TY - JOUR
T1 - Conversion of methanol to hydrocarbons over conventional and mesoporous H-ZSM-5 and H-Ga-MFI: Major differences in deactivation behavior
AU - Mentzel, Uffe Vie
AU - Højholt, Karen Thrane
AU - Holm, Martin Spangsberg
AU - Fehrmann, Rasmus
AU - Beato, Pablo
PY - 2012
Y1 - 2012
N2 - Methanol has been converted to hydrocarbons over conventional and mesoporous H-ZSM-5 and H-Ga-MFI. The gallium based zeotypes are analogous to H-ZSM-5, but the Brønsted acidity is introduced by framework incorporation of gallium rather than aluminum, which leads to lower intrinsic acid strength. In the methanol-to-hydrocarbons (MTH) process, H-ZSM-5 is subjected to coke formation leading to catalyst deactivation. Here we show that when the gallium containing zeotypes are employed in the MTH process, only insignificant amounts of coke are present in the deactivated catalysts, indicating distinct differences in deactivation mechanisms of the two different catalysts. This is investigated further through FT-IR measurements as well as catalytic experiments employing regenerated and steamed catalysts. From this it is concluded that the H-Ga-MFI is subjected to irreversible deactivation by steaming (hydrolysis) of the Ga&sbnd;O bonds in the zeolite structure rather than coke deposition.
AB - Methanol has been converted to hydrocarbons over conventional and mesoporous H-ZSM-5 and H-Ga-MFI. The gallium based zeotypes are analogous to H-ZSM-5, but the Brønsted acidity is introduced by framework incorporation of gallium rather than aluminum, which leads to lower intrinsic acid strength. In the methanol-to-hydrocarbons (MTH) process, H-ZSM-5 is subjected to coke formation leading to catalyst deactivation. Here we show that when the gallium containing zeotypes are employed in the MTH process, only insignificant amounts of coke are present in the deactivated catalysts, indicating distinct differences in deactivation mechanisms of the two different catalysts. This is investigated further through FT-IR measurements as well as catalytic experiments employing regenerated and steamed catalysts. From this it is concluded that the H-Ga-MFI is subjected to irreversible deactivation by steaming (hydrolysis) of the Ga&sbnd;O bonds in the zeolite structure rather than coke deposition.
KW - Gallium
KW - Regeneration
KW - Zeolite
KW - Deactivation
KW - Methanol-to-hydrocarbons (MTH)
U2 - 10.1016/j.apcata.2012.01.003
DO - 10.1016/j.apcata.2012.01.003
M3 - Journal article
SN - 0926-860X
VL - 417-418
SP - 290
EP - 297
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
ER -