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The Significance of Metal Coordination in Imidazole-Functionalized Metal–Organic Frameworks for Carbon Dioxide Utilization |
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| Authors: | William R Webb Matthew E Potter Daniel J Stewart Stuart J Elliott Pier J A Sazio Zhongxing Zhang He-Kuan Luo Jinghua Teng Liling Zhang Chiara Ivaldi Ivana Miletto Enrica Gianotti Prof Robert Raja |
| Institution: | 1. School of Chemistry, University of Southampton, Southampton, SO17 1BJ UK;2. Optoelectronics Research Centre, University of Southampton, Southampton, SO17 1BJ UK;3. Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR), Innovis, 2 Fusionopolis Way, Singapore, 138634 Singapore;4. Institute for High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR), 16-16 Connexis (North), 1 Fusionopolis Way, Singapore, 138632 Singapore;5. Department of Science and Technological Innovation, Università del, Piemonte Orientale, Viale T. Michel 11, 15121 Alessandria, Italy |
| Abstract: | The grafting of imidazole species onto coordinatively unsaturated sites within metal–organic framework MIL-101(Cr) enables enhanced CO2 capture in close proximity to catalytic sites. The subsequent combination of CO2 and epoxide binding sites, as shown through theoretical findings, significantly improves the rate of cyclic carbonate formation, producing a highly active CO2 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). |
| Keywords: | carbon dioxide utilization catalysis cyclic carbonates grafting imidazoles metal–organic frameworks |