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It remains an ongoing challenge to develop cheap, highly active, and stable electrocatalysts to promote the sluggish electrocatalytic oxygen evolution, oxygen reduction, and hydrogen evolution reactions for rechargeable metal–air batteries and water-splitting systems. In this work, we report the morphology-controllable synthesis of zinc cobalt mixed sulfide (Zn–Co–S) nanoarchitectures, including nanosheets, nanoplates, and nanoneedles, grown on conductive carbon fiber paper (CFP) and the micronanostructure dependent electrochemical efficacy for catalyzing hydrogen and oxygen in zinc-air batteries and water electrolysis. The formation of different Zn–Co–S morphologies was attributed to the synergistic effect of decomposed urea products and the corrosion of NH 4 F. Among synthesized Zn–Co–S nanostructures, the nanoneedle arrays supported on CFP exhibit superior trifunctional activity for oxygen reduction, oxygen evolution, and hydrogen evolution reactions than its nanosheet and nanoplate counterparts through half reaction testing. It also exhibited better catalytic durability than Pt/C and RuO 2 . Furthermore, the Zn–Co–S nanoneedle/CFP electrode enables rechargeable Zn-air batteries with low overpotential (0.85 V), high efficiency (58.1%), and long cycling lifetimes (200 cycles) at 10 mA cm –2 as well as considerable performance for water splitting. The superior performance is contributed to the integrated nanoneedle/CFP nanostructure, which not only provides enhanced electrochemical active area, but also facilitates ion and gas transfer between the catalyst surface and electrolyte, thus maintaining an effective solid–liquid–gas interface necessary for electrocatalysis. These results indicate that the Zn–Co–S nanoneedle/CFP system is a low cost, highly active, and durable electrode for highly efficient rechargeable zinc–air batteries and water electrolysis in alkaline solution.
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