Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
Publication date: 18th July 2023
Copper-based nanocatalysts are among the most promising candidates to drive the electrochemical CO2 reduction reaction (CO2RR). However, the stability of Cu catalysts during operation is sub-optimal, and improving this aspect of catalyst behavior is of uttermost importance to move the field forward.
Here, we attempted to tackle this challenge by exploiting the combination of Cu with Ga, a metal which can form alloys with Cu and has rationale to improve CO2RR upon combination with Cu. We used colloidal chemistry to synthesize well-defined alloy nanoparticles (NPs) with varied Ga content, including Cu, Cu-based solid solutions and Cu9Ga4 phases, and studied their structural evolution and performance as CO2RR catalysts.[1] We discovered that alloying Cu with Ga considerably improves the stability of the nanocatalysts, with CuGa NPs containing 17 at. % of Ga preserving half of their CO2RR activity for 20 hours while Cu NPs of the same size reconstruct and completely lose their CO2RR activity within 2 hours. Various characterization techniques, including X-Ray photoelectron spectroscopy and operando X-Ray absorption spectroscopy, suggest that the addition of Ga suppresses Cu oxidation at open circuit potential (ocp), and induces significant electronic interactions between Ga and Cu. Thus, we explain the observed stabilization of the Cu by Ga as a result of the higher oxophilicity and lower electronegativity of Ga, which reduce the propensity of Cu to oxidize at ocp and enhance the bond strength in the alloyed nanocatalysts. In addition to addressing one of the major challenges in CO2RR, this study proposes a strategy to generate NPs which are stable under a reducing reaction environment.
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