基于ClO-—HO2-平衡机制的氯介导电催生1O2机理探究

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摘要鉴于单线态氧(¹O₂)氧化能力强、对环境友好等特点,进一步揭示电化学过程中氯介导产¹O₂的反应机理不仅能够提高废水处理效果,还可以减少活性氯带来的副作用.因此,采用电化学测试、罗丹明B(RhB)模拟废水处理等手段评估Ir-Ta/Ti和Pt/Ti电极的性能,并探讨不同条件(Cl^-浓度、电极析氯活性、外加H₂O₂、通入O₂)对电化学产¹O₂的影响.结果表明,以¹O₂为主导的电化学体系能够去除超过96%的RhB且可缩短降解路径.高效生成¹O₂的基础是维持体系中产生的次氯酸根(ClO^-)与过氧氢根(HO₂^-)之间的平衡,任何一方过量都会抑制¹O₂的产生.本次研究以期为促进不同环境情况下¹O₂的生成和电极的定向制备与改性提供理论依据.

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	孙浩然
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关键词 ：氯介导, 电化学产¹O₂, RhB去除, ClO^-—HO₂^-平衡

Abstract：Because of singlet oxygen (¹O₂)’s strong oxidation capability and environmental friendliness, understanding the mechanism of chlorine-mediated ¹O₂ generation in electrochemical processes can enhance wastewater treatment efficiency and minimize the side effects of active chlorine. Thus, electrochemical tests and treatment of Rhodamine B (RhB) simulated wastewater were used to assess the performance of Ir-Ta/Ti and Pt/Ti electrodes. The effects of different conditions (Cl^- concentration, chlorine evolution activity of electrodes, H₂O₂ addition, O₂ aeration) on electrochemical ¹O₂ generation were also explored. The results demonstrated that the ¹O₂-dominated electrochemical system can remove over 96% of RhB and shorten degradation pathways. Efficient ¹O₂ production depends on balancing hypochlorite (ClO^-) and hydroperoxyl (HO²_-) in the system, as an excess of either suppresses ¹O₂ generation. This study provides a theoretical framework for enhancing ¹O₂ generation under various conditions and the targeted preparation and modification of electrodes.

Key words： chlorine-mediated electrochemical formation of ¹O₂ RhB removal ClO^-—HO₂^- balance

收稿日期: 2024-06-03

PACS:

X522

基金资助:国家自然科学基金资助项目(51978654);江苏省自然科学-金-资助项目(BK20211248)

通讯作者: 王立章,教授,wlzh0731@126.com E-mail: wlzh0731@126.com

作者简介: 孙浩然(1997-),男,江苏徐州人,博士研究生,主要从事电化学水处理理论与技术研究.发表论文7篇.tb22160026a41@cumt.edu.cn.

引用本文:

孙浩然, 殷明明, 唐海亮, 王立章. 基于ClO^-—HO₂^-平衡机制的氯介导电催生¹O₂机理探究[J]. 中国环境科学, 2025, 45(1): 167-174. SUN Hao-rang, YIN Ming-ming, TANG Hai-liang, WANG Li-zhang. Mechanism exploration for chlorine-mediated electrocatalytic generation of ¹O₂ based on the equilibrium between ClO^- and HO₂^-. CHINA ENVIRONMENTAL SCIENCECE, 2025, 45(1): 167-174.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2025/V45/I1/167

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