Highly active Ce, Y, La-modified Cu/SiO2 catalysts for hydrogenation of methyl acetate to ethanol

Zhiheng Ren; Muhammad Naeem Younis; Chunshan Li; Zengxi Li; Xiangui Yang; Gongying Wang

doi:10.1039/C9RA08780J

Highly active Ce, Y, La-modified Cu/SiO₂ catalysts for hydrogenation of methyl acetate to ethanol†

Zhiheng Ren,^abc Muhammad Naeem Younis,

^c Chunshan Li,

*^cd Zengxi Li,^e Xiangui Yang

*^ab and Gongying Wang^ab

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* Corresponding authors

^a Chengdu Institute of Organic Chemistry, Chinese Academy of Sciences, Chengdu, China
E-mail: yangxg@cioc.ac.cn

^b National Engineering Laboratory & Technology, University of Chinese Academy of Science, Beijing 101408, China

^c CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, The National Key Laboratory of Clean and Efficient Coking Technology, Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, PR China

^d Zhengzhou Institute of Emerging Technology Industries, Zhengzhou 450000, PR China
E-mail: csli@ipe.ac.cn

^e School of Chemical Science, University of Chinese Academy of Sciences, Beijing 100049, People's Republic of China

Abstract

Rare earth element (Ce, Y, and La) modified Cu/SiO₂ catalysts via hydrolysis precipitation and impregnation method were fabricated for the vapor-phase hydrogenation of methyl acetate to ethanol. LaO_x showed the most pronounced promotion in the catalytic tests. After detailed characterizations, via N₂ adsorption–desorption, XRD, N₂O chemisorption, FTIR, H₂-TPR, H₂-TPD, TEM, XPS, and TG/DTA, we found that the addition of promoter LaO_x can decrease the particle size while in turn, it can increase the dispersion of copper species. The strong interactions between copper and lanthanum atoms alter the surface chemical states of the copper species. This results in the generation of more Cu⁺ species and high S_Cu⁺ values, which are responsible for the excellent activity and stability during hydrogenation. In addition, the content of additive LaO_x and reaction conditions (reaction temperature and LHSV) were optimized. Then, the long-term stability performance was evaluated over the selected catalyst in contrast with Cu/SiO₂.

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Highly active Ce, Y, La-modified Cu/SiO₂ catalysts for hydrogenation of methyl acetate to ethanol†

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Highly active Ce, Y, La-modified Cu/SiO₂ catalysts for hydrogenation of methyl acetate to ethanol

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