Direct Observation of the Local Reaction Environment during the Electrochemical Reduction of CO2

Journal of the American Chemical Society
Ezra Lee Clark, Alexis T Bell

Abstract

The electrochemical reduction of carbon dioxide is sensitive to electrolyte polarization, which causes gradients in pH and the concentration of carbon dioxide to form near the cathode surface. It is desirable to measure the concentration of reaction-relevant species in the immediate vicinity of the cathode because the intrinsic kinetics of carbon dioxide reduction depend on the composition of the local reaction environment. Meeting this objective has proven difficult because conventional analytical methods only sample products from the bulk electrolyte. In this study, we describe the use of differential electrochemical mass spectrometry to measure the concentration of carbon dioxide and reaction products in the immediate vicinity of the cathode surface. This capability is achieved by coating the electrocatalyst directly onto the pervaporation membrane used to transfer volatile species into the mass spectrometer, thereby enabling species to be sampled directly from the electrode-electrolyte interface. This approach has been used to investigate hydrogen evolution and carbon dioxide reduction over Ag and Cu. We find that the measured CO2 reduction activity of Ag agrees well with what is measured by gas chromatography of the efflue...Continue Reading

References

Dec 14, 2004·Journal of the American Society for Mass Spectrometry·Helmut Baltruschat
Jun 11, 2014·Physical Chemistry Chemical Physics : PCCP·Toru HatsukadeThomas F Jaramillo

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Citations

Oct 23, 2020·Angewandte Chemie·Bjorn HasaFeng Jiao
Mar 13, 2021·Nature Communications·Chen PengGengfeng Zheng
Apr 28, 2021·Analytical Chemistry·Kevin KremplIb Chorkendorff
Jun 1, 2021·ACS Catalysis·Giulia MarcandalliMarc T M Koper
May 24, 2019·Chemical Reviews·Stephanie NitopiIb Chorkendorff
Sep 25, 2018·Langmuir : the ACS Journal of Surfaces and Colloids·Denis ÖhlWolfgang Schuhmann
Apr 15, 2020·Analytical Chemistry·Jie SunZongxiu Nie
Feb 26, 2019·Journal of the American Chemical Society·Ezra L ClarkAlexis T Bell
Feb 12, 2020·Journal of the American Chemical Society·Akansha GoyalMarc T M Koper
Jan 25, 2020·Journal of the American Chemical Society·Xiaoxia ChangBingjun Xu
Jan 1, 2021·Journal of the American Chemical Society·Soo Hong LeeWalter S Drisdell
Dec 11, 2019·The Journal of Physical Chemistry Letters·Haiping PanYan Shen
Sep 29, 2021·ACS Applied Materials & Interfaces·Shijia MuChunhua Cui
Dec 18, 2021·Chemical Reviews·Eric C R McKenzieR Daniel Little

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