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Investigation of Supported Pd-Based Electrocatalysts for the Oxygen Reduction Reaction: Performance Durability and Methanol Tolerance

机译:负载型钯基电催化剂的氧还原反应研究:性能耐久性和耐甲醇性

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摘要

Next generation cathode catalysts for direct methanol fuel cells (DMFCs) must have high catalytic activity for the oxygen reduction reaction (ORR), a lower cost than benchmark Pt catalysts, and high stability and high tolerance to permeated methanol. In this study, palladium catalysts supported on titanium suboxides (Pd/TinO2n–1) were prepared by the sulphite complex route. The aim was to improve methanol tolerance and lower the cost associated with the noble metal while enhancing the stability through the use of titanium-based support; 30% Pd/Ketjenblack (Pd/KB) and 30% Pd/Vulcan (Pd/Vul) were also synthesized for comparison, using the same methodology. The catalysts were ex-situ characterized by physico-chemical analysis and investigated for the ORR to evaluate their activity, stability, and methanol tolerance properties. The Pd/KB catalyst showed the highest activity towards the ORR in perchloric acid solution. All Pd-based catalysts showed suitable tolerance to methanol poisoning, leading to higher ORR activity than a benchmark Pt/C catalyst in the presence of low methanol concentration. Among them, the Pd/TinO2n–1 catalyst showed a very promising stability compared to carbon-supported Pd samples in an accelerated degradation test of 1000 potential cycles. These results indicate good perspectives for the application of Pd/TinO2n–1 catalysts in DMFC cathodes.
机译:用于直接甲醇燃料电池(DMFC)的下一代阴极催化剂必须具有对氧还原反应(ORR)的高催化活性,比基准Pt催化剂低的成本,以及对渗透甲醇的高稳定性和高耐受性。在这项研究中,通过亚硫酸盐络合物路线制备了负载在低价钛氧化物(Pd / TinO2n-1)上的钯催化剂。目的是通过使用钛基载体提高甲醇耐受性并降低与贵金属有关的成本,同时提高稳定性。还使用相同的方法合成了30%Pd /科琴黑(Pd / KB)和30%Pd / Vulcan(Pd / Vul)进行比较。通过理化分析对催化剂进行异位表征,并对其ORR进行了研究,以评估其活性,稳定性和甲醇耐受性。在高氯酸溶液中,Pd / KB催化剂对ORR的活性最高。在甲醇浓度低的情况下,所有基于Pd的催化剂均显示出对甲醇中毒的适当耐受性,从而导致ORR活性高于基准Pt / C催化剂。其中,与碳载Pd样品相比,Pd / TinO2n-1催化剂在1000个潜在循环的加速降解测试中显示出非常有希望的稳定性。这些结果为在DMFC阴极中应用Pd / TinO2n-1催化剂提供了良好的前景。

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