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Degradation study on tin- and bismuth-based gas-diffusion electrodes during electrochemical CO_(2) reduction in highly alkaline media

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Journal of Energy Chemistry 2021年第11期30卷 367-376,I0008页

作者： Fabian Bienen Armin Lowe Joachim Hildebrand Sebastian Hertle dana schonvogel Dennis Kopljar Norbert Wagner Elias Klemm Kaspar Andreas Friedrich Institute of Engineering Thermodynamics German Aerospace CenterPfaffenwaldring 38-4070569 StuttgartGermany Institute of Building Energetics Thermal Engineering and Energy StorageUniversity of StuttgartPfaffenwaldring 3170569 StuttgartGermany Institute of Technical Chemistry University of StuttgartPfaffenwaldring 5570569 StuttgartGermany Institute of Engineering Thermodynamics German Aerospace CenterCarl-von-Ossietzky-Straße 1526129 OldenburgGermany

This work investigated the degradation of tin – based gas-diffusion electrodes (GDE) and also a promising Bi2O3 GDE in electrochemical CO_(2) reduction in highly alkaline media which has not been studied before. The contributions of the electrode wetting (or flooding, if excessively) and catalyst leaching on the degradation were analyzed. Therefore, electrochemical impedance spectroscopy was used to monitor the wetted surface area of the GDE in combination with post-mortem analysis of the penetration depth by visualizing the electrolyte’s cation in the GDE cross-section. Furthermore, to reveal a possible degradation of the electrocatalyst, its distribution was mapped in the GDEs cross-section after operation while the catholyte was additionally analyzed via ICP-MS. The results clearly demonstrate that the SnO_(2) catalyst dissolves in the reaction zone inside the GDE and might be partially redeposited near the GDEs surface. Since the redeposition process occurs only partially a steady loss of catalyst was observed impeding a clear distinction of the two degradation phenomena. Nevertheless, the deterioration of the electrode performance measured as faraday efficiency (FE) of the parasitic hydrogen evolution reaction (HER) qualitatively correlates with the differential double layer capacitance (Cdl). A significant difference of the rate of increase for the hydrogen FE and Cdl can be ascribed to the superposition of both above-mentioned degradation mechanisms. The demonstrated instability of SnO_(2) contrasts with the behavior of Bi2O3 GDE which is stabilized during CO_(2) conversion by redeposition of the diluted dissolved species as metallic Bi which is active for the CO_(2) reduction reaction.

关键词： Electrochemical CO_(2)reduction Heterogeneous catalysis Gas-diffusion electrode Electrochemical impedance spectroscopy Catalyst leaching

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