毕坤豪,马亚亚,莫文龙,迪丽努尔·塔力普,马凤云,艾沙·努拉洪.Zn/HZSM-5催化剂上正/异丁烷芳构化反应性能研究[J].分子催化编辑部,2018,32(1):35-45
Zn/HZSM-5催化剂上正/异丁烷芳构化反应性能研究
Effect of Isobutane Content on the Aromatic Reaction Performance of n-Butane on Zn/HZSM-5 Catalysts
投稿时间:2017-10-19  修订日期:2017-11-30
DOI:
中文关键词:  锌改性  分子筛  丁烷  芳构化  脉冲微反应装置
英文关键词:zinc modifycation  zeolite  butane  aromatization  mini-scale pulse reactor device
基金项目:国家自然科学基金(21563028):金属改性介孔ZnO/ZSM-5复合催化剂的制备及用于合成气制乙酸甲酯体系的研究
作者单位E-mail
毕坤豪 新疆大学 煤炭清洁转化与化工过程自治区重点实验室, 新疆大学化学化工学院, 新疆 乌鲁木齐 830046  
马亚亚 新疆大学 煤炭清洁转化与化工过程自治区重点实验室, 新疆大学化学化工学院, 新疆 乌鲁木齐 830046  
莫文龙 新疆大学 煤炭清洁转化与化工过程自治区重点实验室, 新疆大学化学化工学院, 新疆 乌鲁木齐 830046  
迪丽努尔·塔力普 新疆大学 煤炭清洁转化与化工过程自治区重点实验室, 新疆大学化学化工学院, 新疆 乌鲁木齐 830046  
马凤云 新疆大学 煤炭清洁转化与化工过程自治区重点实验室, 新疆大学化学化工学院, 新疆 乌鲁木齐 830046  
艾沙·努拉洪 新疆大学 煤炭清洁转化与化工过程自治区重点实验室, 新疆大学化学化工学院, 新疆 乌鲁木齐 830046 aisa705@163.com 
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中文摘要:
      采用脉冲微反装置评价了纯正丁烷(原料I)、含有少量异丁烷的混合丁烷(原料Ⅱ)和富含异丁烷的混合丁烷(原料Ⅲ)在锌改性的纳米HZSM-5催化剂上的反应性能.通过红外吸附正丁烷羟基谱图,研究了Zn/HZSM-5催化剂的活性中心.结果表明,反应温度为550℃时,两种混合丁烷在催化剂上的转化率和芳构化选择性都远高于纯正丁烷.即异丁烷比例越高,反应效果越好,说明二者共存时,异丁烷在竞争反应中抑制了正丁烷的转化.另外,芳烃选择性均随Zn负载量的增加而增加.这是因为异丁烷在酸中心作用下脱氢生成叔碳正离子的能力高.而正丁烷的活化方式可能同时存在脱氢活化和脱甲基活化.因此,以工业碳四饱和烃为芳构化原料时,正丁烷和异丁烷可不必分离,直接以混合原料进行芳构化反应.
英文摘要:
      Reactivity and aromatization selectivity of pure butane (raw material Ⅰ), mixed butane (small iso-butane, raw material Ⅱ) and isobutane-rich mixed butane (raw material Ⅲ) on modified nanostructured HZSM-5 catalyst were investigated in this paper. The active center of Zn/HZSM-5 catalyst was studied by infrared absorption n-butane hydroxy spectrum. Results showed that the conversions of the two kinds of mixed butane on zinc modified HZSM-5 catalyst were much higher than that of pure n-butane at the reaction temperature of 550℃, and the selectivity of aromatization was also higher than pure n-butane. The higher the proportion of isobutane, the better the reaction performance, which indicated that isobutane inhibited the conversion of n-butane in the competitive reaction when isobutane and n-butane coexisted. In addition, aromatic selectivity increased with Zn loading increase. This might be related to the ability of isobutane to dehydrogenate to tertiary cations under the action of acid sites, which was higher than n-butane. However, the activation mechanism of n-butane might be dehydrogenation and demethylation. The results also showed that, in the industrial carbon tetra-saturated hydrocarbons for the aromatization of raw materials, n-butane and isobutane did not have to be separated, and could be directly as mixed carbon tetra-hydrocarbon aromatization to conform the reaction.
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