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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]
  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.
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. doi: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. doi: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 = {2017},
month = {12}
}

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