Shi Hainan, Wang Haozhi, Zhou Yichen, Li Jiahui, Zhai Panlong, Li Xiangyang, Gurzadyan Gagik G, Hou Jungang, Yang Hong, Guo Xinwen
State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, and School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, China.
Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou, 350207, China.
Angew Chem Int Ed Engl. 2022 Oct 4;61(40):e202208904. doi: 10.1002/anie.202208904. Epub 2022 Aug 25.
Photoreduction of CO to C 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 CO delivered an excellent ethanol production rate of 28.5 μmol g h 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.
将CO光还原为C太阳能燃料是一种很有前景的可再生能源碳中性技术。由于多电子利用效率低和C-C偶联动力学缓慢，该策略面临着生产率低的挑战。这项工作报道了一种双金属光催化剂，由锚定在聚合氮化碳上的原子分散铟和铜组成（InCu/PCN），在该催化剂上，CO的光还原产生了28.5 μmol g h的优异乙醇产率，选择性高达92%。结合实验研究和DFT计算揭示了该催化剂高性能背后的以下机制。本质上，In-Cu相互作用通过加速电荷从PCN转移到金属位点来增强电荷分离。铟还通过Cu-N-In桥将电子转移到相邻的铜，增加了铜活性位点的电子密度。此外，In-Cu双金属位点促进了*CO中间体的吸附，并降低了C-C偶联的能垒。
