Dual Single-Atomic Ni-N(4)and Fe-N(4)Sites Constructing Janus Hollow Graphene for Selective

Oxygen Electrocatalysis
Chen, JY (Chen, Jiangyue)[ 1 ] ; Li, H (Li, Hao)[ 2 ] ; Fan, C (Fan, Chuang)[ 1 ] ; Meng,

QW (Meng, Qingwei)[ 1 ] ; Tang, YW (Tang, Yawen)[ 1 ] ; Qiu, XY (Qiu, Xiaoyu)[ 1 ]*（邱晓雨

）; Fu, GT (Fu, Gengtao)[ 3,4 ]*; Ma, TY (Ma, Tianyi)[ 5 ]*

 

[ 1 ] Nanjing Normal Univ, Sch Chem & Mat Sci, Jiangsu Collaborat Innovat Ctr Biomed Funct

Mat, Jiangsu Key Lab New Power Batteries, Nanjing 210023, Peoples R China
[ 2 ] Univ Texas Austin, Dept Chem, Austin, TX 78712 USA
[ 3 ] Univ Texas Austin, Mat Sci & Engn Program, Austin, TX 78712 USA
[ 4 ] Univ Texas Austin, Texas Mat Inst, Austin, TX 78712 USA
[ 5 ] Univ Newcastle, Discipline Chem, Callaghan, NSW 2308, Australia

 

ADVANCED MATERIALS，202006,2003134

 

Nitrogen-coordinated metal single atoms in carbon have aroused extensive interest recently

and have been growing as an active research frontier in a wide range of key renewable

energy reactions and devices. Herein, a step-by-step self-assembly strategy is developed to

allocate nickel (Ni) and iron (Fe) single atoms respectively on the inner and outer walls

of graphene hollow nanospheres (GHSs), realizing separate-sided different single-atom

functionalization of hollow graphene. The Ni or Fe single atom is demonstrated to be

coordinated with four N atoms via the formation of a Ni-N(4)or Fe-N(4)planar configuration.

The developed Ni-N-4/GHSs/Fe-N(4)Janus material exhibits excellent bifunctional

electrocatalytic performance, in which the outer Fe-N(4)clusters dominantly contribute to

high activity toward the oxygen reduction reaction (ORR), while the inner Ni-N(4)clusters

are responsible for excellent activity toward the oxygen evolution reaction (OER). Density

functional theory calculations demonstrate the structures and reactivities of Fe-N(4)and

Ni-N(4)for the ORR and OER. The Ni-N-4/GHSs/Fe-N(4)endows a rechargeable Zn-air battery

with excellent energy efficiency and cycling stability as an air-cathode, outperforming

that of the benchmark Pt/C+RuO(2)air-cathode. The current work paves a new avenue for

precise control of single-atom sites on carbon surface for the high-performance and

selective electrocatalysts.

文章链接：
https://onlinelibrary.wiley.com/doi/full/10.1002/adma.202003134

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