采用水合肼还原法制备了镍核,并结合Stöber法制备了镧改性的核壳结构镍基纳米催化剂Ni-La@mSiO2,应用于二苯酮的选择性加氢反应.应用BET、XRD和TEM等测试手段对所制备催化剂的结构特征进行了表征.考察了反应时间对Ni-La@mSiO2作用下二苯酮选择性加氢性能的影响,发现在氢压2.5 MPa,反应温度120 ℃、反应时间120 min的条件下,二苯酮的转化率和二苯甲醇的选择性都达到90%以上;同时,催化剂经5次套用,二苯酮的转化率和二苯甲醇的选择性均没有发生明显下降,表明该催化剂具有良好的稳定性.
The La modified Ni-La@mSiO2 core-shell catalyst was prepared by hydration hydrazine reduction and Stöber method.The catalytic performance of the as-prepared catalyst was tested by hydrogenation of benzophenone to benzhydrol.BET,XRD and TEM were used to investigate the structure characteristics of the catalyst.The influence of the reaction time on the selective hydrogenation of benzophenone over Ni-La@mSiO2 were investigated and optimized.The conversion of benzophenone and selectivity of benzhydrol were both over 90%,while the hydrogen pressure was 2.5 MPa,the reaction temperature was 120 ℃ and the reaction time was 120 min.Furthermore,there was no significant decline of the catalyst when it was recycled for five runs,indicating the good stability of this catalyst.
[1] 刘成运,荣泽明,杜文强,等.高分散[Pd-Pt] /活性炭催化喹啉加氢制备1,2,3,4-四氢喹啉[J].精细化工,2013,30(1):36-40. LIU C Y,RONG Z M,DU W Q,et al.Selective hydrogenation of quinolone to prepare 1,2,3,4-tetraquinoline over highly dispersed[Pd-Pt] /C catalysts[J].Fine Chemical,2013,30(1):36-40.
[2] CIRTIU C M,BRISACH-WITTMEYER A,MENARD H.Comparative study of catalytic and electrocatalytic hydrogenation of benzophenone[J].Catalysis Communications,2007,8:751-754.DOI:10.1016/j.catcom.2006.09.014. NIU X S,LI H H,JIANG K.Research progress on photocatalysis of metal Ion doped nano-TiO2[J].Electromic Components & Materials,2004,23(8):39-45.DOI:10.3969/j.issn.1001-2028.2004.08.014.
[14] 鲁飞,孟凡明.TiO2光催化剂掺杂改性研究进展[J].硅酸盐通报,2011,20(1):116-119. LU F,MENG F M.Research evolution of soping modification on TiO2 photocatalyst[J].Bulletin of The Chinese Ceramic Society,2011,20(1):116-119.
[15] LOWES B J,BOTHRER A G,TRAN TT,et al.Grafting of polystyrene “from” and “through” surface modified titania nanoparticls[J].Polym Bull,2009,62:281-289.DOI: 10.1007/s00289-008-0016-9.
[16] HOJJATI B,SUI R,CHARPENTIER P A.Synthesis of TiO2/ PAA nanocomposite by RAFT polymerization[J].Poly- mer,2007,48:5850-5858.DOI:10.1016/j.polymer.2007.07.054.
[17] 王积森,冯忠彬,孙金全,等.纳米TiO2的光催化机理及其影响因素分析[J].纳米材料与结构,2008,45(1):28-32.DOI:10.3969/j.issn.1671-4776.2008.01.008. WANG J S,FENG Z B,SUN J Q,et al.Photocatalytic mechanism of nano-TiO2 and analysis on factors influencing its photocatalytic activity[J].Nanomaterial &Structure,2008,45(1):28-32.DOI:10.3969/j.issn.1671-4776.2008.01.008.
[18] 杨儒,李敏,张敬畅,等.锐钛矿型纳米TiO2粉体的精细结构及其光催化降解苯酚的活性[J].催化学报,2003,24(8):629-634.DOI:10.3321/j.issn:0253-9837.2003.08.016. YANG R,LI M,ZHANG J C,et al.Fine structure of nanometer anatase titania and its photocatalytic activity for phenol degradation[J].Chinese Journal of Catalysis,2003,24(8):629-634.DOI:10.3321/j.issn:0253-9837.2003.08.016.
[19] WANG Q,CHEN C C,ZHAO D,et al.Change of adsorption modes of dyes on flurinated TiO2 and its effect on photocatalytic degradation of dyes under visible irradiation[J].Langmuir,2008,24:7338-7345.DOI:10.1021/la800313s.
[20] 李发堂,赵地顺,郝勇静,等.氟掺杂纳米TiO2粉体的合成及光催化活性研究[J].化学工程,2009,37(2):54-57. LI F T,ZHAO D S,HAO Y J,et al.Preparation and photocatalytic activities of F-doped nano-TiO2 power[J].Chemical Engineering,2009,37(2):54-57.
[21] PISCOPO A,ROBERT D,WEBER J V.Influence of pH and chloride anion on the photocatalytic degradation of organic compounds:Part 1.Effect on the benzamide and para-hydroxybenzoic acid in TiO2 aqueous solution[J].Applied Catalysis B:Environmental,2001,35(2):117-124.DOI:10.1016/S0926-3373(01)00244-2.
