Synergistic effect of oxygen vacancies and highly dispersed Pd nanoparticles over Pd-loaded TiO2 prepared by a single-step sol–gel process for deoxygenation of triglycerides

除氧 催化作用 加氢脱氧 初湿浸渍 化学 介孔材料 脱碳 化学工程 无机化学 有机化学 选择性 工程类
作者
Tepin Hengsawad,Tossaporn Jindarat,Daniel E. Resasco,Siriporn Jongpatiwut
出处
期刊:Applied Catalysis A-general [Elsevier BV]
卷期号:566: 74-86 被引量:53
标识
DOI:10.1016/j.apcata.2018.08.007
摘要

Renewable diesel has gained attention in recent years due to its superior fuel properties compared to the conventional biodiesel. The uses of Pd supported TiO2 (Pd/TiO2) and Pd supported activated carbon (Pd/C) catalysts for the deoxygenation of triglycerides to renewable diesel were investigated. Two different types of titania supports, i.e. mesoporous titania synthesized by a surfactant-assisted templating sol–gel method (SG-TiO2) and commercial P25-TiO2 (P25-TiO2), were used to investigate the effect of TiO2 crystal structure on the catalytic activity. The prepared catalysts were characterized by N2 adsorption-desorption isotherms, X-ray diffraction (XRD), H2 chemisorption, H2 temperature-programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). The liquid products obtained from the deoxygenation of triglycerides in beef fat over the prepared catalysts at 325 °C, 500 psig, and H2/triglyceride molar ratio of 30 were in the diesel fuel specification range (C15-18). The main liquid products were n-heptadecane (n-C17) and n-pentadecane (n-C15), resulting from the decarboxylation or decarbonylation pathways. It was found that the Pd/P25-TiO2 catalyst exhibited a higher catalytic performance compared to the Pd/C catalyst. The formation of defects (oxygen vacancies and Ti3+) on TiO2, Pd dispersion and inducement of SMSI effect play an important role in the catalytic activity and the diesel yield on Pd/SG-TiO2 catalysts. Furthermore, the Pd incorporation methods, i.e. incipient wetness impregnation (IWI), photochemical deposition (PCD) and single-step sol–gel (SSSG), were also investigated. The Pd/TiO2 prepared by SSSG method exhibited the highest conversion of beef fat and selectivity to the diesel fuel (C15-18) which could be due to its well-dispersed Pd nanoparticles with relatively small size, high defects on TiO2 support and strong SMSI behavior.
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