Nonlinear Dynamics of Electrochemical Reaction Networks

电化学反应网络的非线性动力学

• 批准号: 1900011
• 负责人: Istvan Kiss
• 金额: $ 42万
• 依托单位: Saint Louis University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-08-01 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1900011&HistoricalAwards=false
• 关键词: Nonlinear; Dynamics; Electrochemical; Reaction; Networks

With this award, the Chemical Structure, Dynamics and Mechanisms (CSDM-A) Program of the Division of Chemistry is funding Professor Istvan Z. Kiss and his research group at Saint Louis University to study pattern formation of electrochemical reactions. For most chemical reactions that occur in gaseous or liquid conditions, the reacting atoms or molecules steadily decrease in number, and the product atoms or molecules steadily increase in number until the reaction is complete (or, we say when it reaches "equilibrium"). Prof. Kiss is interested in so-called oscillating chemical reactions, in which the number of molecules of certain substances fall and rise with time. In other words, the reaction sometimes proceeds in the forward direction, and at other times in the reverse! Oscillating reactions can produce solutions that switch from blue to yellow color and back to blue, or they can produce patterns of color that may resemble zebra stripes or leopard spots. Such pattern formation is an example of chemical reaction networks, which are not yet fully understood but are very relevant to how living systems evolve and function. Prof. Kiss' research adds another twist to oscillating reactions: rather than just mixing reactants together in a beaker, he generates reactants with electrodes immersed in the solution. For example, nickel electrodes can generate nickel ions (Ni(2+)) at a precisely controlled rate. This means that the oscillations and patterns created can be controlled, and in turn the chemical network behavior better understood. In addition to its relevance to biological systems, this research also has implications for battery and energy technologies. The graduate students and post-doctoral scientists involved in this project are immersed in a multidisciplinary experience that spans not only chemistry, but data science, mathematics, and biology.The overarching objective of this project is to discover the laws that govern self-organization and pattern formation in complex, far-from-equilibrium charge transfer chemical reactions. The project is following three tracks: 1) Spatially Organized Electrochemical Media on the Microscale. The emergent networks that form in lab-on-chip devices are decoded. The coupling topology among the microelectrodes is used to identify novel types of dynamical structures with simple equilibrium reactions, including metal dissolution systems (Ni(0)/Ni(2+), Cu(0)/Cu(2+)) and the H2 oxidation reaction. 2) Cathode-Anode Interactions: The nature and structure of cathode-anode interactions are determined with bipolar electrodes and serially coupled electrochemical cells. Models of network topology developed in this study are tested for their utility in describing the dynamics of battery cells. 3) Chimera Patterns on Designed Electrochemical Networks: Modular networks of current generating reactions are built with known network configurations. The resilience and the scalability of the localization of the synchronization patterns are explored by changing the number of elements in each module and the number of modules. In addition to the aforementioned formal training of students and post-doctoral researchers, demonstrations of nonlinear chemical dynamics are being incorporated into the undergraduate curriculum, as well as public outreach events.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

化学系化学结构、动力学和机理（CSDM-A）项目将资助圣路易斯大学的Istvan Z. Kiss教授和他的研究小组研究电化学反应的模式形成。对于大多数在气态或液态条件下发生的化学反应来说，反应中的原子或分子的数量稳步减少，而生成物的原子或分子的数量稳步增加，直到反应完成（或者，我们说，当它达到“平衡”时）。基斯教授对所谓的振荡化学反应感兴趣，在振荡化学反应中，某些物质的分子数量随着时间的推移而下降和上升。换句话说，反应有时正向进行，有时反向进行！振荡反应可以产生从蓝色到黄色再变回蓝色的溶液，或者它们可以产生类似斑马条纹或豹纹的颜色模式。这种模式的形成是化学反应网络的一个例子，它还没有完全被理解，但与生命系统如何进化和运作非常相关。基斯教授的研究为振荡反应增添了另一种变化：他不是仅仅在烧杯中混合反应物，而是将电极浸入溶液中生成反应物。例如，镍电极可以以精确控制的速率生成镍离子（Ni(2+)）。这意味着产生的振荡和模式是可以控制的，从而更好地理解化学网络的行为。除了与生物系统相关外，这项研究还对电池和能源技术有影响。参与该项目的研究生和博士后科学家沉浸在不仅跨越化学，而且跨越数据科学，数学和生物学的多学科体验中。这个项目的首要目标是发现在复杂的、远离平衡的电荷转移化学反应中控制自组织和模式形成的规律。项目主要有三个方向：1)微观尺度上的空间组织电化学介质。在芯片实验室设备中形成的紧急网络被解码。利用微电极间的耦合拓扑结构来识别具有简单平衡反应的新型动力学结构，包括金属溶解体系(Ni(0)/Ni(2+), Cu（0)/Cu(2+)）和H2氧化反应。2)阴极-阳极相互作用：阴极-阳极相互作用的性质和结构由双极电极和串联耦合电化学电池决定。本研究中开发的网络拓扑模型在描述电池单元动力学方面的效用进行了测试。3)设计的电化学网络上的嵌合体模式：利用已知的网络结构构建电流生成反应的模块化网络。通过改变每个模块中元素的数量和模块的数量，探索同步模式本地化的弹性和可伸缩性。除了上述对学生和博士后研究人员的正式培训外，非线性化学动力学的演示也被纳入本科课程，以及公共宣传活动。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Anti-phase collective synchronization with intrinsic in-phase coupling of two groups of electrochemical oscillators

两组电化学振荡器具有固有同相耦合的反相集体同步

• DOI: 10.1098/rsta.2019.0095
• 发表时间: 2019
• 期刊: Physical and Engineering Sciences
• 作者: Sebek, Michael;Kawamura, Yoji;Nott, Ashley M.;Kiss, István Z.
• 通讯作者: Kiss, István Z.

A unified and automated approach to attractor reconstruction

• DOI: 10.1088/1367-2630/abe336
• 发表时间: 2021-03-01
• 期刊: NEW JOURNAL OF PHYSICS
• 影响因子: 3.3
• 作者: Kraemer, K. H.;Datseris, G.;Marwan, N.
• 通讯作者: Marwan, N.

Random heterogeneity outperforms design in network synchronization

• DOI: 10.1073/pnas.2024299118
• 发表时间: 2021-05
• 期刊: Proceedings of the National Academy of Sciences
• 作者: Yuanzhao Zhang;J. L. Ocampo-Espindola;I. Kiss;A. Motter

Synchronization of Belousov–Zhabotinsky oscillators with electrochemical coupling in a spontaneous process

Belousov–Zhabotinsky 振荡器与自发过程中电化学耦合的同步

• DOI: 10.1063/5.0096689
• 发表时间: 2022
• 期刊: Chaos: An Interdisciplinary Journal of Nonlinear Science
• 作者: Liu, Yifan;Pérez-Mercader, Juan;Kiss, István Z.
• 通讯作者: Kiss, István Z.

Asymmetry-induced isolated fully synchronized state in coupled oscillator populations

耦合振荡器群体中不对称引起的隔离完全同步状态

• DOI: 10.1103/physreve.104.l022202
• 发表时间: 2021
• 期刊: Physical Review E
• 影响因子: 2.4
• 作者: Omel'chenko, Oleh E.;Ocampo-Espindola, Jorge Luis;Kiss, István Z.
• 通讯作者: Kiss, István Z.