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High-χ ionic homopolymers with humidity responsiveness: effect of microphase separation and thermal properties
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DOI：10.1007/s11426-026-3492-6.png)
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Abstract
En 中文
The introduction of ionizable groups can markedly enhance the microphase separation behavior of homopolymer materials, increasing the affinity of the resulting phase structures toward water molecules and imparting humidity-responsive properties. Such humidity-responsive materials hold significant promise for applications in flexible sensing and intelligent actuation. However, achieving precise structural control at the nanoscale and establishing a direct correlation between microscopic phase morphology and macroscopic responsive performance remain critical challenges in this field. In this study, we successfully synthesized a class of ionic homopolymers, denoted as PSS-(n)N, via the reaction of polystyrene sulfonic acid with long-chain alkyl dimethyl tertiary amines. We demonstrated microphase separation in a non-block copolymer system through a synergistic mechanism involving ionization-driven interactions and side-chain crystallization. This approach yielded ultrahigh-resolution patterns with feature sizes below 4 nm, offering a new strategy for the construction of humidity-responsive materials. By introducing a humid/thermal annealing process, we observed the phase structure transformation behavior of ionic homopolymers under water-assisted conditions for the first time. Based on these findings, we fabricated a homopolymer composite bilayer film that achieved macroscopic deformation across the full humidity range. Collectively, these results establish a new framework for elucidating the structure-property relationships between the microstructure and macroscopic properties of ionic homopolymers and provide new insights into the design and fabrication of moisture-sensitive microphase-separated materials.
Keywords:
ionic homopolymers
microphase separation
thermal properties
water-assisted phase structure transformation
high-χ
humidity responsive
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