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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

Abstract 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 Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1463675
Alternate Identifier(s):
OSTI ID: 1441234
Grant/Contract Number:  
AC02-06CH11357
Resource 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
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. https://doi.org/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. https://doi.org/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 = {Abstract 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.},
doi = {10.1002/anie.201803262},
journal = {Angewandte Chemie (International Edition)},
number = 28,
volume = 57,
place = {United States},
year = {Wed May 09 00:00:00 EDT 2018},
month = {Wed May 09 00:00:00 EDT 2018}
}

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Cited by: 595 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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Decamethylcucurbit[5]uril based supramolecular assemblies as efficient electrocatalysts for the oxygen reduction reaction
journal, January 2019

  • Chen, Ruru; Cao, Minna; Wang, Jinyun
  • Chemical Communications, Vol. 55, Issue 78
  • DOI: 10.1039/c9cc05899k

Gas transport regulation in a MO/MOF interface for enhanced selective gas detection
journal, January 2019

  • Yao, Ming-Shui; Cao, Lin-An; Tang, Yong-Xiang
  • Journal of Materials Chemistry A, Vol. 7, Issue 31
  • DOI: 10.1039/c9ta05226g

The Challenge of Achieving a High Density of Fe-Based Active Sites in a Highly Graphitic Carbon Matrix
journal, February 2019

  • Li, Jingkun; Jia, Qingying; Mukerjee, Sanjeev
  • Catalysts, Vol. 9, Issue 2
  • DOI: 10.3390/catal9020144

A General Method for Transition Metal Single Atoms Anchored on Honeycomb‐Like Nitrogen‐Doped Carbon Nanosheets
journal, January 2020


Efficient Oxygen Reduction Catalysts of Porous Carbon Nanostructures Decorated with Transition Metal Species
journal, June 2019

  • Huang, Xiaoxiao; Shen, Tong; Zhang, Teng
  • Advanced Energy Materials, Vol. 10, Issue 11
  • DOI: 10.1002/aenm.201900375

Atomic‐Local Environments of Single‐Atom Catalysts: Synthesis, Electronic Structure, and Activity
journal, October 2019

  • Lai, Wei‐Hong; Miao, Zongcheng; Wang, Yun‐Xiao
  • Advanced Energy Materials, Vol. 9, Issue 43
  • DOI: 10.1002/aenm.201900722

Tailoring Nitrogen‐Doped Carbons as Hosts for Single‐Atom Catalysts
journal, May 2019


Recent progress in pyrolyzed carbon materials as electrocatalysts for the oxygen reduction reaction
journal, January 2020

  • Ouyang, Chen; Wang, Xun
  • Inorganic Chemistry Frontiers, Vol. 7, Issue 1
  • DOI: 10.1039/c9qi00962k

Atomic Fe Dispersed on N-Doped Carbon Hollow Nanospheres for High-Efficiency Electrocatalytic Oxygen Reduction
journal, December 2018


Iron Single Atoms on Graphene as Nonprecious Metal Catalysts for High‐Temperature Polymer Electrolyte Membrane Fuel Cells
journal, March 2019


Single‐Atom Cr−N 4 Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media
journal, July 2019


Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation
journal, September 2019


Apically Co-nanoparticles-wrapped nitrogen-doped carbon nanotubes from a single-source MOF for efficient oxygen reduction
journal, January 2018

  • Ma, Lin; Wang, Rui; Li, Ya-Hui
  • Journal of Materials Chemistry A, Vol. 6, Issue 47
  • DOI: 10.1039/c8ta08668k

A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation
journal, August 2019


Recent Advances in Isolated Single-Atom Catalysts for Zinc Air Batteries: A Focus Review
journal, October 2019

  • Zhang, Weimin; Liu, Yuqing; Zhang, Lipeng
  • Nanomaterials, Vol. 9, Issue 10
  • DOI: 10.3390/nano9101402

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