Citation: Jinxin Li, Yifan Ren, Jianan Gao, Nadeeshani Nanayakkara, Xin Wang, Meng Liu, Yanbiao Liu. Asymmetric triple-atomic sites with modulated electronic structure toward boosted peroxymonosulfate activation[J]. Chinese Chemical Letters, ;2026, 37(2): 111355. doi: 10.1016/j.cclet.2025.111355 shu

Asymmetric triple-atomic sites with modulated electronic structure toward boosted peroxymonosulfate activation

Jinxin Li ^a ,
Yifan Ren ^{a, *,} ,
Jianan Gao ^b ,
Nadeeshani Nanayakkara ^c ,
Xin Wang ^a ,
Meng Liu ^a ,
Yanbiao Liu ^{a, *,}

a.
School of Environmental Science and Technology, Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), Dalian University of Technology, Dalian 116024, China
b.
Department of Civil Engineering, The University of Hong Kong, Hong Kong SAR 999077, China
c.
Department of Civil Engineering, Faculty of Engineering, University of Peradeniya, Peradeniya 20400, Sri Lanka

yifanren@dlut.edu.cn

yanbiaoliu@dlut.edu.cn

Received Date: 8 January 2025
Revised Date: 20 March 2025
Accepted Date: 20 May 2025
Available Online: 21 May 2025

Figures(4)

Peroxymonosulfate (PMS)-based advanced oxidation technology has been proven to be a viable option for the decontamination of organic pollutants from water bodies. Advanced catalyst design is essential to this technology. Herein, a vanadium-doped LaFeO₃ perovskite (LFO-V) featuring asymmetric Fe-O-V sites was rationally designed. Thanks to orbital electron interaction between Fe and V atoms, the modified electronic structure elevated electron density near the Fermi energy level while reducing the energy barrier toward effective PMS activation. This facilitated concurrent PMS reduction at the Fe sites to generate SO₄^•- and ^•OH (57.7%), and PMS oxidation at V sites to produce ¹O₂ (42.3%). The LFO-V/PMS system demonstrated excellent tetracycline (TC) degradation performance with a 2-fold enhancement in rate constant compared to that of pristine LFO. Further, the LFO-V maintained long-term stability, and the toxicity of degradation intermediates was evaluated through microbial metabolomics. This work establishes an effective route to regulate the PMS activation pathways through precise electronic structure modulation, advancing the rational design of advanced Fenton-like catalysts.
- Electric structure modulation,
- Fe-O-V sites,
- Reduction-oxidation,
- Radical species,
- Non-radical species
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