Sunlight-Induced Interfacial Electron Transfer of Ferrihydrite under Oxic Conditions: Mineral Transformation and Redox Active Species Production

Zhipeng Shu; Zezhen Pan; Xingxing Wang

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Sunlight-Induced Interfacial Electron Transfer of Ferrihydrite under Oxic Conditions: Mineral Transformation and Redox Active Species Production

机译：Sunlight-Induced Interfacial Electron Transfer of Ferrihydrite under Oxic Conditions: Mineral Transformation and Redox Active Species Production

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Fe(II)-catalyzed ferrihydrite transformation under anoxic conditions has been intensively studied, while such mechanisms are insufficient to be applied in oxic environments with depleted Fe(II). Here, we investigated expanded pathways of sunlight-driven ferrihydrite transformation in the presence of dissolved oxygen, without initial addition of dissolved Fe(II). We found that sunlight significantly facilitated the transformation of ferrihydrite to goethite compared to that under dark conditions. Redox active species (hole-electron pairs, reactive radicals, and Fe(Il)) were produced from the ferrihydrite interface via the photoinduced electron transfer processes. Experiments with systematically varied wet chemistry conditions probed the relative contributions of three pathways for the production of hydroxyl radicals: (1) oxidation of water (5.0%); (2) reduction of dissolved oxygen (40.9%); and (3) photolysis of Fe(III)-hydroxyl complexes (54.1%). Results also showed superoxide radicals as the main oxidant for Fe(II) reoxidation under acidic conditions, thus promoting the ferrihydrite transformation. The presence of inorganic ions (chloride, sulfate, and nitrate) did not only affect the hydrolysis and precipitation of Fe(III) but also the generation of radicals via photoinduced charge transfer reactions. The involvement of redox active species and the accompanying mineral transformations would exert a profound effect on the fate of multivalent elements and organic contaminants in aquatic environments.

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《Environmental Science & Technology: ES&T》 |2022年第19期|14188-14197|共10页
作者
Zhipeng Shu; Zezhen Pan; Xingxing Wang;
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作者单位

Cluster of Interfacial Processes Against Pollution (CIPAP), Department of Environmental Science and Engineering, Fudan University, Shanghai 200438, China;

Cluster of Interfacial Processes Against Pollution (CIPAP), Department of Environmental Science and Engineering Fudan University, Shanghai 200438, China;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类环境科学、安全科学;
关键词
Fe redox cycling; photoinduced charge transfer; ferrihydrite transformation; acid mine drainage; reactive radical; ligand;

Sunlight-Induced Interfacial Electron Transfer of Ferrihydrite under Oxic Conditions: Mineral Transformation and Redox Active Species Production

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