Regulating Protein Secondary Structures Enables Versatile Hydrogels with Tunable Mechanical Properties

Abstract

Regulating the mechanical performance of a material, especially for protein hydrogels, in situ from elasticity to plasticity and vice versa would be difficult but highly anticipated due to the diversity of promising applications. Herein, we proposed a strategy to prepare versatile hydrogels with tunable mechanical properties. It was demonstrated that we could rapidly prepare regenerated silk fibroin/gelatin (RSF/Gel) copolymer hydrogels by chemically modifying RSF by glycidyl methacrylate (RSF-MA) and gelatin by methacrylic anhydride (Gel-MA) under UV light in 60 s. Furthermore, the RSF/Gel hydrogels showed tunable mechanical properties by controlling the β-sheet content of SF, which can realize reversible switch between elasticity and plasticity in situ. The significant alteration of tensile stress at break and tensile elastic modulus at 10% strain was achieved with 720 times and 2000 times improvement from an elastic to plastic hydrogel. The compressive elastic modulus at 50% strain of a plastic hydrogel was improved to 3.6 MPa, which was 62 times higher than that of an elastic hydrogel. In addition, the performance of drug release of RSF/Gel hydrogel microneedles could be modulated by controlling the β-sheet content of SF, which could be a drug carrier and also be other promising biomaterials for a variety of biological and clinical applications.

An injectable photocuring silk fibroin-based hydrogel for constructing an antioxidant microenvironment for skin repair

“…2b shows that the pores gradually became smaller with increasing DMA content. The possible reason was that MASF had poor photo-crosslinking performance, 30 while DMA increased the crosslinking density in the hydrogel network, eventually influencing the pore structure. The hydrogels’ swelling performances are shown in Fig.…”

A Bio‐Inspired Free‐Standing Film with Versatility: From Heterogeneous CTCs Programed Isolating to Breast Cancer Molecular Typing

“…It is found from Figure S4 (Supporting Information) and Figure 3c–e that the proliferation effect of MCF‐7 cells and SK‐BR‐3 cells on PDA@TiO 2 NTbs‐SF (peptide‐) was much higher than the one on rigid quartz plate within 7 days. In addition, hard TSF/MDBS with a poor flexibility treated by ethanol [ 15 ] (inducing more β‐sheet conformation in SF film) was used to test the assay above Figure 3f,g. Compared to soft TSF/MDBS with PBS treatment, the capture ability of hard one to MCF‐7 cells and SK‐BR‐3 cells was significantly reduced by 22% and 14%, respectively (Figure 3h–k).…”

Achieving a Reversible and Durable Zn Anode Using the Polyzwitterionic Hydrogel Electrolyte for Efficient Zn-Ion Energy Storage

“…The PHSHE also shows higher elongation at break (207.8%), tensile stress (15.2 kPa), Young's modulus (7.3 kPa), and fracture energy (17.8 kJ m −3 ), compared with those of the PHHE (117.4%, 9.9 kPa, 5.8 kPa, and 6.5 kJ m −3 , respectively) (Figure2e). This comparison indicates the improvement of the PHSHE in mechanical strength and stretchability, which stems from the cross-linked network structure with rich bonding relationships and high cross-linking density of the polymeric matrix 30. Concretely, the covalent bonds construct the cross-linked network, while the synergistic effects of hydrogen bonds and electrostatic interactions dissipate energy effectively during the deformation process 31.…”

“…This comparison indicates the improvement of the PHSHE in mechanical strength and stretchability, which stems from the cross-linked network structure with rich bonding relationships and high cross-linking density of the polymeric matrix. 30 Concretely, the covalent bonds construct the cross-linked network, while the synergistic effects of hydrogen bonds and electrostatic interactions dissipate energy effectively during the deformation process. 31 These results suggest that the PHSHE features excellent mechanical properties, which can shelter energy storage devices against the loss of performance caused by deformations.…”