Performance enhancement and mechanism of electroenhanced peroxymonosulfate activation by single- atom Fe catalyst modified electrodes

• 成果类型: Article
• 署名作者: Li, Shuaishuai; Wang, Wei; Wu, Huizhong; Zhang, Xiuwu; Liang, Ruiheng; Zhang, Xuyang; Song, Ge; Jing, Jiana; Li, Shasha; Zhou, Minghua
• 署名单位: Nankai University
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-9985
• DOI: 10.1073/pnas.2404965121
• 发表日期: 2024-09-10
• 关键词: surfaces; sulfate

摘要

Peroxymonosulfate-based electrochemical advanced oxidation processes (PMS- EAOPs) have great potential for sustainable water purification, so an in- depth understanding of its catalytic mechanism is imperative to facilitate its practical application. Herein, the performance enhancement and mechanism of electroenhanced PMS activation by single- atom Fe catalyst modified carbon felt was investigated. Compared with the anode, the cathode exhibited faster bisphenol A degradation ( k cathode = 0.073 vs. k anode = 0.015 min-1), increased PMS consumption (98.8 vs. 10.3%), and an order of magnitude reduction of Fe dissolution (0.068 vs. 0.787 mg L-1). Mass transfer is a key factor limiting PMS activation, while the electrostriction of water in the hydrophobic region caused by cathode electric field (CEF) significantly increased mass transfer coefficient ( k m, cathode = 1.49 x 10-4 vs. k m, anode = 2.68 x 10-5 m s-1). The enhanced activation of PMS is a synergistic result between electroactivation and catalyst- activation, which is controlled by the applied current density. 1 O 2 and direct electron transfer are the main active species and activation pathway, which achieve high degradation efficiency over pH 3 to 10. Density functional theory calculations prove CEF increases the adsorption energy, lengthens the O-O bond in PMS, and promotes charge transfer. A flow- through convection unit achieves sustainable operation with high removal efficiency (99.5% to 97.5%), low electrical energy consumption (0.15 kWh log-1 m-3), and low Fe leaching (0.81% of the total single atom Fe). This work reveals the critical role of electric fields in modulating Fenton- like catalytic activity, which may advance the development of advanced oxidation processes and other electrocatalytic applications.