In Situ Observation of the pH Gradient near the Gas Diffusion Electrode of CO2 Reduction in Alkaline Electrolyte

Journal of the American Chemical Society
Xu LuHailiang Wang

Abstract

The local pH variation near the surface of CO2 reduction electrodes is important but hard to study. We develop a continuous-flow Raman electrochemical cell that enables the first experimental study of the local pH near a CO2 reduction gas diffusion electrode under reaction conditions. At zero current, CO2 chemically reacts with the 1 M KOH electrolyte at the interface to form HCO3- and CO32-. The local pH on the cathode surface is 7.2, and the HCO3- concentration profile extends a distance of 120 μm into the electrolyte, which verifies that the nominal overpotential reduction from using alkaline electrolyte originates from the Nernst potential of the pH gradient layer at the cathode/electrolyte interface. The CO2-OH- neutralization reaction and the pH gradient layer still persist, albeit to a reduced extent, at CO2 reduction current densities up to 150 mA/cm2.

References

Aug 13, 2011·Physical Chemistry Chemical Physics : PCCP·Michael AuingerKarl J J Mayrhofer
Apr 10, 2016·Angewandte Chemie·Anna LoiudiceRaffaella Buonsanti
Oct 29, 2018·Advanced Materials·Jing-Jing LvFeng Jiao
Feb 3, 2019·The Journal of Chemical Physics·Shan JiangHolger Dau
Aug 11, 2019·Nature Communications·Min WangMarc Robert
Sep 17, 2019·Journal of the American Chemical Society·Kailun YangWilson A Smith
Nov 30, 2019·Nature·Yueshen WuHailiang Wang
Feb 8, 2020·Science·F Pelayo García de ArquerEdward H Sargent

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