Overcoming Surfactant-Induced Morphology Instability of Noncrosslinked Diblock Copolymer Nano-Objects Obtained by RAFT Emulsion Polymerization

Truong, Nghia P.; Zhang, Cheng; Nguyen, Tuan A.H.; Anastasaki, Athina; Schulze, Morgan W.; Quinn, John F.; Whittaker, Andrew K.; Hawker, Craig J.; Whittaker, Michael R.; Davis, Thomas P.

doi:10.1021/acsmacrolett.7b00978

Cited by 37 publications

(38 citation statements)

References 46 publications

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“…For instance, for the triblock copolymer (PDMAc 49 ‐ b ‐PDAAm 92 ) 2 , short worms were observed by TEM when the sample was prepared at 5 °C (Figure S10, Supporting Information), whereas multilamellar vesicles were imaged for the sample prepared at 60 °C (Figure e). Such TIMT has already been reported for PDMAc‐ b ‐PDAAm AB diblock copolymers, but also for other types of diblock polymers prepared by aqueous dispersion polymerization in a PISA process . It was explained by the lower degree of hydration of the core‐forming polymer block at higher temperature, which decreases the effective volume of the stabilizer block and hence increases the packing parameter p .…”

Section: Resultssupporting

confidence: 62%

Beyond Simple AB Diblock Copolymers: Application of Bifunctional and Trifunctional RAFT Agents to PISA in Water

Mellot

Beaunier

Guigner

et al. 2018

Macromol. Rapid Commun.

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The influence of the macromolecular reversible addition-fragmentation chain transfer (macro-RAFT) agent architecture on the morphology of the self-assemblies obtained by aqueous RAFT dispersion polymerization in polymerization-induced self-assembly (PISA) is studied by comparing amphiphilic AB diblock, (AB) triblock, and triarm star-shaped (AB) copolymers, constituted of N,N-dimethylacrylamide (DMAc = A) and diacetone acrylamide (DAAm = B). Symmetrical triarm (AB) copolymers could be synthesized for the first time in a PISA process. Spheres and higher order morphologies, such as worms or vesicles, could be obtained for all types of architectures and the parameters that determine their formation have been studied. In particular, we found that the total DP of the PDMAc and the PDAAm segments, i.e., the same overall molar mass, at the same M (PDMAc)/M (PDAAm) ratio, rather than the individual length of the arms determined the morphologies for the linear (AB) and star shaped (AB) copolymers obtained by using the bi- and trifunctional macro-RAFT agents.

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Section: Resultssupporting

confidence: 62%

Beyond Simple AB Diblock Copolymers: Application of Bifunctional and Trifunctional RAFT Agents to PISA in Water

Mellot

Beaunier

Guigner

et al. 2018

Macromol. Rapid Commun.

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“…In this investigation, the surfactant tolerance was caused by the limited binding of the SDS surfactant to the main-chain of the P(DEGMA-co-HPMA) macro-CTA (constituting the nanoparticle shell). This investigation may stimulate novel application of non-crosslinked nanostructures formed by means of RAFT emulsion polymerization techniques for the preparation surfactant-tolerant nanomaterials [98].…”

Section: Linearmentioning

confidence: 89%

“…In a recent study, the enhancement of the colloidal stability (on the various morphologies of non-crosslinked nano-assemblies) in concentrated solutions of sodium dodecyl sulfate (SDS) surfactant was obtained by means of the RAFT emulsion polymerization, by using poly(di(ethylene glycol) ethyl ether methacrylate-co-N-(2-hydroxypropyl) methacrylamide) P(DEGMA29-co-HPMA6) as a macro-CTA [98]. In this investigation, the surfactant tolerance was caused by the limited binding of the SDS surfactant to the main-chain of the P(DEGMA-co-HPMA) macro-CTA (constituting the nanoparticle shell).…”

Section: Linearmentioning

confidence: 99%

Self-Assembly of Organic Nanomaterials and Biomaterials: The Bottom-Up Approach for Functional Nanostructures Formation and Advanced Applications

et al. 2020

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In this paper, we survey recent advances in the self-assembly processes of novel functional platforms for nanomaterials and biomaterials applications. We provide an organized overview, by analyzing the main factors that influence the formation of organic nanostructured systems, while putting into evidence the main challenges, limitations and emerging approaches in the various fields of nanotechology and biotechnology. We outline how the building blocks properties, the mutual and cooperative interactions, as well as the initial spatial configuration (and environment conditions) play a fundamental role in the construction of efficient nanostructured materials with desired functional properties. The insertion of functional endgroups (such as polymers, peptides or DNA) within the nanostructured units has enormously increased the complexity of morphologies and functions that can be designed in the fabrication of bio-inspired materials capable of mimicking biological activity. However, unwanted or uncontrollable effects originating from unexpected thermodynamic perturbations or complex cooperative interactions interfere at the molecular level with the designed assembly process. Correction and harmonization of unwanted processes is one of the major challenges of the next decades and requires a deeper knowledge and understanding of the key factors that drive the formation of nanomaterials. Self-assembly of nanomaterials still remains a central topic of current research located at the interface between material science and engineering, biotechnology and nanomedicine, and it will continue to stimulate the renewed interest of biologist, physicists and materials engineers by combining the principles of molecular self-assembly with the concept of supramolecular chemistry.

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“…We have recently developed several reversible addition‐fragmentation chain transfer (RAFT) emulsion polymerization techniques that can be used to synthesize nanoparticles with tunable size, shape, and surface chemistry via either polymerization‐induced self‐assembly (PISA) or temperature‐induced morphological transformation . Emulsion polymerization is an environmentally and industrially friendly technique that can be used to reproducibly yield large‐scale, concentrated nanoparticle suspensions in water .…”

Section: Introductionmentioning

confidence: 99%

Elucidating the Influences of Size, Surface Chemistry, and Dynamic Flow on Cellular Association of Nanoparticles Made by Polymerization‐Induced Self‐Assembly

Khor

Pilkington

et al. 2018

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The size and surface chemistry of nanoparticles dictate their interactions with biological systems. However, it remains unclear how these key physicochemical properties affect the cellular association of nanoparticles under dynamic flow conditions encountered in human vascular networks. Here, the facile synthesis of novel fluorescent nanoparticles with tunable sizes and surface chemistries and their association with primary human umbilical vein endothelial cells (HUVECs) is reported. First, a one-pot polymerization-induced self-assembly (PISA) methodology is developed to covalently incorporate a commercially available fluorescent dye into the nanoparticle core and tune nanoparticle size and surface chemistry. To characterize cellular association under flow, HUVECs are cultured onto the surface of a synthetic microvascular network embedded in a microfluidic device (SynVivo, INC). Interestingly, increasing the size of carboxylic acid-functionalized nanoparticles leads to higher cellular association under static conditions but lower cellular association under flow conditions, whereas increasing the size of tertiary amine-decorated nanoparticles results in a higher level of cellular association, under both static and flow conditions. These findings provide new insights into the interactions between polymeric nanomaterials and endothelial cells. Altogether, this work establishes innovative methods for the facile synthesis and biological characterization of polymeric nanomaterials for various potential applications.

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Overcoming Surfactant-Induced Morphology Instability of Noncrosslinked Diblock Copolymer Nano-Objects Obtained by RAFT Emulsion Polymerization

Cited by 37 publications

References 46 publications

Beyond Simple AB Diblock Copolymers: Application of Bifunctional and Trifunctional RAFT Agents to PISA in Water

Beyond Simple AB Diblock Copolymers: Application of Bifunctional and Trifunctional RAFT Agents to PISA in Water

Self-Assembly of Organic Nanomaterials and Biomaterials: The Bottom-Up Approach for Functional Nanostructures Formation and Advanced Applications

Elucidating the Influences of Size, Surface Chemistry, and Dynamic Flow on Cellular Association of Nanoparticles Made by Polymerization‐Induced Self‐Assembly

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