Atomic Layer Deposition of Cu Electrocatalysts on Gas Diffusion Electrodes for CO2 Reduction

• Published in: Nano letters Vol. 23; no. 23; pp. 10779 - 10787
• Main Authors: Lenef, Julia D., Lee, Si Young, Fuelling, Kalyn M., Rivera Cruz, Kevin E., Prajapati, Aditya, Delgado Cornejo, Daniel O., Cho, Tae H., Sun, Kai, Alvarado, Eugenio, Arthur, Timothy S., Roberts, Charles A., Hahn, Christopher, McCrory, Charles C. L., Dasgupta, Neil P.
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 13-12-2023
• Subjects: atomic layer deposition; catalyst; CO2 reduction; copper; ENGINEERING; gas diffusion electrode; copper; atomic layer deposition; CO2 reduction; gas diffusion electrode; catalyst
• ISSN: 1530-6984; 1530-6992
• DOI: 10.1021/acs.nanolett.3c02917

Electrochemical reduction of CO2 using Cu catalysts enables the synthesis of C2+ products including C2H4 and C2H5OH. In this study, Cu catalysts were fabricated using plasma-enhanced atomic layer deposition (PEALD), achieving conformal deposition of catalysts throughout 3-D gas diffusion electrode (GDE) substrates while maintaining tunable control of Cu nanoparticle size and areal loading. The electrochemical CO2 reduction at the Cu surface yielded a total Faradaic efficiency (FE) > 75% for C2+ products. Parasitic hydrogen evolution was minimized to a FE of ∼10%, and a selectivity of 42.2% FE for C2H4 was demonstrated. Compared to a line-of-sight physical vapor deposition method, PEALD Cu catalysts show significant suppression of C1 products compared to C2+, which is associated with improved control of catalyst morphology and conformality within the porous GDE substrate. Finally, PEALD Cu catalysts demonstrated a stable performance for 15 h with minimal reduction in the C2H4 production rate.