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Conversion of Carbon Dioxide into a Versatile Green Solvent with Isoreticular Metal-Organic Frameworks

CSEF · 2023 Chemistry Second Award

Kang Sehoon, Zhang Zhehao · 11

Overview

Recent advances in CO2 capture and fixation allowed the transformation of atmospheric CO2 into useful organic molecules, but they are limited by extreme reaction conditions and the absence of optimal catalysts. Herein, we synthesized two series (zinc and zirconium) of isoreticular metal-organic frameworks (IRMOFs), functionalized porous materials with abundant Lewis-acid sites, in varying pore sizes, and nitrogen sites as heterogeneous catalysts for the cycloaddition of CO2 and epoxides to cyclic carbonates under mild conditions. Notably, the catalytic performances of Zr-IRMOFs with high retention properties due to their structural stability exceeded those of Zn-IRMOFs. In addition, comparing the BPDC and BDC ligands demonstrates that the optimal pore size for catalysis was 12-16 Å. Besides, functionalized nitrogen sites of the BPYDC ligand were exhibited to play a crucial role in providing additional binding sites for CO2 adsorption and abundant Lewis base sites for CO2 activation, with Zr-BPYDC having catalytic performance (98.2% conversion rate and over 99% selectivity at 0.05mol% loading) far exceeding that of the traditional catalysts available. A catalytic mechanism behind the cycloaddition reaction is also proposed based on a literature study and GC-MS analysis of the reaction mixture. Our research adds important insight to the systematic understanding of different physical and chemical properties of MOFs that influence CO2 conversion.

Source coverage

This record comes from a published award list, not a complete project archive. Its abstract comes from CSEF's public project showcase as archived by the Internet Archive before judging (https://web.archive.org/web/20230401224130/https://ca-csef.zfairs.com/showcase/ShowcaseInfo?f=838e60b7-ea75-46e8-865c-fde4864244b3); the version presented may differ.

Awards (1)

Competition history

  • CSEF 2023 Chemistry · Entry S0610

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