In situ X-ray absorption spectroscopy on probing the enhanced electrochemical activity of ternary PtRu@Pb catalysts
In situ X-ray absorption spectroscopy on probing the enhanced electrochemical activity of ternary PtRu@Pb catalysts
复制标题
原位X射线吸收光谱探讨三元PtRu@Pb催化剂增强的电化学活性
DOI：
10.1016/j.electacta.2013.06.087
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发表时间：
2013
影响因子：
6.6
通讯作者：
S. Mukerjee
中科院分区：
文献类型：
--
作者：
Aditi Halder;Q. Jia;Matthew Trahan;S. Mukerjee
各组分组合产生的累积协同效应是开发降低 Pt 含量的活性三元催化剂的一条有前途的途径。在本文中，报道了新型三元催化剂PtRu@Pb/C的合成、电化学性能和原位X射线吸收光谱（XAS）。与商业最先进的 PtRu 催化剂相比，这种三元 PtRu@Pb/C 催化剂的甲醇氧化反应 (MOR) 峰值电流密度增加了十倍。为了了解 PtRu@Pb 较高电流密度背后的机制途径和合理原因，我们进行了 XAS 和 Δμ 分析并结合从头算 FEFF8 计算。结果揭示了从铅到铂的强电荷转移的直接证据，揭示了这种增强的活性。结合原位光谱的电化学研究证实了Pb和Ru所发挥的不同作用，其中配体机制由Pb诱导，双功能机制主要由钌操作，两者都负责增强MOR的高电流密度。
The cumulative synergistic effect generated by the combination of the components is a promising route for developing active ternary catalysts with reduced Pt content. In this article, synthesis, electrochemical property and in situ X-ray absorption spectroscopy (XAS) of a novel ternary catalyst PtRu@Pb/C have been reported. This ternary PtRu@Pb/C catalyst shows tenfold increase in the peak current density for methanol oxidation reaction (MOR) in comparison to the commercial state-of-the-art PtRu catalyst. To understand the mechanistic pathways and plausible reasons behind higher current density of PtRu@Pb, XAS and Δμanalysis in combination with ab initio FEFF8 calculations have been performed. The results reveal the direct evidence of strong charge transfer from lead to platinum shedding the light on this enhanced activity. The electrochemical study in conjunction with the in situ spectroscopy affirms the different role played by Pb and Ru, where ligand mechanism is induced by Pb and the bi-functional mechanism is mostly operated by ruthenium both being responsible in the enhancement of high current density for MOR.