Abstract
AbstractDeveloping single‐atom electrocatalysts with high activity and superior selectivity at a wide potential window for CO2 reduction reaction (CO2RR) still remains a great challenge. Herein, a porous NiNC catalyst containing atomically dispersed NiN4 sites and nanostructured zirconium oxide (ZrO2@Ni‐NC) synthesized via a post‐synthetic coordination coupling carbonization strategy is reported. The as‐prepared ZrO2@Ni‐NC exhibits an initial potential of −0.3 V, maximum CO Faradaic efficiency (F.E.) of 98.6% ± 1.3, and a low Tafel slope of 71.7 mV dec−1 in electrochemical CO2RR. In particular, a wide potential window from −0.7 to −1.4 V with CO F.E. of above 90% on ZrO2@Ni‐NC far exceeds those of recently developed state‐of‐the‐art CO2RR electrocatalysts based on NiN moieties anchored carbon. In a flow cell, ZrO2@Ni‐NC delivers a current density of 200 mA cm−2 with a superior CO selectivity of 96.8% at −1.58 V in a practical scale. A series of designed experiments and structural analyses identify that the isolated NiN4 species act as real active sites to drive the CO2RR reaction and that the nanostructured ZrO2 largely accelerates the protonation process of *CO2− to *COOH intermediate, thus significantly reducing the energy barrier of this rate‐determining step and boosting whole catalytic performance.
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