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Effects of Calcination Temperature on the Acidity and Catalytic Performances of HZSM-5 Zeolite Catalysts for the Catalytic Cracking of n-Butane
作者姓名:陆江银  赵震  徐春明  段爱军  张璞
作者单位:State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing, 102249, China
基金项目:国家重点基础研究发展计划(973计划),中国科学院资助项目,the Scientific Research Key Foundation for the Returned Overseas Chinese Scholars of State Education Ministry
摘    要:The acidic modulations of a series of HZSM-5 catalysts were successfully made by calcination at different treatment temperatures, i.e. 500, 600, 650, 700 and 800 ℃, respectively. The results indicated that the total acid amounts, their density and the amount of B-type acid of HZSM-5 catalysts rapidly decreased, while the amounts of L-type acid had almost no change and thus the ratio of L/B was obviously enhanced with the increase of calcination temperature (excluding 800 ℃). The catalytic performances of modified HZSM-5 catalysts for the cracking of n-butane were also investigated. The main properties of these catalysts were characterized by means of XRD, N2 adsorption at low temperature, NH3-TPD, FTIR of pyridine adsorption and BET surface area measurements. The results showed that HZSM-5 zeolite pretreated at 800 ℃ had very low catalytic activity for n-butane cracking. In the calcination temperature range of 500-700 ℃, the total selectivity to olefins, propylene and butene were increased with the increase of calcination temperature, while, the selectivity for arene decreased with the calcination temperature.The HZSM-5 zeolite calcined at 700 ℃ produced light olefins with high yield, at the reaction temperature of 650 ℃ the yields of total olefins and ethylene were 52.8% and 29.4%, respectively. Besides, the more important role is that high calcination temperature treatment improved the duration stability of HZSM-5zeolites. The effect of calcination temperature on the physico-chemical properties and catalytic performance of HZSM-5 for cracking of n-butane was explored. It was found that the calcination temperature had large effects on the surface area, crystallinity and acid properties of HZSM-5 catalyst, which further affected the catalytic performance for n-butane cracking.

关 键 词:煅烧温度  n-丁烷  HZSM-5沸石催化剂  催化性能  催化裂解
收稿时间:2005-09-30
修稿时间:2005-11-11

Effects of Calcination Temperature on the Acidity and Catalytic Performances of HZSM-5 Zeolite Catalysts for the Catalytic Cracking of n-Butane
Jiangyin Lu,Zhen Zhao,Chunming Xu,Aijun Duan,Pu Zhang.Effects of Calcination Temperature on the Acidity and Catalytic Performances of HZSM-5 Zeolite Catalysts for the Catalytic Cracking of n-Butane[J].Journal of Natural Gas Chemistry,2005,14(4):213-220.
Authors:Jiangyin Lu  Zhen Zhao  Chunming Xu  Aijun Duan  Pu Zhang
Abstract:The acidic modulations of a series of HZSM-5 catalysts were successfully made by calcined the samples at different treatment temperatures, i.e. 500, 600, 650, 700, 800℃, respectively. The results indicated that total acid amounts and density and the amount of B-type acid of HZSM-5 catalysts rapidly decreased, while the amounts of L-type acid had almost no change and thus the ratio of L/B was obviously enhanced with the increase of calcination temperature(excluding 800℃). The catalytic performances of modified HZSM-5 catalysts for the cracking of n-butane were also investigated. The main properties of these catalysts were characterized by means of XRD, N2 adsorption at low temperature, NH3-TPD, FT-IR of pyridine adsorption and BET surface area measurements. The results showed that HZSM-5 zeolite pretreated at 800℃ had very low catalytic activity for n-butane cracking. In the calcination temperature range of 500~700℃, the total selectivity of olefins, propylene and butene were increased with the increasing of calcination temperature,however, the selectivities of arene decreased. The HZSM-5 zeolite calcined at 700℃ produced light olefins with high yield, at the reaction temperature of 650℃ the yields of total olefins and ethylene were 52.8% and 29.4%, respectively. Besides, the more important role is that high calcination temperature treatment could improve the duration stability of HZSM-5 zeolites. The nature of calcination temperature effecting on the physico-chemical properties and catalytic performance of HZSM-5 for cracking of n-butane were explored. It was found that the calcination temperature had large effects on the surface area, crystallinity and acid properties of HZSM-5 catalyst, which further affected the catalytic performance for n-butane cracking.
Keywords:HZSM-5 zeolite catalyst  acidic modification  calcination temperature  n-butane  catalytic cracking  olefin
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