Nanostructured Multiphase Condensation of Complex Coacervates in Polymerization-Induced Electrostatic Self-Assembly

Li, Chao; Wang, Ye; Wang, Xiyu; Gao, Zhanwei; Ma, Lei; Lu, Xinhua; Cai, Yuanli

doi:10.1021/acsmacrolett.1c00308

Cited by 12 publications

(10 citation statements)

References 38 publications

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“…The concept of polymerization-induced electrostatic self-assembly (PIESA) was also reported (Figure ). This process can give easy access to low dimensional PICs nano-objects (e.g., nanospheres, nanowires, large-area nanofilms, porous nanofilms, vesicles and multicompartmental vesicles) that could be of high interest for biomedical applications given its versatility in terms of hydrophilic polymers − and preparation methods. − …”

Section: Polymerization-induced Self-assembly (Pisa)mentioning

confidence: 99%

(Bio)degradable and Biocompatible Nano-Objects from Polymerization-Induced and Crystallization-Driven Self-Assembly

Zhu

Nicolas

2022

Biomacromolecules

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Polymerization-induced self-assembly (PISA) and crystallization-driven self-assembly (CDSA) techniques have emerged as powerful approaches to produce a broad range of advanced synthetic nano-objects with high potential in biomedical applications. PISA produces nano-objects of different morphologies (e.g., spheres, vesicles and worms), with high solids content (∼10−50 wt %) and without additional surfactant. CDSA can finely control the self-assembly of block copolymers and readily forms nonspherical crystalline nano-objects and more complex, hierarchical assemblies, with spatial and dimensional control over particle length or surface area, which is typically difficult to achieve by PISA. Considering the importance of these two assembly techniques in the current scientific landscape of block copolymer self-assembly and the craze for their use in the biomedical field, this review will focus on the advances in PISA and CDSA to produce nano-objects suitable for biomedical applications in terms of (bio)degradability and biocompatibility. This review will therefore discuss these two aspects in order to guide the future design of block copolymer nanoparticles for future translation toward clinical applications.

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Section: Polymerization-induced Self-assembly (Pisa)mentioning

confidence: 99%

(Bio)degradable and Biocompatible Nano-Objects from Polymerization-Induced and Crystallization-Driven Self-Assembly

Zhu

Nicolas

2022

Biomacromolecules

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“…For the scalable synthesis of nanostructured PICs, we − developed polymerization-induced electrostatic self-assembly (PIESA) using our photo-PISA , via our photo-RAFT , aqueous dispersion polymerization of ionic monomer using nonionic macrochain transfer agent (macro-CTA) in the presence of opposite-charge polyion (PIC template). Chain extension led to electrostatic assembly into PICs with sphere, worm, lamella, vesicle, and other higher-ordered or compartmentalized morphologies. − More recently, we proposed a new PIESA chemistry that was driven by guanidinium/sulfonate salt bridges . This PIESA formulation comprises N -(2-guanidinoethyl)methacrylamide (GEMA) monomer, poly(2-acrylamido-2-methylpropanesulfonic acid) (PAMPS), poly( N -(2-hydroxypropyl)methacrylamide) (PHPMA) macro-CTA, and sodium phenyl-2,4,6-trimethylbenzoylphosphinate (SPTP) photoinitiator in water, under visible light at 25 °C.…”

Section: Introductionmentioning

confidence: 99%

Polymerization-Induced Electrostatic Self-Assembly Governed by Guanidinium Ionic Hydrogen Bonds

et al. 2022

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Polymerization-induced electrostatic self-assembly (PIESA) represents a powerful method for the scalable synthesis of polyion complex (PIC) nanoparticles with various morphologies. Previous PIESA was driven by Coulombic interactions. Yet, biomimetic multivalent interactions, e.g., ionic hydrogen bonds omnipresent in proteins and potentially enabling access to new materials, remain unexplored. Herein, we update PIESA using arginine-like full-spectrum guanidinium ionic hydrogen bonds. Kinetic studies unravel that, at guanidinium-starving n + /n − (0.84), guanidinium interactions evolve from opposite-charge (6−73% conversion) into like-charge ionic hydrogen bonds (84 to >99% conversion), leading to ultrasmall clusters (2−5 nm, at 6−84% conversion) and size-tunable "large compound micelles" (14−25 nm, at 90 to >99% conversion). Longer guanidinium-block length results in the transformation of charge-neutral worms to positive-charge micron-scale large-area monolayer lamellae to multilayer platelets to tubular networks to vesicular aggregates, suggesting that the like-charge ionic hydrogen bonds are strong enough to overwhelm Coulombic repulsive interactions, and thus to revolutionize our PIESA chemistry for the precision synthesis of nextgeneration nanostructured biomimetic functional materials.

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“…Understanding the critical components and phenomena which dictate BIC formation has enabled the development of technologies which control association, morphology, and architecture of BICs. BICs have been developed which release cargo or dissociate based on polymer architecture [ 82 ], temperature [ 62 , 71 ], pH [ 83 ], sugar [ 83 ], type of ion [ 84 , 85 ], and hydration [ 86 ]. Additionally, the introduction of metals have yielded magnetic nanoparticles which are effective drug carriers [ 87 ].…”

Section: Introductionmentioning

confidence: 99%

Interpolyelectrolyte Complexes as an Emerging Technology for Pharmaceutical Delivery of Polypeptides

Fay

Kabanov

2022

rev. and adv. in chem.

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Polyelectrolyte complexes and the derivatives thereof comprise some of the most promising vehicles for the encapsulation and delivery of macromolecular therapeutics. In particular, protein therapeutics, which present a host of special considerations, can often be effectively packaged and delivered using interpolyelectrolyte complexes. While the technologies are still in the developmental phase, there are numerous examples of complexes where control is exerted over spacial and temporal delivery of a model protein cargo or candidate protein therapeutic agent. Here we provide a historical and practical background to promote a deeper understanding of interpolyelectrolyte complexes and the derivative technologies. Additionally, we review the physical principles underlying the association of polyelectrolyte complexes and the application of those principles to novel strategies and technologies driving interpolyelectrolyte complexation. Then, the application of polyelectrolyte complex technology to protein therapeutics is discussed in detail including discussions of several types of protein cargo with a special emphasis on Brain-Derived Neurotrophic Factor. Finally, we focus on the use of stealth polymers in block ionomer complexes, specifically PEG; its benefits, flaws, and possible alternatives. Comprehensive understanding of the field may promote the continued development of derivative technologies for the delivery of particularly intransigent protein therapeutics, much as has been accomplished for small molecule drugs. We also aim to link current advances to the historical developments which inaugurated the field. With consideration to the field, industrial and academic researchers can utilize the discussed technologies and continue to elucidate novel modalities for a myriad of therapeutic and commercial applications .

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Nanostructured Multiphase Condensation of Complex Coacervates in Polymerization-Induced Electrostatic Self-Assembly

Cited by 12 publications

References 38 publications

(Bio)degradable and Biocompatible Nano-Objects from Polymerization-Induced and Crystallization-Driven Self-Assembly

(Bio)degradable and Biocompatible Nano-Objects from Polymerization-Induced and Crystallization-Driven Self-Assembly

Polymerization-Induced Electrostatic Self-Assembly Governed by Guanidinium Ionic Hydrogen Bonds

Interpolyelectrolyte Complexes as an Emerging Technology for Pharmaceutical Delivery of Polypeptides

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