Free-standing and fexible air electrodes with long-lasting bifunctional activities for both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)are crucial to the development of wearable Zn-air rec...Free-standing and fexible air electrodes with long-lasting bifunctional activities for both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)are crucial to the development of wearable Zn-air rechargeable batteries.In this work,we synthesize a fexible air electrode consisting of 3D nanoporous N-doped graphene with trimodal shells and Ni particles through repeated chemical vapor deposition(CVD)and acidic etching processes.Our results indicate that such trimodal graphene morphology significantly enhances the active N-dopant sites and graphene-coated Ni surface,which consequentially boosts both the ORR and OER activities,as well as catalytic durability.First-principles density functional theory(DFT)calculations reveal the synergetic effects between the Ni and the N-doped graphene;namely,the Ni nanoparticles boost the bifunctional activities of the coated N-doped graphene,and in turn the graphene-covering layers enhance the stability of Ni.Thanks to the better protection from the triple graphene shells,our trimodal N-doped graphene/Ni-based Zn-air battery can be stably discharged/recharged beyond 2500 h with low overpotentials.It is reasonable to expect that such freestanding trimodal graphene/Ni would be promising in many fexible energy conversion/storage devices.展开更多
基金financially supported by the Development and Reform Commission of Shenzhen Municipalitythe National Natural Science Foundation of China(Grant Nos.51702031,51871077)+1 种基金the Shenzhen Fundamental Research Program(Grant Nos.JCYJ20180306171644942,JCYJ20180507184623297,KQJSCX20180328165656256)the Innovation Project from Harbin Institute of Technology。
文摘Free-standing and fexible air electrodes with long-lasting bifunctional activities for both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)are crucial to the development of wearable Zn-air rechargeable batteries.In this work,we synthesize a fexible air electrode consisting of 3D nanoporous N-doped graphene with trimodal shells and Ni particles through repeated chemical vapor deposition(CVD)and acidic etching processes.Our results indicate that such trimodal graphene morphology significantly enhances the active N-dopant sites and graphene-coated Ni surface,which consequentially boosts both the ORR and OER activities,as well as catalytic durability.First-principles density functional theory(DFT)calculations reveal the synergetic effects between the Ni and the N-doped graphene;namely,the Ni nanoparticles boost the bifunctional activities of the coated N-doped graphene,and in turn the graphene-covering layers enhance the stability of Ni.Thanks to the better protection from the triple graphene shells,our trimodal N-doped graphene/Ni-based Zn-air battery can be stably discharged/recharged beyond 2500 h with low overpotentials.It is reasonable to expect that such freestanding trimodal graphene/Ni would be promising in many fexible energy conversion/storage devices.