Efficient oxygen electrocatalysts with highly-exposed Co-N4 active sites on N-doped graphene-like hierarchically porous carbon nanosheets enhancing the performance of rechargeable Zn-air batteries

摘要

Designing bifunctional oxygen electrocatalysts with high activity,lasting stability,and low-cost for rechargeable zinc-air batteries(RZABs)is a tough challenge.Herein,an advanced electrocatalyst is prepared by anchoring atomically dispersed Co atoms on Ndoped graphene-like hierarchically porous carbon nanosheets(SA-Co-N4-GCs)and thereby forming Co-N4-C architecture.Its unique structure with excellent conductivity,large surface area,and three dimensional(3D)interconnected hierarchically porous architecture exposes not only more Co-N4 active sites to accelerate the kinetics of both oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),but also provides an efficient charge/mass transport environment to reduce diffusion barrier.Consequently,SA-Co-N4-GCs exhibits excellent ORR/OER bifunctional activities and durability,surpassing noble-metal catalysts.Liquid RZABs using SA-Co-N4-GCs cathodes display a high open-circuit voltage of 1.51 V,a remarkable power density of 149.3 mW·cm−2,as well as excellent stability and rechargeability with faint increase in polarization even at a large depth of charge–discharge cycle with 16 h per cycle over an entire 600 h long-term test.Moreover,flexible quasi-solid-state RZABs with SA-Co-N4-GCs cathodes also deliver a considerable power density of 124.5 mW·cm−2,which is even higher than that of liquid batteries using noble-metal catalysts.This work has thrown new insight into development of high-performance and low-cost electrocatalysts for energy conversion and storage.