Uniform segmented platelet micelles with compositionally distinct and selectively degradable cores

Tong, Zaizai; Xie, Yujie; Arno, Maria C.; Zhang, Yifan; Manners, Ian; O’Reilly, Rachel K.; Dove, Andrew P.

doi:10.1038/s41557-023-01177-2

Cited by 40 publications

(49 citation statements)

References 42 publications

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“…Initially batch controls were established; living CDSA was conducted in 1 mL batch scale according to our previous report (Figures S1–S8). , As expected, the incremental addition of the unimer corresponded to a proportional increase in the size of the platelets (Figure S8 and Table S7). After that, epitaxial growth of seeds was scaled up to 10 mL at a 1:10 seed/unimer ratio to investigate the reproducibility and scalability of batch living CDSA.…”

supporting

confidence: 83%

Enhancing the Scalability of Crystallization-Driven Self-Assembly Using Flow Reactors

Xiao,

Parkinson,

Xia

et al. 2023

ACS Macro Lett.

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Anisotropic materials have garnered significant attention due to their potential applications in cargo delivery, surface modification, and composite reinforcement. Crystallization-driven self-assembly (CDSA) is a practical way to access anisotropic structures, such as 2D platelets. Living CDSA, where platelets are formed by using seed particles, allows the platelet size to be well controlled. Nonetheless, the current method of platelet preparation is restricted to low concentrations and small scales, resulting in inefficient production, which hampers its potential for commercial applications. To address this limitation, continuous flow reactors were employed to improve the production efficiency. Flow platforms ensure consistent product quality by maintaining the same parameters throughout the process, circumventing batch-to-batch variations and discrepancies observed during scale-up. In this study, we present the first demonstration of living CDSA performed within flow reactors. A continuous flow system was established, and the epitaxial growth of platelets was initially conducted to study the influence of flow parameters such as temperature, residence time, and flow rate on the morphology of platelets. Comparison of different epitaxial growth manners of seeds and platelets was made when using seeds to perform living CDSA. Size-controllable platelets from seeds can be obtained from a series flow system by easily tuning flow rates. Additionally, uniform platelets were continuously collected, exhibiting improved size and dispersity compared to those obtained in batch reactions.

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confidence: 83%

Enhancing the Scalability of Crystallization-Driven Self-Assembly Using Flow Reactors

Xiao,

Parkinson,

Xia

et al. 2023

ACS Macro Lett.

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“…Nevertheless, as revealed by our previously reported result, the seeded growth of a PCL/ PCL-b-PDMA (PCL = poly(ε-caprolactone), PDMA = poly(dimethylacrylamide)) blend unimer from 2D PHL (PHL = poly(ζ-heptalactone)) platelets was hampered at ambient temperature (25 °C), although the lattice mismatch of PCL and PHL only corresponds to a difference of ∼1.6% (Figure S1 and Table S1). 58 However, heteroepitaxial growth happened in a vice versa process at ambient temperature, i.e., the successful epitaxial growth of the PHL/PHL-b-PDMA blend unimer from 1D PCL seeds or 2D PCL platelets. 58 This one-way epitaxial growth result at room temperature confirms that lattice matching of polymers is required while it is not sufficient for the successful epitaxial growth.…”

Section: ■ Resultsmentioning

confidence: 99%

“…58 However, heteroepitaxial growth happened in a vice versa process at ambient temperature, i.e., the successful epitaxial growth of the PHL/PHL-b-PDMA blend unimer from 1D PCL seeds or 2D PCL platelets. 58 This one-way epitaxial growth result at room temperature confirms that lattice matching of polymers is required while it is not sufficient for the successful epitaxial growth. Therefore, PCL and PHL were selected as typical crystallizable polymers to explore the effect of crystallization temperatures on seeded epitaxial growth.…”

Section: ■ Resultsmentioning

confidence: 99%

“…The precise control of 2D platelet micelles with core–shell structures using the living CDSA approach has been extensively studied, but the fabrication of 2D nanoparticles is limited to homoepitaxial growth in which the core chemistry is compositionally identical. , Recent attention has been given to the expansion of living CDSA using seeded heteroepitaxial growth, and several systems of successful heteroepitaxial growth between different core-forming BCPs have been developed, allowing the formation of precisely controlled 2D platelet micelles with different internal core chemistries. − Our recent work demonstrates that seeded heteroepitaxial growth is successfully extended to a range of polylactone-containing BCPs, and a series of segmented platelet micelles with distinct inner core chemistries and degradable properties are established …”

Section: Introductionmentioning

confidence: 99%

“…54−57 Our recent work demonstrates that seeded heteroepitaxial growth is successfully extended to a range of polylactonecontaining BCPs, and a series of segmented platelet micelles with distinct inner core chemistries and degradable properties are established. 58 Despite the development of heteroepitaxial CDSA, the deep understanding of heteroepitaxial growth has yet to be extensively explored. The guidance of seeded heteroepitaxial growth is limited to the crystallographic matching rule, where a lattice spacing mismatch upper limit ca.…”

Section: ■ Introductionmentioning

confidence: 99%

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Seeded Epitaxial Growth of Crystallizable Polymers Governed by Crystallization Temperatures

et al. 2023

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Seeded growth is generally regarded as an ambient-temperature, living crystallization-driven self-assembly (CDSA) approach of block copolymers (BCPs) with crystallizable cores, which is a powerful method in preparing one-dimensional (1D) or twodimensional (2D) polymer nanomaterials with precise control over size and compositions. Generally, crystallographic matching is considered as a fundamental principle that determines the happening of epitaxial growth. However, crystallization temperature also plays a vital role in governing the seeded growth behavior, which is usually ignored in previous studies. Herein, the effect of crystallization temperatures on seeded epitaxial growth of different crystallizable polymer blends involving a homopolymer and a corresponding BCP is extensively explored. It has been shown that crystallographic matching is essentially required but not sufficient for successful epitaxial growth. Crystallization-temperature-dependent seeded growth demonstrates that the critical size of nuclei generated from a crystalline substrate dominates the occurrence of epitaxial growth. A smaller thickness of deposited crystals than that of the crystalline substrate is required for the happening of epitaxial growth. This important finding provides a theoretical basis for the design of complex polymer nanoparticles with distinct core compositions from an alternative view of crystallization temperatures using the CDSA approach.

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Tailoring Photoweldable Shape Memory Polyurethane with Intrinsic Photothermal / Fluorescence Via Engineering Metal‐Phenolic Systems

Ping,

Xie,

Gong

et al. 2024

Adv Funct Materials

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Multifunctional shape memory polymers are significant for next‐generation intelligent systems as smart materials. However, their practical applications are limited by toughness, manufacturability, and functional integration strategies. Besides, while 4D printing is used to construct deformable devices, the limited accessible shapes and difficulty of integrating multiple materials hindered the development of multifunctional devices. Herein, metal‐phenolic coordination is used as crosslinks to tailor tough shape memory polyurethanes with intrinsic photothermal effect and/or tunable fluorescence. The reversible dissociation of metal‐phenolic complexes upon loading provides an efficient energy dissipation for the polymer network. The photothermal/fluorescent properties of target polyurethane can be effortlessly programmed by changing the coordinated metals and functional ligands. The obtained fluorescent polyurethane displays tunable fluorescence through the reversible dissociation‐association of dynamic bonds upon thermal stimulus. Moreover, relying on light‐triggered hybrid exchange reactions among various metal‐phenolic coordination bonds, heterogeneous interfaces can be merged to manufacture exquisite 3D shape‐shifting devices and integrate more advanced functions. As demonstrations, intrinsic photothermal‐responsive shape memory stent, and 3D fluorescent encryption device are produced based on photo‐welding instead of 4D printing. This study not only provides a convenient supramolecular strategy for constructing multifunctional smart materials but also demonstrates a feasible method for making personalized integrated architectures.

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Uniform segmented platelet micelles with compositionally distinct and selectively degradable cores

Cited by 40 publications

References 42 publications

Enhancing the Scalability of Crystallization-Driven Self-Assembly Using Flow Reactors

Enhancing the Scalability of Crystallization-Driven Self-Assembly Using Flow Reactors

Seeded Epitaxial Growth of Crystallizable Polymers Governed by Crystallization Temperatures

Tailoring Photoweldable Shape Memory Polyurethane with Intrinsic Photothermal / Fluorescence Via Engineering Metal‐Phenolic Systems

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