Ni/Fe3O4催化乙酰丙酸甲酯加氢制γ-戊内酯  

Preparation ofγ-valerolactone by hydrogenation of methyl levulinate over Ni/Fe3O4 catalysts

作　　者：徐天晓 王磊 高歌[1] XU Tian-xiao;WANG Lei;GAO Ge(School of Chemistry and Chemical Engineering,Xinjiang University,Urumqi 830046,China;School of Chemistry and Chemical Engineering,Lingnan Normal University,Zhanjiang 524408,China)

机构地区：[1]新疆大学化学化工学院,新疆乌鲁木齐830046 [2]岭南师范学院化学化工学院,广东湛江524048

出　　处：《天然气化工—C1化学与化工》2020年第3期27-32,44,共7页Natural Gas Chemical Industry

基　　金：国家自然科学基金(21808192、U1703128)。

摘　　要：利用共沉淀法制备了一系列不同Ni含量的Ni/Fe3O4催化剂,用粉末X射线衍射(XRD)、X射线光电子能谱(XPS)、H2程序升温还原(H2-TPR)等方法对催化剂进行表征,并考察了在乙酰丙酸甲酯(ML)液相加氢制γ-戊内酯(GVL)反应中实验条件对其催化性能的影响。实验结果显示,20%Ni/Fe3O4催化剂活性最高,在优化的反应条件:180℃、6.0MPa、反应5.0h,ML浓度为2.25mol/L时,其ML转化率和GVL选择性分别达到72.22%和100%,而相同反应条件下,对比的16%Ni/Al2O3催化剂,ML转化率和GVL选择性分别为21.94%和100%。XRD表征结果说明,20%Ni/Fe3O4催化剂中活性组分Ni-Fe合金结晶程度最高,XPS和H2-TPR表征结果表明,Ni和Fe金属间协同作用强是催化剂具有突出催化活性的主要原因。A series of Ni/Fe3O4 catalysts with different content of Ni species were prepared by co-precipition method,and were characterized by XRD,XPS and H2-TPR.The effect of experimental conditions on the catalytic performance of the catalysts in liquid phase hydrogenation of methyl levulinate(ML)toγ-valerolactone(GVL)was investigated.The results showed that the 20%Ni/Fe3O4 catalyst exhibited the highest activity under the optimized reaction conditions(180℃,6 MPa,5h,2.25mol/L ML),achieving 72.22%conversion of ML and 100%selectivity to GVL,while the ML conversion and GVL selectivity were 21.94%and 100%,respectively,for the compared catalyst 16%Ni/Al2O3 under the same conditions.The XRD result indicated that the crystallization degree of Ni-Fe alloy is the highest in 20%Ni/Fe3O4 catalyst.The XPS and H2-TPR results indicated that the strong synergy between metallic nickel and iron is the main reason that the catalyst has high catalytic activity.

关 键 词：Ni-Fe双金属催化剂 乙酰丙酸甲酯 加氢 γ-戊内酯 

分 类 号：O643.38[理学—物理化学] TQ426[理学—化学]