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干胶法合成ZSM-5/SAPO-34复合分子筛及其甲醇芳构化性能
中国石油化工股份有限公司上海石油化工研究院,绿色化工与工业催化国家重点实验室,上海 201208
Synthesis of ZSM-5/SAPO-34 Composite Molecular Sieves by Dry-Gel Conversion and Its Performance in Methanol-to-Aromatic Reaction
State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Shanghai Research Institute of Petrochemical Technology, SINOPEC, Shanghai 201208, China
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摘要 采用干胶法合成了ZSM-5/SAPO-34复合分子筛。研究了干胶组成、干胶处理条件和晶化时间对复合分子筛的影响。并以甲醇制芳烃为探针反应,考察了干胶法、包埋法和机械混合法制备的ZSM-5/SAPO-34复合分子筛的芳构化性能。结果表明,改变干胶组成可调节ZSM-5/SAPO-34复合分子筛中SAPO-34分子筛的含量;温和的凝胶干燥条件有利于合成ZSM-5/SAPO-34复合分子筛,干燥温度过高或者干燥时间过长会导致ZSM-5/SAPO-5复合分子筛的生成;适当延长晶化时间有利于提高复合分子筛中SAPO-34分子筛的结晶度,而晶化时间延长到96 h后, SAPO-34分子筛将逐渐向SAPO-5分子筛转化;相比于包埋法和机械混合法,采用干胶法制备的复合分子筛的甲醇芳构化活性稍低,但是反应产物对二甲苯的选择性高出10%以上,具有优异的择形性能。
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陈希强
关键词 干胶法ZSM-5/SAPO-34复合分子筛甲醇制芳烃    
Abstract:ZSM-5/SAPO-34 composite molecular sieves were successfully synthesized by dry-gel conversion (DGC) method. The effects of synthesis conditions including dry-gel composition, dry-gel treatment conditions and crystallization time on the composite molecular sieves were studied. Methanol-to-Aromatic (MTA) probe reaction was used to test the catalytic performance of ZSM-5/SAPO-34 composite molecular sieves, which were prepared by DGC, embedding method (EBM) and mechanical blending (MEB) respectively. The results showed that the content of SAPO-34 in the ZSM-5/SAPO-34 composite molecular sieves could be modulated by adjusting dry-gel composition. Mild drying conditions of the dry-gel were in favor of the synthesis of ZSM-5/SAPO-34, and much too high temperature or too long drying time of the dry-gel would lead to the formation of ZSM-5/SAPO-5 composite molecular sieve. Proper prolonging of crystallization time was beneficial to improve the crystallinity of SAPO-34 zeolite in the composite molecular sieve, while after the crystallization time was prolonged to 96 h, the SAPO-34 would gradually be transformed into the SAPO-5. Compared to the EBM and MEB method, the aromatization activity of ZSM-5/SAPO-34 composite molecular sieves prepared by the DGC method was slightly lower, but the selectivity of the reaction product to xylene was more than 10% higher, which exhibited excellent shape-selectivity.
Key wordsdry-gel conversion    ZSM-5/SAPO-34 composite molecular sieves    methanol-to-aromatic   
收稿日期: 2018-01-30     
作者简介: 陈希强(1982—),男,工程师。E-mail: chenxq.sshy@sinopec.com。
引用本文:   
陈希强. 干胶法合成ZSM-5/SAPO-34复合分子筛及其甲醇芳构化性能[J]. 化学反应工程与工艺, 2018, 34(1): 36-42.
Chen Xiqiang. Synthesis of ZSM-5/SAPO-34 Composite Molecular Sieves by Dry-Gel Conversion and Its Performance in Methanol-to-Aromatic Reaction[J]. 化学反应工程与工艺, 2018, 34(1): 36-42.
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