NH3-Induced Challenges in CO2 Hydrogenation over the Cu/ZnO/Al2O3 Catalyst

Gas sources rich in CO2 derived from biomass/waste gasification, anaerobic digestion, or industrial carbon capture often contain impurities such as H2S, H2O, and NH3, which can significantly hinder catalyst performance. Here, we show the role of NH3 on the reverse water-gas shift (RWGS) reaction over a commercial Cu/ZnO/Al2O3 catalyst, examining its effects on both the catalytic activity and the catalyst structure. We found that NH3 reversibly decreases CO2 conversion immediately by suppressing carbonate hydrogenation and CO desorption. This effect intensifies with an increase in NH3 concentration but decreases at higher temperatures. However, prolonged exposure (over 100 h) to RWGS conditions in the presence of 1.4% NH3 leads to near-total and irreversible deactivation of the Cu/ZnO/Al2O3 catalyst. Under NH3 exposure, the catalyst loses Cu+ sites on the surface, causing a spatial separation of Cu and ZnO. Finally, to address this challenge, we propose a novel strategy to mitigate NH3 inhibition by decomposing NH3 into N-2 and H-2.