Ion Transport In Electrolytes Research Articles

Recent Trends in Application of Memristor in Neuromorphic Computing: A Review

Abstract: Recently memristors have emerged as a form of nonvolatile memory that is based on the principle of ion transport in solid electrolytes under the impact of an external electric field. It is perceived as one of the key elements to building next-generation computing systems owing to its peculiar resistive switching characteristics. The switching mechanism in a memristor is mainly governed by filamentary conduction. Further, it can be employed as a memory as well as a logic element, which makes it an ideal candidate for building innovative computer architecture. Moreover, it is capable of mimicking the characteristics of biological synapses, which makes it an ideal candidate for developing a Neuromorphic system. In this review to begin with the switching mechanism of the memristor, primarily focusing on filamentary conduction, is discussed. Few SPICE models of memristor are reviewed, and their critical comparison is performed, which are widely used to build computing systems. An in-depth study on the various crossbar memory architecture augmented with memristors is reviewed. Finally, the application of memristors in neuromorphic computing and hardware implementation of Artificial Neural Networks (ANN) employing memristors is discussed.

Percolating coordinated ion transport cells in polymer electrolytes to realize room-temperature solid-state lithium metal batteries

Polymer electrolytes, notable for their good mechanical properties, superior processability, and high electrochemical stability, are promising for high-energy-density lithium metal batteries. However, the ionic conduction of polymer electrolytes is seriously constrained by either the entanglement of polymer chains or binding of anions, particularly at ambient temperatures, making their practical application impossible. Herein, we employ a high-salt-concentration strategy with poly(vinylene carbonate) to construct a percolating network by linking coordinated ion transport cells. The cells, consisting of lithium-ion at the core surrounded by coordinated poly(vinylene carbonate), N,N-dimethylformamide, or incompletely bonded bis(trifluoromethanesulfonyl)imide, ensure an efficient coordination and de-coordination process for ion transport. Thus, a high rate of Li+ transport is realized, achieving an ionic conductivity of 0.82 mS cm−1 at 30 °C. Consequently, the formulated solid-state lithium metal batteries with the poly(vinylene carbonate) electrolyte enable superior stability in cycling under a wide temperature range (0–60 °C), high working voltage (4.5 V), and high mass load (>10 mg cm−2). This simple strategy for creating an ion-percolating network by linking coordinated ion transport cells not only offers new insights into understanding the mechanism for ion transport in polymer electrolytes but also paves the way for the application of solid-state lithium metal batteries.

Upgrading Gel Electrolytes Through Electrostatic-Induced Dual-Salt Paradigm for Superior Zn-Ion Battery Performance.

Gel electrolytes are gaining attention for rechargeable Zn-ion batteries because of their high safety, high flexibility, and excellent comprehensive electrochemical performances. However, current gel electrolytes still perform at mediocre levels due to incomplete Zn salts dissociation and side reactions. Herein, an electrostatic-induced dual-salt strategy is proposed to upgrade gel electrolytes to tackle intrinsic issues of Zn metal anodes. The competitive coordination mechanism driven by electrostatic repulsion and steric hindrance of dual anions promotes zinc salt dissociation at low lithium salt addition levels, improving ion transport and mechanical properties of gel electrolytes. Li+ ions and gel components coordinate with H2O, reducing active H2O molecules and inhibiting associated side reactions. The dual-salt gel electrolyte enables excellent reversibility of Zn anodes at both room and low temperatures. Zn||Polyaniline cells using the dual-salt gel electrolyte exhibit a high discharge capacity of 180mAhg-1 and long-term cycling stability over 180 cycles at -20°C. The dual-salt strategy offers a cost-effective approach to improving gel electrolytes for high-performance flexible Zn-ion batteries.

Unlocking dual-band electrochromism with stacked structure of amorphous tungsten oxide and Prussian blue

Dual-band electrochromic smart windows can selectively regulate the transmittance of visible and near-infrared (NIR) light, thereby significantly reducing energy consumption in buildings. However, the selective regulation for visible and NIR regions often relies on the integration of multiple components, together with meticulous design and fabrication. Herein, we propose the stacking of amorphous tungsten oxide (a-WO3) on the surface of Prussian blue (PB) through a straightforward magnetron sputtering deposition. Benefiting from the numerous voids-containing structures in the microstructure of a-WO3 films, the stacking structures are conducive to the insertion and transport of electrolyte ions, ensuring the electrochemical activity and electrochromic performance of the inner PB layer. The prepared PB/WO3 bilayer thin film can achieve three functionality modes in dual-band electrochromism: “bright”, “warm”, and “dark”, with high optical modulation of 74.9 % at 700 nm and 80.3 % at 1300 nm, respectively. Additionally, they demonstrate fast coloring/bleaching response (2.9/7.6 s at 700 nm and 6.0/6.2 s at 1300 nm) and satisfying cycling stability (retaining 95.3 % of its initial modulation after 500 cycles). The bilayer thin films based on amorphous electrochromic materials with an intrinsic abundance of voids-containing structures introduce a novel approach to the independent dual-band modulation for demanded light/thermal control.

Enhanced Supercapacitive Performance in Catalyst‐Free Binary Composite SnO2–RuO2 Nanostructured Thin Films for Symmetric Supercapacitor Device

In the present work, thin film electrodes of ruthenium oxide (RuO2), tin oxide (SnO2), and their composite SnO2–RuO2 are deposited on 304 stainless steel substrates using pulsed laser deposition (PLD). These nanostructured electrodes are then evaluated for their suitability in electrochemical energy storage applications. A symmetric supercapacitor device (SSD) is constructed using the SnO2–RuO2 composite electrodes. Compared to individual SnO2 and RuO2 electrodes, the composite electrodes exhibit enhanced specific capacitance and cycle life. This improvement is attributed to modifications in surface morphology and electronic properties. This modified surface morphology of the composite electrode, creates favourable conditions for electrolyte interaction and ion transport, ultimately contributing to the observed increase in specific capacitance. Specifically, the composite electrode demonstrates a specific capacitance of 170.2 Fg−1 at a current density of 0.1 mA cm−2, outperforming SnO2 (37.4 Fg−1). The SnO2–RuO2//SnO2–RuO2 SSD exhibites a specific capacitance of 70.0 Fg−1 at a current density of 0.1 mA cm−2, coupled with energy density and power density values of 19.05 Wh kg−1 and 645 W kg−1, respectively, within a voltage window of 1.4 V. The SSD displays an impressive capacitive retention of 81.27% over 10 000 cycles, indicating its potential for practical energy storage applications.

A rigid free-standing supercapacitor electrode material made from fat coal-based activated carbon foam

A free-standing electrode material is a competitive candidate for supercapacitor due to its excellent capacity and volumetric energy density. Currently, most of the studies are focused on the preparations and performances of flexible free-standing electrode materials, whereas few on the development of rigid free-standing electrode materials. Herein, a vitrinite concentrate of fat coal is used as a raw material and carbon black as an addition agent to prepare a carbon foam by way of high-pressure pyrolysis. The prepared carbon foam is activated by KOH solution to further achieve an activated carbon foam by which we have fabricated a rigid free-standing electrode material. The assembled symmetric device with the rigid free-standing electrode material demonstrates an extremely high areal specific capacitance of 2304.41 mF cm−2 at 4 mA cm−2, an outstanding cycling stability of 100 % after 40 000 cycles, and an excellent volume energy density of 10.23 mWh cm−3 at 31.78 mW cm−3. These fascinating electrochemical performances of the electrode material are attributed to unique 3D interconnected porous structure of the activated carbon foam. The micron-sized 3D interconnected pores facilitate the transport of electrolyte ions within the electrodes. Meanwhile, micropores on the 3D interconnected pore wall provide abundant active sites for electrolyte ions.

Towards optimized cation-exchange membranes for overlimiting current electrodialysis: Correlation between size of resin particles in membranes and mechanism of ion transport through them

Experimental heterogeneous membranes with different particle sizes of cation-exchange resin KU-2–8 (the diameter of resin particles varied from 20 to 71 μm) were manufactured under the production conditions of LLC “IE “Shchekinoazot”. It is established that at currents higher than the limiting current the main mechanisms of electrolyte ion transport are classical electrodiffusion and electroconvection. It is shown for the first time that at the same degree of membrane polarization i/ilim the fraction of electroconvection contribution increases, and the fraction of contribution of water splitting reaction products decreases with decreasing size of resin particles in membranes. The theoretical evaluation of the influence of the size of resin particles in the membrane on the internal parameters of electromembrane systems MK-40/0.01M NaCl solution has shown that the crucial role in the development of electroconvection is played not by the field effect, but by the peculiarities of electrical heterogeneity of the membrane surface.

Molecular-scale interaction between sub-1 nm cluster chains and polymer for high-performance solid electrolyte

Organic-inorganic interface in composite solid electrolyte could lead to increased ion transport for solid-state lithium batteries; however, most inorganic fillers have much larger size than polymer chains, which results in severe aggregation of inorganic fillers and poor ionic conductivity. Herein, functional sub-1 nm inorganic cluster chains were integrated with polymer chains to fabricate composite solid electrolyte with enhanced ionic conductivity. Different from all other inorganic fillers, the sub-1 nm inorganic cluster chains with diameter <1 nm have similar size and geometry compared with polymer chains, exhibiting polymer-like solution properties. A transparent sub-1 nm inorganic filler/polymer mixed solution was generated to realize monodispersion of cluster chains as functional fillers in polymer matrix. Meanwhile, abundant oxygen vacancies on cluster chains interact with polymer chains and lithium salts at molecular-scale, which decreases the complexation of polymer segments with Li+ and promote the dissociation of lithium salts, thereby improving Li+ transport. As a result, the composite solid electrolyte exhibits high ionic conductivity (0.4 mS cm−1) and large mobile Li+ distribution (50.8 %). This work pushes the size of nanofillers down to <1 nm, which is a unique approach to the molecular-scale interaction between nanofillers and polymers to boost ion transport in solid electrolytes.

Ion Transport in Polymer Electrolytes: Building New Bridges between Experiment and Molecular Simulation.

ConspectusPolymer electrolytes constitute a promising type of material for solid-state batteries. However, one of the bottlenecks for their practical implementation lies in the transport properties, often including restricted Li+ self-diffusion and conductivity and low cationic transference numbers. This calls for a molecular understanding of ion transport in polymer electrolytes in which molecular dynamics (MD) simulation can provide both new physical insights and quantitative predictions. Although efforts have been made in this area and qualitative pictures have emerged, direct and quantitative comparisons between experiment and simulation remain challenging because of the lack of a unified theoretical framework to connect them.In our work, we show that by computing the glass transition temperature (Tg) of the model system and using the normalized inverse temperature 1000/(T - Tg + 50), the Li+ self-diffusion coefficient can be compared quantitatively between MD simulations and experiments. This allows us to disentangle the effects of Tg and the polymer dielectric environment on ion conduction in polymer electrolytes, giving rise to the identification of an optimal solvating environment for fast ion conduction.Unlike Li+ self-diffusion coefficients and ionic conductivity, the transference number, which describes the fraction of current carried by Li+ ions, depends on the boundary conditions or the reference frame (RF). This creates a non-negligible gap when comparing experiment and simulation because the fluxes in the experimental measurements and in the linear response theory used in MD simulation are defined in different RFs. We show that by employing the Onsager theory of ion transport and applying a proper RF transformation, a much better agreement between experiment and simulation can be achieved for the PEO-LiTFSI system. This further allows us to derive the theoretical expression for the Bruce-Vincent transference number in terms of the Onsager coefficients and make a direct comparison to experiments. Since the Bruce-Vincent method is widely used to extract transference numbers from experimental data, this opens the door to calibrating MD simulations via reproducing the Bruce-Vincent transference number and using MD simulations to predict the true transference number.In addition, we also address several open questions here such as the time-scale effects on the ion-pairing phenomenon, the consistency check between different types of experiments, the need for more accurate force fields used in MD simulations, and the extension to multicomponent systems. Overall, this Account focuses on building new bridges between experiment and simulation for quantitative comparison, warnings of pitfalls when comparing apples and oranges, and clarifying misconceptions. From a physical chemistry point of view, it connects to concentrated solution theory and provides a unified theoretical framework that can maximize the power of MD simulations. Therefore, this Account will be useful for the electrochemical energy storage community at large and set examples of how to approach experiments from theory and simulation (and vice versa).

Investigation of ion transport in plasticized polymer electrolytes using electrical equivalent circuit (EEC) modeling

Investigation of ion transport in plasticized polymer electrolytes using electrical equivalent circuit (EEC) modeling

Boosting the pseudocapacitance of BiFeO3 by Zn doping for flexible battery-supercapacitor hybrid devices

Perovskite BiFeO3 (BFO) as a type of battery-type electrode materials, usually suffers from poor electrolyte ion transport in the BFO crystal. We propose a novel strategy of Zn doping to improve the ion transport and boost the faradaic pseudocapacitance of BFO for flexible battery-supercapacitor hybrid (BSH) devices. The Zn-doped BFO (Z-BFO-1) with the low Zn doping content, can maintain the crystal structure of BFO and the uniform distributions of elements. The oxygen vacancy content can be increased from BFO to Z-BFO-1, reflecting the influence of the Zn doping on the crystal structure of BFO. The Z-BFO-1 electrode with the stable crystal structure in the charge/discharge process, can provide the highest specific capacitance (223 F g−1 at 0.2 A/g) and the largest Li+ diffusion coefficient (2.386 × 10−11 cm2 s−1) among these BFO-based electrodes with different Zn doping contents. The first-principles calculations reveal that the Zn doping in BFO can significantly enhance the built-in electric fields and greatly lower the Li+ migration energy barriers (from 2.08 eV to 1.43 eV). This flexible MnO2//Z-BFO-1 BSH device with the high energy density (37.5 Wh kg−1 at 0.23 kW kg−1), opens up a new avenue for developing high-performance electrochemical energy storage devices.

Preparation of hierarchical porous carbon sieve through the decomposition-templating of NaHCO3 for high areal energy density micro-supercapacitor

Porous carbon proves a crucial electrode material for micro-supercapacitors (MSCs) due to its favourable electrical conductivity, along with chemical and thermal stability. Nevertheless, the low area accessible to ions and the long electron diffusion paths commonly result in a low energy density for carbon-based MSCs. Here, an alga-based carbon sieve with an interconnected and hierarchical porous structure was prepared and employed as the electrode material to construct MSCs by 3D printing. The interconnected and hierarchical structure facilitates electrolyte diffusion and ion transport, resulting in a high specific capacitance of 145 mF cm−2 and an impressive energy density of 20.14 μWh cm−2 for the MSC. Moreover, the device exhibits excellent mechanical properties and long cycle life. These findings demonstrate the potential of devices for application in microelectronic devices.

Regulating porous structure of coal-derived carbon materials by a dual-activation for high performance supercapacitors

Porous carbon plays an important role in supercapacitors with its favorable electrical conductivity, highly porous structure and superior chemical stability. However, the deep and tortuous ultramicropores in porous carbon greatly restricts the transport and transfer of electrolyte ions, resulting in the inferior electrochemical performance. Therefore, we propose a facile and green chemical activation method that uses KHCO3 and Zn(CH3COO)2·2H2O as dual activators to modulate the porous carbon structure. The synergistic activation between KHCO3 and Zn(CH3COO)2·2H2O endows the obtained porous carbons with hierarchical porous structure, honeycomb-like morphology and large specific surface area (1282 m2 g−1). In the three-electrode system, the optimal sample displays superior rate performance (70 % capacitance retention @ 50 A g−1) and high specific capacitance (321 F g−1 @ 1 A g−1). Symmetric two-electrode configurations were tested in 6 M KOH electrolyte, splendid cycling stability was observed (100 % capacity maintained after 10,000 cycles at 5 A g−1). Moreover, the symmetric supercapacitor assembled with neat EMIM BF4 as the electrolyte reveals a high energy density of 33 Wh kg−1 @ 624.6 W kg−1. This work offers new insights to manipulate the morphology and pore structure of coal-derived porous carbon for high performance supercapacitor electrode.

A Scalable Dendritic Si‐Clad NiSn Anode via One‐Step Electrodeposition with Ultrahigh Areal Capacity for Micro Lithium‐Ion Battery

High energy density, long cyclability, and enhanced stability in a small footprint achieved through microfabrication are crucial for micro lithium‐ion batteries. Herein, a 3D Si‐clad NiSn anode characterized by a dendritic NiSn network and silicon nanoparticles is proposed. The dendritic network facilitates fast ion/electron transfer and provides expansion space for the silicon, while the uniformly distributed silicon enhances capacity and stability. The anode, scalable to the hundred‐micron scale, is fabricated via one‐step electrodeposition incorporating the dynamic template technique. This technique generates interconnected pores extending from the inner to the outer surface of the anode, facilitating electrolyte penetration and ion transport. As a result, the anodes in the Swagelok cells exhibit an ultrahigh areal capacity of up to 28.2 mAh cm−2 and an enhanced stability of 91% capacity retention after 300 cycles. The dendritic Si‐clad NiSn anode, based on microfabrication, presents an excellent opportunity to advance micro energy systems.

Ethylene Glycol‐Containing Acrylic Polyphosphazene Based Cathode Materials via Inverse Vulcanization of Sulfur for Li−S Batteries

AbstractThe cell performance of Li−S batteries can be improved by establishing compatibility with the electrolyte of cathode and enhancing lithium‐ion diffusion (ionic conductivity) or electrical conductivity. In this work, we introduce cathode material based on ethylene glycol‐containing acrylic polyphosphazene. Poly[(2acrylamidoethoxy)‐random‐(methoxyethoxyethoxy)] phosphazenes were synthesized by macromolecular substitution of poly(dichloro)phosphazene with 2‐acrylamidoethanol and diethylene glycol methyl ether in two different ratios (25 and 50 mol% of ethylene glycol methyl ether), abbreviated as MP‐25EG and MP‐50EG, where ethylene glycol chains enhance the electrolyte compatibility and ion transport of the sulfur cathode material. Then, poly[S‐random‐(2acrylamidoethoxy)‐random‐(methoxyethoxyethoxy)] phosphazene polymers, designated as MP‐25EG‐xS or MP‐50EG‐xS (x=50 and 80 wt.% of sulfur) were prepared by inverse vulcanization of polymer with two feed sulfur ratios. Structural characterizations of the polymers were carried out using appropriate standard spectroscopic methods such as 1H and 31P NMR, FT‐IR, DSC and TGA as well as XPS. The electrochemical performance of MP‐25EG‐50S, MP‐25EG‐80S and MP‐50EG‐50S, MP‐50EG‐80S were evaluated and the effect of ethylene glycol was investigated by comparing cell performances. MP‐50EG‐50S demonstrated its promising applicability in Li–S batteries by exhibiting much better electrochemical respond with a discharge capacity of 745 mAh/g at C/5 current density over 100 cycles.

Hierarchically Porous 3D Freestanding Holey-MXene Framework via Mild Oxidation of Self-Assembled MXene Hydrogel for Ultrafast Pseudocapacitive Energy Storage.

The true promise of MXene as a practical supercapacitor electrode hinges on the simultaneous advancement of its three-dimensional (3D) assembly and the engineering of its nanoscopic architecture, two critical factors for facilitating mass transport and enhancing an electrode's charge-storage performance. Herein, we present a straightforward strategy to engineer robust 3D freestanding MXene (Ti3C2Tx) hydrogels with hierarchically porous structures. The tetraamminezinc(II) complex cation ([Zn(NH3)4]2+) is selected to electrostatically assemble colloidal MXene nanosheets into a 3D interconnected hydrogel framework, followed by a mild oxidative acid-etching process to create nanoholes on the MXene surface. These hierarchically porous, conductive holey-MXene frameworks facilitate 3D transport of both electrons and electrolyte ions to deliver an excellent specific capacitance of 359.2 F g-1 at 10 mV s-1 and superb capacitance retention of 79% at 5000 mV s-1, representing a 42.2% and 15.3% improvement over pristine MXene hydrogel, respectively. Even at a commercial-standard mass loading of 10.1 mg cm-2, it maintains an impressive capacitance retention of 52% at 1000 mV s-1. This rational design of an electrode by engineering nanoholes on MXene nanosheets within a 3D porous framework dictates a significant step forward toward the practical use of MXene and other 2D materials in electrochemical energy storage systems.

Urchin-like Ce(HCOO)3 Synthesized by a Microwave-Assisted Method and Its Application in an Asymmetric Supercapacitor.

In this work, a series of urchin-like Ce(HCOO)3 nanoclusters were synthesized via a facile and scalable microwave-assisted method by varying the irradiation time, and the structure-property relationship was investigated. The optimization of the reaction time was performed based on structural characterizations and electrochemical performances, and the Ce(HCOO)3-210 s sample shows a specific capacitance as high as 132 F g-1 at a current density of 1 A g-1. This is due to the optimal mesoporous hierarchical structure and crystallinity that are beneficial to its conductivity, offering abundant Ce3+/Ce4+ active sites and facilitating the transportation of electrolyte ions. Moreover, an asymmetric supercapacitor based on Ce(HCOO)3//AC was fabricated, which delivers a maximum energy density of 14.78 Wh kg-1 and a considerably high power density of 15,168 W kg-1. After 10,000 continuous charge-discharge cycles at 3 A g-1, the ASC device retains 81.3% of its initial specific capacitance. The excellent comprehensive electrochemical performance of this urchin-like Ce(HCOO)3 offers significant promise for practical supercapacitor applications.

Mechanisms of ion transport in lithium salt-doped zwitterionic polymer-supported ionic liquid electrolytes.

Recent experimental results have demonstrated that zwitterionic ionogel comprised of polyzwitterion (polyZI)-supported lithium salt-doped ionic liquid exhibits improved conductivities and lithium transference numbers than the salt-doped base ionic liquid electrolyte (ILE). However, the underlying mechanisms of such observations remain unresolved. In this work, we pursued a systematic investigation to understand the impact of the polyZI content and salt concentration on the structural and dynamic properties of the poly(MPC) ionogel of our model polyZI ionogel, poly(2-methacryloyloxyethyl phosphorylcholine) [poly(MPC)] supported LiTFSI/N-butyl-N-methylpyrrolidinium TFSI base ionic liquid electrolyte. Our structural analyses show strong lithium-ZI interaction consistent with the physical network characteristic observed in the experiments. An increase in polyZI content leads to an increased fraction of Li+ ions coordinated with the polyZI. In contrast, an increase in salt concentration leads to a decreased fraction of Li+ ions coordinated with the polyZI. The diffusivities of the mobile ions in the poly(MPC) ionogel were found to be lower than the base ILE in agreement with experiments at T > 300K. Analysis of ion transport mechanisms shows that lithium ions within the poly(MPC) ionogel travel via a combination of structural, vehicular diffusion, as well as hopping mechanism. Finally, the conductivity trend crossover between the poly(MPC) ionogel and the base ILE was rationalized via a temperature study that showed that the base ILE ions are influenced more by the variation of temperature when compared to the poly(MPC) ions.

Reinforced electrochemical energy storage through controlled construction of hierarchical hollow β-Ni(OH)2 microspheres enriched with oxygen vacancies induced by functionalized MWCNTs

As promising electrode materials, hollow-structured metallic oxides/hydroxides have attracted extensive attention for their significantly enhanced catalyst and electrochemical performances. In practice, however, it is still challenging to construct well-dispersed hollow structures using facile and versatile template-free methods. And, as a result of the weak conductivity of most metallic oxides/hydroxides, it is a particularly effective means to integrate metallic oxides/hydroxides with carbon-based conductive substrates or introduce oxygen vacancies for further promoting reaction kinetics and achieving boosted electrochemical performance. Herein, a novel composite material consisting of oxygen-rich vacancy β-Ni(OH)2 coupled with oxidized multi-wall carbon nanotubes (Ov-Nβ/Cm) was synthesized using a one-step hydrothermal technique without the need for templates. The hierarchical hollow microsphere structure was achieved by utilizing oxidized multi-wall carbon nanotubes (MWCNTs) as an alternative to conventional surfactants or templates. The uniform distribution of multistage pores in the newly designed Ov-Nβ/Cm composite facilitates the transportation of electrolyte ions, thereby endowing it with outstanding electrochemical performance. A straightforward technique for producing high-quality Ni(OH)2-based electrode materials is presented in this investigation, along with fresh perspectives on the formation mechanism of hollow-structured composites. Developing MWCNT-based hollow nanostructured composites with oxygen vacancies-enriched will offer an essential novel avenue to exploit excellent electrode materials for supercapacitors and other energy storage systems.

Ion Transport in (Localized) High Concentration Electrolytes for Li-Based Batteries.

High concentration electrolytes (HCEs) and localized high concentration electrolytes (LHCEs) have emerged as promising candidates to enable higher energy density Li-ion batteries due to their advantageous interfacial properties that result from their unique solvent structures. Using electrophoretic NMR and electrochemical techniques, we characterize and report full transport properties, including the lithium transference numbers (t+) for electrolytes ranging from the conventional ∼1 M to HCE regimes as well as for LHCE systems. We find that compared to conventional electrolytes, t+ increases for HCEs; however the addition of diluents to LHCEs significantly decreases t+. Viscosity effects alone cannot explain this behavior. Using Onsager transport coefficients calculated from our experiments, we demonstrate that there is more positively correlated cation-cation motion in HCEs as well as fast cation-anion ligand exchange consistent with a concerted ion-hopping mechanism. The addition of diluents to LHCEs results in more anticorrelated motion indicating a disruption of concerted cation-hopping leading to low t+ in LHCEs.