Structural Strategies for Supramolecular Hydrogels and Their Applications

Supramolecular structures are of great interest due to their applicability in various scientific and industrial fields. The sensible definition of supramolecular molecules is being set by investigators who, because of the different sensitivities of their methods and observational timescales, may have different views on as to what constitutes these supramolecular structures. Furthermore, diverse polymers have been found to offer unique avenues for multifunctional systems with properties in industrial medicine applications. Aspects of this review provide different conceptual strategies to address the molecular design, properties, and potential applications of self-assembly materials and the use of metal coordination as a feasible and useful strategy for constructing complex supramolecular structures. This review also addresses systems that are based on hydrogel chemistry and the enormous opportunities to design specific structures for applications that demand enormous specificity. According to the current research status on supramolecular hydrogels, the central ideas in the present review are classic topics that, however, are and will be of great importance, especially the hydrogels that have substantial potential applications in drug delivery systems, ophthalmic products, adhesive hydrogels, and electrically conductive hydrogels. The potential interest shown in the technology involving supramolecular hydrogels is clear from what we can retrieve from the Web of Science.

[1]  C. Jandl,et al.  Enzyme-like polyene cyclizations catalyzed by dynamic, self-assembled, supramolecular fluoro alcohol-amine clusters , 2023, Nature Communications.

[2]  P. Rudolf,et al.  Nearly-freestanding supramolecular assembly with tunable structural properties , 2023, Scientific Reports.

[3]  O. B. Usta,et al.  Supramolecular hybrid hydrogels as rapidly on-demand dissoluble, self-healing, and biocompatible burn dressings. , 2022, Bioactive materials.

[4]  A. Demchenko Introduction to Fluorescence Sensing: Volume 2: Target Recognition and Imaging , 2023 .

[5]  E. Scavetta,et al.  Micro- and nano-devices for electrochemical sensing , 2022, Microchimica Acta.

[6]  A. Papagiannopoulos,et al.  Physicochemical properties of electrostatically crosslinked carrageenan/chitosan hydrogels and carrageenan/chitosan/Laponite nanocomposite hydrogels. , 2022, International journal of biological macromolecules.

[7]  R. Janssen,et al.  Determinant Role of Solution‐State Supramolecular Assembly in Molecular Orientation of Conjugated Polymer Films , 2022, Advanced Functional Materials.

[8]  Xuanhe Zhao,et al.  Hydrogel interfaces for merging humans and machines , 2022, Nature Reviews Materials.

[9]  R. Martins,et al.  Carbon-Yarn-Based Supercapacitors with In Situ Regenerated Cellulose Hydrogel for Sustainable Wearable Electronics , 2022, ACS applied energy materials.

[10]  Sajjad Rahmani Dabbagh,et al.  3D-printed microrobots from design to translation , 2022, Nature Communications.

[11]  Sanghyuk Yoon,et al.  A Nanoporous Carbon‐MXene Heterostructured Nanocomposite‐Based Epidermal Patch for Real‐Time Biopotentials and Sweat Glucose Monitoring , 2022, Advanced Functional Materials.

[12]  S. Salmon,et al.  Advances in 3D Gel Printing for Enzyme Immobilization , 2022, Gels.

[13]  X. Guan,et al.  2D MXene Nanomaterials: Synthesis, Mechanism, and Multifunctional Applications in Microwave Absorption , 2022, Small Structures.

[14]  Y. Wen,et al.  Janus Mucosal Dressing with a Tough and Adhesive Hydrogel based on Synergistic Effects of Gelatin, Polydopamine, and Nano-clay. , 2022, Acta biomaterialia.

[15]  A. Poater,et al.  pH-Responsive Gelation in Metallo-Supramolecular Polymers Based on the Protic Pyridinedicarboxamide Ligand , 2022, Chemistry of Materials.

[16]  N. Heshmati,et al.  The Application of Clay-Based Nanocomposite Hydrogels in Wound Healing , 2022, Arabian Journal for Science and Engineering.

[17]  A. Borovik,et al.  Artificial Metalloproteins: At the Interface between Biology and Chemistry , 2022, JACS Au.

[18]  Carmen J Gil,et al.  Tissue engineered drug delivery vehicles: Methods to monitor and regulate the release behavior. , 2022, Journal of controlled release : official journal of the Controlled Release Society.

[19]  C. A. Dreiss,et al.  Supramolecular Hydrogels: Design Strategies and Contemporary Biomedical Applications. , 2022, Chemistry, an Asian journal.

[20]  L. Ruiz‐Rubio,et al.  Spontaneous Gelation of Adhesive Catechol Modified Hyaluronic Acid and Chitosan , 2022, Polymers.

[21]  S. Feng,et al.  Hydrogels as Soft Ionic Conductors in Flexible and Wearable Triboelectric Nanogenerators , 2022, Advanced science.

[22]  F. Iida,et al.  Self-healing ionic gelatin/glycerol hydrogels for strain sensing applications , 2022, NPG Asia Materials.

[23]  W. Świȩszkowski,et al.  Hydrogel-Based Fiber Biofabrication Techniques for Skeletal Muscle Tissue Engineering , 2022, ACS biomaterials science & engineering.

[24]  Yu Qin,et al.  Stretchable slide-ring supramolecular hydrogel for flexible electronic devices , 2022, Communications Materials.

[25]  S. Seiffert,et al.  Defect-controlled softness, diffusive permeability, and mesh-topology of metallo-supramolecular hydrogels. , 2022, Soft matter.

[26]  Yue Zhao,et al.  Supramolecular Adhesive Hydrogels for Tissue Engineering Applications. , 2022, Chemical reviews.

[27]  M. Karbarz,et al.  Autonomous Self-healing Hydrogels: Recent Development in Fabrication Strategies , 2022, European Polymer Journal.

[28]  Michael R. Martinez,et al.  Injectable bottlebrush hydrogels with tissue-mimetic mechanical properties , 2022, Science advances.

[29]  Yiyun Cheng,et al.  All-small-molecule supramolecular hydrogels assembled from guanosine 5′-monophosphate disodium salt and tobramycin for the treatment of bacterial keratitis , 2022, Bioactive materials.

[30]  S Peers,et al.  Chitosan hydrogels incorporating colloids for sustained drug delivery. , 2022, Carbohydrate polymers.

[31]  Dongsheng Liu,et al.  DNA Supramolecular Hydrogel as a Biocompatible Artificial Vitreous Substitute , 2021, Advanced Materials Interfaces.

[32]  P. Ray,et al.  Strategic fabrication of efficient photo-responsive semiconductor electronic diode-devices by Bovine Serum Albumin protein-based Cu(II)-metallohydrogel scaffolds. , 2021, International journal of biological macromolecules.

[33]  Kaikai Zheng,et al.  Recent progress in surgical adhesives for biomedical applications , 2021, Smart Materials in Medicine.

[34]  Guihua Fang,et al.  γ-Cyclodextrin-based polypseudorotaxane hydrogels for ophthalmic delivery of flurbiprofen to treat anterior uveitis. , 2021, Carbohydrate polymers.

[35]  Liangjie Hong,et al.  A chitosan hydrogel sealant with self-contractile characteristic: From rapid and long-term hemorrhage control to wound closure and repair. , 2021, Carbohydrate polymers.

[36]  S. Heilshorn,et al.  3D Bioprinting of Cell‐Laden Hydrogels for Improved Biological Functionality , 2021, Advanced materials.

[37]  C. L. Le Maitre,et al.  One-pot precipitation polymerisation strategy for tuneable injectable Laponite®-pNIPAM hydrogels: Polymerisation, processability and beyond , 2021, Polymer.

[38]  S. Saber-Samandari,et al.  Alginate nanoparticles as ocular drug delivery carriers , 2021, Journal of Drug Delivery Science and Technology.

[39]  S. Seiffert,et al.  Sticker Multivalency in Metallo-supramolecular Polymer Networks , 2021, Macromolecules.

[40]  S. Hahn,et al.  Supramolecular host-guest hyaluronic acid hydrogels enhance corneal wound healing through dynamic spatiotemporal effects. , 2021, The ocular surface.

[41]  Weibing Qin,et al.  Bioprinting of a Blue Light-Cross-Linked Biodegradable Hydrogel Encapsulating Amniotic Mesenchymal Stem Cells for Intrauterine Adhesion Prevention , 2021, ACS omega.

[42]  K. Lee,et al.  3D Printing of Polysaccharide-Based Self-Healing Hydrogel Reinforced with Alginate for Secondary Cross-Linking , 2021, Biomedicines.

[43]  Geoffrey I N Waterhouse,et al.  Photosensitive drug delivery systems for cancer therapy: Mechanisms and applications. , 2021, Journal of controlled release : official journal of the Controlled Release Society.

[44]  M. D. Di Gioia,et al.  Gel-Based Materials for Ophthalmic Drug Delivery , 2021, Gels.

[45]  A. Zvyagin,et al.  Muscle‐Inspired MXene Conductive Hydrogels with Anisotropy and Low‐Temperature Tolerance for Wearable Flexible Sensors and Arrays , 2021, Advanced Functional Materials.

[46]  C. Grey,et al.  Formulation of Metal–Organic Framework-Based Drug Carriers by Controlled Coordination of Methoxy PEG Phosphate: Boosting Colloidal Stability and Redispersibility , 2021, Journal of the American Chemical Society.

[47]  Alejandro H. Espera,et al.  On the progress of 3D-printed hydrogels for tissue engineering , 2021, MRS Communications.

[48]  A. Kalam,et al.  Conductive Zn(ii)-metallohydrogels: the role of alkali metal cation size in gelation, rheology and conductance , 2021, Molecular Systems Design & Engineering.

[49]  Guihua Fang,et al.  Hydrogels-based ophthalmic drug delivery systems for treatment of ocular diseases. , 2021, Materials science & engineering. C, Materials for biological applications.

[50]  M. Devereux,et al.  Preparation and Antimicrobial Properties of Alginate and Serum Albumin/Glutaraldehyde Hydrogels Impregnated with Silver(I) Ions , 2021, Chemistry.

[51]  C. Creton,et al.  Swelling and Mechanical Properties of Polyacrylamide-Derivative Dual-Crosslink Hydrogels Having Metal–Ligand Coordination Bonds as Transient Crosslinks , 2021, Gels.

[52]  Eric A. Appel,et al.  Translational Applications of Hydrogels , 2021, Chemical reviews.

[53]  S. Magdassi,et al.  3D-printed self-healing hydrogels via Digital Light Processing , 2021, Nature Communications.

[54]  Mark W. Tibbitt,et al.  Engineering Hydrogel Adhesion for Biomedical Applications via Chemical Design of the Junction. , 2021, ACS biomaterials science & engineering.

[55]  Mark W. Tibbitt,et al.  Supramolecular engineering of hydrogels for drug delivery. , 2021, Advanced drug delivery reviews.

[56]  Eric A. Appel,et al.  Physical networks from entropy-driven non-covalent interactions , 2021, Nature Communications.

[57]  N. Rosen,et al.  Targeted drug delivery strategies for precision medicines , 2021, Nature Reviews Materials.

[58]  D. Mooney,et al.  Polymeric Tissue Adhesives. , 2021, Chemical reviews.

[59]  E. Fortunato,et al.  Healable Cellulose Iontronic Hydrogel Stickers for Sustainable Electronics on Paper , 2021, Advanced Electronic Materials.

[60]  S. Seiffert,et al.  Coordination Geometry Preference Regulates the Structure and Dynamics of Metallo-Supramolecular Polymer Networks , 2021 .

[61]  S. Stupp,et al.  3D Printing of Supramolecular Polymer Hydrogels with Hierarchical Structure. , 2021, Small.

[62]  E. Pashuck,et al.  (Macro)molecular self-assembly for hydrogel drug delivery. , 2021, Advanced drug delivery reviews.

[63]  Keita Ito,et al.  Hyaluronic acid-based supramolecular hydrogels for biomedical applications , 2021, Multifunctional Materials.

[64]  K. Zhou,et al.  Submerged and non-submerged 3D bioprinting approaches for the fabrication of complex structures with the hydrogel pair GelMA and alginate/methylcellulose , 2021, Additive Manufacturing.

[65]  Hector Lopez Hernandez,et al.  A Quantitative Description for Designing the Extrudability of Shear-Thinning Physical Hydrogels. , 2020, Macromolecular bioscience.

[66]  Peng-Hui Wang,et al.  Efficacy of Applying Hyaluronic Acid Gels in the Primary Prevention of Intrauterine Adhesion after Hysteroscopic Myomectomy: A Meta-Analysis of Randomized Controlled Trials , 2020, Life.

[67]  Jaeyun Kim,et al.  Adhesive Hydrogel Patch with Enhanced Strength and Adhesiveness to Skin for Transdermal Drug Delivery , 2020, Advanced Functional Materials.

[68]  Anam Ahsan,et al.  Thermosensitive Chitosan-Based Injectable Hydrogel as an Efficient Anticancer Drug Carrier , 2020, ACS omega.

[69]  J. Hao,et al.  Enzyme-Regulated Healable Polymeric Hydrogels , 2020, ACS central science.

[70]  A. Mikos,et al.  Nanomaterial Additives for Fabrication of Stimuli‐Responsive Skeletal Muscle Tissue Engineering Constructs , 2020, Advanced healthcare materials.

[71]  Yilong Cheng,et al.  H-Bonding Supramolecular Hydrogels with Promising Mechanical Strength and Shape Memory Property for Postoperative Anti-adhesion Application. , 2020, ACS applied materials & interfaces.

[72]  Ronnie H. Fang,et al.  Nanoparticle-hydrogel superstructures for biomedical applications. , 2020, Journal of controlled release : official journal of the Controlled Release Society.

[73]  Natalie Artzi,et al.  Overcoming the translational barriers of tissue adhesives , 2020, Nature Reviews Materials.

[74]  Luca Gasperini,et al.  The stiffness of living tissues and its implications for tissue engineering , 2020, Nature Reviews Materials.

[75]  S. Seiffert,et al.  Thermodynamic control over energy dissipation modes in dual-network hydrogels based on metal-ligand coordination. , 2020, Soft matter.

[76]  M. Watanabe,et al.  Recent progress in self-healable ion gels , 2020, Science and technology of advanced materials.

[77]  Sahar Salehi,et al.  In Situ Printing of Adhesive Hydrogel Scaffolds for the Treatment of Skeletal Muscle Injuries. , 2020, ACS applied bio materials.

[78]  R. Hoogenboom,et al.  Self-Healing Metallo-Supramolecular Hydrogel Based on Specific Ni2+ Coordination Interactions of Poly(ethylene glycol) with Bistriazole Pyridine Ligands in the Main Chain. , 2020, Macromolecular rapid communications.

[79]  H. Kraatz,et al.  Supramolecular Peptide Gels: Influencing Properties by Metal Ion Coordination and Their Wide-Ranging Applications , 2020, ACS omega.

[80]  A. Pich,et al.  Pros and Cons: Supramolecular or Macromolecular: What Is Best for Functional Hydrogels with Advanced Properties? , 2020, Advanced materials.

[81]  Xuanhe Zhao,et al.  Hydrogel machines , 2020 .

[82]  R. Lal,et al.  Vanadium(V) complex based supramolecular metallogel: self-assembly and (Metallo)gelation triggered by non-covalent and N+H…O hydrogen bonding interactions , 2020 .

[83]  Kyo Seon Hwang,et al.  Highly sensitive three-dimensional interdigitated microelectrode biosensors embedded with porosity tunable hydrogel for detecting proteins , 2020 .

[84]  Luyu Wang,et al.  Recent progress in metal-organic frameworks-based hydrogels and aerogels and their applications , 2019, Coordination Chemistry Reviews.

[85]  Cheng‐Hui Li,et al.  Self‐Healing Polymers Based on Coordination Bonds , 2019, Advanced materials.

[86]  Won-Kyo Jung,et al.  Enhanced rheological behaviors of alginate hydrogels with carrageenan for extrusion-based bioprinting. , 2019, Journal of the mechanical behavior of biomedical materials.

[87]  Jason Y. C. Lim,et al.  Recent advances in supramolecular hydrogels for biomedical applications , 2019, Materials Today Advances.

[88]  D. Das,et al.  Designer Peptide Amphiphiles: Self-Assembly to Applications. , 2019, Langmuir : the ACS journal of surfaces and colloids.

[89]  Yi Cao,et al.  A Highly Stretchable, Tough, Fast Self-Healing Hydrogel Based on Peptide–Metal Ion Coordination , 2019, Biomimetics.

[90]  Z. Suo,et al.  Printing Hydrogels and Elastomers in Arbitrary Sequence with Strong Adhesion , 2019, Advanced Functional Materials.

[91]  A. Khademhosseini,et al.  Sutureless repair of corneal injuries using naturally derived bioadhesive hydrogels , 2019, Science Advances.

[92]  C. Dellago,et al.  A High Coordination of Cross-Links Is Beneficial for the Strength of Cross-Linked Fibers , 2019, Biomimetics.

[93]  Y. Qiao,et al.  Conjoined-network rendered stiff and tough hydrogels from biogenic molecules , 2019, Science Advances.

[94]  Jinglei Wu,et al.  Bioresorbable electrospun gelatin/polycaprolactone nanofibrous membrane as a barrier to prevent cardiac postoperative adhesion. , 2019, Acta biomaterialia.

[95]  Wei Zhang,et al.  Electrically conductive hydrogels for flexible energy storage systems , 2019, Progress in Polymer Science.

[96]  Aldo R Boccaccini,et al.  3D Printing of Electrically Conductive Hydrogels for Tissue Engineering and Biosensors - A Review. , 2019, Acta biomaterialia.

[97]  E. Cohen,et al.  Self-assembly of a metallo-peptide into a drug delivery system using a "switch on" displacement strategy. , 2018, Journal of materials chemistry. B.

[98]  D. Ghosh,et al.  A supramolecular Cd(ii)-metallogel: an efficient semiconductive electronic device. , 2018, Dalton transactions.

[99]  Weiqi Wang,et al.  High performance HKUST-1@PVA-co-PE/PVA hybrid hydrogel with enhanced selective adsorption , 2018, Composites Communications.

[100]  T. Maji,et al.  Charge-Assisted Self-Assembly of ZIF-8 and Laponite Clay toward a Functional Hydrogel Nanocomposite. , 2018, Inorganic chemistry.

[101]  Nicholas Stephanopoulos,et al.  Reversible self-assembly of superstructured networks , 2018, Science.

[102]  Mingjie Liu,et al.  Conductive Hydrogels as Smart Materials for Flexible Electronic Devices. , 2018, Chemistry.

[103]  Jie Song,et al.  Modulating Viscoelasticity, Stiffness, and Degradation of Synthetic Cellular Niches via Stoichiometric Tuning of Covalent versus Dynamic Noncovalent Cross-Linking , 2018, ACS central science.

[104]  Haiyang Yang,et al.  Polyhistidine-Based Metal Coordination Hydrogels with Physiologically Relevant pH Responsiveness and Enhanced Stability through a Novel Synthesis. , 2018, Macromolecular rapid communications.

[105]  Yi Ju,et al.  Supramolecular Metal-Phenolic Gels for the Crystallization of Active Pharmaceutical Ingredients. , 2018, Small.

[106]  A. Ajayaghosh,et al.  Stepwise control of host–guest interaction using a coordination polymer gel , 2018, Nature Communications.

[107]  Sha Jin,et al.  Tissue and Organ 3D Bioprinting , 2018, SLAS technology.

[108]  Natália Noronha Ferreira,et al.  Recent advances in smart hydrogels for biomedical applications: From self-assembly to functional approaches , 2018 .

[109]  Z. Suo,et al.  Hydrogel ionotronics , 2018, Nature Reviews Materials.

[110]  Timothy K Lu,et al.  3D Printing of Living Responsive Materials and Devices , 2018, Advanced materials.

[111]  Mikyung Shin,et al.  Gallol-Rich Hyaluronic Acid Hydrogels: Shear-Thinning, Protein Accumulation against Concentration Gradients, and Degradation-Resistant Properties , 2017 .

[112]  D J Mooney,et al.  Tough adhesives for diverse wet surfaces , 2017, Science.

[113]  B. Jiang,et al.  Spatio‐temporal control strategy of drug delivery systems based nano structures , 2017, Journal of controlled release : official journal of the Controlled Release Society.

[114]  Christian M. Siket,et al.  Instant tough bonding of hydrogels for soft machines and electronics , 2017, Science Advances.

[115]  Fei Gao,et al.  3D-Printed High Strength Bioactive Supramolecular Polymer/Clay Nanocomposite Hydrogel Scaffold for Bone Regeneration. , 2017, ACS biomaterials science & engineering.

[116]  Ri Wang,et al.  B12-dependent photoresponsive protein hydrogels for controlled stem cell/protein release , 2017, Proceedings of the National Academy of Sciences.

[117]  Baolin Guo,et al.  Antibacterial anti-oxidant electroactive injectable hydrogel as self-healing wound dressing with hemostasis and adhesiveness for cutaneous wound healing. , 2017, Biomaterials.

[118]  W. Tsang,et al.  Fabrication of injectable high strength hydrogel based on 4-arm star PEG for cartilage tissue engineering. , 2017, Biomaterials.

[119]  Qiang Zhang,et al.  A Polydopamine Nanoparticle-Knotted Poly(ethylene glycol) Hydrogel for On-Demand Drug Delivery and Chemo-photothermal Therapy , 2017 .

[120]  David J. Mooney,et al.  Designing hydrogels for controlled drug delivery. , 2016, Nature reviews. Materials.

[121]  Lina Zhang,et al.  High‐Strength and High‐Toughness Double‐Cross‐Linked Cellulose Hydrogels: A New Strategy Using Sequential Chemical and Physical Cross‐Linking , 2016 .

[122]  L. Chu,et al.  Smart Hydrogels with Inhomogeneous Structures Assembled Using Nanoclay-Cross-Linked Hydrogel Subunits as Building Blocks. , 2016, ACS applied materials & interfaces.

[123]  C. L. Le Maitre,et al.  Thermally triggered injectable hydrogel, which induces mesenchymal stem cell differentiation to nucleus pulposus cells: Potential for regeneration of the intervertebral disc. , 2016, Acta biomaterialia.

[124]  K. Anseth,et al.  The design of reversible hydrogels to capture extracellular matrix dynamics , 2016, Nature Reviews Materials.

[125]  Abdul Ghaffar,et al.  Injectable biopolymer based hydrogels for drug delivery applications. , 2015, International journal of biological macromolecules.

[126]  A. Khademhosseini,et al.  Elastic sealants for surgical applications. , 2015, European journal of pharmaceutics and biopharmaceutics : official journal of Arbeitsgemeinschaft fur Pharmazeutische Verfahrenstechnik e.V.

[127]  Soong Ho Um,et al.  Tissue Adhesive Catechol‐Modified Hyaluronic Acid Hydrogel for Effective, Minimally Invasive Cell Therapy , 2015 .

[128]  Jeremiah A. Johnson,et al.  Dual Role for 1,2,4,5-Tetrazines in Polymer Networks: Combining Diels-Alder Reactions and Metal Coordination To Generate Functional Supramolecular Gels. , 2015, ACS macro letters.

[129]  Enas M. Ahmed,et al.  Hydrogel: Preparation, characterization, and applications: A review , 2013, Journal of advanced research.

[130]  F. Tezcan,et al.  A designed supramolecular protein assembly with in vivo enzymatic activity , 2014, Science.

[131]  Ran Du,et al.  Hierarchical hydrogen bonds directed multi-functional carbon nanotube-based supramolecular hydrogels. , 2014, Small.

[132]  D. Seliktar Designing Cell-Compatible Hydrogels for Biomedical Applications , 2012, Science.

[133]  Jonathan Seppala,et al.  A healable supramolecular polymer blend based on aromatic pi-pi stacking and hydrogen-bonding interactions. , 2010, Journal of the American Chemical Society.