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:
-
- 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.
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
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.
@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}
}
Web of Science
Works referenced in this record:
Electrocatalytic activity of nitrogen-doped graphene synthesized via a one-pot hydrothermal process towards oxygen reduction reaction
journal, April 2013
- Wu, Jiajia; Zhang, Dun; Wang, Yi
- Journal of Power Sources, Vol. 227
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
Direct Methanol Anion Exchange Membrane Fuel Cell with a Non-Platinum Group Metal Cathode based on Iron-Aminoantipyrine Catalyst
journal, September 2015
- Janarthanan, Rajeswari; Serov, Alexey; Pilli, Satyananda Kishore
- Electrochimica Acta, Vol. 175
Recent Advances in Electrocatalysts for Oxygen Reduction Reaction
journal, February 2016
- Shao, Minhua; Chang, Qiaowan; Dodelet, Jean-Pol
- Chemical Reviews, Vol. 116, Issue 6
Synthesis of nitrogen doped graphene with high electrocatalytic activity toward oxygen reduction reaction
journal, March 2013
- Zheng, Bo; Wang, Jiong; Wang, Feng-Bin
- Electrochemistry Communications, Vol. 28
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
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
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
Soy protein directed hydrothermal synthesis of porous carbon aerogels for electrocatalytic oxygen reduction
journal, January 2016
- Alatalo, Sara-Maaria; Qiu, Kaipei; Preuss, Kathrin
- Carbon, Vol. 96
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
Novel dual templating approach for preparation of highly active Fe-N-C electrocatalyst for oxygen reduction
journal, January 2017
- Gokhale, Rohan; Chen, Yechuan; Serov, Alexey
- Electrochimica Acta, Vol. 224
Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis
journal, August 2017
- Chen, Yechuan; Gokhale, Rohan; Serov, Alexey
- Nano Energy, Vol. 38
Sustainable Hydrothermal Carbonization Synthesis of Iron/Nitrogen-Doped Carbon Nanofiber Aerogels as Electrocatalysts for Oxygen Reduction
journal, September 2016
- Song, Lu-Ting; Wu, Zhen-Yu; Zhou, Fei
- Small, Vol. 12, Issue 46
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
Highly Efficient Oxygen Reduction Catalysts by Rational Synthesis of Nanoconfined Maghemite in a Nitrogen-Doped Graphene Framework
journal, May 2016
- Qiu, Kaipei; Chai, Guoliang; Jiang, Chaoran
- ACS Catalysis, Vol. 6, Issue 6
Self-powered supercapacitive microbial fuel cell: The ultimate way of boosting and harvesting power
journal, April 2016
- Santoro, Carlo; Soavi, Francesca; Serov, Alexey
- Biosensors and Bioelectronics, Vol. 78
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
Critical thickness of single crystal fcc iron on diamond
journal, March 1995
- Hoff, H. A.; Waytena, G. L.; Glesener, J. W.
- Surface Science, Vol. 326, Issue 3
Low-temperature synthesis of nitrogen/sulfur co-doped three-dimensional graphene frameworks as efficient metal-free electrocatalyst for oxygen reduction reaction
journal, October 2013
- Su, Yuezeng; Zhang, Yi; Zhuang, Xiaodong
- Carbon, Vol. 62
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
Direct synthesis of platinum group metal-free Fe-N-C catalyst for oxygen reduction reaction in alkaline media
journal, November 2016
- Gokhale, Rohan; Chen, Yechuan; Serov, Alexey
- Electrochemistry Communications, Vol. 72
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
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
Platinum group metal-free electrocatalysts: Effects of synthesis on structure and performance in proton-exchange membrane fuel cell cathodes
journal, April 2017
- Workman, Michael J.; Dzara, Michael; Ngo, Chilan
- Journal of Power Sources, Vol. 348
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
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
Performance analysis of a non-platinum group metal catalyst based on iron-aminoantipyrine for direct methanol fuel cells
journal, March 2016
- Sebastián, David; Baglio, Vincenzo; Aricò, Antonino S.
- Applied Catalysis B: Environmental, Vol. 182
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
journal, April 2011
- Wu, G.; More, K. L.; Johnston, C. M.
- Science, Vol. 332, Issue 6028, p. 443-447
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
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
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
Mechanistic Insight into Oxide-Promoted Palladium Catalysts for the Electro-Oxidation of Ethanol
journal, July 2014
- Martinez, Ulises; Serov, Alexey; Padilla, Monica
- ChemSusChem, Vol. 7, Issue 8
Facile fabrication of N-doped three-dimensional reduced graphene oxide as a superior electrocatalyst for oxygen reduction reaction
journal, March 2017
- Li, Yi; Yang, Juan; Zhao, Na
- Applied Catalysis A: General, Vol. 534
Structure of C-stabilized fcc Fe on diamond: Epitaxial growth of austenite
journal, September 1995
- Swineford, R. S.; Pappas, D. P.; Harris, V. G.
- Physical Review B, Vol. 52, Issue 11
Cobalt- and iron-containing nitrogen-doped carbon aerogels as non-precious metal catalysts for electrochemical reduction of oxygen
journal, June 2015
- Sarapuu, Ave; Samolberg, Lars; Kreek, Kristiina
- Journal of Electroanalytical Chemistry, Vol. 746
Electrocatalysis of oxygen reduction by iron-containing nitrogen-doped carbon aerogels in alkaline solution
journal, March 2017
- Sarapuu, Ave; Kreek, Kristiina; Kisand, Kaarel
- Electrochimica Acta, Vol. 230
Structure-refinement program for disordered carbons
journal, December 1993
- Shi, H.; Reimers, J. N.; Dahn, J. R.
- Journal of Applied Crystallography, Vol. 26, Issue 6
Structural and magnetic phases of ultrathin Fe wedges and films grown on diamond (100)
journal, April 1998
- Li, Dongqi; Keavney, D. J.; Pearson, J.
- Physical Review B, Vol. 57, Issue 16
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
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, Vol. 128, Issue 40
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