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

被引:9
|
作者
Li, Shuaishuai [1 ]
Wang, Wei [1 ]
Wu, Huizhong [1 ]
Zhang, Xiuwu [1 ]
Liang, Ruiheng [1 ]
Zhang, Xuyang [1 ]
Song, Ge [1 ]
Jing, Jiana [1 ]
Li, Shasha [1 ]
Zhou, Minghua [1 ]
机构
[1] Nankai Univ, Carbon Neutral Interdisciplinary Sci Ctr, Key Lab Pollut Proc & Environm Criteria, Coll Environm Sci & Engn,Minist Educ, Tianjin 300350, Peoples R China
基金
中国国家自然科学基金;
关键词
environment remediation; peroxymonosulfate; electroenhanced activation; iron single atom catalyst; reaction mechanism; SURFACES; SULFATE;
D O I
10.1073/pnas.2404965121
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
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.
引用
收藏
页数:12
相关论文
共 50 条
  • [31] Single-Atom Fe Catalyst Outperforms Its Homogeneous Counterpart for Activating Peroxymonosulfate to Achieve Effective Degradation of Organic Contaminants
    Qian, Kun
    Chen, Hong
    Li, Wenlang
    Ao, Zhimin
    Wu, Yi-nan
    Guan, Xiaohong
    ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2021, 55 (10) : 7034 - 7043
  • [32] Engineered Fe-doped activated carbon from industry waste for peroxymonosulfate activation: Performance and mechanism
    Fan, Xiaohui
    Zhao, Jinjin
    Cheng, Cheng
    Xu, Yin
    Zhang, Hui
    SEPARATION AND PURIFICATION TECHNOLOGY, 2023, 325
  • [33] Molybdenum nitride(γ-Mo2N) as a novel co-catalyst to enhance Fe(III)/Fe (II) cycle for homogeneous and heterogeneous peroxymonosulfate activation: Performance and mechanism
    He, Wentao
    Huang, Lupeng
    Wang, Xinyu
    Zhang, Jing
    JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2024, 12 (02):
  • [34] Lignosulfonate modified zero-valent iron enhanced activation of peroxymonosulfate for sulfamethazine removal: Performance and mechanism
    Duan, Yao
    Li, Xiaoyu
    Gao, Shang
    Yu, Minyi
    Fu, Lichun
    Zhang, Ying
    Sun, Haiyang
    Pan, Yuwei
    CHEMICAL ENGINEERING JOURNAL, 2025, 504
  • [35] Activation of peroxymonosulfate by BiOCl@Fe3O4 catalyst for the degradation of atenolol: Kinetics, parameters, products and mechanism
    Wu, Yanlin
    Fang, Zhongyi
    Shi, Yahong
    Chen, Hongche
    Liu, Yankun
    Wang, Yifan
    Dong, Wenbo
    CHEMOSPHERE, 2019, 216 : 248 - 257
  • [36] Fe-N-C single-atom peroxymonosulfate activator based on natural diatomite: Dispersion and strengthening mechanism
    Tan, Ye
    Yang, Shanshan
    Li, Chunquan
    Zhang, Xiangwei
    Yuan, Fang
    Sun, Zhiming
    SURFACES AND INTERFACES, 2024, 48
  • [37] Co single-atom catalyst outperforms its homogeneous counterpart for peroxymonosulfate activation to achieve efficient and rapid removal of nitenpyram
    Guo, Ruonan
    Bi, Zenghui
    Xi, Beidou
    Guo, Changsheng
    Lv, Ningqing
    Hu, Guangzhi
    Xu, Jian
    CHEMICAL ENGINEERING JOURNAL, 2024, 483
  • [38] Enhanced FeIV═O Generation via Peroxymonosulfate Activation by an Edge-Site Engineered Single-Atom Iron Catalyst
    Lee, Donghyun
    Lee, Jaewoo
    Yu, Gwonho
    Kim, Kang
    Kim, Joohyun
    Mok, Dong Hyeon
    Jang, Alim
    Jung, Muho
    Ahn, Hyunsoo
    Back, Seoin
    Hyeon, Taeghwan
    Lee, Changha
    SMALL, 2025, 21 (08)
  • [39] A cobalt single-atom catalyst with ultralow metal loading for activation of peroxymonosulfate to generate singlet oxygen with almost 100% selectivity
    Zhao, Yuanzhe
    Wang, Xiuheng
    JOURNAL OF MATERIALS CHEMISTRY A, 2025, 13 (05) : 3575 - 3586
  • [40] Iron- and nitrogen-rich Enteromorpha-derived dual-atom catalysts modified by clusters for the activation of peroxymonosulfate: Enhanced performance and synergistic mechanism
    Li, Chunxue
    Tian, Zhen
    Zhang, Dengcai
    Luo, Juan
    He, Zixia
    Ma, Rui
    Sun, Shichang
    SEPARATION AND PURIFICATION TECHNOLOGY, 2025, 361