一种新型磁性可回收的“三唑环-过渡金属”催化剂的制备与研究
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- 英文论文题名：Parts per Million Level, Green, and Magneticallyrecoverable Triazole Ligand-stabilized Au and Pd Nanoparticle Catalysts
- 论文作者：岳国宗 ; 苏松 ; 黄德顺 ; 杨桂英 ; 赖新春 ; 赵鹏翔
- 英文论文作者：Guozong Yue ; Song Su ; Deshun Huang ; Guiying Yang ; Xinchun Lai ; Pengxiang Zhao ; Nano Chemistry Group ; Institute of Materials ; China Academy of Engineering Physics ; College of Materials Science and Engineering ; Southwest University of Science and Technology
- 年：2016
- 作者机构：中国工程物理研究院材料研究所;西南科技大学;
- 论文关键词：三唑环 ; 过渡金属纳米粒子 ; 催化活性 ; 磁性可回收
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十七分会：纳米催化
- 语种：中文
- 分类号：TB383.1;O643.36
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十七分会 ; 纳米催化
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：117k
- 原文格式：D
- 会议级别：全国
摘要
我们制备了一种新型磁性可回收的"三唑环-过渡金属"复合纳米结构催化剂(Fe_3O_4-TrZ-Au/Pd)。经过多种表征方法分析后发现:该催化剂水溶性良好,粒径均一,平均粒径为5nm,形貌规则呈球形分散,金属纳米粒子均匀分布在Fe_3O_4-Trz纳米粒子表面。进一步研究了该磁性复合纳米结构催化剂对4-硝基苯酚(4-NP)的还原反应和Suzuki-Miyaura反应的催化性能。实验研究表明:Fe_3O_4-Trz-Au/Pd对4-NP的还原具备良好的催化活性。其中,过渡金属Pd的催化活性比Au的催化活性强。实验数据得出Au和Pd纳米粒子的负载量分别为0.7wt%和1.4wt%时,mPEG的分子量为500时,催化剂的催化活性最佳;Fe_3O_4-Trz-Pd对Suzuki-Miyaura反应具有较好的痕量催化效果,当催化剂用量低至0.0001mmol%(1ppm)时仍具有一定的催化活性;此外,由于该催化剂的结构特点,可通过外加磁场在上述反应过程中对其进行简单快速回收,循环利用6次后,其催化活性无显著下降。
Triazole ligands with carboxylic acid in one termini and poly ethylene oxide(PEO) in the other termini are synthesized via "Click" chemistry,and subsequently attached on the Fe_3O_4 surface by ligand exchange reaction.Then the small-sized Au or Pd nanoparticles(AuNPs or PdNPs) are encapsulated into this nano composite by their mild coordination with triazole.Generally,the trz ligand associates with AuNPs or PdNPs surface through one pair of electrons on the sp2-hybridized nitrogen atoms to form the trz-AuNPs or trz-PdNPs catalyst.These novel catalysts are investigated in4-nitriphenol(4-NP) reaction and C-C coupling with green solvent,and the results disclosed their excellent catalytic reactivity at ppm level and magnetically recycling.
Triazole ligands with carboxylic acid in one termini and poly ethylene oxide(PEO) in the other termini are synthesized via "Click" chemistry,and subsequently attached on the Fe_3O_4 surface by ligand exchange reaction.Then the small-sized Au or Pd nanoparticles(AuNPs or PdNPs) are encapsulated into this nano composite by their mild coordination with triazole.Generally,the trz ligand associates with AuNPs or PdNPs surface through one pair of electrons on the sp2-hybridized nitrogen atoms to form the trz-AuNPs or trz-PdNPs catalyst.These novel catalysts are investigated in4-nitriphenol(4-NP) reaction and C-C coupling with green solvent,and the results disclosed their excellent catalytic reactivity at ppm level and magnetically recycling.
引文
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[2]Li,N.;Zhao,P.;et al.Chem.Eur.J.,2014,20,8363-8369.
[3]Zhao,P.;Li,N.;Liu,N.et al.Chem.Commun.,2013,49:3218-3220.
[4]Hervés,P.;Pérez-Lorenzo,M.;Liz-Marzan,L.M.et al.Chem.Soc.Rev.,2012,41:5577-587.
[5]Su,S.;Yue,G.;Huang,D.;Yang,G.;Lai,X.;Zhao,P.RSC Advances,2015,55:44018-44021.