2026-10-13T16:44:35Z https://api.figshare.com/v2/oai

oai:figshare.com:article/34046533 2026-10-01T15:13:08Z category_1 category_4 category_915 category_21 category_24 category_873 category_39 category_734 portal_63 item_type_6 month_year_10_2026

Molecular Dynamics Simulation Insight into the Aggregate Structure–Mechanical Property Relationship of Double-Crosslinked Epoxidized Natural Rubber/Polylactic Acid Composites Yuhua Zhang (57349) Bo Wang (86769) Deli Chu (25157116) Wei Shang (94942) Guanyi Hou (6396155) Fengnian Zhao (5738432) Yunxuan Weng (8208321) Biophysics Biochemistry Physical Sciences not elsewhere classified Biotechnology Evolutionary Biology Chemical Sciences not elsewhere classified Ecology Biological Sciences not elsewhere classified using renewable feedstocks tunable structural characteristics strong interfacial compatibility stable interfacial coupling representative biodegradable polymer replacing traditional plastics possesses excellent flexibility polymer backbone provide partially replace petrochemicals offers theoretical guidance isolated local junctions internal elastomer network epoxidized natural rubber enhanced chain orientation elastomer network architecture directly observe molecular active epoxy groups based engineered elastomer promising toughening strategy level structural evolution enr chain length based polymer blends work provides molecular exhibits great potential dual crosslinking networks developing sustainable bio polylactic acid composites polylactic acid enr composites enr blends based materials level insights important strategy crosslinked networks chemical crosslinking enr self enr blending enr ), underlying load superior strain stress analysis severely limits results reveal remains difficult practical applications petroleum resources performance bio nonmonotonic dependence mechanical reinforcement inherent brittleness With the increasing depletion of petroleum resources, using renewable feedstocks to fully or partially replace petrochemicals has become an important strategy for developing sustainable bio-based materials. Polylactic acid (PLA), a representative biodegradable polymer, exhibits great potential for replacing traditional plastics but suffers from inherent brittleness that severely limits its practical applications. Epoxidized natural rubber (ENR), as a bio-based engineered elastomer, possesses excellent flexibility and tunable structural characteristics. The active epoxy groups on its polymer backbone provide the potential for strong interfacial compatibility and chemical crosslinking with PLA, making PLA/ENR blending a promising toughening strategy. Although previous experimental studies have provided valuable macroscopic insights, it remains difficult to directly observe molecular-level structural evolution and the underlying load-bearing mechanisms of crosslinked networks. In this work, coarse-grained molecular dynamics simulations were employed to investigate PLA/ENR blends with different ENR chain lengths and dual crosslinking networks, including PLA–ENR interfacial crosslinks and ENR–ENR self-crosslinks. The results reveal a nonmonotonic dependence of mechanical reinforcement on ENR chain length. Short ENR chains mainly act as isolated local junctions, whereas excessively long chains undergo severe phase aggregation and form self-crosslinked domains. In contrast, intermediate ENR chains construct an effective interwoven bridging network, leading to enhanced chain orientation, stable interfacial coupling, and superior strain-hardening behavior. Bonded-stress analysis further demonstrates that intra-ENR self-crosslinking bonds sustain substantially higher stress than PLA–ENR interfacial bonds, identifying the internal elastomer network as the dominant load-bearing element. This work provides molecular-level insights into the role of elastomer network architecture in PLA/ENR composites and offers theoretical guidance for designing high-performance bio-based polymer blends. 2026-10-01T00:00:00Z Text Journal contribution 10.1021/acsapm.6c03053.s001 https://figshare.com/articles/journal_contribution/Molecular_Dynamics_Simulation_Insight_into_the_Aggregate_Structure_Mechanical_Property_Relationship_of_Double-Crosslinked_Epoxidized_Natural_Rubber_Polylactic_Acid_Composites/34046533 CC BY-NC 4.0