Anomalous Reaction-Diffusion Dynamics of Ru(bpy)3-N-Hydroxysuccinimide and Controlled Unidirectional Deformation in the Self-Oscillating GelsClick to copy article linkArticle link copied!
- Won Seok LeeWon Seok LeeDepartment of Materials Engineering, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, JapanMore by Won Seok Lee
- Takafumi EnomotoTakafumi EnomotoDepartment of Materials Engineering, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, JapanMore by Takafumi Enomoto
- Aya Mizutani AkimotoAya Mizutani AkimotoDepartment of Materials Engineering, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, JapanMore by Aya Mizutani Akimoto
- Ryo Yoshida*Ryo Yoshida*Email: [email protected]. Tel: +81-3-5841-7112. Fax: +81-3-5841-7112.Department of Materials Engineering, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, JapanMore by Ryo Yoshida
Abstract

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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