Nano-nitride Cathode Catalysts of Ti, Ta, and Nb for Polymer Electrolyte Fuel Cells: Temperature-Programmed Desorption Investigation of Molecularly Adsorbed Oxygen at Low Temperature

TiN, NbN, TaN, and Ta3N5 nanoparticles synthesized using mesoporous graphitic (mpg)-C3N4 templates were investigated for the oxygen reduction reaction (ORR) as cathode catalysts for polymer electrolyte fuel cells. The temperature-programmed desorption (TPD) of molecularly adsorbed O2 at 120–170 K from these nanoparticles was examined, and the resulting amount and temperature of desorption were key factors determining the ORR activity. The size-dependent TiN nanoparticles (5–8 and 100 nm) were then examined. With decreasing particle size, the density of molecularly adsorbed O2 per unit of surface area increased, indicating that a decrease in particle size increases the number of active sites. It is hard to determine the electrochemical active surface area for nonmetal electrocatalysts (such as oxides or nitrides), because of the absence of proton adsorption/desorption peaks in the voltammograms. In this study, O2-TPD for molecularly adsorbed O2 at low temperature demonstrated that the amount and strength o...

[1]  Shuqin Song,et al.  Low and non-platinum electrocatalysts for PEMFCs: Current status, challenges and prospects , 2012 .

[2]  K. Domen,et al.  Highly-dispersed Ta-oxide catalysts prepared by electrodeposition in a non-aqueous plating bath for polymer electrolyte fuel cell cathodes. , 2012, Chemical communications.

[3]  P. He,et al.  Nano- and micro-sized TiN as the electrocatalysts for ORR in Li–air fuel cell with alkaline aqueous electrolyte , 2012 .

[4]  S. Woo,et al.  Binary and ternary doping of nitrogen, boron, and phosphorus into carbon for enhancing electrochemical oxygen reduction activity. , 2012, ACS nano.

[5]  M. Willinger,et al.  A one-pot hydrothermal synthesis of sulfur and nitrogen doped carbon aerogels with enhanced electrocatalytic activity in the oxygen reduction reaction , 2012 .

[6]  P. Jégou,et al.  Metal-free nitrogen-containing carbon nanotubes prepared from triazole and tetrazole derivatives show high electrocatalytic activity towards the oxygen reduction reaction in alkaline media. , 2012, ChemSusChem.

[7]  K. Domen,et al.  Composite of TiN nanoparticles and few-walled carbon nanotubes and its application to the electrocatalytic oxygen reduction reaction. , 2012, Chemistry, an Asian journal.

[8]  Gang Wu,et al.  High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt , 2011, Science.

[9]  Bruno Jousselme,et al.  Low-platinum and platinum-free catalysts for the oxygen reduction reaction at fuel cell cathodes , 2011 .

[10]  M. Antonietti,et al.  Synthesis of ordered porous graphitic-C3N4 and regularly arranged Ta3N5 nanoparticles by using self-assembled silica nanospheres as a primary template. , 2011, Chemistry, an Asian journal.

[11]  Masatoshi Suzuki,et al.  Oxygen reduction characteristics of several valve metal oxide electrodes in HClO4 solution , 2010 .

[12]  Egill Skúlason,et al.  The oxygen reduction reaction mechanism on Pt(111) from density functional theory calculations , 2010 .

[13]  M. Antonietti,et al.  Nano-sized TiN on carbon black as an efficient electrocatalyst for the oxygen reduction reaction prepared using an mpg-C3N4 template. , 2010, Chemical communications.

[14]  M. Matsumoto,et al.  Partially oxidized niobium carbonitride as a non-platinum catalyst for the reduction of oxygen in acidic medium , 2010 .

[15]  W. Sugimoto,et al.  Oxygen-reduction activity of silk-derived carbons , 2010 .

[16]  K. Domen,et al.  Improved catalytic performance of nitrided Co–Ti and Fe–Ti catalysts for oxygen reduction as non-noble metal cathodes in acidic media , 2010 .

[17]  K. Domen,et al.  Niobium-based catalysts prepared by reactive radio-frequency magnetron sputtering and arc plasma methods as non-noble metal cathode catalysts for polymer electrolyte fuel cells , 2010 .

[18]  K. Ota,et al.  Zirconium Oxide-Based Compound as New Cathode Without Platinum Group Metals for PEFC , 2010 .

[19]  M. Antonietti,et al.  Highly-active Tantalum (V) nitride nanoparticles prepared from a mesoporous carbon nitride template for photocatalytic hydrogen evolution under visible light irradiation , 2010 .

[20]  K. Domen,et al.  Polymerized Complex Synthesis of Niobium- and Zirconium-Based Electrocatalysts for PEFC Cathodes , 2010 .

[21]  Svitlana Pylypenko,et al.  Cross-laboratory experimental study of non-noble-metal electrocatalysts for the oxygen reduction reaction. , 2009, ACS applied materials & interfaces.

[22]  K. Domen,et al.  Highly Dispersed Niobium Catalyst on Carbon Black by Polymerized Complex Method as PEFC Cathode Catalyst , 2009 .

[23]  Frédéric Jaouen,et al.  Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells , 2009, Science.

[24]  F. Du,et al.  Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction , 2009, Science.

[25]  Kiyoyuki Terakura,et al.  X-ray absorption analysis of nitrogen contribution to oxygen reduction reaction in carbon alloy cathode catalysts for polymer electrolyte fuel cells , 2009 .

[26]  Jong-Won Lee,et al.  Development of high performance carbon composite catalyst for oxygen reduction reaction in PEM Proton Exchange Membrane fuel cells , 2008 .

[27]  K. Domen,et al.  Niobium Oxides as Cathode Electrocatalysts for Platinum-free Polymer Electrolyte Fuel Cells , 2008 .

[28]  Edmar P. Marques,et al.  A review of Fe-N/C and Co-N/C catalysts for the oxygen reduction reaction , 2008 .

[29]  K. Ota,et al.  Partially Oxidized Tantalum Carbonitrides as a New Nonplatinum Cathode for PEFC–1– , 2008 .

[30]  Mahlon Wilson,et al.  Scientific aspects of polymer electrolyte fuel cell durability and degradation. , 2007, Chemical reviews.

[31]  Ashin Marin Thomas,et al.  Growth Confined by the Nitrogen Source: Synthesis of Pure Metal Nitride Nanoparticles in Mesoporous Graphitic Carbon Nitride , 2007 .

[32]  Piotr Zelenay,et al.  A class of non-precious metal composite catalysts for fuel cells , 2006, Nature.

[33]  T. Jacob.  The Mechanism of Forming H2O from H2 and O2 over a Pt Catalyst via Direct Oxygen Reduction , 2006 .

[34]  Ping Yu,et al.  PtCo/C cathode catalyst for improved durability in PEMFCs , 2005 .

[35]  K. Domen,et al.  Tantalum Oxynitride for a Novel Cathode of PEFC , 2005 .

[36]  H. Gasteiger,et al.  Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs , 2005 .

[37]  A. Anderson,et al.  Activation energies for oxygen reduction on platinum alloys: theory and experiment. , 2005, The journal of physical chemistry. B.

[38]  H. Jónsson,et al.  Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode , 2004 .

[39]  Philip N. Ross,et al.  Oxygen Reduction Reaction on Pt and Pt Bimetallic Surfaces: A Selective Review , 2001 .

[40]  L. Carrette,et al.  Fuel Cells - Fundamentals and Applications , 2001 .

[41]  Hubert A. Gasteiger,et al.  Kinetics of the Selective CO Oxidation in H2-Rich Gas on Pt/Al2O3☆ , 1997 .

[42]  M. Niwa,et al.  Determination of the Acidic Properties of Zeolite by Theoretical Analysis of Temperature-Programmed Desorption of Ammonia Based on Adsorption Equilibrium , 1997 .

[43]  Shuichi Kagawa,et al.  Removal of nitrogen monoxide through a novel catalytic process. 1. Decomposition on excessively copper-ion-exchanged ZSM-5 zeolites , 1991 .

[44]  J. Niemantsverdriet,et al.  THERMAL DESORPTION ANALYSIS: COMPARATIVE TEST OF TEN COMMONLY APPLIED PROCEDURES , 1990 .

[45]  G. Fisher,et al.  Oxygen interactions with the Pt(111) surface , 1980 .

[46]  J. Gland.  Molecular and atomic adsorption of oxygen on the Pt(111) and Pt(S)-12(111) × (111) surfaces , 1980 .

[47]  R. Jasinski,et al.  A New Fuel Cell Cathode Catalyst , 1964, Nature.

[48]  P. Redhead.  Thermal desorption of gases , 1962 .

[49]  Piotr Zelenay,et al.  Recent advances in non-precious metal catalysis for oxygen-reduction reaction in polymer electrolyte fuel cells , 2011 .

[50]  K. Domen,et al.  Electrocatalytic Activity and Stability of M-Fe Catalysts Synthesized by Polymer Complex Method for PEFC Cathode , 2011 .

[51]  Matthew Neurock,et al.  First-Principles Analysis of the Initial Electroreduction Steps of Oxygen over Pt(111) , 2009 .

[52]  Ernest Yeager,et al.  Heat-treated polyacrylonitrile-based catalysts for oxygen electroreduction , 1989 .