Product flexibility is key to meeting fluctuating chemicals demands in the future. In this contribution, the methanol to hydrocarbons (MTH) reaction was investigated over two Ge-containing H-ITQ-13 samples, one with needle-like (H-ITQ-13(N), with (Si+Ge)/Al) = 42) and another with plate-like (H-ITQ-13(P), with (Si+Ge)/Al > 100) morphology. The samples were characterised using XRD, BET, SEM/EDS and FTIR spectroscopy, and their MTH performance was compared with the performance of H-ZSM-5 and H-ZSM-22. Similar specific surface areas (413 and 455 m(2) g(-1) for H-ITQ-13(N) and (P), respectively) and similar acid strength (Delta nu similar to -327(-310) cm(-1)) was observed for the two H-ITQ-13 samples. Testing of H-ITQ-13(N) at weight hourly space velocity (WHSV) = 2-8 h(-1) at 350-450 A degrees C revealed that C5+ alkenes were the main products (35-45 % selectivity at 400 A degrees C), followed by propene and butene. A low but significant selectivity for aromatic products was observed (6-8 % selectivity at 400 A degrees C). Product selectivity was found to be independent of deactivation. The methanol conversion capacity of H-ITQ-13(N) was 120-150 g methanol g(-1) catalyst at 400 A degrees C. Testing H-ITQ-13 at high (30 atm) and ambient pressure, respectively, at 350 A degrees C showed that a high pressure led to enhanced C5+ selectivity, but close to a tenfold decrease in methanol conversion capacity. H-ITQ-13(P) was tested at 400 A degrees C and 2 h(-1). It gave lower conversion than H-ITQ-13(N). Furthermore, when compared at the same conversion level, H-ITQ-13(P) gave higher C5+ alkene selectivity, lower aromatics selectivity, and a higher propene to ethene ratio than H-ITQ-13(N). The H-ITQ-13 samples yielded a product spectrum intermediate of H-ZSM-22 and H-ZSM-5. The effluent product cut-off of H-ITQ-13 was similar to that of H-ZSM-5 with tetramethylbenzene as the largest significant product, while H-ZSM-22 produced mainly linear and branched alkenes. The lifetime of H-ITQ-13(N) was clearly enhanced compared to H-ZSM-22, but inferior to H-ZSM-5.

Methanol Conversion to Hydrocarbons (MTH) Over H-ITQ-13 (ITH) Zeolite

BORDIGA, Silvia;
2014-01-01

Abstract

Product flexibility is key to meeting fluctuating chemicals demands in the future. In this contribution, the methanol to hydrocarbons (MTH) reaction was investigated over two Ge-containing H-ITQ-13 samples, one with needle-like (H-ITQ-13(N), with (Si+Ge)/Al) = 42) and another with plate-like (H-ITQ-13(P), with (Si+Ge)/Al > 100) morphology. The samples were characterised using XRD, BET, SEM/EDS and FTIR spectroscopy, and their MTH performance was compared with the performance of H-ZSM-5 and H-ZSM-22. Similar specific surface areas (413 and 455 m(2) g(-1) for H-ITQ-13(N) and (P), respectively) and similar acid strength (Delta nu similar to -327(-310) cm(-1)) was observed for the two H-ITQ-13 samples. Testing of H-ITQ-13(N) at weight hourly space velocity (WHSV) = 2-8 h(-1) at 350-450 A degrees C revealed that C5+ alkenes were the main products (35-45 % selectivity at 400 A degrees C), followed by propene and butene. A low but significant selectivity for aromatic products was observed (6-8 % selectivity at 400 A degrees C). Product selectivity was found to be independent of deactivation. The methanol conversion capacity of H-ITQ-13(N) was 120-150 g methanol g(-1) catalyst at 400 A degrees C. Testing H-ITQ-13 at high (30 atm) and ambient pressure, respectively, at 350 A degrees C showed that a high pressure led to enhanced C5+ selectivity, but close to a tenfold decrease in methanol conversion capacity. H-ITQ-13(P) was tested at 400 A degrees C and 2 h(-1). It gave lower conversion than H-ITQ-13(N). Furthermore, when compared at the same conversion level, H-ITQ-13(P) gave higher C5+ alkene selectivity, lower aromatics selectivity, and a higher propene to ethene ratio than H-ITQ-13(N). The H-ITQ-13 samples yielded a product spectrum intermediate of H-ZSM-22 and H-ZSM-5. The effluent product cut-off of H-ITQ-13 was similar to that of H-ZSM-5 with tetramethylbenzene as the largest significant product, while H-ZSM-22 produced mainly linear and branched alkenes. The lifetime of H-ITQ-13(N) was clearly enhanced compared to H-ZSM-22, but inferior to H-ZSM-5.
2014
57
1-4
143
158
http://link.springer.com/article/10.1007%2Fs11244-013-0170-7
CATALYZED METHYLATION REACTIONS; LARGE-PORE ZEOLITE; REACTION-MECHANISM; PRODUCT SELECTIVITY; SHAPE SELECTIVITY; ACIDIC ZEOLITES; Methanol Conversion to Hydrocarbons; MTH; H-ITQ-13; ITH Zeolite; FTIR spectroscopy; X-ray powder diffraction; SEM; Methanol conversion; Gas chromatography
W. Skistad;S. Teketel;F. L. Bleken;P. Beato;S. Bordiga;M. H. Nilsen;U. Olsbye;S. Svelle;K. P. Lillerud
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2318/153277
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