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Graphite Nanoarrays-Confined Fe and Co Single-Atoms within Graphene Sponges as Bifunctional Oxygen Electrocatalyst for Ultralong Lasting Zinc-Air Battery

  • Chang Chen
    Chang Chen
    School of Chemical Sciences, National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 100049, P. R. China
    More by Chang Chen
  • Yifan Li
    Yifan Li
    School of Chemical Sciences, National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 100049, P. R. China
    More by Yifan Li
  • Dan Cheng
    Dan Cheng
    School of Chemical Sciences, National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 100049, P. R. China
    More by Dan Cheng
  • Hua He*
    Hua He
    School of Chemical Sciences, National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 100049, P. R. China
    *Email: [email protected]
    More by Hua He
  • , and 
  • Kebin Zhou*
    Kebin Zhou
    School of Chemical Sciences, National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 100049, P. R. China
    *Email: [email protected]
    More by Kebin Zhou
Cite this: ACS Appl. Mater. Interfaces 2020, 12, 36, 40415–40425
Publication Date (Web):August 18, 2020
https://doi.org/10.1021/acsami.0c12801
Copyright © 2020 American Chemical Society
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Abstract

The inferior stability of bifunctional oxygen electrocatalysts in the air cathode is one of the main obstacles that impedes the commercialization of zinc-air batteries (ZABs). This work describes a self-assembly technique combined with subsequent calcination to prepare a bifunctional oxygen electrocatalyst of graphite nanoarrays-confined Fe and Co single-atoms within graphene sponges (FeCo-NGS). Specifically, graphene sponges overspread with graphite nanoarrays as a structure regulation, which can prevent the metal single-atoms from aggregating and accelerate the mass/electron transfer, provides a guarantee for the long-term operation. Furthermore, M-N4 (M = Fe/Co) as the intrinsic activity regulation can effectively drive the heterogeneous oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalytic processes. Thanks to the rationally designed regulations, FeCo-NGS shows both extraordinary electrocatalytic activity for ORR and OER, even outperforming commercial Pt/C and IrO2. Remarkably, ZABs with FeCo-NGS air cathode demonstrate a record-breaking cycle lifetime of more than 1500 h (over 9000 cycles) at 10 mA cm–2 with a small charge–discharge gap.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c12801.

  • Experimental section, materials, materials characterization, electrochemical measurements; ORR and OER performance of the optimized samples; Raman spectrum of FeCo-NGS; HRTEM images of FeCo-NGS; HAADF-STEM images of Fe-NGS and Co-NGS; N2 adsorption–desorption isotherms of FeCo-NGS, Fe-NGS, Co-NGS, and NGS; XPS spectra of FeCo-NGS; XANES and EXAFS spectra of Fe-NGS and Co-NGS; CV curves for ORR process of FeCo-NGS and Pt/C; SEM images of FeCo-NGS after long-life cycles; XRD spectra of FeCo-NGS before cycles and after cycles; specific surface areas of FeCo-NGS; ICP-OES analysis results of FeCo-NGS, Fe-NGS, and Co-NGS; CHNS analysis results; EXAFS fitting parameters of FeCo-NGS; EXAFS fitting parameters of Fe-NGS and Co-NGS; ORR and OER performance of all samples; comparison of the ORR/OER performance of FeCo-NGS with the reported bifunctional oxygen electrocatalysts; and comparison of the ZABs performance of FeCo-NGS with the reported ZABs (PDF)

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This article is cited by 8 publications.

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  2. Haiyan Wang, Yakun Jiao, Saijun Wang, Pengcheng Ye, Jiqiang Ning, Yijun Zhong, Yong Hu. Accelerating Triple Transport in Zinc‐Air Batteries and Water Electrolysis by Spatially Confining Co Nanoparticles in Breathable Honeycomb‐Like Macroporous N‐Doped Carbon. Small 2021, 360 , 2103517. https://doi.org/10.1002/smll.202103517
  3. Biao Chen, Xiongwei Zhong, Guangmin Zhou, Naiqin Zhao, Hui‐Ming Cheng. Graphene‐Supported Atomically Dispersed Metals as Bifunctional Catalysts for Next‐Generation Batteries Based on Conversion Reactions. Advanced Materials 2021, 10 , 2105812. https://doi.org/10.1002/adma.202105812
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  7. Chang-Xin Zhao, Jia-Ning Liu, Juan Wang, Ding Ren, Bo-Quan Li, Qiang Zhang. Recent advances of noble-metal-free bifunctional oxygen reduction and evolution electrocatalysts. Chemical Society Reviews 2021, 50 (13) , 7745-7778. https://doi.org/10.1039/D1CS00135C
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