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Evolution of bismuth-based metal?organic frameworks for efficient electroreduction of CO2

Li, Lili, Kang, Xinchen, He, Meng, Sheveleva, Alena, Hu, Kui, Xu, Shaojun, Zhou, Yiqi, Chen, Jin, Sapchenko, Sergei, Whitehead, George, Vitorica-Yrezabal, Iñigo J., Lopez-Odriozola, Laura, Natrajan, Louise S., McInnes, Eric J. L., Schröder, Martin, Yang, Sihai and Tuna, Floriana 2022. Evolution of bismuth-based metal?organic frameworks for efficient electroreduction of CO2. Journal of Materials Chemistry A: materials for energy and sustainability 10 (34) , pp. 17801-17807. 10.1039/D2TA04485D

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Understanding the structural and chemical changes that reactive metal–organic frameworks (MOFs) undergo is crucial for the development of new efficient catalysts for electrochemical reduction of CO2. Here, we describe three Bi(III) materials, MFM-220, MFM-221 and MFM-222, which are constructed from the same ligand (biphenyl-3,3′,5,5′-tetracarboxylic acid) but which show distinct porosity with solvent-accessible voids of 49.6%, 33.6% and 0%, respectively. We report the first study of the impact of porosity of MOFs on their evolution as electrocatalysts. A Faradaic efficiency of 90.4% at −1.1 V vs. RHE (reversible hydrogen electrode) is observed for formate production over an electrode decorated with MFM-220-p, formed from MFM-220 on application of an external potential in the presence of 0.1 M KHCO3 electrolyte. In situ electron paramagnetic resonance spectroscopy confirms the presence of ·COOH radicals as a reaction intermediate, with an observed stable and consistent Faradaic efficiency and current density for production of formate by electrolysis over 5 h. This study emphasises the significant role of porosity of MOFs as they react and evolve during electroreduction of CO2 to generate value-added chemicals.

Item Type: Article
Date Type: Published Online
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: Royal Society of Chemistry
ISSN: 2050-7488
Funders: EPSRC
Date of First Compliant Deposit: 28 September 2022
Date of Acceptance: 3 August 2022
Last Modified: 20 May 2023 18:27

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