Aug 2026· Advanced Functional Materials· 0 citations· 28 references
Abstract
The fabrication of biohydrogel coatings faces a trilemma in balancing gelation speed, functional fidelity, and scalability. Rapid reactions often lead to heterogeneous networks due to kinetic trapping, whereas precise methods tend to be slow and difficult to scale. To address this challenge, we propose an Interfacial confined Mutual Catalysis (ICMC) strategy. This approach constructs a cyclic catalytic cascade in which the MXene surface catalyzes monomer polymerization, while the sulfonate groups on the monomer reciprocally enhance the catalytic activity of MXene, resulting in a self‐accelerating polymerization process. This method enables sub‐minute gelation at low temperatures, yielding self‐growing hydrogel coatings with tunable thickness (20–430 µm) and intrinsic multi‐functionalities, including ultra‐low friction (µ < 0.03), strong antibacterial activity (>99.2%), photothermal effect, and excellent biocompatibility. As a proof of concept, MXene‐hydrogel coated surgical sutures reduce surface friction by 83% relative to commercial sutures and significantly mitigate inflammation and epithelial hyperplasia in a rat wound model. Notably, the ICMC approach is compatible with roll‐to‐roll (R2R) processing, enabling continuous and programmable fabrication of multifunctional hydrogel coatings. This work opens a door for easy and scalable manufacture of hydrogels‐based functional biomaterials and medical devices.
Thermoresponsive polymer coatings have attracted considerable attention for applications in materials science, biotechnology, and surface engineering. Materials exhibiting upper critical solution temperature (UCST) behavior remain comparatively underexplored in comparison to lower critical solution temperature (LCST), particularly in the form of structured thin films. The present work illustrates the use of poly(2‐(methacryloyloxy)ethylureido glycinamide) (PMEGA) as a versatile UCST‐responsive platform for the fabrication of surface‐attached hydrogel coatings with controlled architecture and functionality. This polymer, with straightforward monomer synthesis, exhibits a well‐defined UCST transition in aqueous solution. Based on thiol–ene click chemistry, the herein presented strategy displays the tunable engineering of homogeneous and microstructured hydrogel films by the cross‐linking and grafting (CLAG) approach. This method enables the fabrication of hydrogel coatings with precisely controlled thicknesses, as well as the generation of well‐defined micropatterns via UV‐induced photolithography like for photoresist. Importantly, the thermoresponsive swelling behavior of the surface‐grafted hydrogels can be adjusted by adjusting UV irradiation parameters, providing direct control over the UCST response in confined geometries. Overall, the combination of straightforward polymer synthesis, scalable thin‐film processing, and tunable thermo‐responsive properties opens new opportunities for the development of advanced functional coatings and microstructured surfaces.
Thi Phuong Thu Nguyen, Léa Milenkovic, Bruno Bresson et al.· Advanced Materials Interface...· 0 citations
Integration of hydrogel coatings onto medical devices holds great promise to mitigate tissue-device contact issues, yet achieving robust interfacial bonding and multifunctionality remains challenging. Here, a universal multifunctional zinc ionic semi-interpenetrating network hydrogel coating (Zn-SIHC) is developed onto polymer surfaces for tissue-friendly interventions. Zn-SIHC is generated in situ through surface-initiated polymerization of acrylamide (AM) as the primary covalent network. Chitosan is uniformly dispersed within this network, where zinc ions act as the cross-linkers to establish a complementary ionic network. Incorporation of zinc ions enhances both tensile strength (fourfold increase) and peeling strength (uo tp ∼900 N/m) due to ionic reinforcement and ensures good antibacterial capability. Meanwhile, Zn-SIHC exhibits favorable hydrophilic lubricity (CoF = 0.05), transparency (91%), antifouling properties, and biocompatibility. The clinical applicability of Zn-SIHC in alleviating intubation-related side effects is verified using an in vivo tracheal intubation model in cynomolgus monkeys. The potential mechanism by which Zn-SIHC inhibits intubation injury-induced inflammation and apoptosis is preliminarily deciphered. This work opens a new avenue for surface engineering of medical intervention devices.
Yu-Qing Wei, Baisong Zhao, Meng-Han Bai et al.· Small· 0 citations
Robust polymer nanofilms are increasingly important for applications that require mechanically strong yet compliant membranes with nanoscale thickness and intimate interfacial contact. While biological membranes naturally combine flexibility, adaptability, and adhesion, achieving these features in synthetic nanomembranes remains challenging. Here, we report a one‐step strategy for the synthesis of centimeter‐scale, freestanding nanofilms via redox‐confined interfacial polymerization at a liquid‐liquid interface. Oxidative coupling of a multifunctional thiol monomer is spatially restricted to the aqueous‐organic interface, yielding continuous membranes with precisely tunable thicknesses ranging from tens to hundreds of nanometers. Structural and surface analyses reveal uniform network formation across all film thicknesses, consistent with a diffusion‐controlled growth mechanism. The resulting nanofilms exhibit high Young's modulus (425 MPa) and tensile strength (38 MPa), solid‐like viscoelastic behavior, and intrinsic adhesion to artificial skin despite the absence of dedicated bioadhesive functionalization. Together, these results establish redox‐confined interfacial polymerization as a versatile fabrication route to mechanically robust, freestanding nanomembranes with potential relevance for wearable sensing platforms, therapeutic interfaces, separation membranes, and other applications requiring strong ultrathin films with intrinsic adhesion.
L. Gazzato, Vivek Manish, Giorgio Speranza et al.· Advanced Materials Interface...· 0 citations
Nanocellulose hydrogels are gaining traction as sustainable soft materials, thanks to the high surface area, abundant hydroxyl groups, mechanical strength, biocompatibility, and renewability of cellulose nanocrystals and nanofibers. Unlike conventional synthetic polymer hydrogels, those based on nanocellulose offer distinct advantages in building mechanically robust, multifunctional, and eco-friendly three-dimensional (3D) networks. This review highlights recent advances in the preparation, structural design, functionalization, and emerging applications of nanocellulose hydrogels. We begin by comparing major preparation routes — mechanical, chemical, chemical-mechanical and green solvent-based — in terms of efficiency, cost, environmental footprint, and scalability. Next, we discuss hydrogel fabrication strategies including physical and chemical crosslinking, double networks, interpenetrating polymer networks, and pore‑structure control. Emphasis is placed on how interfacial interactions, energy dissipation, and network topology govern mechanical performance. Functionalization methods to introduce stimuli responsiveness, electrical conductivity, self‑healing capability, and interfacial adhesion are then reviewed. Representative applications are covered in biomedical engineering, flexible electronics, smart devices, 3D printing, food packaging, and agricultural uses such as water retention and nutrient release. Finally, we critically examine key challenges: balancing mechanical strength with multifunctionality, dispersing nanofillers in multicomponent systems, limitations of current reinforcement theories, long‑term stability, biosafety, and scalable green manufacturing. This review aims to guide the rational design, functional integration, and practical translation of nanocellulose hydrogels.
Yanhua Liu, Zheng Xu, Peng-Jun Zhao et al.· Journal of Solid Waste Valor...· 0 citations
This perspective establishes NP–dynamic polymer interfaces as a programmable kinetic design parameter for controlling bond-exchange reactions in dynamic polymer networks, opening a pathway toward spatially defined covalent adaptable materials with application-specific and programmable dynamic behavior.
Klementina Pušnik Črešnar, Tadej Slatinek, L. F. Zemljič et al.· ACS Macro Letters· 0 citations
Superhydrophobic coatings are often limited in practical applications due to the fragile micro/nanostructures and poor mechanical resistance. Herein, a facile one‐pot synthesis strategy was proposed to fabricate an organic–inorganic composite coating with a three‐dimensional interconnected cross‐linked network through in situ photopolymerization of vinyltriethoxysilane (ETS) and its dehydration condensation reaction with natural halloysite nanotubes (HNTs). When the HNT loading reached 25 wt% of ETS, the as‐prepared coating exhibited uniform superhydrophobicity with a contact angle of ~150°. More importantly, owing to its consistent structure and chemical composition throughout the surface and bulk, the coating retained excellent hydrophobic stability even after severe mechanical abrasion. Beyond its simplicity and avoidance of organic solvents or fluorinated reagents, this strategy provides an effective way to prepare durable superhydrophobic coatings, which hold significant potential for many practical applications such as waterproofing and self‐cleaning.
Lei Xiong, Yin-Feng Liu, Deping Chen et al.· Polymer Engineering & Sc...· 0 citations