晶化母液介质中制备多级孔TS-1分子筛
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摘要
将微孔TS-1分子筛晶化过程中产生的母液回收处理后用于多级孔TS-1分子筛制备,考察回收母液作为介质的体系中,模板剂/碱体系和碱浓度等因素对多级孔TS-1制备的影响。结果表明:所制备的多级孔TS-1分子筛在保留MFI结构的同时,产生了较多的介孔,使其在环己酮氨肟化反应中显示出更好的催化性能,在较低的催化剂浓度下(1.6 g/L),环己酮转化率为94%,环己酮肟选择性为99%;将回收晶化母液用于多级孔TS-1分子筛的制备,降低了纯水用量,减少了废液排放,符合绿色化学的发展要求。
The mother liquid of microporous TS-1 crystallization process was recycled and used as the medium for the preparation of hierarchical TS-1 zeolites. In the system of recycled mother liquid as medium,the effects of the template agent and alkali on the preparation of hierarchical TS-1 were investigated,respectively. The results showed that while retaining the MFI structure,the prepared hierarchical TS-1 formed more mesoporous pores and exhibited superior catalytic activity in the cyclohexanone ammoximation. At a lower catalyst concentration(1.6 g/L),the cyclohexanone conversion rate was 94% and the cyclohexanone-oxime selectivity was 99%. The recycled mother liquid reduced the consumption of water and the discharge of waste liquid,and agreed with the development requirements of green chemistry.
The mother liquid of microporous TS-1 crystallization process was recycled and used as the medium for the preparation of hierarchical TS-1 zeolites. In the system of recycled mother liquid as medium,the effects of the template agent and alkali on the preparation of hierarchical TS-1 were investigated,respectively. The results showed that while retaining the MFI structure,the prepared hierarchical TS-1 formed more mesoporous pores and exhibited superior catalytic activity in the cyclohexanone ammoximation. At a lower catalyst concentration(1.6 g/L),the cyclohexanone conversion rate was 94% and the cyclohexanone-oxime selectivity was 99%. The recycled mother liquid reduced the consumption of water and the discharge of waste liquid,and agreed with the development requirements of green chemistry.
引文
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[3] Cheneviere Y,Chieux F,Caps F,et al.Synthesis and catalytic properties of TS-1 with mesoporous/microporous hierarchical structures obtained in the presence of amphiphilic organosilanes[J].J Catal,2010,269:161-168
[4] 夏长久,林民,彭欣欣,等.多尺度孔道分布钛硅分子筛材料制备策略的探讨[J].石油学报(石油加工),2016,32(2):407-417
[5] 方志平,程时标,孙斌,等.四丙基氢氧化铵热稳定性对TS-1分子筛合成的影响[J].石油学报(石油加工),2004,20(4):26-31
[6] Li Huachun,Sakamoto Y,Liu Zheng,et al.Mesoporous silicalite-1 zeolite crystals with unique pore shapes analogous to the morphology[J].Microporous and Mesoporous Mater-ials,2007,106:174-179
[7] Kumar P,Gupta J K,Muralidhar G,et al.Acidity studies on titanium silicalites-1(TS-1) by ammonia adsorption using microcalorimetry[J].Stud Surf Sci Catal,1998,113:463-472
[8] Fraile J M,García J I,Mayoral J A,et al.Catalytic sites in silica-supported titanium catalysts:Silsesquioxane complexes as models[J].J Catal,2005,233:90-99