物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2014年
3期
535-543
,共9页
张少龙%张兰兰%王务刚%闵媛媛%马通%宋宇%巩雁军%窦涛
張少龍%張蘭蘭%王務剛%閔媛媛%馬通%宋宇%鞏雁軍%竇濤
장소룡%장란란%왕무강%민원원%마통%송우%공안군%두도
纳米薄层%HZSM-5分子筛%甲醇%丙烯
納米薄層%HZSM-5分子篩%甲醇%丙烯
납미박층%HZSM-5분자사%갑순%병희
Nanosheet%HZSM-5 zeolite%Methanol%Propylene
在合成系列硅铝比纳米薄层HZSM-5分子筛的基础上,研究了纳米薄层HZSM-5分子筛催化甲醇制丙烯(MTP)的反应性能.在固定床微反装置上详细考察了工艺条件对纳米薄层HZSM-5分子筛催化性能的影响,同时与纳米HZSM-5分子筛对MTP反应的催化性能进行了比较.结果表明,纳米薄层HZSM-5分子筛具有较高的目的产物选择性和较长的催化寿命.在适宜硅铝比(n(SiO2)/n(Al2O3)=213)和反应条件下(温度470°C,甲醇质量空速为3 h-1),丙烯的选择性达到46.7%,三烯(乙烯、丙烯和C4烯烃)选择性达到78.7%.其中,丙烯/乙烯的质量比可达到6.5,是纳米HZSM-5分子筛的2倍,而芳烃的选择性比纳米分子筛明显降低.这是因为纳米薄层HZSM-5分子筛比纳米HZSM-5分子筛具有较宽的(010)晶面、较大的外比表面积和介孔孔容.
在閤成繫列硅鋁比納米薄層HZSM-5分子篩的基礎上,研究瞭納米薄層HZSM-5分子篩催化甲醇製丙烯(MTP)的反應性能.在固定床微反裝置上詳細攷察瞭工藝條件對納米薄層HZSM-5分子篩催化性能的影響,同時與納米HZSM-5分子篩對MTP反應的催化性能進行瞭比較.結果錶明,納米薄層HZSM-5分子篩具有較高的目的產物選擇性和較長的催化壽命.在適宜硅鋁比(n(SiO2)/n(Al2O3)=213)和反應條件下(溫度470°C,甲醇質量空速為3 h-1),丙烯的選擇性達到46.7%,三烯(乙烯、丙烯和C4烯烴)選擇性達到78.7%.其中,丙烯/乙烯的質量比可達到6.5,是納米HZSM-5分子篩的2倍,而芳烴的選擇性比納米分子篩明顯降低.這是因為納米薄層HZSM-5分子篩比納米HZSM-5分子篩具有較寬的(010)晶麵、較大的外比錶麵積和介孔孔容.
재합성계렬규려비납미박층HZSM-5분자사적기출상,연구료납미박층HZSM-5분자사최화갑순제병희(MTP)적반응성능.재고정상미반장치상상세고찰료공예조건대납미박층HZSM-5분자사최화성능적영향,동시여납미HZSM-5분자사대MTP반응적최화성능진행료비교.결과표명,납미박층HZSM-5분자사구유교고적목적산물선택성화교장적최화수명.재괄의규려비(n(SiO2)/n(Al2O3)=213)화반응조건하(온도470°C,갑순질량공속위3 h-1),병희적선택성체도46.7%,삼희(을희、병희화C4희경)선택성체도78.7%.기중,병희/을희적질량비가체도6.5,시납미HZSM-5분자사적2배,이방경적선택성비납미분자사명현강저.저시인위납미박층HZSM-5분자사비납미HZSM-5분자사구유교관적(010)정면、교대적외비표면적화개공공용.
Nanosheets of HZSM-5 zeolite with different SiO2/Al2O3 molar ratios were synthesized, and their catalytic behavior in the methanol-to-propylene (MTP) reaction was evaluated in a fixed bed reactor. The effect of reaction conditions on catalytic performance was studied in detail. The catalytic performance of nanosheets of HZSM-5 zeolites in the MTP reaction was compared with that of the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite had higher propylene selectivity, total three olefins′selectivity (ethylene, propylene, C4 alkenes), and a longer catalytic lifetime than the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite with a SiO2/Al2O3 molar ratio of 213 yielded a propylene selectivity of 46.7%, total three olefins′selectivity of 78.7%at 470 °C, and a methanol weight hourly space velocity (WHSV) of 3 h-1. It also yielded a propylene/ethylene mass ratio of 6.5, which was double that of the nanosized HZSM-5 zeolite. The nanosheets of HZSM-5 zeolite had a lower aromatic selectivity than the nanosized HZSM-5 zeolite. The good MTP catalytic performance of the nanosheets of HZSM-5 zeolite was attributed to their wide (010) surface, high external surface area, and large mesoporous volume.