Efficient Synthesis of Cyclohexanol and Ethanol via the Hydrogenation of Acetic Acid-Derived Cyclohexyl Acetate with the CuxAl1Mn2-x Catalysts

被引:7
|
作者
Song, Tongyang [1 ]
Chen, Wei [1 ]
Qi, Yuanyuan [1 ]
Wu, Peng [1 ]
Zhu, Zhirong [2 ]
Li, Xiaohong [1 ]
机构
[1] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, 3663 North Zhongshan Rd, Shanghai 200062, Peoples R China
[2] Tongji Univ, Dept Chem, 1239 Siping Rd, Shanghai 200092, Peoples R China
基金
中国国家自然科学基金;
关键词
Cu-based catalyst; Chemoselective hydrogenation; Cyclohexyl acetate; Cyclohexanol; Ethanol; CU/SIO2; CATALYSTS; METHYL ACETATE; ETHYL-ACETATE; SELECTIVE HYDROGENATION; REACTIVE DISTILLATION; INDIRECT HYDRATION; DIMETHYL OXALATE; CU; METHANOL; ESTERIFICATION;
D O I
10.1002/cctc.202100284
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The hydrogenation of cyclohexyl acetate (CHA), derived from the esterification of acetic acid and cyclohexene, not only alleviates the overcapacity of acetic acid, but also produces value-added cyclohexanol (CHOL) and ethanol at a low cost. Herein, we prepared Cu1Al1, Cu1Mn1 and CuxAl1Mn2-x catalysts via a deposition-precipitation method for the hydrogenation of CHA to CHOL and ethanol. As a result, the ternary CuxAl1Mn2-x catalysts exhibited superior behaviors to Cu1Al1 and Cu1Mn1. To our delight, Cu1Al1Mn1 had a 95.0 % CHA conversion and 93.6 % selectivity to CHOL along with 97.6 % selectivity to ethanol in a batch reactor. Based on detailed characterization, the ternary CuxAl1Mn2-x catalysts possessed more uniformed dispersion of Cu particles, less aggregation and larger BET specific surface area than the binary catalysts. Furthermore, Cu1Al1Mn1 possessed the highest Cu-0/(Cu-0+Cu+) molar ratio, the highest (Mn2++Mn3+)/Mn4+ molar ratio and the most abundant surface oxygen vacancies, facilitating the adsorption and activation of CHA and hydrogen. In addition, Cu1Al1Mn1 had excellent stability (>500 h) in a fixed-bed reactor.
引用
收藏
页码:3099 / 3111
页数:13
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