Cl对负载型PdO在乙醇/水溶剂混合物中还原的影响

Q1 Materials Science Catalysis Structure & Reactivity Pub Date : 2017-02-21 DOI:10.1080/2055074X.2016.1267296

J. Brazier, M. Newton, Elena M. Barreiro, S. Parry, L. A. Adrio, Christopher J. Mulligan, K. Hellgardt, K. K. Hii, P. Thompson, Rachel Nichols, B. Nguyen

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引用次数: 4

摘要

摘要研究了γ-Al2O3负载PdO在流动乙醇水溶液中的还原反应。在Pd K边缘进行的快速EXAFS（QEXAFS）表明，Cl的存在会对还原过程产生深远影响。在低Pd负载量（1wt%）下，与不含Cl的样品相比，该工艺的尺寸依赖性相反。发现还原程度取决于负载/颗粒尺寸。结果表明，在Cl K-和Pd L3边缘使用原位QEXAFS，即使在350K的高温下，残留的Cl也不会被流动的溶剂混合物去除。这些行为的起源是根据Cl与氧化或还原的金属中心结合时可能产生的不同影响进行讨论的，并将结果与早期关于Cl对商业聚脲包封的Pd ENCAT的影响的观察结果进行了比较™ NP 30催化剂。

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Effects of Cl on the reduction of supported PdO in ethanol/water solvent mixtures

Abstract The reduction of γ-Al2O3-supported PdO in flowing aqueous ethanol was investigated. Quick EXAFS (QEXAFS) performed at the Pd K-edge reveals that the presence of Cl can have a profound effect on the reduction process. At low loadings of Pd (1 wt-%), the size dependency of the process is inverted, compared to Cl-free samples. The extent of reduction was found to be dependent on loading/particles size. It is shown, using in situ QEXAFS at the Cl K- and Pd L3-edges, that residual Cl is not removed by the flowing solvent mixture, even at an elevated temperature of 350 K. The origins of these behaviours are discussed in terms of the differing effects that Cl may have when bonded to oxidic or reduced metal centres and the results were compared to earlier observations made on the effects of Cl on commercial polyurea encapsulated Pd ENCAT™ NP 30 catalysts.

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