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Title: From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]

Here, it remains highly desired but a great challenge to achieve atomically dispersed metals in high loadings for efficient catalysis. Now porphyrinic metal–organic frameworks (MOFs) have been synthesized based on a novel mixed–ligand strategy to afford high–content (1.76 wt %) single–atom (SA) iron–implanted N–doped porous carbon (Fe SA–N–C) via pyrolysis. Thanks to the single–atom Fe sites, hierarchical pores, oriented mesochannels and high conductivity, the optimized Fe SA–N–C exhibits excellent oxygen reduction activity and stability, surpassing almost all non–noble–metal catalysts and state–of–the–art Pt/C, in both alkaline and more challenging acidic media. More far–reaching, this MOF–based mixed–ligand strategy opens a novel avenue to the precise fabrication of efficient single–atom catalysts.
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [1] ;  [1]
  1. Univ. of Science and Technology of China, Anhui (People's Republic of China)
  2. Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chinese Academy of Sciences, Beijing (People's Republic of China)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 57; Journal Issue: 28; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; metal-organic frameworks; oxygen reduction reaction; porous carbon; single-atom catalysts
OSTI Identifier:
1463675
Alternate Identifier(s):
OSTI ID: 1441234

Jiao, Long, Wan, Gang, Zhang, Rui, Zhou, Hua, Yu, Shu -Hong, and Jiang, Hai -Long. From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]. United States: N. p., Web. doi:10.1002/anie.201803262.
Jiao, Long, Wan, Gang, Zhang, Rui, Zhou, Hua, Yu, Shu -Hong, & Jiang, Hai -Long. From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]. United States. doi:10.1002/anie.201803262.
Jiao, Long, Wan, Gang, Zhang, Rui, Zhou, Hua, Yu, Shu -Hong, and Jiang, Hai -Long. 2018. "From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]". United States. doi:10.1002/anie.201803262.
@article{osti_1463675,
title = {From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media [From MOFs to Single Fe Atoms Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media]},
author = {Jiao, Long and Wan, Gang and Zhang, Rui and Zhou, Hua and Yu, Shu -Hong and Jiang, Hai -Long},
abstractNote = {Here, it remains highly desired but a great challenge to achieve atomically dispersed metals in high loadings for efficient catalysis. Now porphyrinic metal–organic frameworks (MOFs) have been synthesized based on a novel mixed–ligand strategy to afford high–content (1.76 wt %) single–atom (SA) iron–implanted N–doped porous carbon (FeSA–N–C) via pyrolysis. Thanks to the single–atom Fe sites, hierarchical pores, oriented mesochannels and high conductivity, the optimized FeSA–N–C exhibits excellent oxygen reduction activity and stability, surpassing almost all non–noble–metal catalysts and state–of–the–art Pt/C, in both alkaline and more challenging acidic media. More far–reaching, this MOF–based mixed–ligand strategy opens a novel avenue to the precise fabrication of efficient single–atom catalysts.},
doi = {10.1002/anie.201803262},
journal = {Angewandte Chemie (International Edition)},
number = 28,
volume = 57,
place = {United States},
year = {2018},
month = {5}
}

Works referenced in this record:

Heat-treated polyacrylonitrile-based catalysts for oxygen electroreduction
journal, January 1989
  • Gupta, S.; Tryk, D.; Bae, I.
  • Journal of Applied Electrochemistry, Vol. 19, Issue 1, p. 19-27
  • DOI: 10.1007/BF01039385

Synthesis, Structure, and Metalation of Two New Highly Porous Zirconium Metal–Organic Frameworks
journal, June 2012
  • Morris, William; Volosskiy, Boris; Demir, Selcuk
  • Inorganic Chemistry, Vol. 51, Issue 12, p. 6443-6445
  • DOI: 10.1021/ic300825s

Introduction to Metal–Organic Frameworks
journal, September 2011
  • Zhou, Hong-Cai; Long, Jeffrey R.; Yaghi, Omar M.
  • Chemical Reviews, Vol. 112, Issue 2, p. 673-674
  • DOI: 10.1021/cr300014x

Zirconium-Metalloporphyrin PCN-222: Mesoporous Metal-Organic Frameworks with Ultrahigh Stability as Biomimetic Catalysts
journal, August 2012
  • Feng, Dawei; Gu, Zhi-Yuan; Li, Jian-Rong
  • Angewandte Chemie, Vol. 124, Issue 41, p. 10453-10456
  • DOI: 10.1002/ange.201204475

Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells
journal, April 2009
  • Lefèvre, Michel; Proietti, Eric; Jaouen, Frédéric
  • Science, Vol. 324, Issue 5923, p. 71-74
  • DOI: 10.1126/science.1170051

A review of Fe–N/C and Co–N/C catalysts for the oxygen reduction reaction
journal, June 2008