NiAl复合催化剂催化乙酰丙酸加氢制备γ-戊内酯  

Hydrogenation of levulinic acid to γ-valerolactone catalyzed by NiAl composite catalysts

作　　者：吕奇珅 李伟乐 唐兴 孙勇 曾宪海 林鹿 LYU Qishen;LI Weile;TANG Xing;SUN Yong;ZENG Xianhai;LIN Lu(College of Energy,Xiamen University,Xiamen 361102,Fujian,China;Fujian Engineering and Research Center of Clean and High-Valued Technologies for Biomass,Xiamen 361102,Fujian,China)

机构地区：[1]厦门大学能源学院,福建厦门361102 [2]福建省生物质清洁高值化技术工程研究中心,福建厦门361102

出　　处：《精细化工》2023年第9期1985-1993,2063,共10页Fine Chemicals

基　　金：广东省重点领域研发计划项目(2020B0101070001);国家自然科学基金项目(22078275、21978248);厦门大学校长基金(20720190014)。

摘　　要：以Ni(NO_(3))_(2)·6H2O、Al(NO_(3))_(3)·9H_(2)O和尿素为原料,通过尿素水解法合成了一系列NiAl复合催化剂,并将其用于乙酰丙酸(LA)加氢反应,实现了在1,4-二氧六环体系中、温和条件下高效催化LA转化为高价值生物质基平台化合物γ-戊内酯(GVL)。采用XRD、H_(2)-TPR、SEM、XPS对催化剂进行了表征。结果表明,NiAl复合催化剂的高催化活性主要来自于Ni^(0)金属位点以及Ni^(0)与Al2O3的相互作用。不同的Ni/Al物质的量比直接影响金属Ni颗粒的粒径大小和分布,较大或较小Ni/Al物质的量比均会降低催化剂的活性。当n(Ni)∶n(Al)=2∶1、反应温度为140℃、H_(2)压力为3 MPa、反应时间为2 h时,GVL产率可达100%。A series of NiAl composite catalysts,synthesized from Ni(NO_(3))_(2)·6H_(2)O,Al(NO_(3))_(3)·9H_(2)O and urea via urea hydrolysis reaction and characterized by XRD,H2-TPR,SEM,and XPS,were applied in the hydrogenation reaction of levuliniv acid(LA).High-efficiency catalytic conversion of LA into high-value biomasum-based platform compound γ-valerolactone(GVL)in 1,4-dioxane system under mild conditions was achieved.The results showed that the high catalytic activity of NiAl composite catalysts was primarily attributed to the Ni^(0)metal sites and the interaction between Ni and AlO_(3).The size and distribution of metal Ni particles were directly affected by the molar ratio of Ni/Al,and the activity of the catalyst was reduced when the molar ratio of Ni/Al was too large or small.Under the conditions of n(Ni):n(Al)=2:1,140℃,3 MPa H_(2) and 2 h,the yield of GVL could achieve 100%.

关 键 词：非贵金属催化剂 乙酰丙酸 加氢还原 γ-戊内酯 1 4-二氧六环 催化技术 

分 类 号：TQ235[化学工程—有机化工]