Phosphorus Tailors the d-Band Center of Copper Atomic Sites for Efficient CO2 Photoreduction under Visible-Light Irradiation

Xiaohui Sun, Lian Sun, Guanna Li, Yongxiao Tuo, Chenliang Ye, Jiarui Yang, Jingxiang Low, Xiang Yu, Johannes H. Bitter, Yongpeng Lei, Dingsheng Wang, Yadong Li*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

9 Citations (Scopus)

Abstract

Photoreduction of CO2 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, Cu1N3@PCN and Cu1P3@PCN were fabricated via selective phosphidation, and tested in visible light-driven CO2 reduction by H2O without sacrificial agents. Cu1N3@PCN was exclusively active for CO production with a rate of 49.8 μmolCO gcat−1 h−1, outperforming most polymeric carbon nitride (C3N4) based catalysts, while Cu1P3@PCN preferably yielded H2. Experimental and theoretical analysis suggested that doping P in C3N4 by replacing a corner C atom upshifted the d-band center of Cu in Cu1N3@PCN close to the Fermi level, which boosted the adsorption and activation of CO2 on Cu1N3, making Cu1N3@PCN efficiently convert CO2 to CO. In contrast, Cu1P3@PCN with a much lower Cu 3d electron energy exhibited negligible CO2 adsorption, thereby preferring H2 formation via photocatalytic H2O splitting.

Original languageEnglish
Article numbere202207677
JournalAngewandte Chemie - International Edition
Volume61
Issue number38
DOIs
Publication statusPublished - 19 Sep 2022

Keywords

  • CO Photoreduction
  • d-Band Center
  • Phosphorus
  • Selectivity
  • Single Cu Atom

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