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Methanol Desorption from Cu-ZSM-5 Studied by in Situ Infrared Spectroscopy and First-Principles Calculations

Wang, Xueting; Arvidsson, Adam A.; Cichocka, Magdalena O.; Zou, Xiaodong; Martin, Natalia M. LU ; Nilsson, Johan; Carlson, Stefan LU ; Gustafson, Johan LU ; Skoglundh, Magnus and Hellman, Anders, et al. (2017) In Journal of Physical Chemistry C 121(49). p.27389-27398
Abstract

The dynamic interaction of methanol and its derivatives with Cu-exchanged ZSM-5 during methanol temperature-programmed desorption from 30 to 450 °C has been investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy and first-principles calculations. The results emphasize that defects in the framework structure of the zeolite and Brønsted acid sites constitute ion-exchange sites for Cu ions. The Cu sites introduced in ZSM-5 actively interact with methanol adsorbed at moderate temperature, i.e., below 250 °C, and take roles in further oxidation of the adsorbed species to formate and CO. Moreover, spectra recorded at higher temperatures, i.e., above 300 °C, after adsorption of methanol show strong interaction... (More)

The dynamic interaction of methanol and its derivatives with Cu-exchanged ZSM-5 during methanol temperature-programmed desorption from 30 to 450 °C has been investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy and first-principles calculations. The results emphasize that defects in the framework structure of the zeolite and Brønsted acid sites constitute ion-exchange sites for Cu ions. The Cu sites introduced in ZSM-5 actively interact with methanol adsorbed at moderate temperature, i.e., below 250 °C, and take roles in further oxidation of the adsorbed species to formate and CO. Moreover, spectra recorded at higher temperatures, i.e., above 300 °C, after adsorption of methanol show strong interaction between methoxy groups and the zeolite framework, suggesting that, under mild conditions, proton extraction for methanol production during direct partial oxidation of methane to methanol over Cu-ZSM-5 is necessary.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
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Journal of Physical Chemistry C
volume
121
issue
49
pages
10 pages
publisher
The American Chemical Society
external identifiers
  • scopus:85037585744
  • wos:000418393900017
ISSN
1932-7447
DOI
10.1021/acs.jpcc.7b07067
language
English
LU publication?
yes
id
dc591d2b-394e-47ce-b124-f9a9c18c8018
date added to LUP
2018-01-05 08:19:00
date last changed
2018-01-16 13:29:18
@article{dc591d2b-394e-47ce-b124-f9a9c18c8018,
  abstract     = {<p>The dynamic interaction of methanol and its derivatives with Cu-exchanged ZSM-5 during methanol temperature-programmed desorption from 30 to 450 °C has been investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy and first-principles calculations. The results emphasize that defects in the framework structure of the zeolite and Brønsted acid sites constitute ion-exchange sites for Cu ions. The Cu sites introduced in ZSM-5 actively interact with methanol adsorbed at moderate temperature, i.e., below 250 °C, and take roles in further oxidation of the adsorbed species to formate and CO. Moreover, spectra recorded at higher temperatures, i.e., above 300 °C, after adsorption of methanol show strong interaction between methoxy groups and the zeolite framework, suggesting that, under mild conditions, proton extraction for methanol production during direct partial oxidation of methane to methanol over Cu-ZSM-5 is necessary.</p>},
  author       = {Wang, Xueting and Arvidsson, Adam A. and Cichocka, Magdalena O. and Zou, Xiaodong and Martin, Natalia M. and Nilsson, Johan and Carlson, Stefan and Gustafson, Johan and Skoglundh, Magnus and Hellman, Anders and Carlsson, Per Anders},
  issn         = {1932-7447},
  language     = {eng},
  month        = {12},
  number       = {49},
  pages        = {27389--27398},
  publisher    = {The American Chemical Society},
  series       = {Journal of Physical Chemistry C},
  title        = {Methanol Desorption from Cu-ZSM-5 Studied by in Situ Infrared Spectroscopy and First-Principles Calculations},
  url          = {http://dx.doi.org/10.1021/acs.jpcc.7b07067},
  volume       = {121},
  year         = {2017},
}