南方科技大学徐强团队近日实现了金属-有机骨架中Cu单原子与Cu掺杂金纳米粒子协同光催化CO₂还原为C₂H₆。2025年6月17日出版的《美国化学会志》发表了这项成果。

光催化CO₂还原为C₂烃被认为更有价值，但由于多电子过程和C-C偶联的缓慢动力学，这需要多个活性位点协同工作，因此极具挑战性。在这项工作中，通过光沉积方法，铜单原子位点和原子铜掺杂的金纳米粒子同时锚定在具有介孔通道的光活性金属有机框架（MOF）上，在封闭环境中紧密整合不同的位点。

由于等离子体金属纳米粒子的电子积累和不同活性位点之间的协同作用，这种MOF复合材料可以实现CO₂到C₂H₆的高效光催化还原，生产率高达69.9 μmol g^–1 h^–1，选择性高达71.1%。对照样品的光催化实验揭示了不同活性位点在每个步骤中的关键作用，这进一步得到了原位表征和理论计算的证实。这一发现突显了MOF作为整合各种活性位点以实现协同催化应用的理想平台的潜力。 

附：英文原文

Title: Synergistic Catalysis by Cu Single Atoms and Atomically Cu-Doped Au Nanoparticles in a Metal–Organic Framework for Photocatalytic CO2 Reduction to C2H6

Author: Di Chen, Bingxian Chu, Fayan Li, Yu-Tao Zheng, Yu Lu, Bing Shao, Lei Li, Ning-Yu Huang, Qiang Xu

Issue&Volume: June 17, 2025

Abstract: Photocatalytic CO2 reduction to C2 hydrocarbons is considered more valuable and yet highly challenging due to the multielectron process and sluggish kinetics of C–C coupling, which requires multiple active sites to work synergistically. In this work, through a photodeposition method, Cu single-atom sites and atomically Cu-doped Au nanoparticles were simultaneously anchored on a photoactive metal–organic framework (MOF) with mesoporous channels, closely integrating distinct sites within a confined environment. Thanks to the electron accumulation of plasmonic metal nanoparticles and the synergy among different active sites, this MOF composite can achieve efficient photocatalytic reduction of CO2  to C2H6 with a production rate as high as 69.9 μmol g–1 h–1 and a selectivity as high as 71.1%. Photocatalytic experiments with control samples unveiled the critical roles of different active sites at each step, which was further confirmed by in situ characterizations and theoretical calculations. This finding highlights the potential of MOFs as an ideal platform for the integration of various active sites for synergistically catalytic applications.

DOI: 10.1021/jacs.5c04364

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c04364