Primary process of illumination effect on the tris(bipyridine)ruthenium(2+)-catalyzed Belousov-Zhabotinskii reaction

Jinguji, M.; Ishihara, Mariko; Nakazawa, Tsutomu

doi:10.1021/j100190a033

Cited by 58 publications

(56 citation statements)

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“…9,15,17 Hanazaki at al. 16,[18][19][20][21] proposed a dual effect of light on the BZ reaction: low-intensity illumination inducing oscillations, due to the generation of HBrO 2 from BrO 3 -, and high-intensity illumination suppressing oscillations, due to the generation of Br -from BrO 3 -.…”

Section: Discussionmentioning

confidence: 99%

Reaction Mechanism for Light Sensitivity of the Ru(bpy)₃²⁺-Catalyzed Belousov−Zhabotinsky Reaction

1997

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The effects of light on the Ru(bpy) 3 2+ -catalyzed Belousov-Zhabotinsky (BZ) reaction are investigated. Experiments were carried out on an organic subset of the reaction comprised of bromomalonic acid, sulfuric acid, and Ru(bpy) 3 2+ as well as on an inorganic subset comprised of bromate, sulfuric acid, and Ru(bpy) 3 2+ . Experiments were also carried out on the full Ru(bpy) 3 2+ -catalyzed BZ system. The experiments, together with modeling studies utilizing an Oregonator scheme modified to account for the light sensitivity, show that irradiation gives rise to two separate processes: the photochemical production of bromide from bromomalonic acid and the photochemical production of bromous acid from bromate.

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Section: Discussionmentioning

confidence: 99%

Reaction Mechanism for Light Sensitivity of the Ru(bpy)₃²⁺-Catalyzed Belousov−Zhabotinsky Reaction

1997

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“…However, competition of (7) with (D2) and (D4) adds a negative term in the dark reaction (2) and henceforth adds a negative term to (3), which reduces [I -] th with increasing P. This does not account for the observation given above. To obtain the increasing tendency of [I -] th with P, the photoassisted multiplication of HIO 2 is essential to compete with (D2) and (D4).…”

Section: Photoregulation Of [I -] Thmentioning

confidence: 95%

Photoinduced Bifurcation and Multistability in the Oscillatory Briggs−Rauscher Reaction

1996

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The effect of continuous light irradiation on the Briggs-Rauscher system has been investigated by the light intensity scanning method. A state diagram has been established in the control parameter plane spanned by the initial concentration of I -([I -] 0 ) and the light power (P). An increase of [I -] 0 leads to a transition from the large-amplitude oscillatory state (OS) to the reduced steady state (SSI), whereas an increase of P gives rise to a transition from OS to the oxidized steady state (SSII). Both transitions are accompanied by hysteresis, resulting in tristability among OS, SSI, and SSII in the overlapped part of the two hysteresis regions. In addition to the photoinhibition reported previously, the photoinduction of oscillations has been found in a certain range of [I -] 0 . In the low-[I -] 0 region, bistability between OS and another oscillatory state with small amplitude (OS′) has also been discovered. The origin of the transitions is discussed on the basis of photoinduced autocatalytic processes.

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“…The BZ system is often referred to as a chemical prototype for complex self-organizing dynamics in biological systems which are seldom directly accessible to quantitative experimental investigation and manipulation. 45 The excited state of the complex Ru͑bpy͒ 3 ‫ء+2‬ is an extremely strong reducing agent. Ru͑bpy͒ 3 2+ as a catalyst 39 plays an important role in the investigation of self-organizing dynamics in the presence of light 40 as an external control parameter.…”

Section: Construction Of a Detailed Photo-bz Modelmentioning

confidence: 99%

Derivation of a quantitative minimal model from a detailed elementary-step mechanism supported by mathematical coupling analysis

Shaik

Kammerer

Górecki

et al. 2005

The Journal of Chemical Physics

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Accurate experimental data increasingly allow the development of detailed elementary-step mechanisms for complex chemical and biochemical reaction systems. Model reduction techniques are widely applied to obtain representations in lower-dimensional phase space which are more suitable for mathematical analysis, efficient numerical simulation, and model-based control tasks. Here, we exploit a recently implemented numerical algorithm for error-controlled computation of the minimum dimension required for a still accurate reduced mechanism based on automatic time scale decomposition and relaxation of fast modes. We determine species contributions to the active (slow) dynamical modes of the reaction system and exploit this information in combination with quasi-steady-state and partial-equilibrium approximations for explicit model reduction of a novel detailed chemical mechanism for the Ru-catalyzed light-sensitive Belousov-Zhabotinsky reaction. The existence of a minimum dimension of seven is demonstrated to be mandatory for the reduced model to show good quantitative consistency with the full model in numerical simulations. We derive such a maximally reduced seven-variable model from the detailed elementary-step mechanism and demonstrate that it reproduces quantitatively accurately the dynamical features of the full model within a given accuracy tolerance.

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Primary process of illumination effect on the tris(bipyridine)ruthenium(2+)-catalyzed Belousov-Zhabotinskii reaction

Cited by 58 publications

References 0 publications

Reaction Mechanism for Light Sensitivity of the Ru(bpy)₃²⁺-Catalyzed Belousov−Zhabotinsky Reaction

Reaction Mechanism for Light Sensitivity of the Ru(bpy)₃²⁺-Catalyzed Belousov−Zhabotinsky Reaction

Photoinduced Bifurcation and Multistability in the Oscillatory Briggs−Rauscher Reaction

Derivation of a quantitative minimal model from a detailed elementary-step mechanism supported by mathematical coupling analysis

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Primary process of illumination effect on the tris(bipyridine)ruthenium(2+)-catalyzed Belousov-Zhabotinskii reaction

Cited by 58 publications

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Reaction Mechanism for Light Sensitivity of the Ru(bpy)32+-Catalyzed Belousov−Zhabotinsky Reaction

Reaction Mechanism for Light Sensitivity of the Ru(bpy)32+-Catalyzed Belousov−Zhabotinsky Reaction

Photoinduced Bifurcation and Multistability in the Oscillatory Briggs−Rauscher Reaction

Derivation of a quantitative minimal model from a detailed elementary-step mechanism supported by mathematical coupling analysis

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Reaction Mechanism for Light Sensitivity of the Ru(bpy)₃²⁺-Catalyzed Belousov−Zhabotinsky Reaction

Reaction Mechanism for Light Sensitivity of the Ru(bpy)₃²⁺-Catalyzed Belousov−Zhabotinsky Reaction