Electrochemical CO 2 Reduction in the Presence of SO 2 Impurities on a Nitrogen-Doped Carbon Electrocatalyst

Electrochemical CO2 reduction to CO offers a sustainable route for converting CO2 into value-added chemicals and fuels. However, CO2 streams derived from industrial sources often contain SO2 impurities that severely poison conventional metal-based catalysts. Here, we report a nitrogen-doped carbon catalyst that exhibits pronounced tolerance and stability for CO2-to-CO conversion in the presence of SO2 (100-10,000 ppm). The catalyst maintains over 90% Faradaic efficiency toward CO during 8 h of electrolysis at -1.0 V vs RHE with 100 ppm of SO2, whereas Ag foil electrodes undergo rapid deactivation. Density functional theory calculations combined with surface analyses indicate that weak SO2 adsorption and the absence of stable sulfur accumulation on nitrogen-doped carbon strengthen its resistance to impurity-induced deactivation, in contrast to Ag catalysts that form Ag2S. Gas-fed tests in a membrane electrode assembly (MEA) electrolyzer further confirm that nitrogen-doped carbon sustains high CO selectivity at elevated current densities, while Ag nanoparticles suffer irreversible sulfur poisoning. These results demonstrate that nitrogen-doped carbon is intrinsically resistant to SO2-induced deactivation and highlight its potential as a robust catalyst for CO2 electroreduction under impurity-containing conditions.