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Abstract
Chemical fixation of carbon dioxide (CO2) may be a pathway to retard the current trend of rapid global warming. However, the current economic cost of chemical fixation remains high because the chemical fixation of CO2 usually requires high temperature or high pressure. The rational design of an efficient catalyst that works at ambient conditions might substantially reduce the economic cost of fixation. Here, we report the rational design of covalent organic frameworks (COFs) as efficient CO2 fixation catalysts under ambient conditions based on the finding of “pore enrichment”, which is concluded by a detailed investigation of the 10994 COFs. The best predicted COF, Zn-Salen-COF-SDU113, is synthesized, and its efficient catalytic performance for CO2 cycloaddition to terminal epoxide is confirmed with a yield of 98.2% and turnover number (TON) of 3068.9 under ambient conditions, which is comparable to the reported leading catalysts. Moreover, this COF achieves the cycloaddition of CO2 to 2,3-epoxybutane under ambient conditions among all porous materials. This work provides a strategy for designing porous catalysts in the economic fixation of carbon dioxide.
Currently the cost of CO2 chemical fixation remains high because of harsh reaction conditions. Here, the authors report a covalent organic framework screened from 10994 candidates as the efficient CO2 fixation catalyst under ambient conditions based on the finding of a “pore enrichment effect”.
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1 Shandong University, Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Qingdao, P. R. China (GRID:grid.27255.37) (ISNI:0000 0004 1761 1174)
2 Shandong University, Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Qingdao, P. R. China (GRID:grid.27255.37) (ISNI:0000 0004 1761 1174); China Three Gorges University, Collage of Hydraulic & Environmental Engineering, Yichang, P. R. China (GRID:grid.254148.e) (ISNI:0000 0001 0033 6389)
3 Shandong University, Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Qingdao, P. R. China (GRID:grid.27255.37) (ISNI:0000 0004 1761 1174); Chinese Academy of Sciences, State Key Laboratory of Molecular Reaction Dynamics, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Dalian, P. R. China (GRID:grid.9227.e) (ISNI:0000000119573309); University of the Chinese Academy of Sciences, Beijing, P. R. China (GRID:grid.410726.6) (ISNI:0000 0004 1797 8419)
4 China Three Gorges University, Collage of Hydraulic & Environmental Engineering, Yichang, P. R. China (GRID:grid.254148.e) (ISNI:0000 0001 0033 6389)
5 Shandong University, Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Qingdao, P. R. China (GRID:grid.27255.37) (ISNI:0000 0004 1761 1174); Chinese Academy of Sciences, State Key Laboratory of Molecular Reaction Dynamics, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Dalian, P. R. China (GRID:grid.9227.e) (ISNI:0000000119573309)