氮掺杂碳纳米管担载CuCoCe对合成气制低碳醇的催化性能  

Catalytic performance of CuCoCe supported on nitrogen-doped carbon nanotubes for the synthesis of higher alcohols from syngas

作　　者：杨展董 马恩娟 张乾[2] 栾春晖[1] 黄伟[2,3] YANG Zhan-dong;MA En-juan;ZHANG Qian;LUAN Chun-hui;HUANG Wei(College of Chemistry and Chemical Engineering,Taiyuan University of Technology,Taiyuan 030024,China;Key Laboratory of Coal Science and Technology of Education Ministry and Shanxi Province,Taiyuan University of Technology,Taiyuan 030024,China;Coal Conversion Technology&Engineering Co.,Ltd.,TYUT,Taiyuan 030024,China)

机构地区：[1]太原理工大学化学化工学院,山西太原030024 [2]太原理工大学煤科学与技术教育部和山西省重点实验室,山西太原030024 [3]山西太原理工煤转化技术工程有限公司,山西太原030024

出　　处：《燃料化学学报》2020年第7期804-812,共9页Journal of Fuel Chemistry and Technology

摘　　要：以三聚氰胺为氮源,控制其与碳纳米管混合比例,经过高温焙烧得到不同氮含量的氮掺杂碳纳米管(xN-CNTs)载体;通过浸渍法制备x N-CNTs担载的CuCoCe催化剂,研究了氮掺杂对其催化合成气制低碳醇性能的影响。采用X射线衍射(XRD)、N2吸附-脱附、H2程序升温还原(H2-TPR)、NH3程序升温脱附(NH3-TPD)和X射线光电子能谱(XPS)等表征手段,分析催化剂结构特性,关联了构效关系。结果表明,氮的掺杂量会影响催化剂活性组分Cu的存在状态及分散情况,减少可还原Co物种的数量,降低催化剂表面酸强度及酸量,使得长链烃类的生成受到抑制,总醇选择性明显提高。分析认为,掺杂在碳管上N的形态分布及掺杂量是影响上述因素的关键。A series of nitrogen-doped carbon nanotubes(xN-CNTs) were obtained by treating the mixture of melamine and carbon nanotubes at high temperature;the CuCoCe catalysts supported on xN-CNTs were then prepared by impregnation method and used in the synthesis of higher alcohols from syngas.The CuCoCe/xNCNTs catalysts were characterized by XRD,N2 sorption,H2-TPR,NH3-TPD and XPS and the effect of nitrogen content in xN-CNTs on the catalytic performance of CuCoCe/xN-CNTs in the higher alcohols synthesis was investigated.The results show that the content of nitrogen in xN-NTs has a significant influence on the existence and dispersion of Cu on the CuCoCe/xN-CNTs catalysts;the presence of nitrogen can reduce the number of reducible Co species and lower the acid strength and amount on the catalyst surface,which helps to suppress the long-chain hydrocarbons formation and improve total alcohol selectivity.It is proposed that the morphological distribution and doping amount of nitrogen on the carbon tubes may play a crucial role in enhancing the catalytic performance of CuCoCe/xN-CNTs in the higher alcohols synthesis.

关 键 词：氮掺杂 碳纳米管 合成气 低碳醇 CuCoCe 

分 类 号：O643.3[理学—物理化学]