Ketonization of Propionic Acid to 3-Pentanone over CexZr1-xO2 Catalysts: The Importance of Acid-Base Balance

被引：39
作者：
Ding, Shuang [1 ]
Wang, Hua [1 ]
Han, Jinyu [1 ]
Zhu, Xinli [1 ]
Ge, Qingfeng [1 ,2 ]
机构：
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
[2] Southern Illinois Univ, Dept Chem & Biochem, Carbondale, IL 62901 USA
来源：
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH | 2018年 / 57卷 / 50期
基金：
中国国家自然科学基金;
关键词：
ACETIC-ACID; CARBOXYLIC-ACIDS; BIO-OIL; MIXED OXIDES; STRUCTURAL-CHARACTERIZATION; PHASE KETONIZATION; RAMAN-SPECTROSCOPY; CEO2; NANOCRYSTALS; CERIA-ZIRCONIA; SURFACE;
D O I：
10.1021/acs.iecr.8b04208
中图分类号：
TQ [化学工业];
学科分类号：
0817 ;
摘要：
Ketonization of biomass-derived propionic acid was investigated at 270-350 degrees C over CexZr1-xO2 mixed oxides with varying Ce/Zr ratios. The acidity of CexZr1-xO2 increases as Zr content is increased. The density of the strong base sites is reduced with increasing Zr content, while the density of the medium-strength base sites is maximized on Ce0.5Zr0.5O2. Diffuse reflectance infrared spectroscopy of propionic acid adsorption indicated that increasing Zr content in CexZr1-xO2 favors monodentate adsorption over bidentate adsorption. The reaction rate varies with the composition of CexZr1-xO2. The intrinsic reaction rate can be correlated with the medium-strength acid/base ratio. The rate maximizes at a medium-strength acid/base ratio of , similar to 1.07 on Ce0.1Zr0.9O2. This value is close to 1, indicating that the balanced medium-strength acid-base sites play a crucial role in the ketonization. The balanced acid- base property influences propionic acid adsorption, enolate formation, and C-C coupling and therefore affects the ketonization rate.
引用
收藏
页码：17086 / 17096
页数：11
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