Citation: Cheng Han, Lanlan Liang, Jiao Yang, Yin Wei, Zhe Zhang, Haonan Chen, Wei Yu, Chuanliang Zhao, Liwei Yang, Bo Lai. Si–O doped layered carbon-based catalyst boosts nonradical oxidation pathways via peroxymonosulfate activation for refractory organic pollutants removal[J]. Chinese Chemical Letters, ;2026, 37(9): 112410. doi: 10.1016/j.cclet.2026.112410 shu

Si–O doped layered carbon-based catalyst boosts nonradical oxidation pathways via peroxymonosulfate activation for refractory organic pollutants removal

Cheng Han ^a ,
Lanlan Liang ^a ,
Jiao Yang ^a ,
Yin Wei ^a ,
Zhe Zhang ^a ,
Haonan Chen ^a ,
Wei Yu ^a ,
Chuanliang Zhao ^{a, *,} ,
Liwei Yang ^{a, *,} ,
Bo Lai ^b

a.
Key Laboratory of Water Supply & Sewage Engineering of Ministry of Housing and Urban-rural Development, School of Civil Engineering, Chang’an University, Xi’an 710061, China
b.
State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China

zhaochuanliang90@sina.com

yanglw61@163.com

Received Date: 20 August 2025
Revised Date: 16 November 2025
Accepted Date: 12 January 2026
Available Online: 13 January 2026

Figures(7)

Traditional carbon-based catalysts often suffer from limited catalytic activity and stability in peroxymonosulfate (PMS) activation for pollutant degradation. In this study, a Si–O doped layered carbonaceous catalyst (Si/C@PDA) was synthesized using natural vermiculite as the hard template, enabling the efficient PMS activation for ultrafast degradation of tetracycline (TC) (k_obs-TC = 0.228 min^–1). The Si/C@PDA/PMS system demonstrated strong resistance to environmental matrix interference by enhanced singlet oxygen (¹O₂) generation and electron transfer processes (ETP). The experimental and density functional theory results prove that the Si–O site induced the cleavage of adsorbed PMS to promote the generation of ¹O₂ through the self-decomposition of peroxymonosulfate anion radical (SO₅^•–) and the disproportionation of superoxide radical (O₂^•–). Meanwhile, the Si–O site also served as the electron transfer bridge facilitating electron migration from the pollutants to the Si/C@PDA/PMS*. In addition, the Si/C@PDA/PMS system integrated with membrane filtration technology achieved continuous degradation of TC with nearly 100% removal efficiency under a low oxidant dosage (0.1 mmol/L PMS). This work underscores the pivotal role of Si–O doping in modulating active sites to selectively promote nonradical pathways, thereby promoting effective pollutant degradation in complex water matrices and offering strategic insights for developing nonradical-dominated carbon-based catalysts.
- Carbon-based catalysts,
- Si–O doped,
- Peroxymonosulfate,
- Singlet oxygen,
- Density functional theory calculations
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