Wide Potential CO2‐to‐CO Electroreduction Relies on Pyridinic‐N/Ni–Nx Sites and Its Zn–CO2 Battery Application

Abstract

Although metal–N‐doped carbons are promising electrocatalysts for CO2‐to‐CO conversion due to their high conversion efficiency and current density, their commercial application is still challenging due to their narrow potential/current range. In general, a wide potential/current electrocatalyst is in high demand for industrial CO2 electrocatalysis. Controllable strategy to tune N configurations toward pyridinic‐enriched metal–Nx active sites is attractive. The synergetic effect of the ability of pyridinic N to capture Lewis acidic CO2 and the characteristics of Ni–N active sites to inhibit the hydrogen evolution reaction (HER) can achieve a wide potential window, which has high practical value. Herein, the well‐chosen precursors resulting in a pyridinic‐enriched Ni–Nx site can selectively catalyze CO2 toward CO generation in aqueous media with a high Faradaic efficiency (FE) of 100% with an overpotential of 680 mV. Continuous CO FE > 90% was recorded under a wide range of potentials without decay. Motivated by its practical characteristics in CO2 electrocatalysts, a Zn–CO2 battery is assembled achieving a CO2–CO conversion efficiency of more than 90% in a wide discharge current window. Therefore, the results highlight that pyridinic‐enriched Ni–Nx holds great promise as simultaneous CO‐selective electrocatalyst by suitably tuning M–N configurations as new perspective strategy.