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Electrochemical ion insertion involves coupled ion-electron transfer reactions, transport of guest species, and redox of the host. The hosts are typically anisotropic solids with two-dimensional conduction planes, but can also be materials with one-dimensional or isotropic transport pathways. These insertion compounds have traditionally been studied in the context of energy storage, but also find extensive applications in electrocatalysis, optoelectronics, and computing. Recent developments in operando, ultrafast, and high-resolution characterization methods, as well as accurate theoretical simulation methods, have led to a renaissance in the understanding of ion-insertion compounds. In this Review, we present a unified framework for understanding insertion compounds across time and length scales ranging from atomic to device levels. Using graphite, transition metal dichalcogenides, layered oxides, oxyhydroxides, and olivines as examples, we explore commonalities in these materials in terms of point defects, interfacial reactions, and phase transformations. We illustrate similarities in the operating principles of various ion-insertion devices ranging from batteries and electrocatalysts to electrochromics and thermal transistors, with the goal of unifying research across disciplinary boundaries.
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We report on resistive switching of memristive electrochemical metallization devices using 3D kinetic Monte Carlo simulations describing the transport of ions through a solid state electrolyte of an Ag/TiO$_{text{x}}$/Pt thin layer system. The ion transport model is consistently coupled with solvers for the electric field and thermal diffusion. We show that the model is able to describe not only the formation of conducting filaments but also its dissolution. Furthermore, we calculate realistic current-voltage characteristics and resistive switching kinetics. Finally, we discuss in detail the influence of both the electric field and the local heat on the switching processes of the device.
In this work we report on kinetic Monte-Carlo calculations of resistive switching and the underlying growth dynamics of filaments in an electrochemical metallization device consisting of an Ag/TiO2/Pt sandwich-like thin film system. The developed model is not limited to i) fast time scale dynamics and ii) only one growth and dissolution cycle of metallic filaments. In particular, we present results from the simulation of consecutive cycles. We find that the numerical results are in excellent agreement with experimentally obtained data. Additionally, we observe an unexpected filament growth mode which is in contradiction to the widely acknowledged picture of filament growth, but consistent with recent experimental findings.
Conjugated polymer-based organic electrochemical transistors (OECTs) are being studied for applications ranging from biochemical sensing to neural interfaces. While new conjugated polymers are being developed that can interface digital electronics with the aqueous chemistry of life, the vast majority of high-performance, high-mobility organic transistor materials developed over the past decades are extremely poor at taking up biologically-relevant ions. Here we incorporate an ion exchange gel into an OECT, demonstrating that this structure is capable of taking up biologically-relevant ions from solution and injecting larger, more hydrophobic ions into the underlying polymer semiconductor active layer in multiple hydrophobic conjugated polymers. Using poly[2,5-bis(3-tetradecylthiophen-2-yl) thieno[3,2-b]thiophene] (PBTTT) as a model semiconductor active layer and a blend of the ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (BMIM TFSI) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) as the ion exchange gel, we demonstrate more than a four order of magnitude improvement in OECT device transconductance and a one hundred-fold increase in ion injection kinetics. We demonstrate the ability of the ion exchange gel OECT to record biological signals by measuring the action potentials of a Venus flytrap plant. These results show the possibility of using interface engineering to open up a wider palette of organic semiconductor materials as OECTs that can be gated by aqueous solutions.
In this work we report on the role of ion transport for the dynamic behavior of a double barrier quantum mechanical Al/Al$_2$O$_3$/Nb$_{text{x}}$O$_{text{y}}$/Au memristive device based on numerical simulations in conjunction with experimental measurements. The device consists of an ultra-thin Nb$_{text{x}}$O$_{text{y}}$ solid state electrolyte between an Al$_2$O$_3$ tunnel barrier and a semiconductor metal interface at an Au electrode. It is shown that the device provides a number of interesting features for potential applications such as an intrinsic current compliance, a relatively long retention time, and no need for an initialization step. Therefore, it is particularly attractive for applications in highly dense random access memories or neuromorphic mixed signal circuits. However, the underlying physical mechanisms of the resistive switching are still not completely understood yet. To investigate the interplay between the current transport mechanisms and the inner atomistic device structure a lumped element circuit model is consistently coupled with 3D kinetic Monte Carlo model for the ion transport. The simulation results indicate that the drift of charged point defects within the Nb$_{text{x}}$O$_{text{y}}$ is the key factor for the resistive switching behavior. It is shown in detail that the diffusion of oxygen modifies the local electronic interface states resulting in a change of the interface properties of the double barrier device.
Metal hydrides are critical materials in numerous technologies including hydrogen storage, gas separation, and electrocatalysis. Here, using Pd-H as a model metal hydride, we perform electrochemical insertion studies of hydrogen via liquid and solid state electrolytes at 1 atm ambient pressure, and achieve H:Pd ratios near unity, the theoretical solubility limit. We show that the compositions achieved result from a dynamic balance between the rate of hydrogen insertion and evolution from the Pd lattice, the combined kinetics of which are sufficiently rapid that operando experiments are necessary to characterize instantaneous PdHx composition. We use simultaneous electrochemical insertion and X-ray diffraction measurements, combined with a new calibration of lattice parameter versus hydrogen concentration, to enable accurate quantification of the composition of electrochemically synthesized PdHx. Furthermore, we show that the achievable hydrogen concentration is severely limited by electrochemomechanical damage to the palladium and/or substrate. The understanding embodied in these results helps to establish new design rules for achieving high hydrogen concentrations in metal hydrides.
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