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Abstract In many electrochemical processes, the transport of charged species is governed by the Nernst–Planck equation, which includes terms for both diffusion and electrochemical migration. In this work, a multi-physics, multi-species model based on the smoothed particle hydrodynamics (SPH) method is presented to model the Nernst–Planck equation in systems with electrodeposition. Electrodeposition occurs when ions are deposited onto an electrode. These deposits create complex boundary geometries, which can be challenging for numerical methods to resolve. SPH is a particularly effective numerical method for systems with moving and deforming boundaries due to its particle nature. This paper discusses the SPH implementation of the Nernst–Planck equations with electrodeposition and verifies the model with an analytical solution and a numerical integrator. A convergence study of migration and precipitation is presented to illustrate the model’s accuracy, along with comparisons of the deposition growth front to experimental results.more » « less
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Lithium metal as an anode has been widely accepted due to its higher negative electrochemical potential and theoretical capacity. Nevertheless, the existing safety and cyclability issues limit lithium metal anodes from practical use in high-energy density batteries. Repeated Li deposition and dissolution processes upon cycling lead to the formation of dendrites at the interface which results in reduced Li availability for electrochemical reactions, disruption in Li transport through the interface and increased safety concerns due to short circuiting. Here, we demonstrate a novel strategy using Ionic Liquid Crystals (ILCs) as the electrolyte cum pseudo-separator to suppress dendrite growth with their anisotropic properties controlling Li-ion mass transport. A thermotropic ILC with two-dimensional Li-ion conducting pathways was synthesized and characterized. Microscopic and spectroscopic analyses elucidate that the ILC formed with a smectic A phase, which can be utilized for wide temperature window operation. The results of electrochemical studies corroborate the efficacy of ILC electrolytes in mitigating dendrite formation even after 850 hours and it is further substantiated by numerical simulation and the mechanism involved in dendritic suppression was deduced.more » « less
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