Bimetallic Tandem Strategy for Effective Modulation of CO2 Electrocatalytic Selectivity on Relatively Inert Cu
Yong Yan1, Huan Zhou1, Tongxian Li1
1State Key Laboratory of Materials Low-Carbon Recycling, Center of Excellence for Environmental Safety and Biological Effects, Department of Chemistry, College of Chemistry and Life Science, Beijing University of Technology, Beijing, 100124, China.
Abstract:
The development of effective strategies to enhance the activity and selectivity of Cu-based catalysts for the CO2 reduction reaction (CO2RR) remains a critical challenge, particularly on relatively inert Cu facets that are highly active in the competitive hydrogen evolution reaction (HER). In this study, a series of Cu-M (M = Au, Ag, Pd) bimetallic tandem interfaces are fabricated on Cu nanocolumn arrays (Cu NCAs) with predominantly exposed Cu (200) facets. These interfaces excited a significant number of Cu+ species and modulated the adsorption behavior of critical intermediates for CO2RR, resulting in improved CO2RR activity and a substantial reduction in the competitive HER. Notably, the Cu-Au, Cu-Ag, and Cu-Pd NCAs displayed excellent selectivity for C2H4, CO, and HCOOH products, with optimized faradaic efficiency (FE) of ≈43.2, ≈48.0, and ≈50.7%, respectively. According to in situ spectroscopic analysis, each Cu-M interface exhibited distinct catalytic pathways: Cu-Au favored *COOH and *CO adsorption followed by C-C coupling for C2H4 production, Cu-Ag promoted *CO desorption for CO generation, and Cu-Pd facilitated *OCHO formation for HCOOH production. This study provides a strategy to design high-performance and more practical bimetallic Cu-based catalytic electrodes by directly modifying various commercial Cu substrates.
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