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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]
+ Show Author Affiliations
  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 Laboratory (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.
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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
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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.
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@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 = {Thu Apr 11 00:00:00 EDT 2019},
month = {Thu Apr 11 00:00:00 EDT 2019}
}
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Works referenced in this record:

Recent Advances in Electrocatalysts for Oxygen Reduction Reaction
journal, February 2016

Synthesis and Characterization of 9 nm Pt–Ni Octahedra with a Record High Activity of 3.3 A/mg Pt for the Oxygen Reduction Reaction
journal, June 2013

  • Choi, Sang-Il; Xie, Shuifen; Shao, Minhua
  • Nano Letters, Vol. 13, Issue 7
  • DOI: 10.1021/nl401881z

A New Fuel Cell Cathode Catalyst
journal, March 1964

  • Jasinski, Raymond
  • Nature, Vol. 201, Issue 4925, p. 1212-1213
  • DOI: 10.1038/2011212a0

Atomic interpretation of high activity on transition metal and nitrogen-doped carbon nanofibers for catalyzing oxygen reduction
journal, January 2017

  • Yan, Xingxu; Liu, Kexi; Wang, Tuo
  • Journal of Materials Chemistry A, Vol. 5, Issue 7
  • DOI: 10.1039/C6TA09462G

A General Approach to Preferential Formation of Active Fe–N x Sites in Fe–N/C Electrocatalysts for Efficient Oxygen Reduction Reaction
journal, November 2016

  • Sa, Young Jin; Seo, Dong-Jun; Woo, Jinwoo
  • Journal of the American Chemical Society, Vol. 138, Issue 45
  • DOI: 10.1021/jacs.6b09470

A Pt-free Electrocatalyst Based on Pyrolized Vinazene-Carbon Composite for Oxygen Reduction Reaction
journal, April 2015

A Pt-free catalyst for oxygen reduction reaction based on Fe–N multiwalled carbon nanotube composites
journal, September 2013

High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
journal, April 2011

Novel dual templating approach for preparation of highly active Fe-N-C electrocatalyst for oxygen reduction
journal, January 2017

Discriminating Catalytically Active FeN x Species of Atomically Dispersed Fe–N–C Catalyst for Selective Oxidation of the C–H Bond
journal, July 2017

  • Liu, Wengang; Zhang, Leilei; Liu, Xin
  • Journal of the American Chemical Society, Vol. 139, Issue 31
  • DOI: 10.1021/jacs.7b05130

Engineering nanostructures of PGM-free oxygen-reduction catalysts using metal-organic frameworks
journal, January 2017

Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts
journal, August 2016

  • Yin, Peiqun; Yao, Tao; Wu, Yuen
  • Angewandte Chemie International Edition, Vol. 55, Issue 36
  • DOI: 10.1002/anie.201604802

Iron porphyrin-based cathode catalysts for PEM fuel cells: Influence of pyrolysis gas on activity and stability
journal, November 2009

Heat-Treated Fe/N/C Catalysts for O2 Electroreduction:  Are Active Sites Hosted in Micropores?
journal, March 2006

  • Jaouen, Frédéric; Lefèvre, Michel; Dodelet, Jean-Pol
  • The Journal of Physical Chemistry B, Vol. 110, Issue 11, p. 5553-5558
  • DOI: 10.1021/jp057135h

Correlations between Mass Activity and Physicochemical Properties of Fe/N/C Catalysts for the ORR in PEM Fuel Cell via 57 Fe Mössbauer Spectroscopy and Other Techniques
journal, January 2014

  • Kramm, Ulrike I.; Lefèvre, Michel; Larouche, Nicholas
  • Journal of the American Chemical Society, Vol. 136, Issue 3
  • DOI: 10.1021/ja410076f

Monocrystalline spinel nanotube fabrication based on the Kirkendall effect
journal, July 2006

  • Jin fan, Hong; Knez, Mato; Scholz, Roland
  • Nature Materials, Vol. 5, Issue 8
  • DOI: 10.1038/nmat1673

Hollow nanostructures based on the Kirkendall effect: Design and stability considerations
journal, February 2005

  • Tu, K. N.; Gösele, U.
  • Applied Physics Letters, Vol. 86, Issue 9
  • DOI: 10.1063/1.1873044

Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation
journal, September 2017

  • Zhang, Hanguang; Hwang, Sooyeon; Wang, Maoyu
  • Journal of the American Chemical Society, Vol. 139, Issue 40
  • DOI: 10.1021/jacs.7b06514

A Multiplet Analysis of Fe K-Edge 1s → 3d Pre-Edge Features of Iron Complexes
journal, July 1997

  • Westre, Tami E.; Kennepohl, Pierre; DeWitt, Jane G.
  • Journal of the American Chemical Society, Vol. 119, Issue 27
  • DOI: 10.1021/ja964352a

Oxygen reduction reaction on Pt(111): effects of bromide
journal, June 1999

  • Marković, N. M.; Gasteiger, H. A.; Grgur, B. N.
  • Journal of Electroanalytical Chemistry, Vol. 467, Issue 1-2
  • DOI: 10.1016/S0022-0728(99)00020-0

Full spectral calculation of non-retarded Hamaker constants for ceramic systems from interband transition strengths
journal, January 1995

Effect of ZIF-8 Crystal Size on the O2 Electro-Reduction Performance of Pyrolyzed Fe–N–C Catalysts
journal, July 2015

  • Armel, Vanessa; Hannauer, Julien; Jaouen, Frédéric
  • Catalysts, Vol. 5, Issue 3
  • DOI: 10.3390/catal5031333

A metal–organic framework-derived bifunctional oxygen electrocatalyst
journal, January 2016

Ordered macro-microporous metal-organic framework single crystals
journal, January 2018

Adsorption of carbon dioxide, methane, nitrogen, oxygen and argon in NaETS-4
journal, August 2008

Durability challenges and perspective in the development of PGM-free electrocatalysts for the oxygen reduction reaction
journal, June 2018

Palladium Monolayer and Palladium Alloy Electrocatalysts for Oxygen Reduction †
journal, December 2006

Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst
journal, August 2017

Active sites of nitrogen-doped carbon materials for oxygen reduction reaction clarified using model catalysts
journal, January 2016

High Performance Fe- and N- Doped Carbon Catalyst with Graphene Structure for Oxygen Reduction
journal, May 2013

  • Peng, Hongliang; Mo, Zaiyong; Liao, Shijun
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep01765

Cheap carbon black-based high-performance electrocatalysts for oxygen reduction reaction
journal, January 2015

  • Song, Ping; Zhang, Yuwei; Pan, Jing
  • Chemical Communications, Vol. 51, Issue 10
  • DOI: 10.1039/C4CC07677J

A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
journal, December 2015

Observations and interpretation of x-ray absorption edges in iron compounds and proteins
journal, May 1976

  • Shulman, G. R.; Yafet, Y.; Eisenberger, P.
  • Proceedings of the National Academy of Sciences, Vol. 73, Issue 5
  • DOI: 10.1073/pnas.73.5.1384

Fe 2 O 3 Nanoparticle Structures Investigated by X-ray Absorption Near-Edge Structure, Surface Modifications, and Model Calculations
journal, August 2002

  • Chen, Lin X.; Liu, Tao; Thurnauer, Marion C.
  • The Journal of Physical Chemistry B, Vol. 106, Issue 34
  • DOI: 10.1021/jp025544x

Molecular stereochemistry of two intermediate-spin complexes. Iron(II) phthalocyanine and manganese(II) phthalocyanine
journal, July 1976

  • Kirner, John F.; Dow, W.; Scheidt, W. Robert.
  • Inorganic Chemistry, Vol. 15, Issue 7
  • DOI: 10.1021/ic50161a042

Activity Descriptor Identification for Oxygen Reduction on Nonprecious Electrocatalysts: Linking Surface Science to Coordination Chemistry
journal, October 2013

  • Ramaswamy, Nagappan; Tylus, Urszula; Jia, Qingying
  • Journal of the American Chemical Society, Vol. 135, Issue 41
  • DOI: 10.1021/ja405149m

Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials
journal, August 2015

  • Zitolo, Andrea; Goellner, Vincent; Armel, Vanessa
  • Nature Materials, Vol. 14, Issue 9
  • DOI: 10.1038/nmat4367

Isolated Single Iron Atoms Anchored on N-Doped Porous Carbon as an Efficient Electrocatalyst for the Oxygen Reduction Reaction
journal, April 2017

  • Chen, Yuanjun; Ji, Shufang; Wang, Yanggang
  • Angewandte Chemie, Vol. 129, Issue 24
  • DOI: 10.1002/ange.201702473

Encapsulation of Iron Carbide in Carbon Nanocapsules
journal, July 1995

  • Kopelev, Nikolai S.; Chechersky, Vladimir; Nath, Amar
  • Chemistry of Materials, Vol. 7, Issue 7
  • DOI: 10.1021/cm00055a022

Evaluation of iron-containing carbon nanotubes by near edge X-ray absorption technique
journal, October 2015

Experimental Observation of Redox-Induced Fe–N Switching Behavior as a Determinant Role for Oxygen Reduction Activity
journal, October 2015

Density functional theory study of the oxygen reduction reaction mechanism in a BN co-doped graphene electrocatalyst
journal, January 2014

  • Kattel, Shyam; Atanassov, Plamen; Kiefer, Boris
  • Journal of Materials Chemistry A, Vol. 2, Issue 26
  • DOI: 10.1039/c4ta01460j

Stability, Electronic and Magnetic Properties of In-Plane Defects in Graphene: A First-Principles Study
journal, March 2012

  • Kattel, Shyam; Atanassov, Plamen; Kiefer, Boris
  • The Journal of Physical Chemistry C, Vol. 116, Issue 14
  • DOI: 10.1021/jp2121609
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    Works referencing / citing this record:

    Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion
    journal, November 2019

    • Zhu, Yuanzhi; Sokolowski, Joshua; Song, Xiancheng
    • Advanced Energy Materials, Vol. 10, Issue 11
    • DOI: 10.1002/aenm.201902844

    Boosting the performance of the Fe–N–C catalyst for the oxygen reduction reaction by introducing single-walled carbon nanohorns as branches on carbon fibers
    journal, January 2019

    • Zhang, Jianshuo; Liu, Yang; Yu, Zhoubin
    • Journal of Materials Chemistry A, Vol. 7, Issue 40
    • DOI: 10.1039/c9ta08938a
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