CO ₂ -philic NiNC nanocatalyst regulation mediated by imidazole-based ZIF for high-efficiency CO ₂ electroreduction

Developing highly efficient catalyst for carbon dioxide reduction (CO₂RR) to convert CO₂ into carbon-based chemicals and reduce anthropogenic carbon emission is desirable but challenging. In this work, a high-activity NiNC-2mIM catalyst has been developed via pyrolysis of 2-methylimidazole Ni-ZIF precursor, it exhibits excellent performance for CO₂ reduction producing CO, with Faradaic efficiency (<em>FE</em>_CO) of about 98% and a current density of 55 mA cm^-2 at -1.0 V (vs. RHE), outperforming the investigated NiNC-IM and NiNC-2eIM (derived from imidazole Ni ZIF precursor and 2-ethylimidazole Ni ZIF precursor, respectively) in this work and many previously reported Ni-based nanocatalysts. Mechanism studies demonstrate that 2-methylimidazole ligand induces higher content of pyridinic N species in the NiNC-2mIM catalyst, which enhances the affinity for CO₂ and provides low-polarity and high-activity Ni-N motif for CO₂RR. This work develops a novel imidazole-based ZIF mediated regulation strategy for engineering pyridinic-N-rich N-doped carbon supported Ni nanocatalyst to highly efficiently catalyze CO₂ reduction producing CO.