Molecular Dynamics Simulation of the Thermosensitive Gelation Mechanism of Phosphorylcholine Groups-Conjugated Methylcellulose Hydrogel

The intelligently thermosensitive 2-methacryloyloxyethyl phosphorylcholine (MPC) groups-conjugated methylcellulose (MC) hydrogel, abbreviated as MPC-g-MC, exhibits good potential for prevention of postoperative adhesions. However, its thermosensitive gelation mechanism and why the MPC-g-MC hydrogel...

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Main Authors: Hongyu Mei, Yaqing Huang, Juzhen Yi, Wencheng Chen, Peng Guan, Shanyue Guan, Xiaohong Chen, Wei Li, Liqun Yang
Format: Article
Language:English
Published: MDPI AG 2025-07-01
Series:Gels
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Online Access:https://www.mdpi.com/2310-2861/11/7/521
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author Hongyu Mei
Yaqing Huang
Juzhen Yi
Wencheng Chen
Peng Guan
Shanyue Guan
Xiaohong Chen
Wei Li
Liqun Yang
author_facet Hongyu Mei
Yaqing Huang
Juzhen Yi
Wencheng Chen
Peng Guan
Shanyue Guan
Xiaohong Chen
Wei Li
Liqun Yang
author_sort Hongyu Mei
collection DOAJ
description The intelligently thermosensitive 2-methacryloyloxyethyl phosphorylcholine (MPC) groups-conjugated methylcellulose (MC) hydrogel, abbreviated as MPC-g-MC, exhibits good potential for prevention of postoperative adhesions. However, its thermosensitive gelation mechanism and why the MPC-g-MC hydrogel shows a lower gelation temperature than that of MC hydrogel are still unclear. Molecular dynamics (MD) simulation was thus used to investigate these mechanisms in this work. After a fully atomistic MPC-g-MC molecular model was constructed, MD simulations during the thermal simulation process and at constant temperatures were performed using GROMACS 2022.3 software. The results indicated that the hydrophobic interactions between the MPC-g-MC molecular chains increased, the interactions between the MPC-g-MC molecular chains and H<sub>2</sub>O molecules decreased with the rise in temperature, and the hydrogen bonding structures were changed during the thermal simulation process. As a result, the MPC-g-MC molecular chains began to aggregate at about 33 °C (close to the gelation temperature of 33 °C determined by the rheological measurement), bringing about the formation of the MPC-g-MC hydrogel in the macroscopic state. The mechanism of MPC-g-MC hydrogel formation showed that its lower gelation temperature than that of the MC hydrogel is attributed to the increase in the interactions (including hydrophobic interactions, hydrogen bonding interactions, Van der Waals and Coulomb forces) induced by the side MPC groups of MPC-g-MC molecules. The thermosensitive gelation mechanism revealed in this study provides an important reference for the development of novel thermosensitive MC-derived hydrogels with gelation temperatures close to human body temperature.
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spelling doaj-art-91e5e0e480bf4e7fb03538aabebc496d2025-08-20T03:35:37ZengMDPI AGGels2310-28612025-07-0111752110.3390/gels11070521Molecular Dynamics Simulation of the Thermosensitive Gelation Mechanism of Phosphorylcholine Groups-Conjugated Methylcellulose HydrogelHongyu Mei0Yaqing Huang1Juzhen Yi2Wencheng Chen3Peng Guan4Shanyue Guan5Xiaohong Chen6Wei Li7Liqun Yang8Institute of Polymer and Material Science, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, ChinaInstitute of Polymer and Material Science, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, ChinaInstitute of Polymer and Material Science, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, ChinaInstitute of Polymer and Material Science, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, ChinaInstitute of Polymer and Material Science, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, ChinaInstrumental Analysis & Research Center, Sun Yat-sen University, Guangzhou 510275, ChinaInstrumental Analysis & Research Center, Sun Yat-sen University, Guangzhou 510275, ChinaInstrumental Analysis & Research Center, Sun Yat-sen University, Guangzhou 510275, ChinaInstitute of Polymer and Material Science, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, ChinaThe intelligently thermosensitive 2-methacryloyloxyethyl phosphorylcholine (MPC) groups-conjugated methylcellulose (MC) hydrogel, abbreviated as MPC-g-MC, exhibits good potential for prevention of postoperative adhesions. However, its thermosensitive gelation mechanism and why the MPC-g-MC hydrogel shows a lower gelation temperature than that of MC hydrogel are still unclear. Molecular dynamics (MD) simulation was thus used to investigate these mechanisms in this work. After a fully atomistic MPC-g-MC molecular model was constructed, MD simulations during the thermal simulation process and at constant temperatures were performed using GROMACS 2022.3 software. The results indicated that the hydrophobic interactions between the MPC-g-MC molecular chains increased, the interactions between the MPC-g-MC molecular chains and H<sub>2</sub>O molecules decreased with the rise in temperature, and the hydrogen bonding structures were changed during the thermal simulation process. As a result, the MPC-g-MC molecular chains began to aggregate at about 33 °C (close to the gelation temperature of 33 °C determined by the rheological measurement), bringing about the formation of the MPC-g-MC hydrogel in the macroscopic state. The mechanism of MPC-g-MC hydrogel formation showed that its lower gelation temperature than that of the MC hydrogel is attributed to the increase in the interactions (including hydrophobic interactions, hydrogen bonding interactions, Van der Waals and Coulomb forces) induced by the side MPC groups of MPC-g-MC molecules. The thermosensitive gelation mechanism revealed in this study provides an important reference for the development of novel thermosensitive MC-derived hydrogels with gelation temperatures close to human body temperature.https://www.mdpi.com/2310-2861/11/7/521thermosensitive hydrogelphosphorylcholine groups-conjugated methylcellulose hydrogelmolecular dynamics simulationgelation mechanism
spellingShingle Hongyu Mei
Yaqing Huang
Juzhen Yi
Wencheng Chen
Peng Guan
Shanyue Guan
Xiaohong Chen
Wei Li
Liqun Yang
Molecular Dynamics Simulation of the Thermosensitive Gelation Mechanism of Phosphorylcholine Groups-Conjugated Methylcellulose Hydrogel
Gels
thermosensitive hydrogel
phosphorylcholine groups-conjugated methylcellulose hydrogel
molecular dynamics simulation
gelation mechanism
title Molecular Dynamics Simulation of the Thermosensitive Gelation Mechanism of Phosphorylcholine Groups-Conjugated Methylcellulose Hydrogel
title_full Molecular Dynamics Simulation of the Thermosensitive Gelation Mechanism of Phosphorylcholine Groups-Conjugated Methylcellulose Hydrogel
title_fullStr Molecular Dynamics Simulation of the Thermosensitive Gelation Mechanism of Phosphorylcholine Groups-Conjugated Methylcellulose Hydrogel
title_full_unstemmed Molecular Dynamics Simulation of the Thermosensitive Gelation Mechanism of Phosphorylcholine Groups-Conjugated Methylcellulose Hydrogel
title_short Molecular Dynamics Simulation of the Thermosensitive Gelation Mechanism of Phosphorylcholine Groups-Conjugated Methylcellulose Hydrogel
title_sort molecular dynamics simulation of the thermosensitive gelation mechanism of phosphorylcholine groups conjugated methylcellulose hydrogel
topic thermosensitive hydrogel
phosphorylcholine groups-conjugated methylcellulose hydrogel
molecular dynamics simulation
gelation mechanism
url https://www.mdpi.com/2310-2861/11/7/521
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