Chemical Industry and Engineering Progree ›› 2015, Vol. 34 ›› Issue (09): 3331-3336.DOI: 10.16085/j.issn.1000-6613.2015.09.019

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Study on the catalytic process of 1,3-butadiene from ethanol and acetaldehyde with ZrO2/SiO2 catalyst

LI Xiang1,2, LIU Zongzhang1,2   

  1. 1. R&D Center for Petrochemical Technology, Tianjin University, Tianjin 300072, China;
    2. Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University, Tianjin 300072, China
  • Received:2014-11-21 Revised:2015-01-23 Online:2015-09-05 Published:2015-09-05

ZrO2/SiO2催化乙醇乙醛制备1,3-丁二烯

李翔1,2, 刘宗章1,2   

  1. 1. 天津大学石油化工技术开发中心, 天津 300072;
    2. 天津大学绿色合成与转化教育部重点实验室, 天津 300072
  • 通讯作者: 刘宗章。E-mail:zzliu@tju.edu.cn
  • 作者简介:李翔(1989-),男,硕士研究生,研究方向为生物质能源及应用催化。

Abstract: Three preparation methods,dry-mixed,impregnation and sol-gel methods,of ZrO2/SiO2 were introduced to study the formation of 1,3-butadiene from bioethanol and acetaldehyde. Catalyst testing device was introduced and the best selectivity of 1,3-butadiene is 64.77% which is obtained by sol-gel method. To study the quantity and quality of acid sites and surface structure of catalysts,thermogravimetry,temperature programmed desorption,X-ray diffraction and transmission electron microscopy were conducted. Zr-Si shows a high selectivity for 1,3-butadiene and corresponding reason was illustrated. NH3-TPD indicates the high intensity of strong acid sites and XRD indicates the high dispersed of ZrO2,while both attributes to the good activity of ZrO2-SiO2. The effects of preparation parameters on sol-gel Zr-Si were also investigated. The result shows that the best roasting temperature,concentration of nitric acid and temperature of agitation are 650℃,2mol/L,30℃,respectively.

Key words: 1,3-butadiene, ZrO2/SiO2, alcohol, acetaldehyde, catalyst, reaction

摘要: 采用干混法、浸渍法、溶胶凝胶法3种制备方法制备ZrO2/SiO2,在固定床微型反应器中进行催化剂的活性评价。通过溶胶凝胶法制备的ZrO2/SiO2对丁二烯选择性最高,达到64.77%。采用氨气程序升温脱附(NH3-TPD)、X射线衍射(XRD)、透射电镜(TEM)等手段对催化剂表面酸性以及表面结构进行了表征,结果表明锆在二氧化硅表面均匀分布有利于乙醇乙醛转化率以及对1,3-丁二烯选择性的提高,同时1,3-丁二烯的生成需要合适的酸性位。以溶胶凝胶法制备的ZrO2/SiO2为催化剂,对其制备条件进行了优化,得出最佳制备条件为焙烧温度650℃、硝酸浓度2mol/L、混合温度30℃。

关键词: 1, 3-丁二烯, ZrO2/SiO2, 醇, 乙醛, 催化剂, 反应

CLC Number: 

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