Pseudocapacitance Facilitates the Electrocatalytic Reduction of Carbon Dioxide

Velasco‐Vélez, Juan‐Jesús; Knop‐Gericke, Axel; Roldan‐Cuenya, Beatriz; Schlögl, Robert; Jones, Travis E.

doi:10.1002/aenm.202400054

Title: Pseudocapacitance Facilitates the Electrocatalytic Reduction of Carbon Dioxide

Journal Article · 24 May 2024 · Advanced Energy Materials

DOI: https://doi.org/10.1002/aenm.202400054 · OSTI ID:2406660

^[1]; Knop‐Gericke, Axel ^[2];

^[3]; Schlögl, Robert ^[2];

^[4]

Max Planck Inst. for Chemical Energy Conversion, Mülheim an der Ruhr (Germany); Fritz Haber Institute of the Max Planck Society, Berlin (Germany); ALBA Synchrotron Light Source, Cerdanyola del Valles (Spain)
Max Planck Inst. for Chemical Energy Conversion, Mülheim an der Ruhr (Germany); Fritz Haber Institute of the Max Planck Society, Berlin (Germany)
Fritz Haber Institute of the Max Planck Society, Berlin (Germany)
Fritz Haber Institute of the Max Planck Society, Berlin (Germany); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Electroreduction of CO₂ to value-added products is a promising strategy for CO₂ reuse, where copper has a unique ability to produce oxygenates and C₂₊ products. Unfortunately, the electronic factors making copper so unique are unknown, which limits the ability to design improved catalysts. By combining in situ surface-sensitive X-ray resonant photoelectron spectroscopy with density functional theory calculations, the complex electronic structure of copper is uncovered during the electrocatalytic reduction of CO₂. It is found that the pseudocapacitive charging of copper, produced by the incorporation of protons and electrons into the subsurface, facilitates the activation of CO₂, while simultaneously increasing the barrier for H-H coupling. The net result is that cathodic pseudocapacitive charge suppresses the hydrogen evolution reaction and promotes the production of hydrocarbons and oxygenated products on copper. These results represent a new paradigm in the understanding of CO₂ reduction, highlighting the key role of pseudocapacitive charge in the reaction.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2406660

Report Number(s):: LA-UR--24-23134

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 31 Vol. 14; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Pseudocapacitance Facilitates the Electrocatalytic Reduction of Carbon Dioxide

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