Interfacial Fabrication of Supramolecular Polymer Networks Using Mussel-Inspired Catechol–Iron Complexes

Li, Kaijuan; Wen, Yunhui; Xia, Zhiqin; Zhang, Zhao; Liu, Jiang; Russell, Thomas P.; Shi, Feng; Shi, Shaowei

doi:10.1021/acs.macromol.3c01591

Cited by 3 publications

(1 citation statement)

References 44 publications

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“…Dynamic interfacial tension (IFT) measurements have been employed to understand the kinetics of adsorption processes at the liquid–liquid interface. − Shi and co-workers used pendant drop tensiometry to investigate the kinetics of the supramolecular polymerization at the liquid–liquid interface . We envisaged that the dynamic IFT profile obtained by tensiometry would unravel the mechanistic insights into interfacial cage-to-COF transformation.…”

Section: Introductionmentioning

confidence: 99%

Unraveling Early-Stage Dynamics of Cage-to-Covalent Organic Framework Transformation at Liquid–Liquid Interface

Shreeraj,

Tiwari,

Dugyala

et al. 2024

Langmuir

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Postsynthetic linker exchange (PLE) has emerged as an emerging synthetic strategy for constructing high-quality covalent organic frameworks (COFs) from preassembled entities such as linear polymers, amorphous networks, COFs, and porous organic cages by using the principles of dynamic covalent chemistry. The PLE strategy has recently been extended at the liquid−liquid interface to fabricate highly crystalline two-dimensional (2D)-COF membranes at a faster time scale (24 h). Examining the early stages of the interfacial PLE dynamics becomes essential to understanding the expedited COF growth process. In this regard, pendant drop tensiometry has been employed to probe the initial reaction dynamics of the imine cageto-COF transformation through dynamic interfacial tension (IFT) measurements. The contrasting trends in IFT profiles between PLE-mediated (from cage) and direct COF synthesis (from parent monomers) are in qualitative agreement with the kinetics of bulkscale interfacial polymerizations. Further, the distinct early-stage interfacial behaviors between the diverse synthetic routes have been experimentally demonstrated using tensiometry, optical microscopy, electron microscopy, and powder X-ray diffraction (PXRD) analysis. The pivotal role of in situ generated imine intermediates (ImIs) and the phenomenon of spontaneous emulsification toward accelerated interfacial COF growth process was delineated. The current study on deploying the pendant drop tensiometric technique to examine early-stage interfacial polymerization dynamics opens up a gripping avenue for mechanistic exploration in PLE-based COF synthesis. The generality of the developed methodology to study the initial COF growth kinetics was extended to a new interfacial PLE-mediated cage-to-COF transformation.

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Section: Introductionmentioning

confidence: 99%

Unraveling Early-Stage Dynamics of Cage-to-Covalent Organic Framework Transformation at Liquid–Liquid Interface

Shreeraj,

Tiwari,

Dugyala

et al. 2024

Langmuir

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Reconfigurable liquids enabled by dynamic covalent chemistry

Li,

Luo,

Wen

et al. 2024

Aggregate

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Nanoparticle surfactants (NPSs) that form via the reversible non‐covalent interactions between nanoparticles (NPs) and polymer ligands at the oil‐water interface have received great attention in constructing structured liquids with unique stimuli‐responsiveness. Introducing dynamic covalent interactions to generate NPSs is expected to achieve a balance between high mechanical strength and dynamic responsiveness of the interfacial assemblies. Here, we present the formation, assembly, and jamming of a new type of NPS by the co‐assembly between polydopamine NPs (PDA NPs) and poly(styrene‐co‐methacrylamidophenylboronic acid) at the oil‐water interface. Dynamic covalent boronate ester bonds form in situ at the interface and show multiple responsiveness when applying stimuli such as pH, H2O2, and temperature, allowing the controlled assembly/jamming of NPSs and reconfiguration of liquid constructs. Due to the photothermal property of PDA NPs, the temperature responsiveness of boronate ester bonds can also be triggered by irradiating the biphasic system with near‐infrared (NIR) light. Moreover, when bringing two droplets encapsulated with NPSs into contact and irradiating the contact area by NIR, thermal welding of droplets can be realized, offering a straightforward to construct droplet networks and modular liquid devices.

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Solvent Vapor/Gas-Induced Guest Transport and Exchange of a Nonporous Organic Crystal to Construct Smart Host–Guest Energetic Materials

Song,

Zhang,

Jin

et al. 2024

ACS Appl. Mater. Interfaces

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Supramolecular materials with advanced properties constructed by intermolecular interactions have attracted extensive attention in many fields, such as sensing, catalysis, and biomedicine. However, in the field of energetic materials, limited by the tight-packed crystal structure of explosives and the strong intermolecular interaction forces, most supramolecular explosives can only be obtained in organic solution or under extreme external loading (high temperature/ high pressure). Given the practical issues such as safety risks, operational difficulties, serious environmental pollution, and large-scale production of the existing technology, a new method of constructing host−guest explosives by solvent vapor/gas induction is proposed. This gas−solid reaction method takes advantage of the metastable properties from the explosives solvate (HNIW/ACN), and cleverly opens a fast channel for gas molecules to enter the explosives cell cavities, which results in the highly efficient preparation of the host−guest explosives (HNIW/CO 2 and HNIW/N 2 O). The embedding of functional gas molecules greatly improves the structural stability and comprehensive performance of the explosive skeleton, and the detonation velocity of HNIW/N 2 O even reaches 9802 m•s −1 , which is higher than that of ε-HNIW (9455 m•s −1 ). In addition, compared with ε-HNIW, HNIW/CO 2 and HNIW/N 2 O exhibit high energy but low sensitivity, enhanced thermal stability, and combustion properties, which present a potential prospect in the field of energetic materials. The new method effectively overcomes the high-energy barrier of nonporous organic explosives, offering the advantages of simplicity, safety, efficiency, and environmental friendliness. This study provides a valuable pathway for constructing advanced supramolecular energetic materials, which contributes to the enrichment of supramolecular engineering systems.

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Interfacial Fabrication of Supramolecular Polymer Networks Using Mussel-Inspired Catechol–Iron Complexes

Cited by 3 publications

References 44 publications

Unraveling Early-Stage Dynamics of Cage-to-Covalent Organic Framework Transformation at Liquid–Liquid Interface

Unraveling Early-Stage Dynamics of Cage-to-Covalent Organic Framework Transformation at Liquid–Liquid Interface

Reconfigurable liquids enabled by dynamic covalent chemistry

Solvent Vapor/Gas-Induced Guest Transport and Exchange of a Nonporous Organic Crystal to Construct Smart Host–Guest Energetic Materials

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