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Synthesis and catalytic properties of a new titanosilicate molecular sieve with the structure analogous to MWW-type lamellar precursor

机译:结构类似于MWW型片状前体的新型钛硅酸盐分子筛的合成与催化性能

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A new titanosilicate molecular sieve structurally analogous to MWW-type lamellar precursors (designated as Ti-YNU-1) was postsynthesized by adjusting the titanium content in the synthesis gel and washing the as-synthesized material with acid under refluxing conditions.The samples were characterized with XRD,TCP,TG/DTA,FTIR,UV-vis,and ~(29)Si MAS NMR techniques as well as N_2,Ar,and H_2O adsorption experiments.It was indicated that compared with Ti-MWW,Ti-YUN-1 had more silanols in the structure and that its interlayer spacing was expanded by nearly 2.5 A.In addition,the local environment of T_1 sites of the proposed structure of Ti-YNU-1 was also different from that of Ti-MWW.This led to a great increase in the pore openings connected to supercages.The formation of Ti-YNU-1 was highly dependent on the Si/Ti ratio in the synthesis gel and also might be related to the removal of about 80% templating molecules by acid treatment before calcination.Extensive evaluation of the catalytic performance of various titanosilicates for the oxidation of different cycloalkenes showed that Ti-YNU-1 behaved like a 12-membered ring (MR) zeolite.This is further confirmed by the results that a strong peak around 6.7 A was present in the pore size distribution curve obtained from Ar adsorption for the Ti-YNU-1 sample but absent in that for the Ti-MWW sample,and that cyclohexene conversion increased but 1 -hexene conversion decreased with increasing Si/Ti ratio.Compared with the other titanosilicate materials,Ti-YNU-1 showed high activity,selectivity,and stability in the liquid-phase epoxidation of bulky cycloalkenes with H_2O_2 as an oxidant.An investigation of the effect of several protic and aprotic solvents on the catalytic property of Ti-YNU-1 in the epoxidation of cyclohexene revealed that acetonitrile should be the solvent of choice considering both conversion and selectivity.
机译:通过调节合成凝胶中的钛含量并在回流条件下用酸洗涤合成后的材料后合成一种结构类似于MWW型片状前体(称为Ti-YNU-1)的新型钛硅酸盐分子筛。 XRD,TCP,TG / DTA,FTIR,UV-vis和〜(29)Si MAS NMR技术以及N_2,Ar和H_2O吸附实验表明,与Ti-MWW,Ti-YUN- 1的结构中含有更多的硅烷醇,其层间距扩大了近2.5 A.此外,拟议的Ti-YNU-1结构的T_1位的局部环境也与Ti-MWW的环境不同。 Ti-YNU-1的形成高度依赖于合成凝胶中的Si / Ti比,并且可能与通过酸处理去除约80%的模板分子有关煅烧前对催化性能的广泛评估各种钛硅酸盐对不同环烯烃的氧化作用表明Ti-YNU-1的行为类似于12元环(MR)沸石。结果进一步证实,孔径分布在6.7 A附近存在一个强峰Ti-YNU-1样品的Ar吸附曲线,但Ti-MWW样品的Ar吸附曲线不存在,并且随着Si / Ti比的增加,环己烯转化率增加而1-己烯转化率下降。与其他钛硅酸盐材料相比,Ti -YNU-1在大分子环烯烃以H_2O_2为氧化剂的液相环氧化中表现出高活性,选择性和稳定性。研究了几种质子传递和非质子传递溶剂对Ti-YNU-1的催化性能的影响。环己烯的环氧化表明,考虑到转化率和选择性,乙腈应该是选择的溶剂。

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