| Autor: |
Song, Wentao, Wang, Cheng, Liu, Yong, Chong, Kok Chan, Zhang, Xinyue, Wang, Tie, Zhang, Yuanming, Li, Bowen, Tian, Jianwu, Zhang, Xianhe, Wang, Xinyun, Yao, Bingqing, Wang, Xi, Xiao, Yukun, Yao, Yingfang, Mao, Xianwen, He, Qian, Lin, Zhiqun, Zou, Zhigang, Liu, Bin |
| Zdroj: |
Journal of the American Chemical Society; October 2024, Vol. 146 Issue: 42 p29028-29039, 12p |
| Abstrakt: |
Solar-driven carbon dioxide (CO2) reduction into C2+products such as ethylene represents an enticing route toward achieving carbon neutrality. However, due to sluggish electron transfer and intricate C–C coupling, it remains challenging to achieve highly efficient and selective ethylene production from CO2and H2O beyond capitalizing on Cu-based catalysts. Herein, we report a judicious design to attain asymmetric C–C coupling through interfacial defect-rendered tandem catalytic centers within a sulfur-vacancy-rich MoSx/Fe2O3photocatalyst sheet, enabling a robust CO2photoreduction to ethylene without the need for copper, noble metals, and sacrificial agents. Specifically, interfacial S vacancies induce adjacent under-coordinated S atoms to form Fe–S bonds as a rapid electron-transfer pathway for yielding a Z-scheme band alignment. Moreover, these S vacancies further modulate the strong coupling interaction to generate a nitrogenase-analogous Mo–Fe heteronuclear unit and induce the upward shift of the d-band center. This bioinspired interface structure effectively suppresses electrostatic repulsion between neighboring *CO and *COH intermediates via d-p hybridization, ultimately facilitating an asymmetric C–C coupling to achieve a remarkable solar-to-chemical efficiency of 0.565% with a superior selectivity of 84.9% for ethylene production. Further strengthened by MoSx/WO3, our design unveils a promising platform for optimizing interfacial electron transfer and offers a new option for C2+synthesis from CO2and H2O using copper-free and noble metal-free catalysts. |
| Databáze: |
Supplemental Index |
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