Exploring the influence of interfacial solvation on electrochemical CO2 reduction using plasmon‐enhanced vibrational sum frequency generation spectroscopy

Rebstock, Jaclyn A.; Zhu, Quansong; Baker, L. Robert

doi:10.1002/cctc.202301301

Exploring the influence of interfacial solvation on electrochemical CO₂ reduction using plasmon‐enhanced vibrational sum frequency generation spectroscopy

Journal Article · Wed Jan 10 00:00:00 EST 2024 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.202301301· OSTI ID:2575859

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The Ohio State Univ., Columbus, OH (United States)

Although interfacial solvation plays an important role in determining carbon dioxide reduction (CO₂R) kinetics, present understanding of the potential dependent properties of the electrochemical double layer under conditions relevant for CO₂R remains limited. This article summarizes the development and recent applications of plasmon-enhanced vibrational sum frequency generation (VSFG) spectroscopy to study the effects of cation hydration and interfacial solvation on CO₂R using CO as a vibrational Stark reporter. Results show that electrolyte cations retain their entire solvation shell upon adsorption to inactive sites, while active sites retain only a single water layer between the gold surface and the cation. Measurements also show that the total interfacial electric field can be separated into two contributions: one from the electrochemical double layer (Stern field) and another from the polar solvation environment (Onsager field). Surprisingly, correlating VSFG spectra with reaction kinetics reveals that it is the solvation-mediated Onsager field that governs the chemical reactivity at the electrode/electrolyte interface. Measuring the interfacial water spectra during electrocatalysis also provides evidence for the proton source during H2 evolution, which competes with CO₂R in aqueous electrolyte. These findings highlight the importance of directly probing cation hydration and interfacial solvation, which mediates reaction kinetics at electrochemical interfaces.

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Research Organization:: The Ohio State Univ., Columbus, OH (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0020977

Other Award/Contract Number:: 1665280

OSTI ID:: 2575859

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Journal Issue: 14 Vol. 16; ISSN 1867-3880; ISSN 1867-3899

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Exploring the influence of interfacial solvation on electrochemical CO2 reduction using plasmon‐enhanced vibrational sum frequency generation spectroscopy

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Exploring the influence of interfacial solvation on electrochemical CO₂ reduction using plasmon‐enhanced vibrational sum frequency generation spectroscopy