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新型铁锰二元氧化物吸附剂对As(III)的去除机制:氧化与吸附

Removal mechanism of As(III) by a novel Fe-Mn binary oxide adsorbent: oxidation and sorption.

作者信息

Zhang Gao-Sheng, Qu Jiu-Hui, Liu Hui-Juan, Liu Rui-Ping, Li Guo-Ting

机构信息

State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China 100085.

出版信息

Environ Sci Technol. 2007 Jul 1;41(13):4613-9. doi: 10.1021/es063010u.

Abstract

A novel Fe-Mn binary oxide adsorbent was developed for effective As(III) removal, which is more difficult to remove from drinking water and much more toxic to humans than As(V). The synthetic adsorbent showed a significantly higher As(III) uptake than As(V). The mechanism study is therefore necessary for interpreting such result and understanding the As(III) removal process. A control experiment was conducted to investigate the effect of Na2SO3-treatment on arsenic removal, which can provide useful information on As(III) removal mechanism. The adsorbent was first treated by Na2SO3, which can lower its oxidizing capacity by reductive dissolution of the Mn oxide and then reacted with As(V) or As(III). The results showed that the As(V) uptake was enhanced while the As(III) removal was inhibited after the pretreatment, indicating the important role of manganese dioxide during the As(III) removal. FTIR along with XPS was used to analyze the surface change of the original Fe-Mn adsorbent and the pretreated adsorbent before and after reaction with As(V) or As(III). Change in characteristic surface hydroxyl groups (Fe-OH, 1130, 1048, and 973 cm(-1)) was observed by the FTIR. The determination of arsenic oxidation state on the solid surface after reaction with As(III) revealed that the manganese dioxide instead of the iron oxide oxidized As(III) to As(V). The iron oxide was dominant for adsorbing the formed As(V). An oxidation and sorption mechanism for As(III) removal was developed. The relatively higher As(III) uptake may be attributed to the formation of fresh adsorption sites at the solid surface during As(III) oxidation.

摘要

开发了一种新型铁锰二元氧化物吸附剂用于有效去除As(III),与As(V)相比,As(III)更难从饮用水中去除且对人体毒性更大。合成吸附剂对As(III)的吸附量明显高于As(V)。因此,有必要进行机理研究以解释该结果并了解As(III)的去除过程。进行了一项对照实验来研究Na2SO3处理对砷去除的影响,这可为As(III)去除机理提供有用信息。吸附剂先用Na2SO3处理,通过MnO2的还原溶解降低其氧化能力,然后与As(V)或As(III)反应。结果表明,预处理后As(V)的吸附量增加而As(III)的去除受到抑制,表明二氧化锰在As(III)去除过程中起重要作用。利用傅里叶变换红外光谱(FTIR)和X射线光电子能谱(XPS)分析了原始铁锰吸附剂以及与As(V)或As(III)反应前后预处理吸附剂的表面变化。通过FTIR观察到特征表面羟基(Fe-OH,1130、1048和973 cm(-1))的变化。与As(III)反应后固体表面砷氧化态的测定表明,氧化As(III)至As(V)的是二氧化锰而非氧化铁。氧化铁在吸附形成的As(V)方面起主导作用。提出了As(III)去除的氧化和吸附机理。相对较高的As(III)吸附量可能归因于As(III)氧化过程中在固体表面形成了新的吸附位点。

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