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Atomically Dispersed Indium‐Copper Dual‐Metal Active Sites Promoting C−C Coupling for CO 2 Photoreduction to Ethanol

2022; Wiley; Volume: 61; Issue: 40 Linguagem: Inglês

10.1002/anie.202208904

1521-3773

Hainan Shi, Haozhi Wang, Yichen Zhou, Jiahui Li, Panlong Zhai, Xiangyang Li, Gagik G. Gurzadyan, Jungang Hou, Hong Yang, Xinwen Guo,

Covalent Organic Framework Applications

Photoreduction of CO2 to C2+ solar fuel is a promising carbon-neutral technology for renewable energy. This strategy is challenged by its low productivity due to low efficiency in multielectron utilization and slow C-C coupling kinetics. This work reports a dual-metal photocatalyst consisting of atomically dispersed indium and copper anchored on polymeric carbon nitride (InCu/PCN), on which the photoreduction of CO2 delivered an excellent ethanol production rate of 28.5 μmol g-1 h-1 with a high selectivity of 92 %. Coupled experimental investigation and DFT calculations reveal the following mechanisms underpinning the high performance of this catalyst. Essentially, the In-Cu interaction enhances the charge separation by accelerating charge transfer from PCN to the metal sites. Indium also transfers electrons to neighboring copper via Cu-N-In bridges, increasing the electron density of copper active sites. Furthermore, In-Cu dual-metal sites promote the adsorption of *CO intermediates and lower the energy barrier of C-C coupling.