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Abbreviation (ISO4): Prog Chem      Editor in chief: Jincai ZHAO

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Progress in Chemistry >

2024 , Vol. 36 >Issue 6: 914 - 927

DOI: https://doi.org/10.7536/PC231002

Review

Hydrogel-Based Textile Composites

  • Wanru Guo 1 ,
  • Zheng Li , 1, 2, * ,
  • Bing Liu 3 ,
  • Jixian Gong 1 ,
  • Songnan Zhang 1 ,
  • Guobao Zheng 4
Expand
  • 1 Key Laboratory of Advanced Textile Composites of Ministry of Education, School of Textiles Science and Engineering, Tiangong University, Tianjin 300387, China
  • 2 National Innovation Center of Advanced Dyeing and Finishing Technology, Taian 271001, China
  • 3 Ningxia Shenju AG Science & Technology, Zhongwei 755000, China
  • 4 Research center of agricultural and biological technologies, Ningxia Academy of Agriculture and Forestry Sciences, Yinchuan 750002, China
* e-mail: ;

Received date: 2023-10-07

  Revised date: 2024-02-27

  Online published: 2024-07-01

Supported by

Ningxia Key Research and Development Project(2022BEG02006)

Tianjin Key Research and Development Project(20YFZCSN00130)

Central Government of Heilongjiang Province Guides Funds(ZY23CG35)

Ningxia Autonomous Region Flexible Introduction of Science and Technology Innovation Team(2021RXTDLX08)

Fold

Abstract

Hydrogel materials are widely used due to their excellent hydrophilicity,biocompatibility,adjustable biomimetic properties,etc.However,their inherent non-uniform microstructure and low-density molecular chains make their mechanical properties poor,which limits their practical applications.the preparation of hydrogel materials with high mechanical strength yet toughness has been a challenge for research in This field.As composites are constantly developing in the direction of functionalization and intelligence,the introduction of polymer hydrogels into the textile field for the preparation of gel-based textile composites not only improves the defects of gel materials,but also gives textiles excellent properties and broadens their potential application prospects.this paper reviews the research progress of hydrogel textile composites,focusing on the design strategy of hydrogel-based textile composites and their enhanced mechanical and antimicrobial properties,discusses the application progress of the composites in the fields of oil-water separation,medical dressings,wearable electronic devices,and flame-retardant protection,and the future research direction is also prospected.

Contents

1 Introduction

2 Methods to prepare hydrogel textile composites

2.1 Sol-gelatinization

2.2 Graft modification treatment

2.3 Lamination

2.4 Hydrogel fiber weaving method

3 Application of hydrogel textile composites

3.1 Oil-water separation

3.2 Medical Dressings

3.3 Wearable electronic devices

3.4 Flame retardant protective products

3.5 Others

4 Conclusion and outlook

Key words： hydrogel textiles; composite material; surface modification

Cite this article

Wanru Guo , Zheng Li , Bing Liu , Jixian Gong , Songnan Zhang , Guobao Zheng . Hydrogel-Based Textile Composites[J]. Progress in Chemistry, 2024 , 36(6) : 914 -927 . DOI: 10.7536/PC231002

1 Introduction

Hydrogel is a kind of polymer material with three-dimensional network structure,which contains a large number of hydrophilic groups such as carboxyl and hydroxyl,and can retain a large amount of water inside[1⇓~3]。 In 1960,Wichterl et al.first proposed the preparation method of hydrogel,and the First hydrogel was prepared with hydroxyethyl methacrylate as monomer and ethylene dimethacrylate as crosslinking agent[4]。 As a new type of material,hydrogel has become the preferred material for tissue engineering,soft robotics,drug delivery and other applications because of its hydrophilicity,good biocompatibility and adjustable biomimetic properties[5,6]。 However,compared with biological tissues,the inherent non-uniform microstructure and low-density polymer network of hydrogels make their mechanical properties relatively poor,which may cause problems such as fragility and fracture during processing and use,and seriously limit their application as structural materials[7]。 Therefore,the preparation of hydrogel materials with high mechanical strength and toughness has been a difficult problem to be solved[8]。
to solve this problem,researchers have adopted a variety of strategies,one of which is To introduce irreversible covalent crosslinking,Reversible physical crosslinking or stretchable network into a polymer matrix from the structural design of the hydrogel itself.reversible cross-linked structures can dissipate energy through gel deformation and reorganize upon stress relief,and covalent cross-linking can distribute stress throughout the network,maintaining the gel shape and ensuring that the original state is restored after unloading[9]。 A variety of high strength hydrogels have been prepared,including double network hydrogels,slip ring hydrogels,nanocomposite hydrogels,hydrophobic association hydrogels and polymer microsphere hydrogels[10][11,12][13][14][15,16]。 On the other hand,the hydrogel is compounded with other materials to prepare the gel-based composite material.Due to the continuous development of composite materials towards functionalization and intellectualization,nanoparticles,fibers and fabrics have also been used to construct composite hydrogel structures to enhance their mechanical properties[17]。
At present,textile reinforced hydrogels belong to a new hot direction.the composite structure was constructed by combining textile materials with Hydrogel,which provided a new idea for improving the mechanical strength of hydrogel.Hydrogel as a matrix promotes the performance of the composite,and the textile material bears the applied load and protects the structure from mechanical damage,which can improve the defects of the gel material,while endowing the textile with special properties such as ultraviolet resistance,self-cleaning,antibacterial,and flame retardancy,showing potential application prospects[18]。 in this paper,the preparation methods of hydrogel textile composites in recent years and the latest research progress in the fields of oil-water separation,medical dressings,wearable electronic devices and flame retardant protection are reviewed,the existing problems in the research of combining hydrogel with textile materials are put forward,and the future research directions are prospected(Figure 1)。
图1 水凝胶纺织复合材料的性能

Fig. 1 Properties of hydrogel textile composites

2 Preparation Strategy of Hydrogel Textile Composites

the preparation of hydrogel textile composites needs to consider the characteristics of textiles and hydrogel materials to coordinate the bonding properties between them and achieve the purpose of synergy.At present,the main methods of combining hydrogel with textiles are as follows(see Table 1):
(1)in-situ gelation of sol:hydrogel precursor solution is coated on the fabric by dipping,spraying or spin coating,and in-situ gelation is directly carried out on the fabric[19]。
(2)Graf modification treatment:adding that functional monome into the polymer,generating active free radicals on the surface of the polymer material by using light,heat,high-energy ray,initiator and the like,and initiating the grafting polymerization of the functional monomer。
(3)Lamination method:the hydrogel material is treated by a bonding and pressing process to be combined with the fabric。
(4)Hydrogel fiber weaving method:gel fibers are prepared by selecting different processing methods,and then gel textile materials are prepared by textile technologies such as non-weaving or weaving,weaving and knitting。
表1 Preparation of Hydrogel Textile Composite

Table 1 Preparation of hydrogel textile composites

Method Content Hydrogel material Other materials Ref
Sol-gel method Dip method The sol-gel immersion technique was used to enhance the nonwoven cotton by immersion in the cellulose solution to form a cellulose hydrogel/nonwoven cotton composite material. Cellulose hydrogel Cotton nonwoven 20
Wool nonwovens were immersed in an aqueous sodium alginate solution and then passed through a calcium chloride solution to form hydrogel composites. Sodium alginate Wool nonwoven 21
Soaking strategy was employed and nonwoven fabrics were introduced to preparation of the hydrogel composites. Gelatin, chitosan Polylactic acid nonwoven 22
The polyvinyl alcohol and sodium alginate mixed solution were evenly injected into the three-dimensional cotton fiber network, and the PVA-SA hydrogel was enhanced by freeze-thaw cycle and high temperature annealing. Poly (vinyl
alcohol), Na-alginate		 Cotton 23
Coating The zwitterionic hydrogel-coated cotton fabrics were prepared by stepwise coating and post-gel route. PSBMA/PVA/Borax Cotton fabric 25
Hydroxyethyl cellulose, poly(acrylic acid) Cotton fabric 26
The dihydrolipoic acid-modified sulfobetaine-derived starch hydrogel coating was covalently immobilized on the PDA/PET surface via Michael addition reaction. Sulfobetaine-derived starch The PET surface modified with PDA 27
Graft modification Chemical grafting The PET fabric surface was graft polymerized by activated acrylic acid and then soybean isolate protein hydrogel was coated on the fabric surface. Soy protein isolate PET fabric 29
Nanohydrogels were synthesized by one-step method, and SCGN nanohydrogels were grafted to the surface of cotton fabric by chemical grafting. NCO-SCG Nanohydrogel Cotton fabric 30
Light grafting Pretreatment with argon plasma, light-induced surface graft polymerization, and PNIPAAm hydrogels were grafted onto polypropylene non-woven fabrics and PET surfaces. Poly(N-isopropylacrylamide) Polypropylene non-woven, PET 33
Bifunctional groups were introduced into the PET surface by the aminolysis reaction of allylamines. The grafted polymer networks were obtained after UV-induced radical photopolymerization by varying acrylate monomer types. N-isopropylacrylamide PET fabric 34
The hydrogel with different structures were obtained by introducing resorcinol acrylic diglycidyl ester into PET surface through dip rolling and baking methods, and initiating free radical polymerization on PET fabric surface under UV light. Polyacrylamide, polyacrylic acid, poly (N-isopropylacrylamide) PET fabric 35
Plasma grafting Three low-temperature plasma gases (oxygen, nitrogen, and argon) were used to activate the surface of cotton fibers to prepare PN/CS hydrogel textiles. Poly(N-isopropylacrylamide), Chitosan Cotton fabric 36
The surface of PET fabric was modified by plasma treatment, and nano gel was synthesized by free radical polymerization to prepare composite materials. N-isopropylacrylamide PET fabric 37
The double network composite hydrogel was enhanced by plasma graft PLA fused-blown nonwoven fabric and polyethylene glycol dimaleate. Polyethylene glycol dimaleate Polylactic acid non-woven 39
Laminating A method was reported to combine hydrogels with elastomers via a glass fiber fabric interphase. Polyampholyte, Polydimethylsiloxane Glass fiber fabric 40
This study constructed a multiscale gel-fabric soft composite synergistically toughened by Pluronic/PMEA hydrogel, hydroxyapatite nanoparticles (HAP NPs) and aramid fabric. Pluronic F127 Diacrylate, Methoxyethyl acrylate Aramid fabric 41
Hydrogel fiber weaving method Nonweaving method This study selected ethanol-soluble PA as the spinning polymer and fabricate the green electrospun EPA fibrous membranes. The composite material was formed by uniformly coating the polyacrylate onto the EPA fibrous membranes. Fluorinated polyacrylate Electrostatic spun polyamide fiber membrane 48
Hydrogel composite materials based on hydroxypropyl cellulose has been produced using the nonwoven solution blown technique followed by thermal cross-linking with citric acid. Hydroxypropyl cellulose /
（nonwoven fabrics）		 50
The gelatin hydrogel nonwoven fabrics were prepared by the solution blow spinning method. Gelatin /
（nonwoven fabrics）		 51
Weaving method 3D fabric-enhanced hydrogel composite materials composed of acrylamide and sodium alginate are expected to be used for cartilage replacement. Acrylamide, sodium alginate / 52
The PVA yarn is dissolved in the fabric and transformed into cross-linked gel structure, which penetrates between yarns in the form of matrix to obtain hydrogel composites. Polyvinyl alcohol Cotton 53
regenerated cellulose fiber 56
The HOGFs were designed via a wet-spinning strategy. Owing to the good knittable feature, the HOGFs can be readily woven to adjusted 2D textiles to function. Poly(ethylene glycol) diacrylate, N-(2-hydroxyethyl) acrylamide, SA / 57
The composite fibers, Ecoflex-polyacrylamide fibers (EPFs), are created through the combination of heterogeneous elastomers and strong interfacial coupling. Acrylamide / 58
A continuous dry-wet spinning method was developed to prepare hydrogel fibers. By tuning the contents of acrylamide and N-acryloylglycinamide, the hydrogel precursor exhibits thermally reversible sol-gel transition. Acrylamide， N-acryloylglycinamide / 59
The hydrogel was compounded with an elastic polyacrylamide hydrogel to produce a hydrogel core sheath fiber, and blended with a liquid metal core sheath fiber to produce a smart fabric. Mineral hydrogel, polyacrylamide, metal fibre / 60

2.1 In situ gelation of sol

Solin situ gelation is a method of fabric surface modification,which forms a stable three-dimensional network structure(sol system)through hydrolysis or alcoholysis in The precursor solvent(inorganic salt or organic compound),and forms an inorganic or organic/inorganic hybrid coating on The surface of fibers or fabrics through gelation reaction.At present,sol in situ gelation plays an important role in the functional finishing of fabrics and the improvement of textile properties.the commonly used methods are sol-gel impregnation and coating technology.the in-situ gelation process of textile materials can be divided into five stages,namely hydrolysis,coagulation(gelation),gel aging,application,and curing,as shown in Fig.2[19]。
图2 纺织材料溶胶原位凝胶化过程的示意图[19]

Fig. 2 Schematic representation of the process of sol-gel in situ gelation of textile materials[19]

sol-gel impregnation is a method in which the fiber or fabric is directly Immersed in the hydrogel precursor solution and gelled in situ on the fabric.Ahmad et al.immersed nonwoven cotton into cellulose solution for reinforcement by Sol-gel impregnation method,and prepared cellulose-based hydrogel nonwoven composites with excellent mechanical properties[20]。 On this basis,they immersed wool nonwovens in sodium alginate aqueous solution,and then gelated in calcium chloride solution to prepare a new biodegradable sodium alginate hydrogel and wool nonwovens composite[21]。 Compared with pure wool nonwovens,the tensile strength and permeability of hydrogel nonwovens are significantly improved.In addition,Wang et al.Used the impregnation method,selected chitosan and gelatin to prepare hydrogel composite,and introduced polylactic acid non-woven fabric as the supporting skeleton[22]。 the hydrogel and the non-woven fabric are entangled with each other through citric acid ion crosslinking,so that the stress in the system is uniformly dispersed,and the mechanical properties of the natural polymer hydrogel are improved.Zhang et al.Immersed cotton fabric in a mixed solution of polyvinyl alcohol(PVA)and sodium alginate(SA),and obtained cotton fabric-reinforced PVA-SA hydrogel through freeze-thaw cycles and high temperature annealing.the mechanical properties of the material were significantly better than those of pure cotton fabric or PVA gel(Fig.3)[23]。
图3 棉织物增强物理交联PVA-SA水凝胶的制备[23]

Fig. 3 The preparation of physically cross-linked PVA-SA hydrogels with cotton fabric reinforced[23]

Sol-gel coating technology is a technology in which the prepared hydrogel precursor solution is evenly coated on the surface of the fabric,and a colloidal layer with specific functions is formed on the fabric by crosslinking methods such as radiation or adding crosslinking agents[24]。 According to the properties of zwitterionic hydrogel,Liu et al.Uniformly coated the prepared polymethacrylic acid sulfobetaine-hydroxyethyl acrylate/polyvinyl alcohol/borax hydrogel polymer precursor solution on the surface of cotton fabric.Then the cotton fabric coated with zwitterionic gel was prepared by freeze-thaw cycle treatment,crosslinking to form dynamic boric acid ester bonds,and step-by-step coating-gelation[25]。 on this basis,they used the same method to polymerize hydroxyethyl cellulose and polyacrylic acid in situ to obtain a cellulose-based hydrogel(AHCH),and used a screen printing device to uniformly coat the gel precursor solution On cotton fabrics to prepare hydrogel-based textile(AHCH@CF)composites with good mechanical properties[26]。 Yao et al.Deposited polydopamine(PDA)on polyethylene terephthalate(PET)surface(PDA/PET)and developed a dihydrolipoic acid modified sulfobetaine-derived starch(SB-ST-D)hydrogel coating[27]。 SB-ST-D was covalently immobilized on the PDA/PET surface by Michael addition reaction to form a disulfide bond to obtain the hydrogel textile composite。

2.2 Graft modification treatment

At present,the commonly used methods of surface grafting modification of materials mainly include chemical grafting,ultraviolet light induced grafting,plasma induced grafting and so on。

2.2.1 Chemical grafting

chemical grafting refers to the use of Chemical modification to graft functional groups onto fibers or fabrics,so that the modified fabrics form active sites that are conducive to the combination of hydrogels,giving fibers and textiles special properties[28]。 Norouzi et al.Grafted activated acrylic acid(AA)onto the surface of PET fabric,and then coated soy protein isolate(SPI)hydrogel on the surface of the fabric.the hydrogel and the modified PET fabric surface formed covalent bonds,which improved the connection between the fabric and the hydrogel[29]。 Han et al.Synthesized SCG nanogels by one-step polymerization of styrene(St),polycaprolactone-hydroxyethyl methacrylate(PCL-HEMA)and polyhexamethylene guanidine hydrochloride(M-PHGC)monomers using free radical polymerization.The NCO-SCG nanogel was modified by isocyanate and grafted onto The surface of cotton fabric by chemical grafting.The finished antibacterial fabric had good antibacterial and thermal stability(Figure 4)[30]。
图4 制备NCO-SCG纳米凝胶及化学接枝法制备凝胶织物过程示意图[30]

Fig. 4 Schematic diagram of the process of preparing NCO-SCG nanogels and chemical grafting[30]

2.2.2 Ultraviolet light grafting

ultraviolet grafting method mainly uses Ultraviolet irradiation to produce free radicals on the surface of polymers to initiate free radical graft copolymerization[31]。 this method is cheap and the product is pure,but there are few reports on the preparation of gel textiles by This method[32]。 Chen et al.Grafted poly(N-isopropylacrylamide)(PNIPAAm)hydrogel onto polypropylene non-woven fabrics by argon plasma pretreatment and UV-induced surface graft polymerization[33]。 Recently,PNIPAAm hydrogel-modified PET textiles have also been prepared.Lorusso et al.Covalently bonded allylamine to the PET surface through ammonolysis reaction,and then obtained a graft polymer network after UV-induced radical polymerization,and successfully grafted PNIPAAm hydrogel to the carboxylated PET fabric surface(Figure 5)[34]。 In contrast,Dai et al.used a simple padding and baking method to modify resorcinol diglycidyl acrylate(RDA)onto the surface of PET fabrics,and induced free radical polymerization of different acrylate monomers by ultraviolet light.Three hydrogel layers with different structures were obtained,namely polyacrylamide(PAAM),polyacrylic acid(PAAC)and PNIPAAM,indicating that the UV grafting method can be Used to obtain hydrogel layers on the surface of PET fabrics[35]。
图5 利用紫外光辐射将水凝胶固定在PET织物上的合成路线图[34]

Fig. 5 Roadmap for the synthesis of hydrogel fixation to the PET fabric using UV radiation[34]

2.2.3 Plasma grafting

plasma grafting method can produce various active groups on the surface of fibers through plasma,so that the grafting monomer can be more easily introduced into the surface of materials to realize the functionalization of textile materials.At present,it is often Used to increase the chemical reactivity of the fiber surface,enhance the adhesion between the coating and the polymer matrix,and improve the hydrophilicity of the material.Tourrette et al.used three low-temperature plasma gases(oxygen,nitrogen,and argon)to modify the surface of cotton fibers,increase the number of functional groups on the surface of the fibers,and increase the roughness of the fibers by etching,resulting in increased contact between the fibers and the microgel particles,thereby enhancing the attachment of PNIPAAm/chitosan hydrogel(PN/CS)to the fabric surface[36]。 In order to maximize the deposition of hydrogel on the fabric while maintaining its pH responsiveness,Štular et al.Selected two plasma gases,ammonia and oxygen,to modify the surface of PET fabric by plasma[37]。 Oxygen plasma can be used to increase the surface energy of polymers and achieve coating deposition on various polymer materials,while ammonia plasma can achieve amino functionalization and weak etching of polymers to achieve pH-responsive effect[38]。 Li et al.Combined the advantages of nonwoven materials,used plasma grafted polylactic acid melt-blown fabric and polyethylene glycol dimaleate to reinforce the composite hydrogel,and constructed the interpenetrating hydrogel composite nonwoven fabric structure[39]。

2.3 Laminating method

Lamination refers to the process of bonding and pressing fabrics with functional films to make them into composite materials with specific functions.Hubbard et al.Developed a composite material in which glass fiber(GF)fabric was used as the interface to physically combine polyampholyte hydrogel(PA)with elastomer(PDMS)[40]。 Due to the interaction between the GF fabric and the soft laminate,the strong bonding of different materials can be achieved without chemical treatment,and the mechanical properties of the composite can be greatly improved.This method can also be used to prepare a variety of gel composites with adjustable mechanical properties.Li et al.Dissolved polyether F127 diacrylate(F127DA)in aqueous solution to form polymer micelles,and at the same time,hydroxyapatite nanoparticles and methoxyethyl acrylate(PMEA)were copolymerized in situ to prepare a nano-hydrogel with double crosslinking of polymer micelles and nanoparticles[41]。 the hydrogel was laminated onto aramid fabric,and the hydrogel fabric composite with good toughness and puncture resistance was developed by using the gel-fabric synergistic toughening mechanism。

2.4 Hydrogel fiber weaving

the development of polymer and textile technology has provided a variety of options For the preparation of hydrogel textile composites.hydrogel fibers can be prepared by selecting suitable processing or modification methods and further processed into gel textiles.for example,the fiber membrane is directly spun by an electrospinning method,or the hydrogel fiber is prepared by wet spinning,dry spinning and the like,and then the hydrogel textile composite material is prepared by combining the existing textile technologies such as weaving,weaving,knitting or non-weaving and the like[42]。 At present,the preparation process of common gel fibers is shown in Table 2[43]。
表2 Common gel fiber manufacturing technology[43]

Table 2 Common gel fiber manufacturing techniques[43]

Setup Concept Ref
Electro-spinning The polymer dissolved in an appropriate solvent is injected by a needle towards a collection plate. Due to the high applied electric field, potential difference generated between the syringe and the plate, the polymer is attracted by the collecting plate, and the polymer solution is converted into nanofibers. 44
Wet-Spinning The polymer is dissolved in an appropriate solvent and later injected through a fiery into a coagulation bath containing a non-solvent liquid. In the coagulation bath, continuous polymerization of the filaments occurs. After the formation of the fibers, they are extracted from the coagulation bath by means of rollers-induced capture. 45
Melt-Spinning The solid polymer is heated above its melting point within the extruder and is then expelled through a die, solidifying on cooling. In a pick-up, the fibers are then recovered and mechanically stretched. 46
Dry-Spinning The polymer is dissolved in a suitable solvent. The initial solution is injected through the spinneret and through a heating column that causes the solvent to evaporate. Consequently, the polymer solidifies, and dry fibers are attained. 47

2.4.1 Nonwoven process

Since the 1990s,electrospinning has become one of the most direct and effective methods for the preparation of nanogel fibers.At present,the mechanical properties of electrospun membranes made from biopolymers such as gelatin,hyaluronic acid and silk fibroin are poor,and the mechanical properties can be improved by promoting the reaction of related groups in the fibers through chemical crosslinking and other methods.Zhou et al.Selected alcohol-soluble polyamide(EPA)as the spinning polymer to prepare amphiphilic polyamide fiber membranes by electrospinning and impregnation techniques[48]。 At the same time,fluorine-containing polyacrylate(WFPA)was uniformly coated on the surface of EPA fiber,so that the fiber membrane had an excellent bonding structure(Fig.6)。
图6 （a）智能纤维膜制造程序示意图；（b）纤维膜性能示意图[48]

Fig. 6 (a) Schematic diagram of smart fiber membrane manufacturing process; (b) Schematic diagram of fiber membrane performance[48]

Compared with electrospinning,solution blow molding combines the scalability of melt blowing and the versatility of electrospinning,and the structure and properties of the prepared gel fibers are significantly improved,and the cost is also greatly reduced[49]。 Yang et al.First proposed the development of a super-porous hydroxypropyl cellulose(HPC)hydrogel textile material using non-woven solution blow molding technology[50]。 Nonwoven fibers were thermally crosslinked with citric acid,and a more stable structure was obtained by forming a crosslinked ester bond between the hydroxyl group in HPC and the carboxylic acid group in the crosslinking agent.in addition,Nakamura et al.Prepared a gelatin hydrogel non-woven fabric(GHNF)by solution blow spinning through a high-speed air nozzle pump,and applied it as a carrier film in a multilayer cell sheet[51]。

2.4.2 Weaving Technology

weaving technology refers to the forming process of interweaving two or more yarns into a whole fabric structure according to certain rules.Currently,three-dimensional braiding patterns have been developed with this method to reinforce hydrogel matrices.Arjmandi et al.Mixed the hydrogel precursor solution with N,N'-methylenebisacrylamide,completed gelation during fabric Weaving,and prepared a three-dimensional fabric reinforced hydrogel composite composed of acrylamide and sodium alginate,which improved the load capacity of the fabric and the wear resistance of the hydrogel matrix[52]。 For the first time,Koc et al.prepared a fabric reinforced hydrogel structure by one-step weaving process.with PVA yarn and cotton as warp yarns and pure PVA yarn as weft yarns,the Prepared PVA/cotton fabric was treated With borax solution to obtain PVA/cotton woven fabric[53]。 PVA can be dissolved in the fabric and converted into a crosslinked gel structure,which penetrates into the yarn in the form of a matrix,thus obtaining a cotton yarn reinforced composite hydrogel material with significantly improved tensile properties[54,55]。 On this basis,they mixed PVA fibers with regenerated cellulose fibers(Fig.7),and prepared fabric reinforced hydrogel composites with PVA and viscose as materials,and the mechanical properties of the hydrogel were significantly improved[56]。
图7 （a）纤维增强水凝胶复合材料制备；（b）粘胶织物和粘胶织物增强水凝胶复合材料的扫描电镜图[56]

Fig. 7 (a) A Schematic representation of the preparation of the fiber-reinforced hydrogel composites; (b) Scanning electron micrographs of viscose fabric and viscose fabric reinforced hydrogel composites[56]

Zhang et al.Prepared hygroscopic organogel fibers(HOGFs)using a wet-spinning process and a solvent displacement strategy,which can be woven into a two-dimensional hygroscopic device for atmospheric water collection[57]。 At present,composite gel fibers can usually achieve stretchability and designability,but fatigue and hysteresis are still difficult to solve.Li et al.Selected PAAm as a model heterogeneous material to prepare an arterial-like heterogeneous layered structure(HHS)by wet spinning,and added an initiator benzophenone to connect the two polymer networks into a whole.Conductive,highly elastic and anti-fatigue hydrogel-elastic composite fibers can be produced continuously,which can be woven into fabrics and applied to wearable devices[58]。 the rapid development of gel fibers has put forward higher requirements for The mechanical properties of fibers.Shuai et al.Reported a continuous dry-wet spinning method to prepare stretchable,conductive and self-healing hydrogel fibers[59]。 By adjusting the content of acrylamide(AAm)and N-acryloylglycinamide(NAGA),the hydrogel precursor exhibited a thermoreversible sol-gel transition,ensuring the success of the spinning process。
Wu et al.Reported a novel thermally stiffened mineral hydrogel material through entropy-mediated polymer-cluster interaction,and the hydrogel was compounded with elastic polyacrylamide hydrogel to prepare hydrogel core-sheath fibers with high tensile strength,high resilience,and thermal stiffability[60]。 When it is mixed with liquid metal core-sheath fiber,the soft and hard States of the fabric can be quickly switched(Fig.8)。
图8 熵驱动热致硬化水凝胶及智能织物[60]

Fig. 8 Entropy-driven thermosetting hydrogels and smart fabrics[60]

3 Application of Hydrogel Textile Composites

Hydrogel textile composite is an ideal polymer composite with good mechanical properties,superhydrophobicity,antibacterial and flame retardancy.Hydrogels synthesized with long chains or monomers containing specific groups can respond to different temperature,pH and electric field environments,and can be used in many fields such as oil-water separation,medical dressings,smart wearable electronic devices and flame retardant protective products(see Table 3)。
表3 Related Applications of Hydrogel Textile Composites

Table 3 The application of hydrogel textile composites

Researcher Content Application Ref
Liu The zwitterionic hydrogel-coated cotton fabrics were prepared by stepwise coating and post-gel route. Oil-water separation 25
Liu A novel Ag/AgCl nanoparticles hybrid cellulose-based hydrogel (AHCH) was successfully prepared, it was coated on a piece of cotton fabric through the facile sol-gel coating method. Oil-water separation 26
You A natural polymer-based hydrogel prepared by konjac glucomannan was coated on glass fabric. Oil-water separation 63
Cai The method of a super hydrophilic fabric composed of basalt fiber and KGM was reported. The composite shows stable super hydrophobic property in water. Oil-water separation 70
Dai A guar gum self-assembled hydrogel for oil-water separation was prepared and coated on cotton fabric by coating method. Oil-water separation 71
Türkoğlu A hydrogel dressing supported by regenerated cellulose non-woven fabric was developed, which has the characteristics of rapid and effective treatment of high swelling wounds. Wound dressing 80
Benltoufa Chitosan hydrogel has been synthetized and applied on cellulosic fabric to impart antimicrobial behavior. It is suitable for medical, surgical and transdermal treatment applications. Wound dressing 81
Ahmad The study fabricated cellulose hydrogel using the sol-gel technique and reinforced it with nonwoven cotton for sustainable wound dressing application. Wound dressing 20
Wang The sandwich-like composite hydrogel wound dressings were developed by intercalating nonwoven fabrics as the middle layer, gelatin and chitosan hydrogel loaded with Centella asiatica as the base materials. Wound dressing 22
Xu A touch sensing fabric system composed of non-woven cellulose fabric was proposed, wearable electronics 87
Kang A flexible and stretchable supercapacitor was assembled by direct interfacial gelation of reduced graphene oxide with carbon nanotubes on a stretchable fabric surface. wearable electronics 88
Xu A breathable paper-cut ionic e-textile with two functions of sensing (touch and strain) was designed by integrating silk fabric and paper-cut ionic hydrogel. wearable electronics 89
Song A designed hybrid crosslinking strategy continuously wet-spins hydrogel fibers, which are transformed into organohydrogel fibers by simple solvent replacement. wearable electronics 90
Li The composite fibers, Ecoflex-polyacrylamide fibers (EPFs), are created through the combination of heterogeneous elastomers and strong interfacial coupling. wearable electronics 58
Illeperuma A new flame retardant material was developed by laminating hydrogel and fabric. flame-resistant dress 96
Yu Hydrogel fabric laminate was developed by using a thermal laminate-sensitive PNIPAAm/SA hydrogel on the surface of the cotton fabric. flame-resistant dress 97
A PNIPAAm/SA/PVA composite hydrogel fabric laminate with high strength and antibacterial properties was prepared by adding PVA as the main component of the hydrogel. flame-resistant dress 92
Nie PAAM/SiO2 nanocomposite hydrogel was filled into the fabric to form a semi interpenetrating structure at the interface, and flame retardant gel/textile composites were prepared. flame-resistant dress 98
Qiu A bullet-proof bicontinuous hydrogel (BH)/ultrahigh-molecular weight polyethylene fabric (UPF) composite was reported. flexible protective materials 101
Li HAP NPs were copolymerized in situ with elastomeric monomers to form hydrogels and the optimal angle was selected to laminate the aramid fabrics. flexible protective materials 41
Li The double-network composite hydrogel is reinforced by plasma grafted polylactic acid
melt-blown non-woven fabric and polyethylene glycol dimaleate.		 Adsorption 39
Zhou a novel Janus photothermal hydrogel-fabric was developed by firmly formatting surface hydrophobized porous photothermal hydrogel on a commercial cotton fabric in large area. seawater desalination 105

3.1 Oil-water separation

Oil-water separation technology is an effective wastewater treatment technology based on special wettable materials[61⇓~63]。 In recent years,hydrogel materials with superhydrophilicity and superoleophobicity have attracted much attention[64]。 Zwitterionic hydrogels have been widely used in the field of oil-water separation due to the presence of both cationic and anionic groups in the molecular chain,which can remain stable in harsh environments[65,66]。 Zhu et al.Prepared a zwitterionic nanohydrogel-grafted polyvinylidene fluoride(PVDF)microfiltration membrane by surface grafting method.Due to the presence of zwitterions,the membrane showed excellent fouling resistance for oil-in-water emulsion separation,and the permeate flux recovery was close to 100%after many cycles of oil-in-water emulsion filtration[67]。 Liu et al.Developed a poly(methacrylic acid sulfobetaine-hydroxyethyl acrylate/polyvinyl alcohol/borax)zwitterionic hydrogel-coated cotton fabric with excellent underwater superoleophobicity and excellent stain resistance[25]。 The hydrogel textile exhibited excellent oil-water separation efficiency even after 50 consecutive cycles.However,these hydrogels for oil-water separation are all synthetic polymers,which are difficult to degrade[68]。 on the basis of this study,they successfully prepared a new nanoparticle hybrid hydrogel using biocompatible cellulose,which was coated On a cotton fabric(AHCH@CF)by a simple in-situ gelation method[26]。 For various oil-water mixtures,it exhibits an excellent oil-water separation function with a separation efficiency of about 99.5%and a water flux up to about 15 246 L-1·m-2·h-1.After 50 cycles,the separation efficiency can still be maintained above 99.0%,providing a new candidate for efficient and durable oil-water separation applications.Konjac glucomannan(KGM)has good film-forming and biocompatibility.You et al.Directly coated the natural polymer hydrogel prepared by KGM on the glass fiber fabric of engineering materials without other chemical reagents[69][63]。 the Developed hydrogel textile composite not only has good oil-water separation property,but also can remove organic dyes and heavy metals in water during The separation process.Cai et al.developed a preparation method of super-hydrophilic fabric composed of basalt fiber(BF)and KGM[70]。 KGM was deacetylated under alkaline conditions to form hydrogel(DA-KGM),which could form a coating on BF fabric.the material has super-hydrophilicity and super-oleophobicity even in alkali,acid and organic solution,and is expected to be used in harsh environments.in addition,Dai et al.Prepared a guar gum self-assembled hydrogel for oil-water separation by coating cotton fabric with guar gum solution,immersed in sodium periodate,and induced the gelation of guar gum through the regioselective oxidation of sodium periodate[71]。 the results showed that the hydrogel-coated cotton fabric could selectively separate different oily wastewater,and the separation efficiency of silicone oil,rapeseed oil and cyclohexane was 98.11%,97.53%and 99.47%,respectively。

3.2 Medical dressing

Medical dressings can avoid the action of bacteria and microorganisms and accelerate wound healing.A variety of dressings have been developed to promote wound repair,including traditional gauze and bandages,as well as newly developed nanofibers,foams,and hydrogels[72⇓~74]。 Hydrogels have become the most competitive candidates because of their good drug delivery ability and high porosity[75,76]。 Current hydrogel dressings are mostly poorly breathable films,which may cause inflammation after prolonged wear.Compared with other forms of dressings,textiles have excellent extensibility and compressive cushioning capacity,which can better withstand the deformation and tension of the skin.Therefore,the combination of hydrogel and textile fabrics can overcome the shortcomings of traditional dressings[77]。 Hydrogels prepared from natural polymer materials,such as sodium alginate,gelatin and chitosan,have been widely used in the field of medical dressings[78,79]。 T Türkoğlu et al.Developed a hydrogel dressing supported by a regenerated cellulose non-woven fabric[80]。 chitosan and sodium alginate were crosslinked with polyethylene glycol to form hydrogels on nonwovens.the prepared material has The characteristics of rapid and effective treatment of swollen wounds,and can be used as an absorption layer of a multilayer composite dressing to promote wound healing.Benltoufa et al.Deposited Chitosan hydrogels on cotton fabrics functionalized by cationic and anionic groups to inhibit bacterial growth while maintaining basic physical and mechanical properties[81]。 nonwoven fabrics are one of the best support materials for textile-based hydrogel wound dressings due to their excellent absorption properties and porosity.Ahmad et al.Immersed nonwoven cotton in cellulose solution to prepare hydrogel nonwoven cotton composites with good water absorption and air permeability[20]。 At that same time,titanium dioxide particle are loaded,so that the antibacterial property is obtain,and the application of the wound dressing is realized.The liquid absorption capacity of the cellulose-based hydrogel non-woven fabric composite was significantly improved compared with that of pure cotton non-woven fabric.In addition,Wang et al.Introduced chitosan and gelatin into polylactic acid non-woven fabrics to prepare a sandwich-type composite hydrogel wound dressing with high mechanical properties,water absorption and water vapor transmission rate（3419±197 g∙m-2∙d-1）,and good drug sustained-release performance(release time 216 H,maximum cumulative release up to 74% )[22]。 Therefore,the combination of hydrogels and textiles can improve the mechanical properties of hydrogels,reduce the adhesive properties of fabrics,and enhance the drug delivery properties of composites,which has great potential in wound healing and drug release[43]。

3.3 Wearable electronic device

In recent years,a variety of smart wearable electronic devices,especially human-computer interaction systems,real-time health monitoring devices,and highly flexible displays,have made tremendous progress[82,83]。 These electronic devices require flexibility,excellent stretchability,and the ability to remain stable under significant deformation[84,85]。 Hydrogels with high ionic conductivity have a variety of additional functions and can be applied in various extreme working environments to prepare ultra-flexible textiles[86]。 Xu et al.Used non-woven cellulose fabric to wrap conductive polyacrylamide-lithium chloride(PAAM-LiCl)hydrogel to assemble an ultra-thin(1 mm)sandwich touch sensing fabric[87]。 the material exhibits low detection threshold(50 Pa),high endurance(100 kshots),and extremely high touch localization accuracy.They also integrated touch-sensitive fabrics into clothing and Developed an intelligent touch-sensitive glove,which can realize human-computer interaction such as remote command.Kang et al.developed a flexible and stretchable supercapacitor by direct in-situ gelation of reduced graphene oxide(rGO)with carbon nanotubes(CNTs)on The surface of stretchable fabric[88]。 the formed CNT-rGO gel composite has a porous structure that achieves excellent electrolyte accessibility,maintaining a high capacity of 90.0%even at up to 50%strain.However,the lack of breathability of most wearable electronic devices hinders their application in real life.Xu et al.Designed a hydrogel electronic textile by combining silk fabric and paper-cut ionic hydrogel,which can accurately perform the functions of touch sensing and strain sensing.It has excellent response time(3 ms),large working strain range(>100%)and long-term stability(>10 000 cycles),which breaks through the bottleneck of traditional wearable ionic electronic devices and has broad application prospects in future wearable skin electronic products[89]。
fiber-based electronic devices have many advantages over traditional thin film electronic devices.Their good weavability allows them to be woven into various 3D shapes to adapt to irregular surfaces.Integrating them into textiles can detect strains in different directions.Song et al.Prepared a new type of organic hydrogel conductive fiber,using alginate and end-functionalized polyethylene glycol(PEG)prepolymer as raw materials to construct a double network and realize the continuous spinning process of hydrogel fiber(Fig.9)[90]。 the obtained organic hydrogel fiber can work at-80 deg C,can be stably stored in the natural environment for a long time,and shows excellent elasticity and negligible hysteresis in the process of cyclic loading and unloading,which is difficult to achieve by the traditional conductive fiber.Li et al.Prepared conductive,highly elastic and anti-fatigue hydrogel-elastomer composite fibers for continuous production through the heterogeneous layered structure of bionic arteries[58]。 The designed fiber can be stretched to 500%,has a conductivity of 3.2 mS/cm,and has no hysteresis or fatigue after 10,000 loading cycles。
图9 有机水凝胶纤维的设计和制造。（a）有机水凝胶纤维中交联聚合物网络的分子设计以及水凝胶纤维的湿纺过程和分子演化示意图；（b）水凝胶纤维通过置换溶剂制备为有机水凝胶纤维的化学过程；（c）在连续卷筒线轴上收集的单根长纤维的照片；（d）有机水凝胶纤维针织物的示意图和照片[90]

Fig.9 Design and fabrication of organohydrogel fibers. (a) Molecular design of hybrid crosslinked polymeric network in organohydrogel fibers and schematic of the wet-spinning process and molecular evolution of hydrogel fibers. (b) Schematic of the preparation of organohydrogel fibers from hydrogel fibers by displacement solvent. (c) Photograph of a long single fiber collected on a continuously winding drum spool. (d) Schematic and photograph of an organohydrogel-fiber knitted textile [90]

3.4 Flame retardant protective article

Fires caused by natural and human activities occur frequently every year,and lightweight and effective personal protective equipment,such as fire-retardant textiles such as fire-resistant blankets,clothing and heat-resistant gloves,are particularly important,but fire-resistant fabrics are expensive and cannot be widely used[91]。 Hydrogel can be used as a phase change agent to promote evaporation,absorb heat and cool temperature,and form a fireproof layer on the surface of the fabric to achieve the effect of flame retardancy[92,93]。 PNIPAAm is a thermosensitive polymer with a low critical solution temperature(32℃).When the temperature exceeds the critical solution temperature,the synthesized hydrogel can rapidly release water through thermal response shrinkage[94,95]。 Illeperuma et al.Prepared a flame-retardant composite fabric laminate,using SA and PNIPAAm as raw materials to synthesize hydrogel under ultraviolet irradiation,and laminated it on aramid fabric as flame-retardant protective equipment[96]。 The water retention ability of hydrogel is another key factor for refractories,which can not play a role when the internal water evaporates.To solve this problem,Yu et al.Developed a new type of hydrogel fabric laminate by laminating heat-sensitive PNIPAAm/SA hydrogel on the surface of cotton fabric,and incorporated CaCl2into the composite hydrogel to improve the water retention performance of the fireproof hydrogel[97]。 the results showed that the presence of hydratable salt successfully prolonged the water retention time of the hydrogel,and the hydrogel fabric laminate could not burn for 30 min at 1 200℃.However,the poor mechanical properties of hydrogel is a major defect that limits its use as a flame retardant material.On the basis of this study,they added PVA hydrogel to prepare a PNIPAAm/SA/PVA composite hydrogel fabric laminate with high strength[92]。 The strong hydrogen bonding between PNIPAAm,SA and PVA and the interpenetrating polymer network(IPN)structure formed between them endow the hydrogel with excellent mechanical properties,which has great potential in the field of flame retardant protective clothing.Nie et al.Developed a simple casting method to fill the PAAM/SiO2nanocomposite hydrogel into the fabric to form a semi-interpenetrating structure at the interface to prepare the flame retardant gel/textile composite(FR-GT),and the interfacial toughness reached 272 J/m2[98]。 Due to the evaporation and heat dissipation of water,even in a high temperature environment,the hydrogel can continuously maintain the form until the water is completely evaporated,thereby achieving the flame retardant effect。

3.5 Other

Flexible protective material is a hot research topic in the field of protection in recent years.Most of the existing protective materials are laminated by aramid or ultra-high molecular weight polyethylene fabrics,which greatly increases the thickness and bending strength of the composite material,and limits the flexibility and comfort of the wearer to a certain extent[99,100]。 Therefore,there is an urgent need to design and prepare a flexible protective material that has excellent protective ability and is comfortable and lightweight.Qiu et al.Prepared bicontinuous hydrogels(BH)with a polymer hard phase and a polymer soft phase by tuning the hydrogen-bonding interactions of the polymer chains[101]。 A hydrogel/high performance fabric flexible protective material(BH-UPF)was developed by compounding BH with hydrophilic modified ultra-high molecular weight polyethylene fabric(UPF).the BH-UPF can stop a bullet with a mass of 2.8 G and an impact velocity of about 300 m/s.Compared with pure UHMWPE fabric with the same areal density,BH-UPF has a 69%reduction in the depth of bulge deformation,which has a certain application potential in the field of flexible protection.Li et al.Proposed a design strategy of soft composites by taking advantage of the bonding interface between high-performance fiber materials and high-strength gel,and prepared gel-fabric synergistic toughened and self-healing soft stab-resistant composites[41]。 the puncture resistance,burst resistance and tear resistance of the composite are 15 times,18 times and 42 times of those of the pure aramid fabric,respectively,and the maximum load of the composite is much higher than the sum of the maximum loads of the pure aramid fabric and the pure water gel,which provides a simple and effective method for constructing materials with high toughness and excellent puncture resistance。
Fiber or Fabric composite hydrogel materials have also been used in the field of heavy metal adsorption.fabric has the advantages of large specific surface area and high porosity,which can improve the adsorption efficiency and adsorption capacity while solving the defects of low strength and difficult regeneration of hydrogel adsorption materials.Li et al.Combined the advantages of non-woven materials,plasma treated non-woven fabrics were used as the skeleton and hydrogel to prepare a hydrogel composite adsorption material with high adsorption rate and stable structure.the adsorption rates of the composite for Pb(Ⅱ)and Ni(Ⅱ)were increased by 25%and 33%,respectively,and the maximum adsorption capacities were 416.07 mg/G and 243.10 mg/G,respectively.After five times of adsorption-desorption,the adsorption efficiency was still 90%,which was of great significance for the treatment of heavy metal ions[39]。
Fabric-based photothermal conversion materials have excellent mechanical strength and flexibility,which can be used to prepare and assemble various efficient photothermal evaporation devices with two-dimensional or three-dimensional special structures,but there is a theoretical limit to their evaporation rate[102]。 Researchers have found that photohydrogels have a strong water activation effect,which can effectively reduce the enthalpy of evaporation of water[103,104]。 Zhou et al.Formed a porous hydrogel layer composed of biomass-derived graphene(BDG)and polyvinyl alcohol(PVA)on cotton cloth by brushing,ternary crosslinking,freezing ice dissolution and other methods.Combining the excellent mechanical properties of fabric-type photothermal materials and the activated water effect of photothermal hydrogel,a large area hydrogel-fabric coupling evaporator was designed,which significantly reduced the enthalpy of water evaporation to 1980 kJ/m2[105]。 Furthermore,a thin layer of polydimethylsiloxane(PDMS)was sprayed on the hydrogel surface of the evaporator to endow the surface with hydrophobicity,and the Janus structure was constructed.the design breaks through the performance limit of planar photothermal materials in the solar evaporation process and obtains long-term stable evaporation performance,which is expected to promote the application of solar evaporation technology in seawater desalination and wastewater treatment。

4 Conclusion and prospect

in this paper,the preparation strategies and applications of hydrogel-based textile composites are reviewed.hydrogel-based textile composites coordinate the advantages of the two materials through different bonding strategies,and synthesize a new class of multifunctional composites(high strength,high toughness,antibacterial,anti-ultraviolet,flame retardant and self-cleaning,etc.),which provides a new idea for the development of hydrogels and textiles.However,there are still some problems to be solved in the research of hydrogel textile composites:(1)Due to the structural differences between hydrogel and textile,How to improve the binding fastness is still a difficult point in the preparation of the composites.(2)How to combine the function and intelligent characteristics of hydrogel with textiles to derive new functional and intelligent gel textile composites is the future development direction.(3)How to achieve the high tensile and self-healing properties of hydrogel smart textiles at the same time is an urgent problem to be solved in the future.(4)the simplification and industrialization of the synthesis method of hydrogel-based textile composites need to be further explored。

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