Protective desilication of highly siliceous H-ZSM-5 by sole tetraethylammonium hydroxide for the methanol to propylene (MTP) reaction

采用四乙基氢氧化铵对高硅H-ZSM-5进行保护性脱硅,用于甲醇制丙烯(MTP)反应

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Abstract

Protective desilication of highly siliceous H-ZSM-5 was effectively realized by dissolution and recrystallization in tetraethylammonium hydroxide (TEAOH) solution. With better balance between dissolution of OH(-) and recrystallization of TEA(+), intracrystalline mesopores could be generated by selective dissolution of Si by the drilling effects of TEAOH on the micropores, and then Si species in the mother liquor near the external surface could be recrystallized into ZSM-5 shell. With a significantly reduced diffusion length provided by the intracrystalline mesopores, TEAOH-treated samples exhibited longer lifetime and higher propylene selectivity than the parent H-ZSM-5 zeolite. The mediumly-treated T-16 h sample possessed the longest MTP lifetime of 140 h, 5.6 times that of the parent H-ZSM-5 zeolite. Furthermore, the coke content and adsorbed methyl benzene species on the T-16 h sample were heavier than those on the parent H-ZSM-5 sample, which were related to the intracrystalline mesopore structure.

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