Boronic ester-based vitrimeric methylvinyl silicone elastomer with “solid-liquid” feature and rate-dependent mechanical performance

Zhao, Yongsheng; Qin, Tian; Jiang, Chaobo; Li, Jialiang; Xiong, Youhao; Liu, Shiyuan; Qin, Jianbin; Shi, Xuetao; Zhang, Guangcheng

doi:10.1016/j.polymer.2022.125545

Cited by 15 publications

(12 citation statements)

References 60 publications

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“…Furthermore, both the crosslinker and the cured networks show vibrations at 1350 cm −1 as expected for Si−O−B bonds. 35 These data are further reinforced by 29 Si NMR (Figure 3b): a distinct peak at δ = 0.8 ppm in the cross-linker shifts to δ = 13 ppm after the addition of PDMS Si− H units to the vinyl groups. Peaks corresponding to Si−H bonds in the PDMS prepolymer that are present between δ = −35 to − 39 ppm also disappear upon coupling.…”

Section: ■ Introductionmentioning

confidence: 77%

Facile Preparation of Tunable Polyborosiloxane Networks via Hydrosilylation

D’Ambra,

Getty,

Eom

et al. 2024

Chem. Mater.

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Polyborosiloxanes are used in a variety of fields due to their unique dynamic properties. Traditionally, cross-linked polyborosiloxanes are prepared by incorporating boric acid into siloxane prepolymers, a process that is timeconsuming, energy intensive, and challenging due to reagent immiscibility. Here, we report a versatile synthetic method to rapidly cure polyborosiloxane networks via hydrosilylation of chain end or backbone functionalized polydimethylsiloxane (PDMS) derivatives with an inexpensive trivinylboronate. Networks synthesized from these readily available building blocks cure in ∼2 min at convenient temperatures (e.g., 90 °C) and exhibit enhanced viscoelastic behavior when compared to traditional polyborosiloxane networks fabricated via the conventional condensation route. By virtue of using efficient hydrosilylation chemistry, another key advantage of this synthetic platform is the ability to synthesize dynamic polyborosiloxanes with different network connectivity by simply using silicones with Si−H moieties placed at the chain ends (end-group) or distributed throughout the repeat-unit structure (pendant-group). The availability of other alkenes amenable to hydrosilylation provides an additional formulation handle to synthesize mixed dynamic−static networks with tunable control over stress relaxation and solvent resistance. In summary, the synthetic approach disclosed herein is a simple and accessible platform for preparing dynamic polyborosiloxanes with tunable material properties.

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Section: ■ Introductionmentioning

confidence: 77%

Facile Preparation of Tunable Polyborosiloxane Networks via Hydrosilylation

D’Ambra,

Getty,

Eom

et al. 2024

Chem. Mater.

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“…[18] The topology freezing transition temperature of the material was determined to be 5.5 °C by the extrapolation of the Arrhenius fitted line to when the stress relaxation time (τ*) was 2.5×10 6 s, which is similar to Zhao et al's reported work (6.4 °C). [10]…”

Section: Thermal Properties Of Fbe15mentioning

confidence: 99%

“…Materials containing boronic esters are interesting as it is possible to selfheal at ambient conditions as the topology freezing transition temperature is often below room temperature which allows for bond exchange to occur at room temperature. [10] Boronic esters also imparts strong covalent linkages to the polymer matrix which undergoes dynamic exchange via both associative and dissociative mechanisms in the presence of free À OH groups or moisture respectively. [11] Evidently, the self-healing capabilities of such materials is an important property to be considered in assessing the bulk material's reusability.…”

Section: Introductionmentioning

confidence: 99%

“…The multitude of self‐healing mechanisms available allows tuning of the material's mechanical properties and self‐healing capabilities by the choice of dynamic interactions and bonds. Materials containing boronic esters are interesting as it is possible to self‐heal at ambient conditions as the topology freezing transition temperature is often below room temperature which allows for bond exchange to occur at room temperature [10] . Boronic esters also imparts strong covalent linkages to the polymer matrix which undergoes dynamic exchange via both associative and dissociative mechanisms in the presence of free −OH groups or moisture respectively [11] …”

Section: Introductionmentioning

confidence: 99%

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Ultrafast Self‐Healing Elastomer with Closed‐Loop Recyclability

Mah,

Li,

Feng

et al. 2024

Chemistry An Asian Journal

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The loss of function after prolonged periods of use is inevitable for all materials including plastics. Hence, self‐healing capabilities are a key development to prolong the service lifetime of materials. One of such self‐healing capabilities can be achieved by integrating dynamic bonds such as boronic ester linkages into polymeric materials, however the rate of self‐healing in these materials is insufficient and current methods to accelerate it are limited. In this study, we report the rational design, synthesis and characterization of a fluorinated elastomer (FBE15) that utilizes enhanced interaction between polymer chains afforded by strong dipole‐dipole interactions from −CF3, which showed a significant increase in binding energy to −7.71 Kcal/mol from −5.51 Kcal/mol, resulting in increased interaction between the boronic ester linkages and improving self‐healing capabilities of boronic ester materials, drastically reducing the time required for stress relaxation by 900 %. The bulk elastomer is capable of ultrafast self‐healing in a one‐click fashion that can happen in mere seconds, which can then be stretched to 150 % of its original length. By utilising the dynamic cross‐linking, FBE15 is also capable of both mechanical reprocessing into the same materials and chemical recycling into its starting materials, respectively, further allowing reconstruction of the elastomers that have comparable properties to the original ones at the end of its service lifespan.

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“…The widely used plastics such as polystyrene, polypropylene, polyvinyl chloride, etc., are composed of stable covalent bond and di cult to degrade, the abandoned plastic products have caused serious pollution to soil and sea. Recently, researchers are committed to build new polymer materials based on dynamic covalent bonds such as typical hydroxyl transesteri cation reactions, disul de bonds [1][2][3], dynamic imine bond [4], borate ester bond [5], etc. Under the stimulation of heat, light, force and pH, the breaking and recombination of dynamic covalent bond in the polymer materials can induce the dynamic adjustment of polymer networks.…”

Section: Introductionmentioning

confidence: 99%

Adaptable bio-based dynamically cross-linked networks via disrupting physical cross-linking and chain entanglement for electromagnetic interference shielding materials

Chen

Jia

et al. 2023

Preprint

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Dynamically cross-linked networks combine the uniqueness of thermoplastics and thermosets to allow for reprocessability while being covalently crosslinked, but the lack of functionality seriously limits practical applications. Here, we propose a strategy to develop tung oil based dynamically cross-linked networks (PNMETs) by introducing primary amine to disrupt the physical cross-linking and chain entanglements, and achieved tunable mechanical strength and toughness, chemical stability, self-healing, solid state plasticity, and topological transformation. The constructed PNMETs based on hydrogen bonds and the dynamic imine bond exhibited multiple stimulus responses for light, heat, microwave and infrared radiation, and achieved excellent recycling and self-healing without any catalyst. By doping multiwalled carbon nanotubes (MWCNTs) and nano Fe3O4 in PNMETs, the resulted electromagnetic interference (EMI) shielding materials (PNMETs/MWCNT@Fe3O4) were fabricated and realized dual characteristics of dynamically cross-linked networks and EMI shielding material for the first time. PNMETs/MWCNT@Fe3O4 composite based on the topological rearrangement of PNMETs showed shape memory behavior, reprocessing, recycling and self-healing property under the conditions of infrared radiation and voltage, as well as exhibited EMI shielding effectiveness of 20–23 dB in the X-band with thickness less than 1 mm, meeting the standards for commercial applications. This work provides a simple but highly practical strategy for the fabrication of functional materials that integrated with dynamically cross-linked polymer and EMI shielding performance suitable for harsh environments.

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Boronic ester-based vitrimeric methylvinyl silicone elastomer with “solid-liquid” feature and rate-dependent mechanical performance

Cited by 15 publications

References 60 publications

Facile Preparation of Tunable Polyborosiloxane Networks via Hydrosilylation

Facile Preparation of Tunable Polyborosiloxane Networks via Hydrosilylation

Ultrafast Self‐Healing Elastomer with Closed‐Loop Recyclability

Adaptable bio-based dynamically cross-linked networks via disrupting physical cross-linking and chain entanglement for electromagnetic interference shielding materials

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