Catalytic properties and deactivation behavior of H-MCM-22 in the conversion of methanol to hydrocarbons

Pengfei Wang; Lizhi Huang; Junfen Li; Mei Dong; Jianguo Wang; Takashi Tatsumi; Weibin Fan

doi:10.1039/C5RA00048C

Catalytic properties and deactivation behavior of H-MCM-22 in the conversion of methanol to hydrocarbons

Pengfei Wang,^a^b Lizhi Huang,^a Junfen Li,^a Mei Dong,^a Jianguo Wang,^a Takashi Tatsumi^c and Weibin Fan*^a

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* Corresponding authors

^a State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
E-mail: fanwb@sxicc.ac.cn
Fax: +86-351-4041153
Tel: +86-351-4199009

^b University of Chinese Academy of Sciences, Beijing 100049, China

^c Chemical Resources Laboratory, Tokyo Institute of Technology, Nagatsuta 4259, Midori-ku, Yokohama 226-8503, Japan

Abstract

The catalytic properties of H-MCM-22 zeolites with Si/Al ratios in the range from 13.5 to 47 and their dealuminated samples were investigated in the conversion of methanol to hydrocarbons. The fresh and spent samples were characterized with XRD, NH₃-TPD, pyridine-adsorption infrared spectroscopy, ²⁷Al MAS NMR spectroscopy, TG-DTA, GC-MS, diffuse reflectance UV-vis, Raman spectroscopy techniques and nitrogen and p-xylene adsorption experiments. Although a decrease in protonic acid sites, as expected, increased the selectivity to light olefins such as propene and butene, the sample with a Si/Al ratio of 25–37 showed higher catalytic stability. It is worth noting that the external surface acid sites have a pronounced effect on the catalytic performance. Selective removal of these acid sites by dealumination with oxalic acid markedly increased the catalytic stability. This is because the acid sites in the supercages and external side pockets quickly induced formation of deposited coke species, which blocked the sinusoidal channels and caused the deactivation of the catalyst.

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Publication details

The article was received on 02 Jan 2015, accepted on 17 Mar 2015 and first published on 17 Mar 2015

Article type: Paper

DOI: 10.1039/C5RA00048C

Citation: RSC Adv., 2015,5, 28794-28802

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Catalytic properties and deactivation behavior of H-MCM-22 in the conversion of methanol to hydrocarbons

P. Wang, L. Huang, J. Li, M. Dong, J. Wang, T. Tatsumi and W. Fan, RSC Adv., 2015, 5, 28794
DOI: 10.1039/C5RA00048C
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Catalytic properties and deactivation behavior of H-MCM-22 in the conversion of methanol to hydrocarbons

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Catalytic properties and deactivation behavior of H-MCM-22 in the conversion of methanol to hydrocarbons

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