Co Nanoparticles/Co, N, S Tri-doped Graphene Templated from In-Situ-Formed Co, S Co-doped g-C3N4 as an Active Bifunctional Electrocatalyst for Overall Water Splitting.

The development of high-performance electrocatalyst with earth-abundant elements for water-splitting is a key factor to improve its cost efficiency. Herein, a noble metal-free bifunctional electrocatalyst was synthesized by a facile pyrolysis method using sucrose, urea, Co(NO3)2 and sulfur powder as raw materials. During the fabrication process, Co, S co-doped graphitic carbon nitride (g-C3N4) was first produced, and then this in-situ-formed template further induced the generation of a Co, N, S tri-doped graphene coupled with Co nanoparticles (NPs) in the following pyrolysis process. The effect of pyrolysis temperature (700, 800, and 900 °C) on the physical properties and electrochemical performances of the final product was studied. Thanks to the increased number of graphene layer encapsulated Co NPs, higher graphitization degree of carbon matrix and the existence of hierarchical macro/meso pores, the composite electrocatalyst prepared under 900 °C presented the best activity for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) with outstanding long-term durability. This work presented a facile method for the fabrication of non-noble-metal-based carbon composite from in-situ-formed template and also demonstrated a potential bifunctional electrocatalyst for the future investigation and application.