Zr对Ni/Ti_(3)C_(2)催化剂结构及催化肉桂醛选择加氢的影响  

Effect of Zr on the structure and the hydrogenation properties for cinnamaldehyde of Ni/Ti_(3)C_(2) catalyst

作　　者：李孟函 苏通明 秦祖赠 纪红兵 LI Menghan;SU Tongming;QIN Zuzeng;JI Hongbing(School of Chemistry and Chemical Engineering,Guangxi Key Laboratory of Petrochemical Resourse Processing and Process Intensification Technology,Guangxi University,Nanning 530004,Guangxi,China;Zhejiang Green Petrochemical and Light Hydrocarbon Transformation Research Institute,Zhejiang University of Technology,Hangzhou 310014,Zhejiang,China)

机构地区：[1]广西大学化学化工学院,广西石化资源加工及过程强化技术重点实验室,广西南宁530004 [2]浙江工业大学浙江绿色石化与轻烃转化研究院,浙江杭州310014

出　　处：《化工进展》2024年第11期6184-6194,共11页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(21968007);广西自然科学基金(2020GXNSFDA297007);广西石化资源加工及过程强化技术重点实验室开放课题(2023K002)。

摘　　要：采用KBH4还原法制备了Zr负载量为5%~15%(质量分数)的NiZr/Ti_(3)C_(2)(MXene)催化剂,通过结构表征结合催化剂上肉桂醛选择加氢活性测试,研究添加Zr对Ni/Ti_(3)C_(2)催化剂结构及其催化肉桂醛选择加氢的影响。结果表明,随着Zr负载量的增加,能减少Ni金属颗粒团聚,载体Ti_(3)C_(2)的层状结构清晰,催化剂比表面积先增加后减小,表面酸性位点的种类变化不大,其中,10Ni10Zr/Ti_(3)C_(2)催化剂的活性金属Ni的平均粒径最小且具有最大比表面积(132.8m^(2)/g),其Br?nsted酸强度和稳定性略微增强,Lewis酸强度和稳定性降低,表现出最佳催化性能;在同一反应条件下,与10Ni/Ti_(3)C_(2)催化剂相比,10Ni10Zr/Ti_(3)C_(2)催化剂上肉桂醛的转化率从92.57%提高到98.34%,苯丙醛的选择性从91.15%增加到94.81%,苯丙醛收率提高了8.86%,在循环实验中表现出较高的稳定性。NiZr/Ti_(3)C_(2)(Ni mass fraction 10%)catalysts with a Zr supporting amount of 5%—15%were prepared by a KBH4 reduction method,and the effect of the Zr addition on the structure of the Ni/Ti_(3)C_(2) catalyst and its catalytic activities for cinnamaldehyde selective hydrogenation were investigated by characterization combined with cinnamaldehyde selective hydrogenation on the catalysts.The results showed that with the increase in the Zr supporting amount,the agglomeration of Ni metal particles decreased,and the Ti_(3)C_(2) support of the catalysts exhibited a well-defined layer structure.The specific surface area of the catalysts increased first and then decreased,while the types of surface acid sites changed little.Among them,the 10Ni10Zr/Ti_(3)C_(2) catalyst exhibited a smallest average Ni active metal particle size and a maximum specific surface area of 132.8m2/g,as well as the Brønsted acid strength and stability was slightly enhanced,and the Lewis acid strength and stability was decreased,showing the optimal catalytic activity.Under the same reaction conditions,on the 10Ni10Zr/Ti_(3)C_(2) catalysts,the cinnamaldehyde conversion was increased from 92.57%to 98.34%,the hydrocinnamaldehyde selectivity was increased from 91.15%to 94.81%,the hydrocinnamaldehyde yield was increased by 8.86%compared with the 10Ni/Ti_(3)C_(2) catalyst.Furthermore,the 10Ni10Zr/Ti_(3)C_(2) exhibited a high stability in cycling experiments.

关 键 词：NiZr/Ti_(3)C_(2) 催化 肉桂醛 选择加氢 KBH4还原 

分 类 号：TQ531.7[化学工程—煤化学工程]