三乙醇胺改性Cu/Zn/Al类水滑石衍生氧化物催化合成气制备低碳醇
Synthesis of Higher Alcohols from Syngas over Cu/Zn/Al Hydrotalcite-Derived Oxides Modified by Triethanolamine
作者单位E-mail
程淑艳 太原理工大学煤科学与技术教育部和山西省重点实验室, 太原 030024
山西大学环境工程系, 太原 030013 
 
郝艳红 山西大学环境工程系, 太原 030013  
寇佳伟 太原理工大学煤科学与技术教育部和山西省重点实验室, 太原 030024 koujiawei2015@163.com 
高阳艳 山西大学环境工程系, 太原 030013  
摘要: 采用共沉淀法制备Cu/Zn/Al类水滑石前驱体,并用配体三乙醇胺(TEA)对其进行改性。前驱体经焙烧后成功获得TEA改性的Cu/Zn/Al催化剂。借助XRD、FTIR、H2-TPR、CO-TPD及SEM等方法对催化剂进行表征,并将其应用于合成气制备异丁醇的活性评价反应中。结果表明,TEA的加入能够改变催化剂形貌,使催化剂表面呈松散絮状结构。TEA可使类水滑石前驱体的结构发生膨胀,其焙烧获得的催化剂中有明显的晶格扭曲和晶格缺陷。TEA对催化剂结构的改变有利于Cu/Zn/Al催化剂中CuO组分的氢还原和CO在催化剂表面的化学吸附,从而促进异丁醇的合成。当TEA的添加比例为nTEA/nZn=0.5时,TEA改性的Cu/Zn/Al催化剂的催化效果达到最佳。
关键词: 三乙醇胺  Cu/Zn/Al类水滑石  合成气  异丁醇
基金项目: 国家自然科学基金(No.21707083)资助项目
Abstract: The Cu/Zn/Al hydrotalcite-like precursor was prepared by co-precipitation method and modified by triethanolamine (TEA), and then the precursor was calcined to obtain TEA-modified Cu/Zn/Al catalysts. The catalysts were characterized by XRD, FTIR, H2-TPR, CO-TPD and SEM techniques, and their catalytic activities for isobutanol synthesis were evaluated. The results revealed that TEA can change morphology of the catalysts and form flocculent structure on the surface of the catalysts. In addition, TEA can result in structural expansion of hydrotalcite-like precursor and thus lead to structural changes in the Cu/Zn/Al catalysts, which facilitate hydrogen reduction of CuO components and CO chemisorption on the surface of the catalysts. These changes promote isobutanol synthesis. The catalytic performance of the TEA-modified Cu/Zn/Al catalysts was optimal when addition ratio of TEA reached to nTEA/nZn=0.5.
Keywords: triethanolamine  Cu/Zn/Al hydrotalcite-like compounds  syngas  isobutanol
投稿时间:2018-10-11 修订日期:2018-11-30
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程淑艳,郝艳红,寇佳伟,高阳艳.三乙醇胺改性Cu/Zn/Al类水滑石衍生氧化物催化合成气制备低碳醇[J].无机化学学报,2019,35(2):300-306.
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