Abstract

If we could realize an autonomous polymer system driven under biological conditions by a tailor-made molecular design, human beings could create unprecedented biomimetic functions and materials such as heartbeats, autonomous peristaltic pumps, etc. In order to achieve this objective, we have investigated the molecular design of such a polymer system. As a result, we were the first to demonstrate a self-oscillating polymer system driven in a solution where only malonic acid existed, which could convert the chemical energy of the Belousov-Zhabotinsky (BZ) reaction into a change in the conformation of the polymer chain. To cause the self-oscillation in solution, we have attempted to construct a built-in system where the required BZ system substrates other than the organic acid are incorporated into the polymer itself. That is, the novel polymer chain incorporated the metal catalyst of the BZ reaction, a pH-control site and an oxidant supply site at the same time. As a result of introducing the pH control and oxidant supply sites into the conventional-type self-oscillating polymer chain, the novel polymer chain caused aggregation-disaggregation self-oscillations in the solution. We clarified that the period of the self-oscillation of the novel self-oscillating polymer chain was proportional to the concentration of the malonic acid. Therefore, the concentration of the malonic acid can be determined by measuring the period of the novel self-oscillating polymer solution. In this review, we introduce the detailed molecular design of the novel self-oscillating polymer chain and its self-oscillating behavior. Moreover, we report an autonomous self-oscillating polymer gel actuator that causes a bending-stretching motion under the constant conditions.

Highlights

  • Under thermodynamic equilibrium conditions, autonomous motions of macroscopic systems are tightly restricted, in the accordance with the Second Law of Thermodynamics

  • We introduce the detailed molecular design of a self-oscillating polymer system to drive the self-oscillation in a solution where only malonic acid exists

  • This is because the polymer chain in the oxidized state contained strongly hydrophilic oxidized Ru(bpy)33+ parts, in addition to the hydrophilic anionic charged AMPS

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Summary

Introduction

Autonomous motions of macroscopic systems are tightly restricted, in the accordance with the Second Law of Thermodynamics. Under thermodynamically open conditions, many living organisms can generate an autonomous motion without external driving stimuli. The mechanisms generating autonomous and stimuliresponsive activities are inherent. All living organisms involve a system capable of isothermal conversion of chemical energy into mechanical work. The biological system is significantly efficient because the chemical energy is directly converted the mechanical energy without intermediate steps. If autonomous polymer systems could be realized by completely synthetic polymers like living organisms acting under biological conditions, unprecedented biomimetic materials would be created

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