Appel Marina, Borisov Galin, Holderer Olaf, Appavou Marie-Sousai, Zorn Reiner, Lehnert Werner, Richter Dieter
Jülich Centre for Neutron Science at MLZ, Forschungszentrum Jülich GmbH Lichtenbergstr. 1 85747 Garching Germany
Institute of Energy and Climate Research, Forschungszentrum Jülich GmbH 52425 Jülich Germany.
RSC Adv. 2019 Nov 20;9(65):37768-37777. doi: 10.1039/c9ra06431a. eCollection 2019 Nov 19.
The present study focuses on quasielastic neutron scattering (QENS) of the proton dynamics in phosphoric acid (PA) inside the catalytic layer of high-temperature polymer electrolyte fuel cells (HT-PEFCs). The nanosecond proton dynamics is investigated on the local length scale around operating temperatures (300 K-430 K) using neutron backscattering spectroscopy. We have investigated the catalyst doped with different amounts of PA in order to understand the distribution of PA inside the layer. Three approaches are considered for the description of proton dynamics: the random jump diffusion model, distribution of diffusion constants and, finally, the trap model. Due to adsorption of the PA on the Pt particles the diffusion of protons in the catalytic layer is different in comparison to the bulk acid. The proton dynamics in the catalytic layer can be described by the random jump diffusion with traps. This diffusion is significantly slower than the diffusion of free PA; this also results in a lower conductivity, which is estimated from the obtained diffusion constant.
本研究聚焦于高温聚合物电解质燃料电池(HT - PEFCs)催化层内磷酸(PA)中质子动力学的准弹性中子散射(QENS)。利用中子背散射光谱在接近工作温度(300 K - 430 K)的局部长度尺度上研究纳秒级质子动力学。我们研究了掺杂不同量PA的催化剂,以了解PA在层内的分布情况。考虑了三种描述质子动力学的方法:随机跳跃扩散模型、扩散常数分布以及最终的陷阱模型。由于PA吸附在Pt颗粒上,催化层中质子的扩散与本体酸相比有所不同。催化层中的质子动力学可以用带有陷阱的随机跳跃扩散来描述。这种扩散明显慢于游离PA的扩散;这也导致电导率较低,电导率是根据所获得的扩散常数估算的。