Modulating Charge Separation of Oxygen-Doped Boron Nitride with Isolated Co Atoms for Enhancing CO2-to-CO Photoreduction

Jianli Liang, Huabin Zhang, Qianqian Song, Zheyang Liu, Jing Xia, Binhang Yan, Xiangmin Meng, Zhifeng Jiang*, Xiong Wen Lou*, Chun Sing Lee*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

To alleviate the greenhouse effect and address the related energy crisis, solar-driven reduction of carbon dioxide (CO2) to value-added products is considered as a sustainable strategy. However, the insufficient separation and rapid recombination of photogenerated charge carriers during photocatalysis greatly limit their reduction efficiency and practical application potential. Here, isolated Cobalt (Co) atoms are successfully decorated into oxygen-doped boron nitride (BN) via an in situ pyrolysis method, achieving greatly improved catalytic activity and selectivity to the carbon monoxide (CO) product. X-ray absorption fine spectroscopy demonstrates that the isolated Co atoms are stabilized by the O and N atoms with an unsaturated CoO2N1 configuration. Further experimental investigation and theoretical simulations confirm that the decorated Co atoms not only work as the real active center during the CO2 reduction process, but also perform as the electron pump to promote the electron/hole separation and transfer, resulting in greatly accelerated reaction kinetics and improved activity. In addition, the CoO2N1 coordination geometry is favorable to the conversion from *CO2 to *COOH, which shall be considered as a selectivity-determining step for the evolution of the CO products. The surface modulation strategy at the atomic level opens a new avenue for regulating the reaction kinetics for photocatalytic CO2 reduction.

Original languageEnglish (US)
Article number2303287
JournalAdvanced Materials
Volume36
Issue number1
DOIs
StatePublished - Jan 4 2024

Bibliographical note

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

Keywords

  • CO reduction reaction
  • coordination environment
  • electron/hole separation
  • photocatalysis
  • single-atom catalysts

ASJC Scopus subject areas

  • General Materials Science
  • Mechanics of Materials
  • Mechanical Engineering

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