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      Responsive peptide-based supramolecular hydrogels constructed by self-immolative chemistry

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          Abstract

          Peptide-based supramolecular hydrogels that are stimuli-responsive under aqueous conditions have many potential biological applications, including drug delivery and sensing.

          Abstract

          Peptide-based supramolecular hydrogels that are stimuli-responsive under aqueous conditions have many potential biological applications, including drug delivery and sensing. Herein, we reported a series of responsive peptide-based supramolecular hydrogels that respond to glutathione (GSH), nitric oxide (NO) and hydrogen sulfide (H 2S), which are biologically important signaling molecules. The responsive hydrogelators were designed by “self-immolative” chemistry and constructed by using self-immolative groups to modify short peptides. The self-immolative capping group could be removed in the presence of a corresponding trigger, thus causing gel–sol phase transitions. The potential of our responsive hydrogels for drug release was also demonstrated in this study. Our study offered several candidates of responsive hydrogels for sensing and drug delivery.

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          Transient assembly of active materials fueled by a chemical reaction.

          Job Boekhoven, Wouter Hendriksen, Ger J M Koper … (2015)
          Fuel-driven self-assembly of actin filaments and microtubules is a key component of cellular organization. Continuous energy supply maintains these transient biomolecular assemblies far from thermodynamic equilibrium, unlike typical synthetic systems that spontaneously assemble at thermodynamic equilibrium. Here, we report the transient self-assembly of synthetic molecules into active materials, driven by the consumption of a chemical fuel. In these materials, reaction rates and fuel levels, instead of equilibrium composition, determine properties such as lifetime, stiffness, and self-regeneration capability. Fibers exhibit strongly nonlinear behavior including stochastic collapse and simultaneous growth and shrinkage, reminiscent of microtubule dynamics.
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            Biological Photothermal Nanodots Based on Self-Assembly of Peptide-Porphyrin Conjugates for Antitumor Therapy.

            Qianli Zou, Xuehai Yan, Guizhi Shen … (2017)
            Photothermal agents can harvest light energy and convert it into heat, offering a targeted and remote-controlled way to destroy carcinomatous cells and tissues. Inspired by the biological organization of polypeptides and porphyrins in living systems, here we have developed a supramolecular strategy to fabricate photothermal nanodots through peptide-modulated self-assembly of photoactive porphyrins. The self-assembling nature of porphyrins induces the formation of J-aggregates as substructures of the nanodots, and thus enables the fabrication of nanodots with totally inhibited fluorescence emission and singlet oxygen production, leading to a high light-to-heat conversion efficiency of the nanodots. The peptide moieties not only provide aqueous stability for the nanodots through hydrophilic interactions, but also provide a spatial barrier between porphyrin groups to inhibit the further growth of nanodots through the strong π-stacking interactions. Thermographic imaging reveals that the conversion of light to heat based on the nanodots is efficient in vitro and in vivo, enabling the nanodots to be applied for photothermal acoustic imaging and antitumor therapy. Antitumor therapy results show that these nanodots are highly biocompatible photothermal agents for tumor ablation, demonstrating the feasibility of using bioinspired nanostructures of self-assembling biomaterials for biomedical photoactive applications.
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              Installing logic-gate responses to a variety of biological substances in supramolecular hydrogel-enzyme hybrids.

              Masato Ikeda, Tatsuya Tanida, Tatsuyuki Yoshii … (2014)
              Soft materials that exhibit stimuli-responsive behaviour under aqueous conditions (such as supramolecular hydrogels composed of self-assembled nanofibres) have many potential biological applications. However, designing a macroscopic response to structurally complex biochemical stimuli in these materials still remains a challenge. Here we show that redox-responsive peptide-based hydrogels have the ability to encapsulate enzymes and still retain their activities. Moreover, cooperative coupling of enzymatic reactions with the gel response enables us to construct unique stimuli-responsive soft materials capable of sensing a variety of disease-related biomarkers. The programmable gel-sol response (even to biological samples) is visible to the naked eye. Furthermore, we built Boolean logic gates (OR and AND) into the hydrogel-enzyme hybrid materials, which were able to sense simultaneously plural specific biochemicals and execute a controlled drug release in accordance with the logic operation. The intelligent soft materials that we have developed may prove valuable in future medical diagnostics or treatments.
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                Author and article information

                Contributors
                Journal
                Journal ID (publisher-id): NANOHL
                Title: Nanoscale
                Abbreviated Title: Nanoscale
                Publisher: Royal Society of Chemistry (RSC)
                ISSN (Print): 2040-3364
                ISSN (Electronic): 2040-3372
                Publication date Created: November 22 2018
                Publication date (Electronic): 2018
                Volume: 10
                Issue: 45
                Pages: 21459-21465
                Affiliations
                [1 ]State Key Laboratory of Medicinal Chemical Biology
                [2 ]College of Pharmacy
                [3 ]Tianjin Key Laboratory of Molecular Drug Research
                [4 ]Nankai University
                [5 ]Tianjin 300071
                [6 ]College of Life Sciences
                [7 ]Key Laboratory of Bioactive Materials
                [8 ]Ministry of Education
                [9 ]and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
                Article
                DOI: 10.1039/C8NR07534D
                SO-VID: f7aa59bb-c3e6-4f05-8fc2-929c2bffe1d0
                Copyright © © 2018
                License:

                http://rsc.li/journals-terms-of-use

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