Silica Supported Binuclear Copper Catalysts PDF Download
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Author: Homiyar N. Choksi
Publisher:
ISBN:
Category : Copper catalysts
Languages : en
Pages : 276
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Author: Homiyar N. Choksi
Publisher:
ISBN:
Category : Copper catalysts
Languages : en
Pages : 276
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Author: Nuwan Dileepa De Silva
Publisher:
ISBN:
Category :
Languages : en
Pages : 130
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The dissertation describes research work on development of bimetallic heterogeneous catalysts for oxidation of organic compounds. Binuclear metal complexes are an interesting class of compounds due to their catalytic activity. The approach involves anchoring a triketone ligand to Cab-O-Sil via a linker. Specifically, silica gel was allowed to react with p-chloromethylphenyltrimethoxysilane followed by coupling with deprotonated triketone compounds. The viability of this approach was verified by performing the benzylation reaction of triketones with benzyl halides under basic conditions. The benzylation of 2,4,6-heptanetrione and 1,5-diphenyl-1,3,5-pentanetrione is achieved with benzyl bromide using n-tetrabutylammonium fluoride as base. These benzylation reaction conditions were used to attach the triketones to the surface-attached linker. Once the ligand is attached to the silica gel, the catalyst is formed by coordinating two copper(II) ions from solution to the deprotonated triketone. The coordination of copper(II) ions to the triketone was monitored using UV-vis spectroscopy. The modified silica gel is characterized by diffuse reflectance infrared Fourier spectroscopy (DRIFTS), and thermal gravimetric analysis (TGA) at the different stages of catalyst formation. All techniques indicated significant attachment of linker and triketone to the support. The oxidation of 3,5-di-tert-butyl catechol (DTBC) and benzyl alcohol was carried out under aerobic conditions using these catalysts. The kinetics of the DTBC oxidation and benzyl alcohol oxidation was studied using bimetallic and monometallic catalytic systems. The copper complexes of the triketone ligands were also evaluated as catalysts for the oxidation of DTBC. New bimetallic metal complexes with triketone ligands having a benzyl group were synthesized and characterized by high resolution mass spectroscopy and IR spectroscopy. In addition to a detailed description of the synthesis and characterization of new triketone compounds, and the heterogeneous catalyst systems, a comparison of the kinetics of the oxidation of DTBC using these catalysts will be discussed.
Author: Samantha Ranaweera
Publisher:
ISBN:
Category :
Languages : en
Pages : 186
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Stable dinuclear complexes bis(heptane-2,4,6-trionato)dicopper(II) [Cu2(daa)2], bis(1,5-diphenyl-1,3,5-pentanetrionato)dicopper(II) [Cu2(dba)2], bis(1,5-diphenyl-1,3,5- pentanetrionato)dicobalt(II) [Co2(dba)2], and [6,11-dimethyl-7,10-diazahexadeca-5,11- diene-2,4,13,15-tetranato(4-)-N7N10O4O13;O2O4O13O15] copper(II)cobalt(II) [(CuCo(daaen)] were supported on Cab-O-Sil by the batch impregnation technique. The upported samples were characterized by UV-Vis, elemental analysis, X-ray powder diffraction (XRD), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and thermal gravimetric analysis (TGA). Elemental analysis and TGA data confirm that the Cu2(daa)2 complex loses one of its coordinated ligands upon adsorption onto silica in THF at greater than 4.43 wt% Cu loading. By contrast, at all Cu loadings the Cu2(dba)2 complex was adsorbed on the silica surface in CH2Cl2 without loss of ligand. XRD and DRIFTS results confirmed the formation of Cu2(dba)2 multilayer films on the Cab-O-Sil surface for samples containing greater than 2.64 wt% copper. The dinuclear cobalt complex and copper-cobalt complex also do not lose their coordination ligands upon adsorption on the surface. These two metal complexes are amorphous and did not produce XRD patterns. However, DRIFTS results confirm that the binuclear cobalt complex and the copper-cobalt complex begin forming multilayer films between 1.21and 2.53 wt% Cu. The Cu2(dba)2/silica precatalysts were subsequently converted to the catalysts by decomposing the organic ligands at 450 degrees Celsius followed by activation with 2% H2 at 250 degrees Celsius and were evaluated for methanol synthesis and methanol decomposition reactions. Kinetic studies demonstrated that the 3.70% Cu/silica[Cu2(dba)2] catalyst is more active for methanol decomposition than it is for methanol synthesis. The supported dinuclear cobalt and copper-cobalt precatalysts were converted to the catalyst by heating at 450 degrees Celsius followed by activation of the catalysts with 50% H2. Four different catalysts, 3.5% Co/silica[Co2(dba)2], 6.7% Co/silica[Co2(dba)2], 2.3% Co/silica[CuCo(daaen)], and 5.5% Co/silica[Co2(daa)2] were evaluated for the Fischer-Tropsch reaction at 350 degrees Celsius in a batch reactor. The supported binuclear cobalt catalyst produced C1−C7 alkanes and a significant amount of CO2. By contrast, the catalyst formed from heterobinuclear CuCo(daaen) showed the ability to convert syngas to aromatics with a narrow product distribution. In addition, the 6.7% Co/silica[Co2(dba)2] multilayer catalysts have above 98% conversion rates and 60% liquid hydrocarbon selectivity in a flow reactor.
Author: James J Spivey
Publisher: Royal Society of Chemistry
ISBN: 1847553303
Category : Technology & Engineering
Languages : en
Pages : 209
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There is an increasing challenge for chemical industry and research institutions to find cost-efficient and environmentally sound methods of converting natural resources into fuels chemicals and energy. Catalysts are essential to these processes and the Catalysis Specialist Periodical Report series serves to highlight major developments in this area. This series provides systematic and detailed reviews of topics of interest to scientists and engineers in the catalysis field. The coverage includes all major areas of heterogeneous and homogeneous catalysis and also specific applications of catalysis such as NOx control kinetics and experimental techniques such as microcalorimetry. Each chapter is compiled by recognised experts within their specialist fields and provides a summary of the current literature. This series will be of interest to all those in academia and industry who need an up-to-date critical analysis and summary of catalysis research and applications. Catalysis will be of interest to anyone working in academia and industry that needs an up-to-date critical analysis and summary of catalysis research and applications. Specialist Periodical Reports provide systematic and detailed review coverage in major areas of chemical research. Compiled by teams of leading experts in their specialist fields, this series is designed to help the chemistry community keep current with the latest developments in their field. Each volume in the series is published either annually or biennially and is a superb reference point for researchers.
Author: Jun Wang
Publisher:
ISBN:
Category : Biomimetics
Languages : en
Pages : 94
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Author: Stephanie Christine Bowman
Publisher:
ISBN:
Category : Biochemistry
Languages : en
Pages : 458
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Author: Katherine Rooney
Publisher:
ISBN:
Category :
Languages : en
Pages : 118
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Author: M. Nomura
Publisher:
ISBN:
Category :
Languages : en
Pages : 12
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Author: Terry S. King
Publisher:
ISBN:
Category : Catalyst supports
Languages : en
Pages : 16
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Author: M. Nomura
Publisher:
ISBN:
Category :
Languages : en
Pages :
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