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二氧化钛负载的钯作为焦油类化合物温和加氢处理的高效稳定催化剂。

TiO-Supported Pd as an Efficient and Stable Catalyst for the Mild Hydrotreatment of Tar-Type Compounds.

作者信息

Raad Zaher, Toufaily Joumana, Hamieh Tayssir, Domine Marcelo E

机构信息

Instituto de Tecnología Química (UPV-CSIC), Universitat Politècnica de València, Consejo Superior de Investigaciones Cientificas, Avda. de los Naranjos s/n, 46022 Valencia, Spain.

Laboratoire de Matériaux, Catalyse, Environnement et Méthodes Analytiques (MCEMA), Faculty of Sciences, Lebanese University, Hadath, Beyrouth 1003, Lebanon.

出版信息

Nanomaterials (Basel). 2021 Sep 13;11(9):2380. doi: 10.3390/nano11092380.

Abstract

The mild hydrotreatment of a model mixture of tar-type compounds (i.e., naphthalene, 1-methylnaphthalene, acenaphthylene, and phenanthrene) to produce partially hydrogenated products in the range of C9-C15 was studied over Pd supported on TiO possessing different crystalline phases. Pd-based catalysts were prepared and characterized by ICP analysis, XRD, N adsorption isotherms, HR-TEM, and NH-TPD, among others. The hydrotreatment activity and selectivity towards the desired hydrogenated products (i.e., tetralin and others) increased with both the acidity and surface area of the catalyst, along with the presence of small and well distributed Pd nanoparticles. For the selected 1.3 wt% Pd/TiO nano catalyst, the operational conditions for maximizing tar conversion were found to be 275 °C, 30 bar of H, and 0.2 g of catalyst for 7 h. The catalyst revealed remarkable hydrotreatment activity and stability after several reuses with practically no changes in TiO structure, quite low carbon deposition, and any Pd leaching detected, thus maintaining both a small Pd particle size and adequate distribution, even after regeneration of the catalyst. Additionally, the Pd/TiO nano catalyst was demonstrated to be more active than other commonly used metal/alumina and more selective than metal/USY zeolites in the mild hydrotreatment of tar-type compounds, thus providing an efficient catalytic route for obtaining partially hydrogenated C9-C15 hydrocarbons useful as jet-fuel components or additives (improvers), as well as chemicals and solvents for industrial applications.

摘要

研究了在具有不同晶相的负载于TiO上的Pd催化剂上,对焦油类化合物(即萘、1-甲基萘、苊烯和菲)的模型混合物进行温和加氢处理,以生成C9 - C15范围内的部分氢化产物。制备了Pd基催化剂,并通过ICP分析、XRD、N吸附等温线、高分辨透射电子显微镜和NH₃-TPD等手段对其进行了表征。加氢处理活性以及对所需氢化产物(即四氢萘等)的选择性随催化剂的酸度和表面积增加而提高,同时还与小尺寸且分布均匀的Pd纳米颗粒的存在有关。对于选定的1.3 wt% Pd/TiO纳米催化剂,发现使焦油转化率最大化的操作条件为275℃、30 bar氢气、0.2 g催化剂,反应7小时。该催化剂在多次重复使用后表现出显著的加氢处理活性和稳定性,TiO结构几乎没有变化,碳沉积相当低,且未检测到任何Pd浸出,因此即使在催化剂再生后仍保持较小的Pd粒径和适当的分布。此外,在焦油类化合物的温和加氢处理中,Pd/TiO纳米催化剂比其他常用的金属/氧化铝更具活性,比金属/USY沸石更具选择性,从而为获得用作喷气燃料组分或添加剂(改进剂)以及工业应用中的化学品和溶剂的部分氢化C9 - C15烃提供了一条有效的催化途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ea3d/8471740/d172366d92e7/nanomaterials-11-02380-g001.jpg

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