HZSM-5分子筛的制备、表征及其催化转化CH3Br为芳烃的研究
首发时间:2010-01-29
摘要:本文以正丁胺为模板剂,采用水热晶化法成功合成了ZSM-5分子筛,在固定床反应装置上评价了其对溴甲烷转化为芳烃的催化性能,系统考察了投料硅铝比、碱度、氯化钠添加量、晶种、晶化时间等因素对ZSM-5分子筛的收率和催化性能的影响。结果表明:当投料中SiO2/Al2O3为70,正丁胺(BTA)/SiO2为0.2847,Na2O/SiO2为0.1237,H2O/SiO2为37.4,NaCl/Al2O3为60,添加自制晶种为5 wt.% /SiO2,晶化条件为100℃/24 h, 170℃/24 h时,合成的HZSM-5分子筛结晶完好, 晶粒尺寸为0.3-0.8 μm, 对溴甲烷转化为芳烃具有较好的催化活性、选择性和稳定性。采用XRD、SEM、NH3-TPD等手段对部分合成的分子筛进行了表征,并关联了催化剂的构效关系,发现HZSM-5分子筛的结晶度越高或者晶粒较小,有利于改善其催化活性、选择性和稳定性;而且分子筛表面酸性适中时有利于溴甲烷高效转化为芳烃。
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Synthesis and characterization of HZSM-5 zeolite and its catalytic application in the conversion of CH3Br into aromatics
Abstract:This paper describes the synthesis, characterization and catalytic application of H-ZSM-5 zeolites. The H-ZMS-5 was prepared by hydrothermal crystallization method, using n-butylamine (BTA) as template. The as-prepared materials were evaluated for the conversion of CH3Br into aromatics in a fixed-bed reactor. The effects of batch SiO2/Al2O3 ratio, alkalinity, NaCl/Al2O3 ratio, seed crystals and crystallization time on the yield, structure/texture, and catalytic performance of ZSM-5 zeolites were systematically studied. Using the optimum sol (SiO2/Al2O3=70, BTA/SiO2=0.2847, Na2O/SiO2=0.1237, H2O/SiO2=37.4, NaCl/Al2O3=60, and Seed crystals/SiO2=5wt.%), and the preferable crystallization conditions of 100oC/24h-170oC/24h, HZSM-5 zeolites with high crystallinity and a small size of 0.3-0.8 μm were obtained and found to exhibit good activity, selectivity and stability towards the CH3Br conversion into aromatics. The structure-catalytic efficiency relationships of the catalysts were also clarified by the characterization techniques of XRD, SEM, and NH3-TPD. It can be deduced that higher crystallinity or smaller crystal size will favor the improvement of the catalytic activity, selectivity and stability of HZSM-5. Moreover, efficient conversion of methyl bromide into aromatics can be obtained only when the surface acidity of the HZSM-5 zeolite is moderate.
Keywords: ZSM-5 zeolite methyl bromide aromatic hydrocarbon.
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