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钯表面氢化物形成的动力学及其对选择性丁二烯加氢反应选择性控制的影响。

Dynamics of Pd Subsurface Hydride Formation and Their Impact on the Selectivity Control for Selective Butadiene Hydrogenation Reaction.

作者信息

Asedegbega-Nieto Esther, Iglesias-Juez Ana, Di Michiel Marco, Fernandez-Garcia Marcos, Rodriguez-Ramos Inmaculada, Guerrero-Ruiz Antonio

机构信息

Dpto. Química Inorgánica y Técnica, Facultad de Ciencias, UNED, Av. de Esparta s/n, 28232 Las Rozas, Madrid, Spain.

Instituto de Catálisis y Petroleoquímica, CSIC, c/Marie Curie No. 2, Cantoblanco, 28049 Madrid, Spain.

出版信息

Nanomaterials (Basel). 2023 Mar 19;13(6):1099. doi: 10.3390/nano13061099.

DOI:10.3390/nano13061099
PMID:36985993
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10058484/
Abstract

Structure-sensitive catalyzed reactions can be influenced by a number of parameters. So far, it has been established that the formation of Pd-C species is responsible for the behavior of Pd nanoparticles employed as catalysts in a butadiene partial hydrogenation reaction. In this study, we introduce some experimental evidence indicating that subsurface Pd hydride species are governing the reactivity of this reaction. In particular, we detect that the extent of formation/decomposition of PdHx species is very sensitive to the Pd nanoparticle aggregate dimensions, and this finally controls the selectivity in this process. The main and direct methodology applied to determine this reaction mechanism step is time-resolved high-energy X-ray diffraction (HEXRD).

摘要

结构敏感的催化反应会受到许多参数的影响。到目前为止，已经确定Pd-C物种的形成是丁二烯部分加氢反应中用作催化剂的钯纳米颗粒行为的原因。在本研究中，我们引入了一些实验证据，表明表面下的钯氢化物物种决定了该反应的反应活性。特别是，我们检测到PdHx物种的形成/分解程度对钯纳米颗粒聚集体尺寸非常敏感，这最终控制了该过程中的选择性。用于确定该反应机理步骤的主要和直接方法是时间分辨高能X射线衍射（HEXRD）。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/a4b297fb45c0/nanomaterials-13-01099-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/dea7978c4b00/nanomaterials-13-01099-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/5a1cf63a30c5/nanomaterials-13-01099-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/7c266b280df4/nanomaterials-13-01099-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/a4b297fb45c0/nanomaterials-13-01099-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/dea7978c4b00/nanomaterials-13-01099-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/5a1cf63a30c5/nanomaterials-13-01099-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/7c266b280df4/nanomaterials-13-01099-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/303a/10058484/a4b297fb45c0/nanomaterials-13-01099-g004.jpg

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本文引用的文献

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Enhancing Catalytic Performance through Subsurface Chemistry: The Case of CH Semihydrogenation over Pd Catalysts.通过表面下化学增强催化性能：Pd 催化剂上 CH 选择加氢反应的实例。
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采用 X 射线衍射和吸收技术对氢化反应中负载在碳上的钯纳米粒子进行时间分辨的原位研究。
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