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
收藏
页码：17269 / 17278
页数：10
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