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Anomalous Reaction-Diffusion Dynamics of Ru(bpy)3-N-Hydroxysuccinimide and Controlled Unidirectional Deformation in the Self-Oscillating Gels

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    Anomalous Reaction-Diffusion Dynamics of Ru(bpy)3-N-Hydroxysuccinimide and Controlled Unidirectional Deformation in the Self-Oscillating Gels
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    ACS Applied Polymer Materials

    Cite this: ACS Appl. Polym. Mater. 2025, 7, 2, 1020–1031
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    https://doi.org/10.1021/acsapm.4c03560
    Published January 12, 2025
    Copyright © 2025 American Chemical Society
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    Abstract

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    Self-oscillating gels represent autonomous and periodic volume oscillation driven by a Belousov–Zhabotinsky (BZ) reaction, mimicking life-like motions without external stimuli. Achieving complex biomimetic deformations relies on the precise spatial distribution of Ru(bpy)3-N-hydroxysuccinimide (Ru(bpy)3-NHS), the catalyst for the BZ reaction, within the gel network. To gain a deeper understanding of and control this distribution, we systematically investigated the reaction-diffusion (R-D) behavior of Ru(bpy)3-NHS during the fabrication process of the self-oscillating gels. The gel matrix is immersed in Ru(bpy)3-NHS for varying durations, and resulting R-D behaviors are analyzed by measuring the distance of Ru(bpy)3-immobilized area during the immersion. Our experimental results reveal that the R-D rate of Ru(bpy)3-NHS depends nonlinearly on the immersion time, aligning with anomalous subdiffusion as indicated by mathematical analysis. Furthermore, the R-D process is influenced by the gel composition, specifically the concentration of N,N′-methylenebis(acrylamide) (MBAAm, cross-linker) and N-3-(aminopropyl)methacrylamide (NAPMAm). The diffusion coefficients under various conditions are determined, and the impact of cross-linker contents on the shape deformation of Ru(bpy)3-patterned gels during the BZ reaction is evaluated. By deepening the understanding of the R-D behavior of Ru(bpy)3-NHS, this work provides foundational insights and a pathway for engineering more life-like functional systems. The refined control over the R-D behavior of Ru(bpy)3-NHS advances manipulation of the gel shape deformations, paving the way for applications in soft robotics, dynamic biomaterials, and artificial muscles.

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    • Additional experimental details: schematic illustration of the fabrication method; photos and gray value profiles of the fabricated gels with various dipping times; the values of calculated reaction-diffusion distance; the result of calculated anomalous diffusion coefficient (Dα) and the anomalous diffusion exponent (α) by mathematical modeling, mathematical modeling over 24 h; the equilibrium swelling ratio results of the base and self-oscillating gels; the gray value profiles of each sample sides; the calculated period and amplitude of the volumetric deformation during the BZ reaction; comparison plot to the state-of-the-art (PDF)

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    ACS Applied Polymer Materials

    Cite this: ACS Appl. Polym. Mater. 2025, 7, 2, 1020–1031
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsapm.4c03560
    Published January 12, 2025
    Copyright © 2025 American Chemical Society
    Request reuse permissions

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