Investigating the interplay between charge transfer and CO 2 insertion in the adsorption of a NiFe catalyst for CO 2 electroreduction on a graphite support through DFT computational approaches - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of Computational Chemistry Année : 2024

Investigating the interplay between charge transfer and CO 2 insertion in the adsorption of a NiFe catalyst for CO 2 electroreduction on a graphite support through DFT computational approaches

Subash Arjunan
  • Fonction : Auteur
Joshua Sims
Carole Duboc
Pascale Maldivi

Résumé

Abstract This article describes a density functional theory (DFT) study to explore a bio‐inspired NiFe complex known for its experimental activity in electro‐reducing CO 2 to CH 4 when adsorbed on graphite. The coordination properties of the complex are investigated in isolated form and when physisorbed on a graphene surface. A comparative analysis of DFT approaches for surface modeling is conducted, utilizing either a finite graphene flake or a periodic carbon surface. Results reveal that the finite model effectively preserves all crucial properties. By examining predicted structures arising from CO 2 insertion within the mono‐reduced NiFe species, whether isolated or adsorbed on the graphene flake, a potential species for subsequent electro‐reduction steps is proposed. Notably, the DFT study highlights two positive effects of complex adsorption: facile electron transfers between graphene and the complex, finely regulated by the complex state, and a lowering of the thermodynamic demand for CO 2 insertion.

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Chimie
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Dates et versions

hal-04530347 , version 1 (03-04-2024)

Identifiants

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Subash Arjunan, Joshua Sims, Carole Duboc, Pascale Maldivi, Anne Milet. Investigating the interplay between charge transfer and CO 2 insertion in the adsorption of a NiFe catalyst for CO 2 electroreduction on a graphite support through DFT computational approaches. Journal of Computational Chemistry, 2024, ⟨10.1002/jcc.27355⟩. ⟨hal-04530347⟩
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