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 mA h 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 electrolyzer. 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.