(590n) Development, Evaluation, and Modeling of Electrochemical CO2 Conversion to C2+ Chemicals at Catalyst and Electrolyzer Level

C₂₊ molecules, including ethylene and ethanol, are essential feedstocks in the plastics, chemical, and fuel industries. The electrochemical reduction of CO₂ (eCO₂RR) to C₂₊ chemicals has gained significant interest as an alternative method to production these chemicals directly from CO₂. However, despite advancements in technology, challenges persist in catalyst performance and system integration, limiting the transition from laboratory-scale processes to industrial applications. Key limitations include improving selectivity and activity, maintaining long-term operational stability, and addressing mass transport constraints in practical systems. A deeper understanding of catalyst behavior and system design is crucial to bridging the gap between fundamental research and large-scale implementation. This work presents a comprehensive study that includes the design and optimization of Cu-based catalysts and electrolyzer systems for improved C₂₊ production, supported by numerical modeling for analyzing electrolyzer behavior.

For experiment, Cu remains the most important and widely studied catalyst to achieve CO₂ to C₂₊ conversion, recognized for its unique ability to facilitate multi-carbon product formation. Our study integrates the modifications of sputtered Cu-based catalyst with the optimization of CO₂ electrolyzer system, achieving over 80% C₂₊ Faradic efficiency (FE) for C₂₊ products at industrially relevant current densities (> 100 mA/cm²) and low cell voltage (< 3.0 V).

To explore electrolyzer design and optimal operating conditions, we develop a computational fluid dynamics (CFD) model of the electrolyzer and validate it against our in-house eCO₂RR experiments. This model is then used to explore and optimize system-level parameters, including temperature, pressure, and geometric properties, providing new insights into factors driving eCO₂RR performance. By combining experimental and computational approaches, this study offers critical insights into the current development stage, key challenges, and future opportunities for advancing eCO₂RR toward practical applications in chemical manufacturing.