Abstract
The synergistic effect of muti-metallic catalysts, possessing noticeable potential in tuning the physicochemical properties, provides a promising strategy to boost the electrocatalytic performance of catalysts for electrochemical CO2 reduction reaction (CO2RR). Herein, a series of trimetallic TM-NiFe (TM = first-row transition metals) catalysts were designed and screened by creating a two-dimensional active volcano curve. Moreover, the catalytic performance of TM-NiFe catalysts for converting CO2 to CO and HCOOH were evaluated via the density functional theory. The results indicate that Zn-NiFe presents better CO2RR-to-CO performance with a low overpotential of 0.697 V. The slightly weak adsorption strength of CO* on Zn-NiFe surface facilitates the kinetics of the potential-determining step (CO* → CO). V-NiFe is an ideal catalyst to produce syngas (CO and H2) due to the equivalent activity of CO2RR and hydrogen evolution reaction (HER). The Cr-NiFe catalyst favors the COOH* pathway over HCOO* pathway in the process of HCOOH generation. The negative charge on the catalyst surface and the low d-band center of Cr atoms promote the production of HCOOH over the Cr-NiFe catalyst at an exceptionally low overpotential of 0.080 V. Furthermore, Cr-NiFe catalyst significantly inhibits its competitive reactions (HER and CO2RR-to-CO). This work lays a reliable foundation for improving the activity and selectivity of trimetallic catalysts in CO2 conversion to essential chemical feedstocks.
Published Version
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