Highly Efficient Multifunctional Co-N-C Electrocatalysts with Synergistic Effects of Co-N Moieties and Co Metallic Nanoparticles Encapsulated in a N-Doped Carbon Matrix for Water-Splitting and Oxygen Redox Reactions.

Electrochemical water-splitting reactions (hydrogen evolution reaction (HER) and oxygen evolution reaction (OER)) and oxygen redox reactions (oxygen reduction reaction (ORR) and OER) are core processes for electrochemical water-splitting devices, rechargeable metal-air batteries, and regenerative fuel cells. Developing highly efficient non-noble multifunctional catalysts in the same electrolyte is an open challenge. Herein, efficient Co-N-C electrocatalysts with a mixed structure comprising Co-N moieties and Co nanoparticles encapsulated in a N-doped carbon layer were prepared via pyrolysis of a new structure of Co-coordinated bis(imino)pyridine polymer constructed by 2,6-diacetylpyridine and 3,3'-diaminobenzidine. Results demonstrate that Co ion sources have a remarkable impact on the final Co-N-C performance. The Co-N-C catalyst prepared using cobalt acetate as a precursor displays remarkable overall multifunctional performance. It needs only a cell voltage of 1.66 V (obtained from the half-cell test) for the water-splitting reaction (HER/OER) to reach 10 mA·cm in 1.0 M KOH, and the overall oxygen redox activity (OER/ORR) is 0.72 V in 0.1 M KOH, outperforming the reported nonprecious metal catalysts. The excellent activity is attributable to the synergistic effects between active sites with encapsulated metallic Co for HER and OER and Co-N moieties for ORR.