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

Gokhale, Rohan; Tsui, Lok-Kun; Roach, Kristin; Chen, Yechuan; Hossen, Md Mosaddek; Artyushkova, Kateryna; Garzon, Fernando; Atanassov, Plamen

doi:10.1002/celc.201700949

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

Journal Article · Thu Dec 07 00:00:00 EST 2017 · ChemElectroChem

DOI:https://doi.org/10.1002/celc.201700949· OSTI ID:1411622

Gokhale, Rohan ^[1]; Tsui, Lok-Kun ^[1]; Roach, Kristin ^[1]; Chen, Yechuan ^[1]; Hossen, Md Mosaddek ^[1]; Artyushkova, Kateryna ^[1]; Garzon, Fernando ^[1]; Atanassov, Plamen ^[1]

Univ. of New Mexico, Albuquerque, NM (United States). Center for Micro-Engineered Materials (CMEM)

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.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1411622

Report Number(s):: SAND-2017-8565J; 656151; TRN: US1800257

Journal Information:: ChemElectroChem, Vol. 5, Issue 14; ISSN 2196-0216

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 8 works

Citation information provided by
Web of Science

References (40)

Electrocatalytic activity of nitrogen-doped graphene synthesized via a one-pot hydrothermal process towards oxygen reduction reaction Wu, Jiajia; Zhang, Dun; Wang, Yi Journal of Power Sources, Vol. 227 https://doi.org/10.1016/j.jpowsour.2012.11.074	journal	April 2013
3D Nitrogen-Doped Graphene Aerogel-Supported Fe ₃ O ₄ Nanoparticles as Efficient Electrocatalysts for the Oxygen Reduction Reaction Wu, Zhong-Shuai; Yang, Shubin; Sun, Yi Journal of the American Chemical Society, Vol. 134, Issue 22 https://doi.org/10.1021/ja3030565	journal	May 2012
Direct Methanol Anion Exchange Membrane Fuel Cell with a Non-Platinum Group Metal Cathode based on Iron-Aminoantipyrine Catalyst Janarthanan, Rajeswari; Serov, Alexey; Pilli, Satyananda Kishore Electrochimica Acta, Vol. 175 https://doi.org/10.1016/j.electacta.2015.03.209	journal	September 2015
Recent Advances in Electrocatalysts for Oxygen Reduction Reaction Shao, Minhua; Chang, Qiaowan; Dodelet, Jean-Pol Chemical Reviews, Vol. 116, Issue 6 https://doi.org/10.1021/acs.chemrev.5b00462	journal	February 2016
Synthesis of nitrogen doped graphene with high electrocatalytic activity toward oxygen reduction reaction Zheng, Bo; Wang, Jiong; Wang, Feng-Bin Electrochemistry Communications, Vol. 28 https://doi.org/10.1016/j.elecom.2012.11.037	journal	March 2013
Growth of fcc Fe films on diamond Pappas, D. P.; Glesener, J. W.; Harris, V. G. Applied Physics Letters, Vol. 64, Issue 1 https://doi.org/10.1063/1.110910	journal	January 1994
Hydrothermal Synthesis of Metal-Polyphenol Coordination Crystals and Their Derived Metal/N-doped Carbon Composites for Oxygen Electrocatalysis Wei, Jing; Liang, Yan; Hu, Yaoxin Angewandte Chemie International Edition, Vol. 55, Issue 40 https://doi.org/10.1002/anie.201606327	journal	September 2016
The influence of pore size distribution on the oxygen reduction reaction performance in nitrogen doped carbon microspheres Ferrero, G. A.; Preuss, K.; Fuertes, A. B. Journal of Materials Chemistry A, Vol. 4, Issue 7 https://doi.org/10.1039/C5TA10063A	journal	January 2016
Soy protein directed hydrothermal synthesis of porous carbon aerogels for electrocatalytic oxygen reduction Alatalo, Sara-Maaria; Qiu, Kaipei; Preuss, Kathrin Carbon, Vol. 96 https://doi.org/10.1016/j.carbon.2015.09.108	journal	January 2016
Crystallite growth in graphitizing and non-graphitizing carbons Franklin, Rosalind E. Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 209, Issue 1097, p. 196-218 https://doi.org/10.1098/rspa.1951.0197	journal	October 1951
Novel dual templating approach for preparation of highly active Fe-N-C electrocatalyst for oxygen reduction Gokhale, Rohan; Chen, Yechuan; Serov, Alexey Electrochimica Acta, Vol. 224 https://doi.org/10.1016/j.electacta.2016.12.052	journal	January 2017
Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis Chen, Yechuan; Gokhale, Rohan; Serov, Alexey Nano Energy, Vol. 38 https://doi.org/10.1016/j.nanoen.2017.05.059	journal	August 2017
Sustainable Hydrothermal Carbonization Synthesis of Iron/Nitrogen-Doped Carbon Nanofiber Aerogels as Electrocatalysts for Oxygen Reduction Song, Lu-Ting; Wu, Zhen-Yu; Zhou, Fei Small, Vol. 12, Issue 46 https://doi.org/10.1002/smll.201602334	journal	September 2016
Graphene/nitrogen-doped porous carbon sandwiches for the metal-free oxygen reduction reaction: conductivity versus active sites Qiao, M.; Tang, C.; He, G. Journal of Materials Chemistry A, Vol. 4, Issue 32 https://doi.org/10.1039/C6TA04578B	journal	January 2016
Highly Efficient Oxygen Reduction Catalysts by Rational Synthesis of Nanoconfined Maghemite in a Nitrogen-Doped Graphene Framework Qiu, Kaipei; Chai, Guoliang; Jiang, Chaoran ACS Catalysis, Vol. 6, Issue 6 https://doi.org/10.1021/acscatal.6b00531	journal	May 2016
Self-powered supercapacitive microbial fuel cell: The ultimate way of boosting and harvesting power Santoro, Carlo; Soavi, Francesca; Serov, Alexey Biosensors and Bioelectronics, Vol. 78 https://doi.org/10.1016/j.bios.2015.11.026	journal	April 2016
Influence of Inner- and Outer-Sphere Electron Transfer Mechanisms during Electrocatalysis of Oxygen Reduction in Alkaline Media Ramaswamy, Nagappan; Mukerjee, Sanjeev The Journal of Physical Chemistry C, Vol. 115, Issue 36 https://doi.org/10.1021/jp204680p	journal	August 2011
Critical thickness of single crystal fcc iron on diamond Hoff, H. A.; Waytena, G. L.; Glesener, J. W. Surface Science, Vol. 326, Issue 3 https://doi.org/10.1016/0039-6028(94)00787-X	journal	March 1995
Low-temperature synthesis of nitrogen/sulfur co-doped three-dimensional graphene frameworks as efficient metal-free electrocatalyst for oxygen reduction reaction Su, Yuezeng; Zhang, Yi; Zhuang, Xiaodong Carbon, Vol. 62 https://doi.org/10.1016/j.carbon.2013.05.067	journal	October 2013
High Performance and Cost-Effective Direct Methanol Fuel Cells: Fe-N-C Methanol-Tolerant Oxygen Reduction Reaction Catalysts Sebastián, David; Serov, Alexey; Artyushkova, Kateryna ChemSusChem, Vol. 9, Issue 15 https://doi.org/10.1002/cssc.201600583	journal	July 2016
Direct synthesis of platinum group metal-free Fe-N-C catalyst for oxygen reduction reaction in alkaline media Gokhale, Rohan; Chen, Yechuan; Serov, Alexey Electrochemistry Communications, Vol. 72 https://doi.org/10.1016/j.elecom.2016.09.013	journal	November 2016
Synthesis and characterization of nitrogen-doped graphene hydrogels by hydrothermal route with urea as reducing-doping agents Guo, Hui-Lin; Su, Peng; Kang, Xiaofeng J. Mater. Chem. A, Vol. 1, Issue 6 https://doi.org/10.1039/C2TA00887D	journal	January 2013
Highly active oxygen reduction non-platinum group metal electrocatalyst without direct metal–nitrogen coordination Strickland, Kara; Miner, Elise; Jia, Qingying Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8343	journal	June 2015
Platinum group metal-free electrocatalysts: Effects of synthesis on structure and performance in proton-exchange membrane fuel cell cathodes Workman, Michael J.; Dzara, Michael; Ngo, Chilan Journal of Power Sources, Vol. 348 https://doi.org/10.1016/j.jpowsour.2017.02.067	journal	April 2017
A one-pot hydrothermal synthesis of sulfur and nitrogen doped carbon aerogels with enhanced electrocatalytic activity in the oxygen reduction reaction Wohlgemuth, Stephanie-Angelika; White, Robin Jeremy; Willinger, Marc-Georg Green Chemistry, Vol. 14, Issue 5 https://doi.org/10.1039/c2gc35309a	journal	January 2012
Fe-N-C Oxygen Reduction Fuel Cell Catalyst Derived from Carbendazim: Synthesis, Structure, and Reactivity Serov, Alexey; Artyushkova, Kateryna; Atanassov, Plamen Advanced Energy Materials, Vol. 4, Issue 10 https://doi.org/10.1002/aenm.201301735	journal	March 2014
Performance analysis of a non-platinum group metal catalyst based on iron-aminoantipyrine for direct methanol fuel cells Sebastián, David; Baglio, Vincenzo; Aricò, Antonino S. Applied Catalysis B: Environmental, Vol. 182 https://doi.org/10.1016/j.apcatb.2015.09.043	journal	March 2016
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt Wu, G.; More, K. L.; Johnston, C. M. Science, Vol. 332, Issue 6028, p. 443-447 https://doi.org/10.1126/science.1200832	journal	April 2011
Cobalt-Containing Nitrogen-Doped Carbon Aerogels as Efficient Electrocatalysts for the Oxygen Reduction Reaction Kreek, Kristiina; Sarapuu, Ave; Samolberg, Lars ChemElectroChem, Vol. 2, Issue 12 https://doi.org/10.1002/celc.201500275	journal	September 2015
Efficient Metal-Free Oxygen Reduction in Alkaline Medium on High-Surface-Area Mesoporous Nitrogen-Doped Carbons Made from Ionic Liquids and Nucleobases Yang, Wen; Fellinger, Tim-Patrick; Antonietti, Markus Journal of the American Chemical Society, Vol. 133, Issue 2, p. 206-209 https://doi.org/10.1021/ja108039j	journal	January 2011
Chemistry of Multitudinous Active Sites for Oxygen Reduction Reaction in Transition Metal–Nitrogen–Carbon Electrocatalysts Artyushkova, Kateryna; Serov, Alexey; Rojas-Carbonell, Santiago The Journal of Physical Chemistry C, Vol. 119, Issue 46 https://doi.org/10.1021/acs.jpcc.5b07653	journal	November 2015
Mechanistic Insight into Oxide-Promoted Palladium Catalysts for the Electro-Oxidation of Ethanol Martinez, Ulises; Serov, Alexey; Padilla, Monica ChemSusChem, Vol. 7, Issue 8 https://doi.org/10.1002/cssc.201402062	journal	July 2014
Facile fabrication of N-doped three-dimensional reduced graphene oxide as a superior electrocatalyst for oxygen reduction reaction Li, Yi; Yang, Juan; Zhao, Na Applied Catalysis A: General, Vol. 534 https://doi.org/10.1016/j.apcata.2017.01.014	journal	March 2017
Structure of C-stabilized fcc Fe on diamond: Epitaxial growth of austenite Swineford, R. S.; Pappas, D. P.; Harris, V. G. Physical Review B, Vol. 52, Issue 11 https://doi.org/10.1103/PhysRevB.52.7890	journal	September 1995
Cobalt- and iron-containing nitrogen-doped carbon aerogels as non-precious metal catalysts for electrochemical reduction of oxygen Sarapuu, Ave; Samolberg, Lars; Kreek, Kristiina Journal of Electroanalytical Chemistry, Vol. 746 https://doi.org/10.1016/j.jelechem.2015.03.021	journal	June 2015
Electrocatalysis of oxygen reduction by iron-containing nitrogen-doped carbon aerogels in alkaline solution Sarapuu, Ave; Kreek, Kristiina; Kisand, Kaarel Electrochimica Acta, Vol. 230 https://doi.org/10.1016/j.electacta.2017.01.157	journal	March 2017
Structure-refinement program for disordered carbons Shi, H.; Reimers, J. N.; Dahn, J. R. Journal of Applied Crystallography, Vol. 26, Issue 6 https://doi.org/10.1107/S0021889893003784	journal	December 1993
Structural and magnetic phases of ultrathin Fe wedges and films grown on diamond (100) Li, Dongqi; Keavney, D. J.; Pearson, J. Physical Review B, Vol. 57, Issue 16 https://doi.org/10.1103/PhysRevB.57.10044	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 Gokhale, Rohan; Unni, Sreekuttan M.; Puthusseri, Dhanya Physical Chemistry Chemical Physics, Vol. 16, Issue 9 https://doi.org/10.1039/c3cp55396e	journal	January 2014
Hydrothermal Synthesis of Metal-Polyphenol Coordination Crystals and Their Derived Metal/N-doped Carbon Composites for Oxygen Electrocatalysis Wei, Jing; Liang, Yan; Hu, Yaoxin Angewandte Chemie, Vol. 128, Issue 40 https://doi.org/10.1002/ange.201606327	journal	September 2016

Cited By (1)

Active‐Site Imprinting: Preparation of Fe–N–C Catalysts from Zinc Ion–Templated Ionothermal Nitrogen‐Doped Carbons Menga, Davide; Ruiz‐Zepeda, Francisco; Moriau, Léonard Advanced Energy Materials, Vol. 9, Issue 43 https://doi.org/10.1002/aenm.201902412	journal	September 2019

Similar Records

Impacts of Imidazolate Ligand on Performance of Zeolitic-Imidazolate Framework-Derived Oxygen Reduction Catalysts

Journal Article · Thu Sep 19 00:00:00 EDT 2019 · ACS Energy Letters · OSTI ID:1411622

Wang, Hao; Grabstanowicz, Lauren R.; Barkholtz, Heather M.; +5 more

Development of Novel Non-Pt Group Metal Electrocatalysts for PEM Fuel Cell Applications

Technical Report · Mon Jan 04 00:00:00 EST 2016 · OSTI ID:1411622

Mukerjee, Sanjeev; Atanassov, Plamen; Barton, Scott; +2 more

PGM-Free Oxygen-Reduction Catalyst Development for Proton-Exchange Membrane Fuel Cells: Challenges, Solutions, and Promises

Journal Article · Thu Jan 20 00:00:00 EST 2022 · Accounts of Materials Research · OSTI ID:1411622

He, Yanghua; Wu, Gang

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Hydrothermal synthesis
imidazole
FCC iron nanoparticles
graphitic lattices
oxygen reduction reaction

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

Citation Formats

References (40)

Cited By (1)

Similar Records

Related Subjects