Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.026
Publication date: 23rd September 2021
The production of value added compounds within CO2 electrolyzers has reached sufficient catalytic performance that system and process performance such as CO2 utilization have come more into consideration. Efforts to assess the limitations of CO2 conversion and crossover within electrochemical systems have been performed, providing valuable information to position CO2 electrolyzers within a larger process. Currently missing, however, is a clear elucidation of the inevitable trade-offs that exist between CO2 utilization and electrolyzer performance, specifically how the Faradaic Efficiency of a system varies with CO2 availability. Such information is needed to properly assess the viability of the technology. In this work, we provide a combined experimental and 3D modelling assessment of the trade-offs between CO2 utilization and selectivity at 200 mA/cm2 within a membrane-electrode assembly CO2 electrolyzer. Using silver gas diffusion electrode and varying inlet flow rates, we demonstrate that the variation in spatial concentration of CO2 leads to spatial variations in Faradaic Efficiency that cannot be captured using common ‘black box’ measurement procedures. Specifically, losses of Faradaic efficiency are observed to occur even at incomplete CO2 consumption (80%). Modelling of the gas channel and diffusion layers indicated at least a portion of the H2 generated is considered as avoidable by proper flow field design and modification. The combined work allows for a spatially resolved interpretation of product selectivity occurring inside the reactor, providing the foundation for design rules in balancing CO2 utilization and device performance in both lab and scaled applications.
The authors would like to acknowledge the co-financing provided by Shell and a PPP-allowance from Top Consortia for Knowledge and Innovation (TKI’s) of the Ministry of Economic Affairs and Climate in the context of the TU Delft e-Refinery Institute. TB would also like to acknowledge the NWO for an individual Veni grant.