Issue 18, 2022

Defect-engineered MOF-801 for cycloaddition of CO2 with epoxides

Abstract

Heterogeneous catalysts based on defective metal–organic frameworks (MOFs) have attracted wide attention due to their facile formation of defects during synthesis. Herein, two MOFs, MOF-801(D) and MOF-801(P), were synthesized by a solvothermal method using a modulation approach. The synthesized MOFs were characterized by using PXRD, N2 BET, TGA, NH3 and CO2-TPD, CO2 adsorption isotherms, XPS, FT-IR, FE-SEM, and HR-TEM. A computational characterization method was developed to approximate the degree of defects using a combination of molecular simulation and a linear programming approach. Master isotherm models for N2 isotherms at 77 K were constructed to match the experimental isotherm data of MOF-801(D) and MOF-801(P), and the pore size distribution and the degree of defects were quantified based on the predicted N2 isotherms at 77 K. MOF-801(D) showed a high conversion of epoxide with >99% selectivity toward cyclic carbonate and 92% conversion under mild and solvent-less reaction conditions. MOF-801(D) was easily separated using a centrifuge and can be recycled up to 5 times without any significant decrease in its initial performance. Density functional theory (DFT) calculations were carried out to corroborate that the increased acid sites, from the cluster defects, are responsible for the increased catalytic conversion of the catalyst.

Graphical abstract: Defect-engineered MOF-801 for cycloaddition of CO2 with epoxides

Supplementary files

Article information

Article type
Paper
Submitted
19 1月 2022
Accepted
30 3月 2022
First published
31 3月 2022

J. Mater. Chem. A, 2022,10, 10051-10061

Defect-engineered MOF-801 for cycloaddition of CO2 with epoxides

Y. Gu, B. A. Anjali, S. Yoon, Y. Choe, Y. G. Chung and D. Park, J. Mater. Chem. A, 2022, 10, 10051 DOI: 10.1039/D2TA00503D

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements