Ce-UiO-66 Derived CeO2 Octahedron Catalysts for Efficient Ketonization of Propionic Acid

被引：33

作者：

Guo, Yonghua ^{[1
]}

Yu, Qiang ^{[1
]}

Fang, Huasu ^{[1
]}

Wang, Hua ^{[1
]}

Han, Jinyu ^{[1
]}

Ge, Qingfeng ^{[2
]}

Zhu, Xinli ^{[1
]}

机构：

[1] Tianjin Univ, Sch Chem Engn & Technol, Minist Educ, Collaborat Innovat Ctr Chem Sci & Engn,Key Lab Gr, Tianjin 300072, Peoples R China

[2] Southern Illinois Univ, Dept Chem & Biochem, Carbondale, IL 62901 USA

来源：

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH | 2020年 / 59卷 / 39期

基金：

中国国家自然科学基金;

关键词：

VAPOR-PHASE KETONIZATION; CARBOXYLIC-ACIDS; ACETIC-ACID; CONVERSION; BIOMASS; CERIA; MORPHOLOGY; OXIDE; HYDROCARBONS; 3-PENTANONE;

D O I：

10.1021/acs.iecr.0c01238

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

CeO2-UiO octahedron catalysts derived from cerium-based metal-organic frameworks Ce-UiO-66 were synthesized for vapor-phase ketonization of propionic acid. Characterizations showed the CeO2-UiO octahedron is assembled from nanosized CeO2 crystallites with mesopores. XPS and Raman results indicated that more oxygen vacancies are formed in CeO2-UiO-450 catalyst than in CeO2-P prepared by a precipitation method. Intrinsic ketonization rates on CeO2-UiO-450 are improved relative to CeO2-P. At 350 degrees C, the turnover frequency based on acid-base pair on CeO2-UiO-450 (7.45 s(-1)) is 1.38 times higher than that on CeO2-P (5.41 s(-1)). Consistently, the activation energy is lowered from 130.5 kJ/mol for CeO2-P to 109.0 kJ/mol for CeO2-UiO-450. Infrared spectroscopy results showed that monodentate carboxylate is the active adsorption configuration, and its consumption is much faster on CeO2-UiO-450 than on CeO2-P. A linear correlation between the concentration of oxygen vacancy and intrinsic ketonization rate is found, indicating that the oxygen vacancy promotes ketonization on CeO2.

引用

页码：17269 / 17278

页数：10

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