Nonconductive Metal Oxide Gas Diffusion Layer for Mitigating Electrowetting during CO2 Electrolysis.

Abstract

Gas diffusion electrodes (GDEs) are extensively used for high current density electrochemical CO2 electrolysis (ECO2R), enabled by significantly reducing mass transfer resistance of CO2 to the catalyst layer. Conventionally, these GDEs are based upon hydrophobic carbon-based gas-diffusion layers (GDLs) that facilitate the gas transport; however, these supports are prone to flood with electrolyte during electrolysis. This potential-induced flooding, known as electrowetting, is related to the inherent conductivity of carbon and limits the activity of ECO2R. To investigate the effect of electrical conductivity more carefully, a GDE is constructed based on a Cu mesh with a nonconductive microporous GDL applied to this substrate, the latter composed of a mixture of metal oxide and polytetrafluoroethylene. With alumina as the metal oxide, a stable operation is obtained at -200 mA cm-2 with 70% selectivity for ECO2R (with over half toward C2+ products) without flooding as observed by in situ microscopy. On the contrary, with a Vulcan carbon-based GDL, the initial activity is rapidly lost as severe flooding ensues. It is reasoned that electrowetting is averted by virtue of the nonconductive nature of alumina, providing a new perspective on alternative GDL compositions and their influence on ECO2R performance.