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Title: Synthesis-Structure-Performance Correlation for Polyaniline-Me-C Non-Precious Metal Cathode Catalysts for Oxygen Reduction in Fuel Cells

Abstract

In this report, we present the systematic preparation of active and durable non-precious metal catalysts (NPMCs) for the oxygen reduction reaction in polymer electrolyte fuel cells (PEFCs) based on the heat treatment of polyaniline/metal/carbon precursors. Variation of the synthesis steps, heat-treatment temperature, metal loading, and the metal type in the synthesis leads to markedly different catalyst activity, speciation, and morphology. Microscopy studies demonstrate notable differences in the carbon structure as a function of these variables. Balancing the need to increase the catalyst's degree of graphitization through heat treatment versus the excessive loss of surface area that occurs at higher temperatures is a key to preparing an active catalyst. XPS and XAFS spectra are consistent with the presence of Me-N{sub x} structures in both the Co and Fe versions of the catalyst, which are often proposed to be active sites. The average speciation and coordination environment of nitrogen and metal, however, depends greatly on the choice of Co or Fe. Taken together, the data indicate that better control of the metal-catalyzed transformations of the polymer into new graphitized carbon forms in the heat-treatment step will allow for even further improvement of this class of catalysts.

Authors:
 [1];  [1];  [1];  [2];  [3];  [1];  [1];  [1];  [4];  [3];  [1]
  1. Los Alamos National Laboratory (LANL)
  2. University of New Mexico, Albuquerque
  3. Argonne National Laboratory (ANL)
  4. ORNL
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Shared Research Equipment Collaborative Research Center
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1024719
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Materials Chemistry; Journal Volume: 21; Journal Issue: 30
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; CARBON; CATALYSTS; CATHODES; FUEL CELLS; GRAPHITIZATION; HEAT TREATMENTS; MICROSCOPY; MORPHOLOGY; NITROGEN; OXYGEN; POLYMERS; PROTON EXCHANGE MEMBRANE FUEL CELLS; SPECTRA; SURFACE AREA; SYNTHESIS; TRANSFORMATIONS; X-RAY PHOTOELECTRON SPECTROSCOPY

Citation Formats

Wu, Gang, Johnston, Christina, Mack, Nathan, Artyushkova, Kateryna, Ferrandon, Magali, Nelson, Mark, Lezama-pacheco, Juan, Conradson, Steven, More, Karren Leslie, Myers, Deborah, and Zelenay, Piotr. Synthesis-Structure-Performance Correlation for Polyaniline-Me-C Non-Precious Metal Cathode Catalysts for Oxygen Reduction in Fuel Cells. United States: N. p., 2011. Web. doi:10.1039/c0jm03613g.
Wu, Gang, Johnston, Christina, Mack, Nathan, Artyushkova, Kateryna, Ferrandon, Magali, Nelson, Mark, Lezama-pacheco, Juan, Conradson, Steven, More, Karren Leslie, Myers, Deborah, & Zelenay, Piotr. Synthesis-Structure-Performance Correlation for Polyaniline-Me-C Non-Precious Metal Cathode Catalysts for Oxygen Reduction in Fuel Cells. United States. doi:10.1039/c0jm03613g.
Wu, Gang, Johnston, Christina, Mack, Nathan, Artyushkova, Kateryna, Ferrandon, Magali, Nelson, Mark, Lezama-pacheco, Juan, Conradson, Steven, More, Karren Leslie, Myers, Deborah, and Zelenay, Piotr. Sat . "Synthesis-Structure-Performance Correlation for Polyaniline-Me-C Non-Precious Metal Cathode Catalysts for Oxygen Reduction in Fuel Cells". United States. doi:10.1039/c0jm03613g.
@article{osti_1024719,
title = {Synthesis-Structure-Performance Correlation for Polyaniline-Me-C Non-Precious Metal Cathode Catalysts for Oxygen Reduction in Fuel Cells},
author = {Wu, Gang and Johnston, Christina and Mack, Nathan and Artyushkova, Kateryna and Ferrandon, Magali and Nelson, Mark and Lezama-pacheco, Juan and Conradson, Steven and More, Karren Leslie and Myers, Deborah and Zelenay, Piotr},
abstractNote = {In this report, we present the systematic preparation of active and durable non-precious metal catalysts (NPMCs) for the oxygen reduction reaction in polymer electrolyte fuel cells (PEFCs) based on the heat treatment of polyaniline/metal/carbon precursors. Variation of the synthesis steps, heat-treatment temperature, metal loading, and the metal type in the synthesis leads to markedly different catalyst activity, speciation, and morphology. Microscopy studies demonstrate notable differences in the carbon structure as a function of these variables. Balancing the need to increase the catalyst's degree of graphitization through heat treatment versus the excessive loss of surface area that occurs at higher temperatures is a key to preparing an active catalyst. XPS and XAFS spectra are consistent with the presence of Me-N{sub x} structures in both the Co and Fe versions of the catalyst, which are often proposed to be active sites. The average speciation and coordination environment of nitrogen and metal, however, depends greatly on the choice of Co or Fe. Taken together, the data indicate that better control of the metal-catalyzed transformations of the polymer into new graphitized carbon forms in the heat-treatment step will allow for even further improvement of this class of catalysts.},
doi = {10.1039/c0jm03613g},
journal = {Journal of Materials Chemistry},
number = 30,
volume = 21,
place = {United States},
year = {Sat Jan 01 00:00:00 EST 2011},
month = {Sat Jan 01 00:00:00 EST 2011}
}