CN106984326A - 一种PtPdAu/负载型纳米磁性催化剂及其制备方法 - Google Patents
一种PtPdAu/负载型纳米磁性催化剂及其制备方法 Download PDFInfo
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Abstract
本发明公开了一种磁性PtPdAu/Fe3O4纳米催化剂的制备方法。所述催化剂载体为Fe3O4，活性组分是Pt、Pd和Au，其平均粒径分别约为10纳米、7纳米和15纳米，催化剂中Pt、Pd和Au的质量分数分别约为2.1％、4.3％和9.3％。本发明的磁性PtPdAu/Fe3O4纳米催化剂具有清洁、环保、高效而又方便的特点，并且本发明的催化剂在Heck反应中具有很高的催化活性。
Description
技术领域
本发明涉及工业催化技术领域，尤其涉及一种PtPdAu/负载型纳米磁性催化剂及其制备方法。
背景技术
近几十年来，负载型纳米催化剂已得到广泛应用。关于金属和载体间的相互作用的研究报道日益增多。众所周知，金属和载体间特殊的相互作用会影响催化剂的表面性能，进而影响它的催化活性。比如，在Al2O3载体担载金属钴的过程中钴离子会迁移到Al2O3的晶格中形成CoAl2O4化合物。铁的氧化物和过渡金属氧化物或其碳酸盐发生固-固作用形成相应的铁氧体氧化物CoFe2O4。铂、钯、金纳米微粒具有高表面能，容易发生团聚。若将铂、钯、金复合贵金属纳米微粒负载在载体上可有效地阻止其团聚，而且更有效对制备的催化剂进行分离回收。从而提高催化剂的催化活性和利用率。
Fe3O4纳米粒子显示典型的超顺磁性，在生物医学、磁记录材料、磁流体复合材料、催化剂等方面有着潜在的应用前景。
Heck反应是有机卤化物与烯烃在强碱和钯催化下生成取代烯烃的偶联反应，是过渡金属催化最重要也是应用最有前景的碳碳键形成的反应之一，在有机中间体，有机功能材料，药物，天然产物等合成中被广泛应用。
在反应中常常会遇到催化剂容易失活、回收利用率不高、破坏环境等问题，且后处理比较麻烦。本方法提供了一种清洁环保而又方便的催化剂。
发明内容
本发明专利的目的是提供一种在Heck反应中有效且易回收的具有优异催化性能的磁性PtPdAu/Fe3O4纳米催化剂的制备方法。
本发明采取的技术方案是：
本发明的PtPdAu/负载型纳米磁性催化剂载体为Fe3O4，活性组分是Pt、Pd和Au，催化剂中Pt、Pd和Au的质量分数分别为1～4％、3～6％和7～15％。
优选：催化剂中Pt、Pd和Au的质量分数分别约为2.1％、4.3％和9.3％。
活性组分Pt、Pd和Au，其平均粒径分别约为10纳米、7纳米和15纳米。
本发明的PtPdAu/负载型纳米磁性催化剂的制备方法的具体步骤如下：
(1)载体的制备及其预处理
通过水热法将铁离子前驱体氧化还原成的Fe3O4纳米颗粒，使用去离子水、无水乙醇进行清洗，直至上层液体透明，然后将其用无水乙醇定容，备用；在清洗过程中通过铁磁体对Fe3O4纳米颗粒进行分离；
(2)Pt-Pd-Au溶胶的制备
向氯铂酸、氯钯酸和氯金酸混合液中添加稳定剂，搅拌均匀后滴加还原剂溶液，继续搅拌制得稳定Pt-Pd-Au溶胶；
(3)磁性PtPdAu/Fe3O4纳米催化剂的制备
将从步骤(1)中所得的载体加入由步骤(2)制得的Pt-Pd-Au溶胶中，机械搅拌后静置，抽滤，烘干，得PtPdAu/Fe3O4催化剂。
步骤(1)中，所述的铁离子前驱体是FeCl3·6H2O、FeCl2·4H2O、FeCl2·2H2O或FeCl2。
步骤(2)中，所述的稳定剂为聚乙烯吡咯烷酮、聚乙二醇或聚乙烯醇；所述的还原剂为硼氢化钠、硼氢化钾或焦性没食子酸。
步骤(2)中，氯铂酸、氯钯酸和氯金酸混合液中摩尔比为2:1:10、当氯铂酸用量是1mol时，稳定剂用量为22mol、当氯铂酸用量是1mol时，还原剂用量为31mol。
步骤(2)中，继续搅拌0.5h。
步骤(3)中，Pt-Pd-Au溶胶与载体质量比为1：72。
本发明的PtPdAu/负载型纳米磁性催化剂可以用于Heck反应。
磁性PtPdAu/Fe3O4纳米催化剂在Heck反应中的具体步骤如下：
向三口烧瓶中加入碘苯、苯乙烯、DMF，再加入一定量的磁性PtPdAu/Fe3O4纳米催化剂，搅拌均匀后，放入油浴锅中进行反应。反应结束后，将催化剂于产物分离，催化剂留待循环使用。
本发明的积极效果如下：
本发明的磁性PtPdAu/Fe3O4纳米催化剂具有清洁、环保、可循环使用而又方便的特点，并且本发明的磁性PtPdAu/Fe3O4纳米催化剂Heck反应中反应条件要求不高，并且具有优异的催化性能。
附图说明
图1是实施例1制备的磁性PtPdAu/Fe3O4纳米催化剂的透射电镜照片。
具体实施方式
下面的实施例是对本发明的进一步详细描述。
实施例1
(1)载体的制备及其预处理
于50ml烧杯中，准确称取0.2125g的FeCl3·6H2O、0.1432g的尿素、0.1663g的聚乙烯吡咯烷酮，随后加入8.5ml的1，2-丙二醇，混合物在磁力搅拌器上搅拌直至溶液混合均匀得黄色透明溶液后转移到反应釜中，密封后在190℃下反应16h。反应结束后，冷却到室温，将产物转移到广口玻璃瓶中，用去离子水、乙醇多次洗涤，并用磁分离倾出广口瓶中的上清液。将洗涤后的黑色沉淀颗粒分散于10mL的乙醇得到Fe3O4纳米磁体材料。
(2))Pt-Pd-Au溶胶的制备
于50mL烧杯中，准确量取0.0789g的聚乙烯吡咯烷酮，用移液管量取3.86×10- 3mol/L的氯铂酸水溶液0.82mL，1.13×10-2mol/L的氯钯酸水溶液1.40mL，4.806×10-3mol/L的氯金酸水溶液3.28mL，然后在磁力搅拌器上搅拌，直至完全溶解。随后将用0.0373g硼氢化钠、1.5mL水配制的溶液逐滴加入混合液中，制得Pt-Pd-Au溶胶。
(3)磁性PtPdAu/Fe3O4纳米催化剂的制备
将(1)中制备的Fe3O4纳米颗粒于上述制得的Pt-Pd-Au溶胶，机械搅拌8小时后静置1小时，使用铁磁体将其分离，烘干得磁性PtPdAu/Fe3O4纳米催化剂。
磁性PtPdAu/Fe3O4纳米催化剂在Heck反应中的应用
向50ml三口烧瓶中加入0.14mmol的碘代苯、3ml的DMF、0.17mmol的苯乙烯、上述制得磁性PtPdAu/Fe3O4纳米催化剂，搅拌均匀后再加入2.0mmol的K2CO3，于90℃下电动搅拌9h。反应结束后，将催化剂于产物分离，催化剂留待循环使用。
碘苯的转化率约为100％，产率高达98％。
而现有催化剂的转化率和产率如表1所示：
表1
参考文献
[1]K.Karami,Z.K.Moghadam,M.Hosseini-Kharat,Catalysis Communications,43(2014)25-28.
[2]M.Bakherad,A.Keivanloo,S.Samangooei,TetrahedronLetters,53(2012)5773-5776.
[3]P.Karthikeyan,P.N.Muskawar,S.A.Aswar,P.R.Bhagat,S.K.Sythana,Journal of Molecular CatalysisA:Chemical,358(2012)112-120.
[4]F.R.Fortea-Pérez,I.Schlegel,M.Julve,Journal of OrganometallicChemistry,743(2013)102-108.
[5]F.Cuenú,R.Abonia,A.A.Cabrera,Journal ofOrganometallicChemistry,696(2011)1834-1839.
循环实验效果：催化剂循环使用六次；
表2
| 循环次数 | 1 | 2 | 3 | 4 | 5 | 6 |
| 转化率(％) | 100 | 99.01 | 98.80 | 93.88 | 87.32 | 80.74 |
尽管已经示出和描述了本发明的实施例，对于本领域的普通技术人员而言，可以理解在不脱离本发明的原理和精神的情况下可以对这些实施例进行多种变化、修改、替换和变型，本发明的范围由所附权利要求及其等同物限定。
Claims (10)
1.一种PtPdAu/负载型纳米磁性催化剂，其特征在于：所述催化剂载体为Fe3O4，活性组分是Pt、Pd和Au，催化剂中Pt、Pd和Au的质量分数分别为1～4％、3～6％和7～15％。
2.如权利要求1所述的PtPdAu/负载型纳米磁性催化剂，其特征在于：催化剂中Pt、Pd和Au的质量分数分别约为2.1％、4.3％和9.3％。
3.如权利要求1所述的PtPdAu/负载型纳米磁性催化剂，其特征在于：活性组分是Pt、Pd和Au，其平均粒径分别约为10纳米、7纳米和15纳米。
4.一种制备如权利要求1-3任一项所述的PtPdAu/负载型纳米磁性催化剂的方法，其特征在于：所述方法的具体步骤如下：
(1)载体的制备及其预处理
通过水热法将铁离子前驱体氧化还原成的Fe3O4纳米颗粒，使用去离子水、无水乙醇进行清洗，直至上层液体透明，然后将其用无水乙醇定容，备用；在清洗过程中通过铁磁体对Fe3O4纳米颗粒进行分离；
(2)Pt-Pd-Au溶胶的制备
向氯铂酸、氯钯酸和氯金酸混合液中添加稳定剂，搅拌均匀后滴加还原剂溶液，继续搅拌制得稳定Pt-Pd-Au溶胶；
(3)磁性PtPdAu/Fe3O4纳米催化剂的制备
将从步骤(1)中所得的载体加入由步骤(2)制得的Pt-Pd-Au溶胶中，机械搅拌后静置，抽滤，烘干，得PtPdAu/Fe3O4催化剂。
5.如权利要求4所述的制备方法，其特征在于：步骤(1)中，所述的铁离子前驱体是FeCl3·6H2O、FeCl2·4H2O、FeCl2·2H2O或FeCl2。
6.如权利要求4所述的制备方法，其特征在于：步骤(2)中，所述的稳定剂为聚乙烯吡咯烷酮、聚乙二醇或聚乙烯醇；所述的还原剂为硼氢化钠、硼氢化钾或焦性没食子酸。
7.如权利要求4所述的制备方法，其特征在于：步骤(2)中，氯铂酸、氯钯酸和氯金酸混合液摩尔比为2:1:10、当氯铂酸用量是1mol时，稳定剂用量为22mol、当氯铂酸用量是1mol时，还原剂用量为31mol。
8.如权利要求4所述的制备方法，其特征在于：步骤(2)中，继续搅拌0.5h。
9.如权利要求4所述的制备方法，其特征在于：步骤(3)中，Pt-Pd-Au溶胶与载体质量比为1：72。
10.如权利要求1-3任一项所述的PtPdAu/负载型纳米磁性催化剂用于Heck反应中的用途。
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