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砷酸盐和亚砷酸盐在RuO₂·xH₂O上的吸附:光谱学和宏观研究

Sorption of arsenate and arsenite on RuO2 x xH2O: a spectroscopic and macroscopic study.

作者信息

Impellitteri Christopher A, Scheckel Kirk G, Ryan James A

机构信息

U.S. EPA, ORD, LRPCD, RCB, 5995 Center Hill Avenue, Cincinnati, Ohio 45224, USA.

出版信息

Environ Sci Technol. 2003 Jul 1;37(13):2936-40. doi: 10.1021/es026423d.

DOI:10.1021/es026423d
PMID:12875397
Abstract

The sorption reactions of arsenate (As(V)) and arsenite (As(III)) on RuO2 x xH2O were examined using macroscopic and spectroscopic techniques. Constant solid:solution isotherms were constructed from batch sorption experiments and sorption kinetics assessed at pH 7. X-ray absorption near edge spectroscopy (XANES) was employed to elucidate the solid-state speciation of sorbed As. At all pH values studied (pH 4-8), RuO2 x xH2O showed a high affinity for As regardless of the initial As species present. Sorption was higher at all pH values when the initial As species was As(III). Oxidation of As(III) (250 mg/L solution) to As(V) was virtually complete (98-100%) within 5 s. XANES results showed the presence of only As(V) on the RuO2 x xH2O regardless of the initial As oxidation state. There was no change in the As oxidation state on the solid phase for 4 weeks in both oxic and anoxic environments. It is speculated that changes in the RuO2 x xH2O structure, due to oxidation reactions, caused the higher total As sorption capacity when As(III) was the initial species. The As sorption capacity of RuO2 x xH2O is greater than that of other metal oxides reviewed in this study. The ability of RuO2 x xH2O to rapidly oxidize As(III) is much greater than other oxides, such as MnO2.

摘要

采用宏观和光谱技术研究了砷酸盐(As(V))和亚砷酸盐(As(III))在RuO₂·xH₂O上的吸附反应。通过批量吸附实验构建了恒定固液等温线,并在pH 7下评估了吸附动力学。利用X射线吸收近边光谱(XANES)来阐明吸附态As的固态形态。在所研究的所有pH值(pH 4 - 8)下,无论初始存在的As形态如何,RuO₂·xH₂O对As都表现出高亲和力。当初始As形态为As(III)时,在所有pH值下的吸附量都更高。As(III)(250 mg/L溶液)在5秒内几乎完全氧化为As(V)(98 - 100%)。XANES结果表明,无论初始As氧化态如何,RuO₂·xH₂O上仅存在As(V)。在有氧和无氧环境中,固相上的As氧化态在4周内都没有变化。据推测,由于氧化反应导致RuO₂·xH₂O结构发生变化,使得当初始形态为As(III)时总As吸附容量更高。RuO₂·xH₂O的As吸附容量大于本研究中所综述的其他金属氧化物。RuO₂·xH₂O快速氧化As(III)的能力远大于其他氧化物,如MnO₂。

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