Citation: Hao Zhang, Qian Liu, Zhurui Shen. Highly efficient photocatalytic conversion of CO₂ into CH₄ over Cu single atom promoted heterojunction: The effect of uplifted d-band center[J]. Chinese Chemical Letters, ;2024, 35(2): 108607. doi: 10.1016/j.cclet.2023.108607 shu

Highly efficient photocatalytic conversion of CO₂ into CH₄ over Cu single atom promoted heterojunction: The effect of uplifted d-band center

School of Materials Science and Engineering, Nankai University, Tianjin 300350, China

shenzhurui@nankai.edu.cn

Received Date: 20 March 2023
Revised Date: 21 April 2023
Accepted Date: 24 May 2023
Available Online: 25 May 2023

Figures(4)

Photoreduction of CO₂ to solar fuels has caused great interest, but suffers from low catalytic efficiency and poor selectivity. Herein, we designed a S-scheme heterojunction (Cu-TiO₂/WO₃) with Cu single atom to significantly boost the photoreduction of CO₂. Notably, the developed Cu-TiO₂/WO₃ achieved the solar-driven conversion of CO₂ to CH₄ with an evolution rate of 98.69 µmol g⁻¹ h⁻¹, and the electron selectivity of CH₄ reached 88.5%. The yield was much higher than those of pristine WO₃, TiO₂/WO₃ and Cu-TiO₂ samples. Experimental and theoretical analysis suggested that the S-scheme heterojunction accelerated charge migration and inhibited the recombination of electron-hole pairs. Importantly, the charge separation effect of the heterojunction meliorated the position of the d-band. The uplifted d-band centers of Cu and Ti on Cu-TiO₂/WO₃ not only improved the electron interaction between Cu single atoms and substrate-TiO₂, accelerated the adsorption and activation of CO₂ on the active sites of Cu single atom, but also optimized the Gibbs free energies of CH₄ formation pathway, leading to excellent selectivity toward CH₄. This work provides new insights into the design of photocatalyst systems with high photocatalytic performance.
- Cu single atom,
- Heterojunction,
- CO₂ photoreduction,
- d-band center,
- DFT
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Highly efficient photocatalytic conversion of CO2 into CH4 over Cu single atom promoted heterojunction: The effect of uplifted d-band center

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通讯作者: 陈斌, bchen63@163.com

Highly efficient photocatalytic conversion of CO₂ into CH₄ over Cu single atom promoted heterojunction: The effect of uplifted d-band center