CuNiAl催化乙酰丙酸转移加氢制备γ-戊内酯的研究  

Catalytic transfer hydrogenation of levulinic acid to γ-valerolactone over CuNiAl catalysts

作　　者：张子健 遇治权[1] 王瑶[1,2] 黄卉 刘颖雅 孙志超 王安杰[1,2] ZHANG Zi-jian;YU Zhi-quan;WANG Yao;HUANG Hui;LIU Ying-ya;SUN Zhi-chao;WANG An-jie(State Key Laboratory of Fine Chemicals,Dalian University of Technology,Dalian 116024,China;Liaoning Provincial Key Laboratory of Petrochemical Technology and Equipment,Dalian 116024,China)

机构地区：[1]大连理工大学精细化工国家重点实验室,辽宁大连116024 [2]辽宁省省级高校石油化工技术与装备重点实验室,辽宁大连116024

出　　处：《现代化工》2021年第12期107-112,119,共7页Modern Chemical Industry

基　　金：国家自然科学基金(21972014,21473017,21603024,U1508205);科技部国家重点研发计划(2016YFE0109800);中央高校基本科研业务费(DUT19GJ205)。

摘　　要：通过共沉淀法成功合成CuNiAl-LDH前体,将其直接还原制备一系列CuNiAl催化剂,并考察其在催化乙酰丙酸转移加氢制备γ-戊内酯的反应性能,研究了活性组分、还原温度、供氢溶剂、反应温度和反应时间对催化性能的影响。结果表明,Cu组分加入后生成CuNi合金,显著提高了催化活性,且当n(Cu)∶n(Ni)∶n(Al)为1∶14∶5、还原温度为500℃时,催化性能最佳。以异丙醇为供氢溶剂,在170℃下反应120 min,乙酰丙酸的转化率和γ-戊内酯的选择性分别达到98.2%和83.1%。A series of CuNiAl catalysts are prepared through direct reduction of CuNiAl-LDH precursors which are obtained by coprecipitation method, and utilized to catalyze the transfer hydrogenation(CTH) of levulinic acid to produce γ-valerolactone.The effects of active components, reduction temperature, hydrogen donor, reaction temperature and reaction time on the catalytic performance of the catalysts are investigated.The results show that the addition of Cu into the catalyst can lead to generate CuNi alloy, which improve the catalytic activity greatly.CuNiAl catalyst that is made with a molar ratio of 1∶14∶5 between three elements at a reduction temperature of 500℃ exhibits the highest activity in CTH.The selectivity of γ-valerolactone reaches 83.1% and the conversion of levulinic acid reaches 98.2% when the catalyst with the highest activity is used, 2-propanol is used as the hydrogen donor and solvent, and the reaction has performed at 170℃ for 120 min.

关 键 词：CuNiAl 转移加氢 乙酰丙酸 异丙醇 γ-戊内酯 

分 类 号：O643[理学—物理化学]