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用单原子Fe催化剂修改电极对电气增强型氧硫酸盐激活的性能增强和机制

Shuaishuai Li¹, Wei Wang¹, Huizhong Wu¹

¹Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria, Tianjin Key Laboratory of Environmental Technology for Complex Trans-Media Pollution, Carbon Neutrality Interdisciplinary Science Centre, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.

Proceedings of the National Academy of Sciences of the United States of America

|September 5, 2024

概括

这项研究表明,阴极电场增强过氧硫酸盐激活,用于净化水. 这种电催化方法促进了污染物的降解,并减少了用于可持续水处理的催化剂漏.

科学领域:

环境科学与工程环境科学与工程
电化学电化学电化学
催化剂是一种催化剂.

背景情况:

基于氧硫酸盐的电化学先进氧化工艺 (PMS-EAOPs) 对可持续的水净化有希望.
了解PMS-EAOPs的催化机制对于实际应用至关重要.
单原子催化剂在催化过程中提供高效率和选择性.

研究的目的:

为了研究使用单原子Fe催化剂改性碳的电化学增强过氧硫酸盐 (PMS) 激活的性能增强和机制.
阐明阴极电场 (CEF) 在调节PMS激活和污染物降解中的作用.
评估用于净化水的通流对流装置的可持续性和效率.

主要方法:

电化学实验比较 bisphenol A 降解的阳极和阴极性能.
对PMS消耗,铁溶解和质量转移系数的分析.
密度函数理论 (DFT) 计算,以了解CEF对PMS激活的影响.
通过流通的对流装置的运行,以评估长期性能.

主要成果:

与阳极相比,阴极显示出明显更快的双甲降解 (k=0.073分−1) 和更高的PMS消耗 (98.8%).
阴极操作导致Fe溶解的数量减少,并且由于CEF诱导的水电收缩,质量转移系数大幅增加.
单点氧 (1O2) 和直接电子转移被确定为关键的活性物种和通路,在广泛的pH范围 (3-10) 上有效.
据DFT的计算证实,CEF增强了吸附能量,削弱了PMS中的O-O键,并促进了电荷转移.
通过流量单元实现了高去除效率 (99.5%至97.5%),低能耗 (0.15 kWh log−1 m−3) 和最小的Fe漏 (0.81%).

结论:

阴极电场在通过协同电气和催化剂激活来增强PMS激活中发挥着关键作用,主要是通过1O2和直接电子转移.
CEF显著改善了质量转移和催化剂稳定性,从而实现了高效和可持续的水净化.
这项工作为电催化芬顿式反应提供了基本的见解,并推动了先进的氧化过程的发展.

关键词:

电气增强激活方式环境整治环境整治铁单原子催化剂是铁单原子的催化剂.过氧单硫酸盐的使用反应机制的反应机制.

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