Synthesis, Self-Assembly and Characterization of Tandem Triblock BPOSS-PDI-X Shape Amphiphiles

Shao, Yu; Chen, Jia; Ren, Xiang‐Kui; Zhang, Xinlin; Yin, Guang‐Zhong; Li, Xiaopeng; Wang, Jing; Wesdemiotis, Chrys; Zhang, Wenbing; Shen, Yang; Sun, Bin; Zhu, Meifang

doi:10.3390/molecules24112114

Cited by 4 publications

(4 citation statements)

References 68 publications

(78 reference statements)

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“…Zhu and co-workers hypothesised that by increasing molecular complexity of PDI, for example by incorporating isobutyl-functionalised polyhedral oligomeric silsesquioxanes (BPOSS) and fullerene (C 60 ), the synthesised shape amphiphile could display varying properties depending on self-assembled morphology, binding mode and quantum efficiency. 57 Travelling wave ion mobility mass spectrometry (TWIM-MS) was utilised in combination with collision activated dissociation (CAD) within the quadrupole ToF MS. Within the CAD experiment, drift gas collides with the ionic species causing any self-associated species to dissociate; the energy required to overcome these supramolecular interactions is then determined.…”

Section: Mass Spectrometry (Ms)mentioning

confidence: 99%

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Tools to enable the study and translation of supramolecular amphiphiles

Allam,

Balderston,

Chahal

et al. 2023

Chem. Soc. Rev.

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Section: Mass Spectrometry (Ms)mentioning

confidence: 99%

“…4. 57 Analysis of these dimers with TWIM-MS can be used to indicate how changes in molecular binding mode may alter quantum efficiency and subsequent photo-and/or electroproperties of aggregation induced emission (AIE) events. 58 While HRMS provides data relating to the non-covalent binding mode in only the gas-phase.…”

Section: Mass Spectrometry (Ms)mentioning

confidence: 99%

Tools to enable the study and translation of supramolecular amphiphiles

Allam,

Balderston,

Chahal

et al. 2023

Chem. Soc. Rev.

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“…Branched silsesquioxane units of [RSiO 1.5 ] n composition are among the most popular blocks for creating numerous hybrid nanomaterials and composites. − Two general approaches in this chemistry are actively developing nowadays(i) the use of fully condensed silsesquioxanes generally based on octameric [RSiO 1,5 ] 8 cubane-like units and (ii) the application of partly condensed derivatives. Among many fascinating and functional structures, available via the first approach, we can mention polyhedral oligomeric silsesquioxanes (POSS) bearing chromophore groups, , materials for sorption of heavy-metal ions/dyes/organic solvents from water, − additives for polymers, components of nanoscale building blocks, , shape amphiphiles, organocatalysts, building blocks for the construction of magnetic materials, and luminescent devices or light-harvesting systems. , …”

Section: Introductionmentioning

confidence: 99%

“…2−5 Two general approaches in this chemistry are actively developing nowadays�(i) the use of fully condensed silsesquioxanes generally based on octameric [RSiO 1,5 ] 8 cubane-like units and (ii) the application of partly condensed derivatives. Among many fascinating and functional structures, available via the first approach, we can mention polyhedral oligomeric silsesquioxanes (POSS) bearing chromophore groups, 6,7 materials for sorption of heavy-metal ions/ dyes/organic solvents from water, 8−11 additives for polymers, 12 components of nanoscale building blocks, 13,14 shape amphiphiles, 15 organocatalysts, 16 building blocks for the construction of magnetic materials, 17 and luminescent devices or lightharvesting systems. 18,19 The investigation of partly condensed POSS is also appealing, 20 leading to the design of new monomers for copolymerization reactions, 21 H-bond donor catalysts, 22 OLED's emission layers, 23 three-dimensional emulsifiers, 24 different films (e.g., transparent, 25 scratch resistant, 26 selfhealing, 27 or Langmuir−Blodgett/Langmuir−Schaefer films 28 ), and spin-on-glass networks with ultralow dielectric constants.…”

Section: ■ Introductionmentioning

confidence: 99%

Acetone Factor in the Design of Cu₄-, Cu₆-, and Cu₉-Based Cage Coppersilsesquioxanes: Synthesis, Structural Features, and Catalytic Functionalization of Alkanes

et al. 2022

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The present study describes a new feature in the self-assembly of cagelike copperphenylsilsesquioxanes: the strong influence of acetone solvates on cage structure formation. By this simple approach, a series of novel tetra-, hexa-, or nonacoppersilsesquioxanes were isolated and characterized. In addition, several new complexes of Cu4 or Cu6 nuclearity bearing additional nitrogen-based ligands (ethylenediamine, 2,2′-bipyridine, phenanthroline, bathophenanthroline, or neocuproine) were produced. Single-crystal X-ray diffraction studies established molecular architectures of all of the synthesized products. Several coppersilsesquioxanes represent a novel feature of cagelike metallasilsesquioxane (CLMS) in terms of molecular topology. A Cu4–silsesquioxane complex with ethylenediamine (En) ligands was isolated via the unprecedented self-assembly of a partly condensed framework of silsesquioxane ligands, followed by the formation of a sandwich-like cage. Two prismatic Cu6 complexes represent the different conformersregular and elliptical hexagonal prisms, “cylinders”, determined by the different orientations of the coordinated acetone ligands (“shape-switch effect”). A heterometallic Cu4Na4-sandwich-like derivative represents the first example of a metallasilsesquioxane complex with diacetone alcohol ligands formed in situ due to acetone condensation reaction. As a selected example, the compound [(Ph6Si6O11)2Cu4En2]·(acetone)2 was explored in homogeneous oxidation catalysis. It catalyzes the oxidation of alkanes to alkyl hydroperoxides with hydrogen peroxide and the oxidation of alcohols to ketones with tert-butyl hydroperoxide. Radical species take part in the oxidation of alkanes. Besides, [(Ph6Si6O11)2Cu4En2]·(acetone)2 catalyzes the mild oxidative functionalization of gaseous alkanes (ethane, propane, n-butane, and i-butane). Two different model reactions were investigated: (1) the oxidation of gaseous alkanes with hydrogen peroxide to give a mixture of oxygenates (alcohols, ketones, or aldehydes) and (2) the carboxylation of C n gaseous alkanes with carbon monoxide, water, and potassium peroxodisulfate to give C n+1 carboxylic acids (main products), along with the corresponding C n oxygenates. For these reactions, the effects of acid promoter, reaction time, and substrate scope were explored. As expected for free-radical-type reactions, the alkane reactivity follows the trend C2H6 < C3H8 < n-C4H10 < i-C4H10. The highest total product yields were observed in the carboxylation of i-butane (up to 61% based on i-C4H10). The product yields and catalyst turnover numbers (TONs) are remarkable, given an inertness of gaseous alkanes and very mild reaction conditions applied (low pressures, 50–60 °C temperatures).

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Mass spectrometry of polymers: A tutorial review

Wesdemiotis

Williams-Pavlantos

Keating

et al. 2023

Mass Spectrometry Reviews

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Ever since the inception of synthetic polymeric materials in the late 19th century, the number of studies on polymers as well as the complexity of their structures have only increased. The development and commercialization of new polymers with properties fine‐tuned for specific technological, environmental, consumer, or biomedical applications requires powerful analytical techniques that permit the in‐depth characterization of these materials. One such method with the ability to provide chemical composition and structure information with high sensitivity, selectivity, specificity, and speed is mass spectrometry (MS). This tutorial review presents and exemplifies the various MS techniques available for the elucidation of specific structural features in a synthetic polymer, including compositional complexity, primary structure, architecture, topology, and surface properties. Key to every MS analysis is sample conversion to gas‐phase ions. This review describes the fundamentals of the most suitable ionization methods for synthetic materials and provides relevant sample preparation protocols. Most importantly, structural characterizations via one‐step as well as hyphenated or multidimensional approaches are introduced and demonstrated with specific applications, including surface sensitive and imaging techniques. The aim of this tutorial review is to illustrate the capabilities of MS for the characterization of large, complex polymers and emphasize its potential as a powerful compositional and structural elucidation tool in polymer chemistry.

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Synthesis, Self-Assembly and Characterization of Tandem Triblock BPOSS-PDI-X Shape Amphiphiles

Cited by 4 publications

References 68 publications

Tools to enable the study and translation of supramolecular amphiphiles

Tools to enable the study and translation of supramolecular amphiphiles

Acetone Factor in the Design of Cu₄-, Cu₆-, and Cu₉-Based Cage Coppersilsesquioxanes: Synthesis, Structural Features, and Catalytic Functionalization of Alkanes

Mass spectrometry of polymers: A tutorial review

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Synthesis, Self-Assembly and Characterization of Tandem Triblock BPOSS-PDI-X Shape Amphiphiles

Cited by 4 publications

References 68 publications

Tools to enable the study and translation of supramolecular amphiphiles

Tools to enable the study and translation of supramolecular amphiphiles

Acetone Factor in the Design of Cu4-, Cu6-, and Cu9-Based Cage Coppersilsesquioxanes: Synthesis, Structural Features, and Catalytic Functionalization of Alkanes

Mass spectrometry of polymers: A tutorial review

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Acetone Factor in the Design of Cu₄-, Cu₆-, and Cu₉-Based Cage Coppersilsesquioxanes: Synthesis, Structural Features, and Catalytic Functionalization of Alkanes