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Journal ArticleDOI

Injectable Magnetic-Responsive Short-Peptide Supramolecular Hydrogels: Ex Vivo and In Vivo Evaluation.

TL;DR: In this article, the behavior of biocompatible and biodegradable hydrogels made with Fmoc-diphenylalanine (Fmoc)-FF) and RGD short peptides to which MNP were incorporated was studied in detail with physicochemical, mechanical, and biological methods.
Abstract: The inclusion of magnetic nanoparticles (MNP) in a hydrogel matrix to produce magnetic hydrogels has broadened the scope of these materials in biomedical research. Embedded MNP offer the possibility to modulate the physical properties of the hydrogel remotely and on demand by applying an external magnetic field. Moreover, they enable permanent changes in the mechanical properties of the hydrogel, as well as alterations in the micro- and macroporosity of its three-dimensional (3D) structure, with the associated potential to induce anisotropy. In this work, the behavior of biocompatible and biodegradable hydrogels made with Fmoc-diphenylalanine (Fmoc-FF) (Fmoc = fluorenylmethoxycarbonyl) and Fmoc-arginine-glycine-aspartic acid (Fmoc-RGD) short peptides to which MNP were incorporated was studied in detail with physicochemical, mechanical, and biological methods. The resulting hybrid hydrogels showed enhance mechanical properties and withstood injection without phase disruption. In mice, the hydrogels showed faster and improved self-healing properties compared to their nonmagnetic counterparts. Thanks to these superior physical properties and stability during culture, they can be used as 3D scaffolds for cell growth. Additionally, magnetic short-peptide hydrogels showed good biocompatibility and the absence of toxicity, which together with their enhanced mechanical stability and excellent injectability make them ideal biomaterials for in vivo biomedical applications with minimally invasive surgery. This study presents a new approach to improving the physical and mechanical properties of supramolecular hydrogels by incorporating MNP, which confer structural reinforcement and stability, remote actuation by magnetic fields, and better injectability. Our approach is a potential catalyst for expanding the biomedical applications of supramolecular short-peptide hydrogels.
Citations
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Journal ArticleDOI
TL;DR: This Review will analyze the last 5-year progress on the incorporation of bioactive motifs into self-assembling peptides to mimic functional proteins of the extracellular matrix and guide cell fate inside hydrogel scaffolds.
Abstract: Proteins are functional building blocks of living organisms that exert a wide variety of functions, but their synthesis and industrial production can be cumbersome and expensive. By contrast, short peptides are very convenient to prepare at a low cost on a large scale, and their self-assembly into nanostructures and gels is a popular avenue for protein biomimicry. In this Review, we will analyze the last 5-year progress on the incorporation of bioactive motifs into self-assembling peptides to mimic functional proteins of the extracellular matrix (ECM) and guide cell fate inside hydrogel scaffolds.

8 citations

Journal ArticleDOI
11 Oct 2022-ACS Nano
TL;DR: Heterochiral carbon-nanotube-short-peptide materials made by the combination of two different chiral sources are developed, showing that the presence of a small amount of glucono-δ-lactone with fixed chirality can alter the supramolecular chiralities of the medium, thereby modulating the sign of the spin signal from "up" to "down" and vice versa.
Abstract: Supramolecular short-peptide assemblies have been widely used for the development of biomaterials with potential biomedical applications. These peptides can self-assemble in a multitude of chiral hierarchical structures triggered by the application of different stimuli, such as changes in temperature, pH, solvent, etc. The self-assembly process is sensitive to the chemical composition of the peptides, being affected by specific amino acid sequence, type, and chirality. The resulting supramolecular chirality of these materials has been explored to modulate protein and cell interactions. Recently, significant attention has been focused on the development of chiral materials with potential spintronic applications, as it has been shown that transport of charge carriers through a chiral environment polarizes the carrier spins. This effect, named chirality-induced spin selectivity or CISS, has been studied in different chiral organic molecules and materials, as well as carbon nanotubes functionalized with chiral molecules. Nevertheless, this effect has been primarily explored in homochiral systems in which the chirality of the medium, and hence the resulting spin polarization, is defined by the chirality of the molecule, with limited options for tunability. Herein, we have developed heterochiral carbon-nanotube-short-peptide materials made by the combination of two different chiral sources: that is, homochiral peptides (l/d) + glucono-δ-lactone. We show that the presence of a small amount of glucono-δ-lactone with fixed chirality can alter the supramolecular chirality of the medium, thereby modulating the sign of the spin signal from "up" to "down" and vice versa. In addition, small amounts of glucono-δ-lactone can even induce nonzero spin polarization in an otherwise achiral and spin-inactive peptide-nanotube composite. Such "chiral doping" strategies could allow the development of complementary CISS-based spintronic devices and circuits on a single material platform.

7 citations

Journal ArticleDOI
TL;DR: An overview of innovation in material design for smart hydrogel systems, current technical approaches toward 4D printing, and emerging 4D printed novel structures for drug delivery applications is provided.
Abstract: Advancements in the material design of smart hydrogels have transformed the way therapeutic agents are encapsulated and released in biological environments. On the other hand, the expeditious development of 3D printing technologies has revolutionized the fabrication of hydrogel systems for biomedical applications. By combining these two aspects, 4D printing (i.e., 3D printing of smart hydrogels) has emerged as a new promising platform for the development of novel controlled drug delivery systems that can adapt and mimic natural physio-mechanical changes over time. This allows printed objects to transform from static to dynamic in response to various physiological and chemical interactions, meeting the needs of the healthcare industry. In this review, we provide an overview of innovation in material design for smart hydrogel systems, current technical approaches toward 4D printing, and emerging 4D printed novel structures for drug delivery applications. Finally, we discuss the existing challenges in 4D printing hydrogels for drug delivery and their prospects.

6 citations

Journal ArticleDOI
TL;DR: In this paper , the role of magnetic nanoparticles in the self-assembly process of magnetic supramolecular hydrogels is discussed, as well as the applications of these materials in biomedical and biotechnological applications.
Abstract: Most recent advances in the synthesis of supramolecular hydrogels based on low molecular weight gelators (LMWGs) have focused on the development of novel hybrid hydrogels, combining LMWGs and different additives. The dynamic nature of the noncovalent interactions of supramolecular hydrogels, together with the specific properties of the additives included in the formulation, allow these novel hybrid hydrogels to present interesting features, such as stimuli-responsiveness, gel-sol reversibility, self-healing and thixotropy, which make them very appealing for multiple biomedical and biotechnological applications. In particular, the inclusion of magnetic nanoparticles in the hydrogel matrix results in magnetic hydrogels, a particular type of stimuli-responsive materials that respond to applied magnetic fields. This review focuses on the recent advances in the development of magnetic supramolecular hydrogels, with special emphasis in the role of the magnetic nanoparticles in the self-assembly process, as well as in the exciting applications of these materials.

4 citations

Journal ArticleDOI
TL;DR: The characterization, biocompatibility, controlled release effect on antigen, immune cell recruitment ability, and antitumor properties of a self-assembly peptide named DRF3, which provide a reliable basis for the application of peptide hydrogels in biomedical and preclinical trials.
Abstract: Self-assembly peptide nanotechnology has attracted much attention due to its regular and orderly structure and diverse functions. Most of the existing self-assembly peptides can form aggregates with specific structures only under specific conditions and their assembly time is relatively long. They have good biocompatibility but no immunogenicity. To optimize it, a self-assembly peptide named DRF3 was designed. It contains a hydrophilic and hydrophobic surface, using two N-terminal arginines, leucine, and two c-terminal aspartate and glutamic acid. Meanwhile, the c-terminal of the peptide was amidated, so that peptide segments were interconnected to increase diversity. Its characterization, biocompatibility, controlled release effect on antigen, immune cell recruitment ability, and antitumor properties were examined here. Congo red/aniline blue staining revealed that peptide hydrogel DRF3 could be immediately gelled in PBS. The stable β-sheet secondary structure of DRF3 was confirmed by circular dichroism spectrum and IR spectra. The observation results of cryo-scanning electron microscopy, transmission electron microscopy, and atomic force microscopy demonstrated that DRF3 formed nanotubule-like and vesicular structures in PBS, and these structures interlaced with each other to form ordered three-dimensional nanofiber structures. Meanwhile, DRF3 showed excellent biocompatibility, could sustainably and slowly release antigens, recruit dendritic cells and promote the maturation of dendritic cells (DCs) in vitro. In addition, DRF3 has a strong inhibitory effect on clear renal cell carcinoma (786-0). These results provide a reliable basis for the application of peptide hydrogels in biomedical and preclinical trials.

3 citations

References
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Journal ArticleDOI

4,511 citations

Journal ArticleDOI
17 Feb 2012-Science
TL;DR: The specific features of supramolecular polymers that can lead to applications in a variety of fields are reviewed, including: materials—in which processability and self-healing properties are of interest; biomedicine— in which the concerns are dynamic functionality and biodegradability; and hierarchical assembly and electronic systems—with an interest in unidirectionality of charge flow.
Abstract: Supramolecular polymers can be random and entangled coils with the mechanical properties of plastics and elastomers, but with great capacity for processability, recycling, and self-healing due to their reversible monomer-to-polymer transitions. At the other extreme, supramolecular polymers can be formed by self-assembly among designed subunits to yield shape-persistent and highly ordered filaments. The use of strong and directional interactions among molecular subunits can achieve not only rich dynamic behavior but also high degrees of internal order that are not known in ordinary polymers. They can resemble, for example, the ordered and dynamic one-dimensional supramolecular assemblies of the cell cytoskeleton and possess useful biological and electronic functions.

2,777 citations

Journal ArticleDOI
TL;DR: This Review discusses how different mechanisms interact and can be integrated to exert fine control in time and space over the drug presentation, and collects experimental release data from the literature and presents quantitative comparisons between different systems to provide guidelines for the rational design of hydrogel delivery systems.
Abstract: Hydrogel delivery systems can leverage therapeutically beneficial outcomes of drug delivery and have found clinical use. Hydrogels can provide spatial and temporal control over the release of various therapeutic agents, including small-molecule drugs, macromolecular drugs and cells. Owing to their tunable physical properties, controllable degradability and capability to protect labile drugs from degradation, hydrogels serve as a platform in which various physiochemical interactions with the encapsulated drugs control their release. In this Review, we cover multiscale mechanisms underlying the design of hydrogel drug delivery systems, focusing on physical and chemical properties of the hydrogel network and the hydrogel-drug interactions across the network, mesh, and molecular (or atomistic) scales. We discuss how different mechanisms interact and can be integrated to exert fine control in time and space over the drug presentation. We also collect experimental release data from the literature, review clinical translation to date of these systems, and present quantitative comparisons between different systems to provide guidelines for the rational design of hydrogel delivery systems.

2,457 citations

Journal ArticleDOI
TL;DR: From Wichterle’s pioneering work to the most recent hydrogel-based inventions and products on the market, it provides the reader with a detailed introduction to the topic and perspective on further potential developments.

1,788 citations

Journal ArticleDOI
TL;DR: In this paper, the self assembly of peptide hydrogelators that carry aromatic substituents can be modeled by a novel nanocylindrical architecture, which is consistent with the structures observed in TEM and the data obtained by a variety of spectroscopic techniques.
Abstract: The self assembly of peptide hydrogelators that carry aromatic substituents can be modeled by a novel nanocylindrical architecture. The proposed model suggests that the nanocylinders are formed by anti-parallel β-sheets interlocked by the π-stacking interactions of fluorenyl groups and phenyl rings. This explanation is consistent with the structures observed in TEM and the data obtained by a variety of spectroscopic techniques.

803 citations