期刊
ACS CATALYSIS
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c04563
关键词
single-atoms; phase junction; synergetic effect; photocatalytic; CO2 reduction
资金
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- [21936005]
- [2020TQ0166]
- [2021M691771]
Reducing CO2 emissions through artificial photosynthesis is a significant strategy for converting solar energy into useful chemical feedstocks. However, most photocatalytic systems currently have low efficiency due to insufficient active sites and the lack of a directional charge-transfer channel. This study introduces single Cu atoms on nitrogen-doped carbon anchored on TiO2, which shows excellent performance in the photocatalytic reduction of CO2, achieving high CO selectivity and apparent quantum efficiency.
Reducing CO2 through artificial photosynthesis is a remarkable strategy for converting solar energy into useful chemical feedstocks. However, most photocatalytic systems suffer from low efficiency owing to insufficient active sites and the lack of a directional charge-transfer channel. Herein, we develop Cu single atoms (SAs) on the nitrogen-doped carbon anchored on TiO2 with the anatase-rutile mixed phase (Cu SAs/TiO2), which shows 100% CO selectivity and high apparent quantum efficiency of 2.0% at 420 nm in photocatalytic CO2 reduction with H2O vapor. Such a high performance is ascribed to the synergetic effect of Cu SAs and phase junction, where Cu SAs act as adsorption and activation sites of CO2 and phase junction accelerates the migration of photogenerated electrons along the Ti-N-Cu-(O-CO2) channel. Theoretical calculation further shows that the strong hybridization of Cu 3d and CO2-O 2p orbitals promotes the electron transfer from Cu SAs to CO2, effectively optimizing the rate-limiting step (CO2* -> COOH*).
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