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Title: Synergistic effect of Ru-N₄ sites and Cu-N₃ sites in carbon nitride for highly selective photocatalytic reduction of CO₂ to methane
Authors: Zeng, Lei
Chen, Jie-Wei
Zhong, Lixiang
Zhen, Wenlong
Tay, Yee Yan
Li, Shuzhou
Wang, Yanggang
Huang, Limin
Xue, Can
Keywords: Engineering::Materials
Issue Date: 2022
Source: Zeng, L., Chen, J., Zhong, L., Zhen, W., Tay, Y. Y., Li, S., Wang, Y., Huang, L. & Xue, C. (2022). Synergistic effect of Ru-N₄ sites and Cu-N₃ sites in carbon nitride for highly selective photocatalytic reduction of CO₂ to methane. Applied Catalysis B: Environmental, 307, 121154-.
Project: MOE2018-T2-1-017 
MOE2019-T1- 002-012 
Journal: Applied Catalysis B: Environmental 
Abstract: Developing single-atom photocatalysts for selective conversion of CO2 to valuable fuel is of great attraction but remains challenging. In this work, ruthenium and copper single atoms are for the first time simultaneously incorporated into polymeric carbon nitride (PCN) through a simple preassembly-coprecipitation-pyrolysis process. The obtained PCN-RuCu sample exhibited much higher selectivity (95%) for CH4 production than the individual Ru or Cu decorated PCN during photocatalytic CO2 reduction under visible-light irradiation. The atomically dispersed Ru-N4 and Cu-N3 moieties were confirmed by spherical aberration-corrected electron microscopy and extended X-ray absorption fine structure spectroscopy. Density function theory (DFT) calculations revealed that the co-existence of Ru-N4 sites and Cu-N3 sites can effectively tune the electronic structure of PCN, making the Ru sites account for photogenerated electron-hole pairs and the Cu sites for CO2 hydrogenation. Moreover, the synergetic effect between Ru and Cu single atoms significantly promotes the consecutive hydrogenation processes of *CO species towards CH4 production. Our studies provide a new understanding of the mechanism for photocatalytic reduction of CO2 to CH4, and pave a new way to design photocatalysts for the selective production of solar fuels.
ISSN: 0926-3373
DOI: 10.1016/j.apcatb.2022.121154
Schools: School of Materials Science and Engineering 
Research Centres: Facility for Advanced Characterization
Rights: © 2022 Elsevier B.V. All rights reserved. This paper was published in Applied Catalysis B: Environmental and is made available with permission of Elsevier B.V.
Fulltext Permission: embargo_20240707
Fulltext Availability: With Fulltext
Appears in Collections:MSE Journal Articles

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