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| 1.
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論文
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Begun, Zinnat A. ; Rahman, Ismail M.M. ; Hasegawa, Hiroshi ; 長谷川, 浩
概要:
金沢大学理工研究域物質化学系<br />The complexation of SrII and geochemically-related elements (MgII, CaII, BaII, and YIII) with biodeg
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radable aminopolycarboxylate chelators (DL-2-(2-carboxymethyl)nitrilotriacetic acid (GLDA) and 3-hydroxy-2,2′-iminodisuccinic acid (HIDS)) was evaluated with the objective of using in the chemical-induced washing remediation of radioactive solid waste. The stability constants (log10KML) for metal-chelator (ML) complexes between M (MgII, CaII, SrII, BaII, or YIII) and L (GLDA or HIDS) in the aqueous matrix was derived from experimental potentiometric data (M:L = 1:1; ionic strength, I = 0.10 mol·dm− 3; T = 25 ± 0.1 °C). The formation of ML2 − species was dominant in the systems with MgII, CaII, SrII, or BaII, while M(OH)L2 − or M(OH)2L3 − was the major species with YIII. The stability of YIII-L complexes was higher than that of MgII, CaII, SrII, or BaII, while the order for complexation strength of GLDA and HIDS was not similar with divalent ions: M-GLDA (log10KMg-L < log10KCa-L > log10KSr-L > log10KBa-L), M-HIDS (log10KMg-L > log10KCa-L > log10KSr-L > log10KBa-L). The conditional stability constants for the ML systems was also derived in terms of pH (2 to 12), and compared with that of EDTA and EDDS. The data trend indicated that the overall stability of the complexes of MgII, CaII, SrII, BaII, or YIII with GLDA or HIDS was better than the biodegradable chelator EDDS, which was frequently recommended as the alternative to EDTA. © 2017 Elsevier B.V.<br />Embargo Period 12 months
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| 2.
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Hasegawa, Hiroshi ; Barua, Suman ; Wakabayashi, Tomoya ; Mashio, Asami ; Maki, Teruya ; Furusho, Yoshiaki ; Rahman, Ismail M.M. ; 長谷川, 浩 ; 牧, 輝弥
概要:
金沢大学理工研究域物質化学系<br />End-of-life electrical and electronic equipment is the potential secondary resource for economically
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-viable precious metals (PMs), e.g., gold (Au), palladium (Pd), or platinum (Pt). The hydrometallurgical processes produce acidic leachates during the recovery of PMs from waste sources, while the selective recovery of Au, Pd, or Pt from such a matrix is challenging either due to the chemical similarities of elements or complexities in the sources and matrices. A total of nine solid-phase extraction (SPE) systems, all claimed to designed for separation of PMs from complex matrices, was evaluated at varying solution pH (≤2 to 10) based on the selectivity towards Au, Pd, or Pt. The observation was used to develop a technique for selective Au, Pd, or Pt separation from acidic waste solutions using a macrocycle-equipped SPE. The feed solution flow-rates, eluent-type or compositions has been optimized to achieve maximum separation efficiency of the target analytes. The relative affinity of the macrocycles in solid-phase towards the ions (Pd > Au > Pt) is the core phenomenon of the proposed technique, and the host-guest type interaction is expected to be more stable than the resin-based separation processes. Furthermore, application of the macrocycle-equipped SPE system is advantageous regarding economics as it minimizes the impact of coexisting ions in the matrix and provides unaltered separation performance for several loading-elution cycles. © 2018 Elsevier B.V.<br />Embargo Period 12 months
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| 3.
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Begum, Zinnat A. ; Rahman, Ismail M.M. ; Tate, Yousuke ; Ichijo, Toshiharu ; Hasegawa, Hiroshi ; 長谷川, 浩
概要:
金沢大学理工研究域物質化学系<br />The bioavailability of trivalent iron (Fe3+) to plants can be enhanced using fertilizer solutions co
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ntaining humic acids (HA) as manifested from the increased crop yield at an iron stress conditions. The lignite-derived HA (HAlignite) facilitates higher diffusion of Fe3+ between the soil layers as attributable to more number of reactive sites in the assemblage compared to those from other origins. In the current work, the proton-binding of HAlignite size-fractions (5–10, 10–30, 30–100, and >100 kDa), as segmented based on the molecular weight distribution, and their complexation with Fe3+ have been studied at varying pH ranging from low to high. The protonation or formation of Fe3+-complexes exhibited a comparable pattern despite the differences in the conformational distribution of HAlignite size-fractions. The protonation behavior specified that the behavior of HAlignite size-fractions has similarity with that of a dibasic acid. The results are interpreted using reactive structural units (RSU) concept to show that the carboxyl and phenolic-hydroxyl groups in the HAlignite size-fractions simultaneously available as the Fe3+-binding sites. The stability constants for larger MW fractions of HAlignite (>100 kDa) was the lowest, as attributed to the increased aggregation rate in an aqueous matrix. The trend in conditional stability constants of HAlignite-size fractions and other Fe-chelators point to a better Fe-binding capability of HAlignite (30–100 kDa) size-fraction than the biodegradable alternatives (GLDA, HIDS, EDDS, IDSA, or NTA), while the Fe-interaction was stronger with classical synthetic chelators (EDTA, DTPA, or EDDHA). © 2018 Elsevier B.V.<br />Embargo Period 12 months
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| 4.
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Hasegawa, Hiroshi ; Rahman, Ismail M. M. ; Nakano, Masayoshi ; Begum, Zinnat A. ; Egawa, Yuji ; Maki, Teruya ; Furusho, Yoshiaki ; Mizutani, Satoshi
概要:
Aminopolycarboxylate chelants (APCs) are extremely useful for a variety of industrial applications, including the treatm
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ent of toxic metal-contaminated solid waste materials. Because non-toxic matrix elements compete with toxic metals for the binding sites of APCs, an excess of chelant is commonly added to ensure the adequate sequestration of toxic metal contaminants during waste treatment operations. The major environmental impacts of APCs are related to their ability to solubilize toxic heavy metals. If APCs are not sufficiently eliminated from the effluent, the aqueous transport of metals can occur through the introduction of APCs into the natural environment, increasing the magnitude of associated toxicity. Although several techniques that focus primarily on the degradation of APCs at the pre-release step have been proposed, methods that recycle not only the processed water, but also provide the option to recover and reuse the metals, might be economically feasible, considering the high costs involved due to the chelants used in metal ion sequestration. In this paper, we propose a separation process for the recovery of metals from effluents that contain an excess of APCs. Additionally, the option of recycling the processed water using a solid phase extraction (SPE) system with an ion-selective immobilized macrocyclic material, commonly known as a molecular recognition technology (MRT) gel, is presented. Simulated effluents containing As(V), Cd(II), Cr(III), Pb(II) or Se(IV) in the presence of APCs at molar ratios of 1:50 in H2O were studied with a flow rate of 0.2 mL min-1. The 'captured' ions in the SPE system were quantitatively eluted with HNO3. The effects of solution pH, metal-chelant stability constants and matrix elements were assessed. Better separation performance for the metals was achieved with the MRT-SPE compared to other SPE materials. Our proposed technique offers the advantage of a non-destructive separation of both metal ions and chelants compared to conventional treatment options for such effluents. © 2011 Elsevier Ltd. All rights reserved.
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| 5.
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Maki, Teruya ; Hirota, Wakana ; Motojima, Hiroyuki ; Hasegawa, Hiroshi ; Rahman, Mohammad Azizur
概要:
金沢大学理工研究域物質化学系<br />Aquatic arsenic cycles mainly depend on microbial activities that change the arsenic chemical forms
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and influence human health and organism activities. The microbial aggregates degrading organic matter are significantly related to the turnover between inorganic arsenic and organoarsenic compounds. We investigated the effects of microbial aggregates on organoarsenic mineralization in Lake Kahokugata using lake water samples spiked with dimethylarsinic acid (DMA). The lake water samples converted 1μmolL-1 of DMA to inorganic arsenic for 28d only under anaerobic and dark conditions in the presence of microbial activities. During the DMA mineralization process, organic aggregates >5.0μm with bacterial colonization increased the densities. When the organic aggregates >5.0μm were eliminated from the lake water samples using filters, the degradation activities were reduced. DMA in the lake water would be mineralized by the microbial aggregates under anaerobic and dark conditions. Moreover, DMA amendment enhanced the degradation activities in the lake water samples, which mineralized 50μmolL-1 of DMA. The DMA-amended aggregates >5.0μm completely degraded 1μmolL-1 of DMA with a shorter incubation time of 7d. The supplement of KNO3 and NaHCO3 to lake water samples also shortened the DMA-degradation period. Presumably, the bacterial aggregates involved in the chemical heterotrophic process would contribute to the DMA-biodegradation process in Lake Kahokugata, which is induced by the DMA amendment. © 2011 Elsevier Ltd.
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| 6.
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Azizur Rahman, Mohammad ; Hasegawa, Hiroshi
概要:
Phytoremediation, a plant based green technology, has received increasing attention after the discovery of hyperaccumula
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ting plants which are able to accumulate, translocate, and concentrate high amount of certain toxic elements in their above-ground/harvestable parts. Phytoremediation includes several processes namely, phytoextraction, phytodegradation, rhizofiltration, phytostabilization and phytovolatilization. Both terrestrial and aquatic plants have been tested to remediate contaminated soils and waters, respectively. A number of aquatic plant species have been investigated for the remediation of toxic contaminants such as As, Zn, Cd, Cu, Pb, Cr, Hg, etc. Arsenic, one of the deadly toxic elements, is widely distributed in the aquatic systems as a result of mineral dissolution from volcanic or sedimentary rocks as well as from the dilution of geothermal waters. In addition, the agricultural and industrial effluent discharges are also considered for arsenic contamination in natural waters. Some aquatic plants have been reported to accumulate high level of arsenic from contaminated water. Water hyacinth (Eichhornia crassipes), duckweeds (Lemna gibba, Lemna minor, Spirodela polyrhiza), water spinach (Ipomoea aquatica), water ferns (Azolla caroliniana, Azolla filiculoides, and Azolla pinnata), water cabbage (Pistia stratiotes), hydrilla (Hydrilla verticillata) and watercress (Lepidium sativum) have been studied to investigate their arsenic uptake ability and mechanisms, and to evaluate their potential in phytoremediation technology. It has been suggested that the aquatic macrophytes would be potential for arsenic phytoremediation, and this paper reviews up to date knowledge on arsenic phytoremediation by common aquatic macrophytes.. © 2011 Elsevier Ltd.
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| 7.
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Azizur Rahman, Mohammad ; Mamunur, Rahman ; Kadohashi, K. ; Maki, Teruya ; Hasegawa, Hiroshi
概要:
This study was conducted to investigate the effect of external iron status and arsenic species on chelant-enhanced iron
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bioavailability and arsenic uptake. Rice seedlings (Oryza sativa L.) were used as model plant, and were grown in artificially contaminated sandy soils irrigated with Murashige and Skoog (MS) culture solution. Arsenate uptake in roots and shoots of rice seedlings were affected significantly (p > 0.05) while dimethylarsinic acid (DMAA) was not by the additional iron and chelating ligand treatments. Regardless of iron concentrations in the soil solution, HIDS increased arsenic uptake for roots more than EDTA and EDDS. Chelating ligands and arsenic species also influenced iron uptake in rice roots. Irrespective of arsenic species, HIDS was found to be more effective in the increase of iron bioavailability and uptake in rice roots compared to other chelants. There was a significant positive correlation (r = 0.78, p < 0.05) between arsenate and iron concentrations in the roots of rice seedlings grown with or without additional iron indicating that arsenate inhibit iron uptake. In contrast, there was no correlation between iron and DMAA uptake in roots. Poor correlation between iron and arsenic in shoots indicated that iron uptake in shoots was neither affected by additional iron nor by arsenic species. Compared to the control, chelating ligands increased iron uptake in shoots of rice seedlings significantly (p < 0.05). Regardless of additional iron and arsenic species, iron uptake in rice shoots did not differed among EDTA, EDDS, and HIDS treatments. © 2011 Elsevier Ltd. All rights reserved.
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| 8.
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Habibullah, M. ; Rahman, Ismail M. M. ; Uddin, M. Ashraf ; Iwakabe, Koichi ; Azam, Anisul ; Hasegawa, Hiroshi
概要:
Densities and viscosities of the binary systems of phenylmethanol with 2-butanone were measured for the entire compositi
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on range at T = (303.15, 308.15, 313.15, 318.15, and 323.15) K and at the atmospheric pressure. The excess molar volumes were derived from the experimental data and were fitted with the Redlich-Kister equation to obtain their coefficients and standard deviations. The Grunberg-Nissan equation was used to correlate the viscosity data. Furthermore, kinematic viscosities were compared with those predicted by the UNIFAC-VISCO model. The cause of relatively large deviations between the experimental and predicted kinematic viscosities was explored by comparing the combinatorial and residual terms of the UNIFAC-VISCO model. © 2011 American Chemical Society.
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| 9.
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論文
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Rahman, Ismail M. M. ; Furusho, Yoshiaki ; Begum, Zinnat A. ; Sabarudin, Akhmad ; Motomizu, Shoji ; Maki, Teruya ; Hasegawa, Hiroshi
概要:
A simple flow-based method was developed for the simultaneous separation of certain transition metal ions (Co, Ni, Cu, Z
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n, Cd) from aqueous systems, which ions show ecotoxic effects when present at elevated concentrations. A silica-gel-bonded macrocycle system, commonly known as molecular recognition technology (MRT) gel, was used for solid phase extraction (SPE) of the target analytes. The collection behavior of the MRT-SPE system was studied based on pH. Fortified deionized water samples containing 250 μg L-1 of each of the elements were treated at the flow rate of 1 mL min-1. The collected analytes were then eluted by 3 M HNO3 and analyzed using inductively coupled plasma spectrometry. Detection limits of the proposed technique were in the range of 0.004-0.040 μg L-1 for the studied metal ions. The validity of this separation technique was checked with spiked 'real' water samples, which produced satisfactory recoveries of 96-102%. The non-destructive nature and highly selective ion-extraction capability of the SPE material are the most important aspects of the proposed method and they are the main focus of this paper. © 2011 © Versita Warsaw and Springer-Verlag Wien.
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| 10.
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論文
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Hasegawa, Hiroshi ; Rahman, Ismail M. M. ; Nakano, Masayoshi ; Begum, Zinnat A. ; Egawa, Yuji ; Maki, Teruya ; Furusho, Yoshiaki ; Mizutani, Satoshi
概要:
Aminopolycarboxylate chelants (APCs) are extremely useful for a variety of industrial applications, including the treatm
…
ent of toxic metal-contaminated solid waste materials. Because non-toxic matrix elements compete with toxic metals for the binding sites of APCs, an excess of chelant is commonly added to ensure the adequate sequestration of toxic metal contaminants during waste treatment operations. The major environmental impacts of APCs are related to their ability to solubilize toxic heavy metals. If APCs are not sufficiently eliminated from the effluent, the aqueous transport of metals can occur through the introduction of APCs into the natural environment, increasing the magnitude of associated toxicity. Although several techniques that focus primarily on the degradation of APCs at the pre-release step have been proposed, methods that recycle not only the processed water, but also provide the option to recover and reuse the metals, might be economically feasible, considering the high costs involved due to the chelants used in metal ion sequestration. In this paper, we propose a separation process for the recovery of metals from effluents that contain an excess of APCs. Additionally, the option of recycling the processed water using a solid phase extraction (SPE) system with an ion-selective immobilized macrocyclic material, commonly known as a molecular recognition technology (MRT) gel, is presented. Simulated effluents containing As(V), Cd(II), Cr(III), Pb(II) or Se(IV) in the presence of APCs at molar ratios of 1:50 in H2O were studied with a flow rate of 0.2mL min-1. The 'captured' ions in the SPE system were quantitatively eluted with HNO3. The effects of solution pH, metal-chelant stability constants and matrix elements were assessed. Better separation performance for the metals was achieved with the MRT-SPE compared to other SPE materials. Our proposed technique offers the advantage of a non-destructive separation of both metal ions and chelants compared to conventional treatment options for such effluents. © 2011 Elsevier Ltd.
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