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氯对白铅矿和羟氯铅矿氧化的动力学及机理研究。

Investigation of the kinetics and mechanisms of the oxidation of cerussite and hydrocerussite by chlorine.

作者信息

Liu Haizhou, Korshin Gregory V, Ferguson John F

机构信息

Department of Civil and Environmental Engineering, University of Washington, Box 352700, Seattle, Washington 98195-2700, USA.

出版信息

Environ Sci Technol. 2008 May 1;42(9):3241-7. doi: 10.1021/es7024406.

Abstract

Reactions of representative lead (II) solid phases (hydrocerussite, cerussite) with chlorine were examined in this study. Chlorine consumption profiles for these solids exhibited a lag phase, during which little consumption of chlorine occurred, and an ensuing rapid reaction phase. The durations of these phases were affected by the pH, carbonate, and chlorine concentrations. SEM and XRD data showed that hydrocerussite started to be transformed into cerussite during the lag phase. Kinetic analysis indicated that only the protonated form of HClO drives the autocatalytic oxidation step, which is mediated by dispersed PbO2 crystals. The rate of the noncatalytic oxidation decreased with the increase of carbonate due to the formation of unreactive surface carbonate Pb(II) complexes.

摘要

本研究考察了代表性的铅(II)固相(羟氯铅矿、白铅矿)与氯的反应。这些固体的氯消耗曲线呈现出一个滞后阶段,在此期间氯的消耗量很少,随后是快速反应阶段。这些阶段的持续时间受pH值、碳酸盐和氯浓度的影响。扫描电子显微镜(SEM)和X射线衍射(XRD)数据表明,在滞后阶段羟氯铅矿开始转化为白铅矿。动力学分析表明,只有HClO的质子化形式驱动由分散的PbO2晶体介导的自催化氧化步骤。由于形成了无反应性的表面碳酸盐Pb(II)络合物,非催化氧化速率随碳酸盐的增加而降低。

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