A Precious-Metal-Free Hybrid Electrolyzer for Alcohol Oxidation Coupled to CO<sub>2</sub> -to-Syngas Conversion.
Angewandte Chemie (International ed. in English)
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Bajada, M., Roy, S., Warnan, J., Abdiaziz, K., Wagner, A., Roessler, M. M., & Reisner, E. (2020). A Precious-Metal-Free Hybrid Electrolyzer for Alcohol Oxidation Coupled to CO<sub>2</sub> -to-Syngas Conversion.. Angewandte Chemie (International ed. in English), 59 (36), 15633-15641. https://doi.org/10.1002/anie.202002680
Electrolyzers combining CO2 reduction (CO2R) with organic substrate oxidation can produce fuel and chemical feedstocks with a relatively low energy requirement when compared to systems that source electrons from water oxidation. Here, we report an anodic hybrid assembly based on a (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO) electrocatalyst modified with a silatrane-anchor (STEMPO), which is covalently immobilized on a mesoporous indium tin oxide (mesoITO) scaffold for efficient alcohol oxidation (AlcOx). This molecular anode was subsequently combined with a cathode consisting of a polymeric cobalt phthalocyanine on carbon-nanotubes to construct a hybrid, precious-metal-free coupled AlcOx–CO2R electrolyzer. After three hour electrolysis, glycerol is selectively oxidized to glyceraldehyde with a turnover number (TON) of 1000 and Faradaic efficiency (FE) of 83% and the cathode generated a stoichiometric amount of syngas with a CO:H2 ratio of 1.25±0.25 and an overall cobalt- based TON of 894 with a FE of 82%. This prototype device inspires the design and implementation of nonconventional strategies for coupling CO2R to less energy demanding, and value-added, oxidative chemistry.
Christian Doppler Forschungsgesellschaft (unknown)
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (701192)
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (744317)
European Commission Horizon 2020 (H2020) Marie Sk?odowska-Curie actions (745604)
External DOI: https://doi.org/10.1002/anie.202002680
This record's URL: https://www.repository.cam.ac.uk/handle/1810/304184
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