Issue 14, 2021

Noble metal-free Cu(i)-anchored NHC-based MOF for highly recyclable fixation of CO2 under RT and atmospheric pressure conditions

Abstract

The utilization of CO2 as a C1 feedstock for the synthesis of high-value chemicals and fuels is an important step towards mitigating the increasing concentration of atmospheric carbon dioxide as well as the production of value-added chemicals. Herein, we demonstrate the development of an efficient recyclable catalyst for the conversion of CO2 into oxazolidinones, which are important commodity chemicals for antibiotics, by utilizing an N-heterocyclic carbene (NHC)-based metal–organic framework (MOF). The NHC-centers lined in the pore walls of the MOF were utilized to anchor catalytically active Cu(I) ions by post-synthetic modification (PSM). The Cu(I)-embedded MOF showed highly recyclable and selective CO2 uptake properties with a high heat of interaction energy of 43 kJ mol−1. The presence of a high density of CO2-philic NHC and catalytic Cu(I) sites in the 1D channels of the MOF render highly efficient catalytic activity for fixation of CO2 into α-alkylidene cyclic carbonates and oxazolidinones at RT and atmospheric pressure conditions. Notably, Cu(I)@NHC–MOF showed excellent recyclability for up to 10 cycles of regeneration with retention of catalytic activity as well as chemical stability. To the best of our knowledge, Cu(I)@NHC–MOF is the first example of a noble metal-free MOF-based heterogeneous catalyst for the utilization of CO2 to synthesize important value-added chemicals under mild conditions.

Graphical abstract: Noble metal-free Cu(i)-anchored NHC-based MOF for highly recyclable fixation of CO2 under RT and atmospheric pressure conditions

Supplementary files

Article information

Article type
Paper
Submitted
15 Apr 2021
Accepted
15 Jun 2021
First published
15 Jun 2021

Green Chem., 2021,23, 5195-5204

Noble metal-free Cu(I)-anchored NHC-based MOF for highly recyclable fixation of CO2 under RT and atmospheric pressure conditions

R. Das and C. M. Nagaraja, Green Chem., 2021, 23, 5195 DOI: 10.1039/D1GC01312B

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