A Low‐Cost, Durable Bifunctional Electrocatalyst Containing Atomic Co and Pt Species for Flow Alkali‐Al/Acid Hybrid Fuel Cell and Zn–Air Battery

Abstract Transition metal single atoms anchored on nitrogen‐doped carbon (M‐N‐C) matrix with M‐N‐C active sites have shown to be promising catalysts for both hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). Herein, a hybrid catalyst with low‐level loading of atomic Pt and Co species encapsulated in nitrogen‐doped graphene (Pt@CoN₄‐G) is developed. The Pt@CoN₄‐G shows low overpotential for HER in wide‐pH electrolyte and manifests improved mass activity with almost eight times greater than that of Pt/C at an overpotential of 50 mV. The Pt@CoN₄‐G also exhibits a top‐level ORR activity (half‐wave potential, E_1/2 = 0.893 V) and robust stability (>200 h) in alkaline medium. Using theoretical calculations and comprehensive characterizations , the strong metal–support interactions between Pt species and CoN₄‐G support and synergistical cooperation of multiple active sites are clarified. A flow alkali‐Al/acid hybrid fuel cell using Pt@CoN₄‐G as cathode catalyst delivers a large power density of 222 mW cm⁻² with excellent stability to achieve simultaneously hydrogen evolution and electricity generation. In addition, Pt@CoN₄‐G endows a flow Zn‐air battery with high power density (316 mW cm⁻²), good stability under large current density (>100 h at 100 mA cm⁻²), and long cycle life (over 600 h at 5 mA cm⁻²).