A bistable switch from a low pH (unreacted "off") state to a high pH (reacted "on") state was obtained in enzyme-loaded gel beads in response to supra-threshold substrate concentrations.
Synchronizations of oscillatory regimes of the
Belousov−Zhabotinskii (BZ) reaction in a circular array
of
three identical CSTRs coupled via symmetric passive
diffusion/convection mass transfer were studied
experimentally. Stability of symmetric and asymmetric
phase-shifted oscillatory regimes with respect to
variations of the coupling strength among the reaction cells was
examined. The all-in-phase regime was
found to be the only regime stable over the entire range of coupling
strength values. Phase-shifted oscillatory
regimes were found to be stable only within a narrow interval of very
low coupling strength values.
Spontaneous transitions of the phase-shifted regimes to the
synchronized mode due to stochastic fluctuations
of the coupling strength were observed. Numerical simulations with
the four-variable Oregonator based model
of the BZ reaction qualitatively confirmed the experimental findings.
Propagation of an excitable response
to periodic pulsed stimulations in a linear three-array of coupled
chemical excitators (Belousov−Zhabotinskii
reaction) was studied in dependence on the coupling strength, on the
excitability level of the reaction mixture,
and on the period and amplitude of pulse stimulation. Regimes of
complete and partial propagation of the
excitable response and the regimes of partial and complete propagation
failure were observed. Numerical
simulations predict qualitatively well excitatory regimes observed in
experiments.
The reaction of hydrogen peroxide with thiosulfate and sulfite in acidic solution is characterized by marked temporal pH variations suggesting autocatalytic nature of hydrogen ions. When carried out in a continuous-flow stirred tank reactor this reaction provides nonlinear dynamical regimes including periodic oscillations, chaotic behavior, and multiple steady states coexisting over a range of operating conditions. The aim of the presented experimental study is a classification of the role of species and the underlying mechanism in the periodic oscillatory mode by applying single pulse additions of chosen reaction species. The external perturbations at various phases of the periodically oscillating system may cause phase advance or phase delay of the oscillations. The resulting phase transition curves are obtained for hydrogen ions, hydroxide ions, thiosulfate ions, sulfite ions, and hydrogen sulfite ions. These curves are compared with the phase transition curves calculated using the prototype mechanisms representing categories of chemical oscillators established in previous work. We found our system to be compatible with the mechanism of the category 1CX.
We examine experimentally a chemical system in a flow-through stirred reactor, which is known to provide large-amplitude oscillations of the pH value. By systematic variation of the flow rate, we find that the system displays hysteresis between a steady state and oscillations, and more interestingly, a transition to chaos involving mixed-mode oscillations. The basic pattern of the measured pH in the mixed-mode regime includes a large-scale peak followed by a series of oscillations on a much smaller scale, which are usually highly irregular and of variable duration. The bifurcation diagram shows that chaos sets in via a period-doubling route observed on the large-amplitude scale, but simultaneously small-amplitude oscillations are involved. Beyond the apparent accumulation of period doubling bifurcations, a mixed-mode regime with irregular oscillations on both scales is observed, occasionally interrupted by windows of periodicity. As the flow rate is further increased, chaos turns into quasiperiodicity and later to a simple small-amplitude periodic regime. Dynamics of selected typical regimes were examined with the tools of nonlinear time-series analysis, which include phase space reconstruction of an attractor and calculation of the maximal Lyapunov exponent. The analysis points to deterministic chaos, which appears via a period doubling route from below and via a route involving quasiperiodicity from above, when the flow rate is varied.
Two diffusively coupled reaction cells with a nonlinear reaction are used to perform chemical computing based on targeted perturbations switching between two Turing patterns defining two states of a logical device.
Dynamical regimes arising due to mutual interactions of oscillatory and excitatory modes of the Belousov-Zhabotinskii (BZ) reaction in a two-array and linear and circular three-arrays (with different arrangements of intrinsic connections) of identical continuous stirred tank reactors (CSTRs) coupled via symmetric passive diffusion/convection mass exchange were studied both experimentally and by numerical simulations. The coupling strength among individual CSTRs and the threshold of excitability of the BZ reaction mixture were varied systematically. Firing numbers (vectors) were used for classification of observed oscillatory-excitatory modes. Full spectra of firing numbers ranging from 0 to 1 were detected in all CSTR arrays investigated in experiments. The numbers of oscillators and excitators, threshold of excitability, and the way of coupling and coupling strengths within the array are principal factors affecting firing patterns of the array. Numerical simulations with the dimensionless three-variable Oregonator based model of the BZ reaction predict qualitatively well dynamical regimes encountered in experiments. Noisy coupling among the individual CSTRs due to hydrodynamical fluctuations is suggested to explain some of the observed differences.
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