The Role of a Diluent in Deformation-Induced Bonding of Glassy Polymer Bidisperse Blends

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Main Authors: Vallabh, Ajay, Tsavalas, John G
Format: Preprint
Published: 2024
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author Vallabh, Ajay
Tsavalas, John G
author_facet Vallabh, Ajay
Tsavalas, John G
contents Bonding between polymers below the glass transition temperature through molecular-scale dilatation (or densification)-based interdiffusion of macromolecules has recently been introduced. In this mechanism, short timeframe plastic deformation enables polymer chains to interdiffuse and form entanglements at the interface, facilitating rapid bonding below the glass transition temperature ($T_g$). Here, we are addressing the role of a lower molecular weight diluent in bonding polymer interfaces of bidisperse blends through deformation-induced bonding (DIB) at temperatures well below both the surface and bulk glass transition temperatures, $T_g^s$ and $T_g^b$, respectively, by using molecular simulations. These simulations reveal that addition of the diluent ($ϕ\le$20\%) drastically enhances the number of chain-ends at the interfacial region compared to a pure glass sample ($ϕ=0\%$) during deformation below $T_g^s$, which improves the possibility of opposite side entanglement formation. The changes in stress-strain response of debonded samples correlate with the normalized entanglement density. Likewise, the maximum interfacial fracture energy $G_{I,max}$ of debonded samples is correlated with the diluent concentration ($ϕ$), below $T_g^s$. Furthermore, the optimization of material and process conditions for DIB has yielded a notable advancement for the conditions tested here: achieving a higher bonding strength, approximately one-third of the bulk, all while remaining below $T_g$.
format Preprint
id arxiv_https___arxiv_org_abs_2405_11362
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle The Role of a Diluent in Deformation-Induced Bonding of Glassy Polymer Bidisperse Blends
Vallabh, Ajay
Tsavalas, John G
Soft Condensed Matter
Bonding between polymers below the glass transition temperature through molecular-scale dilatation (or densification)-based interdiffusion of macromolecules has recently been introduced. In this mechanism, short timeframe plastic deformation enables polymer chains to interdiffuse and form entanglements at the interface, facilitating rapid bonding below the glass transition temperature ($T_g$). Here, we are addressing the role of a lower molecular weight diluent in bonding polymer interfaces of bidisperse blends through deformation-induced bonding (DIB) at temperatures well below both the surface and bulk glass transition temperatures, $T_g^s$ and $T_g^b$, respectively, by using molecular simulations. These simulations reveal that addition of the diluent ($ϕ\le$20\%) drastically enhances the number of chain-ends at the interfacial region compared to a pure glass sample ($ϕ=0\%$) during deformation below $T_g^s$, which improves the possibility of opposite side entanglement formation. The changes in stress-strain response of debonded samples correlate with the normalized entanglement density. Likewise, the maximum interfacial fracture energy $G_{I,max}$ of debonded samples is correlated with the diluent concentration ($ϕ$), below $T_g^s$. Furthermore, the optimization of material and process conditions for DIB has yielded a notable advancement for the conditions tested here: achieving a higher bonding strength, approximately one-third of the bulk, all while remaining below $T_g$.
title The Role of a Diluent in Deformation-Induced Bonding of Glassy Polymer Bidisperse Blends
topic Soft Condensed Matter
url https://arxiv.org/abs/2405.11362