Hastings Harold M, Sobel Sabrina G, Field Richard J, Bongiovi Dominick, Burke Brianna, Richford Daniel, Finzel Kara, Garuthara Melissa
J Phys Chem A. 2008 May 29;112(21):4715-8. doi: 10.1021/jp8019073. Epub 2008 May 7.
The unstirred, ferroin (Fe(phen)3(2+)) catalyzed Belousov-Zhabotinsky (BZ) reaction is the prototype oscillatory chemical system. Reaction media with added Br(-) appear red (reduced, low [Fe(phen)3(3+)]) during an induction period of several minutes, followed by the "spontaneous" formation of "pacemaker" sites, which oscillate between a blue, oxidized state (high [Fe(phen)3(3+)]) and the red, reduced state and generate target patterns of concentric, outwardly moving waves of oxidation (blue). Auto-oscillatory behavior is also seen in the Oregonator model of Field, Koros and Noyes (FKN), a robust, reduced model that captures qualitative BZ kinetics in the auto-oscillatory regime. However, the Oregonator model predicts a blue (oxidized) induction phase. Here we develop a generalized Oregonator-like model with no explicit bifurcation parameter that yields the observed transition from a red initial state to oscillatory dynamics, and displays a new bifurcation mechanism not seen in the original Oregonator.
未搅拌的亚铁菲罗啉(Fe(phen)₃²⁺)催化的贝洛索夫 - 扎博廷斯基(BZ)反应是典型的振荡化学体系。在添加了Br⁻的反应介质中,在几分钟的诱导期内呈现红色(还原态,低[Fe(phen)₃³⁺]),随后“自发”形成“起搏器”位点,这些位点在蓝色的氧化态(高[Fe(phen)₃³⁺])和红色的还原态之间振荡,并产生同心的、向外移动的氧化波(蓝色)的目标图案。在菲尔德(Field)、科罗斯(Koros)和诺伊斯(Noyes)的俄勒冈模型(FKN)中也观察到自振荡行为,这是一个强大的简化模型,能够捕捉自振荡区域中BZ反应的定性动力学。然而,俄勒冈模型预测有一个蓝色(氧化)诱导期。在此,我们开发了一个类似俄勒冈模型的广义模型,该模型没有明确的分岔参数,能够产生从红色初始状态到振荡动力学的观测转变,并展示了一种在原始俄勒冈模型中未见的新分岔机制。