TY - JOUR
T1 - Methanol Desorption from Cu-ZSM-5 Studied by in Situ Infrared Spectroscopy and First-Principles Calculations
AU - Wang, Xueting
AU - Arvidsson, Adam A.
AU - Cichocka, Magdalena O.
AU - Zou, Xiaodong
AU - Martin, Natalia M.
AU - Nilsson, Johan
AU - Carlson, Stefan
AU - Gustafson, Johan
AU - Skoglundh, Magnus
AU - Hellman, Anders
AU - Carlsson, Per Anders
PY - 2017/12/14
Y1 - 2017/12/14
N2 - 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.
AB - 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.
U2 - 10.1021/acs.jpcc.7b07067
DO - 10.1021/acs.jpcc.7b07067
M3 - Article
AN - SCOPUS:85037585744
SN - 1932-7447
VL - 121
SP - 27389
EP - 27398
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 49
ER -