-fold higher than the average in the extracts from the soil samples.
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早川, 和一 ; Hayakawa, Kazuichi
概要:
環日本海域の7都市,瀋陽(中国),ウラジオストク(ロシア),ソウル(韓国),北九州,金沢,東京,札幌(日本)で,冬及び夏に大気粉塵を捕集した。更に,家庭石炭燃焼ストーブ排出粉塵及びディーゼル車排出粉塵も捕集した。粉塵抽出物について,多環芳香
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族炭化水素9種類(フルオランテン,ピレン,ベンツ[a]アントラセン,クリセン,ベンゾ[b]フルオランテン,ベンゾ[k]フルオランテン,ベンゾ[a]ピレン,ベンゾ[ghi]ペリレン,インデノ[1,2,3-cd]ピレン)とニトロ多環芳香族炭化水素4種類(1,3-,1,6-,1,8-ジニトロピレン,1-ニトロピレン)を,それぞれ蛍光,化学発光検出HPLCで測定した。瀋陽とウラジオストクの平均大気中多環芳香族炭化水素濃度はソウル,北九州,金沢,東京,札幌より著しく高かったが,平均大気中ニトロ多環芳香族炭化水素濃度は北九州以外を除くと同レベルであった。いずれの都市でも多環芳香族炭化水素とニトロ多環芳香族炭化水素濃度には明確な季節変動(冬>夏)が見られた。各都市の多環芳香族炭化水素とニトロ多環芳香族炭化水素の発生源を明らかにする為に,クラスター分析及び因子分析を行った結果,3つの主要クラスターが見出された。更に,瀋陽とウラジオストク,北九州のピレンに対する1-ニトロピレンの濃度比は石炭燃焼ストーブ排出粉塵のそれに近似し,ソウル,金沢,東京,札幌の値はディーゼル車排出粉塵のそれに近似していた。本研究は,ピレンに対する1-ニトロピレンの濃度比が,都市大気粉塵の発生源である石炭燃焼システムとディーゼル車の指標として有用なことを示している。<br />Airborne particulates were collected in seven cities in the Pan-Japan Sea countries, Shenyang (China), Vladivostok (Russia), Seoul (South Korea), Kitakyushu, Kanazawa, Tokyo and Sapporo (Japan), in winter and summer. In addition, particulates from domestic coal-burning stoves and particulates from diesel-engine automobiles were collected. Nine polycyclic aromatic hydrocarbons (PAHs), fluoranthene, pyrene (Pyx), benz[a]anthracene, chrysene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[a]pyrene, benzo[ghi]perylene and indeno[1,2,3-cd]pyrene, and four nitropolycyclic aromatic hydrocarbons (NPAHs), 1,3-, 1,6-, 1,8-dinitropyrenes, and 1-nitropyrenes (1-Np) in the extracts from the particulates were analyzed by HPLC with fluorescence and chemiluminescence defections, respectively. The mean atmospheric concentrations of PAHs in Shenyang and Vladivostok were substantially higher than those in Seoul, Tokyo, Sapporo, Kitakyushu and Kanazawa. However, the mean atmospheric concentrations of NPAHs were at the same levels in every city except for Kitakyushu. Obvious seasonal variations (winter > summer) in the PAR and NPAH concentrations were observed in each city. In order to study the major contributors of atmospheric PAHs and NPAHs in these cities, cluster analysis and factor analysis were used and three large clusters were identified. Furthermore, the concentration ratios of 1-Np to Pyr were significantly smaller in Shenyang, Vladivostok and Kitakyushu and the values were close to those of particulates in the exhaust from coal stoves. However, the ratios were larger in Seoul, Kanazawa, Tokyo and Sapporo and the values were close to those of particulates in the exhaust from diesel-engine automobiles. Our results show that the concentration ratio of 1-Np to Pyr is an useful indicator of the contributions made by diesel-engine vehicles and coal combustion systems to particulates in urban air.<br />研究課題/領域番号:15406001, 研究期間(年度):2003–2004<br />出典：「環日本海都市の多環芳香族炭化水素/ニトロ多環芳香族炭化水素の発生と曝露の国際比較」研究成果報告書 課題番号15406001 (KAKEN：科学研究費助成事業データベース（国立情報学研究所）) 本文データは著者版報告書より作成
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早川, 和一 ; Hayakawa, Kazuichi
概要:
(1)金沢市市街地の大気中1,3-,1,6-,1,8-ジニトロピレン(DNP)及び1-ニトロピレン(1-NP)の平均濃度は,それぞれfmol m^<-3>,サブpmol m^<-3>〜pmol m^<-3>レベルであった.これらの化合物濃度
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は,日中に高く夜間から早朝に低い日内変動を示し,交通量と高い相関が認められたことより,主要発生源は自動車と推定された.また,これらの化合物濃度は春から夏に低く,秋から冬に高い季節変動を示し,その要因の一つとして,前者には太陽光による光分解が,後者には逆転層による大気の安定が考えられた. (2)ガソリン車とディーゼル車の排ガス中DNP,1-NP濃度及び粉じん量を比較すると,DNP濃度は大差ないが,後者は前者に比べて1-NP濃度が遙かに高く,粉じん量も多い.これらに基づいて金沢市市街地の大気中DNP,1-NPについて発生源としてのディーゼル車の寄与率を求めると,それぞれ約90%,99%以上と試算された. (3)金沢市,東京都,札幌市の大気中DNP及び1-NP濃度には,都市の特徴によって多少の違いがあるものの,類似した日内及び季節変動が認められた.3都市の中では,札幌市がDNP濃度に対する1-NP濃度の比が最も大きく,その理由として,ガソリン車に対するディーゼル車の保有台数の割合が高いことが考えられた. (4)大気中1,3-,1,6-,1,8-DNP及び1-NP濃度推移と,Ames試験による大気直接変異原活性推移との相関は高く,上記化合物の大気直接変異原活性における寄与率は,YG1024株では約30%,TA98株では約10%と試算された.粒径別では,肺胞に沈積する割合の高い1.1μm以下の最微細粉じんに,化合物と変異原活性のいずれも最も多く分布していることが明らかとなった.大気変異原性に寄与するDNP,1-NP以外の化合物は,シリカゲルカラムクロマトグラフィーにより,DNPよりも低極性であると推定された.<br />(1) Each mean concentration of 1,3-dinitropyrene (1,3-DNP), 1,6-DNP,1,8-DNP and 1-nitropyrene (1-NP) in air in downtown Kanazawa were in the levels of fmol m^<-3> and sub pmol m^<33>-pmol m^<-3>, respectively. The concentrations were high in the daytime and low in the midnight and early in the morning. This diurnal variation gave a good correlation to the traffic volume, suggesting automobiles were the main contributors. The concentrations were high in spring and summer and low in autumn and winter. As reasons for this, degradation by sunlight in the former seasons and low atmospheric mixing dephts in the latter seasons were considered.(2) Concentrations of 1,3-, 1,6-and 1,8-DNPs and 1-NP in air in winter and summer in downtown Kanazawa, Sapporo and Tokyo were determined. Although the mean concentrations in Kanazawa were lower than those in Tokyo and Sapporo, there were similar tendencies as described above. The 1-NP to DNPs ratio in Sapporo was the largest in the three cities, suggest ing the largest diesel-engine vehicles to gasoline-engine vehicles ratio.(3) Concentrations of 1,3-, 1,6-and 1,8-DNPs in diesel Particulate were at the same levels as those in gasoline particulate. However, the concentration of 1-NP in diesel particulate was much higher than that in gasoline particulate. Considering the amount of particulates emitted from diesel-engine much larger than that of gasoline-engine, the contribution of diesel-engine vehicles to the amount of the above compounds in urban air was much larger than that of gasoline-engine vehicles.(4) In both diurnal and seasonal variation studies, good correlation coefficients were observed between the four concentrations and direct-acting mutagenic activities by the Ames test using three stains, TA98, YG1021 and YG1024. In the three, the YG1024 gave the largest coefficient. The contributions of the four compounds to the activities of air in YG1024 and TA98 strains were about 30% and 10%, respectively. The silica gel column chromatography suggested that the other contributors were less polar. When particulates were separately collected into five fractions of different particulate sizes, both the compounds and the activity were mainly contained in the finest particulate fraction (less than 1.1um) which was most adsorbed in alveoli of the lung.<br />研究課題/領域番号:06672138, 研究期間(年度):1994–1995<br />出典：「ニトロアレーンの環境動態解析とその軽減に関する基礎研究」研究成果報告書 課題番号06672138(KAKEN：科学研究費助成事業データベース（国立情報学研究所）) 本文データは著者版報告書より作成
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早川, 和一 ; Hayakawa, Kazuichi
概要:
金沢大学医薬保健研究域薬学系<br />東アジアの大気質は急激変化している。本研究では，強毒性でPM2.5の主要成分であるPAH, NPAHに焦点を合わせて，これ等とその反応（代謝）物の高性能分析法を開発し，実試料分析を行った。1990年代
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後半から日本では自動車排ガス規制の効果により大気中PAH, NPAH濃度が大幅に減少したが，中国やロシアでは濃度が増加傾向を示す都市もあった。測定結果から，この地域におけるPAHの排出インベントリと大気化学輸送モデルを開発し，長距離輸送も再現できた。また大気輸送中のPAH, NPAH二次生成物を同定し，これらと代謝物の中に変異原性や内分泌撹乱作用など，強い生物活性を示すものがある事を明らかにした。<br />East Asian countries surrounding Japan Sea, such as Japan, China, Korea and Russia, have shown significant change of atmospheric conditions with fast industrial development. Atmospheric behaviors of carcinogenic polycyclic aromatic hydrocarbon (PAH) and nitropolycyclic aromatic hydrocarbon (NPAH) were studied in this area. Their atmospheric concentrations decreased in Japanese cities by the effective countermeasures against automobile exhaust. However, several cities in China and Russia showed the increasing tendency of the concentrations. By using the analytical results, the emission inventory and the chemical transport model were newly developed. In the atmosphere, on the other hand, several oxidized derivatives of PAHs and NPAHs formed through secondary formation were identified. Several compound of metabolites and secondary formed derivatives of PAHs and NPAHs showed strong biological activities such as mutagenicity and endocrine disruption.<br />研究課題/領域番号:21256001, 研究期間(年度):2009-04-01 – 2014-03-31
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早川, 和一 ; Hayakawa, Kazuichi
概要:
本研究では, 環日本海域の主要大気汚染物質の一つである多環芳香族炭化水素(PAH)及びニトロ多環芳香族炭化水素(NPAH)について次の成果を得た。1) 大気中のガス状と粒子状とを分別捕集する装置を開発し, 実大気中の存在状態を明らかにした。
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2) 能登半島先端の大気中PAH及びフッ素の一部が中国から長距離輸送され, 前者は中国の冬季の石炭暖房, 後者は黄砂嵐が主発生要因であることを明らかにした。3) 最近の環日本海域の大気汚染傾向と毒性の強さ及びPAH,NPAH濃度との関係を明らかにした。4) ヒトのNPAHの曝露を, 尿中代謝物を用いて明らかにするLC-MS/MS分析法を開発した。これを用いて, 中国瀋陽市の住民(学童)の尿中1-NP代謝物は日本人より高いことを明らかにした。<br />研究課題/領域番号:18256002, 研究期間(年度):2006–2008<br />出典：「環日本海都市の多環芳香族炭化水素/ニトロ多環芳香族炭化水素の発生と曝露の国際比較」研究成果報告書 課題番号18256002 (KAKEN：科学研究費助成事業データベース（国立情報学研究所）)（https://kaken.nii.ac.jp/report/KAKENHI-PROJECT-18256002/18256002seika/)を加工して作成
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早川, 和一 ; Hayakawa, Kazuichi
概要:
金沢大学自然科学研究科<br />経気道曝露する未規制多環芳香族炭化水素の健康リスクについて,研究班員及びその関連領域の最近の研究に関する調査を実施した。さらに平成15年1月10-11日に金沢でシンポジウム及び会議を行い,次の成果を得た。デ
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ィーゼル粉じんを曝露したマウスでは,肺内サイトカインmRNAに変化を来すだけでなく,副腎,卵巣機能にも影響を及ぼしていること,また,精子産生能の低下及びライディッヒ細胞の変化が生じること,さらに胎仔期の曝露が生殖系だけでなく記憶能力の低下も引き起こしている可能性が明らかになった。しかし,これらの影響がディーゼル粉じんに含まれるいかなる成分によるかは明らかにされていない。一方,ディーゼル粉じんに多く含まれ,主要大気汚染物質である多環芳香族炭化水素についてヒト培養細胞を用いて評価すると,エストロゲン様作用及び抗エストロゲン作用,あるいは抗アンドロゲン作用を呈するものがあり,いずれの活性も多環芳香族炭化水素の環数の違い及び異性体により異なるだけでなく,前者の作用は細胞内でCYPにより代謝を受けた多環芳香族炭化水素の水酸化体が活性の本体であり,後者の作用は多環芳香族炭化水素及びその代謝物も活性発現に関与する可能性があることがわかった。以上の研究結果は,大気汚染物質の健康リスクとして,呼吸によって曝露する量が多い多環芳香族炭化水素の内分泌攪乱作用の調査研究が重要なことを示している。また,研究班では,これら有害大気汚染物質の浄化方法の一つとして,金属・光触媒作用による分解除去法の可能性についても検討したが,多環芳香族炭化水素については現段階では有用な基材は見出せていない。<br />研究課題/領域番号:14608019, 研究期間(年度):2002<br />出典：「経気道曝露する未規制多環芳香族炭化水素の健康リスク評価に関する研究」研究成果報告書 課題番号14608019（KAKEN：科学研究費助成事業データベース（国立情報学研究所））（https://kaken.nii.ac.jp/ja/grant/KAKENHI-PROJECT-14608019/)を加工して作成
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