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Electrochemically Determined O-H Bond Dissociation Free Energies of NiO Electrodes Predict Proton-Coupled Electron Transfer Reactivity.

Electrochemically Determined O-H Bond Dissociation Free Energies of NiO Electrodes Predict... Redox reactions at metal oxide (MOx) surfaces are implicated in many catalytic and energy conversion processes involving proton-coupled electron transfer (PCET). Nonetheless, the fundamental thermodynamics dictating PCET reactivity at the MOx/solution interface are not well understood. Herein, we connect the pH-dependent electrochemical response of MOx thin films with the bond dissociation free energies (BDFEs) of their electroactive surface O-H bonds, using NiO as a case study. Complementary voltammetric and spectroscopic experiments show that the electrochemically determined BDFEs predict much of the observed PCET reactivity at the NiO surface. Analyzing the reactivity of MOx materials in terms of BDFEs could enable new approaches for designing more active and efficient (electro)catalysts for important PCET reactions. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Journal of the American Chemical Society Pubmed

Electrochemically Determined O-H Bond Dissociation Free Energies of NiO Electrodes Predict Proton-Coupled Electron Transfer Reactivity.

Journal of the American Chemical Society , Volume 141 (38): 5 – Jun 11, 2020

Electrochemically Determined O-H Bond Dissociation Free Energies of NiO Electrodes Predict Proton-Coupled Electron Transfer Reactivity.


Abstract

Redox reactions at metal oxide (MOx) surfaces are implicated in many catalytic and energy conversion processes involving proton-coupled electron transfer (PCET). Nonetheless, the fundamental thermodynamics dictating PCET reactivity at the MOx/solution interface are not well understood. Herein, we connect the pH-dependent electrochemical response of MOx thin films with the bond dissociation free energies (BDFEs) of their electroactive surface O-H bonds, using NiO as a case study. Complementary voltammetric and spectroscopic experiments show that the electrochemically determined BDFEs predict much of the observed PCET reactivity at the NiO surface. Analyzing the reactivity of MOx materials in terms of BDFEs could enable new approaches for designing more active and efficient (electro)catalysts for important PCET reactions.

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References (23)

ISSN
0002-7863
eISSN
1520-5126
DOI
10.1021/jacs.9b07923
pmid
31513390

Abstract

Redox reactions at metal oxide (MOx) surfaces are implicated in many catalytic and energy conversion processes involving proton-coupled electron transfer (PCET). Nonetheless, the fundamental thermodynamics dictating PCET reactivity at the MOx/solution interface are not well understood. Herein, we connect the pH-dependent electrochemical response of MOx thin films with the bond dissociation free energies (BDFEs) of their electroactive surface O-H bonds, using NiO as a case study. Complementary voltammetric and spectroscopic experiments show that the electrochemically determined BDFEs predict much of the observed PCET reactivity at the NiO surface. Analyzing the reactivity of MOx materials in terms of BDFEs could enable new approaches for designing more active and efficient (electro)catalysts for important PCET reactions.

Journal

Journal of the American Chemical SocietyPubmed

Published: Jun 11, 2020

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