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.
机构:
Tongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
Tongji Univ, Int Joint Res Ctr Sustainable Urban Water Syst, Shanghai 200092, Peoples R China
Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R ChinaTongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
Qian, Kun
Chen, Hong
论文数: 0引用数: 0
h-index: 0
机构:
Southern Univ Sci & Technol, Sch Environm Sci & Engn, Guangdong Prov Key Lab Soil & Groundwater Pollut, Key Lab Municipal Solid Waste Recycling Technol &, Shenzhen 518055, Peoples R ChinaTongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
Chen, Hong
Li, Wenlang
论文数: 0引用数: 0
h-index: 0
机构:
Guangdong Univ Technol, Sch Environm Sci & Engn, Inst Environm Hlth & Pollut Control, Guangdong Key Lab Environm Catalysis & Hlth Risk, Guangzhou 510006, Peoples R ChinaTongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
Li, Wenlang
Ao, Zhimin
论文数: 0引用数: 0
h-index: 0
机构:
Guangdong Univ Technol, Sch Environm Sci & Engn, Inst Environm Hlth & Pollut Control, Guangdong Key Lab Environm Catalysis & Hlth Risk, Guangzhou 510006, Peoples R ChinaTongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
Ao, Zhimin
Wu, Yi-nan
论文数: 0引用数: 0
h-index: 0
机构:
Tongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R ChinaTongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
Wu, Yi-nan
Guan, Xiaohong
论文数: 0引用数: 0
h-index: 0
机构:
Tongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
Tongji Univ, Int Joint Res Ctr Sustainable Urban Water Syst, Shanghai 200092, Peoples R China
Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R ChinaTongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resources Reuse, Shanghai 200092, Peoples R China
机构:
Sichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R ChinaSichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R China
He, Wentao
Huang, Lupeng
论文数: 0引用数: 0
h-index: 0
机构:
Sichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R ChinaSichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R China
Huang, Lupeng
Wang, Xinyu
论文数: 0引用数: 0
h-index: 0
机构:
Sichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R ChinaSichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R China
Wang, Xinyu
Zhang, Jing
论文数: 0引用数: 0
h-index: 0
机构:
Sichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R China
Sichuan Univ, Coll Water Resource & Hydropower, Chengdu 610065, Peoples R China
Sichuan Univ, Yibin Ind Technol Res Inst, Yibin 644000, Peoples R China
2, Sect 2, Chuanda Rd, Chengdu 610207, Sichuan, Peoples R ChinaSichuan Univ, Coll Architecture & Environm, Chengdu 610065, Peoples R China
Zhang, Jing
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING,
2024,
12
(02):
机构:
China Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Changsha Univ Sci & Technol, Sch Chem & Chem Engn, Hunan Prov Key Lab Mat Protect Elect Power & Trans, Changsha 410114, Peoples R ChinaChina Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Tan, Ye
Yang, Shanshan
论文数: 0引用数: 0
h-index: 0
机构:
China Univ Geosci Beijing, Sch Water Resources & Environm, Beijing 100083, Peoples R ChinaChina Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Yang, Shanshan
Li, Chunquan
论文数: 0引用数: 0
h-index: 0
机构:
China Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R ChinaChina Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Li, Chunquan
Zhang, Xiangwei
论文数: 0引用数: 0
h-index: 0
机构:
China Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R ChinaChina Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Zhang, Xiangwei
Yuan, Fang
论文数: 0引用数: 0
h-index: 0
机构:
China Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R ChinaChina Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
Yuan, Fang
Sun, Zhiming
论文数: 0引用数: 0
h-index: 0
机构:
China Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R ChinaChina Univ Min & Technol Beijing, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
机构:
Chinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
Tsinghua Univ, Sch Environm, Beijing 100084, Peoples R ChinaChinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
Guo, Ruonan
Bi, Zenghui
论文数: 0引用数: 0
h-index: 0
机构:
Yunnan Univ, Inst Ecol Res & Pollut Control Plateau Lakes, Sch Ecol & Environm Sci, Kunming 650504, Peoples R ChinaChinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
Bi, Zenghui
Xi, Beidou
论文数: 0引用数: 0
h-index: 0
机构:
Chinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
Tsinghua Univ, Sch Environm, Beijing 100084, Peoples R ChinaChinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
Xi, Beidou
Guo, Changsheng
论文数: 0引用数: 0
h-index: 0
机构:
Chinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R ChinaChinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
Guo, Changsheng
Lv, Ningqing
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h-index: 0
机构:
Chinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R ChinaChinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
Lv, Ningqing
Hu, Guangzhi
论文数: 0引用数: 0
h-index: 0
机构:
Yunnan Univ, Inst Ecol Res & Pollut Control Plateau Lakes, Sch Ecol & Environm Sci, Kunming 650504, Peoples R ChinaChinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
Hu, Guangzhi
Xu, Jian
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h-index: 0
机构:
Chinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R ChinaChinese Res Inst Environm Sci, State Key Lab Environm Criteria & Risk Assessment, Beijing 100012, Peoples R China
机构:
Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
Harbin Inst Technol, Sch Environm, Harbin 150090, Peoples R ChinaHarbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
Zhao, Yuanzhe
Wang, Xiuheng
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h-index: 0
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Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
Harbin Inst Technol, Sch Environm, Harbin 150090, Peoples R ChinaHarbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China