Abstract

AbstractIonomeric polymer‐metal composites (IPMC) are advanced materials designed to mimic biological systems. Their performance depends on various factors, including electrical stimulus intensity, membrane hydration, ionic migration, and Young's modulus. However, there is a lack of studies in the literature investigating how the water absorption capacity and elastic modulus change over time in IPMCs. Understanding the hydration level variation as a function of time is essential because as this parameter deviates, the ionic migration capacity and Young's modulus also change, altering the device's electromechanical efficiency over time. To address this research gap, Nafion/Pt‐based IPMC devices exchanged with four monovalent cations (H+, Li+, Na+, and K+) and one ionic liquid (1‐butyl‐3‐methylimidazolium—BMIM+) were prepared, and a comprehensive investigation on how the water absorption capacity and Young's modulus vary as a function of time, relative humidity (RH), and counterion size was performed. The results revealed that the water uptake capacity is significantly higher and occurs more rapidly at higher RH levels and when the counterion's ionic radius decreases. Consequently, the time required for the device to reach osmotic equilibrium can range from 40 to 270 min, depending on the RH and counterion used. Furthermore, it was observed that the first natural frequency and Young's modulus also exhibit time‐dependent behavior. Under constant RH conditions, the mechanical properties of the IPMC can vary by up to 50% in less than 60 min. Notably, the combined results from water uptake capacity, Young's modulus, electrochemical impedance spectroscopy, and electromechanical response analyses (including blocking force, displacement, displacement rate, current, coulombic efficiency, and voltage) suggest that a morphological transformation within the polymer is likely to occur once RH exceeds 60%. This finding strengthens the hypothesis that ion migration is mainly influenced by their movement through Nafion's ionomeric channels rather than the filling of ionic agglomerates.

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