核壳型介微孔复合分子筛MCM-41@TS-1的合成及其催化性能  

Synthesis and Catalytic Performance of Core-shell Micro-Mesoporous Composite Zeolite MCM-41@TS-1 Catalysts

作　　者：王英杰 李博文 何佳丽 王星 许佳洁 李佳妮 吴妹 蒋金龙 丑凌军[2] 宋焕玲[2] WANG Yingjie;LI Bowen;HE Jiali;WANG Xing;XU Jiajie;LI Jiani;WU Mei;JIANG Jinlong;CHOU Lingjun;SONG Huanling(Faculty of Chemical Engineering,Huaiyin Institute of Technology,Key Laboratory for Palygorskite Science and Applied Technology of Jiangsu Province,Huai'an 223003,Jiangsu China;State Key Laboratory for Oxo Synthesis and Selective Oxidation,Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences,Lanzhou 730000,China)

机构地区：[1]淮阴工学院化学工程学院,江苏省凹土资源利用重点实验室,江苏淮安223003 [2]中国科学院兰州化学物理研究所,羰基合成与选择性氧化国家重点实验室,兰州730000

出　　处：《硅酸盐学报》2022年第10期2611-2621,共11页Journal of The Chinese Ceramic Society

基　　金：江苏省青蓝工程“优秀青年骨干教师”项目;江苏省高校自然科学研究重大项目(20KJA530002);江苏省凹土资源利用重点实验室自主课题(HPZ202001);江苏省医用材料及高端医疗器械工程研究中心开放课题(CEMD-2001);江苏省研究生科研与实践创新计划项目(SJCX21_1498)。

摘　　要：为解决具有MFI拓扑结构的沸石类分子筛(TS-1)孔道适用性窄的问题,以原位晶化法合成核壳型介微孔复合分子筛xMCM-41@TS-1。结果表明:xMCM-41@S-1具有结晶完整的微孔核相和孔道规整的介孔壳层,可以有效提高反应传质效率、降低扩散阻力,促使活性钛中心的有效利用,同时介孔复合结构有利于缩短物质的扩散路径,使微孔中的积碳前驱体能及时扩散到表面。催化性能结果表明,xMCM-41-41@TS-1在丁二烯环氧化和环己烷氧化反应中的催化活性分别可以达到TS-1的3倍和2倍,且循环稳定性远高于TS-1。To solve the problem of a narrow pore applicability of zeolite molecular sieves with MFI topology(TS-1),a core-shell mesoporous composite molecular sieve xMCM-41@TS-1 was synthesized by an in-situ crystallization method.The results show that xMCM-41@TS-1 has a well-crystallized microporous core and mesoporous shell with regular pores,thus effectively improving the reaction mass transfer efficiency,reducing the diffusion resistance,and promoting the effective utilization of active titanium centers.Also,the core-shell mesoporous composite structure is beneficial to shortening the diffusion path of the material,so that the carbon deposition precursor in the microporous can diffuse to the surface in time.According to the catalytic performance results,the catalytic activity of xMCM-41-41@TS-1 in butadiene epoxidation and cyclohexane oxidation can reach 3 times and 2 times greater than that of TS-1,respectively,and the cycle stability is greater than that of TS-1.

关 键 词：核壳结构 介微孔复合结构 活性钛中心 丁二烯环氧化 环己烷氧化 

分 类 号：TQ028.8[化学工程]