摘要
在连续流动的固定床反应装置上,研究了不同硅铝比的MCM-22分子筛催化剂用于液化气中丁烯芳构化反应的催化性能。采用X射线衍射、X射线荧光光谱、低温N_2吸附-脱附及氨程序升温脱附等方法研究了MCM-22分子筛的结构及MCM-22分子筛催化剂的孔结构性质和酸性。实验结果表明,配料硅铝比(n(SiO_2):n(Al_2O_3))为30~600的MCM-22分子筛的晶化度均较高,由其制备的催化剂初始丁烯转化率均达97%以上,但催化剂的芳构化活性随反应时间的延长而降低;配料硅铝比为50~200的MCM-22分子筛催化剂表现出较高的反应稳定性;MCM-22分子筛催化剂的失活主要源于酸中心数量的减少和微孔孔道堵塞,并且两者的影响程度与MCM-22分子筛的硅铝比相关。
Aromatization of butene in liquefied petroleum gas on MCM-22 molecular sieve catalysts with different silica to alumina ratios( n( SiO2 ): n( Al2O3 ) ) were carried out in a continuous fixed bed reactor. The structural characteristics, pore structure and acidity distribution of MCM-22 molecular sieves catalysts were investigated by means of XRD, XRF, N2 adsorption-desorption at low temperature(77.4 K) and NH3-TPD. All MCM-22 molecular sieves with n( SiO2): n( Al2O3 ) from 30 to 600 are high in crystallinity. The initial butene conversion is more than 97% on all MCM-22 molecular sieves catalysts with different n (SiO2 ): n (Al2O3 ), but their aromatization activities decrease with reaction time on stream. Appreciable aromatization stability can be achieved on MCM-22 molecular sieve catalysts with proper n( SiO2 ) : n( Al2O3 ) of 50 - 200. The main reasons of catalyst deactivation are decrease of acid sites and/or blockage of pore channels, which strongly depend upon n(SiO2) : n(Al2O3) of MCM-22 molecular sieves.
出处
《石油化工》
CAS
CSCD
北大核心
2008年第1期22-28,共7页
Petrochemical Technology
基金
国家重点基础研究发展计划"973"项目(2003CB615802)
中国石油天然气股份有限公司科技风险创新项目(060511-4-3)。
关键词
MCM-22分子筛
液化气
丁烯芳构化
硅铝比
催化剂
MCM-22 molecular sieve
liquefied petroleum gas
butene aromatization
ratio of silica to alumina
catalyst