Constructing Fe4+-N4S Coordination via S+ Ion Implantation for Highly Activating Photocatalytic CO_2RR

Tao Jiang ¹Shixin Wu ²Zhuo Xing ³Wenbin Zuo ⁴Liqiu Huang ²Derun Li ⁵Shuangfeng Jia ⁶Hengyi Wu ²Feng Ren⁶

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作者信息

1. School of Physics and Technology Center for Ion Beam Application Hubei Key Laboratory of Nuclear Solid Physics Wuhan University Wuhan 430072, China||Department of Physics Wuhan University of Technology Wuhan 430070, China
2. School of Physics and Technology Center for Ion Beam Application Hubei Key Laboratory of Nuclear Solid Physics Wuhan University Wuhan 430072, China
3. College of Physical Science and Technology Central China Normal University Wuhan 430079, China
4. School of Integrated Circuits Huazhong University of Science and Technology Wuhan 430074, China
5. School of Materials Science and Engineering HubeiNormal University Huangshi 435002, China
6. Center for Electron Microscopy MOEKey Laboratory of ArtificialMicro- and Nano-Structures Wuhan University Wuhan 430072, China
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Abstract

Although metal single atoms in photocatalysts can promote the CO_2 adsorption and reduction, it is still limited by the low valence state of metal single atoms. Here, S-Fe single-atom-loaded (S-Fe-hCN) nanosheets are synthesized by spark plasma sintering (SPS) and following S+ ion implantation. Benefiting from the mandatory nature of ion implantation technique, it not only reaches high content of S-doping, but also forms a high valence state of Fe and a special metal single-atom coordination structure, which greatly improves CO_2RR performance, and achieves 1100 times enhancement in CO yield with high yield of 110 μmol g~(-1) h~(-1), 100% CO selectivity, and a high quantum efficiency of 10.1% at 420 nm. EXAFS, in situ Mössbauer spectroscopy, and DFT calculations all reveal that S+ ion implantation constructs a Fe4+-N4S coordination structure, leading to the high electron transfer, which builds a stable CO_2-Fe-N4S adsorption state, opens the C═O double bond, and activates the O atom.

Key words

CO_2RR/Electron transfer/Ion implantation/Single atom catalysts/S-doping

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出版年

2026

Advanced materials for optics and electronics

ISSN：1616-301X

参考文献量41

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