Load-bearing entanglements in polymer glasses.

Sci Adv

Polymer Science and Engineering Department, University of Massachusetts Amherst, Amherst, MA 01003, USA.

Published: September 2021

Through a combined approach of experiment and simulation, this study quantifies the role of entanglements in determining the mechanical properties of glassy polymer blends. Uniaxial extension experiments on 100-nm films containing a bidisperse mixture of polystyrene enable quantitative comparison with molecular dynamics (MD) simulations of a coarse-grained model for polymer glasses, where the bidisperse blends allow us to systematically tune the entanglement density of both systems. In the MD simulations, we demonstrate that not all entanglements carry substantial load at large deformation, and our analysis allows the development of a model to describe the number of effective, load-bearing entanglements per chain as a function of blend ratio. The film strength measured experimentally and the simulated film toughness are quantitatively described by a model that only accounts for load-bearing entanglements.

Download full-text PDF

Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8448454PMC
http://dx.doi.org/10.1126/sciadv.abg9763DOI Listing

Publication Analysis

Top Keywords

load-bearing entanglements
12
polymer glasses
8
entanglements polymer
4
glasses combined
4
combined approach
4
approach experiment
4
experiment simulation
4
simulation study
4
study quantifies
4
quantifies role
4

Similar Publications

Form-function relationships often have tradeoffs: if a material is tough, it is often inflexible, and vice versa. This is particularly relevant for the elephant trunk, where the skin should be protective yet elastic. To investigate how this is achieved, we used classical histochemical staining and second harmonic generation microscopy to describe the morphology and composition of elephant trunk skin.

View Article and Find Full Text PDF

Nanoconfinements are utilized to program how polymers entangle and disentangle as chain clusters to engineer pseudo bonds with tunable strength, multivalency, and directionality. When amorphous polymers are grafted to nanoparticles that are one magnitude larger in size than individual polymers, programming grafted chain conformations can "synthesize" high-performance nanocomposites with moduli of ≈25GPa and a circular lifecycle without forming and/or breaking chemical bonds. These nanocomposites dissipate external stresses by disentangling and stretching grafted polymers up to ≈98% of their contour length, analogous to that of folded proteins; use both polymers and nanoparticles for load bearing; and exhibit a non-linear dependence on composition throughout the microscopic, nanoscopic, and single-particle levels.

View Article and Find Full Text PDF

Hydrogels with high sacrifice efficiency of sacrificial bonds and with high strength and toughness due to dense entanglements of polymer chains.

J Colloid Interface Sci

January 2025

School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China; State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai 200240, China. Electronic address:

Article Synopsis
  • Introducing sacrificial bonds enhances the toughness of hydrogels, and this study focuses on the efficiency of these bonds using polyacrylamide hydrogels with highly entangled polymer chains and carboxyl-zirconium (-COO-Zr) bonds.
  • The research finds that physical entanglements significantly increase tensile strength and Young's modulus without compromising overall toughness, as they enable more polymer chains to engage during deformation.
  • While dense entanglements improve sacrificial bond efficiency, excessive chemical crosslinking limits this efficiency due to restrictions on chain movement, indicating a need for balance in hydrogel design for engineering applications.
View Article and Find Full Text PDF

Tailoring Network Topology in Mechanically Robust Hydrogels for 3D Printing and Injection.

ACS Appl Mater Interfaces

May 2024

Advanced Functional Polymers (AFP) Laboratory, Institute for Materials Research (imo-imomec), Hasselt University, Martelarenlaan 42, Hasselt 3500, Belgium.

Tissue engineering and regenerative medicine are confronted with a persistent challenge: the urgent demand for robust, load-bearing, and biocompatible scaffolds that can effectively endure substantial deformation. Given that inadequate mechanical performance is typically rooted in structural deficiencies─specifically, the absence of energy dissipation mechanisms and network uniformity─a crucial step toward solving this problem is generating synthetic approaches that enable exquisite control over network architecture. This work systematically explores structure-property relationships in poly(ethylene glycol)-based hydrogels constructed utilizing thiol-yne chemistry.

View Article and Find Full Text PDF

Articular cartilage has an appropriate multilayer structure and superior tribological properties and provides a structural paradigm for design of lubricating materials. However, mimicking articular cartilage traits on prosthetic materials with durable lubrication remains a huge challenge. Herein, an ingenious three-in-one strategy is developed for constructing an articular cartilage-like bilayer hydrogel coating on the surface of ultra-high molecular weight polyethylene (BH-UPE), which makes full use of conceptions of interfacial interlinking, high-entanglement crosslinking, and interface-modulated polymerization.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!