Kramm Ulrike I, Lefèvre Michel, Bogdanoff Peter, Schmeißer Dieter, Dodelet Jean-Pol
†Brandenburg Technical University of Cottbus - Senftenberg, Chair of Applied Physics and Sensors, Konrad-Wachsmann-Allee 17, 03046 Cottbus, Germany.
‡Canetique Electrocatalysis, Inc., 1650 Boulevard Lionel-Boulet, Varennes, Québec J3X 1S2, Canada.
J Phys Chem Lett. 2014 Nov 6;5(21):3750-6. doi: 10.1021/jz501955g. Epub 2014 Oct 16.
The applicability of analyzing by Mößbauer 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 Mößbauer 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 Mößbauer spectroscopy, energy-dispersive X-ray cross-sectional imaging, and neutron activation analysis. Our results show that the absorption probability of γ 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.
证明了用穆斯堡尔光谱分析在质子交换膜(PEM)燃料电池的膜电极组件阴极上测试过的Fe-N-C催化剂结构变化的适用性。相同催化剂粉末的穆斯堡尔表征最近在我们之前的出版物中有描述。在此通过穆斯堡尔光谱、能量色散X射线截面成像和中子活化分析研究了在燃料电池中测试时铁物种可能发生的变化。我们的结果表明,Fe-N-C中铁核吸收γ射线的概率受Nafion的存在和含水量的强烈影响。对PEM燃料电池中非贵金属阴极进行氧化处理(1.2 V)的效果的详细研究表明,观察到的活性衰减主要归因于碳氧化导致碳基质中活性铁位点的浸出。