Oxidative Dehydrogenation of 1-Butene to 1,3-Butadiene Using CO2 over Cr-SiO2 Catalysts Prepared by Sol-gel Method

doi:10.1007/s40242-018-8063-8

Chemical Research in Chinese Universities ›› 2018, Vol. 34 ›› Issue (4): 609-615.doi: 10.1007/s40242-018-8063-8

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Oxidative Dehydrogenation of 1-Butene to 1,3-Butadiene Using CO₂ over Cr-SiO₂ Catalysts Prepared by Sol-gel Method

GAO Biao¹, LUO Yajun¹, MIAO Changxi², YUE Yinghong¹, YANG Weimin², HUA Weiming¹, GAO Zi¹

1. Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, P. R. China;
2. Shanghai Research Institute of Petrochemical Technology, SINOPEC, Shanghai 201208, P. R. China

Received:2018-02-28 Online:2018-08-01 Published:2018-04-28
Contact: MIAO Changxi, HUA Weiming E-mail:miaocx.sshy@sinopec.com;wmhua@fudan.edu.cn
Supported by:
Supported by the National Key R&D Program of China(No.2017YFB0602200), the National Natural Science Foundation of China(No.91645201), the Science and Technology Commission of Shanghai Municipality, China(No.13DZ2275200) and the Fund of Shanghai Research Institute of Petrochemical Technology, SINOPEC, China(No.17ZC06070001).

Abstract

Abstract: A series of Cr-SiO₂ catalysts with a Cr content(mass fraction) ranging from 0.5% to 9% was prepared by a sol-gel method. The catalysts were characterized by XRD, N₂ adsorption, EDX elemental mapping, Raman spectroscopy, UV-Vis spectroscopy, XPS and H₂-TPR, and their catalytic behavior in the dehydrogenation of 1-butene to 1,3-butadiene(BD) using CO₂ as a soft oxidant was studied. The initial BD yield is well correlated with the amount of Cr⁶⁺ in the fresh catalysts. The highest BD yield of ca. 34% is achieved on the catalysts with 5%-9% Cr at 600℃ and weight hourly space velocity(WHSV) of 4.5 g·g_cat^-1·h^-1. The promoting effect of CO₂ on the BD yield was observed, which can be attributed to the reaction coupling between a simple dehydrogenation of 1-butene and the reverse water-gas shift reaction as well as regaining the oxidation state(lattice oxygen) of reduced Cr³⁺ species due to the mild oxidation ability of CO₂. The Cr-SiO₂ catalyst exhibits higher BD yield than the Cr catalyst supported on SBA-15, which is attributed to the higher amount of Cr⁶⁺ present on the former catalyst.

Key words: 1,3-Butadiene, CO₂ oxidative dehydrogenation, Cr-based catalyst, Sol-gel method

GAO Biao, LUO Yajun, MIAO Changxi, YUE Yinghong, YANG Weimin, HUA Weiming, GAO Zi. Oxidative Dehydrogenation of 1-Butene to 1,3-Butadiene Using CO₂ over Cr-SiO₂ Catalysts Prepared by Sol-gel Method[J]. Chemical Research in Chinese Universities, 2018, 34(4): 609-615.

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Oxidative Dehydrogenation of 1-Butene to 1,3-Butadiene Using CO₂ over Cr-SiO₂ Catalysts Prepared by Sol-gel Method

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