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Dynamic Growth of Macroscopically Structured Supramolecular Hydrogels through Orchestrated Reaction-Diffusion
Authors:Hucheng Wang  Dr. Xiaoming Fu  Guanyao Gu  Shengyu Bai  Dr. Runlai Li  Prof. Weimin Zhong  Prof. Xuhong Guo  Dr. Rienk Eelkema  Prof. Jan H. van Esch  Prof. Zhixing Cao  Prof. Yiming Wang
Affiliation:1. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Meilong Road 130, Shanghai, 200237 P. R. China

These authors contributed equally to this work.;2. Key Laboratory of Smart Manufacturing in Energy Chemical Process, East China University of Science and Technology, Meilong Road 130, Shanghai, 200237 P. R. China

These authors contributed equally to this work.;3. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Meilong Road 130, Shanghai, 200237 P. R. China;4. Department of Chemistry, National University of Singapore, Singapore, 119077 Singapore;5. Key Laboratory of Smart Manufacturing in Energy Chemical Process, East China University of Science and Technology, Meilong Road 130, Shanghai, 200237 P. R. China;6. Department of Chemical Engineering, Delft University of Technology, van der Maasweg 9, 2629 HZ Delft, The Netherlands

Abstract:Living organisms are capable of dynamically changing their structures for adaptive functions through sophisticated reaction-diffusion processes. Here we show how active supramolecular hydrogels with programmable lifetimes and macroscopic structures can be created by relying on a simple reaction-diffusion strategy. Two hydrogel precursors (poly(acrylic acid) PAA/CaCl2 and Na2CO3) diffuse from different locations and generate amorphous calcium carbonate (ACC) nanoparticles at the diffusional fronts, leading to the formation of hydrogel structures driven by electrostatic interactions between PAA and ACC nanoparticles. Interestingly, the formed hydrogels are capable of autonomously disintegrating over time because of a delayed influx of electrostatic-interaction inhibitors (NaCl). The hydrogel growth process is well explained by a reaction-diffusion model which offers a theoretical means to program the dynamic growth of structured hydrogels. Furthermore, we demonstrate a conceptual access to dynamic information storage in soft materials using the developed reaction-diffusion strategy. This work may serve as a starting point for the development of life-like materials with adaptive structures and functionalities.
Keywords:Hydrogels  Non-Equilibrium Systems  Reaction-Diffusion  Self-Assembly  Supramolecular Materials
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