Webb William R, Potter Matthew E, Stewart Daniel J, Elliott Stuart J, Sazio Pier J A, Zhang Zhongxing, Luo He-Kuan, Teng Jinghua, Zhang Liling, Ivaldi Chiara, Miletto Ivana, Gianotti Enrica, Raja Robert
School of Chemistry, University of Southampton, Southampton, SO17 1BJ, UK.
Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR), Innovis, 2 Fusionopolis Way, Singapore, 138634, Singapore.
Chemistry. 2020 Oct 27;26(60):13606-13610. doi: 10.1002/chem.202001561. Epub 2020 Sep 29.
The grafting of imidazole species onto coordinatively unsaturated sites within metal-organic framework MIL-101(Cr) enables enhanced CO capture in close proximity to catalytic sites. The subsequent combination of CO and epoxide binding sites, as shown through theoretical findings, significantly improves the rate of cyclic carbonate formation, producing a highly active CO utilization catalyst. An array of spectroscopic investigations, in combination with theoretical calculations reveal the nature of the active sites and associated catalytic mechanism which validates the careful design of the hybrid MIL-101(Cr).
将咪唑类物质接枝到金属有机框架MIL-101(Cr)内的配位不饱和位点上，能够在靠近催化位点的位置增强对CO的捕获。理论研究结果表明，随后将CO结合位点和环氧化物结合位点相结合，可显著提高环状碳酸酯的生成速率，从而制得一种高活性的CO利用催化剂。一系列光谱研究与理论计算相结合，揭示了活性位点的性质及相关催化机理，这证实了对混合材料MIL-101(Cr)的精心设计。
