Dynamic Response of Concentrated Electrolytes to Chirp Signals

IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
ACS Nano Pub Date : 2025-04-06 DOI:10.1021/acsnano.4c14099
Emily Krucker-Velasquez, Martin Z. Bazant, Alfredo Alexander-Katz, James W. Swan
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引用次数: 0

Abstract

Electrolytes, chirp signals, Brownian dynamics, conductivity, Maxwell–Wagner relaxation This study investigates the dynamic response of electrolyte/macroion solutions to time-varying electric fields, which is vital for applications from water desalination to neuromorphic computing and sensor technologies. Using large-scale Brownian dynamics simulations coupled with Poisson’s equation, we examined the frequency-dependent conductivity of symmetric and binary electrolytes/nanoparticles across various concentrations. We reveal a comprehensive picture of charge transport mechanisms by employing chirp signals that excite multiple frequencies. Our results identify three distinct dynamic regimes: (1) instantaneous response at low frequencies, (2) increased lagging and imaginary conductivity at intermediate frequencies, and (3) diminished conductivity at high frequencies due to short-time ion/macroion dynamics. Significant deviations from ideal behavior at low frequencies and high concentrations are attributed to packing and many–body interactions. We propose a modified Maxwell–Wagner relaxation time that incorporates excluded volume effects, offering a more accurate time scale for the dynamic response of concentrated electrolytes/macroions. This new framework scales the frequency-dependent conductivity, revealing universal responses across different concentrations and interaction strengths.

Abstract Image

浓缩电解质对啁啾信号的动态响应
本研究探讨了电解质/宏观离子溶液对时变电场的动态响应,这对于从海水淡化到神经形态计算和传感器技术的应用至关重要。利用大规模布朗动力学模拟和泊松方程,研究了对称电解质和二元电解质/纳米颗粒在不同浓度下的频率依赖性电导率。我们通过使用激发多个频率的啁啾信号揭示了电荷传输机制的全面图景。我们的研究结果确定了三种不同的动态机制:(1)低频时的瞬时响应;(2)中频时滞后和虚电导率增加;(3)由于短时间离子/宏离子动力学,高频时电导率降低。在低频率和高浓度下与理想行为的显著偏差归因于堆积和多体相互作用。我们提出了一个修正的麦克斯韦-瓦格纳弛豫时间,其中包含了排除的体积效应,为浓缩电解质/宏离子的动态响应提供了更准确的时间尺度。这个新的框架衡量了频率相关的电导率,揭示了不同浓度和相互作用强度下的普遍反应。
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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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