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Accelerated Stress Tests of Pt/HSAC Electrocatalysts: an Identical-Location Transmission Electron Microscopy Study on the Influence of Intermediate Characterizations

机译:Pt / HSAC电催化剂的加速应力测试:相同位置的透射电子显微镜研究中间表征的影响

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The influence of intermediate characterizations used in long-term accelerated stress tests (ASTs) to monitor the changes of the electrochemically active surface area of carbon-supported Pt nanoparticles (Pt/HSAC) was investigated. Our results indicate that, in the studied experimental protocol (potentiostatic polarization at E = 1.0 V vs. RHE during 96 h), the loss of the electrochemically active surface area is greatly exacerbated by intermediate characterizations such as cyclic voltammetry or stripping of a saturated CO_(ad) surface layer. These results can be understood in view of the breakdown of the passivation layer formed on the Pt/HSAC electrocatalyst during the polarization at is E= 1.0 V vs. RHE. By using identical location transmission electron microscopy, the structural modifications of the Pt/HSAC nanoparticles could be monitored. The migration/agglomeration of Pt nanocrystallites, the growth of Pt nanocrystallites by electrochemical OstWald ripening, and the corrosion of the high surface area carbon support are more pronounced when cyclic or CO_(ad) stripping voltammograms are implemented in the AST. A detailed analysis of the identical-location transmission electron microscopy images also indicates that adsorbed CO molecules minor the dissolution of Pt~(2+) ions into the electrolyte.
机译:研究了长期加速应力测试(ASTs)中用于监测碳载Pt纳米颗粒(Pt / HSAC)的电化学活性表面积变化的中间表征的影响。我们的结果表明,在研究的实验方案中(E = 1.0 V时的恒电位极化与96小时内的RHE相比),电化学活性表面积的损失由于循环伏安法或饱和CO_的汽提等中间特征而大大加剧。 (广告)表面层。考虑到在E = 1.0V对RHE的极化期间在Pt / HSAC电催化剂上形成的钝化层的击穿,可以理解这些结果。通过使用相同的位置透射电子显微镜,可以监测Pt / HSAC纳米颗粒的结构修饰。当在AST中实施循环或CO_(ad)溶出伏安图时,Pt纳米晶体的迁移/聚集,通过电化学OstWald成熟的Pt纳米晶体的生长以及高表面积碳载体的腐蚀更加明显。对相同位置的透射电子显微镜图像的详细分析还表明,吸附的CO分子使Pt〜(2+)离子溶解到电解质中的现象变少了。

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