Indirect methanol synthesis from CO2 through high-efficient dimethyl carbonate hydrogenation as a bridge below 100℃

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Abstract

Developing an energy-efficient process for transformation of chemically inert CO 2 to methanol is of great significance. Herein, we report an indirect CO 2 transformation for methanol synthesis below 100 ℃, utilizing dimethyl carbonate (DMC), a readily available compound produced from CO 2 , as a bridge. A Lewis acidic combination of spatially intimate In 5 sites and In 4 ··· ּ In 4 pairs is constructed on In 2 O 3 through regulating oxygen vacancies for effective activation of H 2 and DMC, respectively. Their spatial intimacy facilitates the transfer of generated H* for DMC hydrogenation, giving a methanol generation rate of 31.6 mmol ּ g cat -1 h -1 with a selectivity exceeding 99.99% at 100 ℃. Coupling the capability of In 2 O 3 for DMC synthesis from CO 2 , we demonstrate a sequential DMC synthesis and hydrogenation process within the same reactor by alternating gaseous reactants to yield methanol with a rate of 6.4 mmol ּ g cat -1 h -1 at 100 ℃, surpassing the performance of previous catalysts through direct CO 2 hydrogenation, even at temperatures over 200 ℃.

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