Step-by-Step Synthesis of Non-Noble Metal Electrocatalysts for O2 Reduction under Proton Exchange Membrane Fuel Cell Conditions

Fe-based catalysts for O2 reduction under proton exchange membrane fuel cell conditions were prepared on a commercial N234 carbon black support using both a “classical” and a step-by-step procedure to determine if parameters other than microporosity and nitrogen loading of the carbon support are important in the synthesis of Fe/N/C electrocatalysts. The “classical” procedure for obtaining Fe/N/C electrocatalysts is to use a single-step synthesis, in which a carbon support loaded with a metal precursor is heat treated at high temperatures (900−950 °C) in pure NH3. In the step-by-step procedure, microporosity is first etched into the carbon support followed, if necessary, by the addition of N-bearing functionalities and, last, the loading of the metal precursor. Similar maximum microporous contents can be etched into N234, using either NH3 or O2 (air). However, unlike O2 (air), etching with NH3 has the added benefit of creating N-bearing functionalities on the carbon surface. For carbon supports etched in O...

[1]  A. Ōya,et al.  Structures, physicochemical properties and oxygen reduction activities of carbons derived from ferrocene-poly(furfuryl alcohol) mixtures , 2006 .

[2]  Soojin Park,et al.  Influence of plasma treatment of carbon blacks on electrochemical activity of Pt/carbon blacks catalysts for DMFCs , 2006 .

[3]  Frédéric Jaouen,et al.  Heat-treated Fe/N/C catalysts for O2 electroreduction: are active sites hosted in micropores? , 2006, The journal of physical chemistry. B.

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

[5]  H. Tributsch,et al.  Thermogravimetry/Mass Spectrometry Investigations on the Formation of Oxygen Reduction Catalysts for PEM Fuel Cells on the Basis of Heat‐Treated Iron Phenanthroline Complexes , 2002 .

[6]  E. Yeager,et al.  Transition metal macrocycles supported on high area carbon: pyrolysis-mass spectrometry studies , 1986 .

[7]  Frédéric Jaouen,et al.  Fe-Based Catalysts for Oxygen Reduction in PEMFCs Importance of the Disordered Phase of the Carbon Support , 2006 .

[8]  K. Sawai,et al.  Highly Active Nonplatinum Catalyst for Air Cathodes , 2004 .

[9]  K. Oyaizu,et al.  Modifying carbon particles with polypyrrole for adsorption of cobalt ions as electrocatatytic site for oxygen reduction , 2005 .

[10]  J. Maruyama,et al.  Fuel Cell Cathode Catalyst with Heme-Like Structure Formed from Nitrogen of Glycine and Iron , 2007 .

[11]  I. Abe,et al.  Formation of Platinum-Free Fuel Cell Cathode Catalyst with Highly Developed Nanospace by Carbonizing Catalase , 2005 .

[12]  K. Sasaki,et al.  Stabilization of Platinum Oxygen-Reduction Electrocatalysts Using Gold Clusters , 2007, Science.

[13]  A. Vijh,et al.  Cobalt-carbonized aerogel nanocomposites electrocatalysts for the oxygen reduction reaction , 2005 .

[14]  Frédéric Jaouen,et al.  Average turn-over frequency of O2 electro-reduction for Fe/N/C and Co/N/C catalysts in PEFCs , 2007 .

[15]  J. Dahn,et al.  Co – C – N Oxygen Reduction Catalysts Prepared by Combinatorial Magnetron Sputter Deposition , 2007 .

[16]  K. Stevenson,et al.  Influence of nitrogen doping on oxygen reduction electrocatalysis at carbon nanofiber electrodes. , 2005, The journal of physical chemistry. B.

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

[18]  Hubert A. Gasteiger,et al.  Oxygen reduction on a high-surface area Pt/Vulcan carbon catalyst: a thin-film rotating ring-disk electrode study , 2001 .

[19]  J. Amouroux,et al.  Surface modification of polyethylene powder by nitrogen and ammonia low pressure plasma in a fluidized bed reactor , 2004 .

[20]  Michel Lefèvre,et al.  Fe-based catalysts for the reduction of oxygen in polymer electrolyte membrane fuel cell conditions: determination of the amount of peroxide released during electroreduction and its influence on the stability of the catalysts , 2003 .

[21]  H. Tributsch Multi-electron transfer catalysis for energy conversion based on abundant transition metals , 2007 .

[22]  Philip N. Ross,et al.  Improved Oxygen Reduction Activity on Pt3Ni(111) via Increased Surface Site Availability , 2007, Science.

[23]  J. Dahn,et al.  Fe-C-N Oxygen Reduction Catalysts Prepared by Combinatorial Sputter Deposition , 2006 .

[24]  S. Marcotte,et al.  Oxygen Reduction Catalysts for Polymer Electrolyte Fuel Cells from the Pyrolysis of Iron Acetate Adsorbed on Various Carbon Supports , 2003 .

[25]  O. Antoine,et al.  RRDE study of oxygen reduction on Pt nanoparticles inside Nafion®: H2O2 production in PEMFC cathode conditions , 2000 .

[26]  Frédéric Jaouen,et al.  Non-Noble Electrocatalysts for O2 Reduction: How Does Heat Treatment Affect Their Activity and Structure? Part I. Model for Carbon Black Gasification by NH3: Parametric Calibration and Electrochemical Validation , 2007 .

[27]  Ruizhi Yang,et al.  Thermal Evolution of the Structure and Activity of Magnetron-Sputtered TM–C–N ( TM = Fe , Co ) Oxygen Reduction Catalysts , 2007 .

[28]  Göran Lindbergh,et al.  Oxygen reduction by Fe-based catalysts in PEM fuel cell conditions: Activity and selectivity of the catalysts obtained with two Fe precursors and various carbon supports , 2006 .

[29]  Umit S. Ozkan,et al.  The role of nanostructure in nitrogen-containing carbon catalysts for the oxygen reduction reaction , 2006 .

[30]  K. Oyaizu,et al.  Cobaltporphyrin‐adsorbed carbon black: highly efficient electrocatalysts for oxygen reduction , 2005 .

[31]  S. Campbell,et al.  Oxygen Reduction by Sol Derived [Co, N, C, O]-Based Catalysts for Use in Proton Exchange Membrane Fuel Cells , 2005 .

[32]  Volkmar M. Schmidt,et al.  Electrochemical characteristics and performance of CoTMPP/BP oxygen reduction electrocatalysts for PEM fuel cell , 2006 .

[33]  Soojin Park,et al.  Influence of plasma treatment on microstructures and acid-base surface energetics of nanostructured carbon blacks: N2 plasma environment , 2001 .

[34]  Alfred B. Anderson,et al.  O2 reduction on graphite and nitrogen-doped graphite: experiment and theory. , 2006, The journal of physical chemistry. B.

[35]  H. Tributsch,et al.  Catalysts for the Oxygen Reduction from Heat-Treated Iron(III) Tetramethoxyphenylporphyrin Chloride: Structure and Stability of Active Sites , 2003 .

[36]  B. Popov,et al.  Studies on Co-based catalysts supported on modified carbon substrates for PEMFC cathodes , 2006 .

[37]  Patrick Bertrand,et al.  Non-noble electrocatalysts for O-2 reduction: How does heat treatment affect their activity and structure? Part II. Structural changes observed by electron microscopy, Raman, and mass spectroscopy , 2007 .

[38]  J. Maruyama,et al.  Two-Step Carbonization as a Method of Enhancing Catalytic Properties of Hemoglobin at the Fuel Cell Cathode , 2007 .

[39]  Elizabeth J. Biddinger,et al.  Oxygen reduction reaction catalysts prepared from acetonitrile pyrolysis over alumina-supported metal particles. , 2006, The journal of physical chemistry. B.