A Thermoreversible Gelation Pathway to Plant Cuticle-Inspired Biopolymer Aerogel Monoliths Based on Network-Spherulitic Crystal Assemblies.

Authors

Anthony V Tuccitto, Zeineb Ben Rejeb, Rafaela Aguiar, Nello D Sansone, Sumaiya Farzana, Isaac Ali, Jun Uk Lee, Daniel J Davidson, Ailsa K Edward, Chul B Park, Patrick C Lee

Published in

Advanced materials (Deerfield Beach, Fla.). Pages e75136. Sep 29, 2026. Epub Sep 29, 2026.

Abstract

Plant-based and compostable biopolymers are vital in global shifts toward green materials. However, their adoption in aerogel fabrication is limited by material and structure-performance deficiencies (e.g., hydrophilicity, low surface area, brittleness, limited tactile tailorability). Nevertheless, stereocomplexation, or co-crystallization between polymeric enantiomers, offers a pathway toward overcoming such limitations. Herein, stereocomplexation is used to fabricate poly(lactide) (PLA)-based aerogels, with stereocomplex crystals (SCs) assembling into a highly ordered morphology/topology within aerogel precursors. To tailor aerogel bulk properties, a blending approach is implemented during sol-gel processing, leading to sequential crystallization of sol-gel system constituents. This pathway yields hierarchically macro-/meso-porous aerogels (S_BET up to ∼186 m²·g^-1), offering a variety of superstructures that resemble cuticular plant tissue. These aerogels resist brittle failure under compression (70% strain) and withstand cyclic loading (100 cycles, 20% strain) without significant densification. Such aerogels also exhibit functional properties including superhydrophobicity/superoleophilicity and are well-suited for continuous oil-water separation. Additionally, fantastic geometric-thermal stability, insulation/heat dissipation ability (k_Cond ∼36 mW·m^-1·K^-1), and phase-change insulation characteristics are achieved. These functionalities arise from multi-scale structural features and demonstrate how coupling stereocomplexation and sequential crystallization offers pathways to construct intricate superstructure morphologies/topologies, and overcome material/structure-performance limitations in green aerogels.

PMID:
42806887
Bibliographic data and abstract were imported from PubMed on 29 Sep 2026.

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