通过直接电子转移增强高铁酸盐（VI）对有机污染物的氧化作用。
Enhanced ferrate(VI) oxidation of organic pollutants through direct electron transfer.
作者信息
Wang Yunpeng, Xiao Zijun, Liu Yulei, Tian Wenjie, Huang Zhuangsong, Zhao Xiaona, Wang Lu, Wang Shaobin, Ma Jun
机构信息
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China; School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia.
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.
出版信息
Water Res. 2023 Oct 1;244:120506. doi: 10.1016/j.watres.2023.120506. Epub 2023 Aug 19.
Fe(VI) is a versatile agent for water purification, and various strategies have been developed to improve its pollutant removal efficiency. Herein, it was found that in addition to intermediate iron species [Fe(IV)/Fe(V)], direct electron transfer (DET) played a significant role in the abatement of organic pollutants in Fe(VI)/carbon quantum dots (CQDs) system. Around 86, 83, 73, 64, 52, 45 and 17% of BPA, DCF, SMX, 4-CP, phenol, p-HBA, and IBP (6 μM) could be oxidized by 30 μM of Fe(VI), whereas with the addition of CQDs (4 mg/L), the oxidation ratio of these pollutants increased to 98, 99, 80, 88, 87, 66 and 57%, respectively. The negative impact induced by solution pH and background constituents on Fe(VI) abatement of pollutants could be alleviated by CQDs, and CQDs acted as catalysts for mediating DET from organic pollutants to Fe(VI). Theoretical calculation revealed that iron species [Fe(VI)/Fe(V)/Fe(IV)] was responsible for the oxidation of 36% of phenol, while DET contributed to the oxidation of 64% of phenol in the Fe(VI)/CQDs system. Compared with iron species oxidation, the CQDs mediated DET from pollutants to Fe(VI) was more efficient for utilizing the oxidation capacity of Fe(VI). The DET mechanism presented in the study provides a prospective strategy for improving the pollution control potential of Fe(VI).
高铁酸盐（Fe(VI)）是一种用于水净化的多功能试剂，人们已经开发了各种策略来提高其污染物去除效率。在此，研究发现，除了中间铁物种[Fe(IV)/Fe(V)]外，直接电子转移（DET）在Fe(VI)/碳量子点（CQDs）体系中有机污染物的去除过程中发挥了重要作用。30 μM的Fe(VI)可氧化约86%、83%、73%、64%、52%、45%和17%的双酚A（BPA）、二氯芬酸（DCF）、磺胺甲恶唑（SMX）、4-氯苯酚（4-CP）、苯酚、对羟基苯甲酸（p-HBA）和异丁基苯酚（IBP，6 μM），而添加CQDs（4 mg/L）后，这些污染物的氧化率分别提高到98%、99%、80%、88%、87%、66%和57%。CQDs可以减轻溶液pH值和背景成分对Fe(VI)去除污染物的负面影响，并且CQDs作为催化剂介导从有机污染物到Fe(VI)的直接电子转移。理论计算表明，在Fe(VI)/CQDs体系中，铁物种[Fe(VI)/Fe(V)/Fe(IV)]负责36%苯酚的氧化，而直接电子转移促成了64%苯酚的氧化。与铁物种氧化相比，CQDs介导的从污染物到Fe(VI)的直接电子转移在利用Fe(VI)的氧化能力方面更有效。该研究中提出的直接电子转移机制为提高Fe(VI)的污染控制潜力提供了一种前瞻性策略。
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