Liu Dong-Cheng, Ouyang Ting, Xiao Ran, Liu Wen-Ju, Zhong Di-Chang, Xu Zhengtao, Lu Tong-Bu
Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China.
ChemSusChem. 2019 May 21;12(10):2166-2170. doi: 10.1002/cssc.201900338. Epub 2019 Apr 2.
Using solar energy to convert CO into valuable fuels or chemicals offers a powerful solution to urgent energy and environmental problems. However, the development of efficient and selective catalysts remains a considerable scientific challenge. To address this, catalytically active Co centers can be anchored into the porous matrix of metal-organic frameworks (MOFs) by utilizing a robust Zr-based MOF (Zr-DMBD) functionalized with freestanding thiol groups to enable efficient post-synthetic metal insertion. The thus-prepared Zr-DMBD-Co MOF solids are modified by well-defined Co-thiolate units and have the capability of photocatalytically converting CO into CO with high efficiency and selectivity under visible-light irradiation in a water-containing system. The turnover number and CO selectivity reach as high as 97 941 and 98 %, respectively.
利用太阳能将一氧化碳转化为有价值的燃料或化学品,为解决紧迫的能源和环境问题提供了有力的解决方案。然而,开发高效且具有选择性的催化剂仍然是一个重大的科学挑战。为了应对这一挑战,可以通过利用一种带有独立硫醇基团功能化的坚固锆基金属有机框架(Zr-DMBD),将具有催化活性的钴中心锚定到金属有机框架(MOF)的多孔基质中,以实现高效的合成后金属插入。如此制备的Zr-DMBD-Co MOF固体由明确的钴硫醇盐单元修饰,并且能够在含水体系的可见光照射下,将一氧化碳高效且选择性地光催化转化为一氧化碳。其转化数和一氧化碳选择性分别高达97941和98%。