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Carboxysome-Inspired Electrocatalysis using Enzymes for the Reduction of CO2 at Low Concentrations**
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Orientador(es)
Resumo(s)
The electrolysis of dilute CO2 streams suffers from low concentrations of dissolved substrate and its rapid depletion at the electrolyte-electrocatalyst interface. These limitations require first energy-intensive CO2 capture and concentration, before electrolyzers can achieve acceptable performances. For direct electrocatalytic CO2 reduction from low-concentration sources, we introduce a strategy that mimics the carboxysome in cyanobacteria by utilizing microcompartments with nanoconfined enzymes in a porous electrode. A carbonic anhydrase accelerates CO2 hydration kinetics and minimizes substrate depletion by making all dissolved carbon available for utilization, while a highly efficient formate dehydrogenase reduces CO2 cleanly to formate; down to even atmospheric concentrations of CO2. This bio-inspired concept demonstrates that the carboxysome provides a viable blueprint for the reduction of low-concentration CO2 streams to chemicals by using all forms of dissolved carbon.
Descrição
Funding Information: This work was supported by a European Research Council (ERC) Consolidator Grant (MatEnSAP, no. 682833; S.J.C, E.R.), the Leverhulme Trust for a research project grant (P80336; to S.J.C., E.R.) and Early Career Fellowship (ECF-2021-072, S.J.C.), the Isaac Newton Trust(20.08(r), S.J.C.) the Winston Churchill Foundation of the United States (A.D.), the Fundação para a Ciência e Tecnologia (FCT, Portugal) for fellowship SFRH/BD/116515/2016 (A.R.O.), grant PTDC/BII-BBF/2050/2020 (I.A.C.P.) and MOSTMICRO-ITQB unit (UIDB/04612/2020 and UIDP/04612/2020), and Associate Laboratory LS4FUTURE (LA/P/0087/2020). We thank Dr. Vivek Badiani for useful discussions. Funding Information: This work was supported by a European Research Council (ERC) Consolidator Grant (MatEnSAP, no. 682833; S.J.C, E.R.), the Leverhulme Trust for a research project grant (P80336; to S.J.C., E.R.) and Early Career Fellowship (ECF‐2021‐072, S.J.C.), the Isaac Newton Trust(20.08(r), S.J.C.) the Winston Churchill Foundation of the United States (A.D.), the Fundação para a Ciência e Tecnologia (FCT, Portugal) for fellowship SFRH/BD/116515/2016 (A.R.O.), grant PTDC/BII‐BBF/2050/2020 (I.A.C.P.) and MOSTMICRO‐ITQB unit (UIDB/04612/2020 and UIDP/04612/2020), and Associate Laboratory LS4FUTURE (LA/P/0087/2020). We thank Dr. Vivek Badiani for useful discussions. Publisher Copyright: © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
Palavras-chave
Carbon Dioxide Reduction Electrochemistry Enzyme Catalysis Metalloenzymes Protein Film Electrochemistry Catalysis General Chemistry