Citation: Lina Zou, Dengke Wang, Shiqin Lai, Xunheng Jiang, Siqi Chen, Lanqing Deng, Dong Fan, Hengshuai Li, Zhigang Zhou, Denglong Chen, Xiangyang Yao, Jianping Zou. Local spin-state manipulation of iron single-atom sites induced by sulfur modification to boost Fenton-like reaction[J]. Chinese Chemical Letters, ;2025, 36(12): 111094. doi: 10.1016/j.cclet.2025.111094 shu

Local spin-state manipulation of iron single-atom sites induced by sulfur modification to boost Fenton-like reaction

Lina Zou ^a ,
Dengke Wang ^{a, *,} ,
Shiqin Lai ^a ,
Xunheng Jiang ^b ,
Siqi Chen ^a ,
Lanqing Deng ^a ,
Dong Fan ^c ,
Hengshuai Li ^{c, *,} ,
Zhigang Zhou ^a ,
Denglong Chen ^d ,
Xiangyang Yao ^e ,
Jianping Zou ^{a, *,}

a.
National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, China
b.
College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China
c.
School of Physics Science and Information Technology & Shandong Key Laboratory of Optical Communication Science and Technology, Liaocheng University, Liaocheng 252000, China
d.
Quangang Research Institute of Petrochemical Technology, Fujian Normal University, Fuzhou 350007, China
e.
Fujian Longking New Land Tech Co., Ltd., Fuzhou 350015, China

dengkewanglab@nchu.edu.cn

lihengshuai@lcu.edu.cn

zjp_112@126.com

Received Date: 29 October 2024
Revised Date: 24 January 2025
Accepted Date: 14 March 2025
Available Online: 14 March 2025

Figures(3)

A strategy based on local spin-state manipulation was achieved through S-modification on single-Fe-atom catalysts (Fe₁NSC). Spectral analyses and theoretical calculations elucidated that a medium-spin reconfiguration of Fe species in Fe₁NSC endowed an increased orbital overlap between Fe 3d and O 2p, reinforcing the peroxymonosulfate (PMS) dissociation kinetics. Consequently, Fe₁NSC delivered excellent performance in PMS conversion and pollutant degradation. The specific activity of PMS activation over Fe₁NSC reached 36.1 × 10^–3 L min^-1 m^-2, 4.2-folds that of Fe₁NC (8.61 × 10^–3 L min^-1 m^-2) and superior to the state-of-the-art catalysts reported to date. Importantly, the atomic spin-state modulation via S-modification can extend to other metals (Mn, Co and Cu) for improved PMS activation with > 3 times higher than those without S-modification. This work provides a universal scheme for electronic configuration regulation and highlights the significance of local environment modulation in designing high-performance catalysts for PMS activation.
- Single-atom catalyst,
- Iron spin state,
- Sulfur modification,
- Peroxymonosulfate activation,
- Organic pollutant
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