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Boosting the activity of Fe-Nx moieties in Fe-N-C electrocatalysts via phosphorus doping for oxygen reduction reaction

  • Jin-Cheng Li (李金成)
  • Hong Zhong (钟泓)
  • Mingjie Xu (徐明杰)
  • Tao Li (李涛)
  • Liguang Wang (王利光)
  • Qiurong Shi (石秋容)
  • Shuo Feng (冯硕)
  • Zhaoyuan Lyu (吕昭媛)
  • Dong Liu (刘栋)
  • Dan Du (杜丹)
  • Scott P. Beckman
  • Xiaoqing Pan (潘晓晴)
  • Yuehe Lin (林跃河)Email author
  • Minhua Shao (邵敏华)Email author
Articles Special Topic: Single-atom Catalysts
  • 89 Downloads

Abstract

The Fe-N-C material is a promising non-noble-metal electrocatalyst for oxygen reduction reaction (ORR). Further improvement on the ORR activity is highly desired in order to replace Pt/C in acidic media. Herein, we developed a new-type of single-atom Fe-N-C electrocatalyst, in which Fe-Nx active sites were modified by P atoms. The half-wave potential of the optimized material reached 0.858 V, which is 23 mV higher than that of the pristine one in a 0.1 mol L−1 HClO4 solution. Density functional theory (DFT) calculations revealed that P doping can reduce the thermodynamic over potential of the rate determining step and consequently improve the ORR activity.

Keywords

P-doping single-atom catalysts oxygen reduction 

P掺杂提高Fe–N–C催化剂中Fe–Nx活性基团的氧还原催化活性

摘要

Fe–N–C材料是一类有前景的非贵金属氧还原催化剂. 为了在酸性介质中取代Pt/C催化剂, 需要大幅度地改善其氧还原催化活性. 本文提出一种通过P原子掺杂的方法来调节单原子Fe–N–C材料中Fe–Nx活性位点的活性. 优化得到的材料在0.1 mol L−1 HClO4溶液中表现出优异的氧还原性能, 其半波电位为0.858 V(比没有P掺杂的Fe–N–C材料高23 mV). 密度泛函理论计算表明, P掺杂能降低限制步骤的热力学过电位, 从而提高其氧还原催化活性.

Notes

Acknowledgements

This work was supported by the National Key R&D Program of China (2017YFB0102900), the Research Grant Council (N_HKUST610117) of Hong Kong Special Administrative Region. It used resources of the Advanced Photon Source, Office of Science user facilities, supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (DE-AC02-06CH11357). Lin Y would like to acknowledge the WSU start-up fund. Li T is thankful for the NIU start-up fund.

Conflict of interest The authors declare that they have no conflict of interest.

Supplementary material

40843_2019_1207_MOESM1_ESM.pdf (2.7 mb)
Boosting the activity of atomic Fe-Nx moieties in Fe-N-C electrocatalysts via phosphorus doping towards efficient oxygen reduction in acidic conditions

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Copyright information

© Science China Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  • Jin-Cheng Li (李金成)
    • 1
    • 2
  • Hong Zhong (钟泓)
    • 1
  • Mingjie Xu (徐明杰)
    • 2
    • 3
  • Tao Li (李涛)
    • 4
    • 5
  • Liguang Wang (王利光)
    • 4
  • Qiurong Shi (石秋容)
    • 1
  • Shuo Feng (冯硕)
    • 1
  • Zhaoyuan Lyu (吕昭媛)
    • 1
  • Dong Liu (刘栋)
    • 1
  • Dan Du (杜丹)
    • 1
  • Scott P. Beckman
    • 1
  • Xiaoqing Pan (潘晓晴)
    • 3
  • Yuehe Lin (林跃河)
    • 1
    Email author
  • Minhua Shao (邵敏华)
    • 2
    • 6
    Email author
  1. 1.School of Mechanical and Materials EngineeringWashington State UniversityPullmanUSA
  2. 2.Fok Ying Tung Research InstituteHong Kong University of Science and TechnologyGuangzhouChina
  3. 3.Department of Chemical Engineering and Materials ScienceUniversity of California IrvineIrvineUSA
  4. 4.Department of Chemistry and BiochemistryNorthern Illinois UniversityDeKalbUSA
  5. 5.X-ray Science DivisionArgonne National LaboratoryLemontUSA
  6. 6.Department of Chemical and Biological EngineeringHong Kong University of Science and TechnologyKowloon, Hong KongChina

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