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Synthesis, characterization and catalytic evaluation of cubic ordered mesoporous iron-silicon oxides

MARTINS, T. S.; MAHMOUD, A.; Silva, Luis Carlos Cides da; COSENTINO, I. C.; Tabacniks, Manfredo Harri; MATOS, J. R.; FREIRE, R. S.; Fantini, Marcia Carvalho de Abreu
Fonte: ELSEVIER SCIENCE SA Publicador: ELSEVIER SCIENCE SA
Tipo: Artigo de Revista Científica
ENG
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Iron was successfully incorporated in FDU-1 type cubic ordered mesoporous silica by a simple direct synthesis route. The (Fe/FDU-1) samples were characterized by Rutherford back-scattering spectrometry (RBS), small angle X-ray scattering (SAXS). N(2) sorption isotherm, X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS). The resulting material presented an iron content of about 5%. Prepared at the usual acid pH of -0.3, the composite was mostly formed by amorphous silica and hematite with a quantity of Fe(2+) present in the structure. The samples prepared with adjusted pH values (2 and 3.5) were amorphous. The samples` average pore diameter was around 12.0 nm and BET specific surface area was of 680 m(2) g(-1). Although the iron-incorporated material presented larger lattice parameter, about 25 nm compared to pure FDU-1, the Fe/FDU-1 composite still maintained its cubic ordered fcc mesoporous structure before and after the template removal at 540 degrees C. The catalytic performance of Fe/FDU-1 was investigated in the catalytic oxidation of Black Remazol B dye using a catalytic ozonation process. The results indicated that Fe/FDU-1 prepared at the usual acid pH exhibited high catalytic activity in the mineralization of this pollutant when compared to the pure FDU-1. Fe(2)O(3) and Fe/FDU-1 prepared with higher pH of 2 and 3.5. (C) 2010 Elsevier B.V. All rights reserved.; Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP); Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP); Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq); Conselho Nacional de Desenvolvimento Cientifico e Tecnologico (CNPq)

Synthesis and structure of cage-like mesoporous silica using different precursors

Fantini, Marcia Carvalho de Abreu; Kanagussuko, Cíntia Fabiana; Zilioti, George José Martins; MARTINS, T. S.
Fonte: ELSEVIER SCIENCE SA Publicador: ELSEVIER SCIENCE SA
Tipo: Artigo de Revista Científica
ENG
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In this work the synthesis of cubic, FDU-1 type, ordered mesoporous silica (OMS) was developed from two types of silicon source, tetraethyl orthosilicate (TEOS) and a less expensive compound, sodium silicate (Na(2)Si(3)O(7)), in the presence of a new triblock copolymer template Vorasurf 504 (EO(38)BO(46)EO(38)). For both silicon precursors the synthesis temperature was evaluated. For TEOS the effect of polymer dissolution in methanol and the acid solution (HCl and HBr) on the material structure was analyzed. For Na(2)Si(3)O(7) the influence of the polymer mass and the hydrothermal treatment time were the explored experimental parameters. The samples were examined by Small Angle X-ray Scattering (SAXS) and Nitrogen Sorption. For both precursors the decrease on the synthesis temperature from ambient, -25 degrees C, to -15 degrees C improved the ordered porous structure. For TEOS, the SAXS results showed that there is an optimum amount of hydrophobic methanol that contributed to dissolve the polymer but did not provoke structural disorder. The less electronegative Br-ions, when compared to Cl-, induced a more ordered porous structure, higher surface areas and larger lattice parameters. For Na(2)Si(3)O(7) the increase on the hydrothermal treatment time as well as the use of an optimized amount of polymer promoted a better ordered porous structure. (C) 2011 Elsevier B.V. All rights reserved.

Síntese e caracterização de catalisadores de níquel suportados em sílica mesoporosa altamente ordenada para hidrogenação de óleos vegetais; Synthesis and characterization of highly ordered mesoporous silica supported nickel catalysts for the hydrogenation of vegetable oils

Oliveira, Nara Andréa de
Fonte: Biblioteca Digitais de Teses e Dissertações da USP Publicador: Biblioteca Digitais de Teses e Dissertações da USP
Tipo: Dissertação de Mestrado Formato: application/pdf
Publicado em 14/04/2008 PT
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Este trabalho teve como objetivo a síntese e caracterização de sílicas mesoporosas suportadas com níquel para atuarem como catalisadores na hidrogenação de óleos vegetais. Foram escolhidas as sílicas mesoporosas ordenadas do tipo SBA-15 e FDU-1, sintetizadas a partir de TEOS como fonte de sílica e copolímeros triblocos como agentes direcionadores de estrutura em meio HCl. O Ni(NO3)2.6H2O foi utilizado como fonte de metal, cuja solução aquosa com a concentração de níquel desejada foi adicionada à sílica antes da remoção do molde polimérico, originando os precursores dos catalisadores. Após a impregnação, as amostras foram submetidas à calcinação sob atmosfera de ar, gerando o precursor na forma de óxido que ao ser tratado com H2 é reduzido Nio , forma ativa do catalisador. As técnicas de termogravimetria, termogravimetria derivada, difração de raios X a alto e baixo ângulo, isotermas de adsorção de nitrogênio e absorção atômica foram empregadas para a caracterização destes materiais. A TG/DTG foi utilizada para a simulação das melhores condições de calcinação/redução. As amostras foram calcinadas em um forno tubular com controlador de temperatura. Os ensaios de DRX confirmaram a fase NiO após calcinação e a fase Nio na redução...

About the thermal stability and pore elimination in the ordered hexagonal mesoporous silica SBA-15

Silveira, T. da; Awano, C. M.; Donatti, D. A.; Vicente, F. S. de; Vollet, D. R.
Fonte: Elsevier B.V. Publicador: Elsevier B.V.
Tipo: Artigo de Revista Científica Formato: 227-233
ENG
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Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP); Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq); Ordered hexagonal mesoporous silica was prepared using Pluronic P123 template and removal of the polymer by washing in ethanol. The thermal stability and the pore elimination was studied under heat treatment by a fixed time at 500, 600, 750, 825, 900, and 1050 degrees C. The most part of the porosity is built up by cylindrical pores belonging to the ordered hexagonal 2D pore structure. The lattice parameter and the pore volume of the hexagonal 20 structure diminish regularly with the temperature up to 900 degrees C. All porosity is eliminated at 1050 degrees C. The porosity elimination occurs in a mechanism described by a geometric model of contracting area, in which the diameter of the cylindrical pore diminishes while its length is kept constant. An activation energy of (92 +/- 2) kJ/mol was estimated for the process. The ordered porosity of an ethanol-washed and vacuum dried sample was found to be even larger with a narrower pore size distribution in comparison to a sample directly calcined at 500 degrees C without previous washing in ethanol. (C) 2014 Elsevier Inc. All rights reserved.

Adsorption properties of activated carbons and ordered mesoporous materials for organic pollutants in aqueous systems

Cansado, Isabel; Galacho, Cristina; Nunes, Angela; Carrott, Manuela; Carrott, Peter
Fonte: CIIEM - 2009 Publicador: CIIEM - 2009
Tipo: Artigo de Revista Científica
POR
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Adsorption properties of activated carbons and ordered mesoporous materials for organic pollutants in aqueous systems. livro de resumos do III Congresso Internacional de Engenharia e Gestão da Energia e Meio Ambiente

Pt-Ru Catalysts supported on mesoporous carbons for polymer electrolyte membrane fuel cells

Calderon, J. C.; Figueiredo, J. L.; Mahata, N.; Pereira, M. F. R.; Fernandes, Vitor R.; Rangel, C. M.; Pastor, E.; Calvillo, L.; Lázaro, M. J.
Fonte: Laboratório Nacional de Energia e Geologia Publicador: Laboratório Nacional de Energia e Geologia
Tipo: Conferência ou Objeto de Conferência
Publicado em 19/04/2010 ENG
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Pt-Ru electrocatalysts supported on xerogels and CMK-3 ordered mesoporous carbons were synthesized by reduction with formate ions (SFM method). Some of the carbon supports were chemically treated with HNO3 in order to generate oxygen groups on the surface, while other supports were heat treated. Physical characterization of the catalyst was obtained using X-ray dispersive energy (EDX) and X-ray diffraction (XRD) techniques. Results showed that Pt-Ru catalysts with similar metal content (20%) and atomic ratios (Pt:Ru 1:1) were obtained. The electrochemical activity was studied by cyclic voltammetry and chronoamperometry. Higher methanol oxidation current densities were found for catalyst deposited on chemically treated supports. Electrode preparation and MEA assembly allowed an in-house built direct methanol fuel to be fitted with the synthesized catalysts and supports in order to assess their performance. Cell and reactants were conditioned by a direct methanol test station. Polarisation curves were measured and confirmed data obtained by voltammetry, regarding the effect of heat treatment of the carbon support. Normalised power curves per weight of catalyst are discussed in terms of the significant impact on noble metal loading and attained cell maximum power...

Pineapple fruit bromelain recovery using recyclable functionalized ordered mesoporous silica synthesized from sugarcane leaf ash

Arumugam,A.; Ponnusami,V.
Fonte: Brazilian Society of Chemical Engineering Publicador: Brazilian Society of Chemical Engineering
Tipo: Artigo de Revista Científica Formato: text/html
Publicado em 01/09/2013 EN
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Bromelain, a protease enzyme found in Ananas comosus (Pineapple), was recovered from the fruit juice by adsorption using recyclable functionalized Santa Barbara Acid-15 (SBA-15) synthesized from sugarcane leaf ash. In this work, highly ordered mesoporous silica was synthesized from sugarcane leaf ash by a template-assisted method. It was successfully used as an adsorbent for the recovery of bromelain from pineapple fruit pulp. Amine-functionalized mesoporous silica exhibited a recovery efficiency of 97.89% and a 6.2-fold purification. It was also established that the adsorbent could be easily regenerated by adjusting the pH. In this study, the adsorbent was reused for three cycles without noticeable loss in recovery efficiency. Thus, adsroption using functionalized SBA-15 appears to be a promising alternate separation technique for the recovery of fruit bromelain.

Ordered mesoporous silica carrier system applied in nanobiothecnology

Sousa,Andreza de; Sousa,Edésia Martins Barros de
Fonte: Instituto de Tecnologia do Paraná - Tecpar Publicador: Instituto de Tecnologia do Paraná - Tecpar
Tipo: Artigo de Revista Científica Formato: text/html
Publicado em 01/10/2005 EN
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Ordered mesoporous materials like SBA15 possess a network of channels and pores of well-defined size in the nanoscale range (2-50 nm). This particular pore architecture makes them suitable candidates for hosting and delivery under appropriate conditions of a variety of molecules of pharmaceutical interest, including radiopharmaceuticals. The characteristics of SBA-15 prepared in different temperatures and the behavior of this system regarding microencapsulation of a model drug were investigated. The calcined samples were formed in 0.2 g disks and were soaked in a solution of atenolol used as a model drug. The modification of the aging temperature provoked changes in the structure of the pores, indicating the presence of microporosity and connections between mesopores. Aging the materials at a higher temperature resulted in no microporosity and this fact influenced the control of the release of the model drug.

Template Synthesis of Three-Dimensional Cubic Ordered Mesoporous Carbon With Tunable Pore Sizes

Dai, Weijie; Zheng, Mingbo; Zhao, Yu; Liao, Shutian; Ji, Guangbin; Cao, Jieming
Fonte: Springer Publicador: Springer
Tipo: Artigo de Revista Científica
Publicado em 14/10/2009 EN
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Three-dimensional cubic ordered mesoporous carbons with tunable pore sizes have been synthesized by using cubic Ia3d mesoporous KIT-6 silica as the hard template and boric acid as the pore expanding agent. The prepared ordered mesoporous carbons were characterized by powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and nitrogen adsorption–desorption analysis. The results show that the pore sizes of the prepared ordered mesoporous carbons with three-dimensional cubic structure can be regulated in the range of 3.9–9.4 nm. A simplified model was proposed to analyze the tailored pore sizes of the prepared ordered mesoporous carbons on the basis of the structural parameters of the silica template.

Influence of spatial configurations on electromagnetic interference shielding of ordered mesoporous carbon/ordered mesoporous silica/silica composites

Wang, Jiacheng; Zhou, Hu; Zhuang, Jiandong; Liu, Qian
Fonte: Nature Publishing Group Publicador: Nature Publishing Group
Tipo: Artigo de Revista Científica
Publicado em 19/11/2013 EN
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Ordered mesoporous carbons (OMCs), obtained by nanocasting using ordered mesoporous silicas (OMSs) as hard templates, exhibit unique arrangements of ordered regular nanopore/nanowire mesostructures. Here, we used nanocasting combined with hot-pressing to prepare 10 wt% OMC/OMS/SiO2 ternary composites possessing various carbon mesostructure configurations of different dimensionalities (1D isolated CS41 carbon nanowires, 2D hexagonal CMK-3 carbon, and 3D cubic CMK-1 carbon). The electric/dielectric properties and electromagnetic interference (EMI) shielding efficiency (SE) of the composites were influenced by spatial configurations of carbon networks. The complex permittivity and the EMI SE of the composites in the X-band frequency range decreased for the carbon mesostructures in the following order: CMK-3-filled > CMK-1-filled > CS41-filled. Our study provides technical directions for designing and preparing high-performance EMI shielding materials. Our OMC-based silica composites can be used for EMI shielding, especially in high-temperature or corrosive environments, owing to the high stability of the OMC/OMS fillers and the SiO2 matrix. Related shielding mechanisms are also discussed.

An ordered mesoporous WS₂ anode material with superior electrochemical performance for lithium ion batteries; An ordered mesoporous WS(2) anode material with superior electrochemical performance for lithium ion batteries

Liu, H.; Su, D.; Wang, G.; Qiao, S.
Fonte: Royal Soc Chemistry Publicador: Royal Soc Chemistry
Tipo: Artigo de Revista Científica
Publicado em //2012 EN
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Ordered mesoporous tungsten sulfide (WS₂) with high surface area and narrow pore size distribution was synthesized by a vacuum assisted impregnation route. The as-prepared mesoporous WS₂ exhibited a high lithium storage capacity of 805 mA h g−1 at a current of 0.1 A g−1 and an excellent high rate capability.; Hao Liu, Dawei Su, Guoxiu Wang and Shi Zhang Qiao

Adsorption performance of VOCs in ordered mesoporous silicas with different pore structures and surface chemistry

Dou, B.; Hu, Q.; Li, J.; Qiao, S.; Hao, Z.
Fonte: Elsevier Science BV Publicador: Elsevier Science BV
Tipo: Artigo de Revista Científica
Publicado em //2011 EN
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Ordered mesoporous silicas with different pore structures, including SBA-15, MCM-41, MCM-48 and KIT-6, were functionalized with phenyltriethoxysilane by a post-synthesis grafting approach. It was found that phenyl groups were covalently anchored onto the surface of mesoporous silicas, and the long-range ordering of the mesoporous channels was well retained after the surface functionalization. The static adsorption of benzene and the dynamic adsorption of single component (benzene) and bicomponent (benzene and cyclohexane) on the original and functionalized materials were investigated. As indicated by the adsorption study, the functionalized silicas exhibit improvement in the surface hydrophobicity and affinity for aromatic compounds as compared with the original silicas. Furthermore, the pore structure and the surface chemistry of materials can significantly influence adsorption performance. A larger pore diameter and cubic pore structure are favorable to surface functionalization and adsorption performance. In particular, the best adsorption performance observed with phenyl-grafted KIT-6 is probably related to the highest degree of surface functionalization, arising from the relatively large mesopores and bi-continuous cubic pore structure which allow great accessibility for the functional groups. In contrast...

Highly ordered mesoporous cobalt oxide nanostructures: synthesis, characterisation, magnetic properties, and applications for electrochemical energy devices

Wang, G.; Liu, H.; Horvat, J.; Wang, B.; Qiao, S.; Park, J.; Ahn, H.
Fonte: Wiley-V C H Verlag GMBH Publicador: Wiley-V C H Verlag GMBH
Tipo: Artigo de Revista Científica
Publicado em //2010 EN
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Highly ordered mesoporous Co₃O₄ nanostructures were prepared using KIT-6 and SBA-15 silica as hard templates. The structures were confirmed by small angle X-ray diffraction, high resolution transmission electron microscopy, and N₂ adsorption–desorption isotherm analysis. Both KIT-6 cubic and SBA-15 hexagonal mesoporous Co₃O₄ samples exhibited a low Néel temperature and bulk antiferromagnetic coupling due to geometric confinement of antiferromagnetic order within the nanoparticles. Mesoporous Co₃O₄ electrode materials have demonstrated the high lithium storage capacity of more than 1200 mAh g⁻¹ with an excellent cycle life. They also exhibited a high specific capacitance of 370 F g⁻¹ as electrodes in supercapacitors.; Guoxiu Wang, Hao Liu, Josip Horvat, Bei Wang, Shizhang Qiao, Jinsoo Park, and Hyojun Ahn

Highly ordered mesoporous MoS₂ with expanded spacing of the (002) crystal plane for ultrafast lithium ion storage; Highly ordered mesoporous MoS(2) with expanded spacing of the (002) crystal plane for ultrafast lithium ion storage

Liu, H.; Su, D.; Zhou, R.; Sun, B.; Wang, G.; Qiao, S.
Fonte: Wiley - VCH Verlag GmbH & Co KGaA Publicador: Wiley - VCH Verlag GmbH & Co KGaA
Tipo: Artigo de Revista Científica
Publicado em //2012 EN
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Highly ordered mesoporous MoS₂ with a high surface area and narrow pore-size distribution is synthesized by a vacuum assisted impregnation route. The mesoporous MoS₂ demonstrates an expanded d₀₀₂ spacing of 0.66 nm. The mesoporous MoS₂ electrode achieves an excellent high rate capacity of 608 mAh g⁻¹ at the discharge current of 10 A g⁻¹ (∼15C), which places MoS₂ as a viable next generation high power source for electric vehicles.; Hao Liu, Dawei Su, Ruifeng Zhou, Bing Sun, Guoxiu Wang, and Shi Zhang Qiao

Highly ordered mesoporous NiO anode material for lithium ion batteries with an excellent electrochemical performance

Liu, H.; Wang, G.; Liu, J.; Qiao, S.; Ahn, H.
Fonte: Royal Soc Chemistry Publicador: Royal Soc Chemistry
Tipo: Artigo de Revista Científica
Publicado em //2011 EN
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In this work, we have synthesized highly ordered mesoporous NiO materials by a nanocasting method using mesoporous silica KIT-6 as the hard templates. Mesoporous NiO particles were characterized by small angle X-ray diffraction (XRD), nitrogen adsorption/desorption, and transmission electron microscopy (TEM). The results demonstrated that the as-prepared mesoporous NiO had an ordered Ia3d symmetric mesostructure, with a high surface area of 96 m²/g. Mesoporous NiO materials were tested as an anode material for lithium ion batteries, exhibiting much lower activation energy (20.75 kJ mol⁻¹) compared to the bulk NiO (45.02 kJ mol⁻¹). We found that the mesoporous NiO electrode has higher lithium intercalation kinetics than its bulk counterpart. The specific capacity of mesoporous NiO after 50 cycles was maintained 680 mAh/g at 0.1 C, which was much higher than that of the commercial bulk NiO (188 mAh/g). Furthermore, at a high rate of 2C, the discharge capacity of mesoporous NiO was as high as 515 mAh/g, demonstrating the potential to be used for high power lithium ion batteries.; Hao Liu, Guoxiu Wang, Jian Liu, Shizhang Qiao and Hyojun Ahn

Highly ordered mesoporous Cr₂O₃ materials with enhanced performance for gas sensors and lithium ion batteries; Highly ordered mesoporous Cr(2)O(3) materials with enhanced performance for gas sensors and lithium ion batteries

Liu, H.; Du, X.; Xing, X.; Wang, G.; Qiao, S.
Fonte: Royal Soc Chemistry Publicador: Royal Soc Chemistry
Tipo: Artigo de Revista Científica
Publicado em //2012 EN
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Highly ordered mesoporous Cr₂O₃ materials with high specific surface area and narrow pore size distribution were successfully prepared by a vacuum assisted impregnation method. Both 2-dimensional hexagonal and 3-dimensional cubic Cr₂O₃ mesoporous replicas from SBA-15 and KIT-6 templates exhibit enhanced performance for gas sensors and lithium ion batteries, compared to the bulk Cr₂O₃ counterpart.; Hao Liu, Xiwen Du, Xianran Xing, Guoxiu Wang and Shi Zhang Qiao

Direct synthesis of ordered mesoporous carbons

Ma, T.Y.; Liu, L.; Yuan, Z.Y.
Fonte: Royal Society of Chemistry Publicador: Royal Society of Chemistry
Tipo: Artigo de Revista Científica
Publicado em //2013 EN
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Ordered mesoporous carbon materials have recently aroused great research interest because of their widespread applications in many areas such as adsorbents, catalysts and supports, gas storage hosts, and electrode materials. The direct synthesis strategy from organic-organic self-assembly involving the combination of polymerizable precursors and block copolymer templates is expected to be more flexible in preparing mesoporous carbons, compared with the traditional nanocasting strategy of complicated and high-cost procedures using mesoporous silica materials as the hard template. In this review, we present the fundamentals and recent advances related to the field of ordered mesoporous carbon materials from the direct synthesis strategy of block copolymer soft-templating, with a focus on their controllable preparation, modification and potential applications. Under the guidance of their formation mechanism, the preparation of ordered mesoporous carbons are discussed in detail by consulting different experimental conditions, including synthetic pathways, precursors, catalysts and templates. Both the mesopore size and morphology control are introduced. The potential applications of pure mesoporous carbons, nonmetallic- and metallic-modified mesoporous carbons...

Obtenção de sílicas mesoporosas altamente ordenadas a partir das cinzas da casca de arroz e do bagaço de cana-de-açúcar; Obtaining highly ordered mesoporous silica from rice husk and sugar cane bagasse ashes

Oliveira, Juliana Ferreira de
Fonte: Biblioteca Digitais de Teses e Dissertações da USP Publicador: Biblioteca Digitais de Teses e Dissertações da USP
Tipo: Dissertação de Mestrado Formato: application/pdf
Publicado em 11/12/2014 PT
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O presente trabalho propõe o uso das cinzas de dois resíduos agroindustriais - casca de arroz e bagaço de cana-de-açúcar - como fonte de sílica (SiO2) para a síntese de sílicas mesoporosas altamente ordenadas. Esta aplicação, além de agregar valor aos resíduos, busca uma alternativa ao tetraetil ortossicato, uma fonte de sílica dispendiosa, cuja obtenção resulta em danos ambientais. Amostras de cascas arroz de quatro procedências distintas foram caracterizadas por termogravimetria/ termogravimetria derivada (TG/DTG), calorimetria exploratória diferencial (DSC) e análise elementar de CHN. Com base nestes resultados, duas amostras foram selecionadas para obtenção de sílica. Outras duas amostras de bagaço de cana-de-açúcar de origens diferentes foram também caracterizadas por esta metodologia. Para melhor entender as etapas de degradação térmica da matéria orgânica, os resultados de TG/DTG foram associados aos de FT-IR e um estudo cinético por TG foi realizado. Diferentes tratamentos em meio ácido, com o objetivo de remover impurezas e reduzir o tempo necessário para calcinação dos materiais, foram realizados. O método escolhido para cada um dos materiais foi definido a partir dos testes e por avaliação de resultados de TG/DTG. As cinzas obtidas após calcinação em mufla dos materiais com e sem tratamento ácido prévio...

MESOPOROUS SILICA MATERIALS IN ASYMMETRIC CATALYSIS AND SELECTIVE FUNCTIONALIZATION

Seki, Tomohiro
Fonte: Quens University Publicador: Quens University
Tipo: Tese de Doutorado
EN; EN
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This thesis describes the synthesis and application of three types of selectively functionalized mesoporous materials. In the first section, periodically ordered mesoporous organosilicas (PMOs) are prepared that have the axially chiral bidentate phosphine ligand 2,2'-Bis(diphenylphosphino)-1,1'-binaphthyl (BINAP) embedded in the wall structure. Asymmetric hydrogenation of β-ketoesters under high-pressure hydrogen gas and hydrogen transfer reduction were carried out using Ru catalysts resulting from these materials. In the next chapter, our new methodology to selectively functionalize the internal/external surface of SBA-15, a mesoporous silica whose pore diameter is ~8 nm, by blocking the pore surface with reloaded Pluronic P123® micelles is presented. Multiple tests were attempted to validate the efficiency of the methodology including nitrogen adsorption, quantitative analysis by solid state NMRs, fluorescence measurements, elemental analysis and XPS. Eventually SS NMR proved to be the most appropriate. Finally, chapter four describes ordered organic materials in catalysis, namely star-shaped polymers containing chiral core-gels synthesized from chiral 1,1’- binaphthalene-2,2’-diol (BINOL) and 1,1’-binaphthalene-2,2’-diamine (BINAM). The kinetic resolution of 1-phenyl ethanol was carried out expecting to see differential affinity of the chiral core-gel to one enantiomer of the substrate in hydrogen transfer oxidation reaction.; Thesis (Ph.D...

New route toward building active ruthenium nanoparticles on ordered mesoporous carbons with extremely high stability

Yang, Ying; Sun, Chengjun; Ren, Yang; Hao, Shijie; Jiang, Daqiang
Fonte: Nature Publishing Group Publicador: Nature Publishing Group
Tipo: Artigo de Revista Científica
Publicado em 01/04/2014 EN
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Creating highly active and stable metal catalysts is a persistent goal in the field of heterogeneous catalysis. However, a real catalyst can rarely achieve both of these qualities simultaneously due to limitations in the design of the active site and support. One method to circumvent this problem is to fabricate firmly attached metal species onto the voids of a mesoporous support formed simultaneously. In this study, we developed a new type of ruthenium catalyst that was firmly confined by ordered mesoporous carbons through the fabrication of a cubic Ia3d chitosan-ruthenium-silica mesophase before pyrolysis and silica removal. This facile method generates fine ruthenium nanoparticles (ca. 1.7 nm) that are homogeneously dispersed on a mesoporous carbonaceous framework. This ruthenium catalyst can be recycled 22 times without any loss of reactivity, showing the highest stability of any metal catalysts; this catalyst displays a high activity (23.3 molLAh−1gmetal−1) during the catalytic hydrogenation of levulinic acid (LA) when the metal loading is 6.1 wt%. Even at an ultralow loading (0.3 wt%), this catalyst still outperforms the most active known Ru/C catalyst. This work reveals new possibilities for designing and fabricating highly stable and active metal catalysts by creating metal sites and mesoporous supports simultaneously.