Constructing Dual‐Phase Co₉S₈‐CoMo₂S₄ Heterostructure as an Efficient Trifunctional Electrocatalyst for Oxygen Reduction, Oxygen Evolution and Hydrogen Evolution Reactions

Designing robust, efficient and inexpensive trifunctional electrocatalysts for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is significant for rechargeable zinc-air batteries and water-splitting devices. To this end, constructing heterogenous structures based on transition metals stands out as an effective strategy. Herein, a dual-phase Co₉S₈-CoMo₂S₄ heterostructure grown on porous N, S-codoped carbon substrate (Co₉S₈-CoMo₂S₄/NSC) via a one-pot synthesis is investigated as the trifunctional ORR/OER/HER electrocatalyst. The optimized Co₉S₈-CoMo₂S₄/NSC2 exhibits that ORR has a half-wave potential of 0.86 V (vs. RHE) and the overpotentials at 10 mA cm^-2 for OER and HER are 280 and 89 mV, respectively, superior to most transition-metal based trifunctional electrocatalysts reported to date. The Co₉S₈-CoMo₂S₄/NSC2-based zinc-air battery (ZAB) has a high open-circuit voltage (1.41 V), large capacity (804 mAh g^-1) and highly stable cyclability (97 h at 10 mA cm^-2). In addition, the prepared Co₉S₈-CoMo₂S₄/NSC2-based ZAB in series can self-drive the corresponding water-splitting device. The dual-phase Co₉S₈-CoMo₂S₄ heterostructure provides not only multi-type active sites to drive the ORR, OER and HER, but also high-speed charge transfer channels between two phases to improve the synergistic effect and reaction kinetics.