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Preparation of Bimetallic DTNs and Catalytic Hydrogenation of NBR

Author: LuXiaoRan
Tutor: PengXiaoHong
School: South China University of Technology
Course: Polymer Chemistry and Physics
Keywords: PPI dendrimer 15-membered tri-olefinic macrocyles Bimetallic DTNs NBR hydrogenation
CLC: TQ333
Type: Master's thesis
Year: 2011
Downloads: 83
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Abstract


In this paper, a series of bimetallic dendrimer-templated nanoparticles(DTNs) were prepared with Pd and Pt. The size, distribution, morphology and catalytic activity of DTNs were characterized and analysed.First of all, low generation poly(propyleneimine) dendrimers (PPI) were synthesized via divergent method (Micheal addition reaction and hydrogenation reaction of cyano groups). And then, 15-membered tri-olefinic macrocyles were synthesized through adopting 2,4,6-triisopropyl phenyl sulfonamide and 1,4-dibromo-2-buteneas raw materials. The products were characterized by FTIR and NMR to analyse structure. The results showed that the existence of the unique structure of PPI dendrimers and 15-membered tri-olefinic macrocyles, and proved the successful synthesis of desired products.Secondly, amino groups on the surface of PPI were modified by macrocyles which were used as end-group modifier and heterozygous modified PPI dendrimers was obtained. Made Pd(PPh3)4 and Pt(PPh3)4 react with heterozygous PPI dendrimers to synthesize a series of single metallic DTNs and bimetallic DTNs catalysts via ligand synchronous exchange method. The NMR analysis results showed that the chemical shift of double bond proton hydrogen changed before and after the metal encapsulated. The surface morphology of nanoparticles and particle size distribution were investigated by AFM. The results showed that the metal nanoparticles were spherical, well distributed and the particle size were small. The PPI dendrimers modified by macrocyles can be used as carrier for metal atoms, and it can effectively hinder metal atoms reunion.Finally, some bimetallic DTNs as catalyst were used to participate hydrogenation reaction of nitrile butadiene rubber(NBR). Adding HNBR to methanol and churned the mixture, then recover the DTNs catalysts by using the mixture of methanol and chlorobenzene. Test the relative hydrogenation degree of HNBR to evaluate the catalytic activity of catalysts. The experimental results showed that the catalytic activity of bimetallic DENs catalysts was better than single metallic DTNs catalysts, and it depend on the synergies between two metal particles each other and the role of electronic ligands. Bimetallic heterozygous PPI DTNs still had catalytic activity after repeatedly recovery cycles, compared to macrocyles encapsulated nanoparticles.

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