Fundamentals of Gas Diffusion Electrodes and Electrolysers for Carbon Dioxide Utilisation: Challenges and Opportunities

Electrocatalysis plays a prominent role in the development of carbon dioxide utilisation technologies. Many new and improved CO(2)conversion catalysts have been developed in recent years, progressively achieving better performance. However, within this flourishing field, a disconnect in catalyst performance evaluation has emerged as the Achilles heel of CO(2)electrolysis. Too often, catalysts are assessed in electrochemical settings that are far removed from industrially relevant operational conditions, where CO(2)mass transport limitations should be minimised. To overcome this issue, gas diffusion electrodes and gas-fed electrolysers need to be developed and applied, presenting new challenges and opportunities to the CO(2)electrolysis community. In this review, we introduce the reader to the fundamentals of gas diffusion electrodes and gas-fed electrolysers, highlighting their advantages and disadvantages. We discuss in detail the design of gas diffusion electrodes and their operation within gas-fed electrolysers in both flow-through and flow-by configurations. Then, we correlate the structure and composition of gas diffusion electrodes to the operational performance of electrolysers, indicating options and prospects for improvement. Overall, this study will equip the reader with the fundamental understanding required to enhance and optimise CO(2)catalysis beyond the laboratory scale.