Local compressive strain regulation of atomically dispersed NiN4 sites for enhancing CO2 electroreduction to CO†
Abstract
Electroreduction of CO2 to valuable chemicals powered by renewable electricity provides a sustainable approach to reduce the environmental issues originating from CO2 emission. However, insufficient current density and production selectivity hinder its further application. In this case, precisely regulating the CO2 reduction reaction (CO2RR) active sites is an excellent strategy to simultaneously reduce the reaction barrier and suppress the hydrogen evolution reaction (HER) pathway. Herein, the strain regulation of atomically dispersed NiN4 active sites is investigated in helical carbon. Ni–N coordination in the curved carbon lattice displays a reduced distance compared to that in a straight lattice, inflicting local compressive strain on NiN4. The resultant catalyst shows the highest CO selectivity of up to 99.4% at −1.4 V (vs. RHE), the FECO is maintained at over 85% over a wide potential range from −0.8 to −1.8 V (vs. RHE), and the maximum partial current density for CO reaches a high of 458 mA cm−2 at −1.8 V (vs. RHE). Theoretical investigations show the superior CO2 electroreduction performance of curved NiN4 stems from its remarkable ability to generate the *COOH intermediate and to suppress the hydrogen combination simultaneously. Our findings offer a novel strategy to rationally regulate the local three-dimensional structure of single-atom sites for efficient electrocatalysis.
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