Recent Development of Fibrous Hydrogels: Properties, Applications and Perspectives

Abstract

Fibrous hydrogels (FGs), characterized by a 3D network structure made from prefabricated fibers, fibrils and polymeric materials, have emerged as significant materials in numerous fields. However, the challenge of balancing mechanical properties and functions hinders their further development. This article reviews the main advantages of FGs, including enhanced mechanical properties, high conductivity, high antimicrobial and anti-inflammatory properties, stimulus responsiveness, and an extracellular matrix (ECM)-like structure. It also discusses the influence of assembly methods, such as fiber cross-linking, interfacial treatments of fibers with hydrogel matrices, and supramolecular assembly, on the diverse functionalities of FGs. Furthermore, the mechanisms for improving the performance of the above five aspects are discussed, such as creating ion carrier channels for conductivity, in situ gelation of drugs to enhance antibacterial and anti-inflammatory properties, and entanglement and hydrophobic interactions between fibers, resulting in ECM-like structured FGs. In addition, this review addresses the application of FGs in sensors, dressings, and tissue scaffolds based on the synergistic effects of optimizing the performance. Finally, challenges and future applications of FGs are discussed, providing a theoretical foundation and new insights for the design and application of cutting-edge FGs.

Keywords: ECM‐like; conductivity; fibrous hydrogels; mechanical; stimulus.

Figure 1

Schematic illustration of regulation properties and applications of fibrous hydrogels.

Figure 2

a) Schematic of three strategies to enhance mechanical properties. b) Schematic about the fabrication process of the FGs. c) The photo of the hydrogel in the initial and stretched states. Reproduced with permission.^{[ 56 ]} Copyright 2023, Elsevier. d) Preparation process and SEM image e) of the hydrogel film. f) Illustration of the PU fibers embedded structure and bonding mechanisms. g) The photo of the FGs film adhere to skin. (h) Modulus matching range of the FGs. Reproduced with permission.^{[ 24 ]} Copyright 2023, Springer Nature.

Figure 3

a) images of hydrogel at macroscopic and b,c) microscopic. d) Three stages of solvent‐exchange strategy for the preparation of FGs. Reproduced with permission.^{[ 66 ]} Copyright 2024, Wiley‐VCH. e) The mechanisms behind performance enhancements the at each length scale. Reproduced with permission.^{[ 68 ]} Copyright 2024, American Association for the Advancement of Science.

Figure 4

a) Schematic of three strategies to enhance conductivity properties. b) Schematics of the template about nanofibers and the conductivity c) of hydrogel. Reproduced with permission.^{[ 84 ]} Copyright 2023, Springer Nature. d) Schematic illustrations of the microstructure for the hydrogels. e) Schematic diagram of ions movement. f) The photos about luminance of LEDs by hydrogel at different temperatures. Reproduced with permission.^{[ 86 ]} Copyright 2022, Springer Nature. g) The preparation process of silk ionotropic hydrogel fibers. Reproduced with permission.^{[ 88 ]} Copyright 2024, Springer Nature. h) The process of the melt spinning of hydrogel fiber. Reproduced with permission.^{[ 89 ]} Copyright 2024, American Association for the Advancement of Science. i) Schematic of spider‐silk‐inspired iongel structure. Reproduced with permission.^{[ 90 ]} Copyright 2024, Wiley‐VCH. j,k) The preparation process of hydrogel fiber. Reproduced with permission.^{[ 91 ]} Copyright 2024, Springer Nature.

Figure 5

a) Schematic of two strategies for high antibacterial and anti‐inflammatory. b) Schematic illustrations of FGs generation. Reproduced with permission.^{[ 102 ]} Copyright 2023, Wiley‐VCH. c) Schematic diagrams of the preparation route to FGs. Reproduced with permission.^{[ 103 ]} Copyright 2023, American Association for the Advancement of Science. d) Schematic diagrams for the synthetic route and mechanism of polycationic hydrogel with exudate. Reproduced with permission.^{[ 105 ]} Copyright 2023, IOP Publishing.

Figure 6

a) Schematic of two strategies for designing stimulus responsive. b) Schematic diagrams for the preparation route, c) pH‐responsive delivery about drugs and the wound healing d) of FGs. Reproduced with permission.^{[ 111 ]} Copyright 2024, Elsevier. e) Illustrations for the preparation hydrogel. Reproduced with permission.^{[ 112 ]} Copyright 2024, Wiley‐VCH. f) Schematic diagrams of FGs under different PH.^{[ 113 ]} Copyright 2024, Springer Nature.

Figure 7

a) Diagrams of Electrical stimulation reversible sol layer. b) Demonstration about FGs movement under an electric field. Reproduced with permission.^{[ 118 ]} Copyright 2023, American Association for the Advancement of Science. c) The Schemes shows the composition and function of the patch.^{[ 121 ]} Copyright 2024, Wiley‐VCH. d) Schematic diagrams of self‐assembling and application peptide FGs. Reproduced with permission.^{[ 53 ]} Copyright 2024, Elsevier. e) UV‐induced polymerization and schematic structure of the NCPN hydrogels. f) The macroscopic and microscopic photographs of hydrogels by restricting the flow of solvents. g) The photos of hydrogels under different times and temperature. h) The encryption and decryption process of hydrogels. Reproduced with permission.^{[ 126 ]} Copyright 2022, Wiley‐VCH. i,j) The components and hydrogen bond clusters in fibers hydrogel. k,l) The deformation process of stress‐responsive fibers hydrogel. Reproduced with permission.^{[ 27 ]} Copyright 2024, Wiley‐VCH.

Figure 8

a) Schematic of four strategies for the construction ECM‐like structures. b) The preparation process, SEM images and performance tests of 3D‐printed tissue scaffolds. Reproduced with permission.^{[ 136 ]} Copyright 2023, Springer Nature. c,d) The s‐b‐s electrospinning process and SEM images of Janus hydrogel fibers. Reproduced with permission.^{[ 137 ]} Copyright 2024, Royal Society of Chemistry. The preparation process f) and SEM images e) of APA/CMCS/KGN @ PGF/GM hydrogels. Reproduced with permission.^{[ 138 ]} Copyright 2023, Wiley‐VCH.

Figure 9

a) Schematic diagrams for design strategy and cells delivery b) of the FGs. Reproduced with permission.^{[ 45 ]} Copyright 2023, Elsevier BV. c) Diagrams for supramolecular assembly and multiple layer structures of C₈C₈, C₁₀C₁₀ and C₁₂C₁₂ were printed. Reproduced with permission.^{[ 142 ]} Copyright 2023, American Association for the Advancement of Science. d) Schematic representation of protein assembly. Reproduced with permission.^{[ 130 ]} Copyright 2023, Wiley‐VCH. e) The design strategy diagram for FGs. Reproduced with permission.^{[ 151 ]} Copyright 2023, American Chemical Society. f,g) The components and SEM images of the hydrogel. Reproduced with permission.^{[ 146 ]} Copyright 2024, Elsevier.

Figure 10

a) Schematics of producing and detecting body fluids by SEB sensor in the human body. b) Schematics of the SEB sensor structure. Reproduced with permission.^{[ 153 ]} Copyright 2024, Springer Nature. c) Schematics of the assembled piezoresistive sensor. Reproduced with permission.^{[ 159 ]} Copyright 2024, Elsevier. d) Schematics for the gestures of a robot by man touching the SIH‐based textiles. Reproduced with permission.^{[ 88 ]} Copyright 2024, Springer Nature. e) The preparation process of PPC hydrogel and f) schematics of TENG sensor. g,h) Schematics shows that the detection and processing of the driver state and the vehicle state. Reproduced with permission.^{[ 164 ]} Copyright 2023, Wiley‐VCH.

Figure 11

a) Schematic diagram of the preparation process of Dual‐Gel and application for wound healing. Reproduced with permission.^{[ 168 ]} Copyright 2024, Wiley‐VCH. b,c) the preparation process of composite material and application for wound healing. Reproduced with permission.^{[ 169 ]} Copyright 2023, Elsevier. d) The preparation and properties of the composite hydrogel. Reproduced with permission.^{[ 175 ]} Copyright 2024, Elsevier. e,f) The preparation process of hydrogel and application for wound healing. Reproduced with permission.^{[ 176 ]} Copyright 2024, Elsevier. g) Schematic diagram of the preparation process of HGO‐C hydrogel. h,i) The photos and diagrams in emergency hemostasis and promoting wound healing in rat liver. Reproduced with permission.^{[ 177 ]} Copyright 2024, Wiley‐VCH.

Figure 12

a,b) Schematic diagram of the preparation process and SEM images of FGs. c) The photos about cells culture with FGs. Reproduced with permission.^{[ 180 ]} Copyright 2024, Wiley‐VCH. d) The preparation process of hydrogel. e,f) Illustrations of the MTJ defect process and mechanism in rats of the hydrogel. Reproduced with permission.^{[ 182 ]} Copyright 2024, American Association for the Advancement of Science. g) Schematic diagrams of the post‐bioprinting strategy and application for repair bone defects. h,i) (µCT) images of bone and blood vessels after surgery. Reproduced with permission.^{[ 183 ]} Copyright 2024, Springer Nature. j) Illustrations of IGF‐1 gels with NSCs for promoting the repair of neurons and myelin sheaths. k) The SCI model with the implantation of IGF‐1 gels and electrical signaling transmission in SC. l,m) Double immunostaining in the IGF‐1+NSC groups and tEVs Gel. Reproduced with permission.^{[ 186 ]} Copyright 2024, Wiley‐ VCH. n) The process of meniscus tears modeling and adhesives heal. o) Macrograph, H&E staining and immunofluorescence of repaired meniscus. Reproduced with permission.^{[ 187 ]} Copyright 2024, Springer Nature.

Figure 13

a,b) Fish fillet packaging experiment between control and CF‐H‐25 group at different days. Reproduced with permission.^{[ 188 ]} Copyright 2024, Elsevier. c) Diagrams of continuous water capture and directional water movement. d) Schematic diagram of condensed water collection. e) Comparative data of condensed water collection between HWTs and others. Reproduced with permission.^{[ 189 ]} Copyright 2023, Oxford University Press. f,g) Schematic of fluid‐induced techniques and short‐distance coagulation bath technique. h) The photos of fibrous hydrogels. i) SEM images of the fibrous hydrogels under different directions. j) The photos of the unidirectional water transport. Reproduced with permission.^{[ 190 ]} Copyright 2024, Springer Nature.