Analyzing Structural Changes of Fe-N-C Cathode Catalysts in PEM Fuel Cell by Mossbauer Spectroscopy of Complete Membrane Electrode Assemblies

被引:88
作者
Kramm, Ulrike I. [1 ]
Lefevre, Michel [2 ]
Bogdanoff, Peter [3 ]
Schmeisser, Dieter [1 ]
Dodelet, Jean-Pol [4 ]
机构
[1] Brandenburg Tech Univ Cottbus Senftenberg, Chair Appl Phys & Sensors, D-03046 Cottbus, Germany
[2] Canet Electrocatalysis Inc, Varennes, PQ J3X 1S2, Canada
[3] Helmholtz Ctr Berlin Mat & Energy, D-14109 Berlin, Germany
[4] INRS Energie, Mat & Telecommun, Varennes, PQ J3X 1S2, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
OXYGEN REDUCTION REACTION; FE/N/C-CATALYSTS; IRON; CARBON; ELECTROCATALYSTS; DENSITY; SITES; POLYANILINE; ORR;
D O I
10.1021/jz501955g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The applicability of analyzing by MoBbauer spectroscopy the structural changes of Fe-N-C catalysts that have been tested at the cathode of membrane electrode assemblies in proton exchange membrane (PEM) fuel cells is demonstrated. The MoBbauer characterization of powders of the same catalysts was recently described in our previous publication. A possible change of the iron species upon testing in fuel cell was investigated here by MoBbauer spectroscopy, energy-dispersive X-ray cross-sectional imaging, and neutron activation analysis. Our results show that the absorption probability of gamma rays by the iron nuclei in Fe-N-C is strongly affected by the presence of Nafion and water content. A detailed investigation of the effect of an oxidizing treatment (1.2 V) of the non-noble cathode in PEM fuel cell indicates that the observed activity decay is mainly attributable to carbon oxidation causing a leaching of active iron sites hosted in the carbon matrix.
引用
收藏
页码:3750 / 3756
页数:7
相关论文
共 22 条
[1]   SIMULTANEOUS ELECTROCHEMICAL AND MOSSBAUER MEASUREMENTS ON POLYMERIC IRON PHTHALOCYANINE OXYGEN ELECTRODES [J].
BLOMQUIST, J ;
HELGESON, U ;
MOBERG, LC ;
JOHANSSON, LY ;
LARSSON, R .
ELECTROCHIMICA ACTA, 1982, 27 (10) :1453-1460
[2]  
de Frank Bruijn A., 2013, ENCY SUSTAINABLE SCI, P7694
[3]  
Debrunner P.G., 1989, IRON PORPHYRINS, V3, P139, DOI DOI 10.1002/ANIE.201608539
[4]   Multitechnique Characterization of a Polyaniline-Iron-Carbon Oxygen Reduction Catalyst [J].
Ferrandon, Magali ;
Kropf, A. Jeremy ;
Myers, Deborah J. ;
Artyushkova, Kateryna ;
Kramm, Ulrike ;
Bogdanoff, Peter ;
Wu, Gang ;
Johnston, Christina M. ;
Zelenay, Piotr .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (30) :16001-16013
[5]   Degradation of Fe/N/C catalysts upon high polarization in acid medium [J].
Goellner, Vincent ;
Baldizzone, Claudio ;
Schuppert, Anna ;
Sougrati, Moulay Tahar ;
Mayrhofer, Karl ;
Jaouen, Frederic .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (34) :18454-18462
[6]   Heat-treated iron(III) tetramethoxyphenyl porphyrin supported on high-area carbon as an electrocatalyst for oxygen reduction - I. Characterization of the electrocatalyst [J].
Gojkovic, SL ;
Gupta, S ;
Savinell, RF .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1998, 145 (10) :3493-3499
[7]   Unveiling N-Protonation and Anion-Binding Effects on Fe/N/C Catalysts for O2 Reduction in Proton-Exchange-Membrane Fuel Cells [J].
Herranz, Juan ;
Jaouen, Frederic ;
Lefevre, Michel ;
Kramm, Ulrike I. ;
Proietti, Eric ;
Dodelet, Jean-Pol ;
Bogdanoff, Peter ;
Fiechter, Sebastian ;
Abs-Wurmbach, Irmgard ;
Bertrand, Patrick ;
Arruda, Thomas M. ;
Mukerjee, Sanjeev .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (32) :16087-16097
[8]   Influence of the Electron-Density of FeN4-Centers Towards the Catalytic Activity of Pyrolyzed FeTMPPCl-Based ORR-Electrocatalysts [J].
Kramm, U. I. ;
Abs-Wurmbach, I. ;
Herrmann-Geppert, I. ;
Radnik, J. ;
Fiechter, S. ;
Bogdanoff, P. .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2011, 158 (01) :B69-B78
[9]   Effect of iron-carbide formation on the number of active sites in Fe-N-C catalysts for the oxygen reduction reaction in acidic media [J].
Kramm, Ulrike I. ;
Herrmann-Geppert, Iris ;
Fiechter, Sebastian ;
Zehl, Gerald ;
Zizak, Ivo ;
Dorbandt, Iris ;
Schmeisser, Dieter ;
Bogdanoff, Peter .
JOURNAL OF MATERIALS CHEMISTRY A, 2014, 2 (08) :2663-2670
[10]   Correlations between Mass Activity and Physicochemical Properties of Fe/N/C Catalysts for the ORR in PEM Fuel Cell via 57Fe Mossbauer Spectroscopy and Other Techniques [J].
Kramm, Ulrike I. ;
Lefevre, Michel ;
Larouche, Nicholas ;
Schmeisser, Dieter ;
Dodelet, Jean-Pol .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (03) :978-985