Affine deformation and self-assembly alignment in hydrogel nanocomposites

17 August 2023, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Tailoring order in hierarchical structures is a key goal of bioinspired nanocomposite design. Recently, nacre-like materials have been developed by solvent evaporation methods that are scalable and attain advanced functionalities. However, understanding the alignment mechanisms of 2D-fillers, nanosheets or platelets, remains challenging. This work explores the possible pathways for nanocomposite ordering via orientation distribution functions. We demonstrate how the immobilization of 2D-materials via a (pseudo)-network formation is crucial to alignment based on evaporation. We show a modified affine deformation model that describes such evaporative methods. In this, a gel network develops enough yield stress and uniformly deforms as drying proceeds, along with the immobilized particles, causing in-plane orientation. Herein, we tested the dominance of this approach by using a thermo-reversible gel for rapid montmorillonite (MMT) particle fixation. We researched gelatin/MMT as a model system to investigate the effects of high loadings, orientational order, and aspect ratio. The nacre-like nanocomposites showed a semi-constant order parameter ( ~0.7) over increasing nanofiller content up to 64 vol.% filler. This remarkable alignment resulted in continuously improved mechanical and water vapor barrier properties over unusually high filler fractions. Some variations in stiffness and diffusion properties were observed, possibly correlated to the applied drying conditions of the hybrid hydrogels. The affine deformation strategy holds promise for developing next-generation advanced materials with tailored properties even at (very) high filler loadings. Furthermore, a gelling approach offers the advantages of simplicity and versatility in the formulation of the components, which is useful for large-scale fabrication methods.

Keywords

gel
polymer nanocomposites
nacre
orientation
self-assembly
mechanical properties
water diffusion

Comments

Comments are not moderated before they are posted, but they can be removed by the site moderators if they are found to be in contravention of our Commenting Policy [opens in a new tab] - please read this policy before you post. Comments should be used for scholarly discussion of the content in question. You can find more information about how to use the commenting feature here [opens in a new tab] .
This site is protected by reCAPTCHA and the Google Privacy Policy [opens in a new tab] and Terms of Service [opens in a new tab] apply.