Organic/inorganic hydrogels by simultaneous self-assembly and mineralization of aromatic short-peptides

Mañas‐Torres, Mari C.; Ramírez-Rodríguez, Gloria Belén; Garcia-Peiro, Jose I.; Parra-Torrejón, Belén; Cuerva, Juan M.; López–López, Modesto T.; Cienfuegos, Luı́s Álvarez de; Delgado-López, José Manuel

doi:10.1039/d1qi01249e

Cited by 16 publications

(11 citation statements)

References 62 publications

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“…Short-peptide supramolecular hydrogels have turned out to be excellent materials with multiple bio- and technological applications. − Some of these applications are due to the way these peptides self-assemble to form the hydrogel. In particular, aromatic short-peptides such as Fmoc (fluorenylmethoxicarbonyl)- or Nap (2-naphthylacetic acid)-dipeptides, are extremely versatile, being able to self-assemble under the influence of multiple and diverse stimuli, such as solvent and pH switch, change in temperature, the presence of different salts, the action of enzymes, etc. − This versatility has been very useful to develop hydrogels for different applications, such as tissue engineering , and drug delivery, , and to control the type and morphology of the polymeric fibers and the macroscopic and physical properties of the resulting gels. − Furthermore, the stimulus process has also been key in obtaining hybrid or composite materials . Composite materials have been obtained mainly by the combination of two different organic materials, such as the combination of two aromatic peptides that can be copolymerized or independently homopolymerized by controlling the stimulus process.…”

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confidence: 99%

“…14−18 Furthermore, the stimulus process has also been key in obtaining hybrid or composite materials. 19 Composite materials have been obtained mainly by the combination of two different organic materials, such as the combination of two aromatic peptides that can be copolymerized 20 or independently homopolymerized 21 also been a success, since these peptides can self-assemble in the presence of a multitude of inorganic, metallic, and carbonbased materials. 22,23 Particular types of interesting hybrid hydrogels are those containing carbon nanotubes (CNTs).…”

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confidence: 99%

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Chirality-Induced Spin Selectivity in Heterochiral Short-Peptide–Carbon-Nanotube Hybrid Networks: Role of Supramolecular Chirality

et al. 2022

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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 chiralityinduced 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−shortpeptide materials made by the combination of two different chiral sources: that is, homochiral peptides (L/D) + glucono-δlactone. 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.

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Chirality-Induced Spin Selectivity in Heterochiral Short-Peptide–Carbon-Nanotube Hybrid Networks: Role of Supramolecular Chirality

et al. 2022

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“…We have observed a similar process in the biomineralization of hydroxyapatite but in this case mediated by Ca 2+ . 30 Composite hydrogels (Fmoc-FF 20 mM; HmIm/ Zn ratio of 5:1) were also observed by confocal laser scanning microscopy (CLSM) as Fmoc-peptides and ZIF-8 are fluorescent. Figure 3L shows a uniform basal green fluorescence emission from peptide fibers decorated with tiny spherical particles corresponding to ZIF-8 composite particles (see Figure S4 for CLSM of ZIF-8 grown in water and Fmoc-FF hydrogels).…”

Section: Diffusion Protocolmentioning

confidence: 99%

Short-Peptide Supramolecular Hydrogels for In Situ Growth of Metal–Organic Framework-Peptide Biocomposites

Illescas‐Lopez

Martin-Romera

Mañas‐Torres

et al. 2023

ACS Appl. Mater. Interfaces

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The development of bio-MOFs or MOF biocomposites through the combination of MOFs with biopolymers offers the possibility of expanding the potential applications of MOFs, making use of more environmentally benign processes and reagents and giving rise to a new generation of greener and more bio-oriented composite materials. Now, with the increasing use of MOFs for biotechnological applications, the development of new protocols and materials to obtain novel bio-MOFs compatible with biomedical or biotechnological uses is needed. Herein, and as a proof of concept, we have explored the possibility of using short-peptide supramolecular hydrogels as media to promote the growth of MOF particles, giving rise to a new family of bio-MOFs. Short-peptide supramolecular hydrogels are very versatile materials that have shown excellent in vitro and in vivo biomedical applications such as tissue engineering and drug delivery vehicles, among others. These peptides self-assemble by noncovalent interactions, and, as such, these hydrogels are easily reversible, being more biocompatible and biodegradable. These peptides can self-assemble by a multitude of stimuli, such as changes in pH, temperature, solvent, adding salts, enzymatic activity, and so forth. In this work, we have taken advantage of this ability to promote peptide self-assembly with some of the components required to form MOF particles, giving rise to more homogeneous and well-integrated composite materials. Hydrogel formation has been triggered using Zn 2+ salts, required to form ZIF-8, and formic acid, required to form MOF-808. Two different protocols for the in situ MOF growth have been developed. Finally, the MOF-808 composite hydrogel has been tested for the decontamination of water polluted with phosphate ions as well as for the catalytic degradation of toxic organophosphate methyl paraoxon in an unbuffered solution.

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“…All of these factors have contributed to broadening the use of these peptides to develop and explore materials. − Another key characteristic of these peptides is their ability to self-assemble under the application of different stimuli, such as solvent or pH switch, addition of salts, or enzymatic reactions. , This can be exploited to induce gelation under physiological conditions, making them highly compatible with biomedical applications . Furthermore, their resulting macroscopic and physical properties can also be affected or tuned by different stimuli offering an extra degree of versatility. , In addition, control over the stimulus-induced transition is also crucial to obtain composite or hybrid hydrogels made by the combination of several organic compounds , or mixtures of organic and inorganic/metallic substrates. ,− At such, Adams et al have shown that mixtures of different Nap-dipeptides, under specific pH conditions, can form copolymers (co-assembly) or individual homopolymers (self-sorting) based on the relative p K a of the amino acids involved. − We have recently shown that Fmoc-FF (Fmoc-diphenylalanine) is able to promote the co-assembly of different Fmoc- and Nap-dipeptides giving rise to hydrogels having different mechanical properties . The mechanism of growth of these peptides usually follows a nucleation–elongation mechanism in which, starting from an initial metastable phase, the formation of fibers is triggered when the conditions allow overpassing the free energy barrier of polymerization. − We have shown that metastable intermediates formed by the combination of two different peptides had a lower free energy barrier of polymerization; therefore, the co-assembly was favored vs the self-assembly of individual peptides .…”

Section: Introductionmentioning

confidence: 99%

Biocompatible Short-Peptides Fibrin Co-assembled Hydrogels

Gila-Vilchez

Mañas‐Torres

García-García

et al. 2023

ACS Appl. Polym. Mater.

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Fibrin hydrogels made by self-assembly of fibrinogen obtained from human plasma have shown excellent biocompatible and biodegradable properties and are widely used in regenerative medicine. The fibrinogen self-assembly process can be triggered under physiological conditions by the action of thrombin, allowing the injection of pregel mixtures that have been used as cell carriers, wound-healing systems, and bio-adhesives. However, access to fibrinogen from human plasma is expensive and fibrin gels have limited mechanical properties, which make them unsuitable for certain applications. One solution to these problems is to obtain composite gels made of fibrin and other polymeric compounds that improve their mechanical properties and usage. Herein, we prepared composite hydrogels made by the self-assembly of fibrinogen together with Fmoc-FF (Fmoc-diphenylalanine) and Fmoc-RGD (Fmoc-arginine-glycine-aspartic acid). We have shown that the mixture of these three peptides co-assembles and gives rise to a unique type of supramolecular fiber, whose morphology and mechanical properties can be modulated. We have carried out a complete characterization of these materials from chemical, physical, and biological points of view. Composite gels have improved mechanical properties compared to pure fibrin gels, as well as showing excellent biocompatibility ex vivo. In vivo experiments have shown that these gels do not cause any type of inflammatory response or tissue damage and are completely resorbed in short time, which would enable their use as vehicles for cell, drug, or growth factor release.

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Organic/inorganic hydrogels by simultaneous self-assembly and mineralization of aromatic short-peptides

Abstract: Self-assembled peptides and proteins have turned out to be excellent templates for the growth of inorganic minerals trying to emulate natural biomineralization processes. Doing this, researchers have developed complex sophisticate...

Cited by 16 publications

References 62 publications

Chirality-Induced Spin Selectivity in Heterochiral Short-Peptide–Carbon-Nanotube Hybrid Networks: Role of Supramolecular Chirality

Chirality-Induced Spin Selectivity in Heterochiral Short-Peptide–Carbon-Nanotube Hybrid Networks: Role of Supramolecular Chirality

Short-Peptide Supramolecular Hydrogels for In Situ Growth of Metal–Organic Framework-Peptide Biocomposites

Biocompatible Short-Peptides Fibrin Co-assembled Hydrogels

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