Galanics Csenge, Szalai István
Eötvös Loránd University, Institute of Chemistry, Pázmány Péter sétány 1/A, Budapest, H-1117, Hungary.
Chemphyschem. 2024 Dec 2;25(23):e202400610. doi: 10.1002/cphc.202400610. Epub 2024 Oct 28.
Complex reaction networks with positive and negative feedback can produce diverse nonlinear phenomena in open reactors, such as multistability and oscillations. pH oscillators driven by hydrogen or hydroxide autocatalytic processes show sustained oscillations in continuously stirred tank reactors (CSTR) but only a sharp pH switch in batch. Here, we present a numerical study on the dynamics of pH oscillators in a series of CSTRs. We show a critical residence time under which bistability and above which oscillations develop. The dynamics of the CSTR cascade show the cross-shaped phase diagram of nonlinear activatory inhibitory systems. In the domain of oscillations, one reactor starts to oscillate autonomously and induces forced complex oscillations in the following tanks with damped amplitudes. These results, with their practical implications, may contribute to understanding the recent experimental observations of nonlinear phenomena in the presence of a residence time ramp and inspire further research in this area.
具有正反馈和负反馈的复杂反应网络可以在开放反应器中产生多种非线性现象,如多重稳定性和振荡。由氢或氢氧根自催化过程驱动的pH振荡器在连续搅拌釜式反应器(CSTR)中表现出持续振荡,但在间歇反应中仅出现急剧的pH切换。在此,我们对一系列CSTR中pH振荡器的动力学进行了数值研究。我们发现了一个临界停留时间,低于该时间会出现双稳性,高于该时间则会产生振荡。CSTR级联的动力学呈现出非线性激活-抑制系统的十字形相图。在振荡区域,一个反应器开始自主振荡,并在随后的反应釜中诱导出振幅衰减的强迫复杂振荡。这些结果及其实际意义,可能有助于理解最近在存在停留时间斜坡情况下的非线性现象的实验观察结果,并激发该领域的进一步研究。