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活性炭介导的快速三价砷氧化:活性物种与直接氧化

Rapid As(III) oxidation mediated by activated carbons: Reactive species vs. direct oxidation.

作者信息

Zhu Changyin, Xue Chenyan, Huang Mingquan, Zhu Fengxiao, Fang Guodong, Wang Dixiang, Liu Shaochong, Chen Ning, Wu Song, Zhou Dongmei

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, PR China.

School of Environment, Nanjing Normal University, Nanjing 210023, PR China.

出版信息

Sci Total Environ. 2022 May 20;822:153536. doi: 10.1016/j.scitotenv.2022.153536. Epub 2022 Jan 29.

Abstract

Activated carbon (AC) is widely used in pollutant removal, due to its adsorption capacity, conductivity and catalytic performance. However, few studies focus on the redox activity of AC and its role in pollutant transformation. In this study, we found that AC could efficiently mediate the oxidation of As(III) and the process of As(III) oxidation was pH and oxygen concentration dependent. In general, the presence of O promoted As(III) oxidation at pH 3.0-9.5. Acidic and alkaline conditions favored As(III) oxidation regardless of whether there was oxygen, but the mechanisms involved were quite different when there was oxygen. At pH 3.0, reactive species (HO and ·OH) were generated and accounted for As(III) oxidation; at pH 9.5, As(III) was directly oxidized by O (electron transfer from As(III) to O mediated by carbon matrix) under aerobic conditions. Pre-oxidation and cyclic experiments results indicated the ability of AC to oxidize As(III) at pH 9.5 was sustainable and recyclable. This study provided a new insight in pollutant oxidation by AC in the environment.

摘要

活性炭(AC)因其吸附能力、导电性和催化性能而被广泛用于去除污染物。然而,很少有研究关注活性炭的氧化还原活性及其在污染物转化中的作用。在本研究中,我们发现活性炭能够有效地介导As(III)的氧化,并且As(III)的氧化过程取决于pH值和氧气浓度。一般来说,在pH 3.0 - 9.5时,氧气的存在促进了As(III)的氧化。无论是否存在氧气,酸性和碱性条件都有利于As(III)的氧化,但存在氧气时所涉及的机制有很大不同。在pH 3.0时,会产生活性物种(HO和·OH)并导致As(III)氧化;在pH 9.5时,在有氧条件下,As(III)被O直接氧化(电子从As(III)通过碳基质转移到O)。预氧化和循环实验结果表明,活性炭在pH 9.5时氧化As(III)的能力是可持续且可循环利用的。本研究为环境中活性炭对污染物的氧化提供了新的见解。

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