Iron-modified mesoporous silica as efficient heterogeneous lewis acid catalysts

Iron-modified mesoporous silica as efficient heterogeneous lewis acid catalysts PDF Author: Wan Xu
Publisher:
ISBN:
Category :
Languages : en
Pages : 101

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Book Description
Les catalyseurs hétérogènes acides de Lewis ont principalement attiré beaucoup d'attention à cause de leurs applications dans de nombreux processus chimiques tels que le raffinage de pétrole. De plus, la facilité de séparer avec la phase liquide, et peu de déchets dangereux générés dans les processus répondent aux exigences de la chimie verte. Par conséquent, il est nécessaire de concevoir les catalyseurs acides de Lewis de façon simple, efficace, et peu couteux. Pour ce faire, la silice mésoporeuse peut agir comme support potentiel pour ce type de catalyseurs hétérogènes. La silice mésoporeuse possède les propriétés physiques et chimiques adaptées tel que la surface spécifique élevés, le volume de pore grand, la taille des pores accordable et ajustable, et la facilité de fonctionnalisation de la surface. Par conséquent, l'objectif de cette thèse est d'explorer un procédé de synthèse facile pour préparer 'un catalyseur d'acide de Lewis hétérogène efficace en utilisant la silice mésoporeuse ordonnée fonctionnalisé par des métaux peu couteux. Pour cela, les silices mésoporeuses du type MCM-41, et SBA-15 ont été choisis comme supports de catalyseur. Par la suite, Fe- MCM-41 et Fe-SBA-15 ont été correctement synthétisé en utilisant un procédé polyvalent. Le traitement de l'ammoniac au cours de la synthèse a été trouvé être un moyen efficace d'augmenter la teneur en fer tout en préservant la dispersion convenable des cations métalliques. Les paramètres physicochimiques de la silice mésoporeuse finale contenant du fer ont été obtenus par l'analyse d'adsorption-désorption d'azote à la base température, et l'environnement de la coordination des éléments en fer a été validé par la spectroscopie de UV-Vis réflectance diffusée et la spectroscopie photoélectronique à rayons X. L'acidité de surface a été sondé à l'aide des indicateurs de Hammett. Pour distinguer en outre les sites acides de Lewis sur la surface, l'adsorption de pyridine suivie par FTIR a été mise en oeuvre. Ces catalyseurs préparés ont été criblés dans la réaction d'aldolisation de Mukaiyama, qui est une réaction modèle catalysée par l'acide de Lewis. L'activité catalytique acide de Lewis des matériaux était peaufinées et les produits aldol ont été obtenus avec un bon rendement et la sélectivité. De plus, les catalyseurs hétérogènes sont très stables et peuvent être réutilisés au moins neuf fois en conservant l'activité catalytique.

Iron-modified mesoporous silica as efficient heterogeneous lewis acid catalysts

Iron-modified mesoporous silica as efficient heterogeneous lewis acid catalysts PDF Author: Wan Xu
Publisher:
ISBN:
Category :
Languages : en
Pages : 101

Get Book Here

Book Description
Les catalyseurs hétérogènes acides de Lewis ont principalement attiré beaucoup d'attention à cause de leurs applications dans de nombreux processus chimiques tels que le raffinage de pétrole. De plus, la facilité de séparer avec la phase liquide, et peu de déchets dangereux générés dans les processus répondent aux exigences de la chimie verte. Par conséquent, il est nécessaire de concevoir les catalyseurs acides de Lewis de façon simple, efficace, et peu couteux. Pour ce faire, la silice mésoporeuse peut agir comme support potentiel pour ce type de catalyseurs hétérogènes. La silice mésoporeuse possède les propriétés physiques et chimiques adaptées tel que la surface spécifique élevés, le volume de pore grand, la taille des pores accordable et ajustable, et la facilité de fonctionnalisation de la surface. Par conséquent, l'objectif de cette thèse est d'explorer un procédé de synthèse facile pour préparer 'un catalyseur d'acide de Lewis hétérogène efficace en utilisant la silice mésoporeuse ordonnée fonctionnalisé par des métaux peu couteux. Pour cela, les silices mésoporeuses du type MCM-41, et SBA-15 ont été choisis comme supports de catalyseur. Par la suite, Fe- MCM-41 et Fe-SBA-15 ont été correctement synthétisé en utilisant un procédé polyvalent. Le traitement de l'ammoniac au cours de la synthèse a été trouvé être un moyen efficace d'augmenter la teneur en fer tout en préservant la dispersion convenable des cations métalliques. Les paramètres physicochimiques de la silice mésoporeuse finale contenant du fer ont été obtenus par l'analyse d'adsorption-désorption d'azote à la base température, et l'environnement de la coordination des éléments en fer a été validé par la spectroscopie de UV-Vis réflectance diffusée et la spectroscopie photoélectronique à rayons X. L'acidité de surface a été sondé à l'aide des indicateurs de Hammett. Pour distinguer en outre les sites acides de Lewis sur la surface, l'adsorption de pyridine suivie par FTIR a été mise en oeuvre. Ces catalyseurs préparés ont été criblés dans la réaction d'aldolisation de Mukaiyama, qui est une réaction modèle catalysée par l'acide de Lewis. L'activité catalytique acide de Lewis des matériaux était peaufinées et les produits aldol ont été obtenus avec un bon rendement et la sélectivité. De plus, les catalyseurs hétérogènes sont très stables et peuvent être réutilisés au moins neuf fois en conservant l'activité catalytique.

Synthesis of Functionalised Mesoporous Silica for Capture and Transformation of Carbon Dioxide

Synthesis of Functionalised Mesoporous Silica for Capture and Transformation of Carbon Dioxide PDF Author: Maria Zakharova
Publisher:
ISBN:
Category :
Languages : en
Pages : 191

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Book Description
Nowadays over 80% of the chemical industry is based on heterogeneous catalytic processes supplying us with energy, aliments, medicines, crop protection, and new commodities. Even though catalysis remains a strategic field of chemistry, the level of understanding of heterogeneous catalysis is still quite limited, especially when compared to that of homogeneous catalysis. In the present work, we try to expand the knowledge of heterogeneous catalytic systems based on functionalized hybrid mesoporous silica and probe them in different green chemistry processes, especially in relation to the capture and transformation of CO2. For CO2 capture, the well-known concept of frustrated Lewis pairs is translated on the surface of mesoporous silica, resulting in the synthesis of stable heterogenized Lewis acid-base pairs. Firstly, the synthesis of Al-, Ti-, Zr-SBA-15 mesoporous silica carrying very strong Lewis acidic character through the reaction of surface silanol groups with homogeneous metallic complexes is presented. The ability of these materials to catalyse the direct amidation of electron-poor and bulky amines supports the presence of highly active Lewis acidic metallic centers and their water-tolerance. Furthermore, the development of solid supported frustrated Lewis pairs (sFLPs) using Al-, Ti-, Zr-SBA-15 mesoporous silica is discussed. A series of conventional Lewis bases, such as diethylenetriamine, diphenylphosphine derivatives, triethylamine, and tetramethylpiperidine are grafted or impregnated on the surface of Ti-, Al-, Zr-SBA-15 to generate air-stable solid-supported Lewis acid-base pairs. The preservation of both Lewis acidic and basic properties after the solid Lewis acid-base pairs are formed is examined. Study of their interactions with CO2 is performed using solid state NMR spectroscopy and CO2 adsorption experiments, which provides a new insight in their applicability as solid CO2 adsorbents. A correlation between the solid supported Lewis acid-base pair strength and the affinity to CO2 is proposed based on the calculation of isosteric heat of adsorption. For CO2 transformation, the study of confinement effect in silica nanopores and its application in catalytic cycloaddition of carbon dioxide to epoxides is presented. The synthesis of hybrid mesoporous adsorbents of CO2 on the base of MCM-41 and SBA-15 silica is performed and the criteria for an efficient catalytic system are defined and optimised, providing a novel and very efficient heterogeneous catalyst, capable of performing the transformation of carbon dioxide at room temperature under an atmospheric pressure without any chemical pre-activation of starting materials.

Micro-Mesoporous Metallosilicates

Micro-Mesoporous Metallosilicates PDF Author: Peng Wu
Publisher: John Wiley & Sons
ISBN: 3527350942
Category : Technology & Engineering
Languages : en
Pages : 501

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Book Description
Micro-Mesoporous Metallosilicates Up-to-date and in-depth text bridging the technology gap between fundamental research and industry-scale applications of porous materials for catalysis Micro-Mesoporous Metallosilicates: Synthesis, Characterization, and Catalytic Applications comprehensively introduces the chemistry and catalytic technologies of metallosilicates, an important family of microporous crystalline zeolite and heteroatom-containing mesoporous materials, with a primary focus on design synthesis, characterization, theoretical studies, and catalytic applications of titanosilicates, tin-silicates, germanosilicates and Ti-mesosilica, and more. The text covers recent advances in the synthesis of titanosilicates, including hydrothermal synthesis, dry-gel conversion, fluoride-assisted synthesis, and post-synthesis methods, along with the synthesis of metallosilicates with two-dimensional lamellar structures and their structural modifications as well as applications in selective oxidation reactions. The text also discusses synthesis of germanosilicates with specially designed organic structure-directing agents, synthesis and catalytic applications of heteroatom-containing mesoporous silica, and dendritic mesoporous silica nanoparticles with unique wrinkled center-radial structures. Overall, every important porous metallosilicate and its synthesis, characterization, pore engineering, catalytic application, and industrial technique and process are covered. Specific sample topics discussed in Micro-Mesoporous Metallosilicates include: Chemical post-modifications of titanosilicates, in terms of the effects on transfer, adsorption/desorption, and surface reactions X-Ray based techniques, ultraviolet-visible-near infrared spectroscopy, Raman spectroscopy, and solid-state NMR spectroscopy Theoretical calculation as an effective tool and supplement to understand the catalytic active center, structural character, and Brønsted/Lewis acidity Titanosilicates in the liquid-phase epoxidation reaction of propylene and propylene chloride to corresponding epoxides Effects of particle sizes, oxidation state, and location sites of Au nanoparticles, and epoxidation performance of Ti-containing materials Delivering cutting-edge research and bridging the technology gap between fundamental research and industrial applications, Micro-Mesoporous Metallosilicates is a valuable resource for chemists, materials scientists, chemical engineers, and experienced researchers in related fields.

Microporous and Mesoporous Solid Catalysts

Microporous and Mesoporous Solid Catalysts PDF Author: Eric G. Derouane
Publisher: John Wiley & Sons
ISBN: 9780470094204
Category : Science
Languages : en
Pages : 258

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Book Description
This series offers practical help for advanced undergraduate, graduate and postgraduate students, as well as experienced chemists in industry and academia working with catalysts in organic and organometallic synthesis. It features tested and validated procedures, authoritative reviews on classes of catalysts, and assessments of all types of catalysts. Micro- and Mesoporous Solid Catalysts describes the use of zeolites and mesoporous solids as catalysts for the production of fine and specialty chemicals. Specific tips and hints are provided and some typical procedures are described in detail In addition to discussing the pros and cons, several major organic transformations are examined including aromatic substitutions, heterocyclic ring formation, amines synthesis, oligomerisation, oxidation and hydroxylation, and other regioselective and stereoselective reactions Features tutorial introductory chapters, including tips and hints for achieving successful organic transformations Important reactions are featured together with recommendations to resolve potential problems.

Mesoporous Zeolites

Mesoporous Zeolites PDF Author: Javier García-Martínez
Publisher: John Wiley & Sons
ISBN: 3527335749
Category : Technology & Engineering
Languages : en
Pages : 608

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Book Description
Authored by a top-level team of both academic and industrial researchers in the field, this is an up-to-date review of mesoporous zeolites. The leading experts cover novel preparation methods that allow for a purpose-oriented fine-tuning of zeolite properties, as well as the related materials, discussing the specific characterization methods and the applications in close relation to each individual preparation approach. The result is a self-contained treatment of the different classes of mesoporous zeolites. With its academic insights and practical relevance this is a comprehensive handbook for researchers in the field and related areas, as well as for developers from the chemical industry.

Characterization of a Silica-supported Iron Lewis Acid Catalyst

Characterization of a Silica-supported Iron Lewis Acid Catalyst PDF Author: Daniel J. Casper
Publisher:
ISBN:
Category : Catalysts
Languages : en
Pages : 128

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Book Description


Modern Organic Synthesis

Modern Organic Synthesis PDF Author: George S. Zweifel
Publisher: John Wiley & Sons
ISBN: 1119086760
Category : Science
Languages : en
Pages : 416

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Book Description
This book bridges the gap between sophomore and advanced / graduate level organic chemistry courses, providing students with a necessary background to begin research in either an industry or academic environment. • Covers key concepts that include retrosynthesis, conformational analysis, and functional group transformations as well as presents the latest developments in organometallic chemistry and C–C bond formation • Uses a concise and easy-to-read style, with many illustrated examples • Updates material, examples, and references from the first edition • Adds coverage of organocatalysts and organometallic reagents

Green Chemistry and Catalysis

Green Chemistry and Catalysis PDF Author: R. A. Sheldon
Publisher: John Wiley & Sons
ISBN: 3527611010
Category : Science
Languages : en
Pages : 448

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Book Description
This first book to focus on catalytic processes from the viewpoint of green chemistry presents every important aspect: · Numerous catalytic reductions and oxidations methods · Solid-acid and solid-base catalysis · C-C bond formation reactions · Biocatalysis · Asymmetric catalysis · Novel reaction media like e.g. ionic liquids, supercritical CO2 · Renewable raw materials Written by Roger A. Sheldon -- without doubt one of the leaders in the field with much experience in academia and industry -- and his co-workers, the result is a unified whole, an indispensable source for every scientist looking to improve catalytic reactions, whether in the college or company lab.

Highly Efficient and Shape Selective Solid Acid Catalysts Based on Mesoporous Silica

Highly Efficient and Shape Selective Solid Acid Catalysts Based on Mesoporous Silica PDF Author: Yong Wang
Publisher:
ISBN:
Category : Chemical engineering
Languages : en
Pages : 2

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Book Description


Production of Biofuels and Chemicals with Bifunctional Catalysts

Production of Biofuels and Chemicals with Bifunctional Catalysts PDF Author: Zhen Fang
Publisher: Springer
ISBN: 9811051372
Category : Medical
Languages : en
Pages : 396

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Book Description
This book provides state-of-the-art reviews, current research, prospects and challenges of the production of biofuels and chemicals such as furanic biofuels, biodiesel, carboxylic acids, polyols and others from lignocellulosic biomass, furfurals, syngas and γ-valerolactone with bifunctional catalysts, including catalytic, and combined biological and chemical catalysis processes. The bifunctionality of catalytic materials is a concept of not only using multifunctional solid materials as activators, but also design of materials in such a way that the catalytic materials have synergistic characteristics that promote a cascade of transformations with performance beyond that of mixed mono-functional catalysts. This book is a reference designed for researchers, academicians and industrialists in the area of catalysis, energy, chemical engineering and biomass conversion. Readers will find the wealth of information contained in chapters both useful and essential, for assessing the production and application of various biofuels and chemicals by chemical catalysis and biological techniques.