Developing mechanically robust, self-healable, and antibacterial poly(dimethylsiloxane) elastomers through the introduction of metal-polyphenol networks†

Yan Huang^a, Qingqing Hao^a, Hao Chen^a, Jianyu Liu^a, Jie Liu^a, Yusheng Qin^a, Zhengfeng Ma^bc, Zhuhui Qiao^bc, Zhirong Xin*^a and Chunyang Bao*^a
aSchool of Chemistry & Chemical Engineering, Yantai University, Yantai 264005, China. E-mail: baochunyang_chem@163.com; xinzhirong2012@126.com
^bState Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou, Gansu 730000, PR China
^cShandong Laboratory of Advanced Materials and Green Manufacture, Yantai Zhongke Research Institute of Advanced Materials and Green Chemical Engineering, Yantai, Shandong 264006, PR China

First published on 14th July 2025

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Introduction

Poly(dimethylsiloxane) (PDMS) elastomers are widely adopted in medical devices, such as catheters and indwelling needles, due to their inherent chemical stability, biocompatibility, and antimicrobial properties.^1–5 These attributes not only minimize infection risks but also extend device longevity and enhance patient comfort. However, the practical utility of PDMS in sustained medical applications is critically limited by its intrinsic mechanical deficiencies, including low tensile strength and poor fatigue resistance, which often lead to premature material failure, increased replacement costs, and compromised clinical outcomes. To address these limitations, imparting self-healing functionality to PDMS elastomers has emerged as a transformative strategy.^6–10 By integrating dynamic reversible bonds, including non-covalent interactions or covalent adaptable networks, into polymer networks, these materials can restore their original performance after mechanical damage, thereby prolonging service life and reducing healthcare expenditures.^{7–9,11–17} For example, Bao and coworkers reported a class of tough and self-healing PDMS elastomers by rationally constructing multivalent hydrogen bonding interactions in the polymer networks.⁹ The resultant PDMS elastomers exhibited good tensile strength of ∼1.8 MPa, high stretchability of ∼1200%, high toughness of ∼12000 J m⁻², and autonomous self-healing ability at room temperature. Similarly, Xia and coworkers engineered poly(siloxane-urethane) elastomers with thermally reversible Diels–Alder reactions, enabling tuneable mechanical strength (∼1.0 MPa to ∼5.8 MPa) via soft-segment modification.⁷ In addition to developing self-healing PDMS elastomers using single reversible non-covalent bonds or covalent bonds, some strategies including building dual physical cross-linking networks or constructing dynamic nano-micro structures in the polymer networks have been developed to fabricating high-performance self-healable PDMS elastomers.^5,6,12 For example, Li and coworkers developed dual physically cross-linked PDMS networks with competitive supramolecular interactions, yielding materials that combine high tensile strength of ∼4.0 MPa, toughness of ∼16.0 MJ m⁻³, and near-perfect self-healing efficiency of ∼98% at body temperature.⁶ Concurrently, Fu and coworkers employed the concept of in situ manipulating nanostructure transformation through a molecular engineering strategy, producing PDMS polyurea materials with high tensile stress of ∼2.6 MPa, tensile strain of ∼1680%, and toughness of ∼22.6 MJ m⁻³, respectively.¹² Despite these advancements, a critical challenge persists that the inherent trade-off between mechanical robustness and healing efficiency in PDMS elastomers. Current systems typically prioritize one property at the expense of the other, with high-strength elastomers (>5 MPa) often requiring elevated healing temperatures or prolonged recovery times.^{8,12,13,15,18–21} This limitation underscores the urgent need for material design strategies that balance these competing requirements, enabling next-generation medical devices that simultaneously withstand physiological stresses and autonomously maintain functional integrity.

Metal-phenolic networks (MPNs), first pioneered by Caruso and coworkers in 2013, are supramolecular assemblies formed through the coordination of natural polyphenolic ligands with metal ions.^22,23 These dynamic networks have since been engineered to exhibit multifunctionality, including antibacterial activity, bone regeneration, fluorescence, bioadhesion, and flame retardancy, by judiciously selecting phenolic precursors (e.g., tannic acid, gallic acid) and metal ion counterparts (e.g., Fe³⁺, Cu²⁺).^23–29 Their structural versatility arises from an intricate interplay of supramolecular interactions, such as hydrogen bonds, metal–ligand coordination, and cation-π interactions, which have enabled their widespread use as functional coatings in biomedical, environmental, and energy applications.^{24–27,30,31} Capitalizing on these attributes, we propose that in situ integration of MPNs into poly(dimethylsiloxane) (PDMS) elastomer networks offers a transformative strategy to simultaneously enhance mechanical strength, confer self-healing capability, and impart antimicrobial functionality. This approach addresses critical limitations in conventional PDMS-based medical devices while leveraging the inherent biodegradability and bioactivity of MPNs for advanced therapeutic applications. In this study, we developed mechanically robust and self-healable PDMS-based polyurea elastomers (denoted IPPU-GF_x) through the in situ construction of MPNs within the polymer networks of PDMS-based polyurea elastomers (IPPU). The IPPU was synthesized via condensation polymerization between aminopropyl-terminated PDMS (NH₂-PDMS-NH₂) and isophorone diisocyanate (IPDI), followed by chain extension using 1,3-bis(3-aminopropyl)-1,1,3,3-tetramethyldisiloxane (ATTI). MPNs were subsequently incorporated as dynamic cross-linkers during network formation, creating a hierarchical architecture with tunable mechanical properties. By systematically modulating MPN content, we achieved precise control over tensile strength, ranging from ∼3.4 MPa to ∼7.7 MPa, a 133% enhancement compared to unmodified IPPU. The synergistic interplay of reversible hydrogen bonds and metal-coordination motifs enabled exceptional self-healable performance, with damaged IPPU-GF_1% specimens recovering 99.7% of their original mechanical integrity after thermal treatment at 75 °C. Furthermore, leveraging the intrinsic bioactivity of polyphenol-based MPNs, the composites exhibited potent antibacterial efficacy against clinically relevant pathogens (S. aureus and E. coli). This work establishes a supramolecular design paradigm that reconciles the historical trade-off between mechanical robustness and functional adaptability in PDMS elastomers. The successful integration of high strength, autonomous self-healing, and antimicrobial activity positions IPPU-GF_x elastomers as promising candidates for next-generation medical devices, wearable sensors, and soft robotics requiring sustained performance in biologically active environments.

Experimental section

Synthesis of IPPU elastomer

The synthesis process of IPPU elastomer is as follows: first, IPDI (0.29 g, 1.3 mmol) was dissolved in 5 ml THF in a three-neck flask. Subsequently, NH₂-PDMS-NH₂ (2.5 g, 1.0 mmol) dissolved in 5 ml THF was slowly added to the three-neck flask, and nitrogen was continuously injected into the reaction system during the drip process, and the temperature of the reaction system is cooled to 0 °C with an ice-water bath, and the prepolymer is obtained by stirring at 0 °C for 3 h. Then, ATTI (94 mg, 0.365 mmol) in 5 mL THF was slowly dripped into the reaction system, and reacted at 0 °C for 6 h until the chain extension was completed. Finally, the obtained IPPU polymer was poured into the silica mold and placed in the fume hood overnight. To remove excess solvent in the film, the resulting transparent film was first placed in a hot-plate for 24 h, and then transferred to a vacuum drying oven at 40 °C for 48 h for subsequent characterization and testing.

Fabrication of IPPU-GF_x composites

First, IPPU, GTPs and FeCl₃ were dissolved into THF to prepare a solution of 0.125 mg L⁻¹, 0.14 mol L⁻¹, and 0.096 mol L⁻¹, respectively. Then, GTPs solution (0.25 ml) was added into the IPPU solution. After stirring for 10 min, the FeCl₃ solution (0.25 ml) was added into the above mixture. After further stirring at room temperature for 20 min, the composites solution was poured into a peri dish, and placed in the fume hood for 24 h to remove the solvent. Finally, the obtained IPPU-GF_x composite film was put into the vacuum oven at 40 °C for 48 h to fully remove the remained solvent. It is worth noting that other IPPU-GF_x composites are prepared using the same method.

Self-healing procedures of IPPU and IPPU-GF_x

The IPPU and IPPU-GF_x samples were cut into two separate two halves with a surgical blade and then the cutting surfaces of the two halves were fully contacted and placed in a rubber mold and healed at 75 °C for different times (3 h, 6 h, 9 h, 12 h, 15 h).

Antibacterial experiment

Before the antibacterial experiment, all the instruments and equipment were aseptically treated. IPPU, IPPU-GF_x, and PE control films with the size of 1.5 × 1.5 cm² were placed in a 6-well plate and S. aureus suspension (25 μL) was added at the center region of the films. PE film was used to cover the S. aureus suspension subsequently. After cultivated at 37 °C for 6 h, the samples were immersed in 1 mL of phosphate-buffered saline (PBS) buffer and the adherent bacteria was released into PBS solution via ultrasound. The bacterial stock solution (80 μL) was dropped onto the medium, evenly coated, and cultured in an incubator at 37 °C for 24 h for colony counting.

Results and discussion

Synthesis and characterization of MPNs-based PDMS elastomers (IPPU-GF_x)

For the preparation of MPNs-based PDMS elastomers, a PDMS-based polyurea elastomer (IPPU) was first synthesized. As shown in Fig. 1a, NH₂-PDMS-NH₂ was first reacted with IPDI to produce the polyurea prepolymer. Then, ATTI was introduced as chain extender to obtain the IPPU elastomer (Fig. S1 and S2†). Subsequently, the MPNs were introduced into the polymer networks of IPPU elastomer by continuous addition of GTPs and FeCl₃. The detailed fabrication process of MPNs-based PDMS elastomers was shown in Fig. 1b and c. First, the IPPU elastomer film was dissolved in THF. Then, the GTPs dissolved in THF are added to the above THF solution to produce the IPPU-GTPs composites solution. After that, different amounts of FeCl₃ were slowly added into the IPPU-GTPs composites solution. Finally, the targeted IPPU-GF_x (where “x” represented the mass ratio between the sum of the masses of GTPs and FeCl₃ and the IPPU) films with different MPNs contents were obtained after fully removing solvent. By tailoring the content of GTPs and FeCl₃, three IPPU-GF_x were fabricated as IPPU-GF_0.5%, IPPU-GF_1%, and IPPU-GF_2%, respectively. Fig. 1c shows the schematic representation of the fabrication process of IPPU-GF_x. In the pure IPPU elastomer film, the urea bonds will form multiple hydrogen-bonding interactions in the polymer network, promoting the formation of microphase structures in the polymer network. After complexing with GTPs, the hydroxyl groups and ester bonds in GTPs will further form hydrogen bonds with the urea bonds in IPPU, which will further improve the cross-linking density of the polymer networks. When adding FeCl₃ into the above networks, the MPNs will in situ generate in the polymer networks of IPPU via the metal–ligand interaction between Fe³⁺ and catechol structures. The interactions between the hydroxyl groups in GTPs and Fe³⁺ were tested using FTIR spectra. As shown in Fig. S4,† the characteristic peak of –COOH in GTPs at 1645 cm⁻¹ disappeared in the FTIR spectra of all the three GTP:Fe³⁺ composites, which indicated that the carboxyl group forms a coordination bond with the trivalent iron ion. Meanwhile, the characteristic peak of –OH in GTPs at 3388 cm⁻¹ increased to 3410 cm⁻¹ in the GTP:Fe³⁺ composites, indicating the formation of metal–ligand interaction between polyphenols and trivalent iron in the GTP:Fe³⁺ composites. Meanwhile, the transparent IPPU elastomer film transformed into to a dark coloured IPPU-GF_x film (Fig. 1c). This apparent colour changing can be attributed to the ligand-to-metal charge-transfer (LMCT) of the MPNs (Fig. 1d).^22,30 The ability of GTPs to coordinate with metal ions and form coordination polymers depends on the incomplete filling of d-orbitals in transition metal ions. When FeCl₃ was added to the IPPU-GTPs solution, the previously introduced GTPs in the polymer networks can combine with Fe³⁺ through the coordination reaction, thus forming polyurethane composite with a metal-polyphenol cross-linked structure. Small-angle X-ray diffraction (SAXS) experiments were conducted to evaluate the phase separation structures of the IPPU and IPPU-GF_x elastomers. As shown in Fig. S5,† all the elastomers showed distinct scattering peaks and the periodicity of the phase-separated domains in the PDMS-based elastomers were gradually increased from 5.92 nm to 6.16 nm with the increasing content of MPNs.

Mechanical and thermal properties of IPPU and IPPU-GF_x elastomers

The successful construction of the MPNs in the polymer networks of IPPU endowed the PDMS-based IPPU-GF_x elastomers with excellent mechanical and thermal properties. Then, the mechanical properties of IPPU and IPPU-GF_x elastomers were evaluated using tensile tests (Fig. 2a). The introduction of MPNs will increase the cross-linking density of the polymer networks through the formation of multiple hydrogen-binding interactions and metal–ligand interactions, which will also restrict the motion of the polymer chain segment during stretching the IPPU-GF_x samples, thus, resulting in the increase of their modulus and strength. As shown in Fig. 2a, the Young's modulus increased from ∼3.2 MPa for IPPU to ∼7.1 MPa for IPPU-GF_x and the tensile strength increased from ∼3.4 MPa for IPPU to ∼7.7 MPa for IPPU-GF_x. Meanwhile, with the increasing content of MPNs in the polymer networks, their toughness and tensile strain also increased (Table S1†). To further confirm the effectiveness of the above strategy, two control sample IPPU-GTPS and IPPU-Fe³⁺ were fabricated and their tensile stress–strain curves were recorded in Fig. S6.† As shown in Fig. S6,† the mechanical properties of both the IPPU-GTPS and IPPU-Fe³⁺ increased after complexing IPPU with 1% GTPs and 1% Fe³⁺. This increase in mechanical properties can be attributed to the increased physical cross-linking including multiple hydrogen binding interactions of GTPS and IPPU and metal ligand interactions of Fe³⁺ and IPPU. However, the mechanical strength and Young's modulus of IPPU-GTPS and IPPU-Fe³⁺ were much lower than those of IPPU-GF_x elastomers, which indicated that simply introducing GTPS or Fe³⁺ into the polymer networks of IPPU was not enough to enhance the mechanical properties. Therefore, we can conclude that introducing both GTPS or Fe³⁺ into the polymer networks of IPPU to construct MPNs is necessary for the enhancement of the mechanical properties of IPPU-GF_x elastomers. It also should be noted that the mechanical strength and toughness of IPPU-GF_x elastomers are comparable to those of the recently reported PDMS-based elastomers (Fig. 2b).^{6,12,13,16,32–40} The thermal properties of IPPU and IPPU-GF_x elastomers were evaluated with DMA, DSC, and TGA. The DMA results show that the IPPU and IPPU-GF_x elastomers exhibit two T_gs due to the presence of soft and segments in the polymer network of PDMS-based polyurea elastomer. All four PDMS-based polyurea elastomers exhibited the same T_g value of −115 °C attributed to the soft segment of PDMS (Fig. 2c). Interestingly, with the increasing of MPNs content in the polymer networks, the T_g value of the hard segments gradually increased from 80.3 °C for IPPU to 90.1 °C for IPPU-GF_2%, which can be attributed to the cross-linking effect of hydrogen bonds and metal–ligand interactions from MPNs. At the same time, the storage modulus (E′) of IPPU and IPPU- GF_x elastomers also increase in the same trend as that of the T_g value of the hard segments at 25 °C (Fig. 2d). When the temperature was further increased from 25 °C to 100 °C, the E′ values decrease rapidly, which can be ascribed to the dynamic association-dissociation process of the hydrogen bonds and metal–ligand interactions at high temperatures. It can be seen from the DSC curve that the IPPU and IPPU-GF_x elastomers have no obvious glass transition or melt point in their heating curves, indicating that the prepared elastomers are amorphous (Fig. 3e). The TGA results show that the initial decomposition temperatures (T_d5%) of all IPPU and IPPU-GF_x elastomers were near 280 °C (Fig. 3f), which indicated that the as-prepared IPPU and IPPU-GF_x elastomers also exhibited good thermal stability.

Healing ability of the IPPU and IPPU-GF_x elastomers

Based on the existence of numerous reversible hydrogen bonds and metal–ligand interactions in their polymer networks and the sufficient mobility of the PDMS chain segments, the IPPU and IPPU-GF_x elastomers exhibited excellent healing ability. To explore their healing capacity, the specimens of the PDMS-based elastomers were first cut into two halves with a knife, and then the cutting surfaces of the two halves were fully contacted and undergo a healing process for different durations. As shown in Fig. 3a, the fully damaged IPPU-GF_1% elastomers can be healed after healing at 75 °C for 15 h. Meanwhile, the healed specimen could be arbitrary bending, twisting, and even hold a ∼200 g in weight without fracture (Fig. 3a). Fig. 3b depicts the representative stress–strain curves for the healed and original IPPU elastomer samples, which indicated that the healing efficiency of the IPPU elastomer was dependent on time. After healing for 6 h at 75 °C, the healing efficiency can reach nearly ∼97.2% (Fig. 3c). As the increasing of physical cross-linking density derived from the construction of MPNs, the polymer chain segment mobility will be restricted, leading to the decrease in the healing capacity of IPPU-GF_x elastomers. As shown in Fig. 3d, e, and S5,† with the increase content of MPNs in their polymer networks, the healing efficiency of IPPU-GF_x elastomers exhibited remarkable decreases. For example, the healing efficiency of the damaged IPPU-GF_1% sample was only 14.5% after healing 9 h at 75 °C. Due to the time-dependent healing behavior, the damaged IPPU-GF_x elastomers still can be fully healed by prolonging the healing times. For example, after healing for 15 h, the healing efficiency of IPPU-GF_1% sample can reach ∼99.7% (Fig. 3e). Besides, the damaged IPPU-GF_0.5% samples can also be healed with a high healing efficiency of ∼87.1% within 15 h, and the damaged IPPU-GF_2% samples can be healed with a high healing efficiency of ∼90.9% within 15 h (Fig. S7†). It should be pointed out that the healing ability of the IPPU-GF_x elastomers is comparable to that of the reported PDMS-based elastomers in comparison with stress, healing temperature, and healing time (Fig. 3f).^{6,7,9,12,13,15,18–20,32,37–45} In situ variable-temperature FTIR experiments were conducted on IPPU and IPPU-GF_x elastomers to confirm the self-healing mechanism. As shown in Fig. S8,† the characteristic peak of the free CO in urea bonds gradually moved to high wavenumbers with the increase in temperature, and the characteristic peak of the free –NH in urea bonds gradually moved to low wavenumbers with the increase in temperature. These results indicated the dissociation of hydrogen bonds under heating. Meanwhile, the characteristic peak of the free –OH in GTPs moved to low wavenumbers with the increase in temperature (Fig. S8c†), which indicates the dissociation of hydrogen bonds and metal ligand interactions under heating. The healing mechanism of IPPU and IPPU-GF_x elastomers is as follows: under heating, the exchange reaction of hydrogen bonds and metal–ligand interactions on the fractured surface of the damaged sample is activated and the polymer chain segment is also activated. When the damaged surfaces touch each other, the polymer chain segments on the damaged surface will diffuse through the surfaces and the dynamic bonds gradually approach each other and rebuild over time (Fig. S9†). When the bonded elastomers are cooled to room temperature, the integrity of the broken elastomer was restored and regain their original mechanical properties. It should be pointed out that the normal human body temperature is around ∼37 °C, and local tissue temperatures during normal operation rarely exceed 40 °C–42 °C. Therefore, to be honest, the healing temperature of 75 °C is relatively high for most medical applications, especially those involving the human body. However, we think that when the medical devices are primarily applied in external or wearable applications where controlled heating is feasible and safe, the healing temperature of 75 °C may be suitable. For these devices, we can use warm compress or mild heating to carry out the self-healing process when they were damaged. In the future, we will explore more advanced methods to develop spontaneous self-healing PDMS-based PU elastomers that can be directly used in in vivo or inside the body.

Antibacterial properties of IPPU and IPPU-GF_x elastomers

For practical usage of the PDMS-based elastomers in the field of medical devices, it is necessary to endow them with well antibacterial ability.^18,46 The natural polyphenol-based MPNs usually seemed as a class of antibacterial materials.^26,27 Therefore, it can be inferred that IPPU-GF_x elastomers which composed of PDMS-based polyurea elastomers and metal-natural polyphenol complexes would exhibit excellent antibacterial ability. To verify their antibacterial ability, the antibacterial experiments were carried out by co-culturing IPPU and IPPU-GF_x elastomer membranes and E. coli or S. aureus. Fig. 4a and b show the optical images of bacterial colony-forming units (CFUs) on the Agar plates. As a control, commercial PE film was selected as the negative group and it exhibited antibacterial activity against E. coli or S. aureus after 6 h exposure. In contrast, IPPU and IPPU-GF_x elastomers showed good antibacterial ability after co-cultured with E. coli or S. aureus for 6 h. The antibacterial efficiency of IPPU film against E. coli or S. aureus was 98% after 6 hours of exposure. Interestingly, the antibacterial efficiency of IPPU-GF_x elastomers against E. coli or S. aureus increased with the increasing contents of MPNs in the polymer networks. As shown in Fig. 4d, the antibacterial efficiency of IPPU-GF_x film against E. coli increased from 62% to 83%, while the antibacterial efficiency of IPPU-GF_x film against S. aureus increased from 82% to 100%, respectively. The above results show that IPPU and IPPU-GF_x elastomers have good antibacterial activity. Fig. 4d describes the antimicrobial mechanism of IPPU and IPPU-GF_x elastomers. When the E. coli or S. aureus contact with IPPU and IPPU-GF_x elastomers, special chemical structure, including amino groups on the end of IPPU and the phenolic hydroxyl groups in GTPs will interact with the microbial, making collapse of the bacteria and leakage of the cytoplasm, which will lead to the death of E. coli or S. aureus (Fig. 4d).

Conclusions

In summary, we have demonstrated a supramolecular engineering strategy to fabricate high-performance PDMS-based polyurea elastomers (IPPU-GF_x) that simultaneously achieve exceptional mechanical strength, excellent self-healing ability, and intrinsic antibacterial activity through the in situ integration of metal-phenolic networks (MPNs). The incorporation of MPNs introduces a dual dynamic cross-linking system including hydrogen-binding interactions and metal–ligand interactions in the polymer networks of PDMS-based polyurea elastomers. The resultant IPPU-GF_x exhibited excellent mechanical properties including both high mechanical strength and toughness, which are remarkable to those of recently reported PDMS-based elastomers. Meanwhile, the mechanical properties of IPPU-GF_x elastomers can be finely controlled by simply tailoring the content of MPNs in the polymer networks of IPPU-GF_x. For example, the IPPU-GF_1% elastomer exhibited the best comprehensive mechanical properties including high tensile strength of ∼7.7 MPa, elongation at break of ∼823.4%, and toughness is ∼39.2 MJ m⁻³, respectively. At the same time, all the IPPU and IPPU-GF_x elastomers exhibited good healing ability. For example, the damaged IPPU elastomer can effectively healed within 6 h at 75 °C with a high healing efficiency of ∼97.2% and the damaged IPPU-GF_1% elastomer can also be healed with near ∼99.7% healing efficiency at 75 °C in 15 h. Moreover, the IPPU and IPPU-GF_x elastomers exhibited good antibacterial activity against S. aureus and E. coli, which showed good potential application in the field of medical devices. Overall, the strategy we designed to create high-performance PDMS-based elastomers by simply constructing MPNs in their polymer networks pave an efficient way to develop high performance PDMS elastomers that occupy the potential for use in medical devices.

Author contributions

The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript.

Conflicts of interest

There are no conflicts to declare.

Data availability

The data supporting this article have been included as part of the ESI.†

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 22005261 and 22303077), Fundamental Research Projects of Science & Technology Innovation and Development Plan in Yantai City (No. 2023JCYJ082), Science Fund of Shandong Laboratory of Advance Materials and Green Manufacturing at Yantai (No. AMGM2024F1), National Science Foundation of Shandong Province (No. ZR2023QB163), and Taishan Scholar Project of Shandong Province (tsqn202306160).

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Footnote

† Electronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d5py00629e

This journal is © The Royal Society of Chemistry 2025