Publication date: 21st July 2025
The electrochemical reduction of carbon dioxide (CO2) has emerged as a promising approach for cutting CO2 emissions, tackling climate change, and enabling the transition toward a renewable energy-driven chemical industry. To mitigate the inefficiencies of current separation and purification processes and facilitate industrial application, direct utilization of CO2 from point sources, such as industrial facilities or power plants, is gaining much interest.[1,2] However, such untreated exhaust gases do not possess optimal compositions[3] and are characterized by a low concentration of CO2 (with N2 dilutant) and several impurities (e.g., O2, NOx, and SOx). Both dilution and impurities can affect performance; thus, understanding their impact is becoming critical and attracting extensive research efforts. Here, we explored the influence of CO2 availability on a Cu2O/SnO2-based catalyst, tested in the presence of a potassium bicarbonate electrolyte within a 10 cm2 continuous flow cell. A concentration-dependent restructuring of the pristine core-shell nano-cubes was revealed, likely responsible for the shift in selectivity from formate to CO at mild current density values, moving from 25% to 100% CO2 in the feed. However, as the current density was increased to a value of 100 mA cm-2, local pH effects began to dominate the CO2 reduction reaction, specifically controlling the selective production of formate or CO. We demonstrated a stable syngas production at 100 mA cm-2 over 8 hours of operations, with a CO to H2 ratio higher than 1.5 at a measured cathodic potential of approximately -2 V vs Ag/AgCl. Significant effects began to manifest in the presence of 1% O2 in the feed at low current densities. Building upon recent studies,[4] we aimed to address oxygen reduction at the cathode by playing on mass transport. The knowledge about the long-term effect of oxygen impurity on Cu2O/SnO2-based catalysts will guide the future design of impurity-tolerant GDEs and facilitate its practical application for electrochemical CO2 conversion technology.
The financial support of the SunCoChem project (Grant Agreement No 862192) and the PNRR – Partneriati estesi – “NEST – Network 4 Energy Sustainable Transition” is acknowledged.
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