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Electrocatalytic Scission of Unactivated C(sp3)-C(sp3) Bonds through Real-Time Manipulation of Surface-Bound Intermediates.
Bakshi, Harshal B; Lucky, Christine; Chen, Hsiang-Sheng; Schreier, Marcel.
Afiliación
  • Bakshi HB; Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Lucky C; Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Chen HS; Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Schreier M; Department of Chemical and Biological Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
J Am Chem Soc ; 145(25): 13742-13749, 2023 Jun 28.
Article en En | MEDLINE | ID: mdl-37279178
Electrocatalysis plays a critical role in future technologies for energy storage and sustainable synthesis, but the scope of reactions achievable using electricity remains limited. Here, we demonstrate an electrocatalytic approach to cleave the C(sp3)-C(sp3) bond in ethane at room temperature over a nanoporous Pt catalyst. This reaction is enabled by time-dependent electrode potential sequences, combined with monolayer-sensitive in situ analysis, which allows us to gain independent control over ethane adsorption, oxidative C-C bond fragmentation, and reductive methane desorption. Importantly, our approach allows us to vary the electrode potential to promote the fragmentation of ethane after it is bound to the catalyst surface, resulting in unprecedented control over the selectivity of this alkane transformation reaction. Steering the transformation of intermediates after adsorption constitutes an underexplored lever of control in catalysis. As such, our findings widen the parameter space for catalytic reaction engineering and open the door to future sustainable synthesis and electrocatalytic energy storage technologies.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos