Heterointerfacial Cobalt/Zinc Sulfides on Molybdenum Disulfide Coated Carbon Cloth as Self‐Supporting Electrode for Flexible Metal‐Air Batteries

Abstract Rational design of effective non‐precious metal for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is urgently demanded for flexible metal‐air batteries. Engineering heterointerfaces between metal compounds is an attractive strategy for fabricating high‐performance bifunctional electrocatalysts. Herein, a facile spontaneous sulfurization strategy is developed to fabricate the self‐supporting electrode consisting of homogeneous Co 3 S 4 and ZnS on MoS 2 with abundant sulfur vacancies, as well as the unique heterointerfaces and conductive carbon skeleton. Owing to the hierarchical structure and more exposed active sites, the optimal Co(Zn 0.5 )@MoS 2 /CC electrode exhibits excellent bifunctional catalytic activity with the smaller ΔE value (E j=10,OER −E 1/2,ORR ) and durability. Furthermore, Co(Zn 0.5 )@MoS 2 /CC based all‐solid‐state zinc‐air and aluminum‐air batteries also deliver high open‐circle voltage, desirable power density and flexibility. This approach offers a novel method to obtain the self‐supporting electrodes with porous structure and highly active metal sulfides.