固相合成法制备甲苯甲醇烷基化的ZSM-5@silicalite-1核壳分子筛催化剂Preparation of ZSM-5@silicalite-1 core-shell zeolite catalysts by solid-phase synthesis method for alkylation of toluene with methanol
龙奕华,刘闯,武晓珂,杨艳伟,王正宝
摘要(Abstract):
以ZSM-5晶体为核,将二氧化硅(SiO2)、四丙基溴化铵(TPABr)和氟化铵(NH4F)固体研磨成粉作为原料,采用固相合成法制备ZSM-5@silicalite-1核壳分子筛催化剂;并借助X射线衍射仪(XRD)、扫描电镜(SEM)、X射线能谱仪(EDS)、透射电子显微镜(TEM)、X射线光电子能谱仪(XPS)和2,6-二叔丁基吡啶吸附红外光谱(DTBPy-IR)等手段,对核壳分子筛催化剂的结构进行表征,考察其对甲苯甲醇烷基化反应的催化性能。结果表明,通过固相合成法,ZSM-5核晶体外表面外延生长出了全硅MFI型分子筛(silicalite-1)壳层,且该核壳催化剂表现出较高的对二甲苯(PX)选择性。还考察了核晶体尺寸对核壳结构催化剂的影响。研究发现,随着核晶体尺寸的增大,核壳分子筛的甲苯转化率下降、PX选择性上升。作为对比,采用传统水热合成法(液相合成法)制备了核壳分子筛,考察了核晶体尺寸的影响。研究发现,随核晶体尺寸增大,水热合成法制备的核壳分子筛的甲苯转化率呈现先减后增的趋势,PX选择性则相反。由此得出,固相合成法对于较大核晶体的壳层生长具有更好的适用性,表现出广阔的应用前景。
关键词(KeyWords): MFI型分子筛;核壳结构;甲苯甲醇烷基化;对二甲苯;固相合成法;核晶体尺寸
基金项目(Foundation): 国家自然科学基金(21676238)
作者(Author): 龙奕华,刘闯,武晓珂,杨艳伟,王正宝
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