Excellent Shape Research Articles

Novel sustainable, smart, and multifunctional 4D-printed nanocomposites with reprocessing and shape memory capabilities

Abstract The present paper explores the development of novel recyclable and reprocessable nanocomposites with enhanced shape memory (SM) capability Digital Light Processing 3D printing technology. More specifically, the developed Covalent Adaptable Network is based on polyurethane containing Diels Alder bonds reinforced with carbon nanotubes (CNTs), where the dynamic bonds enable recyclability and reprocessability, whereas CNT addition allows obtaining electrically conductive nanocomposites. In this sense, the nanocomposites exhibited significant Joule heating capabilities, which were used to trigger the SM cycle.
First, CNT contents and thermal treatments were tuned to optimize SM capabilities in a conventional oven, seeking for obtaining a stable temporary shape at room temperature. Then, the SM capabilities triggered by Joule heating were characterized. Here, the optimized nanocomposites showed excellent shape fixity and recovery ratios (both above 95 %) when triggering the SM by the Joule effect. This heating method was proven to be low energy-consuming (around 1 W), as well as allowing fast, remote, and selective activation, being the latter the ability to trigger the SM in a specific area of the specimen as desired, which was demonstrated with a hand-like proof-of-concept by selectively recovering the permanent shape of each finger.
Finally, the 3D-printed specimens were turned into powder and reprocessed using a powder processing tool, obtaining a still electrically conductive part with a different geometry given the DA adduct formations.
In summary, the multifunctional and smart capabilities of the developed nanocomposites make them suitable for applications such as soft robotics or actuators with an extended useful life, promoting sustainability.

Robust Mechanically Interlocked Network Ionogels.

Ionogels have attracted considerable attention as versatile materials due to their unique ionic conductivity and thermal stability. However, relatively weak mechanical performance of many existing ionogels has hindered their broader application. Herein, we develop robust, tough, and impact-resistant mechanically interlocked network ionogels (IGMINs) by incorporating ion liquids with mechanical bonds that can dissipate energy while maintain structural stability. Profiting from the dynamic yet stable nature of the mechanically interlocked networks, IGMINs exhibit high tensile strength (9.6 MPa), fracture energy (39 kJ/m2), and toughness (25.9 MJ/m3), along with a high elongation rate (473%) and excellent impact resistance and shape memory, resulting in overall performance that surpasses most reported ionogels. Furthermore, in the application of strain sensors for monitoring the gait of crawling robots, the toughness and robustness of IGMINs ensure their ability to consistently output stable electrical signals during the stretching and contraction processes, thereby highlighting their practical application potential. Our work provides a new research strategy for toughening ionogels and promotes the development of mechanically interlocked materials.

Analysis and prediction of tensile properties based on a novel wide‐angle fabric/EPDM composite under different temperatures

AbstractThis study investigated the tensile properties of the wide‐angle fabric/ethylene‐propylene‐diene monomer (EPDM) composite (WFRC) under varying temperature conditions based on the macro‐ and mesoscopic structural characterization. The wide‐angle fabric was modeled using an improved “cross‐sectional path” method that precisely represents the yarn geometry by integrating warp and weft orientations within a non‐orthogonal coordinate system derived from optical micrographs. Tensile tests conducted across a temperature range from 25 to 150°C revealed that both stress and strain decrease with increasing temperature. Numerical simulations closely aligned with the experimental data, exhibiting a maximum relative error of only 2.5% at 90°C, thereby demonstrating the robustness of the simulation models in capturing the mechanical responses of WFRC. The findings underscore the predominant role of the rubber matrix in determining the mechanical properties of WFRC, while also highlighting that the fabric maintains excellent shape conformity with the rubber. This paper presents an effective methodology for analyzing the mechanical properties of WFRC under varying temperatures, laying the groundwork for future studies on the long‐term durability and failure mechanisms of WFRC under cyclic thermal loads, and broadening its applications across various engineering domains.Highlights The improved “cross section path” method is employed for fabric modeling. Macro‐ and mesoscopic modeling of the wide‐angle fabric/EPDM composite. The superelasticity of the rubber is integrated into the VUMAT subroutine. The numerical simulations closely align with the experimental data.

Use of corn carbon as an additive to enhance magnesium metal self-corrosion and recover phosphorus from swine wastewater in the form of struvite.

Recovery of phosphate from swine wastewater is significant for alleviating eutrophication in aquatic ecosystems and addressing the increasing scarcity of phosphorus resources. In this study, a method for phosphate recovery from swine wastewater using corn carbon as an additive and non-dynamic magnesium metal self-corrosion was studied. The effects of reaction time, C:Mg mass ratio, stirring rate, and aeration rate on phosphate recovery were discussed, and eight experimental models were explored. The results demonstrated that when the optimal reaction time was 7h, the mass ratio of corn carbon to the magnesium plate was 5:1. When the stirring rate was 800rpm/min and the aeration rate was 0.48m3/L·h, the pH value of wastewater was 9.24, and the phosphate recovery rate was 95.61%. The recovered precipitate was characterized by SEM-EDS and XRD as struvite with excellent crystal shape. This method not only successfully achieved waste treatment but also recovered phosphorus from swine wastewater.

Shape Memory Performance and Microstructural Evolution in PLA/PEG Blends: Role of Plasticizer Content and Molecular Weight.

Poly(lactic acid) (PLA) exhibits excellent shape memory properties but suffers from brittleness and a high glass transition temperature (Tg), limiting its utility in flexible and durable applications. This study explored the modification of PLA properties through the incorporation of poly(ethylene glycol) (PEG), varying in both content (5-20 wt%) and molecular weight (4000-12,000 g/mol), to enhance its suitability for specific applications, such as medical splints. The PLA/PEG blend, containing 15 wt% PEG and with a molecular weight of 12,000 g/mol, exhibited superior shape fixity (99.27%) and recovery (95.77%) in shape memory tests conducted at a programming temperature (Tp) of 45 °C and a recovery temperature (Tr) of 60 °C. Differential scanning calorimetry (DSC) analysis provided insights into the thermal mechanisms driving shape memory behavior of the PLA/PEG blend. The addition of PEG to the PLA blend resulted in a reduction in Tg and an increase in crystallinity, thereby facilitating enhanced chain mobility and structural reorganization. These thermal changes enhanced the shape fixity and recovery of the PLA/PEG blend. Synchrotron wide-angle X-ray scattering (WAXS) was further employed to elucidate the microstructural evolution of PLA/PEG blends during the shape memory process. Upon stretching, the PLA/PEG chains aligned predominantly along the tensile direction, reflecting strain-induced orientation. During recovery, the PLA/PEG chains underwent isotropic relaxation, reorganizing into their original configurations. This structural reorganization highlighted the critical role of chain mobility and alignment in driving the shape memory behavior of PLA/PEG blends, enabling them to effectively return to their initial shape. Mechanical testing confirmed that increasing PEG content and molecular weight enhanced elongation at break and impact strength, balancing flexibility and strength. These findings demonstrated that PLA/PEG blends, especially with 15 wt% PEG at 12,000 g/mol, offer an optimal combination of shape memory performance and mechanical properties, positioning them as promising candidates for customizable and biodegradable medical applications.

Universal Construction of Electrical Insulation and High-Thermal-Conductivity Composites Based on the In Situ Exfoliation of Boron Nitride-Graphene Hybrid Filler.

Hexagonal boron nitride (h-BN), with excellent thermal conductivity and insulation capability, has garnered significant attention in the field of electronic thermal management. However, the thermal conductivity of the h-BN-enhanced polymer composite material is far from that expected because of the insurmountable interfacial thermal resistance. In order to realize the high thermal conductivity of polymer composite thermal interface materials, herein, an in situ exfoliation method has been employed to prepare a boron nitride nanosheet-graphene (BNNS-Gr) hybrid filler. After being incorporated into a poly(ethylene glycol) (PEG) matrix, the thermal conductivity of composites is significantly improved on the premise of electrical insulation. Furthermore, a three-dimensional (3D) thermally conductive framework using this hybrid filler as the raw material has also been constructed. After incorporating poly(ethylene glycol) (PEG) through a vacuum impregnation method, this ordered structure effectively resolves the leakage issue in phase-change composites during actual working conditions and showcases enhanced thermal conductivity of 2.45 W m-1 K-1 at 10 vol %, along with excellent electrical insulation, shape stability, and cyclic stability. The modified Hashin-Shtrikman model and the Foygel nonlinear model prove that compounding graphene with BN reduces the interfacial thermal resistance of polymer composites for both disordered and ordered systems. This indicates that the in situ exfoliation strategy is an effective method to fabricate the nanofiller for reducing the interfacial thermal resistance of composites.

Construction and Characterization of Multi‐Stimuli Responsive Shape Memory Assisted Self‐Healing Thermoplastic Elastomeric Materials Based on TPU/ENR/Fe3O4 Blends

AbstractIn this work, multi‐stimuli responsive shape memory‐assisted self‐healing thermoplastic elastomeric materials are designed by incorporating Fe3O4 particles in dynamically vulcanized thermoplastic elastomeric materials based on thermoplastic polyurethane (TPU)/epoxidized natural rubber (ENR) blends. A thermodynamic perspective is employed to predict the potential distribution of Fe3O4 in the developed blends in which Fe3O4 is selectively distributed in the ENR phase. Interestingly, the Fe3O4‐loaded TPV exhibited multi‐stimuli responsive shape memory‐assisted self‐healing functionality, more specifically in the presence of an alternating magnetic field, infrared light, and heat. The resulting dynamically vulcanized TPU/ENR/Fe3O4 blends demonstrated healing efficiencies of ≈53%, ≈78%, and ≈69% under oven heat, under a magnetic field, and under infrared light exposure, respectively. Thermal image mapping is used to understand the stimulus‐dependent healing mechanisms. The developed Fe3O4 filled dynamically vulcanized TPV also shows excellent shape memory properties with a shape recovery ratio in the range of 88%–90% under the aforementioned conditions. The incorporation of Fe3O4 possibly induces coordination interactions with zinc dimethacrylate (ZDMA), used as a coagent during dynamic vulcanization, as evidenced by FTIR and XRD analyses, thereby enhancing the functional properties of the developed TPVs.

Strategy for Fabricating Multiple-Shape Memory Polymeric Materials Based on Solid State Mixing.

Traditionally, multiple shape memory polymers (multiple-SMPs) are created by forming either immiscible blends with high phase continuity (cocontinuous or multilayer phase morphology) or miscible blends that exhibit compositional heterogeneity at the nanoscale. Here, a new strategy for the fabrication of multiple-SMPs is proposed. It consists of the possibility of homogeneous mixing of immiscible polymers in the solid state under high pressure and shear deformation conditions. The blends formed in this way exhibit homogeneity of mixing down to the nanoscale, up to 40-95 nm. The transition from immiscible to miscible blends leads to an improvement not only in shape memory but also in the mechanical performance of the blends formed. Polypropylene (PP) and polystyrene (PS) were selected as pairs of immiscible polymers. The method of solid phase mixing is high pressure torsion (HPT). It was shown that the HPT-processed 50% PP/50% PS blend is able to exhibit an excellent triple shape memory effect (shape fixation of ∼94-95%, and recovery of ∼85-95%) with widely tunable (low and high) transition temperatures.

Intrinsic Anti-Freezing, Tough, and Transparent Hydrogels for Smart Optical and Multi-Modal Sensing Applications.

Hydrogels have received great attention due to their molecular designability and wide application range. However, they are prone to freeze at low temperatures due to the existence of mass water molecules, which can damage their flexibility and transparency, greatly limiting their use in cold environments. Although adding cryoprotectants can reduce the freezing point of hydrogels, it may also deteriorate the mechanical properties and face the risk of cryoprotectant leakage. Herein, the microphase-separated structures of hydrogels are regulated to confine water molecules in sub-6nm nanochannels and increase the proportion of bound water, endowing the hydrogels with intrinsic anti-freezing properties, high mechanical strength, good stretchability, remarkable fracture energy, and puncture resistance. Even after being kept in liquid nitrogen for 1000h, the hydrogel still maintains good transparency. The hydrogel can exhibit excellent low-temperature shape memory and intelligent optical waveguide properties. Additionally, the hydrogel can be assembled into strain and pressure sensors for flexible sensing at both room and low temperatures. The intrinsically anti-freezing microphase-separated hydrogel offers broad prospects in low-temperature electronic and optical applications.

Robust shape memory chlorobutyl rubber/boron nitride polymer nanocomposites for oil-water separation application

BackgroundBoron nitride (h-BN), an excellent 2D material finds exceptional applications in various fields owing to its unique characteristics including excellent hydrophobicity. Incorporation of boron nitride in polymer matrices is a captivating strategy by the scientific community to tune the properties of polymer. Interestingly, the possibilities of incorporating h-BN in chlorobutyl rubber (CIIR) matrix has never been considered and tried till now. Moreover, the use of CIIR to create a clean environment and reduce water pollution is an unexplored area even though the CIIR rubber possess excellent barrier properties. MethodsIn this work, two techniques were used for the fabrication of BNNS/CIIR nanocomposite. We exfoliated h-BN via chemical exfoliation method and tried the reinforcement of CIIR with BNNS via solution intercalation method. Shape memory analysis was performed with the help of stearic acid and oil-water separation analysis was achieved through an easy experimental technique. Significant findingsEnhanced mechanical strength of 11.57 MPa, improved thermal degradation temperature and char yield, higher glass transition temperature of -45.98° were observed for BNNS/CIIR nanocomposite reinforced with higher BNNS loading owing to the uniform distribution and better intercalation of BNNS in CIIR. Excellent shape memory was exhibited by CIIR matrix when reinforced up to 5 g BNNS. In addition, the nanocomposites displayed excellent ability to perform oil-water separation with increase in BNNS loading owing to the good hydrophobic character of h-BN and inherent barrier properties of CIIR. Thus, the study proved successful towards the fabrication of advanced CIIR nanocomposites with excellent shape memory and oil water separation efficiency.

Corrigendum to “Bio-based eutectic composite phase change materials with enhanced thermal conductivity and excellent shape stabilization for battery thermal management” [J. Energy Storage 100 (2024) 113712

Corrigendum to “Bio-based eutectic composite phase change materials with enhanced thermal conductivity and excellent shape stabilization for battery thermal management” [J. Energy Storage 100 (2024) 113712

Preparation of thermoresponsive & enzymatically crosslinkable gelatin-gellan gum bioink: A protein-polysaccharide hydrogel for 3D bioprinting of complex soft tissues.

Developing superior bioinks presents several challenges in achieving ideal properties such as biocompatibility, viscosity, degradation rates & mechanical properties which are required to make functional tissue constructs. Various attempts have been made to prepare excellent bioink compositions that are suitable to address the above challenges. Herein, a versatile combination of gelatin (GL) - gellan gum (GG) bioink was successfully formulated & the bioink 7.5GL/2GG was found to be ideal for printing complex and highly intricate structures with excellent shape fidelity. Two different crosslinkers namely transglutaminase (TG) and calcium chloride (CaCl2) were utilized for crosslinking. The rheological properties of GL/GG bioink indicated that TG and dual (TG + CaCl2) crosslinked constructs had storage modulus equivalent to the that of native skin. Direct and indirect cytotoxicity assays revealed that the developed constructs were cytocompatible as well as hemocompatible. The 3D bioprinted GL/GG constructs crosslinked with only TG showed better cell viability, proliferation, cell spreading and wound healing efficiency in vitro compared to dual crosslinked constructs. In conclusion, TG crosslinking of 7.5GL/2GG bioink was ideal for bioprinting of skin tissue constructs for regenerative medicine applications. By altering the concentrations & printing conditions, this bioink may be tuned for other soft tissue engineering applications.

A One-Stone-Two-Birds Strategy for Photothermal Shape Memory Polyurethane Utilizing Lignin as Monomer and Internal Photothermal Agent.

Photothermal-triggering shape memory polyurethane allows for precise and controllable shape transformation under remote light stimulation, making it highly desirable for applications in intelligent devices. This study develops a sustainable and high-performance lignin-based polyurethane (LPU) using a one-stone-two-birds strategy, wherein lignin serves as both a synthetic monomer and an internal photothermal agent. The incorporation of lignin significantly improved the mechanical properties of LPU, achieving a tensile strength of 42.1MPa and an impressive elongation at break of 1558%. Additionally, the LPU exhibited exceptional photothermal heating capabilities due to the inherent intramolecular π-π conjugations and intermolecular π-π stacking effects of lignin, which facilitated the precise and contactless remote photoheating. Furthermore, the rigid structure of lignin and robust hydrogen bonding interactions provided LPU with excellent multi-cycle shape memory performance, with shape fixation and shape recovery rates exceeding 93% after five cycles. Under near-infrared irradiation, LPU demonstrated precise non-contact heating and remote photothermal shape-control capabilities. This research not only offers a sustainable and high-value application for lignin but also advances the development of environmentally friendly intelligent shape memory polyurethane materials.

3D Bioprinting and Artificial Intelligence-Assisted Biofabrication of Personalized Oral Soft Tissue Constructs.

Regeneration of oral soft tissue defects, including mucogingival defects associated with the recession or loss of gingival and/or mucosal tissues around teeth and implants, is crucial for restoring oral tissue form, function, and health. This study presents a novel approach using three-dimensional (3D) bioprinting to fabricate individualized grafts with precise size, shape, and layer-by-layer cellular organization. A multicomponent polysaccharide/fibrinogen-based bioink is developed, and bioprinting parameters are optimized to create shape-controlled oral soft tissue (gingival) constructs. Rheological, printability, and shape-fidelity assays, demonstrated the influence of thickener concentration and print parameters on print resolution and shape fidelity. Artificial intelligence (AI)-derived tool enabled streamline the iterative bioprinting parameter optimization and analysis of the interaction between the bioprinting parameters. The cell-laden polysaccharide/fibrinogen-based bioinks exhibited excellent cellular viability and shape fidelity of shape-controlled, full-thickness gingival tissue constructs over the 18-day culture period. While variations in thickener concentrations within the bioink minimally impact the cellular organization and morphogenesis (gingival epithelial, connective tissue, and basement membrane markers), they influence the shape fidelity of the bioprinted constructs. This study represents a significant step toward the biofabrication of personalized soft tissue grafts, offering potential applications in the repair and regeneration of mucogingival defects associated with periodontal disease and dental implants.

High-Performance Triple-Network Hydrogels Derived from Chrome Leather Scraps: Ultrahigh Compressive Strength, Adhesion, and Self-Recovery.

The development of engineered hydrogels with high strength, self-recovery, and adhesion is essential for applications requiring resistance to large deformations and cyclic loading. Herein, a triple-network (TN) hydrogel with ultrahigh compressive strength, strong adhesion, and good self-recovery was constructed by using tannic acid-modified chrome leather scrap hydrolysate as the first network, polyacrylamide as the second network, and poly-2-propenamide-2-methylpropanesulfonic acid as the third network. The ultrahigh (70 MPa compressive strength and 95% compression deformation) TN hydrogels were effectively created, which is attributed to the synergy of the three networks. The TN hydrogels display adhesion (adhesion strength > 20 kPa) ascribed to the introduction of phenolic hydroxyl groups in tannic acid. Intriguingly, the TN hydrogels exhibit excellent self-recovery performance (93.6% dissipated energy recovery at 70 °C) and shape memory performance (restored to the original shape in 20 s). These properties are essential for the development of high-performance hydrogels and promote the resource utilization of leather waste.

Modeled Networks Shape Memory Polyurethanes Based on a Four-Armed Regularized Structural Crosslinking Agent of Pentaerythritol Propylene Oxide (PO-PTOL)

To improve the shape recovery degree, the chemical cross-linking mode effectively prevents slippage between molecular chains of shape memory polyurethanes (SMPUs). However, the irregular crosslinked network structure formed tends to be unevenly stressed when subjected to external forces, and stress concentrations occur, leading to a decrease in the mechanical properties of the polymer. To obtain better shape memory properties and mechanical properties, we introduced a four-armed, regularized structure of the pentaerythritol propylene oxide (PO-PTOL) into the SMPUs networks to prepare shape memory polyurethanes (PUX) with the model networks, and controlled the topology of the PUX network by adjusting the content of the PO-PTOL. Among them, PU0.15 exhibited ultra-high mechanical properties (tensile strength, elongation at break, and Young’s modulus of 32 MPa, 2011.7%, and 1.59 MPa, respectively) and excellent shape memory properties (shape recovery time of less than 1 s, shape fixation degree, and shape recovery degree of 92.7% and 98.5%, respectively). This study provides new ideas for designing network structures for SMPUs and is a new paradigm for introducing modeled structures into SMPU networks.

Novel fabrication of polyethylene glycol/ceramic composite pellets with an excellent phase change shape stable trait and their potential applications for greenhouse insulation

Organic solid–liquid phase change materials (PCMs) face challenges in practical applications due to their susceptibility to leakage during phase transitions. To address this issue, we constructed the polyethylene glycol (PEG)/ceramic pellets (CPs) composite phase change shape stable materials (PCSHs) with thermal energy storage capability, thermal stability, and a firm texture using the melting impregnation method. The PCSHs exhibit remarkable shape stability in the leakage test due to the capillary action and surface tension generated by the micropore structure on their surface. They also can convert light energy into heat and store it as latent heat, achieving an optimal photothermal conversion efficiency of 45.21 % and a maximum melting enthalpy of 13.33 kJ/kg at a PEG loading of ∼ 12 %. An outdoor greenhouse insulation simulation experiment confirmed that the PCSHs can maintain soil temperatures above 30 °C for over 30 min after illumination ceases. This work presents a facile synthesis strategy for shape-stable PCMs with potential applications in greenhouse insulation.

Polyethylene glycol/carboxymethyl cellulose/montmorillonite composite phase change materials for thermal management

The fabrication of composite phase change materials (CPCMs) with excellent shape stability, reasonable thermal conductivity and good mechanical properties using simple process to obtain an effective energy storage and conversion maintains an issue of the utmost importance. In this work, carboxymethylcellulose sodium (CMC)/montmorillonite (MMT) aerogels with various MMT loading is initially prepared by gelation and freeze-drying technique. The prepared CMC/MMT aerogels have a uniformly distributed pore structure, of which the compressive strength can reach 26.4 kPa when the MMT loading content is 40 wt%. When the MMT loading content is 40 wt%, the thermal conductivity of the PEG/CMC/40MMT CPCM can reach up to 0.78 W/m·K, which is 225 % higher than that of pure PEG. In particular, the rigid CMC/MMT composite aerogel is conducive to the storage of PEG, obtaining a maximum loading percentage of 96.8 %, phase change enthalpy of 179.2 J/g, and high enthalpy efficiency of 98.6 % for CMC/40MMT aerogel. The rigid supporting matrix and adsorption capacity of the CMC/MMT framework meliorate the shape stability and cyclic stability during the phase transition, which can also cool the surface temperature of a simulated central processing unit (CPU) from 90 °C to 54.7 °C. In summary, the as-prepared novel PEG/CMC/40MMT CPCM offers a novel strategy for thermal management of next-generation electronic devices.

Thermal and Mechanical Robust Solid‐Solid Phase Change Materials Enabled by Reactive Crosslinkable Poly(Ethylene Glycol)s via Facile Thiol‐Ene Photo‐Click Chemistry

AbstractSolid–solid phase change materials (SSPCMs) are among the most promising candidates for thermal energy storage and management. Excellent shape stability, high heat storage capacity, and satisfying mechanical properties are essential for the practical applications of SSPCMs, yet giving PCMs these characteristics at the same time remains an unmet challenge. Herein, the synthesis of PEG‐PVEG copolymers is reported with various vinyl content using a synergistic catalysis strategy, leading to novel cross‐linked PEG‐based SSPCMs via a thiol‐ene photo‐crosslinking reaction. These PCMs exhibit excellent shape stability and remarkable energy storage capabilities with latent heat up to 128.3 J g−1. The materials exhibit exceptional thermal stability and retain their energy storage capacity after 500 heating‐cooling cycles. Notably, the materials show superior mechanical strength and excellent toughness. Furthermore, the latent heat enthalpy can be further improved to 146.8 J g−1 without erosion of shape stability by the encapsulation of PEG into present SSPCM. The enhancement of both thermal and electrical conductivities is also demonstrated by the phase change composites (PCCs) incorporating multi‐walled carbon nanotubes (MWCNTs). Overall, this study presents a convenient and feasible strategy for developing SSPCMs with excellent shape stability, high latent heat and satisfying mechanical properties for thermal management.

Smart hydrogel dressing for machine learning-enabled visual monitoring and promote diabetic wound healing

Diabetic wounds are complex complications characterized by long-term chronic inflammation, vascular damage, and difficulties in healing. Monitoring wound pH can serve as an early warning system for infection risk and enhance wound management by tracking changes in wound pH. In this study, a machine learning-assisted analysis smart hydrogel as wound dressing was developed by utilizing a double cross-linked network hydrogel of gelatin methacrylate (GelMA) and chitosan methacrylate (CMCSMA) as the matrix, a compound of cobalt-gallic acid based metal-phenolic nanoparticles (GACo MPNs) as the active ingredients, and phenol red as the pH indicator. This smart hydrogel exhibits excellent injection performance, shape adaptability and mechanical strength. Besides, a series of in vitro experiments demonstrated the favorable biocompatibility and bioactivity of GelMA/CMCSMAP-GACo hydrogel, encompassing its antibacterial, anti-inflammatory, antioxidant, and angiogenic properties. In vivo experiments show that this hydrogel significantly improved the repair of diabetic wounds in mice. Interestingly, the hydrogel exhibited unique visual pH monitoring properties, which can be seamlessly integrated with a smartphone for image visualization and further enable reliable wound pH assessment using machine learning algorithms to enhance wound management based on wound pH. Overall, this study presented a comprehensive regenerative strategy for the management of diabetic wounds.