摘要
分别采用溶液燃烧法(SCM)、等体积浸渍法(IMP)、水热合成法(HTP)和浸渍燃烧法(ICM)制备了Ni负载量为18%(质量分数)的Ni-Al_2O_3催化剂,通过X射线衍射(XRD)、H_2程序升温还原(H_2-TPR)、NH_3程序升温脱附(NH_3-TPD)、N_2吸附-脱附、透射电镜(TEM)等表征手段和1,4-丁炔二醇(BYD)加氢制1,4-丁二醇(BDO)评价实验,考察了制备方法对催化剂结构和性能的影响。结果显示,溶液燃烧法制备的SCM催化剂晶粒尺寸最小,仅为6.5 nm;低温还原峰面积大,峰型最为弥散;弱酸中心与强酸中心的面积比适中(3.0);孔径分布除在2～5 nm之间有明显的介孔外,在10～30 nm之间还有较为弥散的分布,即具有典型的介孔-介孔多级孔道结构。评价结果表明,SCM催化剂性能最好,BYD转化率为90.75%;BDO选择性为93.84%,收率也高达85.16%。这与活性组分晶粒尺寸小、低温还原峰面积大、弱酸中心与强酸中心比例适中、以及具有多级孔道结构和比表面积高达97.40 m^2/g有关。
Ni-Al2O3 catalysts with Ni mass fraction of 18% were prepared by solution combustion method (SCM),impregnation method (IMP),hydrothermal synthesis method (HTP) and impregnation combustion method (ICM),respectively.X-ray diffraction (XRD),H 2 temperature programmed reduction (H 2-TPR),NH 3 temperature programmed desorption (NH 3-TPD),N 2 adsorption-desorption curves,transmission electron microscope (TEM) and were introduced to investigate the structure properties.And the prepared catalysts were evaluated by the 1 ,4-butynediol (BYD) hydrogenation to produce 1 ,4-butanediol (BDO).Results show that the SCM catalyst is of the smallest grain size of only 6.5 nm,with the largest low-temperature reduction peak area,which indicates the most highly dispersed active components.The ratio of the weak acid centers to the strong ones was moderate (3.0).Besides the 2-5 nm pores observed in SCM catalyst,there was a wide pore size distribution between 10 nm and 30 nm,which means SCM catalyst has typical mesoporous-mesoporous multi-stage pore structure.Evaluation results show that the performance of SCM catalyst was the best one,with BYD conversion of 90.75%,BDO selectivity of 93.84%,and BDO yield of 85.16%,respectively.The well performance of the SCM catalyst is correlated to the small grain size of the active component,the large area of the low temperature reduction peak,the moderate ratio of weak acid centers to strong ones,the multi-stage pore structure and high specific surface area up to 97.40 m 2/g.
作者
莫文龙
郑霜
马亚亚
马凤云
艾沙.努拉洪
席龙飞
MO Wenlong;ZHENG Shuang;MA Yaya;MA Fengyun;AISHA·Nulahong;XI Longfei(Key Laboratory of Coal Clean Conversion & Chemical Engineering Process (Xinjiang Uyghur Autonomous Region),College of Chemistry and Chemical Engineering,Xinjiang University,Urumqi 830046,China)
出处
《石油学报（石油加工）》
EI
CAS
CSCD
北大核心
2019年第2期252-260,M0004,共10页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家高技术研究发展计划("863"计划)项目(2015AA050502)
新疆维吾尔自治区重点研发计划项目(2017B02012)
新疆大学自然科学基金项目(BS160221)
新疆大学2017年度自治区级大学生创新创业训练计划项目(201710755077)资助
