期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 10, 期 34, 页码 17801-17807出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2ta04485d
关键词
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资金
- EPSRC [NS/A000055/1, EP/P001386, EP/I011870]
- Royal Society
- China Scholarship Council (CSC)
- European Research Council (ERC) under the European Union [742401]
- Royal Society Newton International Fellowships
- University of Manchester
This study investigates the impact of porosity of MOFs on their evolution as electrocatalysts for CO2 reduction and demonstrates the significance of porosity in the generation of value-added chemicals.
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 center dot 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.
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