POS10-0613
Dissipative Particle Dynamics Simulation of Sequence-Dependent Micellar Network Formation in PLGA-PEG-PLGA Hydrogels
Topic
S10. AI-assisted Design and Simulation of Polymers
When and Where
Sep 30, 2026
08:30 - 09:30
Room 301 (Grand Ballroom)
Session Chairs
Heesuk KIM
Jinhye BAE
Presenter(s)
Sangheon Lee (seoul national university of science and technology)
Co-Author(s)
Abstract
PLGA–PEG–PLGA triblock copolymer hydrogels are widely investigated as thermoresponsive biomaterials for drug delivery and tissue engineering. Their sol–gel transition is generally governed by the self-assembly of amphiphilic polymer chains into micelles and interconnected micellar networks. While the effects of molecular weight and LA/GL composition have been extensively studied, the role of PLGA monomer sequence distribution in mesoscale micelle assembly remains less understood.
In this study, dissipative particle dynamics (DPD) simulations were used to investigate how the sequence arrangement of PLGA segments affects micellar morphology and network formation in aqueous PLGA–PEG–PLGA copolymer systems. Two limiting PLGA sequence models, block and random sequences, were compared at polymer volume fractions ranging from 5 to 30 vol% under a fixed reduced temperature. The simulations aimed to clarify the structural origin of sequence-dependent gelation behavior rather than directly reproduce temperature-dependent sol–gel transitions.
With increasing polymer concentration, both block and random sequence copolymers evolved from isolated micelles into three-dimensional network structures. Blocky PLGA sequences produced well-defined micellar structures and promoted intermicellar bridge formation, leading to a gradual transition toward a connected network. In contrast, random PLGA sequences resulted in less favorable core packing, causing micelles to merge upon contact rather than forming distinct bridges.
These results indicate that PLGA monomer sequence distribution regulates mesoscale self-assembly by altering micelle organization, intermicellar bridging, and network connectivity. Overall, DPD simulations provide a mechanistic explanation for sequence-dependent gelation behavior and highlight monomer sequence control as an important design parameter for tunable PLGA–PEG–PLGA hydrogels.
In this study, dissipative particle dynamics (DPD) simulations were used to investigate how the sequence arrangement of PLGA segments affects micellar morphology and network formation in aqueous PLGA–PEG–PLGA copolymer systems. Two limiting PLGA sequence models, block and random sequences, were compared at polymer volume fractions ranging from 5 to 30 vol% under a fixed reduced temperature. The simulations aimed to clarify the structural origin of sequence-dependent gelation behavior rather than directly reproduce temperature-dependent sol–gel transitions.
With increasing polymer concentration, both block and random sequence copolymers evolved from isolated micelles into three-dimensional network structures. Blocky PLGA sequences produced well-defined micellar structures and promoted intermicellar bridge formation, leading to a gradual transition toward a connected network. In contrast, random PLGA sequences resulted in less favorable core packing, causing micelles to merge upon contact rather than forming distinct bridges.
These results indicate that PLGA monomer sequence distribution regulates mesoscale self-assembly by altering micelle organization, intermicellar bridging, and network connectivity. Overall, DPD simulations provide a mechanistic explanation for sequence-dependent gelation behavior and highlight monomer sequence control as an important design parameter for tunable PLGA–PEG–PLGA hydrogels.
