A critical appraisal of advances in integrated CO2 capture and electrochemical conversion.

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This perspective work examines the current advancements in integrated CO2 capture and electrochemical conversion technologies, comparing the emerging methods of (1) electrochemical reactive capture (eRCC) though amine- and (bi)carbonate-mediated processes and (2) direct (flue gas) adsorptive capture and conversion (ACC) with the conventional approach of sequential carbon capture and conversion (SCCC). We initially identified and discussed a range of cell-level technological bottlenecks inherent to eRCC and ACC including, but not limited to, mass transport limitations of reactive species, limitation of dimerization, impurity effects, inadequate in situ generation of CO2 to sustain industrially relevant current densities, and catalyst instabilities with respect to some eRCC electrolytes, amongst others. We followed this with stepwise perspectives on whether these are considered intrinsic challenges of the technologies - otherwise recommendations were disclosed where appropriate. Furthermore, technoeconomic analysis (TEA) was conducted using a net present value (NPV) model to determine the minimum selling prices (MSPs) for CO, HCOOH, CH3OH, C2H5OH, and C2H4 as target products based on cell-performance metrics from contemporary literature for SCCC, eRCC, and ACC. Additionally, sensitivity analyses were performed, focusing on cell-level parameters (voltage requirements, Faradaic efficiencies, current density), production scale factors, and other relevant variables (levelized costs of electricity and stack). This analysis sheds light on the cost-driving factors influencing commercial viability, revealing key techno-economic challenges for eRCC, particularly with liquid products. However, it also identifies optimization opportunities in current designs. By pinpointing critical areas for improvement, this work helps advance electrochemical CO2 reduction technologies towards more sustainable and economically competitive applications at different scales.