Дисертації з теми "Crystalline Covalent Organic Frameworks"
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Baldwin, Luke Adam. "Synthesis of Dehydrobenzoannulene-Based Covalent Organic Frameworks." The Ohio State University, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=osu1491561788473597.
Повний текст джерелаDogru, Mirjam. "Functionalization of covalent organic frameworks." Diss., Ludwig-Maximilians-Universität München, 2012. http://nbn-resolving.de/urn:nbn:de:bvb:19-140963.
Повний текст джерелаSpasic, Marko. "Redox-active covalent organic frameworks." Thesis, Uppsala universitet, Institutionen för kemi - BMC, 2021. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-449962.
Повний текст джерелаCARNEIRO, LEONARDO SIMÕES DE ABREU. "CARBAZOLE-BASED COVALENT ORGANIC FRAMEWORKS: CONCEPTION, SYNTHESIS AND CHARACTERIZATION." PONTIFÍCIA UNIVERSIDADE CATÓLICA DO RIO DE JANEIRO, 2016. http://www.maxwell.vrac.puc-rio.br/Busca_etds.php?strSecao=resultado&nrSeq=28356@1.
Повний текст джерелаCONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICO
Materiais bidimensionais apresentam possibilidades de funcionalização que os tornam versáteis para diversas aplicações, tais como em dispositivos eletrônicos. A presença de poros nesses materiais pode trazer novas funções, como adsorção de gases, liberação controlada de fármacos e catálise. Os covalent organic frameworks (COFs) são uma nova classe de materiais orgânicos porosos cristalinos que têm recebido destaque em química reticular. O objetivo dessa dissertação é apresentar a síntese e caracterização de quatro novos COFs baseados em carbazóis, que constitui uma classe de compostos utilizada na obtenção de polímeros condutores. O bloco de montagem principal utilizado foi o 3,6-diamino-9H-carbazol e as fontes de aldeído foram triformilfloroglucinol, triformilfenol, 1,3,5-tri(4-formilfenil)benzeno e triformilbenzeno para a síntese do RIO2, RIO3, RIO5 e RIO6, respectivamente. RIO2 e RIO3 apresentaram-se sob a forma ceto enamina e imina, respectivamente, além de pouca cristalinidade e baixa área específica. Através de cálculos baseados na Teoria do Funcional da Densidade (DFT), foi verificado que esses COFs apresentam suas folhas deslocadas e rotacionadas devido às interações eletrostáticas e para minimizar os momentos de dipolo das ligações N-H dos carbazóis. RIO5 e RIO6 também se apresentaram pouco cristalinos e com áreas específicas baixas. Apesar desses resultados, esses materiais ainda podem ser aplicados em eletrônica orgânica por apresentarem estrutura química compatível com tal aplicação.
Two-dimensional materials have functionalization possibilities that make them versatile for various applications such as in electronic devices. The presence of pores in these materials can give new features to them, such as gas adsorption, drug delivery and catalysis. The covalent organic frameworks (COFs) are a new class of crystalline porous organic materials that have been prominent in reticular chemistry. The purpose of this work is to present the synthesis and characterization of four new COFs based on carbazoles, which are a class of compounds used to obtain conductive polymers. The main building block used was 3,6-diamine-9H-carbazole with the aldehyde sources were triformylphloroglucinol, triformylphenol, 1,3,5-tri(4 formylphenyl)benzene and triformylbenzene to obtain RIO2, RIO3, RIO5 and RIO6, respectively. RIO2 and RIO3 are in keto-enamine and imine form, respectively, as well as have low crystallinity and low specific area. Calculus based on Density Functional Theory (DFT) found that these COFs present their sheets displaced and rotated due to electrostatic interactions and to minimize the dipole moments of the N-H bonds of carbazoles. In an attempt to avoid the absence of pores, RIO5 and RIO6 materials were synthesized, however these COFs also performed poorly crystalline and with low specific areas. Despite these results, these materials can also be applied in organic electronics by presenting chemical structure compatible with such application.
Crowe, Jonathan William. "Design and Synthesis of Dehydrobenzoannulene Based Covalent Organic Frameworks." The Ohio State University, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=osu1492098595103764.
Повний текст джерелаDogru, Mirjam [Verfasser], and Thomas [Akademischer Betreuer] Bein. "Functionalization of covalent organic frameworks / Mirjam Dogru. Betreuer: Thomas Bein." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2012. http://d-nb.info/1020790482/34.
Повний текст джерелаDienstmaier, Jürgen. "From supramolecular self-assembly to two-dimensional covalent organic frameworks." Diss., Ludwig-Maximilians-Universität München, 2013. http://nbn-resolving.de/urn:nbn:de:bvb:19-156623.
Повний текст джерелаBeirl, Toni Marie. "Synthesis and Characterization of Novel Imine-Linked Covalent Organic Frameworks." The Ohio State University, 2015. http://rave.ohiolink.edu/etdc/view?acc_num=osu1437559176.
Повний текст джерелаHunt, Joseph Ray. "Synthesis, characterization, and gas adsorption properties of covalent organic frameworks." Diss., Restricted to subscribing institutions, 2009. http://proquest.umi.com/pqdweb?did=1779835631&sid=1&Fmt=2&clientId=1564&RQT=309&VName=PQD.
Повний текст джерелаTurangan, Nikka Maria Joezar. "Synthesis and characterisation of covalent organic frameworks as thin films." Thesis, Queensland University of Technology, 2019. https://eprints.qut.edu.au/129108/1/Nikka_Turangan_Thesis.pdf.
Повний текст джерелаRager, Sabrina [Verfasser], and Thomas [Akademischer Betreuer] Bein. "Tailoring the features of covalent organic frameworks / Sabrina Rager ; Betreuer: Thomas Bein." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2019. http://d-nb.info/1214593186/34.
Повний текст джерелаGreenwood, John. "Investigations into surface-confined covalent organic frameworks : towards developing novel enantioselective heterogeneous catalysts." Thesis, University of St Andrews, 2013. http://hdl.handle.net/10023/4293.
Повний текст джерелаCalik, Mona Julia [Verfasser], and Thomas [Akademischer Betreuer] Bein. "Development of functional covalent organic frameworks for optoelectronics / Mona Julia Calik ; Betreuer: Thomas Bein." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2016. http://d-nb.info/1138922811/34.
Повний текст джерелаKatekomol, Phisan [Verfasser], and Arne [Akademischer Betreuer] Thomas. "From Low-Temperature Carbons to Novel Covalent-Organic Frameworks / Phisan Katekomol. Betreuer: Arne Thomas." Berlin : Universitätsbibliothek der Technischen Universität Berlin, 2013. http://d-nb.info/1035802236/34.
Повний текст джерелаLohse, Maria [Verfasser], and Thomas [Akademischer Betreuer] Bein. "Structural investigations and postsynthetic modifications in covalent organic frameworks / Maria Lohse ; Betreuer: Thomas Bein." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2017. http://d-nb.info/1180981723/34.
Повний текст джерелаYazdi, Amirali. "Nanoengineering composites made of metal- and covalent- organic frameworks and inorganic nanoparticles using encapsulation techniques." Doctoral thesis, Universitat Autònoma de Barcelona, 2018. http://hdl.handle.net/10803/666772.
Повний текст джерелаThe present PhD Thesis has been dedicated to the design and synthesis of a new type of composites of metal-organic frameworks (MOFs) or covalent-organic frameworks (COFs) with inorganic nanoparticles (iNPs) and the use of these composites for heterogeneous catalysis. In the first chapter, we introduce the family of composites made by supporting iNPs on/in different materials, focusing on those constructed with MOFs and COFs. Then, the general objectives of the Thesis are described in Chapter 2. Chapter 3 shows the results in “The influence of the MOF shell thickness on the catalytic performance of composites made of inorganic (hollow) nanoparticles encapsulated into MOFs”, Catalysis Science & Technology (2016). Herein, we report the encapsulation of hollow Pt or Pd nanoparticles (NPs) into ZIF-8, making a series of composites in which the ZIF-8 shell thickness has been systematically varied. By using these composites as catalysts for the reduction of 4-nitrophenol and Eosin Y, we show that the MOF shell thickness plays a key role in the catalytic performance of this class of composites. In Chapter 4, hybrid core-shell Au/CeO2 NPs dispersed in UiO-66 shaped into microspherical beads are created using the spray-drying continuous-flow method. The combined catalytic properties of nanocrystalline CeO2 and Au in a single particle and the support and protective function of porous UiO-66 beads make the resulting composites show good performances as catalysts for CO oxidation (T50 = 72 °C; T100 = 100 °C) and recyclability. The results are included in the manuscript entitled “Core-shell Au/CeO2 nanoparticles supported in UiO-66 beads exhibiting full CO conversion at 100 °C”, Journal of Materials Chemistry A (2017). Finally, in Chapter 5, we demonstrated a two-step method that enables imparting new functionalities to COFs by nanoparticle confinement. The direct reaction between 1,3,5-tris(4-aminophenyl)benzene and 1,3,5-benzenetricarbaldehyde in the presence of a variety of metallic/metal-oxide nanoparticles resulted in the embedding of the nanoparticles in amorphous and nonporous imine-linked polymer organic spheres. Post-treatment reactions of these polymers with acetic acid under reflux led to crystalline and porous imine-based COF- hybrid spheres. Interestingly, porous imine-based COF-hybrids with Au and Pd NPs were found to be catalytically active. These results have been reported in the publication entitled “Confining Functional Nanoparticles into Colloidal Imine-Based COF Spheres by a Sequential Encapsulation-Crystallization Method”. Chemistry a European Journal (2017).
Dienstmaier, Jürgen [Verfasser], and Markus [Akademischer Betreuer] Lackinger. "From supramolecular self-assembly to two-dimensional covalent organic frameworks / Jürgen Dienstmaier. Betreuer: Markus Lackinger." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2013. http://d-nb.info/1034813374/34.
Повний текст джерелаWang, Mingchao, Marco Ballabio, Mao Wang, Hung-Hsuan Lin, Bishnu P. Biswal, Xiaocang Han, Silvia Paasch, et al. "Unveiling Electronic Properties in Metal–Phthalocyanine-Based Pyrazine-Linked Conjugated Two-Dimensional Covalent Organic Frameworks." American Chemical Society, 2019. https://tud.qucosa.de/id/qucosa%3A72450.
Повний текст джерелаSchwartz, Heidi Annemarie [Verfasser]. "Metal-Organic Frameworks as Crystalline Porous Hosts for Photoactive Molecules / Heidi Annemarie Schwartz." München : Verlag Dr. Hut, 2018. http://d-nb.info/1168534356/34.
Повний текст джерелаSick, Torben [Verfasser], and Thomas [Akademischer Betreuer] Bein. "Synthesis and characterization of nanoporous covalent organic frameworks for optoelectronic applications / Torben Sick ; Betreuer: Thomas Bein." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2018. http://d-nb.info/121549971X/34.
Повний текст джерелаKeller, Niklas [Verfasser], and Thomas [Akademischer Betreuer] Bein. "Design principles to enhance optoelectronic properties in oligothiophene-based covalent organic frameworks / Niklas Keller ; Betreuer: Thomas Bein." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2020. http://d-nb.info/1228270562/34.
Повний текст джерелаBasagni, Andrea. "Covalent stabilization of 2D self-assembled nanostructures on surfaces." Doctoral thesis, Università degli studi di Padova, 2016. http://hdl.handle.net/11577/3424495.
Повний текст джерелаLa scoperta del grafene ha suscitato grande interesse verso i materiali a bassa dimensionalità (0D, 1D e 2D) e uno sforzo congiunto tra i diversi rami della scienza è orientato verso la produzione di nuovi materiali con proprietà analoghe a quelle del grafene, ma controllabili. La sintesi su superficie in condizioni di ultra-alto vuoto (UHV) sembra essere promettente per la produzione di nanostrutture organiche. Infatti, in queste condizioni, è possibile avere un’ampia varietà di materiali, un perfetto controllo delle condizioni di reazione, della simmetria della superficie e della sua corrugazione. Questi sono solo alcuni dei vantaggi che l’UHV offre. Sebbene varie reazioni siano state testate negli ultimi anni, sembra chiaro che per realizzare monostrati polimerici ordinati siano necessiari approcci più complessi. In questo lavoro di Tesi, la sintesi di nanostrutture polimeriche su superficie è stata studiata per diverse reazioni, substrati e condizioni di reazione. La microscopia ad effetto tunnel e la spettroscopia di fotoemissione a raggi X sono state utilizzate per la caratterizzazione dei diversi sistemi permettendo un'analisi complementare delle strutture molecolari e dei loro stati chimici. In particolare, le reazioni attivate termicamente sono state utilizzate per polimerizzare gradualmente il 4,4"-dibromo-terfenile e ottenere, in un primo step di reazione, per mezzo della reazione di Ullmann su Au (111), il poli-parafenilene, ,e poi nanoribbons di grafene dopo l'attivazione del legami C-H. Un delicato equilibrio tra l'attività catalitica della superficie, la mobilità molecolare e l’organizzazione molecolare ha permesso di ottenere strutture ordinate estese. Inoltre, sfruttando questa metodica, sono stati ottenuti tre differenti polimeri 1D, caratterizzati da un crescente contenuto di azoto. Campioni macroscopicamente anisotropici sono stati preparati sfruttando l'effetto templante delle superfici vicinali e, grazie alla spettroscopia di fotoemizzione risolta in angolo, è stato rivelato che la struttura elettronica dei polimeri drogati è rigidamente spostata verso energie minori rispetto al livello di Fermi del metallo all'aumentare del contenuto di azoto. Infine, è stata esplorata l'attivazione fotochimica di diversi gruppi funzionali. Questi studi rappresentano un passo avanti verso l’applicazione della fotochimica alla sintesi su superficie, che attualmente sfrutta solo gruppi diacetilenici, e apre nuove opportunità per l'utilizzo di diversi gruppi funzionali organici come centri fotoattivi.
Pyles, David Andrew. "Design and Application of Novel Benzobisoxazole and Benzobisthiazole Linked Porous Polymers." The Ohio State University, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=osu155428770646841.
Повний текст джерелаStegbauer, Linus Martin [Verfasser], and Bettina [Akademischer Betreuer] Lotsch. "Two-dimensional covalent organic frameworks as platforms for renewable energy and environmental applications / Linus Martin Stegbauer ; Betreuer: Bettina Lotsch." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2016. http://d-nb.info/1184794065/34.
Повний текст джерелаGottschling, Kerstin [Verfasser], and Bettina [Akademischer Betreuer] Lotsch. "Towards single-site heterogeneous catalysts for the hydrogen evolution reaction based on covalent organic frameworks / Kerstin Gottschling ; Betreuer: Bettina Lotsch." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2020. http://d-nb.info/1218466081/34.
Повний текст джерелаMotegi, Hirofumi. "Synthesis and Characterization of Crystalline Coordination Networks Constructed From Neutral Imidazole Containing Ligand and Rigid Aromatic Carboxylate." Diss., Virginia Tech, 2010. http://hdl.handle.net/10919/77201.
Повний текст джерелаPh. D.
Brunet, Gabriel. "Investigating the Single Crystal to Single Crystal Transformations of Highly Porous Metal-Organic Frameworks Through the Crystalline Sponge Method." Thesis, Université d'Ottawa / University of Ottawa, 2016. http://hdl.handle.net/10393/34308.
Повний текст джерелаBushell, Alexandra. "Mixed matrix membranes of a polymer of intrinsic microporosity with crystalline porous solids." Thesis, University of Manchester, 2012. https://www.research.manchester.ac.uk/portal/en/theses/mixed-matrix-membranes-of-a-polymer-of-intrinsic-microporosity-with-crystalline-porous-solids(6166d350-d969-49bc-8108-1c9afcaaa2f9).html.
Повний текст джерелаTian, Yuyang. "Synthesis and characterization of crystalline microporous materials : investigation of new synthetic routes." Thesis, University of St Andrews, 2014. http://hdl.handle.net/10023/6371.
Повний текст джерелаSchwartz, Heidi Annemarie [Verfasser], Uwe [Gutachter] Ruschewitz, Dominik [Gutachter] Schaniel, and Christoph [Gutachter] Janiak. "Metal-Organic Frameworks as Crystalline Porous Hosts for Photoactive Molecules / Heidi Annemarie Schwartz ; Gutachter: Uwe Ruschewitz, Dominik Schaniel, Christoph Janiak." Köln : Universitäts- und Stadtbibliothek Köln, 2018. http://d-nb.info/1165256169/34.
Повний текст джерелаHaase, Frederik [Verfasser], and Bettina [Akademischer Betreuer] Lotsch. "Tuning the structure and properties of nitrogen-rich covalent organic frameworks by molecular design and solid state reactions / Frederik Haase ; Betreuer: Bettina Lotsch." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2018. http://d-nb.info/1184202494/34.
Повний текст джерелаGarzón, Tovar Luis Carlos. "Confining Reactions in a Droplet: Synthesis of MOFs, COFs and Composites using Spray-Drying." Doctoral thesis, Universitat Autònoma de Barcelona, 2018. http://hdl.handle.net/10803/664004.
Повний текст джерелаA new age in materials chemistry started with the discovery of Metal-Organic Frameworks and Covalent-Organic frameworks. In particular, the introduction of reticular chemistry represented a revolutionary strategy that gave chemists infinite opportunities toward the design and construction of novel functional materials with exceptional properties, such as their high porosity, high structural/compositional flexibility and low densities (for COFs). Indeed, these properties render MOFs and COFs as promising materials for multiple applications of commercial interest, including gas storage and separation, catalysis, sensing, drug delivery, water harvesting and adsorptive heat transformation systems. These possibilities have promoted a rapid and explosive pace of expansion in this field and as a result, academia and industry have begun to propose several initiatives towards the commercialization of these porous materials. However, despite these efforts, the scientific community has also recognized that the use of these materials could be limited by the challenges pertaining to their production methods at large scale since harsh conditions are usually needed to synthesize them. In this sense, novel approaches for their synthesis have been developed recently. In particular, the spray-drying method has emerged as a promising technology for the synthesis of MOFs at large scale. However, spray-drying is still in its embryonic stage and therefore, there are many challenges that need to be overcome. In this Thesis, we have developed new strategies to synthesize MOFs. In particular, we describes a new methodology based on coupling two processes —spray-drying and continuous flow— for continuous synthesis of MOFs assembled from high-nuclearity secondary building units (SBUs). In addition, we demonstrated that the spray-drying-continuous flow method can be used not only to synthesize MOF superstructures but also to incorporate functional species, thereby providing a new route for the synthesis of MOF-based composites. In this thesis, we extend the use of spray-drying technique to covalent chemistry. To this end, we show that different imines can be synthesized from Schiff-base condensation reactions between discrete aldehydes and amines using the spray-drying. We also show that this chemistry can be extended to post-synthetically modify MOFs. For example, we show the post-synthetic modification of two MOFs, the amine-terminated UiO-66-NH2 and the aldehyde-terminated ZIF-90. Moreover, we demonstrate that the Schiff-base condensation reactions can be extended to the synthesis of COFs. Thus, we prove that spherical superstructures made from the assembly of imine-based COF nanocrystals can be obtained by combining the spray-drying technique with a dynamic covalent chemistry process. In addition, we show that this methodology enables the integration of other functional materials such as dyes and magnetic nanoparticles into these superstructures forming COF-based composites.
Wang, Zhiyong, Gang Wang, Haoyuan Qi, Mao Wang, Mingchao Wang, SangWook Park, Huaping Wang, et al. "Ultrathin Two-Dimensional Conjugated Metal-Organic Framework Single-Crystalline Nanosheets Enabled by Surfactant-Assisted Synthesis." Royal Society of Chemistry, 2020. https://tud.qucosa.de/id/qucosa%3A72508.
Повний текст джерелаJuvenal, Frank. "Polymères de coordination luminescents 1D et 2D avec des ligands rigides contenant du Pt(II) montrants des propriétés d’adsorption du CO2." Mémoire, Université de Sherbrooke, 2017. http://hdl.handle.net/11143/10578.
Повний текст джерелаAbstract: The design of new functional materials has a long history. For the past two decades, the field of organic and inorganic polymers has attracted attention of researchers. More importantly, porous materials such as Metal Organic Frameworks (MOFs), Covalent Organic Frameworks (COFs) as well as porous coordination polymers are now being intensively studied due to their potential applications including gas storage, gas separations, catalyst and sensing. On another hand, Pt-containing polymers have shown potential applications in solar cells and light emitting diodes. The masters’ thesis is mainly divided into three main sections presenting new results. In the first section; Chapter 2 mainly discusses the formation of coordination polymers with CuX salts (X= Cl, Br, I) and trans-[p-MeSC6H4C≡C-Pt(PMe3)2-C≡CC6H4SMe] (L1), in either PrCN or PhCN. The resulting polymers obtained were 2D (bidimensional) CPs or 1D (unidimensional) CPs in all cases. However, 2D CPs obtained when CuBr salt is used by either using PrCN or PhCN did not incorporate the solvents in their cavities. On the other hand, the 2D CP and the rest of 1D CPs obtained had either the crystallization molecules in the cavities or coordinated to the copper cluster. The copper-halide clusters were either the rhomboids Cu2X2 fragments or the step cubane Cu4I4. The photophysical measurements in the presence and absence of solvent crystallization molecules were performed. In addition, the porosity of the CPs was evaluated by adsorption isotherms. The vapochromism of the solvent-free 2D and 1D CPs were investigated as well as CO2 sorption measurements were perfomed. Furthermore, we then attempted to use CuCN and L1 in MeCN which is reported in the second section as Chapter 3. The obtained CP was unexpected as L1 broke and a cyanide (CN‾) ion coordinated to the Pt atom leading to the formation of zigzag 1D CP. The coordination bonds Cu-S or/and Cu([eta]2-C≡C) were generally observed with L1, but not in the CuCN case. Instead a 1D chain of (CuCN)n was made and the broken L1 now binds the chain via a Cu-N bond. The photophysical and thermal stability properties were studied. Lastly, the third section, Chapter 4 deals with a potential predictability of CP formation by using CuX salts (X= Cl, Br, I) and either trans-[p-MeSC6H4C≡C-Pt(PMe3)2-C≡CC6H4SMe] (L1) or trans-[p-MeSC6H4C≡C-Pt(PEt3)2-C≡CC6H4SMe] (L2) in MeCN as the solvent. The use of L1 resulted in either 2D or 1D CPs with the MeCN trapped inside of the cavities while L2 resulted in 1D CPs without MeCN being present in their cavities. The thermogravimetric, photophysical as well as gas sorption measurements (only for those with crystalisation molecules) were perfomed.
Werner, Veronika [Verfasser], and Paul [Akademischer Betreuer] Knochel. "Regioselective functionalization of aromatics and heterocycles bearing a bis-silyl-methyl group, one-pot procedure for the preparation of tertiary amines via iminium ions and preparation of new benzodithiophene building blocks for covalent organic frameworks / Veronika Werner ; Betreuer: Paul Knochel." München : Universitätsbibliothek der Ludwig-Maximilians-Universität, 2015. http://d-nb.info/1127528041/34.
Повний текст джерелаAssi, Hala. "Nouveaux polymères de coordination à base de titane et de dérivés phénoliques." Thesis, Université Paris-Saclay (ComUE), 2016. http://www.theses.fr/2016SACLV072/document.
Повний текст джерелаCrystalline Metal-Organic Frameworks MOFs are one of the most recent classes of crystalline porous coordination polymers. Due to the variety of their structure and composition, they are currently considered as promising candidates in various domains (gas storage, fluid separation, catalysis, biomedicine…). However, the literature on the photocatalytic activity of these solids has exploded only very recently, although the many advantages of using these materials as heterogeneous photocatalysts in comparison with classical semiconductors. Considering the well-established photocatalytic properties of TiO2, it seems logical to focus on titanium in order to design new MOFs for such applications. Nevertheless, because of the difficulty in controlling the reactivity of these ions in solution (especially out of the very acidic conditions), very few crystalline titanium-based MOFs have been described, among the numerous MOFs known in the literature. Thus, obtaining titanium-based MOFs in water and basic medium remains a big challenge. In our work, some strategies has been followed in order to benefice from the advantages of the titanium ions and at the same time confront their limitations by focusing on the exploration of the chemistry of Ti4+ ions (titanium alkoxides, complexes and oxo-clusters) with various polytopic ligands, especially hydroxycarboxylate and polycatecholate derivatives in order to design new stable titanium-based MOFs. Such ligands provide important advantages in comparison with pure carboxylates, such as a potentially higher structural diversity, stronger Ti-O bonds leading to an enhanced chemical stability in basic medium, and a strong absorption in the visible range ensured by ligand to metal charge transfer. On the other hand, the use of titanium molecular complexes or oxo-clusters will be a promising opportunity in order to control the spontaneous hydrolysis and the high activity of Ti4+ ions. By privileging the solvo- and hydrothermal synthesis using the «high-throughput system», these strategies lead to obtain new crystalline solids (molecular and 1D/2D/3D polymeric compounds). The synthesis, the structural characterization by a combination of different technics (X-ray diffraction, TGA analysis, IR spectroscopy, Solid State NMR, sorption measurement…), the study of some properties and the preliminary photocatalytic experiments (water splitting reaction) of these new solids will be discussed in this manuscript
Santos, Rúben Filipe Pinto. "Modulation of crystalline structures of metal-organic frameworks." Master's thesis, 2021. http://hdl.handle.net/10773/32751.
Повний текст джерелаO maior foco da investigação da área de MOFs nos últimos anos tem sido a sintese e possíveis aplicações destes materiais. Uma das etapas importante desse processo é a caracterização dos mesmos. Para isso, os investigadores recorrem a técnicas como DRX (Diffraction X-Ray) para efetuar modelação dos dados experimentais e refinar as estruturas. Porém estas técnicas muitas vezes estão dependentes de parâmetros que nem sempre são fáceis de definir. Este facto leva a que os investigadores por vezes não conheçam com exatidão as estruturas cristalinas de alguns materiais. O objetivo desta dissertação é o de dar os primeiros passos na criação de um programa de modulação que gere uma biblioteca de possíveis estruturas que possam ser depois ser comparadas com os dados experimentais, obtendo assim uma possível solução para este problema. Sendo o campo da Matemática aplicada aos MOFs um campo praticamente inexplorado, a primeira abordagem foi a de explorar estururas químicas com ligações à Matemática bem documentadas. Neste contexto surgiram os Fulerenos onde foram estudados diversos aspetos matemáticos como aplicações da Teoria dos Grafos e de Geometria. Dada a natureza simétrica dos MOFs, foram também explorados conceitos de Simetria como os grupos de frisos e papéis de parede, bem como de Cristalografia com o estudo dos diferentes tipos de reticulados. Procedeu-se ainda a um estudo estatístico sobre a natureza e possíveis distorções das esferas de coordenação dos centros metálicos presentes nos MOFs (focado na primeira serie dos metais de transição).
Mestrado em Matemática e Aplicações
Gagnon, Kevin James. "Crystalline Metal-Organic Frameworks Based on Conformationally Flexible Phosphonic Acids." Thesis, 2013. http://hdl.handle.net/1969.1/151137.
Повний текст джерелаAbuzeid, Hesham Rashed, and 何杉. "Construction of Covalent Benzoxazine/Organic Frameworks for CO2 Uptake and Supercapacitors Applications." Thesis, 2019. http://ndltd.ncl.edu.tw/handle/vk8v3v.
Повний текст джерела國立中山大學
材料與光電科學學系研究所
107
In this thesis, we report the first covalent benzoxazine framework (CBF-1) in addition to new dual-pore and single-pore Covalent organic frameworks and their application for CO2 uptake and supercapacitor. First, Covalent benzoxazine framework (CBF-1) was synthesized via a solvothermal method using trifunctional aminophenyl triazine (TAPT), and trifunctional hydroxyphenyl triazine (THPT) paraformaldehyde through Mannich condensation reaction. This new CBF-1 underwent thermal cross-linked curing to generate a highly cross-linked CBF (CCBF-1), which, with carbonization followed by KOH activation, was converted into nitrogen-doped microporous carbon (N-DMC). The thermal curing, carbonization, and activation for CBF-1 have dramatically enhanced the thermal properties and BET surface area. Interestingly, the formed N-DMC exhibited a spherical morphology with excellent thermal stability (up to Td5 of 663 ºC and char yield of 85%), high BET surface areas (up to 1469 m2 g-1), and pore size of 2.07 nm. The thermal transformation from CBF-1 to CCBF-1, then to N-DMC directly enhanced the CO2 capture and electrochemical capacitance. N-DMC showed excellent CO2 capture capacities of 3.85 and 7.46 mmol/g at 298 and 273 K, respectively. Moreover, N-DMC showed high electrochemical capacitance of 185 Fg-1 at current density 1.0 Ag-1, and excellent stability performance of 86% average retention at 20 Ag-1 after 4000 cycles. In addition, we report a conceptual strategy to study the effect of supramolecular interactions on the topological regulating of 2D COFs as a new technique to manage their properties. Our strategy was achieved by introducing pristine and substituted diamines monomers; Benzidine (BD) and 1,4-dihydroxybenzidine (DHBD) into the skeleton of bicarbazole monomer. The newly designed microporous bicarbazole COFs (Cz-BD and Cz-DHBD) with 1D open micropores were designed using a [C2 + C2] topology diagram and successfully synthesized via a Schiff-base condensation reaction of tetraformyl-bicarbazole as C2 knot and aromatic diamines as C2 linker. The resulting COFs have two different topologies, Cz-BD bears a single-pore with tetragonal structure, while Cz-DHBD has a kagome structure bearing two different kinds of pores; one is hexagonal and the other is triangular. These COFs feature high crystallinity, aqueous and organic and solvents stability, large surface area and high porosity with open one-dimensional (1D) microporous channels and densely aligned π-arrays of crystalline sheets. These COFs exhibited synergistic structural effects and achieved ultrahigh-performance of CO2 uptake.
Kuo, Cheng-Han, and 郭承翰. "Synthesis of Novel Two Dimensional Covalent Organic Frameworks and Their Gas Adsorption/Desorption Properties." Thesis, 2018. http://ndltd.ncl.edu.tw/handle/7b77z2.
Повний текст джерела國立中山大學
材料與光電科學學系研究所
106
In this study, we synthesized a series of related monomers and polymers based on covalent organic frameworks (COFs) materials. In the first place, we prepared different five monomer derivatives, including TPA-3NH2, TPT-3NH2, TPA-3CHO, TPP-3CHO, and TPT-3CHO, which were characterized by Fourier transform infrared (FTIR) and nuclear magnetic resonance (NMR) spectroscopies. Secondly, we used the condensation polymerization to synthesize six different COFs via the Schiff base reaction to possess various two-dimensional crosslink structures, named TPA-TPA-COF (COF-1), TPA-TPP-COF (COF-2), TPA-TPT-COF (COF-3), TPT-TPA-COF (COF-4), TPT-TPP-COF (COF-5) and TPT-TPT-COF (COF-6), based on FTIR, TGA, solid state nuclear magnetic resonance (solid state NMR), elemental analysis (EA), powder X-ray diffractometer (PXRD), and BET analyses. The successfully synthesized of these COFs could be confirmed by using FTIR and solid state NMR analyses. All degradation temperatures of COFs are higher than 480 oC based on TGA analyses, indicating that the planar molecular for center group in the COFs make the structure having more stable and better thermal stability. The well-defined crystalline structures were observed of these COFs with hexagonal packed cylinder based on PXRD analyses. Finally, we utilized the surface area and pore size distribution to make further analyses about the relative N2(g) and CO2(g) sorption of different functional groups for center structures. We can observe that the capacity of carbon dioxide (CO2) capture was improved upon increasing the nitrogen content and planarity in COFs.
Costa, Sebastião Melo Refoios da. "Synthesis and characterization of new zeolite membranes and crystalline meta-organic frameworks." Master's thesis, 2018. http://hdl.handle.net/10773/25514.
Повний текст джерелаA utilização de membranas para a separação de misturas gasosas tem ganho grande importância devido às suas vantagens quando comparadas com processos de separação convencionais, como o moderado consumo energético e simplicidade de operação. Apesar de as membranas poliméricas dominarem o mercado, estas são limitadas por temperaturas de operação e seletividades relativamente baixas seletividades. As membranas inorgânicas, por possuírem elevadas estabilidades térmica, química e mecânica, tornam-se particularmente interessantes para processos de separação. Recentemente, as redes metalo-orgânicas cristalinas (MOFs), têm sido alvo de grande investigação, já que a sua estrutura é composta por uma componente orgânica e outra inorgânica, revelando características típicas de ambos os elementos, como flexibilidade e maior controlo na distribuição do tamanho dos poros. Na presente dissertação pretendeu-se sintetizar e, posteriormente, caracterizar, membranas inorgânicas microporosas de zeólitos e, paralelamente, MOFs. No total, quinze membranas foram preparadas. A estrutura e morfologia das membranas mais promissoras foram estudadas pelas técnicas de difração de raios-X (DRX) e de microscopia eletrónica de varrimento (SEM). A caracterização dinâmica foi realizada por ensaios de permeação de gases puros a temperatura fixa e programada, usando diferentes gases (i.e., moléculas com diâmetros cinéticos distintos). Relativamente às membranas zeolíticas, suportadas em tubos de α- alumina, recorreu-se ao método de crescimento secundário, seguido de síntese hidrotérmica. Estudou-se o efeito do tempo de síntese e da presença de rotação durante a mesma. Concluiu-se que com tempos de síntese superiores são preparadas membranas melhores, enquanto a ausência de rotação origina defeitos na estrutura. Comprovou-se o caráter hidrofílico das redes cristalinas através de ensaios de aquecimento-arrefecimento preliminares. A melhor membrana (denominada por MFI93) foi estudada em maior detalhe na gama de temperaturas de 25-110 ºC utilizando He, N2 e O2. Confirmou-se que a permeância e o diâmetro cinético dos gases relacionam-se: hélio, que possui o menor diâmetro, obteve maiores valores de permeância. Pelos testes de permeação a temperatura programada, verificou-se que para baixas temperaturas o mecanismo de escoamento viscoso contribui para o transporte do gás. A sua contribuição diminui progressivamente com o aumento da temperatura, passando a difusão gasosa ativada a ser o mecanismo de transporte dominante. Através da caracterização por DRX e SEM provou-se a preparação de uma camada contínua de ZSM-5 no interior do suporte. Em paralelo, procedeu-se à síntese de redes cristalinas de MOFs. A não deposição de uma camada uniforme foi evidenciada pela caracterização dinâmica das amostras, já que não se verificou qualquer separação. Porém, confirmou-se a formação de pequenos cristais de ZIF-8 na superfície interna do tubo, através de análises de DRX e SEM
Mestrado em Engenharia Química
Troschke, Erik. "Novel Synthetic Pathways for Tailored Covalent Triazine Frameworks with Catalytic and Electrochemical Applications." Doctoral thesis, 2018. https://tud.qucosa.de/id/qucosa%3A32350.
Повний текст джерелаHong, Ying-Hui, and 洪穎慧. "Strategic Design of Two-Dimensional Covalent Organic Frameworks for High-Performance Supercapacitor and Gas Storage Applications." Thesis, 2019. http://ndltd.ncl.edu.tw/handle/e2axeb.
Повний текст джерела國立中山大學
材料與光電科學學系研究所
107
Covalent organic frameworks (COFs) are new class of crystalline porous materials with high surface area and thermal stability. Recently, COFs have gained significant scientific attention due to their potential applications for gas and energy storage. In this study, we report the design and construction of four keto-enamine-based covalent organic frameworks; TFP-TPB, TFP-TPA, TFP-TPP, and TFP-Car COFs through the Schiff-base condensation reaction between 1,3,5-triformylphloroglucinol (TFP) and 1,3,5-tris(4-aminophenyl)benzene (TPB-3NH2), tris(4-aminophenyl)amine (TPA-3NH2), 2,4,6-tris(4-aminophenyl)pyridine (TPP-3NH2), and 9-(4-aminophenyl)-carbazole-3,6-diamine (Car-3NH2) under solvothermal conditions, respectively. The chemical structures of the prepared COFs were confirmed using Fourier transform infrared (FTIR) spectroscopy, solid state 13C CP MAS NMR spectroscopy, and elemental analysis. The resultant COFs exhibited high BET surface area up to ~ 686 m2/g, excellent crystallinity, and thermal stability up to 475 ℃. For applications, our synthesized COFs exhibited high-performance capacities for supercapacitor and gas storage. TFP-TPA, TFP-TPP, and TFP-Car COFs synthesized from nitrogen-content building monomers; TPP-3NH2, TPA-3NH2, and Car-3NH2 exhibited higher CO2 uptake capacities than TFP-TPB COF synthesized from TPB-3NH2. Moreover, the synthesized COFs exhibited excellent electrochemical properties because of their keto-enamine and conjugated structures containing redox-active triphenylamine groups.
Bhattacharya, Saurav. "Syntheses Structural Transformations, Magnetism, Ferroelectricity and Proton Conduction of Metal Organic Frameworks (MOF) Compounds." Thesis, 2015. http://etd.iisc.ernet.in/2005/3546.
Повний текст джерелаPinela, Sara Cristina Ribeiro Grincho. "Evaluation of nanoporous materials for biotoxin capture." Master's thesis, 2016. http://hdl.handle.net/1822/47331.
Повний текст джерелаBiotoxins are metabolites produced by some microalgae species that can reach high concentrations when a massive proliferation of them occur. These kind of compounds are especially dangerous when concentrated in digestive glands of seafood. In general, biotoxins do not affect mollusks, however, the presence of biotoxins turns the mollusks unappropriated for human consumption. In this way, it is very important to improve monitoring methods of biotoxins in water in order to generate an early warning system before seafood becomes toxic. This thesis proposes an improvement in Solid Phase Adsorption Toxin Tracking (SPATT) devices for early warning of the presence of biotoxins in water. To do so, instead of using the chromatographic resins commonly used in SPATT devices, a new nanoporous material, Covalent Organic Frameworks (COFs), was evaluated due to their pore uniform size to be similar to the toxins size. Adsorption/desorption tests of the lipophilic toxin okadaic acid (OA) in COFs were performed, at laboratorial scale, as well as tests of the reuse of the adsorbent material. Adsorption kinetics and adsorption isotherm at 19 ºC were determinated. Finally, diffusion of the toxin into the pores was studied. The results showed that COFs could improve SPATT devices performance since they can capture much more quantity of toxin (about 30 times more) that common chromatographic resins and faster due to the fact that toxin diffusion in pores is almost instantaneous. The determined Freundlich isotherm showed a favorable linear tendency. Finally, COFs can be reused, once desorption can be successfully made using solvents, such as 70 % ethanol and acetonitrile.
As biotoxinas são metabolitos produzidos por algumas espécies de microalgas, que podem atingir altas concentrações aquando uma proliferação maciça das mesmas ocorre. Este tipo de compostos é especialmente perigoso quando concentrados nos sistemas digestivos do marisco. Geralmente, as biotoxinas não afetam o marisco, porém, a sua presença torna-o impróprio para consumo humano. Neste sentido, é importante que se melhorem os métodos de monotorização de biotoxinas na água, de maneira a que se possa estabelecer um sistema de alerta antecipado, antes de o marisco se tornar tóxico. Esta dissertação propõe um aperfeiçoamento de dispositivos de Solid Phase Adsorption Toxin Tracking (SPATT), para uma deteção atempada da presença de biotoxinas na água. Para tal, em vez das resinas geralmente usadas nos dispositivos SPATT, foi avaliado um novo material nanoporoso, Covalent Organic Frameworks (COFs), devido à uniformidade do tamanho de poro deste material ser mais semelhante ao tamanho das toxinas. Testes de adsorção/desorção da toxina lipofílica ácido ocadaíco (OA) foram feitos, à escala laboratorial, assim como testes de reuso do material adsorvente. As cinéticas de adsorção e a isotérmica de adsorção a 19 ºC foram determinadas. Por fim, a difusão da toxina nos poros do COF foi outro ponto estudado. Os resultados dos testes laboratoriais realizados mostram que os COFs podem melhorar o desempenho dos dispositivos de SPATT, uma vez que conseguem capturar muito mais quantidade de toxina (cerca de 30 vezes mais) que as resinas geralmente usadas nos dispositivos de SPATT e conseguem fazê-lo muito mais rapidamente, devido ao facto de a difusão da toxina nos poros ser quase instantânea. A isotérmica de Freundlich determinada mostrou ter uma tendência linear favorável. Por fim, o COF pode também ser reutilizado, uma vez que a dessorção de toxina pode ser feita com sucesso, usando solventes orgânicos, como o etanol a 70 % e o acetonitrilo.