改性zsm-5及zsm-11沸石六上甲醇制汽油反应性能研究.docxVIP

分子筛催化剂上甲醇制汽油的反应性能研究The 分子筛催化剂上甲醇制汽油的反应性能研究 The Conversion of Methanol to Gasoline(MTG)over Modified ZSM一5 and ZSM一1 1 Zeolites Abstract Methan01．．to．．gasoline process has gained much more attention of researchers for its simple operation technology and qualified gasoline it produces．111e design of surperior catalysts plays a vital role in MTG technology．ZSM一5 with great hydrothermal stability and shape selectivity serves as the catalyst of MTG reaction．In this paper．we investigated the effects of crystalline size and framework aluminum distribution for MTG in a fixed-bed reactor．At the sanle time．two catalysts modified bv TPAOH and NaOH were also evaluated in MTG reaction．Considering that ZSM．1l has similar pore structure and pore size with ZSM一5．ZSM一11嘶th different temperature hydrothermal treatment were studied and an optimal hydrothermal treatment temperature was obtained． The influence of crystalline size for M1’G reaction was investigated based on ZSM一5 catalyst．It Was found that smaller crystals had higher reactivity and stronger anti-carbon deposition ability，which showed better catalytic stability and longer lifetime in MTG reaction． The impact of framework aluminum distribution over ZSM一5 catalyst for MTG reaction was studied．ZSM一5 witll heterogeneous aluminum distribution showed higher initial methanol conversion．but much more extemal acid sites led to faster deactivation．W11ile ZSM．5 with homogeneous aluminum distribution showed stronger stability．Its lifetime was 224 h．which Was 3．8 times than the former． ZSM．5 synthesized using TPAOH as the template had a silicon—rich interior，while bonl hjgh and 10W temperature desilication 1ed to hollow structure．The Al content enhanced a lot after selective desilication by NaOH treatment especially for outer Al content which was prone to faster deactivation．The desilication，recrystallization by TPAOH treatment caused a silicon-rich external surface．while the bulk S淞l kept nearly unchanged with the migration of a part