介孔分子筛改性Y沸石表面的苯酚叔丁基化  

Tert-BUTYLATION OF PHENOL OVER ZEOLITE Y MODIFIED BY MESOPOROUS MATERIAL

作　　者：郭群[1] 张喜文[1,2] 马静红[1] 孙万富[2] 李瑞丰[1] 

机构地区：[1]教育部煤科学与技术重点实验室太原理工大学精细化工研究所,山西太原030024 [2]中国石化抚顺石油化工研究院,辽宁抚顺113001

出　　处：《石油学报（石油加工）》2008年第B10期213-218,共6页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：中国石化科学基金项目（107009）资助

摘　　要：通过在细小Y型沸石晶粒表面嫁接介孔分子筛的途径，对Y型沸石表面进行改性。采用X射线衍射、透射电子显微镜、低温N2吸附、NH3程序升温脱附和吡啶吸附红外光谱方法对改性样品进行了表征，并详细考察了其在苯酚叔丁基化反应中的催化性能。结果表明，优化合成条件，使Y沸石晶粒均匀地分布于介孔分子筛的孔壁之中，形成核壳／包覆结构，对沸石表面的酸性能起到调节作用，在苯酚转化率90％以上时，叔丁基苯酚的选择性达到100％。Micro-/mesoporous composite Y/MCM was successfully synthesized by grafting mesoporous material on the surface of nano-Y zeolite. The Y/MCM composites with different micro-/mesoporous component ratios were characterized by powder X-ray diffraction, transmission electron microscopy and N2 adsorption-desorption methods. The results showed the micro-and mesoporous properties of Y/MCM and its core-shell enwrapped structure. NHa temperature-programmed desorption and in-situ pyridine adsorbed infrared spectra results indicated medium and strong acid sites and the distribution of Bronsted and Lewis acid sites on the Y/MCM surface. The number of acid sites and the ratio of Bronsted to Lewis acid sites can be adjusted by changing the ratio of micro-/mesoporous component in the Y/MCM composite. During the alkylation of phenol with tert-butanol, the Y/MCM catalyst displayed higher conversion of phenol and selectivity for tert-butyl phenol than the single microporous Y or mesoporous MCM-41 catalyst. At the reaction temperature of 180℃, a high phenol conversion of 92% and tert- butyl phenol selectivity of 100% over Y/MCM are observed. The mesoporous size （2--3 nm） in the Y/MCM is beneficial to the effective diffusion of reactants and productsl obvious catalyst deactivation of Y/MCM is not observed even after reaction for 6 h. And Y/MCM can be very well recycled in the tert-butylation of phenol.

关 键 词：Y/MCM复合分子筛 苯酚 叔丁醇 烷基化 叔丁基苯酚 2 4-二叔丁基苯酚 

分 类 号：O643[理学—物理化学]