Jiang Hua, Gong Shuaiqi, Xu Shu, Shi Penghui, Fan Jinchen, Cecen Volkan, Xu QunJie, Min YuLin
Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, Shanghai University of Electric Power, Shanghai 200090, P.R. China.
Department of Chemical Engineering and Biointerfaces Institute, University of Michigan, Ann Arbor, MI 48109, USA.
Dalton Trans. 2020 Apr 28;49(16):5074-5086. doi: 10.1039/c9dt04935e.
A major challenge in the field of photocatalytic carbon dioxide (CO2) reduction is to design catalyst systems featuring high selectivity for CO production, long-term stability and a composition of Earth-abundant elements. Here, we present a metal-organic framework (MOF) based catalyst to mitigate the technical problems associated with the above-mentioned features. We report a carbon-coated CuNi alloy nanocatalyst obtained by high temperature vacuum treatment of a MOF material (CuNiBTC). The resulting carbon encapsulated CuNi (denoted as CuNi/C) nanoparticles possess a well-designed core-shell composite structure with graphene shells. Meanwhile, we investigated the reaction mechanism of CO2 on the surface of the CuNi/C photocatalyst in an aqueous solution containing triethanolamine. The experimental results show that the activity and catalytic yield of CuNi/C are much higher than those of Cu/C and Ni/C alone. At the same time, the catalytic activity of CuNi/C is also affected by changing the reaction temperature in the preparation process. As a result, the CuNi/C samples can achieve nearly 90% selectivity for NIR-light-driven CO2 reduction to CO. Our approach demonstrates the potential of non-semiconductor materials as catalysts for efficient and selective reduction of CO2 to CO.
光催化二氧化碳（CO₂）还原领域的一个主要挑战是设计出对一氧化碳（CO）生成具有高选择性、长期稳定性且由地球上储量丰富的元素组成的催化剂体系。在此，我们展示一种基于金属有机框架（MOF）的催化剂，以缓解与上述特性相关的技术问题。我们报道了一种通过对MOF材料（CuNiBTC）进行高温真空处理而获得的碳包覆CuNi合金纳米催化剂。所得的碳包覆CuNi（记为CuNi/C）纳米颗粒具有设计良好的核壳复合结构，外壳为石墨烯。同时，我们研究了在含有三乙醇胺的水溶液中CO₂在CuNi/C光催化剂表面的反应机理。实验结果表明，CuNi/C的活性和催化产率远高于单独的Cu/C和Ni/C。同时，在制备过程中改变反应温度也会影响CuNi/C的催化活性。结果，CuNi/C样品在近红外光驱动的CO₂还原为CO反应中可实现近90%的选择性。我们的方法证明了非半导体材料作为高效且选择性地将CO₂还原为CO的催化剂的潜力。
