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Preparation Of The Amino-functionalized SBA-15 Loaded HKUST-1 Composite Materialand Study Of The Catalytic Reduction Properties

Posted on:2024-04-05Degree:MasterType:Thesis
Country:ChinaCandidate:C QianFull Text:PDF
GTID:2531307085966339Subject:Chemical Engineering and Technology
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In recent years,energy shortage and environmental problems have become important problems facing human society.Organic matter,heavy metals and their compounds are the main pollution sources of fresh water resources,which have a very serious impact on human health.In these organic pollutants,nitrophenol,nitrobenzene pollutants(such as4-nitrophenol,nitrobenzene,dinitrophenol,etc.)is a common pollutant,commonly used as chemical,pesticide,pharmaceutical intermediates,is a highly dangerous and carcinogens,at the same time has good water soluble and very stable in water,so how to deal with the pollutants is imminent.In this paper,two kinds of amino functionalized SBA-15 supported HKUST-1 composite materials were designed and prepared,and the catalytic properties of these two kinds of composite materials were investigated by the reduction reaction system of 4-nitrophenol(4-NP).The main contents of this paper include:(1)Post-synthetic grafting combined hydrothermal technique:Firstly,ordered mesoporous silica(SBA-15)was prepared using P123 as template,hydrochloric acid as acidic medium,and tetraethyl orthosilicate(TEOS)as silicon source.Secondly,amino functionalized SBA-15(SBA-15-NH2)was synthesized using SBA-15 as the carrier,N,N-dimethylformamide(DMF)as the solvent and 3-aminopropyl triethoxysilane(APTES)as the silane coupling reagent.Finally,the metal-organic frame compound(HKUST)functional composite(x)HKUST-1/SBA-15-NH2was synthesized by using SBA-15-NH2as a vehicle.By N2adsorption-desorption isotherm and pore size distribution,small-angle X-ray powder diffraction,scanning electron microscope and transmission electron microscopy techniques show that HKUST-1/SBA-15-NH2composite has an orderly two-dimensional hexagonal mesoporous structure;The structure and composition of the composite were characterized by infrared spectroscopy,wide-angle X-ray powder diffraction and X-ray photoelectron spectroscopy.The analysis showed that the surface of SBA-15 was aminozed,and HKUST-1 was successfully synthesized on the surface of SBA-15-NH2.Subsequently,the catalytic activity of HKUST-1/SBA-15-NH2was examined using the reduction reaction of 4-NP as the model reaction.The results show that the composite has certain reduction catalytic activity and stability.(2)One-step co-condensation combined with hydrothermal technology:Amino functionalized ordered mesoporous silicon dioxide(PMO-pr-NH2)was prepared by one-step co-condensation method using TEOS as the precursor of silicon source,P123 as the template and APTES as the coupling reagent.Then HKUST-1 functionalized composite HKUST-1@PMO-pr-NH2(x)was prepared in situ using PMO-pr-NH2as the carrier by adsorption and in-situ synthesis technology,so that the amino group on its surface directly adsorbed Cu2+.The results of N2adsorption-desorption isotherm and pore size distribution,small-angle X-ray powder diffraction,scanning electron microscopy and transmission electron microscopy showed that HKUST-1@PMO-pr-NH2composite has an ordered two-dimensional hexagonal mesoporous structure with high specific surface area,and HKUST-1 grows in the pore of PMO-pr-NH2.The structure and composition of the composite were characterized by infrared spectroscopy,thermogravimetry,wide-angle X-ray powder diffraction and X-ray photoelectron spectroscopy.The results showed that the surface of SBA-15 was aminated,and HKUST-1 through the amino group on the surface of PMO-pr-NH2is successfully synthesized and fixed in the pore of PMO-pr-NH2,and the interaction between PMO-pr-NH2and HKUST-1.HKUST-1@PMO-pr-NH2composites showed good catalytic activity in the 4-NP reduction reaction,and its catalytic activity remained stable after five cycles.
Keywords/Search Tags:SBA-15, amino-functionalization, HKUST-1, 4-nitrophenol, reduction
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