Manipulating the Properties of Polymer Vitrimer Nanocomposites by Designing Dual Dynamic Covalent Bonds

Li, Zhenyuan; Zhao, Hengheng; Duan, Pengwei; Zhang, Liqun; Liu, Jun

doi:10.1021/acs.langmuir.4c00699

Cited by 2 publications

(4 citation statements)

References 53 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The results demonstrated that the nanocomposite systems that retain a higher nanorod orientation exhibited a superior modulus and mechanical strength [116]. Another recent simulation effort containing unentangled (with N = 60 monomers) vitrimers and spherical nanoparticles was implemented by MD using coarse-grained models [117]. It was shown be independent of BERs in the vitrimer matrix and interface [117].…”

Section: Coarse-grained Modeling On Vitrimer Nanocompositesmentioning

confidence: 99%

“…It was shown be independent of BERs in the vitrimer matrix and interface [117]. By varying the ∆E sw in the matrix and interface, it was shown that an appropriate ∆E sw value is beneficial not only to ensure enough BERs to homogenize the fracture region but also to obtain a certain network strength in achieving a high dissipation work [117].…”

Section: Coarse-grained Modeling On Vitrimer Nanocompositesmentioning

confidence: 99%

“…Another recent simulation effort containing unentangled (with N = 60 monomers) vitrimers and spherical nanoparticles was implemented by MD using coarse-grained models [117]. It was shown be independent of BERs in the vitrimer matrix and interface [117]. By varying the ∆E sw in the matrix and interface, it was shown that an appropriate ∆E sw value is beneficial not only to ensure enough BERs to homogenize the fracture region but also to obtain a certain network strength in achieving a high dissipation work [117].…”

Section: Coarse-grained Modeling On Vitrimer Nanocompositesmentioning

confidence: 99%

See 2 more Smart Citations

Molecular Simulation of Covalent Adaptable Networks and Vitrimers: A Review

Karatrantos,

Couture,

Hesse

et al. 2024

Polymers

View full text Add to dashboard Cite

Covalent adaptable networks and vitrimers are novel polymers with dynamic reversible bond exchange reactions for crosslinks, enabling them to modulate their properties between those of thermoplastics and thermosets. They have been gathering interest as materials for their recycling and self-healing properties. In this review, we discuss different molecular simulation efforts that have been used over the last decade to investigate and understand the nanoscale and molecular behaviors of covalent adaptable networks and vitrimers. In particular, molecular dynamics, Monte Carlo, and a hybrid of molecular dynamics and Monte Carlo approaches have been used to model the dynamic bond exchange reaction, which is the main mechanism of interest since it controls both the mechanical and rheological behaviors. The molecular simulation techniques presented yield sufficient results to investigate the structure and dynamics as well as the mechanical and rheological responses of such dynamic networks. The benefits of each method have been highlighted. The use of other tools such as theoretical models and machine learning has been included. We noticed, amongst the most prominent results, that stress relaxes as the bond exchange reaction happens, and that at temperatures higher than the glass transition temperature, the self-healing properties are better since more bond BERs are observed. The lifetime of dynamic covalent crosslinks follows, at moderate to high temperatures, an Arrhenius-like temperature dependence. We note the modeling of certain properties like the melt viscosity with glass transition temperature and the topology freezing transition temperature according to a behavior ruled by either the Williams–Landel–Ferry equation or the Arrhenius equation. Discrepancies between the behavior in dissociative and associative covalent adaptable networks are discussed. We conclude by stating which material parameters and atomistic factors, at the nanoscale, have not yet been taken into account and are lacking in the current literature.

show abstract

Section: Coarse-grained Modeling On Vitrimer Nanocompositesmentioning

confidence: 99%

Section: Coarse-grained Modeling On Vitrimer Nanocompositesmentioning

confidence: 99%

Section: Coarse-grained Modeling On Vitrimer Nanocompositesmentioning

confidence: 99%

See 1 more Smart Citation

Molecular Simulation of Covalent Adaptable Networks and Vitrimers: A Review

Karatrantos,

Couture,

Hesse

et al. 2024

Polymers

View full text Add to dashboard Cite

show abstract

“…Moreover, accurately establishing the quantitative relationship between the microstructures of these materials and their macroscopic properties is still a challenge, severely limiting the optimization of material properties. Interestingly, previous studies have acknowledged that the molecular dynamics (MD) simulation method is a powerful technique capable of providing insights into materials with complex compositions and revealing the structure–mechanics relationship at the molecular level. − MD simulations have proven to be an effective method for studying the role of hydrogen bonds, facilitating a deeper understanding of this interaction. − These studies also illustrate the feasibility of employing MD simulations to investigate NR containing hydrogen bonds.…”

Section: Introductionmentioning

confidence: 99%

Impact of Sacrificial Hydrogen Bonds on the Structure and Properties of Rubber Materials: Insights from All-Atom Molecular Dynamics Simulations

Chen,

Huang,

Zhang

et al. 2024

Langmuir

Self Cite

View full text Add to dashboard Cite

The inclusion of sacrificial hydrogen bonds is crucial for advancing high-performance rubber materials. However, the molecular mechanisms governing the impact of these bonds on material properties remain unclear, hindering progress in advanced rubber material research. This study employed all-atom molecular dynamics simulations to thoroughly investigate how hydrogen bonds affect the structure, dynamics, mechanics, and linear viscoelasticity of rubber materials. As the modified repeating unit ratio (β) increased, both interchain and intrachain hydrogen bond content rose, with interchain bonds playing a predominant role. This physical cross-linking network formed through interchain hydrogen bonds restricts molecular chain movement and relaxation and raises the glass transition temperature of rubber. Within a certain content of hydrogen bonds, the mechanical strength increases with increasing β. However, further increasing β leads to a subsequent decrease in the mechanical performance. Optimal mechanical properties were observed at β = 6%. On the other hand, a higher β value yields an elevated stress relaxation modulus and an extended stress relaxation plateau, signifying a more complex hydrogen-bond cross-linking network. Additionally, higher β increases the storage modulus, loss modulus, and complex viscosity while reducing the loss factor. In summary, this study successfully established the relationship between the structure and properties of natural rubber containing hydrogen bonds, providing a scientific foundation for the design of high-performance rubber materials.

show abstract

Manipulating the Properties of Polymer Vitrimer Nanocomposites by Designing Dual Dynamic Covalent Bonds

Cited by 2 publications

References 53 publications

Molecular Simulation of Covalent Adaptable Networks and Vitrimers: A Review

Molecular Simulation of Covalent Adaptable Networks and Vitrimers: A Review

Impact of Sacrificial Hydrogen Bonds on the Structure and Properties of Rubber Materials: Insights from All-Atom Molecular Dynamics Simulations

Contact Info

Product

Resources

About