Poly( L-lysine)- block-poly(ethylene glycol)- block-poly( L-lysine) triblock copolymers for the preparation of flower micelles and their irreversible hydrogel formation

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ABSTRACT

Poly( _L-lysine)- block-poly(ethylene glycol)- block-poly( _L-lysine) (PLys- block-PEG- block-PLys) triblock copolymers formed polyion complex (PIC) with poly(acrylic acid) (PAAc) or sodium poly(styrenesulfonate) (PSS), leading to the formation of flower micelle-type nanoparticles (Nano ^Lys/PAAc or Nano ^Lys/PSS) with tens of nanometers size in water at a polymer concentration of 10 mg/mL. The flower micelles exhibited irreversible temperature-driven sol-gel transitions at physiological ionic strength, even at low polymer concentrations such as 40 mg/mL, making them promising candidates for injectable hydrogel applications. Rheological studies showed that the chain length of PLys segments and the choice of polyanions significantly impacted irreversible hydrogel formation, with PSS being superior to PAAc for the formation. The incorporation of silica gel nanoparticles into the PIC flower micelles also resulted in irreversible gelation phenomena. The highest storage modulus exceeded 10 kPa after gelation, which is sufficient for practical applications. This study demonstrates the potential of these PIC-based hydrogels as biomaterials with tunable properties for biomedical applications.

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A polyion complex-based flower micelle, formed by poly( _L-lysine)- block-PEG- block-poly( _L-lysine) triblock copolymers and polyanions, shows irreversible hydrogel formation; incorporating silica enhanced its modulus to exceeding 10 kPa, promising for biomedical applications.

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Biodegradable block copolymers as injectable drug-delivery systems.

Byeongmoon Jeong, You Bae, Doo Sung Lee … (1997)

Polymers that display a physicochemical response to stimuli are widely explored as potential drug-delivery systems. Stimuli studied to date include chemical substances and changes in temperature, pH and electric field. Homopolymers or copolymers of N-isopropylacrylamide and poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide) (known as poloxamers) are typical examples of thermosensitive polymers, but their use in drug delivery is problematic because they are toxic and non-biodegradable. Biodegradable polymers used for drug delivery to date have mostly been in the form of injectable microspheres or implant systems, which require complicated fabrication processes using organic solvents. Such systems have the disadvantage that the use of organic solvents can cause denaturation when protein drugs are to be encapsulated. Furthermore, the solid form requires surgical insertion, which often results in tissue irritation and damage. Here we report the synthesis of a thermosensitive, biodegradable hydrogel consisting of blocks of poly(ethylene oxide) and poly(L-lactic acid). Aqueous solutions of these copolymers exhibit temperature-dependent reversible gel-sol transitions. The hydrogel can be loaded with bioactive molecules in an aqueous phase at an elevated temperature (around 45 degrees C), where they form a sol. In this form, the polymer is injectable. On subcutaneous injection and subsequent rapid cooling to body temperature, the loaded copolymer forms a gel that can act as a sustained-release matrix for drugs.

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Self-Healing Injectable Hydrogels for Tissue Regeneration

Pascal Bertsch, Mani Diba, David J. Mooney … (2022)

Biomaterials with the ability to self-heal and recover their structural integrity offer many advantages for applications in biomedicine. The past decade has witnessed the rapid emergence of a new class of self-healing biomaterials commonly termed injectable, or printable in the context of 3D printing. These self-healing injectable biomaterials, mostly hydrogels and other soft condensed matter based on reversible chemistry, are able to temporarily fluidize under shear stress and subsequently recover their original mechanical properties. Self-healing injectable hydrogels offer distinct advantages compared to traditional biomaterials. Most notably, they can be administered in a locally targeted and minimally invasive manner through a narrow syringe without the need for invasive surgery. Their moldability allows for a patient-specific intervention and shows great prospects for personalized medicine. Injected hydrogels can facilitate tissue regeneration in multiple ways owing to their viscoelastic and diffusive nature, ranging from simple mechanical support, spatiotemporally controlled delivery of cells or therapeutics, to local recruitment and modulation of host cells to promote tissue regeneration. Consequently, self-healing injectable hydrogels have been at the forefront of many cutting-edge tissue regeneration strategies. This study provides a critical review of the current state of self-healing injectable hydrogels for tissue regeneration. As key challenges toward further maturation of this exciting research field, we identify (i) the trade-off between the self-healing and injectability of hydrogels vs their physical stability, (ii) the lack of consensus on rheological characterization and quantitative benchmarks for self-healing injectable hydrogels, particularly regarding the capillary flow in syringes, and (iii) practical limitations regarding translation toward therapeutically effective formulations for regeneration of specific tissues. Hence, here we (i) review chemical and physical design strategies for self-healing injectable hydrogels, (ii) provide a practical guide for their rheological analysis, and (iii) showcase their applicability for regeneration of various tissues and 3D printing of complex tissues and organoids.

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Effect of beta-hydroxy-beta-methylbutyrate, arginine, and lysine supplementation on strength, functionality, body composition, and protein metabolism in elderly women.

Paul Flakoll, Rick Sharp, Shawn Baier … (2004)

With advancing age, there is a gradual loss of muscle mass, strength, and functionality. The current studies were conducted to determine whether a mixture of specific nutrients, arginine and lysine, which support protein synthesis, and beta-hydroxy-beta-methylbutyrate (HMB), which can slow protein breakdown, could blunt the gradual loss of muscle that occurs in the elderly, thus improving strength and functionality. In double-blind studies conducted at two separate sites, women (mean 76.7 y) were randomized to a placebo group (n = 23) or an experimental treatment group (2 g beta-hydroxy-beta-methylbutyrate, 5 g arginine, and 1.5 g lysine daily; n = 27). After 12 wk, there was a 17% improvement in the "get-up-and-go" functionality test in the experimental group (-2.3 +/- 0.5 s) but no change in the placebo group (0.0 +/- 0.5 s; P = 0.002). The improvement in functionality also was reflected by increased limb circumference, leg strength, and handgrip strength (all P < 0.05) and positive trends in fat-free mass (P = 0.08). Whole-body protein synthesis, estimated with the (15)N-glycine tracer technique over a 24-h free-living period, increased approximately 20% in the experimental treatment group as opposed to the placebo group (P = 0.03). These studies indicated that daily supplementation of beta-hydroxy-beta-methylbutyrate, arginine, and lysine for 12 wk positively alters measurements of functionality, strength, fat-free mass, and protein synthesis, suggesting that the strategy of targeted nutrition has the ability to affect muscle health in elderly women.

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Journal

Journal ID (nlm-ta): Sci Technol Adv Mater

Journal ID (iso-abbrev): Sci Technol Adv Mater

Title: Science and Technology of Advanced Materials

Publisher: Taylor & Francis

ISSN (Print): 1468-6996

ISSN (Electronic): 1878-5514

Publication date (Electronic, pub): 25 November 2024

Publication date (Electronic, collection): 2025

Publication date PMC-release: 25 November 2024

Volume: 26

Issue: 1

Electronic Location Identifier: 2432856

Affiliations

[a ]Department of Materials Science, Institute of Pure and Applied Sciences, University of Tsukuba; , Tsukuba, Ibaraki, Japan

[b ]Master’s School of Medical Sciences, Graduate School of Comprehensive Human Sciences, University of Tsukuba; , Tsukuba, Ibaraki, Japan

[c ]Center for Research in Radiation, Isotope and Earth System Sciences (CRiES), University of Tsukuba; , Tsukuba, Ibaraki, Japan

[d ]Department of Chemistry, Graduate School of Science, The University of Tokyo; , Bunkyo-ku, Tokyo, Japan

[e ]High-value Biomaterials Research and Commercialization Center (HBRCC), National Taipei University of Technology; , Taipei, Taiwan

Author notes

CONTACT Yuta Koda koda@ 123456ims.tsukuba.ac.jp Department of Materials Science, Institute of Pure and Applied Sciences, University of Tsukuba, 1-1-1 Tennoudai, Tsukuba, Ibaraki 305–8573, Japan

Author information

Yuta Koda https://orcid.org/0000-0003-1724-2359

Yukio Nagasaki https://orcid.org/0000-0001-7975-6510

Article

Publisher ID: 2432856

DOI: 10.1080/14686996.2024.2432856

PMC ID: 11703508

SO-VID: 3fb7fd53-3622-4d50-823f-d150267b5724

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This is an Open Access article distributed under the terms of the Creative Commons Attribution License ( http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. The terms on which this article has been published allow the posting of the Accepted Manuscript in a repository by the author(s) or with their consent.

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Figures: 5, Tables: 1, References: 36, Pages: 1, Words: 6165

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Poly( _L-lysine)- block-poly(ethylene glycol)- block-poly( _L-lysine) triblock copolymers for the preparation of flower micelles and their irreversible hydrogel formation

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Most cited references 36

Biodegradable block copolymers as injectable drug-delivery systems.

Self-Healing Injectable Hydrogels for Tissue Regeneration

Effect of beta-hydroxy-beta-methylbutyrate, arginine, and lysine supplementation on strength, functionality, body composition, and protein metabolism in elderly women.

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