Insights into the Phase Diagram of Pluronic L64 Using Coarse-Grained Molecular Dynamics Simulations. 2022

Mangesh Bhendale, and Arpita Srivastava, and Jayant K Singh
Department of Chemical Engineering, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, India.

We investigate the concentration-dependent phase diagram of pluronic L64 in aqueous media at 300 and 320 K using coarse-grained (CG) molecular dynamics (MD) simulations. The CG model is derived by adapting the Martini model for nonbonded interactions along with the Boltzmann inversion (BI) of bonded interactions from all-atom (AA) simulations. Our derived CG model successfully captures the experimentally observed micellar-, hexagonal-, lamellar-, and polymer-rich solution phase. The end-to-end distance reveals the conformational change from an open-chain structure in the micellar phase to a folded-chain structure in the lamellar phase, increasing the orientational order. An increase in temperature leads to expulsion of water molecules from the L64 moiety, suggesting an increase in L64 hydrophobicity. Thermodynamic analysis using the two-phase thermodynamics (2PT) method suggests the entropy of the system decreases with increasing L64 concentration and the decrease in free energy (F) with temperature is mainly driven by the entropic factor (-TS). Further, the increase in aggregation number at lower concentrations and self-assembly at very high concentrations is energetically driven, whereas the change from the micellar phase to the lamellar phase with increasing L64 concentration is entropically driven. Our model provides molecular insights into L64 phases which can be further explored to design functionality-based suprastructures for drug delivery and tissue engineering applications.

UI MeSH Term Description Entries
D008823 Micelles Particles consisting of aggregates of molecules held loosely together by secondary bonds. The surface of micelles are usually comprised of amphiphatic compounds that are oriented in a way that minimizes the energy of interaction between the micelle and its environment. Liquids that contain large numbers of suspended micelles are referred to as EMULSIONS. Micelle
D013816 Thermodynamics A rigorously mathematical analysis of energy relationships (heat, work, temperature, and equilibrium). It describes systems whose states are determined by thermal parameters, such as temperature, in addition to mechanical and electromagnetic parameters. (From Hawley's Condensed Chemical Dictionary, 12th ed) Thermodynamic
D014867 Water A clear, odorless, tasteless liquid that is essential for most animal and plant life and is an excellent solvent for many substances. The chemical formula is hydrogen oxide (H2O). (McGraw-Hill Dictionary of Scientific and Technical Terms, 4th ed) Hydrogen Oxide
D056004 Molecular Dynamics Simulation A computer simulation developed to study the motion of molecules over a period of time. Molecular Dynamics Simulations,Molecular Dynamics,Dynamic, Molecular,Dynamics Simulation, Molecular,Dynamics Simulations, Molecular,Dynamics, Molecular,Molecular Dynamic,Simulation, Molecular Dynamics,Simulations, Molecular Dynamics
D020442 Poloxamer A nonionic polyoxyethylene-polyoxypropylene block co-polymer with the general formula HO(C2H4O)a(-C3H6O)b(C2H4O)aH. It is available in different grades which vary from liquids to solids. It is used as an emulsifying agent, solubilizing agent, surfactant, and wetting agent for antibiotics. Poloxamer is also used in ointment and suppository bases and as a tablet binder or coater. (Martindale The Extra Pharmacopoeia, 31st ed) Pluronic,Poloxamers,Pluronic F-108,Pluronic F-127,Pluronic F-68,Pluronic F68,Pluronic L-101,Pluronic L-121,Pluronic L-81,Pluronics,Poloxalkol,Poloxamer 188,Poloxamer 213,Poloxamer 2930,Poloxamer 338,Poloxamer 407,188s, Poloxamer,213s, Poloxamer,2930s, Poloxamer,338s, Poloxamer,407s, Poloxamer,F68s, Pluronic,Pluronic F 108,Pluronic F 127,Pluronic F 68,Pluronic F108,Pluronic F127,Pluronic F68s,Pluronic L 101,Pluronic L 121,Pluronic L 81,Pluronic L101,Pluronic L121,Pluronic L81,Poloxalkols,Poloxamer 188s,Poloxamer 213s,Poloxamer 2930s,Poloxamer 338s,Poloxamer 407s

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