含碳Cu-Zn-Al乙炔选择性加氢催化剂制备及性能
Preparation and Performance of Carbon-Containing Cu-Zn-Al Catalysts for Selective Hydrogenation of Acetylene
石传玮 1曾傲楠 1徐波 1刘佳明 1王安杰 2刘颖雅 2孙志超 2王瑶2
作者信息
- 1. 大连理工大学化工学院,辽宁大连 116024
- 2. 大连理工大学化工学院,辽宁大连 116024;大连理工大学精细化工国家重点实验室,辽宁大连 116024
- 折叠
摘要
采用共沉淀法制备不同Cu/Zn摩尔比铜-锌-铝水滑石前体,焙烧后经过乙炔预处理和H2还原得到CumZn3-mAl-LDO(T140-R150)催化剂(m取值为1、1.5、2、3).对上述含碳铜-锌-铝催化剂进行N2物理吸附、X射线衍射、扫描电子显微镜和透射电镜表征,研究其在大量乙烯存在时乙炔选择性加氢反应中的催化性能.结果表明:在铜-铝水滑石中引入锌,可提高前体中铜的分散度,有利于碳化铜(CuxC)加氢活性相的生成,提高乙炔选择性加氢反应的性能.催化剂最佳制备条件为:Cu/Zn摩尔比1,乙炔处理温度140 ℃,乙炔处理时间2 h,氢气还原温度150 ℃,氢气还原时间3 h.在温度100 ℃和压力0.1 MPa条件下,Cu1.5Zn1.5Al-LDO(T140-R150)催化乙炔选择性加氢反应的乙炔转化率达100％,乙烯选择性为53.9％,C4选择性为15.5％,乙烷选择性为30.6％.
Abstract
Copper-zinc-aluminum hydrotalcite precursors with different molar ratios of Cu/Zn were prepared by co-precipitation method,pretreated with acetylene and reduced in-situ with hydrogen after calcination.Then CumZn3-mAl-LDO(T140-R150)catalysts(m=1,1.5,2,3)were obtained,and further characterized by N2 physical adsorption,X-ray diffraction,scanning electron microscopy and transmission electron microscopy,which aims to investigate their catalytic performance in the selective hydrogenation of acetylene in the presence of a large amount of ethylene.The results show that the dispersion of copper in precursors can be improved by introducing zinc into Cu-Al hydrotalcite,which is beneficial to the formation of CuxC hydrogenation active phase,and improve the performance of selective hydrogenation of acetylene.The optimal preparation conditions of the catalyst are as follows:Cu/Zn molar ratio of 1,acetylene treatment temperature of 140 ℃,acetylene treatment time of 2 h,hydrogen reduction temperature of 150 ℃,and hydrogen reduction time of 3 h.At temperature of 100 ℃ and atmospheric pressure,the acetylene conversion of the Cu1.5Zn1.5Al-LDO(T140-R150)catalyst can reach 100％;the ethene selectivity,C4 selectivity and ethane selectivity is 53.9％,15.5％and 30.6％respectively.
关键词
铜-锌-铝水滑石/共沉淀法/乙炔/选择性加氢Key words
copper-zinc-aluminum hydrotalcite/coprecipitation method/acetylene/selective hydrogenation引用本文复制引用
基金项目
国家自然科学基金项目(22172015)
国家自然科学基金项目(21972017)
出版年
2024
NETL
NSTL
万方数据