Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.175
Publication date: 18th July 2023
The Single-site MNC catalysts offer a ground-breaking non-precious-metal platform for CO2 electrolysis, demonstrating exceptional faradaic efficiency towards CO (> 90% FECO) at industrial-relevant current densities (> 250 mA cm-2) in regular membrane electrode assembly electrolyzer.[1] However, achieving such performance requires a cell potential (ECell) above 3 V, resulting in energy efficiency (EE) below 40% (EE = ECO2-to-CO * FECO / ECell) [2, 3]. To address this challenge, a crucial technical solution involves further enhancing the catalyst material to minimize catalytic potential loss (for reduced ECell).
The metal center highly influences the intrinsic activity-potential relationship of the MNC catalysts. FeNx exhibits superior binding energy to the crucial intermediate, *COOH, for CO formation, compared to other metal centers. However, the FeNC ones suffer poisoning during the reaction, restricting their practical application in large-scale electrolyzers at high current densities.[4] Hence, to address this limitation, we designed a novel experimental approach to deactivate and reactivate the FeNC catalyst under CO2 electrolysis conditions using pulsed potentials. Interestingly, coupled with a millisecond-resolution differential electrochemical mass spectrometer, we defined an uncommon but potential-dependent recoverable CO2 poisoning phenomenon on the FeNC catalyst. This comprehensive investigation unravels the mechanisms of CO2 poisoning and recovery of the FeNC catalyst at the molecular level. Also, it offers practical guidance for mitigating the poisoning issue in large-scale applications.
European Union's Horizon 2020 research and innovation program under grant agreement no. 851441, SELECTCO2
European Union's Horizon 2020 research and innovation program under grant agreement no. 101006701, ECOFUEL
Carlsberg Foundation (CF21-0144)
Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) Grant No. STR 596/18-1
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