Continuous increase of anthropogenic CO2 is a major concern of modern world. Therefore, mitigation strategies such as CO2 capture, conversion and storage are major interest in energy research. Among all the mitigation strategies, electrochemical CO2 conversion is most viable due to its low operating costs. This is because the proton source comes from aqueous solution and designing of efficient catalyst facilitates CO2 conversion to valuable chemicals at low applied potentials. In this work we designed a Cu-templated Cu@CuAu core-shell nanocrystal by epitaxial growth of Au on Cu in a one-pot synthesis method. The Cu core was acid washed forming CuAu alloy nanocages for electroreduction of CO2. The CuAu alloy nanocages exhibit pinholes on the surface therefore availing both Au rich (outer shell) and Cu rich (inner shell) accessible for reactants. CuAu alloy nanocages are then used for electroreduction of CO2 at -0.6, -0.7, -0.8 and -0.9 V vs RHE in 0.5 KCl. This resulted in selective conversion of CO2 to CO with maximum faradaic efficiency of 74.58% at -0.8V vs RHE with H2 as sole byproduct. DFT calculation was carried out on the CuAu alloy nanocage for mechanistic understanding. This indicated the Cu-rich inner wall of CuAu alloy nanocage enhances the CO2 conversion efficiency to CO (by stabilizing *COOH adsorption), while suppressing HER (by adsorbing hydrogen too tightly).

Selective CO2 electroreduction to CO using Cu-rich inner surface CuAu alloy beveled nanobox

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