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Immunity of the Fe-N-C catalysts to electrolyte adsorption: Phosphate but not perchloric anions
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2018-03-19 , DOI: 10.1016/j.apcatb.2018.03.056
Yang Hu , Jens Oluf Jensen , Chao Pan , Lars Nilausen Cleemann , Illia Shypunov , Qingfeng Li

Non-precious metal catalysts (NPMCs), particularly the type based on carbon-supported FeNx functionalities (Fe-N-C) are a very promising material for replacing the rare and costly platinum-based catalysts in polymer electrolyte membrane fuel cells (PEMFCs). Evaluation of these materials is most often carried out, like for Pt-based catalysts, in dilute perchloric acid by assuming its non-adsorbing nature on the active sites. The assumption is however not true. In this work, a typical Fe-N-C catalyst was first synthesized by high-pressure pyrolysis in the presence of a carbon support and thoroughly characterized in terms of morphology, structure and active site distribution. The subsequent electrochemical characterization of the catalyst shows strong adsorption and poisoning effect of, in addition to the known Cl, perchloric anions on the oxygen reduction reaction (ORR) activity. On the contrary, phosphate anions exhibit negligible poisoning effect on the catalyst activity. At 0.8 V vs. RHE, the ORR activity of the catalyst is found to decrease in the order of H3PO4 (8.6 mA mg−1) > H2SO4 (5.3 mA mg−1) > HClO4 (3.1 mA mg−1) > HCl (0.7 mA mg−1). The results suggest potential applications of NPMC in high-temperature PEMFCs based on phosphoric acid doped polymer membranes, where high-loading platinum catalysts are currently used. As demonstrated in the low current density range of high-temperature PEMFCs, the catalyst shows a comparable performance to the Pt/C catalysts.



中文翻译:

Fe-NC催化剂对电解质吸附的抗性:磷酸根而不是高氯酸根阴离子

非贵金属催化剂(NPMC),尤其是基于碳载FeN x的类型功能性(Fe-NC)是一种非常有前途的材料,可替代聚合物电解质膜燃料电池(PEMFC)中稀有且昂贵的铂基催化剂。像对于基于Pt的催化剂一样,最经常在稀高氯酸中评估这些物质,方法是假设其在活性位点上不具有吸附性。但是,该假设是不正确的。在这项工作中,典型的Fe-NC催化剂首先是在碳载体存在下通过高压热解合成的,并在形态,结构和活性位点分布方面进行了全面表征。催化剂的随后的电化学表征显示强吸附和中毒除了已知的Cl,效果-,高氯酸根阴离子对氧还原反应(ORR)的活性。相反,磷酸根阴离子对催化剂活性的毒性作用可忽略不计。在相对于RHE的0.8 V下,发现催化剂的ORR活性按H 3 PO 4(8.6 mA mg -1)> H 2 SO 4(5.3 mA mg -1)> HClO 4(3.1 mA )的顺序降低。mg -1)> HCl(0.7 mA毫克-1)。结果表明,NPMC在基于磷酸掺杂的聚合物膜的高温PEMFC中的潜在应用,目前正在使用高负载的铂催化剂。如在高温PEMFC的低电流密度范围内所证明的,该催化剂表现出与Pt / C催化剂相当的性能。

更新日期:2018-03-19
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