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• W4313340037 abstract "Immobilization of porphyrin complexes into crystalline metal-organic frameworks (MOFs) enables high exposure of porphyrin active sites for CO2 electroreduction. Herein, well-dispersed iron-porphyrin-based MOF (PCN-222(Fe)) on carbon-based electrodes revealed optimal turnover frequencies for CO2 electroreduction to CO at 1 wt.% catalyst loading, beyond which the intrinsic catalyst activity declined due to CO2 mass transport limitations. In situ Raman suggested that PCN-222(Fe) maintained its structure under electrochemical bias, permitting mechanistic investigations. These revealed a stepwise electron transfer-proton transfer mechanism for CO2 electroreduction on PCN-222(Fe) electrodes, which followed a shift from a rate-limiting electron transfer to CO2 mass transfer as the potential increased from -0.6 V to -1.0 V vs. RHE. Our results demonstrate how intrinsic catalytic investigations and in situ spectroscopy are needed to elucidate CO2 electroreduction mechanisms on PCN-222(Fe) MOFs." @default.
• W4313340037 created "2023-01-06" @default.
• W4313340037 creator A5074568396 @default.
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• W4313340037 date "2023-01-18" @default.
• W4313340037 modified "2023-10-17" @default.
• W4313340037 title "Mechanistic Elucidations of Highly Dispersed Metalloporphyrin Metal‐Organic Framework Catalysts for CO₂ Electroreduction" @default.
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• W4313340037 doi "https://doi.org/10.1002/anie.202218208" @default.
• W4313340037 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/36584349" @default.
• W4313340037 hasPublicationYear "2023" @default.
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