能源化学(英文) ›› 2019, Vol. 28 ›› Issue (7): 64-71.DOI: 10.1016/j.jechem.2018.09.003

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Hierarchical sulfur and nitrogen co-doped carbon nanocages as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air battery

Hao Fana, Yu Wanga, Fujie Gaoa, Longqi Yangb,c, Meng Liua, Xiao Dua, Peng Wangb,c, Lijun Yanga, Qiang Wua, Xizhang Wanga, Zheng Hua   

  1. a Key Laboratory of Mesoscopic Chemistry of MOE and Collaborative Innovation Center of Chemistry for Life Sciences, Jiangsu Provincial Laboratory for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, Jiangsu, China;
    b National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210023, Jiangsu, China;
    c College of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, Jiangsu, China
  • 收稿日期:2018-08-02 修回日期:2018-09-11 出版日期:2019-07-15 发布日期:2019-07-15
  • 通讯作者: Peng Wang, Qiang Wu, Xizhang Wang
  • 基金资助:
    We appreciate the financial support from the National Natural Science Foundation of China (21773111, 21473089, 21573107 and 51571110), the National Key Research and Development Program of China (2017YFA0206503, 2018YFA0209103), Priority Academic Program Development of Jiangsu Higher Education Institutions, Fundamental Research Funds for the Central Universities, and the program B for outstanding PhD candidate of Nanjing University (201702B049).

Hierarchical sulfur and nitrogen co-doped carbon nanocages as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air battery

Hao Fana, Yu Wanga, Fujie Gaoa, Longqi Yangb,c, Meng Liua, Xiao Dua, Peng Wangb,c, Lijun Yanga, Qiang Wua, Xizhang Wanga, Zheng Hua   

  1. a Key Laboratory of Mesoscopic Chemistry of MOE and Collaborative Innovation Center of Chemistry for Life Sciences, Jiangsu Provincial Laboratory for Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, Jiangsu, China;
    b National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210023, Jiangsu, China;
    c College of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, Jiangsu, China
  • Received:2018-08-02 Revised:2018-09-11 Online:2019-07-15 Published:2019-07-15
  • Contact: Peng Wang, Qiang Wu, Xizhang Wang
  • Supported by:
    We appreciate the financial support from the National Natural Science Foundation of China (21773111, 21473089, 21573107 and 51571110), the National Key Research and Development Program of China (2017YFA0206503, 2018YFA0209103), Priority Academic Program Development of Jiangsu Higher Education Institutions, Fundamental Research Funds for the Central Universities, and the program B for outstanding PhD candidate of Nanjing University (201702B049).

摘要: Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages (hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared hSNCNC exhibits a positive half-wave potential of 0.792 V (vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2, which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries.

关键词: 3D hierarchical, Carbon nanocages, S, N co-doping, Bifunctional electrocatalysis, Zn-air battery

Abstract: Exploring inexpensive and efficient bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is critical for rechargeable metal-air batteries. Herein, we report a new 3D hierarchical sulfur and nitrogen co-doped carbon nanocages (hSNCNC) as a promising bifunctional oxygen electrocatalyst by an in-situ MgO template method with pyridine and thiophene as the mixed precursor. The as-prepared hSNCNC exhibits a positive half-wave potential of 0.792 V (vs. reversible hydrogen electrode, RHE) for ORR, and a low operating potential of 1.640 V at a 10 mA cm-2 current density for OER. The reversible oxygen electrode index is 0.847 V, far superior to commercial Pt/C and IrO2, which reaches the top level of the reported bifunctional catalysts. Consequently, the hSNCNC as air cathodes in an assembled Zn-air battery features low charge/discharge overpotential and long lifetime. The remarkable properties arises from the introduced multiple heteroatom dopants and stable 3D hierarchical structure with multi-scale pores, which provides the abundant uniform high-active S and N species and efficient charge transfer as well as mass transportation. These results demonstrate the potential strategy in developing suitable carbon-based bi-/multi-functional catalysts to enable the next generation of the rechargeable metal-air batteries.

Key words: 3D hierarchical, Carbon nanocages, S, N co-doping, Bifunctional electrocatalysis, Zn-air battery