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Highly Selective Electrochemical Reduction of CO₂ into Methane on Nanotwinned Cu.

ABSTRACT: The electrochemical carbon dioxide reduction reaction (CO₂RR) is a promising route to close the carbon cycle by reducing CO₂ into valuable fuels and chemicals. Electrocatalysts with high selectivity toward a single product are economically desirable yet challenging to achieve. Herein, we demonstrated a highly (111)-oriented Cu foil electrocatalyst with dense twin boundaries (TB) (tw-Cu) that showed a high Faradaic efficiency of 86.1 ± 5.3% toward CH₄ at -1.2 ± 0.02 V vs the reversible hydrogen electrode. Theoretical studies suggested that tw-Cu can significantly lower the reduction barrier for the rate-determining hydrogenation of CO compared to planar Cu(111) under working conditions, which suppressed the competing C-C coupling, leading to the experimentally observed high CH₄ selectivity.

SUBMITTER: Cai J

PROVIDER: S-EPMC10141442 | biostudies-literature | 2023 Apr

REPOSITORIES: biostudies-literature

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Highly Selective Electrochemical Reduction of CO2 into Methane on Nanotwinned Cu.

Cai Jin J Zhao Qing Q Hsu Wei-You WY Choi Chungseok C Liu Yang Y Martirez John Mark P JMP Chen Chih C Huang Jin J Carter Emily A EA Huang Yu Y

Journal of the American Chemical Society 20230418 16

The electrochemical carbon dioxide reduction reaction (CO2RR) is a promising route to close the carbon cycle by reducing CO2 into valuable fuels and chemicals. Electrocatalysts with high selectivity toward a single product are economically desirable yet challenging to achieve. Herein, we demonstrated a highly (111)-oriented Cu foil electrocatalyst with dense twin boundaries (TB) (tw-Cu) that showed a high Faradaic efficiency of 86.1 ± 5.3% toward CH4 at -1.2 ± 0. ...[more]

PMID: 37070601

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Project description:The electrochemical CO2 reduction reaction (CO2RR) holds enormous potential as a carbon-neutral route to the sustainable production of fuels and platform chemicals. The durability for long-term operation is currently inadequate for commercialization, however, and the underlying deactivation process remains elusive. A fundamental understanding of the degradation mechanism of electrocatalysts, which can dictate the overall device performance, is needed. In this work, we report the structural dynamics and degradation pathway of Cu oxide nanoparticles (CuOx NPs) during the CO2RR by using in situ small-angle X-ray scattering (SAXS) and X-ray absorption spectroscopy (XAS). The in situ SAXS reveals a reduction in the size of NPs when subjected to a potential at which no reaction products are detected. At potentials where the CO2RR starts to occur, CuOx NPs are agglomerated through a particle migration and coalescence process in the early stage of the reaction, followed by Ostwald ripening (OR) as the dominant degradation mechanism for the remainder of the reaction. As the applied potential becomes more negative, the OR process becomes more dominant, and for the most negative applied potential, OR dominates for the entire reaction time. The morphological changes are linked to a gradual decrease in the formation rate for multicarbon products (C2H4 and ethanol). Other reaction parameters, including reaction intermediates and local high pH, induce changes in the agglomeration process and final morphology of the CuOx NPs electrode, supported by post-mortem ex situ microscopic analysis. The in situ XAS analysis suggests that the CuOx NPs reduced into the metallic state before the structural transformation was observed. The introduction of high surface area carbon supports with ionomer coating mitigates the degree of structural transformation and detachment of the CuOx NPs electrode. These findings show the dynamic nature of Cu nanocatalysts during the CO2RR and can serve as a rational guideline toward a stable catalyst system under electrochemical conditions.

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Highly Selective Electrochemical Reduction of CO₂ into Methane on Nanotwinned Cu.

Publications

Highly Selective Electrochemical Reduction of CO<sub>2</sub> into Methane on Nanotwinned Cu.

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