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Synthesis, Design And Catalytic Property Studies Of Supported Porous Materials

Posted on:2016-03-31Degree:MasterType:Thesis
Country:ChinaCandidate:Y S PengFull Text:PDF
GTID:2191330473461712Subject:Chemistry
Abstract/Summary:PDF Full Text Request
Porous materials are a kind of important applied materials andhave many important applications inheterogeneous catalysis,gas storage and separation, and photoelectric sensors, etc. Some research were made on novel catalytic supported porous materials. Novel supported porous materials were designed and prepared, and some research were made on their structures and catalytic properties.(1)gold (Au) nanoparticle (NP)-mesoporous silica (SiO2) composite nanotubes were prepared by a bottom-up approach in which Au NPs were anchored to the inner wall of mesoporous SiO2 tubular shells. In this composite, the agglomeration, exfoliation, andgraingrowth of Au NPs were restricted, and the loading and size of the catalyst NPs were easily tuned. The mesoporous shell, open ends, and one-dimensional passage of the SiO2 nanotubes all promote the diffusion of reactants, which enhanced the catalytic efficiency of this composite in the reduction of 4-nitrophenol. The Au NP-mesoporous SiO2 composite nanotubes also demonstratedgood reusability, and no leaching or agglomeration of the Au NPs was observed during the catalytic reaction.(2) Two linear shaped dialdehyde monomers with analogous structures, namely 2,2’-bipyridine-5,5’-dicarbaldehyde (2,2’-BPyDCA) containing bipyridine units and 4,4’-biphenyl dialdehyde without bipyridine units, were chosen as building blocks to make adjustments to the nitrogen content within the 2D structures of the COFs by means of the pore surface engineering strategy. Four members of 2D imine-linked COFs were fabricated in this way and nominated as X% BPy COF (X=25,50,75,100), where X% represented the molar percentage of 2,2’-BPyDCA present in the dialdehyde blend and the precise content control of the nitrogen ligands within 2D COFs were researched.(3) Monometallic Pd(OAc)2 was docked into X% BPy COF (X=25,50,75,100), TF-BD COF and BiPh COF.given that iminegroups and bipyridinegroups can be uniformly distributed throughout COFs, their one-to-one interaction with catalysts allows for the effective isolation of the active sites of the catalyst at a molecular level. The relationship between the molar percentage of 2,2’-BPyDCA present in the dialdehyde blend and the content control of the nitrogen ligands within 2D COFs were researched. (4) Pd(II)@ X% BPy COF(X=25,50,75,100),Pd(II)@TF-BD COF,Pd(II)@BiPh COF were characterized by means of physical absorption and XPS to research the docking location and mechanism of Pd(OAc)2 molecules.The catalytic performance of Pd(Ⅱ)@ X% BPy COF (X=25,50,75,100) were tested inheck reactions.(5) Rh(Ⅰ) and Pd(Ⅱ) were docked into X% BPy COF(X=25,50,75,100) successfully toget Rh(I)/Pd(Ⅱ)@ X% BPy COF(X=25,50,75,100) and they were characterized to research the docking location and mechanism of Rh(I) and Pd(II).
Keywords/Search Tags:porous materials, gold-mesoporous silica nanotubes, X% BPy COF, the content control of the nitrogen ligands, bimetallic docking
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