Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 36, Pages 15633-15641Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202002680
Keywords
alcohols; carbon dioxide; catalyst immobilization; electrocatalysis; energy conversion
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Funding
- Endeavour Scholarship Scheme
- Christian Doppler Research Association (Austrian Federal Ministry for Digital and Economic Affairs)
- National Foundation for Research, Technology and Development
- OMV
- Marie Skodowska-Curie Fellowship from the European Commission H2020 [GAN745604]
- Leverhulme Trust [RPG-2018-183]
- EPRSC [EP/L011972/1]
- EPSRC [EP/L011972/1] Funding Source: UKRI
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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 (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 approximate to 1000 and Faradaic efficiency (FE) of 83 %. The cathode generated a stoichiometric amount of syngas with a CO:H-2 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.
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