Chinese Journal of Catalysis ›› 2019, Vol. 40 ›› Issue (9): 1375-1384.DOI: 10.1016/S1872-2067(19)63378-4

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Stabilizing copper species using zeolite for ethanol catalytic dehydrogenation to acetaldehyde

Dongni Yua, Weili Daia, Guangjun Wua, Naijia Guana,b, Landong Lia,b   

  1. a School of Materials Science and Engineering & National Institute for Advanced Materials, Nankai University, Tianjin 300350, China;
    b Key Laboratory of Advanced Energy Materials Chemistry of the Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, Nankai University, Tianjin 300071, China
  • Received:2019-02-28 Online:2019-09-18 Published:2019-07-06
  • Contact: S1872-2067(19)63378-4
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21872072, 21573113), Municipal Natural Science Foundation of Tianjin (18JCZDJC37400) and Sinopec (417012).

Abstract: The selective dehydrogenation of ethanol to acetaldehyde is a promising route for acetaldehyde production. Although Cu-based catalysts exhibit high activity in ethanol dehydrogenation, a rapid deactivation due to Cu sintering always occurs. In this study, highly dispersed Cu species were stabilized using the silanol defects in Beta zeolite (denoted as Beta) resulting from dealumination, and applied as robust catalysts for ethanol-to-acetaldehyde conversion. Typically, a long catalyst lifetime of 100 h with an acetaldehyde yield of ~70% could be achieved over 5% Cu/Beta. The presence of Cu+ and Cu0 species and the agglomeration of Cu particles after a long-term reaction for 180 h were revealed by transmission electron microscopy, thermogravimetric analysis, and CO-diffuse-reflectance infrared Fourier transform spectroscopy, and were responsible for the deactivation of the Cu/Beta catalyst in the ethanol-to-acetaldehyde conversion.

Key words: Ethanol dehydrogenation, Acetaldehyde, Zeolite, Cu-based catalyst, Deactivation