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Nonredox CO 2 fixation in solvent-free conditions using a Lewis acid metal–organic framework constructed from a sustainably sourced ligand
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Das, Satarupa, Zhang, Jinfang, Chamberlain, Thomas W., Clarkson, Guy J. and Walton, Richard I. (2022) Nonredox CO 2 fixation in solvent-free conditions using a Lewis acid metal–organic framework constructed from a sustainably sourced ligand. Inorganic Chemistry, 61 (46). pp. 18536-18544. doi:10.1021/acs.inorgchem.2c02749 ISSN 0020-1669.
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WRAP-nonredox-CO2-fixation-solvent-free-conditions-using-Lewis-acid-metal–organic-framework-constructed-sustainably-sourced-ligand-2022.pdf - Published Version - Requires a PDF viewer. Available under License Creative Commons Attribution 4.0. Download (3070Kb) | Preview |
Official URL: https://doi.org/10.1021/acs.inorgchem.2c02749
Abstract
CO2 epoxidation to cyclic carbonates under mild, solvent-free conditions is a promising pathway toward sustainable CO2 utilization. Metal–organic frameworks (MOFs) explored for such applications so far are commonly composed of nonrenewable ligands such as benzene dicarboxylate (BDC) or synthetically complex linkers and therefore are not suitable for commercial utilization. Here, we report new yttrium 2,5-furandicarboxylate (FDC)-based MOFs: “UOW-1” and “UOW-2” synthesized via solvothermal assembly, with the former having a unique structural topology. The FDC linker can be derived from biomass and is a green and sustainable alternative to conventionally used BDC ligands, which are sourced exclusively from fossil fuels. UOW-1, owing to unique coordination unsaturation and a high density of Lewis active sites, promotes a high catalytic activity (∼100% conversion; ∼99% selectivity), a high turnover frequency (70 h–1), and favorable first-order kinetics for CO2 epoxidation reactions using an epichlorohydrin model substrate under solvent-free conditions within 6 h and a minimal cocatalyst amount. A systematic catalytic study was carried out by broadening the epoxide substrate scope to determine the influence of electronic and steric factors on CO2 epoxidation. Accordingly, higher conversion efficiencies were observed for substrates with high electrophilicity on the carbon center and minimal steric bulk. The work presents the first demonstration of sustainable FDC-based MOFs used for efficient CO2 utilization.
Item Type: | Journal Article | ||||||||
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Subjects: | Q Science > QD Chemistry | ||||||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||
SWORD Depositor: | Library Publications Router | ||||||||
Library of Congress Subject Headings (LCSH): | Carbon sequestration, Metal-organic frameworks, Addition reactions, Carbon dioxide -- Absorption and adsorption, Carbon dioxide mitigation, Chemical reactions | ||||||||
Journal or Publication Title: | Inorganic Chemistry | ||||||||
Publisher: | American Chemical Society | ||||||||
ISSN: | 0020-1669 | ||||||||
Official Date: | 21 November 2022 | ||||||||
Dates: |
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Volume: | 61 | ||||||||
Number: | 46 | ||||||||
Page Range: | pp. 18536-18544 | ||||||||
DOI: | 10.1021/acs.inorgchem.2c02749 | ||||||||
Status: | Peer Reviewed | ||||||||
Publication Status: | Published | ||||||||
Access rights to Published version: | Open Access (Creative Commons) | ||||||||
Date of first compliant deposit: | 16 December 2022 | ||||||||
Date of first compliant Open Access: | 16 December 2022 | ||||||||
RIOXX Funder/Project Grant: |
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