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Cluster-based MOFs with accelerated chemical conversion of CO₂ through C–C bond formation
- XiongThese authors contributed equally to this work., Gang, Yu, Bing, Dong, Jie, Shi, Ying, Zhao, Bin, He, Liang-Nian
- Chemical communications 2017 v.53 no.44 pp. 6013-6016
- alkynes, carbon dioxide, carboxylation, catalysts, catalytic activity, chemical bonding, coordination compounds, feedstocks, greenhouse gas emissions, solvents
- Investigations on metal–organic frameworks (MOFs) as direct catalysts have been well documented, but direct catalysis of the chemical conversion of terminal alkynes and CO₂ as chemical feedstock by MOFs into valuable chemical products has never been reported. We report here two cluster-based MOFs I and II assembled from a multinuclear Gd-cluster and Cu-cluster, displaying high thermal and solvent stabilities. I and II as heterogeneous catalysts possess active catalytic centers [Cu₁₂I₁₂] and [Cu₃I₂], respectively, exhibiting excellent catalytic performance in the carboxylation reactions of CO₂ with 14 kinds of terminal alkynes under 1 atm and mild conditions. For the first time catalysis of the carboxylation reaction of terminal alkynes with CO₂ by MOF materials without any cocatalyst/additive is reported. This work not only reduces greenhouse gas emission but also provides highly valuable materials, opening a wide space in seeking recoverable catalysts to accelerate the chemical conversion of CO₂.