Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Hydrothermal Synthesis of Platinum-Group-Metal-Free Catalysts: Structural Elucidation and Oxygen Reduction Catalysis

Abstract

In this paper, a hydrothermal approach to generate a platinum-group-metal-free (PGM-free) Fe-N-C catalyst for the oxygen reduction reaction (ORR) is introduced. The process involves partial carbonization by hydrothermal means followed by thermal treatment to obtain the final catalysts. Detailed X-ray scattering analysis of the glucose-imidazole catalysts (termed as GLU-IMID-C catalysts), obtained for the first time with the use of CarbonXS GUI program, reveals the presence of face-centered cubic (FCC) iron nanoparticles embedded in partially graphitic carbon in all catalyst variations. We also report the physical characterization of these catalysts by using X-ray photoelectron spectroscopy, Brunauer-Emmett-Teller surface area analysis, and transmission electron microscopy. The electrocatalytic behavior of the catalysts towards oxygen reduction is studied separately in acidic and alkaline electrolytes by rotating ring disk electrode measurements. The catalysts exhibit high ORR activity in acidic (0.5 M H2SO4) and alkaline (0.1 M KOH) electrolytes. Lastly, a precursor structure-performance relationship of these catalysts and their performance trends in both electrolytes has been discussed in this work.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
+ Show Author Affiliations
  1. Univ. of New Mexico, Albuquerque, NM (United States). Center for Micro-Engineered Materials (CMEM)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1411622
Report Number(s):
SAND-2017-8565J
Journal ID: ISSN 2196-0216; 656151; TRN: US1800257
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
ChemElectroChem
Additional Journal Information:
Journal Volume: 5; Journal Issue: 14; Journal ID: ISSN 2196-0216
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Hydrothermal synthesis; imidazole; FCC iron nanoparticles; graphitic lattices; oxygen reduction reaction

Citation Formats

Gokhale, Rohan, Tsui, Lok-Kun, Roach, Kristin, Chen, Yechuan, Hossen, Md Mosaddek, Artyushkova, Kateryna, Garzon, Fernando, and Atanassov, Plamen. Hydrothermal Synthesis of Platinum-Group-Metal-Free Catalysts: Structural Elucidation and Oxygen Reduction Catalysis. United States: N. p., 2017. Web. doi:10.1002/celc.201700949.
Copy to clipboard
Gokhale, Rohan, Tsui, Lok-Kun, Roach, Kristin, Chen, Yechuan, Hossen, Md Mosaddek, Artyushkova, Kateryna, Garzon, Fernando, & Atanassov, Plamen. Hydrothermal Synthesis of Platinum-Group-Metal-Free Catalysts: Structural Elucidation and Oxygen Reduction Catalysis. United States. https://doi.org/10.1002/celc.201700949
Copy to clipboard
Gokhale, Rohan, Tsui, Lok-Kun, Roach, Kristin, Chen, Yechuan, Hossen, Md Mosaddek, Artyushkova, Kateryna, Garzon, Fernando, and Atanassov, Plamen. Thu . "Hydrothermal Synthesis of Platinum-Group-Metal-Free Catalysts: Structural Elucidation and Oxygen Reduction Catalysis". United States. https://doi.org/10.1002/celc.201700949. https://www.osti.gov/servlets/purl/1411622.
Copy to clipboard
@article{osti_1411622,
title = {Hydrothermal Synthesis of Platinum-Group-Metal-Free Catalysts: Structural Elucidation and Oxygen Reduction Catalysis},
author = {Gokhale, Rohan and Tsui, Lok-Kun and Roach, Kristin and Chen, Yechuan and Hossen, Md Mosaddek and Artyushkova, Kateryna and Garzon, Fernando and Atanassov, Plamen},
abstractNote = {In this paper, a hydrothermal approach to generate a platinum-group-metal-free (PGM-free) Fe-N-C catalyst for the oxygen reduction reaction (ORR) is introduced. The process involves partial carbonization by hydrothermal means followed by thermal treatment to obtain the final catalysts. Detailed X-ray scattering analysis of the glucose-imidazole catalysts (termed as GLU-IMID-C catalysts), obtained for the first time with the use of CarbonXS GUI program, reveals the presence of face-centered cubic (FCC) iron nanoparticles embedded in partially graphitic carbon in all catalyst variations. We also report the physical characterization of these catalysts by using X-ray photoelectron spectroscopy, Brunauer-Emmett-Teller surface area analysis, and transmission electron microscopy. The electrocatalytic behavior of the catalysts towards oxygen reduction is studied separately in acidic and alkaline electrolytes by rotating ring disk electrode measurements. The catalysts exhibit high ORR activity in acidic (0.5 M H2SO4) and alkaline (0.1 M KOH) electrolytes. Lastly, a precursor structure-performance relationship of these catalysts and their performance trends in both electrolytes has been discussed in this work.},
doi = {10.1002/celc.201700949},
journal = {ChemElectroChem},
number = 14,
volume = 5,
place = {United States},
year = {Thu Dec 07 00:00:00 EST 2017},
month = {Thu Dec 07 00:00:00 EST 2017}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/celc.201700949
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

3D Nitrogen-Doped Graphene Aerogel-Supported Fe 3 O 4 Nanoparticles as Efficient Electrocatalysts for the Oxygen Reduction Reaction
journal, May 2012

  • Wu, Zhong-Shuai; Yang, Shubin; Sun, Yi
  • Journal of the American Chemical Society, Vol. 134, Issue 22
  • DOI: 10.1021/ja3030565

Direct Methanol Anion Exchange Membrane Fuel Cell with a Non-Platinum Group Metal Cathode based on Iron-Aminoantipyrine Catalyst
journal, September 2015

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

Synthesis of nitrogen doped graphene with high electrocatalytic activity toward oxygen reduction reaction
journal, March 2013

Growth of fcc Fe films on diamond
journal, January 1994

  • Pappas, D. P.; Glesener, J. W.; Harris, V. G.
  • Applied Physics Letters, Vol. 64, Issue 1
  • DOI: 10.1063/1.110910

Hydrothermal Synthesis of Metal-Polyphenol Coordination Crystals and Their Derived Metal/N-doped Carbon Composites for Oxygen Electrocatalysis
journal, September 2016

  • Wei, Jing; Liang, Yan; Hu, Yaoxin
  • Angewandte Chemie International Edition, Vol. 55, Issue 40
  • DOI: 10.1002/anie.201606327

The influence of pore size distribution on the oxygen reduction reaction performance in nitrogen doped carbon microspheres
journal, January 2016

  • Ferrero, G. A.; Preuss, K.; Fuertes, A. B.
  • Journal of Materials Chemistry A, Vol. 4, Issue 7
  • DOI: 10.1039/C5TA10063A

Soy protein directed hydrothermal synthesis of porous carbon aerogels for electrocatalytic oxygen reduction
journal, January 2016

Crystallite growth in graphitizing and non-graphitizing carbons
journal, October 1951

  • Franklin, Rosalind E.
  • Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 209, Issue 1097, p. 196-218
  • DOI: 10.1098/rspa.1951.0197

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

Graphene/nitrogen-doped porous carbon sandwiches for the metal-free oxygen reduction reaction: conductivity versus active sites
journal, January 2016

  • Qiao, M.; Tang, C.; He, G.
  • Journal of Materials Chemistry A, Vol. 4, Issue 32
  • DOI: 10.1039/C6TA04578B

Self-powered supercapacitive microbial fuel cell: The ultimate way of boosting and harvesting power
journal, April 2016

Influence of Inner- and Outer-Sphere Electron Transfer Mechanisms during Electrocatalysis of Oxygen Reduction in Alkaline Media
journal, August 2011

  • Ramaswamy, Nagappan; Mukerjee, Sanjeev
  • The Journal of Physical Chemistry C, Vol. 115, Issue 36
  • DOI: 10.1021/jp204680p

Critical thickness of single crystal fcc iron on diamond
journal, March 1995

High Performance and Cost-Effective Direct Methanol Fuel Cells: Fe-N-C Methanol-Tolerant Oxygen Reduction Reaction Catalysts
journal, July 2016

  • Sebastián, David; Serov, Alexey; Artyushkova, Kateryna
  • ChemSusChem, Vol. 9, Issue 15
  • DOI: 10.1002/cssc.201600583

Direct synthesis of platinum group metal-free Fe-N-C catalyst for oxygen reduction reaction in alkaline media
journal, November 2016

Synthesis and characterization of nitrogen-doped graphene hydrogels by hydrothermal route with urea as reducing-doping agents
journal, January 2013

  • Guo, Hui-Lin; Su, Peng; Kang, Xiaofeng
  • J. Mater. Chem. A, Vol. 1, Issue 6
  • DOI: 10.1039/C2TA00887D

Highly active oxygen reduction non-platinum group metal electrocatalyst without direct metal–nitrogen coordination
journal, June 2015

  • Strickland, Kara; Miner, Elise; Jia, Qingying
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8343

A one-pot hydrothermal synthesis of sulfur and nitrogen doped carbon aerogels with enhanced electrocatalytic activity in the oxygen reduction reaction
journal, January 2012

  • Wohlgemuth, Stephanie-Angelika; White, Robin Jeremy; Willinger, Marc-Georg
  • Green Chemistry, Vol. 14, Issue 5
  • DOI: 10.1039/c2gc35309a

Fe-N-C Oxygen Reduction Fuel Cell Catalyst Derived from Carbendazim: Synthesis, Structure, and Reactivity
journal, March 2014

  • Serov, Alexey; Artyushkova, Kateryna; Atanassov, Plamen
  • Advanced Energy Materials, Vol. 4, Issue 10
  • DOI: 10.1002/aenm.201301735

Performance analysis of a non-platinum group metal catalyst based on iron-aminoantipyrine for direct methanol fuel cells
journal, March 2016

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

Cobalt-Containing Nitrogen-Doped Carbon Aerogels as Efficient Electrocatalysts for the Oxygen Reduction Reaction
journal, September 2015

  • Kreek, Kristiina; Sarapuu, Ave; Samolberg, Lars
  • ChemElectroChem, Vol. 2, Issue 12
  • DOI: 10.1002/celc.201500275

Efficient Metal-Free Oxygen Reduction in Alkaline Medium on High-Surface-Area Mesoporous Nitrogen-Doped Carbons Made from Ionic Liquids and Nucleobases
journal, January 2011

  • Yang, Wen; Fellinger, Tim-Patrick; Antonietti, Markus
  • Journal of the American Chemical Society, Vol. 133, Issue 2, p. 206-209
  • DOI: 10.1021/ja108039j

Chemistry of Multitudinous Active Sites for Oxygen Reduction Reaction in Transition Metal–Nitrogen–Carbon Electrocatalysts
journal, November 2015

  • Artyushkova, Kateryna; Serov, Alexey; Rojas-Carbonell, Santiago
  • The Journal of Physical Chemistry C, Vol. 119, Issue 46
  • DOI: 10.1021/acs.jpcc.5b07653

Mechanistic Insight into Oxide-Promoted Palladium Catalysts for the Electro-Oxidation of Ethanol
journal, July 2014

Structure of C-stabilized fcc Fe on diamond: Epitaxial growth of austenite
journal, September 1995

Cobalt- and iron-containing nitrogen-doped carbon aerogels as non-precious metal catalysts for electrochemical reduction of oxygen
journal, June 2015

Electrocatalysis of oxygen reduction by iron-containing nitrogen-doped carbon aerogels in alkaline solution
journal, March 2017

Structure-refinement program for disordered carbons
journal, December 1993

Structural and magnetic phases of ultrathin Fe wedges and films grown on diamond (100)
journal, April 1998

Synthesis of an efficient heteroatom-doped carbon electro-catalyst for oxygen reduction reaction by pyrolysis of protein-rich pulse flour cooked with SiO2 nanoparticles
journal, January 2014

  • Gokhale, Rohan; Unni, Sreekuttan M.; Puthusseri, Dhanya
  • Physical Chemistry Chemical Physics, Vol. 16, Issue 9
  • DOI: 10.1039/c3cp55396e
    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Active‐Site Imprinting: Preparation of Fe–N–C Catalysts from Zinc Ion–Templated Ionothermal Nitrogen‐Doped Carbons
    journal, September 2019

    • Menga, Davide; Ruiz‐Zepeda, Francisco; Moriau, Léonard
    • Advanced Energy Materials, Vol. 9, Issue 43
    • DOI: 10.1002/aenm.201902412
      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: