Effect of cross‐linking on the mechanical properties, degree of crystallinity and thermal stability of polyethylene vitrimers

Montoya-Ospina, Maria Camila; Verhoogt, H.; Ordner, Mark; Tan, Xiao; Osswald, Tim A.

doi:10.1002/pen.26178

Cited by 31 publications

(27 citation statements)

References 41 publications

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“…For all samples, HDPE exhibited higher E′ compared to HDPE-V. Previous research has demonstrated a linear relationship between crystallinity and stiffness [ 35 ]. Higher crystallinity in HDPE explains its higher modulus compared to HDPE-V. HDPE samples tested in the 0° orientation showed a drop of approximately 100 MPa in E′ relative to compression-molded HDPE, while the 90° orientation showed a drop of around 300 MPa.…”

Section: Resultsmentioning

confidence: 85%

“…HDPE-V was obtained from the reaction of HDPE-MAH and the diamine crosslinker containing disulfide bonds—4,4′ dithiodianiline (DTA)—as described in a previous work [ 35 ]. The concentration of MAH was 0.3% wt., and a molar ratio of 1:0.5 (MAH:DTA) was used.…”

Section: Methodsmentioning

confidence: 99%

“…In a previous study, it was shown that vitrimers prepared from HDPE (HDPE-V) significantly affect the properties of the material in the melt and solid states [ 35 ]. In the melt state, the crosslinks in HDPE-V were responsible for its superior dimensional stability at elevated temperatures, due to the presence of a rubbery plateau compared to un-crosslinked HDPE.…”

Section: Introductionmentioning

confidence: 99%

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Material Extrusion Additive Manufacturing with Polyethylene Vitrimers

et al. 2023

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Polyethylene (PE) is one of the most widely used polymers in conventional polymer manufacturing processes. However, it remains a challenge to use PE in extrusion-based additive manufacturing (AM). Some of the challenges that this material presents include low self-adhesion and shrinkage during the printing process. These two issues lead to higher mechanical anisotropy when compared to other materials, along with poor dimensional accuracy and warpage. Vitrimers are a new class of polymers that have a dynamic crosslinked network, allowing the material to be healed and reprocessed. Prior studies on polyolefin vitrimers suggest that the crosslinks reduce the degree of crystallinity and increase the dimensional stability at elevated temperatures. In this study, high-density polyethylene (HDPE) and HDPE vitrimers (HDPE-V) were successfully processed using a screw-assisted 3D printer. It was demonstrated that HDPE-V were able to reduce shrinkage during the printing process. This shows that 3D printing with HDPE-V will provide better dimensional stability when compared to regular HDPE. Furthermore, after an annealing process, 3D-printed HDPE-V samples showed a decrease in mechanical anisotropy. This annealing process was only possible in HDPE-V due to their superior dimensional stability at elevated temperatures, with minimal deformation above melting temperature.

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Section: Resultsmentioning

confidence: 85%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Material Extrusion Additive Manufacturing with Polyethylene Vitrimers

et al. 2023

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“…Since the cross-linking density of PCG- X s increases as the content of the cross-linker (PEG-NH 3 ) increases, the glass-transition temperature ( T g ) and elastic modulus of PCG- X s also increase as the PEG-NH 3 content increases up to 7.5 wt % (Table ). , However, when the content of PEG-NH 3 increases to 10.0 wt %, the T g and elastic modulus decrease due to the increase in the content of the flexible ethylene oxide units . The strong mechanical strength of the polymer binder can improve the cell performance of the Si anode because it can help maintaining the electrode structure from the Si volume change during the charging/discharging process. , Although the T g value of PCG-7.5 is the highest at 65.8 °C, the difference is less than 4 °C, so it is unlikely to significantly affect the cell performance.…”

Section: Resultsmentioning

confidence: 99%

Ion-Conducting Cross-Linked Polyphosphazene Binders for High-Performance Silicon Anodes in Lithium-Ion Batteries

Hong

Jeong

Koong

et al. 2023

ACS Appl. Polym. Mater.

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A cross-linked polyphosphazene-based polymeric material was prepared using NH3-neutralized poly[bis(4-carboxyphenoxy)phosphazene] (PCPP-NH3) as the base polymer and poly(ethylene glycol)bisamine (PEG-NH3) as a cross-linker for use as a silicon (Si) anode binder in lithium-ion batteries. PCPP was prepared by two-step polymer modification reactions from poly(dichlorophosphazene). When an optimum amount of PEG-NH3 (7.5 wt % of PCPP-NH3) was used as the cross-linker, the resulting cross-linked polyphosphazene exhibited the highest glass-transition temperature, elastic modulus, and peeling force values. The battery performance of the cells with the Si anode fabricated with this cross-linked polyphosphazene-based binder was found to be better than that of cells with Si anodes fabricated with the poly(acrylic acid) binder. The better performance of the cell with the polyphosphazene-based binder was ascribed to the composition and structure of the binder material: the flexible polyphosphazene backbone, the carboxylic acid group with hydrogen bonding ability, and the cross-linked network structure maintained the electrode structure during charge/discharge cycling of the cell. Furthermore, the ion-conducting PEG moieties increased the ion-transfer conductivity inside the Si anode.

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“…Thus, incorporating DCBs within self-assembled systems offers one way to realize reprocessable high-performance materials. Recent work has shown that incorporating dynamic bonds within crystalline systems is useful to modulate rheological properties, − crystallinity, and mechanical properties. , A less explored opportunity, however, is the possibility to exploit bond exchange reactions to modulate pathways of self-assembly. Preliminary work in block copolymer , and semicrystalline , polymers suggests that nano- and mesoscale assembly and morphologyand thus emergent propertiesare altered by DCBs.…”

mentioning

confidence: 99%

Catalytic Control of Crystallization in Dynamic Networks

Kuenstler

Bowman

2023

ACS Macro Lett.

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The effect of catalysts with varying nucleophilic strength on thiol−thioester bond exchange dynamics and concomitant crystallization was studied in a model semicrystalline polymer network. It was found that the characteristic time scale of covalent bond exchange, τ, could be tuned over a ∼10 1 −10 3 s range simply by changing the nucleophilicity of the catalyst. Using isothermal crystallization measurements via differential scanning calorimetry, thermodynamic and kinetic features of crystallization were considered. A depression in melting temperature was observed with increasing bond exchange rate, suggesting a dependence of crystalline organization on network dynamics. Furthermore, a systematic slowing of crystallization kinetics with faster covalent bond exchange rates was observed. Lauritzen−Hoffman analysis showed a near doubling in the barrier for secondary nucleation for dynamic networks, suggesting that that bond exchange slows crystallization by limiting secondary nucleation and further growth. Finally, longitudinal DSC studies reveal a long-term increase in melting temperature for samples held at ambient temperature with bond exchange activated at room temperature, indicating that while bond exchange slows crystallization on short time scales it facilitates isothermal long-term crystal rearrangement and growth on longer time scales.

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Effect of cross‐linking on the mechanical properties, degree of crystallinity and thermal stability of polyethylene vitrimers

Cited by 31 publications

References 41 publications

Material Extrusion Additive Manufacturing with Polyethylene Vitrimers

Material Extrusion Additive Manufacturing with Polyethylene Vitrimers

Ion-Conducting Cross-Linked Polyphosphazene Binders for High-Performance Silicon Anodes in Lithium-Ion Batteries

Catalytic Control of Crystallization in Dynamic Networks

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