Li Ning, Delgado Jorge, González-Ochoa Hector O, Epstein Irving R, Fraden Seth
Department of Physics, Brandeis University, Waltham, MA 02454-9110, USA.
Phys Chem Chem Phys. 2014 Jun 14;16(22):10965-78. doi: 10.1039/c4cp00957f.
We study the dynamical behavior of one-dimensional arrays of ∼100 μm diameter aqueous droplets containing the oscillatory Belousov-Zhabotinsky (BZ) reaction, separated by narrow gaps of a fluorinated oil. In this closed system, the malonic acid concentration decreases as the reaction proceeds. Starting with a low initial malonic acid concentration, we observe a series of attractors as a function of time in the following order: anti-phase attractors; in-phase attractors, which evolve into traveling waves; and mixed modes that contain either regions of in-phase droplets separated by anti-phase oscillators, or in-phase oscillators combined with non-oscillatory droplets. Most of the observations are consistent with numerical chemical models of the BZ reaction in which components that participate in the excitatory (bromine dioxide and bromous acid) and inhibitory (bromine) pathways diffuse between the droplets. The models are used to quantitatively assess the inter-drop coupling strength as a function of drop separation, drop size and malonic acid concentration. To experimentally establish the mechanism of excitatory coupling between the BZ droplets, we verify the transport through the fluorinated oil of chlorine dioxide and several weak acids, including malonic acid.
我们研究了直径约100μm、含有振荡贝洛索夫-扎博京斯基(BZ)反应的水滴一维阵列的动力学行为,这些水滴被氟化油的窄间隙隔开。在这个封闭系统中,随着反应进行,丙二酸浓度降低。从低初始丙二酸浓度开始,我们观察到一系列随时间变化的吸引子,顺序如下:反相吸引子;同相吸引子,其演变成行波;以及混合模式,其中包含由反相振荡器隔开的同相液滴区域,或同相振荡器与非振荡液滴相结合的区域。大多数观察结果与BZ反应的数值化学模型一致,在该模型中,参与兴奋(二氧化溴和溴酸)和抑制(溴)途径的成分在液滴之间扩散。这些模型用于定量评估作为液滴间距、液滴大小和丙二酸浓度函数的液滴间耦合强度。为了通过实验确定BZ液滴之间的兴奋耦合机制,我们验证了二氧化氯和几种弱酸(包括丙二酸)通过氟化油的传输。