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偕-OH 基团还原铁对水冶工业中铁矾稳定性及砷释放的影响。

Effect of iron reduction by enolic hydroxyl groups on the stability of scorodite in hydrometallurgical industries and arsenic mobilization.

机构信息

Key Laboratory of Pollution Ecology and Environmental Engineering, Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang, 110016, China.

Institute of Environmental Protection, Shenyang University of Chemical Technology, Shenyang, 110142, China.

出版信息

Environ Sci Pollut Res Int. 2017 Dec;24(34):26534-26544. doi: 10.1007/s11356-017-0016-0. Epub 2017 Sep 26.

Abstract

Scorodite (FeAsO·2HO) is an important arsenic-bearing solid waste in hydrometallurgical industries, but its stability in reducing environments is not well understood. This study investigated the effect of Fe(III) reduction by enolic hydroxyl groups on the stability of scorodite and arsenic mobilization at various pH values and ascorbic acid/scorodite molar ratios (AH/Sc). The results showed that 47-89% Fe(III) reduction by ascorbic acid caused approximately 10-69% (~ 37-260 mg L) arsenic release and 4.5-63% (~ 13-176 mg L) Fe(II) release at pH 5-8. The releases of arsenic and Fe(II) increased with increasing AH/Sc, whereas they decreased as pH increased. The results of the solid characterization and chemical analysis indicated that the mixture of poorly crystalline parasymplesite and probably amorphous FeHAsO⋅xHO was the new arsenic sink. The high solubility of this ferrous arsenate with the Fe(II)/As(V) molar ratio > 1 was deemed to be a major contributor to the relatively high arsenic release. This work differed from our previous finding that almost all arsenic was retained in the solid phase after similar Fe(III) reduction in scorodite with hydroquinone. Phenolic hydroxyl groups complexed with aqueous Fe(II), unlike enolic hydroxyl groups, was possibly the dominant reason for the formation of different secondary minerals, which strongly influenced arsenic redistribution between aqueous and solid phases.

摘要

羟高铁砷铁矿 (FeAsO·2HO) 是湿法冶金工业中一种重要的含砷固体废弃物,但人们对其在还原环境中的稳定性了解甚少。本研究考察了烯醇羟基还原 Fe(III) 对羟高铁砷铁矿稳定性的影响,以及在不同 pH 值和抗坏血酸/羟高铁砷铁矿摩尔比 (AH/Sc) 下砷的迁移。结果表明,抗坏血酸还原 47-89% 的 Fe(III) 会导致约 10-69%(37-260mg/L)的砷释放和 4.5-63%(13-176mg/L)的 Fe(II) 释放,pH 值为 5-8。砷和 Fe(II) 的释放随 AH/Sc 的增加而增加,而随 pH 的增加而减少。固相中元素的特征和化学分析结果表明,砷的新沉淀相为结晶度较差的砷铁矿和可能是非晶态的 FeHAsO⋅xHO。这种具有 Fe(II)/As(V)摩尔比>1 的亚铁砷酸盐具有较高的溶解度,被认为是导致较高砷释放的主要原因。这项工作与我们之前的研究结果不同,之前研究表明,在使用对苯二酚还原羟高铁砷铁矿时,几乎所有的砷都留在了固相。与烯醇羟基不同,与水合 Fe(II) 配位的酚羟基可能是形成不同次生矿物的主要原因,这强烈影响了砷在水相和固相之间的重新分配。

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