能源化学(英文版)

能源化学(英文版) ›› 2019, Vol. 39 ›› Issue (12): 152-159.

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Defective ZnS nanoparticles anchored in situ on N-doped carbon as a superior oxygen reduction reaction catalyst

Libing Hua, Zengxi Weib, Feng Yua, Huifang Yuana, Mincong Liua, Gang Wanga, Banghua Penga, Bin Daia, Jianmin Mab,c,d   

  1. a Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832003, Xinjiang, China;
    b School of Physics and Electronics, Hunan University, Changsha 410082, Hunan, China;
    c Institute of Advanced Electrochemical Energy, Xi'an University of Technology, Xi'an 710048, Shaanxi, China;
    d Key Laboratory of Materials Processing and Mold(Zhengzhou University), Ministry of Education, Zhengzhou University, Zhengzhou 450002, Henan, China
  • 收稿日期:2018-12-06 修回日期:2019-01-18 出版日期:2019-12-15 发布日期:2020-12-18
  • 通讯作者: Feng Yu, yufeng05@mail.ipc.ac.cn; Bin Dai, db_tea@shzu.edu.cn; Jianmin Ma, nanoelechem@hnu.edu.cn
  • 基金资助:
    This work was supported by the National Natural Science Foundation of China (21865025), and the Program for Changjiang Scholars and Innovative Research Team in University (No. IRT_15R46).

Defective ZnS nanoparticles anchored in situ on N-doped carbon as a superior oxygen reduction reaction catalyst

Libing Hua, Zengxi Weib, Feng Yua, Huifang Yuana, Mincong Liua, Gang Wanga, Banghua Penga, Bin Daia, Jianmin Mab,c,d   

  1. a Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832003, Xinjiang, China;
    b School of Physics and Electronics, Hunan University, Changsha 410082, Hunan, China;
    c Institute of Advanced Electrochemical Energy, Xi'an University of Technology, Xi'an 710048, Shaanxi, China;
    d Key Laboratory of Materials Processing and Mold(Zhengzhou University), Ministry of Education, Zhengzhou University, Zhengzhou 450002, Henan, China
  • Received:2018-12-06 Revised:2019-01-18 Online:2019-12-15 Published:2020-12-18
  • Contact: Feng Yu, yufeng05@mail.ipc.ac.cn; Bin Dai, db_tea@shzu.edu.cn; Jianmin Ma, nanoelechem@hnu.edu.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21865025), and the Program for Changjiang Scholars and Innovative Research Team in University (No. IRT_15R46).

摘要： Defect engineering has been used to develop low-cost and effective catalysts to boost oxygen reduction reactions. However, the development of catalysts that use metal cation vacancies as the active sites for oxygen reduction reaction is lacking. In this study, ZnS nanoparticles on N-doped carbon serve as an oxygen reduction reaction catalyst. These catalysts were prepared via a one-step method at 900℃. Amazingly, the high-resolution transmission electron microscope image revealed obvious defects in the ZnS nanoparticles. These facilitated the catalyst synthesis, and the product displayed good electrocatalytic performance for the oxygen reduction reaction in an alkaline medium, including a lower onset potential, lower mid-wave potential, four electron transfer process, and better durability compared with 20 wt% Pt/C. More importantly, the density functional theory results indicated that using the Zn vacancies in the prepared catalyst as active sites required a lower reaction energy to produce OOH* from *OO toward oxygen reduction reaction. Therefore, the proposed catalyst with Zn vacancies can be used as a potential electrocatalyst and may be substitutes for Pt-based catalysts in fuel cells, given the novel catalyst's resulting performance.

关键词: Defective ZnS nanoparticle, Zn vacancy, Electrocatalyst, Oxygen reduction reaction, Density functional theory calculations

Abstract: Defect engineering has been used to develop low-cost and effective catalysts to boost oxygen reduction reactions. However, the development of catalysts that use metal cation vacancies as the active sites for oxygen reduction reaction is lacking. In this study, ZnS nanoparticles on N-doped carbon serve as an oxygen reduction reaction catalyst. These catalysts were prepared via a one-step method at 900℃. Amazingly, the high-resolution transmission electron microscope image revealed obvious defects in the ZnS nanoparticles. These facilitated the catalyst synthesis, and the product displayed good electrocatalytic performance for the oxygen reduction reaction in an alkaline medium, including a lower onset potential, lower mid-wave potential, four electron transfer process, and better durability compared with 20 wt% Pt/C. More importantly, the density functional theory results indicated that using the Zn vacancies in the prepared catalyst as active sites required a lower reaction energy to produce OOH* from *OO toward oxygen reduction reaction. Therefore, the proposed catalyst with Zn vacancies can be used as a potential electrocatalyst and may be substitutes for Pt-based catalysts in fuel cells, given the novel catalyst's resulting performance.

Key words: Defective ZnS nanoparticle, Zn vacancy, Electrocatalyst, Oxygen reduction reaction, Density functional theory calculations