Ni/Ti_(3)C_(2)(MXene)催化剂制备及催化肉桂醛选择加氢性能  

Preparation of Ni/Ti_(3)C_(2)(MXene)catalyst and its catalytic performance for selective hydrogenation of cinnamaldehyde

作　　者：李孟函 苏通明[1] 罗轩[1] 谢新玲[1] 秦祖赠[1] 纪红兵[1,2] LI Menghan;SU Tongming;LUO Xuan;XIE Xinling;QIN Zuzeng;JI Hongbing(School of Chemistry and Chemical Engineering,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：《精细化工》2024年第10期2238-2248,共11页Fine Chemicals

基　　金：国家自然科学基金项目(21968007);广西自然科学基金项目(2020GXNSFDA297007);广西八桂学者专项基金项目。

摘　　要：以氢氟酸为蚀刻剂,Ti_(3)AlC_(2)为原料制备的多层Ti_(3)C_(2)(MXene)为载体,采用KBH4还原法制备了Ni负载量(即Ni的理论质量分数,下同)5%~20%的Ni/Ti_(3)C_(2)催化剂,通过XRD、FTIR、SEM、N_(2)吸附-脱附、NH_(3)-TPD、CO_(2)-TPD对Ni/Ti_(3)C_(2)进行了表征,考察了其催化肉桂醛选择加氢的性能。结果表明,Ni负载量为10%的Ni/Ti_(3)C_(2)催化剂(记为10Ni/Ti_(3)C_(2))具有最佳的性能,其Ni金属颗粒均匀负载在Ti_(3)C_(2)表面上,层状结构清晰,比表面积为9.6 m^(2)/g,具有最小的金属Ni平均粒径(43.59 nm)和最高的分散度(0.21%)。随着Ni负载量的增加,Ni/Ti_(3)C_(2)的比表面积和酸位点强度逐渐增加,表面酸性位点种类变化不大,10Ni/Ti_(3)C_(2)具有强Lewis酸位点(NH_(3)脱附峰在511℃左右),热稳定性较好。在H_(2)压力2.0 MPa、30 mL异丙醇为溶剂、反应温度120℃的条件下,0.5000 g 10Ni/Ti_(3)C_(2)催化1.0000 g肉桂醛选择加氢反应3.0 h,肉桂醛转化率和苯丙醇选择性分别为100%和99.29%;在4次循环中,10Ni/Ti_(3)C_(2)表现较高的催化稳定性,肉桂醛转化率100%,苯丙醇选择性99.29%~92.07%。A series of Ni/Ti_(3)C_(2)catalysts with Ni loading(theoretical mass fraction of Ni,the same below)of 5%~20%were prepared by KBH4 reduction method from multilayered Ti_(3)C_(2)(MXene)carrier,which was obtained using hydrofluoric acid as etchant and Ti_(3)AlC_(2) as raw material,characterized by XRD,FTIR,SEM,N_(2)adsorption-desorption,NH_(3)-TPD,CO_(2)-TPD and analyzed for their catalytic performance for selective hydrogenation of cinnamaldehyde.The results showed that The Ni/Ti_(3)C_(2)catalyst with 10%Ni loading(denoted as 10Ni/Ti_(3)C_(2))exhibited the best performance,with a well-defined layer structure and its Ni metal particles uniformly loaded on the surface of Ti_(3)C_(2),a specific surface area of 9.6 m^(2)/g,the smallest average metallic Ni particle size(43.59 nm)and the highest dispersion(0.21%).The specific surface area and acid site strength of Ni/Ti_(3)C_(2)increased gradually with the increment of Ni loading,but the types of acid sites on the surface showed no much change.10Ni/Ti_(3)C_(2)exhibited strong Lewis acid sites(NH_(3) desorption peak at approximately 511℃)and good thermal stability.Under the conditions of H_(2) pressure 2.0 MPa,30 mL isopropyl alcohol as solvent and reaction temperature 120℃,0.5000 g 10Ni/Ti_(3)C_(2)catalyzed 1.0000 g cinnamaldehyde for selective hydrogenation for 3.0 h,the cinnamaldehyde conversion and phenylpropyl alcohol selectivity reached 100%and 99.29%,respectively.In four cycles,10Ni/Ti_(3)C_(2)exhibited high catalytic stability with 100%cinnamaldehyde conversion and 99.29%~92.07%hydrocinnamyl alcohol selectivity.

关 键 词：MXene Ni/Ti_(3)C_(2) 催化 肉桂醛 苯丙醇 选择加氢 KBH4还原 

分 类 号：TQ426[化学工程]