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Title: Nitrogen-coordinated single iron atom catalysts derived from metal organic frameworks for oxygen reduction reaction

Abstract

Iron and nitrogen co-doped carbon (Fe-N-C) catalysts hold great promise to replace platinum group metal used for the oxygen reduction reaction (ORR) in low-temperature fuel cells. However, general synthesis routes require tedious acid washing and extensive heat treatment, usually resulting in uncontrollable morphologies and undesirable compounds. In this work, a zeolitic imidazolate framework (ZIF-8) was employed as a self-template for one-pot synthesis of a Fe-N-C catalyst consisting of uniformly dispersed Fe single atoms. Atomically dispersed Fe atoms were well distributed along the edges of the porous carbon matrix. Each of the Fe atoms was coordinated with four N atoms in the plane and two O atoms in the axial direction. The optimized Fe-N-C catalyst showed excellent ORR activities with half-wave potentials of 0.81 and 0.90 V in acidic and alkaline solutions, respectively. The results may be important for the optimization of single-atom-based catalysts for various reactions.

Authors:
 [1];  [2];  [2];  [3];  [4];  [5];  [5];  [1];  [6];  [7];  [8];  [9];  [10];  [1]
  1. Hong Kong Univ. of Science & Technology (Hong Kong)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Hong Kong Univ. of Science & Technology (Hong Kong); Univ. of California, Irvine, CA (United States)
  4. Chinese Academy of Sciences (CAS), Zhangjiang High Tech. Park (China)
  5. South Univ. of Science and Technology of China, Guangdong (China)
  6. Northwestern Polytechnical Univ., Xi'an (China)
  7. Chongqing Univ. (China)
  8. Univ. of California, Irvine, CA (United States)
  9. Hong Kong Univ. of Science & Technology (Hong Kong); Northwestern Polytechnical Univ., Xi'an (China)
  10. Argonne National Lab. (ANL), Argonne, IL (United States); Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1531159
Alternate Identifier(s):
OSTI ID: 1637195
Grant/Contract Number:  
AC02-06CH11357; AC0-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 61; Journal Issue: C; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; metal organic framework; non-precious metal catalysts; oxygen reduction reaction; single-atom catalyst

Citation Formats

Xiao, Fei, Xu, Gui-Liang, Sun, Cheng-Jun, Xu, Mingjie, Wen, Wen, Wang, Qi, Gu, Meng, Zhu, Shangqian, Li, Yueying, Wei, Zidong, Pan, Xiaoqing, Wang, Jiangan, Amine, Khalil, and Shao, Minhua. Nitrogen-coordinated single iron atom catalysts derived from metal organic frameworks for oxygen reduction reaction. United States: N. p., 2019. Web. doi:10.1016/j.nanoen.2019.04.033.
Xiao, Fei, Xu, Gui-Liang, Sun, Cheng-Jun, Xu, Mingjie, Wen, Wen, Wang, Qi, Gu, Meng, Zhu, Shangqian, Li, Yueying, Wei, Zidong, Pan, Xiaoqing, Wang, Jiangan, Amine, Khalil, & Shao, Minhua. Nitrogen-coordinated single iron atom catalysts derived from metal organic frameworks for oxygen reduction reaction. United States. https://doi.org/10.1016/j.nanoen.2019.04.033
Xiao, Fei, Xu, Gui-Liang, Sun, Cheng-Jun, Xu, Mingjie, Wen, Wen, Wang, Qi, Gu, Meng, Zhu, Shangqian, Li, Yueying, Wei, Zidong, Pan, Xiaoqing, Wang, Jiangan, Amine, Khalil, and Shao, Minhua. Thu . "Nitrogen-coordinated single iron atom catalysts derived from metal organic frameworks for oxygen reduction reaction". United States. https://doi.org/10.1016/j.nanoen.2019.04.033. https://www.osti.gov/servlets/purl/1531159.
@article{osti_1531159,
title = {Nitrogen-coordinated single iron atom catalysts derived from metal organic frameworks for oxygen reduction reaction},
author = {Xiao, Fei and Xu, Gui-Liang and Sun, Cheng-Jun and Xu, Mingjie and Wen, Wen and Wang, Qi and Gu, Meng and Zhu, Shangqian and Li, Yueying and Wei, Zidong and Pan, Xiaoqing and Wang, Jiangan and Amine, Khalil and Shao, Minhua},
abstractNote = {Iron and nitrogen co-doped carbon (Fe-N-C) catalysts hold great promise to replace platinum group metal used for the oxygen reduction reaction (ORR) in low-temperature fuel cells. However, general synthesis routes require tedious acid washing and extensive heat treatment, usually resulting in uncontrollable morphologies and undesirable compounds. In this work, a zeolitic imidazolate framework (ZIF-8) was employed as a self-template for one-pot synthesis of a Fe-N-C catalyst consisting of uniformly dispersed Fe single atoms. Atomically dispersed Fe atoms were well distributed along the edges of the porous carbon matrix. Each of the Fe atoms was coordinated with four N atoms in the plane and two O atoms in the axial direction. The optimized Fe-N-C catalyst showed excellent ORR activities with half-wave potentials of 0.81 and 0.90 V in acidic and alkaline solutions, respectively. The results may be important for the optimization of single-atom-based catalysts for various reactions.},
doi = {10.1016/j.nanoen.2019.04.033},
journal = {Nano Energy},
number = C,
volume = 61,
place = {United States},
year = {2019},
month = {4}
}

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