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Fast CO2 hydration kinetics impair heterogeneous but improve enzymatic CO2 reduction catalysis.
Cobb, Samuel J; Badiani, Vivek M; Dharani, Azim M; Wagner, Andreas; Zacarias, Sónia; Oliveira, Ana Rita; Pereira, Inês A C; Reisner, Erwin.
Afiliación
  • Cobb SJ; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK.
  • Badiani VM; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK.
  • Dharani AM; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK.
  • Wagner A; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK.
  • Zacarias S; Instituto de Tecnologia Química e Biológica António Xavier, Universidade NOVA de Lisboa, Oeiras, Portugal.
  • Oliveira AR; Instituto de Tecnologia Química e Biológica António Xavier, Universidade NOVA de Lisboa, Oeiras, Portugal.
  • Pereira IAC; Instituto de Tecnologia Química e Biológica António Xavier, Universidade NOVA de Lisboa, Oeiras, Portugal.
  • Reisner E; Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK. reisner@ch.cam.ac.uk.
Nat Chem ; 14(4): 417-424, 2022 04.
Article en En | MEDLINE | ID: mdl-35228690
ABSTRACT
The performance of heterogeneous catalysts for electrocatalytic CO2 reduction suffers from unwanted side reactions and kinetic inefficiencies at the required large overpotential. However, immobilized CO2 reduction enzymes-such as formate dehydrogenase-can operate with high turnover and selectivity at a minimal overpotential and are therefore 'ideal' model catalysts. Here, through the co-immobilization of carbonic anhydrase, we study the effect of CO2 hydration on the local environment and performance of a range of disparate CO2 reduction systems from enzymatic (formate dehydrogenase) to heterogeneous systems. We show that the co-immobilization of carbonic anhydrase increases the kinetics of CO2 hydration at the electrode. This benefits enzymatic CO2 reduction-despite the decrease in CO2 concentration-due to a reduction in local pH change, whereas it is detrimental to heterogeneous catalysis (on Au) because the system is unable to suppress the H2 evolution side reaction. Understanding the role of CO2 hydration kinetics within the local environment on the performance of electrocatalyst systems provides important insights for the development of next-generation synthetic CO2 reduction catalysts.
Asunto(s)

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Dióxido de Carbono / Anhidrasas Carbónicas Idioma: En Revista: Nat Chem Asunto de la revista: QUIMICA Año: 2022 Tipo del documento: Article País de afiliación: Reino Unido Pais de publicación: ENGLAND / ESCOCIA / GB / GREAT BRITAIN / INGLATERRA / REINO UNIDO / SCOTLAND / UK / UNITED KINGDOM

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Dióxido de Carbono / Anhidrasas Carbónicas Idioma: En Revista: Nat Chem Asunto de la revista: QUIMICA Año: 2022 Tipo del documento: Article País de afiliación: Reino Unido Pais de publicación: ENGLAND / ESCOCIA / GB / GREAT BRITAIN / INGLATERRA / REINO UNIDO / SCOTLAND / UK / UNITED KINGDOM