A Precious-metal-free Hybrid Electrolyzer for Alcohol Oxidation Coupled to CO2-to-syngas Conversion

Bajada, Mark, Roy, Souvik, Warnan, Julien , Aziz, Kaltum, Wagner, Andreas, Roessler, Maxie M. and Reisner, Erwin (2020) A Precious-metal-free Hybrid Electrolyzer for Alcohol Oxidation Coupled to CO2-to-syngas Conversion. Angewandte Chemie International Edition, 59 (36). pp. 15633-15641. ISSN 1433-7851

Full content URL: https://doi.org/10.1002/anie.202002680

Hybrid Electrolyzer for Alcohol Oxidation Coupled to CO2‐to‐syngas Conversion
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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 (meso ITO) 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.

Keywords:catalysis, carbon dioxide, alcohols, electrochemistry, energy conversion
Subjects:J Technologies > J910 Energy Technologies
F Physical Sciences > F100 Chemistry
Divisions:College of Science > School of Chemistry
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ID Code:40556
Deposited On:09 Apr 2020 10:27

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