Characteristic and mechanism of methane dehydroaromatization over Zn-based/HZSM-5 catalysts under conditions of atmospheric pressure and supersonic jet expansion

B. S. Liu; Y. Zhang; J. F. Liu; M. Tian; F. M. Zhang; C. T. Au; A. S.C. Cheung

doi:10.1021/jp2027065

Characteristic and mechanism of methane dehydroaromatization over Zn-based/HZSM-5 catalysts under conditions of atmospheric pressure and supersonic jet expansion

B. S. Liu^*, Y. Zhang, J. F. Liu, M. Tian, F. M. Zhang, C. T. Au, A. S.C. Cheung

^*Corresponding author for this work

Department of Chemistry

Research output: Contribution to journal › Journal article › peer-review

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Abstract

The catalytic performance of Zn-based/HZSM-5 catalysts prepared by wet impregnation method was investigated for the methane dehydroaromatization (MDA) reaction under the conditions of atmospheric pressure and supersonic jet expansion (SJE). The physical properties of the catalysts were characterized by Brunauer-Emmett-Teller (BET), Fourier transform infrared (FT-IR), temperature-programmed reduction of H₂ (H₂-TPR), temperature-programmed desorption of NH₃ (NH₃-TPD), X-ray photoelectron spectroscopy (XPS), thermogravimetric and differential thermogravimetric (TG/DTG), and high-resolution transmission electron microscopy (HRTEM) techniques. The results revealed that under SJE condition the Zn/HZSM-5 catalyst exhibited high catalytic activity. It was found that because of the rapid migration of H⁺ ions on the catalyst, the activation of CH ₄ at active sites of nano-ZnO is facile. A new reaction mechanism that involves an active "ZnO-CH₃⁺... ^-HZnO" intermediate formed as a result of synergetic action between ZnO and HZSM-5 has been proposed for CH₄ dissociation and dehydrogenation. Under atmospheric pressure, however, the catalytic activity of Zn/HZSM-5 is low.

Original language	English
Pages (from-to)	16954-16962
Number of pages	9
Journal	Journal of Physical Chemistry C
Volume	115
Issue number	34
DOIs	https://doi.org/10.1021/jp2027065
Publication status	Published - 1 Sept 2011

Scopus Subject Areas

Electronic, Optical and Magnetic Materials
General Energy
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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title = "Characteristic and mechanism of methane dehydroaromatization over Zn-based/HZSM-5 catalysts under conditions of atmospheric pressure and supersonic jet expansion",

abstract = "The catalytic performance of Zn-based/HZSM-5 catalysts prepared by wet impregnation method was investigated for the methane dehydroaromatization (MDA) reaction under the conditions of atmospheric pressure and supersonic jet expansion (SJE). The physical properties of the catalysts were characterized by Brunauer-Emmett-Teller (BET), Fourier transform infrared (FT-IR), temperature-programmed reduction of H2 (H2-TPR), temperature-programmed desorption of NH3 (NH3-TPD), X-ray photoelectron spectroscopy (XPS), thermogravimetric and differential thermogravimetric (TG/DTG), and high-resolution transmission electron microscopy (HRTEM) techniques. The results revealed that under SJE condition the Zn/HZSM-5 catalyst exhibited high catalytic activity. It was found that because of the rapid migration of H+ ions on the catalyst, the activation of CH 4 at active sites of nano-ZnO is facile. A new reaction mechanism that involves an active {"}ZnO-CH3+... -HZnO{"} intermediate formed as a result of synergetic action between ZnO and HZSM-5 has been proposed for CH4 dissociation and dehydrogenation. Under atmospheric pressure, however, the catalytic activity of Zn/HZSM-5 is low.",

author = "Liu, {B. S.} and Y. Zhang and Liu, {J. F.} and M. Tian and Zhang, {F. M.} and Au, {C. T.} and Cheung, {A. S.C.}",

note = "The work described here was supported by a grant from the Research Grants Council of the Hong Kong Special Administrative Region, China (project no. HKU 7015/07P). ",

year = "2011",

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doi = "10.1021/jp2027065",

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T1 - Characteristic and mechanism of methane dehydroaromatization over Zn-based/HZSM-5 catalysts under conditions of atmospheric pressure and supersonic jet expansion

AU - Liu, B. S.

AU - Zhang, Y.

AU - Liu, J. F.

AU - Tian, M.

AU - Zhang, F. M.

AU - Au, C. T.

AU - Cheung, A. S.C.

N1 - The work described here was supported by a grant from the Research Grants Council of the Hong Kong Special Administrative Region, China (project no. HKU 7015/07P).

PY - 2011/9/1

Y1 - 2011/9/1

N2 - The catalytic performance of Zn-based/HZSM-5 catalysts prepared by wet impregnation method was investigated for the methane dehydroaromatization (MDA) reaction under the conditions of atmospheric pressure and supersonic jet expansion (SJE). The physical properties of the catalysts were characterized by Brunauer-Emmett-Teller (BET), Fourier transform infrared (FT-IR), temperature-programmed reduction of H2 (H2-TPR), temperature-programmed desorption of NH3 (NH3-TPD), X-ray photoelectron spectroscopy (XPS), thermogravimetric and differential thermogravimetric (TG/DTG), and high-resolution transmission electron microscopy (HRTEM) techniques. The results revealed that under SJE condition the Zn/HZSM-5 catalyst exhibited high catalytic activity. It was found that because of the rapid migration of H+ ions on the catalyst, the activation of CH 4 at active sites of nano-ZnO is facile. A new reaction mechanism that involves an active "ZnO-CH3+... -HZnO" intermediate formed as a result of synergetic action between ZnO and HZSM-5 has been proposed for CH4 dissociation and dehydrogenation. Under atmospheric pressure, however, the catalytic activity of Zn/HZSM-5 is low.

AB - The catalytic performance of Zn-based/HZSM-5 catalysts prepared by wet impregnation method was investigated for the methane dehydroaromatization (MDA) reaction under the conditions of atmospheric pressure and supersonic jet expansion (SJE). The physical properties of the catalysts were characterized by Brunauer-Emmett-Teller (BET), Fourier transform infrared (FT-IR), temperature-programmed reduction of H2 (H2-TPR), temperature-programmed desorption of NH3 (NH3-TPD), X-ray photoelectron spectroscopy (XPS), thermogravimetric and differential thermogravimetric (TG/DTG), and high-resolution transmission electron microscopy (HRTEM) techniques. The results revealed that under SJE condition the Zn/HZSM-5 catalyst exhibited high catalytic activity. It was found that because of the rapid migration of H+ ions on the catalyst, the activation of CH 4 at active sites of nano-ZnO is facile. A new reaction mechanism that involves an active "ZnO-CH3+... -HZnO" intermediate formed as a result of synergetic action between ZnO and HZSM-5 has been proposed for CH4 dissociation and dehydrogenation. Under atmospheric pressure, however, the catalytic activity of Zn/HZSM-5 is low.

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Characteristic and mechanism of methane dehydroaromatization over Zn-based/HZSM-5 catalysts under conditions of atmospheric pressure and supersonic jet expansion

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