Lee, Tse-AnTse-AnLeeCHU-CHEN CHUEHRU-JONG JENG2025-11-272025-11-272025-1110229760https://www.scopus.com/record/display.uri?eid=2-s2.0-105019701827&origin=resultslisthttps://scholars.lib.ntu.edu.tw/handle/123456789/734191Despite the widespread applications of lithium-ion batteries (LIBs) in electronics and energy systems, their safety remains a significant concern. In this regard, gel polymer electrolytes (GPEs) based on hydrogels with superior mechanical stability and resistance to leakage have emerged as promising alternatives. To date, most studies have focused on ionic conductivity rather than structural stability, resulting in limited understanding of how water content affects hydrogel properties. To address this, this study utilized molecular dynamics simulations to investigate the effects of water content and temperature on the mechanical behavior of cellulose-reinforced composite hydrogels. The results revealed that excessive water disrupts hydrogen bonding, whereas 40% water content yields optimal mechanical strength. When the water content exceeds 50%, polymer-water interactions weaken, causing the system to transition to a water-dominated system. Temperature analysis shows that while binding energy exhibits polymer-specific fluctuations within the range of 338–358 K, the cohesive energy density and binding energy generally decrease with increasing temperature. Phase transitions may drive these fluctuations; notably, hydrogen bonds between water molecules tend to increase bond angles, while hydrogen bonds between water and polymers primarily shorten bond lengths. These distinct bonding behaviors collectively modulate structural dynamics. Further structural analyses revealed enhanced water mobility, phase transitions, and hydrogen bond rearrangements, providing valuable insights for the rational design and stability optimization of high-performance hydrogels.falseCellulose compositeGel polymer electrolyteHydrogelsMechanical propertiesMolecular dynamics[SDGs]SDG7journal article10.1007/s10965-025-04642-32-s2.0-105019701827