Han Bin, Ou Xinwen, Deng Ziqi, Song Yao, Tian Chen, Deng Hong, Xu Yi-Jun, Lin Zhang
School of Environment and Energy, Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters (Ministry of Education), South China University of Technology, Guangzhou, P. R. China.
Guangdong Engineering and Technology Research Center for Environmental Nanomaterials, South China University of Technology, Guangzhou, 510006, P. R. China.
Angew Chem Int Ed Engl. 2018 Dec 17;57(51):16811-16815. doi: 10.1002/anie.201811545. Epub 2018 Nov 21.
Photocatalytic conversion of diluted CO into solar fuel is highly appealing yet still in its infancy. Herein, we demonstrate the metal-node-dependent performance for photoreduction of diluted CO by constructing Ni metal-organic framework (MOF) monolayers (Ni MOLs). In diluted CO (10 %), Ni MOLs exhibit a highest apparent quantum yield of 1.96 % with a CO selectivity of 96.8 %, which not only exceeds reported systems in diluted CO but also is superior to most catalysts in pure CO . Whereas isostructural Co MOLs is almost inactive in diluted CO , indicating the performance is dependent on the metal nodes. Experimental and theoretical investigations show that strong CO binding affinity of Ni MOLs is the crucial factor, which stabilizes the Ni-CO adducts and facilitates CO -to-CO conversion.
将稀释后的一氧化碳光催化转化为太阳能燃料极具吸引力，但仍处于起步阶段。在此，我们通过构建镍金属有机框架（MOF）单层（Ni MOLs），展示了其对稀释一氧化碳光还原的金属节点依赖性性能。在稀释的一氧化碳（10%）中，Ni MOLs表现出最高1.96%的表观量子产率和96.8%的一氧化碳选择性，这不仅超过了报道的在稀释一氧化碳中的体系，而且优于大多数在纯一氧化碳中的催化剂。而异结构的钴MOLs在稀释的一氧化碳中几乎没有活性，这表明性能取决于金属节点。实验和理论研究表明，Ni MOLs对一氧化碳的强结合亲和力是关键因素，它稳定了镍-一氧化碳加合物并促进了一氧化碳到一氧化碳的转化。
