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Systematic design of chemical oscillators using complexation and precipitation equilibria


Concentration oscillations are ubiquitous in living systems, where they involve a wide range of chemical species. In contrast, early in vitro chemical oscillators were all derived from two accidentally discovered reactions1,2,3 based on oxyhalogen chemistry. Over the past 25 years, the use of a systematic design algorithm4,5, in which a slow feedback reaction periodically drives a bistable system in a flow reactor between its two steady states, has increased the list of oscillating chemical reactions to dozens of systems. But these oscillating reactions are still confined to a handful of elements that possess multiple stable oxidation states: halogens, sulphur and some transition metals6. Here we show that linking a ‘core’ oscillator to a complexation or precipitation equilibrium can induce concentration oscillations in a species participating in the equilibrium. We use this method to design systems that produce periodic pulses of calcium, aluminium or fluoride ions. The ability to generate oscillations in elements possessing only a single stable oxidation state (for example, Na+, F-, Ca2+) may lead to reactions that are useful for coupling to or probing living systems, or that help us to understand new mechanisms by which periodic behaviour may arise.

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Figure 1: Schematic diagram of the basic elements for oscillator design.
Figure 2: Oscillations of pH in the core BrO3-–SO32-–Fe(CN)64- oscillator.
Figure 3: Oscillatory pulses of free Ca2+.
Figure 4: Periodic changes in the concentration of free Al3+.
Figure 5: Oscillations in [F-].

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This work was supported by the Hungarian Academy of Sciences (HAS), the US National Science Foundation (NSF) and a US-Hungarian Cooperative Research Grant from NSF and HAS. We thank L. Yang for assistance in preparing the figures.

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Correspondence to Irving R. Epstein.

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Kurin-Csörgei, K., Epstein, I. & Orbán, M. Systematic design of chemical oscillators using complexation and precipitation equilibria. Nature 433, 139–142 (2005).

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