Abstract
In this study, we investigated the lifetime and self-oscillating behavior of a polymer chain with a high lower critical solution temperature (LCST). The polymer chain comprised 4-vinyl-4´-methyl-2,2´-bipyridinebis(2,2´-bipyridine)bis(hexafluorophosphate) ruthenium as catalyst for the Belousov–Zhabotinsky reaction and N-ethylacrylamide as the polymer main-chain with a high LCST when compared to N-isopropylacrylamide. We demonstrated that the self-oscillating behavior was significantly affected by the polymer concentration and measuring temperature. Moreover, we established that the lifetime of the transmittance self-oscillation can be predicted from the polymer concentration and measuring temperature.
Highlights
The Belousov-Zhabotinsky (BZ) reaction is a famous self-oscillating reaction that occurs under constant temperature conditions [1–8]
The self-oscillating polymer chain cannot undergo self-oscillation at high temperatures. This occurs because the NIPAAm-based self-oscillating polymer chain is aggregated in the reduced state that originates from the hydrophobic main-chain and interactions between the hydrophobic reduced Ru(bpy)[3] moiety
The activation energy of the polymer solution was determined as 86.7 kJ/mol
Summary
The Belousov-Zhabotinsky (BZ) reaction is a famous self-oscillating reaction that occurs under constant temperature conditions [1–8]. Under strong acid conditions comprising nitric acid (HNO3) or sulfuric acid (H2SO4), the organic substrate [malonic acid (MA)] in the BZ reaction is oxidized by an oxidizing agent [sodium bromate (NaBrO3)] in the presence of a transition-metal catalyst. In this investigation, we adopted poly(Nethylacrylamide) [poly(NEAAm), Figure 1] as a selfoscillating polymer main-chain with a high lower critical solution temperature (LCST). The LCST values of these solutions in the reduced and oxidized states were determined as 16 °C and 44 °C, respectively This difference in solubility originated from the transmittance self-oscillation induced by the BZ reaction. The higher LCST in the oxidized Ru(bpy)[3] moiety allowed self-oscillation at higher temperatures when compared to the NIPAAmbased self-oscillating polymer solution
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