Metal-organic frameworks MOF-808-X as highly efficient catalysts for direct synthesis of dimethyl carbonate from CO2 and methanol

doi:10.1016/S1872-2067(19)63291-2

Abstract

Abstract:

A series of metal-organic frameworks MOF-808-X (6-connected) were synthesized by regulating the ZrOCl₂·8H₂O/1,3,5-benzenetricarboxylic acid (BTC) molar ratio (X) and tested for the direct synthesis of dimethyl carbonate (DMC) from CO₂ and CH₃OH with 1,1,1-trimethoxymethane (TMM) as a dehydrating agent. The effect of the ZrOCl₂·8H₂O/BTC molar ratio on the physicochemical properties and catalytic performance of MOF-808-X was investigated. Results showed that a proper ZrOCl₂·8H₂O/BTC molar ratio during MOF-808-X synthesis was fairly important to reduce the redundant BTC or zirconium clusters trapped in the micropores of MOF-808-X. MOF-808-4, with almost no redundant BTC or zirconium clusters trapped in the micropores, exhibited the largest surface area, micropore size, and the number of acidic-basic sites, and consequently showed the best activity among all MOF-808-X, with the highest DMC yield of 21.5% under the optimal reaction conditions. Moreover, benefiting from the larger micropore size, MOF-808-4 outperformed our previously reported UiO-66-24 (12-connected), which had even more acidic-basic sites and larger surface area than MOF-808-4, mainly because the larger micropore size of MOF-808-4 provided higher accessibility for the reactant to the active sites located in the micropores. Furthermore, a possible reaction mechanism over MOF-808-4 was proposed based on the in situ FT-IR results. The effects of different reaction parameters on DMC formation and the reusability of MOF-808-X were also studied.

Key words: Metal-organic frameworks, MOF-808, Micropore size, Carbon dioxide utilization, Dimethyl carbonate

Keng Xuan, Yanfeng Pu, Feng Li, Jing Luo, Ning Zhao, Fukui Xiao. Metal-organic frameworks MOF-808-X as highly efficient catalysts for direct synthesis of dimethyl carbonate from CO₂ and methanol[J]. Chinese Journal of Catalysis, 2019, 40(4): 553-566.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(19)63291-2

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Metal-organic frameworks MOF-808-X as highly efficient catalysts for direct synthesis of dimethyl carbonate from CO₂ and methanol

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