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Phosphorus Tailors the<i>d</i>‐Band Center of Copper Atomic Sites for Efficient CO<sub>2</sub>Photoreduction under Visible‐Light Irradiation

Xiaohui SunDepartment of Chemistry Tsinghua University Beijing 100084 P. R. ChinaLian Feng SunState Key Laboratory of Powder Metallurgy Central South University Changsha 410083 P. R. ChinaGuanna LiBiobased Chemistry and Technology Wageningen University & Research Bornse Weilanden 9 Wageningen 6708WG The NetherlandsYongxiao TuoDepartment of Materials Science and Engineering China University of Petroleum (Huadong) Qingdao 266580 P. R. ChinaChenliang YeDepartment of Chemistry Tsinghua University Beijing 100084 P. R. ChinaJiarui YangDepartment of Chemistry Tsinghua University Beijing 100084 P. R. ChinaJingxiang LowHefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Hefei 230026 P. R. ChinaXiang YuInstitute of Microscale Optoelectronics Shenzhen University Shenzhen 518060 P. R. ChinaJohannes H. BitterBiobased Chemistry and Technology Wageningen University & Research Bornse Weilanden 9 Wageningen 6708WG The NetherlandsYongpeng LeiState Key Laboratory of Powder Metallurgy Central South University Changsha 410083 P. R. ChinaDingsheng WangDepartment of Chemistry Tsinghua University Beijing 100084 P. R. ChinaYadong LiDepartment of Chemistry Tsinghua University Beijing 100084 P. R. China

2022en

ABI

Annotatsiya

Abstract Photoreduction of CO 2 into solar fuels has received great interest, but suffers from low catalytic efficiency and poor selectivity. Herein, two single‐Cu‐atom catalysts with unique Cu configurations in phosphorus‐doped carbon nitride (PCN), namely, Cu 1 N 3 @PCN and Cu 1 P 3 @PCN were fabricated via selective phosphidation, and tested in visible light‐driven CO 2 reduction by H 2 O without sacrificial agents. Cu 1 N 3 @PCN was exclusively active for CO production with a rate of 49.8 μmol CO g cat −1 h −1 , outperforming most polymeric carbon nitride (C 3 N 4 ) based catalysts, while Cu 1 P 3 @PCN preferably yielded H 2 . Experimental and theoretical analysis suggested that doping P in C 3 N 4 by replacing a corner C atom upshifted the d ‐band center of Cu in Cu 1 N 3 @PCN close to the Fermi level, which boosted the adsorption and activation of CO 2 on Cu 1 N 3 , making Cu 1 N 3 @PCN efficiently convert CO 2 to CO. In contrast, Cu 1 P 3 @PCN with a much lower Cu 3d electron energy exhibited negligible CO 2 adsorption, thereby preferring H 2 formation via photocatalytic H 2 O splitting.

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Identifikatorlar

DOI: 10.1002/anie.202207677

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