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Research Article

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

Nengfei Yu1( ), Hui Chen1, Jingbiao Kuang1, Kailin Bao1, Wei Yan2, Jilei Ye1( ), Zhongtang Yang1, Qinghong Huang1, Yuping Wu1( ), Shigang Sun2( )
School of Energy Sciences and Engineering, Nanjing Tech University, Nanjing 211816, China
State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative innovation center of Chemistry for Energy Materials, Xiamen University, Xiamen 361005, China
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Graphical Abstract

Atomically dispersed Co-N4 is anchored on N-doped graphene-like hierarchically porous carbon nanosheets (SA-Co-N4-GCs) where high exposed Co-N4 active sites and three dimensional (3D) interconnected hierarchically porous carbon provide efficient reactive sites and charge/mass transport environment. As a result, the rechargeable zinc-air batteries based on SA-Co-N4-GCs air electrodes exhibit superior charge–discharge performance and ultra-stable cyclability with no increase in polarization, even in the depth charging and discharging operation with 16 h per cycle over 600 h at 10 mA·cm−2.

Abstract

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 N-doped 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.

Keywords

bifunctional electrocatalystsCo-N4 active sites oxygen reduction reactionoxygen evolution reactionrechargeable Zn-air batteries

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Nano Research
Volume 15 Issue 8,
August 2022
Pages 7209-7219
DOI: 10.1007/s12274-022-4382-7
Cite this article:
Yu N, Chen H, Kuang J, et al. 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. Nano Research, 2022, 15(8): 7209-7219. https://doi.org/10.1007/s12274-022-4382-7
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Received: 08 March 2022
Revised: 31 March 2022
Accepted: 31 March 2022
Published: 17 May 2022
© Tsinghua University Press 2022
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