Au催化剂论文负载型Au催化剂的制备及其在肉桂醛选择性加氢反应中的应用研究

Au催化剂论文：负载型Au催化剂的制备及其在肉桂醛选择性加氢反应中的应用研究【中文摘要】负载型纳米Au催化剂在许多化合物的【英文摘要】Supportedgoldcatalystsareakindofpromisingcatalystsforselectivehydrogenationbasedontheirgoodactivityandselectivityforthereductionofmanycompounds.Inthispaper,usingseveralmetaloxidesdopedTiO2assupports,whichwerepreparedbythesol-gelmethod,aseriesofgoldcatalystswerepreparedbythedeposition-precipitation（DP）method.Additionally,aseriesofAu/La（OH）3catalystswerepreparedbycocipitation（CP）method.Allthecatalystweretestedincinnamaldehydehydrogenation.Theirphisico-chemicalpropertieswereinvestigatedbyXRD,TEM,XPS,BETandTPRtechniques.Thereactionconditionsofcinnamaldehydeselectivehydrogenationwereoptimized.TheresultsshowthattheperformanceofAu/TiO2catalystisinfluencedbythetypeandthecontentofadditives.Amongthemetaloxidepromoterstested,La2O3modifiedAu/TiO2showsthebestselectivityforthereductionofcarbon-carbondoublebondincinnamaldehyde.ThemoderateamountofLa2O3（10wt%）canobviouslyimprovethecatalyticactivityandselectivityofAu/TiO2forcinnamaldehydehydrogenation.ThepresenceofLa2O3inTiO2restrainsthegrowthofTiO2crystallites,increasesthesurfaceareaofcatalystsandmakestheparticlesizedistributionofAucrystallitesmoreevenly.ThegoldonthesurfaceofAu/TiO2existsmainlyasAu0,butontheLa2O3dopedcatalystthereisasmallportionofAu3+speciesbesidesAu0,whichmaybenefittheactivationoftheC=Obondofcinnamaldehyde.TheresultsshowthatLa（OH）3supportedgoldcatalystshowshighselectivityforthereductionofcarbon-carbondoublebond.Withthecharacterizationresults,thereasonofthehighselectivityisthatthesupporterLa（OH）3andAuinteracttoformauniquestructure.ThepreparationconditionsofAu/La（OH）3catalystareoptimizedasfollows:2wt%ofgoldcontent,calcinationtemperature100°Candreductiontemperature150°C.ThereactionconditionsofcinnamaldehydeselectivehydrogenationoverAu/La（OH）3catalystareoptimizedasfollows:reactiontemperature180°C,reactionpressure2.0MPa,catalystdosage0.25g,solventisopropanol.Undertheoptimalconditions,theconversionofcinnamaldehydeandtheselectivitytocinnamylalcoholcanreach100%and75.7%,respectively,afterreaction22h.【关键词】Au催化剂助剂La（OH）3选择性加氢肉桂醛肉桂醇【英文关键词】goldcatalystpromoterLa（OH）3selectivehydrogenationcinnamaldethydecinnamylalcohol【目录】负载型Au催化剂的制备及其在肉桂醛选择性加氢反应中的应用研究摘要4-6ABSTRACT6-7第一章文献综述11-301.1肉桂醛催化加氢合成肉桂醇的研究进展11-201.1.1肉桂醇的用途111.1.2肉桂醇的合成方法11-131.1.3非贵金属催化剂在肉桂醛选择性加氢中的应用进展13-161.1.4贵金属催化剂在肉桂醛选择性加氢中的应用进展16-201.2纳米Au催化剂的研究进展20-281.2.1负载型Au催化剂的制备20-221.2.2负载型纳米Au催化剂性能的影响因素22-251.2.3Au催化剂在液相加氢中的应用25-281.3立题依据及主要研究内容28-301.3.1论文立题依据和意义28-291.3.2论文主要研究内容29-30第二章实验部分30-362.1试剂与主要仪器30-312.1.1主要试剂30-312.1.2主要仪器及设备312.2实验方案与步骤31-322.2.1实验方案312.2.2实验步骤31-322.3催化剂的制备32-332.3.1Au/M_xO_y–Ti0_2催化剂的制备32-332.3.2Au/La(OH)_3催化剂的制备332.4催化剂的活性评价33-342.4.1实验方法332.4.2产物分析33-342.5催化剂的表征34-362.5.1X射线衍射(XRD)342.5.2比表面和孔结构的测定(BET)342.5.3元素分析(STEM-EDX)342.5.4高分辨透射电镜(HRTEM)34-352.5.5X射线光电子能谱仪(XPS)352.5.6程序升温还原(H_2-TPR)35-36第三章助剂对Au/Ti0_2催化剂加氢性能的影响研究36-533.1前言363.2助剂对Au/Ti0_2催化性能的影响36-393.2.1助剂种类的影响36-373.2.2助剂添加方式的影响37-383.2.3助剂添加量的影响38-393.3助剂La_20_3对Au/Ti0_2催化性能的影响39-513.3.1助剂La_20_3添加量对Au/Ti0_2性能的影响39-483.3.2焙烧温度对Au/10%La_20_3-Ti0_2催化剂加氢性能的影响48-493.3.3还原温度对Au/10%La_20_3-Ti0_2催化剂加氢性能的影响49-503.3.4还原时间对Au/10%La_20_3-Ti0_2催化剂加氢性能的影响50-513.4本章小结51-53第四章纳米Au/La(OH)_3催化剂加氢性能的研究53-684.1前言534.2载体种类对Au催化剂性能的影响53-564.2.1载体种类对Au催化剂加氢性能的影响53-544.2.2不同载体负载的Au催化剂的表征54-564.3Au/La(OH)_3催化剂上肉桂醛选择性加氢反应研究56-674.3.1Au负载量对Au/La(OH)_3催化剂加氢性能的影响56-574.3.2焙烧温度对Au/La(OH)_3催化剂加氢性能的影响57-634.3.3还原温度对Au/La(OH)_3催化剂加氢性能的影响63-674.4本章小结67-68第五章Au/La(OH)_3催化剂上肉桂醛加氢反应条件的优化68-735.1前言685.2不同溶剂的影响68-695.3反应温度的影响695.4反应压力的影响69-705.5催化剂用量的影响70-715.6本章小结71-73第六章结论与展望73-756.1结论73-746.2展望74-75参考文献75-84