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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]

Abstract

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:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1463675
Alternate Identifier(s):
OSTI ID: 1441234
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Volume: 57; Journal Issue: 28; Journal ID: ISSN 1433-7851
Publisher:
Wiley
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

Citation Formats

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., 2018. 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. Wed . "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. https://www.osti.gov/servlets/purl/1463675.
@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)},
issn = {1433-7851},
number = 28,
volume = 57,
place = {United States},
year = {2018},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 47 works
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Figures / Tables:

Scheme 1 Scheme 1: Illustration of the rational fabrication of single Fe atoms-involved FeSA-N-C catalyst via a mixed-ligand strategy.

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.