载体及镍源对镍催化剂催化苯酐选择性加氢反应的影响Effects of Support and Nickel Precursor on the Properties of Nickel Catalyst for Selective Hydrogenation of Phthalic Anhydride
刘迎新,魏作君,程向炜,严巍
摘要(Abstract)：
分别以SiO2、TiO2、TiO2-SiO2、TiO2-Al2O3和TiO2-ZrO2为载体,以硝酸镍为镍源,采用浸渍法制备出一系列镍基催化剂,考察了不同载体对镍催化剂催化苯酐选择性加氢合成苯酞性能的影响;并考察了以TiO2-ZrO2为载体,分别以硝酸镍、乙酸镍和柠檬酸镍为镍源制备的镍催化剂的加氢性能。通过BET、XRD、SEM等方法对催化剂进行了表征。结果表明,载体对镍催化剂上苯酐加氢反应的影响较大,其中复合氧化物TiO2-SiO2和TiO2-ZrO2负载的镍催化剂上Ni0活性组分晶粒度较小,分散度较高,催化剂表现出很好的催化活性和苯酞选择性。此外,以不同镍源制备的Ni/TiO2-ZrO2催化剂性能差异较明显,由乙酸镍制备的催化剂上Ni0物种粒度较大,活性较低,由硝酸镍和柠檬酸镍制备的催化剂表现出很高的催化活性和选择性,其中由柠檬酸镍制备的催化剂性能略高于硝酸镍,在实验反应条件下,苯酐转化率为97.1%,苯酞收率为92.9%。
关键词(KeyWords)： 镍催化剂;载体;镍源;苯酐;加氢;苯酞
基金项目(Foundation): 浙江省自然科学基金(Y405108);; 浙江省教育厅科技计划项目(20051409);; 浙江省工业催化重中之重学科开放基金资助项目
作者(Author): 刘迎新,魏作君,程向炜,严巍
参考文献(References)：
- [1]YANG Cui-fen(杨翠芬),ZHU Jia-ling(朱佳玲).One-step synthesis of phthalide(邻羟甲基苯甲酸内酯的一步合成)[J].Chemical World(化学世界),2000,41(8):426-427.
- [2]Hara Y,Wada K.Hydrogenation reaction of carboxylic anhydrides catalyzed by a new and highly-active cationic ruthenium complex[J].Chem Letters,1991,20(4):553-554.
- [3]Massonne K,Becker R,Neuhauser H et al.Process for preparing phthalides[P].USP:6147227,2000-11-14.
- [4]Massonne K,Becker R,Reif W et al.Process for preparing phthalides[P].USP:6028204,2000-02-22.
- [5]QI Yun-shi(戚蕴石),WANG Pei(王培),LI Ming-shi(李明时)et al.Study on catalyst for selective hydrogenation of phthalic anhydride to phthalide(苯酐选择性加氢制苯酞催化剂的研究)[J].Chinese Journal of Catalysis(催化学报),1994,15(6):409-413.
- [6]Rautanen P A,Aittamaa J R,Krause A O I.Liquid phase hydrogenation of tetralin on Ni/Al2O3[J].Chem Eng Sci,2001,56(4):1247-1254.
- [7]Suh D J,Park T J,Lee S H et al.Nickel–alumina composite aerogels as liquid-phase hydrogenation catalysts[J].J Non-Cryst Solids,2001,285(1-3):309-316.
- [8]Liu Y X,Wei Z J,Zhang J Y et al.Effects of the preparation methods on the properties of Ni-La2O3-SiO2catalysts for m-dinitrobenzene hydrogenation[J].React Kinet Catal Lett,2007,92(1):121-127.
- [9]Cabrera M I,Grau R J.Liquid-phase hydrogenation of methyl oleate on a Ni/alpha-Al2O3catalyst:A study based on kinetic models describing extreme and intermediate adsorption regimes[J].J Mol Catal A,2006,260(1-2):269-279.
- [10]LIU Ying-xin(刘迎新),WEI Zuo-jun(魏作君),CHEN Ji-xiang(陈吉祥)et al.Effects of preparation methods of support on the properties of nickel catalyst for hydrogenation of m-dinitrobenzene(载体制备方法对Ni催化剂催化间二硝基苯加氢反应的影响)[J].J Chem Eng of Chinese Univ(高校化学工程学报),2006,20(5):723-727.
- [11]HUANG Li-ming(黄立明),WU Su-fang(吴素芳).Study on the Ni supported catalysts used for hydrogenation of IPN to produce MXDA(IPN加氢制备MXDA镍负载型催化剂研究)[J].J Chem Eng of Chinese Univ(高校化学工程学报),2006,20(5):787-791.
- [12]Lensveld D J,Mesu J G,van Dillen A J et al.Synthesis and characterisation of MCM-41supported nickel oxide catalysts[J].Micropor Mesopor Mater,2001,44-45:401-407.
- [13]Kim P,Kim H,Joo J B et al.Effect of nickel precursor on the catalytic performance of Ni/Al2O3catalysts in the hydrodechlorination of1,1,2-trichloroethane[J].J Mol Catal A,2006,256(1-2):178-183.