Lithium Cations Research Articles

Structure and Dynamics in Solid Electrolyte Composites of the Organic Ionic Plastic Crystal HMGFSI and Lithium Sulphonamide Functional Acrylate Polymer Nanoparticles.

Solid electrolyte composites between organic ionic plastic crystals (OIPCs) and polymers can potentially show enhanced mechanical properties and ion conduction. These properties can be determined by the formation of interfacial regions which affect the structure, thermal properties, and ion transport of the composite material. Here we studied the properties of composites between the OIPC hexamethylguanidinium bis(fluorosulfonyl)imide (HMGFSI) and acrylate polymer nanoparticles functionalised with lithium, using various techniques including solid-state NMR spectroscopy. An enhancement in ionic conductivity of three orders of magnitude as well as increased lithium and OIPC cation and anion dynamics were observed in the composite as prepared with 40 v% of polymer nanoparticles with respect to the pure OIPC at 50 °C. This was attributed to the increased overall structural disorder as a result of the formation of disordered interfacial regions, which were evidenced by solid-state NMR spectroscopy. In addition, the importance of the thermal history of these composites is highlighted, with differences in the conductivity and ion dynamics observed after melting and recrystallizing the OIPC component, leading to less disordered interfacial regions. This study enriches our fundamental understanding of the formation of interfacial regions in OIPC composites and their effect on the bulk properties of the electrolyte.

High Performance Perovskite Solar Cells Based on Multifunctional Additives of Crown‐Ether‐Iodine Supra‐Molecules

AbstractThe efficiency and stability of perovskite solar cells (PSCs) are influenced by various factors, such as controlling the migration of iodide anion (I−) and lithium cation (Li+), oxidizing the hole‐transport material of 2,2′,7,7′‐tetras(N,N‐p‐methoxyaniline)‐9,9′‐spirodifluorene (Spiro), and passivating the perovskite film. Herein, three multifunctional crown‐ether‐iodine (crown‐ether‐I2) supra‐molecules are investigated as activities in the hole transport layers (HTLs). Results indicate that the crown‐ether‐I2 can slowly release I2 to gently oxidize Spiro, and significantly improve the efficiency of PSCs. Moreover, the crown‐ether can contribute to stabilizing Li+ in HTL and passivating the defect sites on the upper interface of the perovskite layer, which can enhance the long‐term stability of PSCs. Furthermore, crown‐ether‐I2 can absorb I− to produce crown‐ether‐I3−, which can discharge I− to promote the self‐healing of I− defects and inhibit the migration of I− in the perovskite film, thereby further enhancing PSC's long‐term stability. PSC based on Dbenzo‐24‐Crown‐8‐Ether‐Iodine (DB24C8‐I2) achieves an impressive efficiency of 24.29%, which is much higher than that of the control device (22.28%). Additionally, the stability of the un‐encapsulated PSC with DB24C8‐I2 is significantly enhanced, while maintaining 96.9% of its original efficiency after 2000 h. This work provides an effective strategy for improving the efficiency and long‐term stability of PSCs.

Analysis of a constant-volume diafiltration system with the ability to remove lithium cations when using poly(2-acrylamido-2-methyl-1-propanesulfonic acid) in water

This study describes the synthesis of a poly(2-acrylamido-2-methyl-1-propanesulfonic acid) (PAMPS) and its application for the removal of Li+ in water using a constant-volume diafiltration system. PAMPS with molecular weights exceeding 100 kDa (88 % w/w), polymerisation yields of 97 % and high acidity was obtained. A block experimental design characterized the diafiltration system reporting: Regenerated cellulose (RC) and polyethersulfone (PES) ultrafiltration membranes with a molecular cut-off of 100 kDa can retain up to 1 % Li+ ions through surface charges. But when PAMPS 2000 kDa was used, 89 % of Li+ was removed (%R). Permeate flux (Js) decreases with increasing PAMPS:Li+ ratio, whereas the %R value increases. The filtration process is controlled by diffusion mechanisms according to the Peclet dimensionless number. Using PAMPS 100 kDa with a PAMPS:Li+ ratio (20:1), %R decreases to 76 %, whereas Js increases slightly. PAMPS can be reused 3 consecutive times, maintaining a Li+ cation rejection efficiency of >60 %. Additionally, it was found that the percentage of Li+ rejection capacity exercised with PAMPS is reduced to 60 % when Ca2+, K+, Mg2+ and Na+ cations are present.

FFF/FDM 3D-Printed Solid Polymer Electrolytes Based on Acrylonitrile Copolymers for Lithium-Ion Batteries.

Lithium-ion batteries (LIBs) are essential in modern electronics, particularly in portable devices and electric vehicles. However, the limited design flexibility of current battery shapes constrains the development of custom-sized power sources for advanced applications like wearable electronics and medical devices. Additive manufacturing (AM), specifically Fused Filament Fabrication (FFF), presents a promising solution by enabling the creation of batteries with customized shapes. This study explores the use of novel poly(acrylonitrile-co-polyethylene glycol methyl ether acrylate) (poly(AN-co-PEGMEA)) copolymers as solid polymer electrolytes for lithium-ion batteries, optimized for 3D printing using FFF. The copolymers were synthesized with varying AN:PEGMEA ratios, and their physical, thermal, and electrochemical properties were systematically characterized. The study found that a poly(AN-co-PEGMEA) 6:1 copolymer ratio offers an optimal balance between printability and ionic conductivity. The successful extrusion of filaments and subsequent 3D printing of complex shapes demonstrate the potential of these materials for next-generation battery designs. The addition of succinonitrile (SCN) as a plasticizer significantly improved ionic conductivity and lithium cation transference numbers, making these copolymers viable for practical applications. This work highlights the potential of combining polymer chemistry with additive manufacturing to provide new opportunities in lithium-ion battery design and function.

Abstraction of Trifluoroborane from Tetrafluoroborate: Li+‐Assisted Borylation of Nucleophilic Carbenes

AbstractThe small, lipophilic tetrafluoroborate anion is ubiquitous in the imidazol(in)ium and iminium precursors to N‐heterocyclic carbenes (NHCs), including cyclic (alkyl)(amino)carbenes (CAACs). Its symmetrical distribution of charge over four highly electronegative fluorine atoms confers high stability, attenuating basicity while shielding the boron center. Here we report that this inertness does not withstand the nucleophilicity of free carbenes, when combined with a polarizing lithium cation. Reaction of CAAC ⋅ HBF4 salts with LiN(SiMe3)2, a protocol widely used to liberate free CAACs, generates zwitterionic CAAC‐BF3 adducts within minutes at 80 °C, or hours at room temperature, even for bulky N‐diisopropylphenyl (DIPP) CAACs. Imidazol(in)ium tetrafluoroborates likewise form NHC‐BF3 adducts in excellent yields.

Structure and Physicochemical Properties of Solutions of Lithium Polysulfides in Tetrasolvate of Lithium Perchlorate with Sulfolane Molecular Dynamics Modeling.

Lithium polysulfides are intermediate products formed during the discharge and charge of lithium-sulfur batteries and have good solubility in electrolyte solutions. Therefore, the properties and structure of solutions of lithium polysulfides in electrolyte solutions affect the energy characteristics of the lithium-sulfur battery. In this work, the structure and physicochemical properties (density, ionic conductivity, and self-diffusion coefficients) of solutions of lithium disulfide, tetrasulfide, and octasulfide in lithium perchlorate tetrasolvate with sulfolane in a wide range of concentrations (0.2-12 M) were studied using the molecular dynamics method. With increasing concentrations of lithium polysulfides, the proportion of sulfur atoms in the coordination sphere of the lithium cation increases and the proportion of sulfolane molecules decreases. It has been established that the ability of the polysulfide anion to act as a bridging ligand leads to the formation of clusters, including lithium perchlorate, lithium polysulfides, and sulfolane. It has been shown that the tendency to form clusters increases with an increasing number of sulfur atoms in the polysulfide anion. At high concentrations of lithium polysulfides, regardless of their size, the electrolyte system becomes a single cluster. With an increase in the concentration of lithium polysulfides in the electrolyte system, its density increases and the ionic conductivity and diffusion coefficients of the system components decrease.

Innovative proposal for N2 capturing in Liquid Argon using the Li-FAU molecular Sieve

In this work, we unveil the potential of nitrogen (N2) adsorption from Liquid Argon (LAr) through the molecular sieves (zeolites) Li-FAU Adsorbents. We report detailed studies about N2 gas adsorption at T = 89 K using a commercial Micromeritics ASAP-2420 equipment and N2 purification from LAr using the Purification Cryostat (PuLArC) at IFGW/Unicamp. We argue that the N2 adsorption by the Li-FAU is possible thanks to the stronger interaction of N2 with the lithium cations present in zeolite Li-FAU. In fact, the experiments performed in PuLArC have unequivocally shown that the Li-FAU adsorbent was capable of capturing N2, reducing a N2 contamination of 20–50 ppm to 0.1–1.0 ppm in 1–2 hours of circulation time in LAr for several runs.This result demonstrated the great potential of the Li-FAU adsorbent for N2 capturing in LAr and invoke further tests of this material in larger scale LAr cryostats in order to confirm the innovative proposal of using the Li-FAU molecular sieve in replacement of Molecular Sieve 4A, currently used in LAr cryostats for neutrino experiments.

Utilization of Matrix Effect for Enhancing Resolution in Cation Exchange Chromatography.

In ion chromatography studies, the matrix effect of other inorganic ions present in the sample is a well-known phenomenon. In this work, the behavior of inorganic and organic ions was studied in a system overloaded with ammonium ions. The ammonium ions came from a solution of ammonium hydroxide in various concentrations (0.25-1.25%). In this system, which was significantly overloaded with ammonium ions, the behavior of three ions were tested (lithium, tris, and sodium cations). The measurements were performed at different eluent concentrations (6-17 mM), chromatographic column temperatures (25-40 °C), and injected volumes (15-40 µL). The retention times of sodium and lithium ions increased with increasing amounts of injected ammonium, while tris remained essentially unchanged, indicating that the resolution of these ions can be influenced by varying the concentration of the matrix. The results suggested that the observed effect was due to a combination of the pH change caused by the injected matrix, the dissociation of tris ions, the dissociation of the carbocylic ion-exchange groups of stationary phase, the change in buffer capacity, and the amount of ammonium ion introduced. It has been shown that in a well-designed experiment, the addition of ammonium hydroxide to the sample at concentrations greater than 1% can improve the efficiency of organic and inorganic cation separation. It was found that 8 mM methanesulfonic acid eluent, 30 °C, 1% ammonium hydroxide matrix concentration, and 25 µL injection were optimal for the baseline separation of tris and sodium ions on the high-capacity Dionex CS16 column. These ions could not be separated on this column without the presence of the ammonium matrix.

Controlled Migration of Lithium Cations by Diamine Bridges in Water-Processable Polymer-Based Solid-State Electrolyte Memory Layers for Organic Synaptic Transistors.

Synaptic transistors require sufficient retention (memory) performances of current signals to exactly mimic biological synapses. Ion migration has been proposed to achieve high retention characteristics but less attention has been paid to polymer-based solid-state electrolytes (SSEs) for organic synaptic transistors (OSTRs). Here, OSTRs with water-processable polymer-based SSEs, featuring ion migration-controllable molecular bridges, which are prepared by reactions of poly(4-styrenesulfonic acid) (PSSA), diethylenetriamine (DETA), and lithium hydroxide (LiOH) are demonstrated. The ion conductivity of PSSA:LiOH:DETA (1:0.4:X, PLiD) films is remarkably changed by the molar ratio (X) of DETA, which is attributed to the extended distances between the PSSA chains by the DETA bridges. The devices with the PLiD layers deliver noticeably changed hysteresis reaching an optimum at X = 0.2, leading to the longest retention of current signals upon single/double pulses. The long-term potentiation test confirms that the present OSTRs can gradually build up the postsynaptic current by gate pulses of -2V, while the long-term depression can be adjusted by varying the depression gate pulses (≈0.2-1.2V). The artificial neural network simulations disclose that the present OSTRs with the ion migration-controlled PLiD layers can perform synaptic processes with an accuracy of ≈96%.

Structure of vanadia-titania catalysts doped with alkali metals according to solid-state NMR, ESR spectroscopies and DFT

In this work, V/M/TiO2 catalysts (M = Li, Na, K, Rb and Cs) were investigated with Solid-state nuclear magnetic resonance (SSNMR), electron paramagnetic resonance (ESR) and first-principles calculations. The total vanadium content corresponds to half monolayer (4 V atoms·nm−2 of TiO2 support surface), with V/M atomic ratio being 4/0.6. Static 51V and MAS 1H, 7Li, 51V, 23Na, 133Cs NMR spectra were acquired. Surface moieties of vanadium oxide on (001) anatase surface were modeled using density functional theory (DFT); their 51V NMR parameters were calculated with the Gauge-Including Projected Augmented Wave (GIPAW) method and compared to experimental data obtained with 51V SSNMR spectroscopy. It was found that mainly strongly bound vanadium sites (V3) are formed on anatase samples, located on TiO2 terminal oxygen atoms. Weakly bound vanadium sites (V1, V2) are formed on bridged anatase oxygen atoms. Supported alkali metals (Li, Na, K, Rb and Cs) on TiO2 were found to interact with protons located on the terminal and bridged TiO2 oxygen atoms. The relative ratio of weakly bound vanadium sites (V1, V2) increased on alkali-containing samples. Calculations performed showed lithium cation to prefer V-O-Ti or V-O-V bonds over VO, unsystematically deshielding vanadium nuclei. The presence of V3+ is likely to cause a loss of intensity in 51V NMR spectra.

In Situ Hydrophobization of Lithium Aluminate Particles for Flotations by Dry Grinding in the Presence of Punicines

The engineered artificial mineral (EnAM) lithium aluminate (LiAlO2) is a promising candidate for the recycling of lithium from slags, which can originate from the reprocessing of batteries, for example. Derivatives of the natural product Punicine (1-(2′,5′-dihydroxyphenyl)-pyridinium) from Punica granatum have been proven to be effective switchable collectors for the flotation of this mineral as they react to light. In the present study, three Punicines were added to a planetary ball mill before grinding LiAlO2 to particle sizes suitable for flotation. We investigated the influence of Punicine and two derivatives with C10 and C17 side chains on the grinding results at different grinding times and conditions as well as on the yields in flotations. SEM images of the particles, IR and ICP–OES measurements provided insights into the Punicine–particle interactions. They showed that Punicines not only prevent the formation of hydrophilic and thus undesirable lithium aluminate hydroxide hydrate (LiAl2(OH)7 ▪ x H2O) surfaces in this process, as is unavoidable in aqueous flotation without this pretreatment, they also prevent the undesired release of lithium cations into the aqueous phase. Due to considerable hydrophobization of the particle surface of LiAlO2, nearly quantitative recovery rates of this engineered artificial mineral are achieved using the process described here.

Tuning Ion Mobility in Lithium Argyrodite Solid Electrolytes via Entropy Engineering.

The development of improved solid electrolytes (SEs) plays a crucial role in the advancement of bulk-type solid-state battery (SSB) technologies. In recent years, multicomponent or high-entropy SEs are gaining increased attention for their advantageous charge-transport and (electro)chemical properties. However, a comprehensive understanding of how configurational entropy affects ionic conductivity is largely lacking. Herein we investigate a series of multication-substituted lithium argyrodites with the general formula Li6+x[M1aM2bM3cM4d]S5I, with M being P, Si, Ge, and Sb. Structure-property relationships related to ion mobility are probed using a combination of diffraction techniques, solid-state nuclear magnetic resonance spectroscopy, and charge-transport measurements. We present, to the best of our knowledge, the first experimental evidence of a direct correlation between occupational disorder in the cationic host lattice and lithium transport. By controlling the configurational entropy through compositional design, high bulk ionic conductivities up to 18 mS cm-1 at room temperature are achieved for optimized lithium argyrodites. Our results indicate the possibility of improving ionic conductivity in ceramic ion conductors via entropy engineering, overcoming compositional limitations for the design of advanced electrolytes and opening up new avenues in the field.

الدراسة التركيبية والطاقية لأيونات الليثيوم مع الأحماض الدهنية ميثيل استر [[FAME (9Z-18:1) + Li+ باستخدام الطريقة الكيميائية الكمومية (PM3)

Lithium (Li) ions are being used in a variety of fields ranging from energy storage to the treatment of mental illnesses including bipolar disorder and schizophrenia. Lithium caton (Li+) is able to form cationic adducts with various compounds and they can stabilize the biomacromolecules that interact with. Here, the interaction of lithium ions with fatty acid methyl ester [FAME (9Z-18:1)] has been theoretically investigated to gain insight into the structure and energetics of [FAME (9Z-18:1) + Li+]. All theoretical calculations were performed using Gaussian09 software via a graphic user interface. Geometry optimisations with harmonic vibrational analysis of conformations for chelated and extended forms of [FAME (9Z-18:1) + Li+] were carried out using semi-empirical method PM3. To obtain accurate energetic, zero-point energy (ZPE) corrections were included in all optimized energies and relative energies between conformers. The calculations indicated that the chelated form is relatively more stable than extended forms by 25 and 118 kJmol-1 when lithium is bound to the carbonyl oxygen (O-Li+) or olefin (C=C-Li+), respectively. The comparison between the relative stabilization energies of extended (O-Li+) versus extended (C=C-Li+) reveals that the lithium cation energetically prefers to bind to with carbonyl oxygen over the carbon-carbon double bond. Keywords: lithium ions, geometry optimization, sim-empirical method, Gaussian 09.

Selective Extraction of Lithium Cations from Mixture of Alkali Metal Chlorides Using Electrobaromembrane Process

Selective Extraction of Lithium Cations from Mixture of Alkali Metal Chlorides Using Electrobaromembrane Process

A new concept of ternary aqueous electrolytes based on lithium 4,5-dicyanoimidazolate hydrates

A new concept of aqueous electrolytes based on heterocyclic anions (hydrated anionic triplet electrolyte, HATE) has been presented. Structural studies showed that dimeric lithium 4,5-dicyanoimidazolate (LiTDI) dihydrate molecules, in the presence of acetonitrile, form an ionic system preserved in high concentrations and solid states. X-ray diffraction measurements show that electroneutral dihydrate units can coordinate additional lithium cations acting as charge carriers. The crystalline ionic phase was characterized using spectroscopic, thermal, and electrochemical methods and was used to prepare model electrolytes based on LiTDI hydrates. Linear sweep voltammetry and impedance spectroscopy measurements show, in this system, the depletion of water activity, high conductivity, and reversible cycling of full cells comprising examined electrolytes. We will prove that a concentrated triplet solution acts similarly to the anhydrous electrolyte; regardless of the concentration, it reaches high ionic conductivity values (12–16 mS/cm at room temperature) and is electrochemically stable.

Iodine-doped carbon nanotubes boosting the adsorption effect and conversion kinetics of lithium-sulfur batteries

Compared with lithium-ion batteries (LIBs), lithium-sulfur batteries (LSBs), based on electrochemical reactions involving multi-step 16-electron transformations provide higher specific capacity (1672 mAh g−1) and specific energy (2600 Wh kg−1), exhibiting great potential in the field of energy storage. However, the inherent insulation of sulfur, slow electrochemical reaction kinetics and detrimental shuttle-effect of lithium polysulfides (LiPSs) restrict the development of LSBs in practical applications. Herein, the iodine-doped carbon nanotubes (I-CNTs) is firstly reported as sulfur host material to the enhance the adsorption-conversion kinetics of LSBs. Iodine doping can significantly improve the polarity of I-CNTs. Iodine atoms with lone pair electrons (Lewis base) in iodine-doped CNTs can interact with lithium cations (Lewis acidic) in LiPSs, thereby anchoring polysulfides and suppressing subsequent shuttling behavior. Moreover, the charge transfer between iodine species (electron acceptor) and CNTs (electron donor) decreases the gap band and subsequently improves the conductivity of I-CNTs. The enhanced adsorption effect and conductivity are beneficial for accelerating reaction kinetics and enhancing electrocatalytic activity. The in-situ Raman spectroscopy, quasi in-situ electrochemical impedance spectroscopy (EIS) and Li2S potentiostatic deposition current–time (i-t) curves were conducted to verify mechanism of complex sulfur reduction reaction (SRR). Owing to above advantages, the I-CNTs@S composite cathode exhibits an ultrahigh initial capacity of 1326 mAh g−1 as well as outstanding cyclicability and rate performance. Our research results provide inspirations for the design of multifunctional host material for sulfur/carbon composite cathodes in LSBs.

Selective Solid-Liquid Extraction of Lithium Cation Using Tripodal Sulfate-Binding Receptors Driven by Electrostatic Interactions.

Owing to the important role of and increasing demand for lithium resources, lithium extraction is crucial. The use of molecular extractants is a promising strategy for selective lithium recovery, in which the interaction between lithium and the designed extractant can be manipulated at the molecular level. Herein, we demonstrate that anion receptors of tripodal hexaureas can selectively extract Li2SO4 solids into water containing DMSO (0.8% water) compared to other alkali metal sulfates. The hexaurea receptor with terminal hexyl chains displays the best Li+ extraction selectivity at 2-fold over Na+ and 12.5-fold over K+. The driving force underpinning selective lithium extraction is due to the combined interactions of Li+-SO42- electrostatics and the ion-dipole interaction of the lithium-receptor (carbonyl groups and N atoms); the latter was found to be cation size dependent, as supported by computational calculations. This work indicates that anion binding receptors could drive selective cation extraction, thus providing new insights into the design of receptors for ion recognition and separation.

A Comparative Study on Electrochemical Performance of Single versus Dual Networks in Lithium Metal/Polysulfide-Polyoxide Co-Network/Lithium Titanium Oxide Cathode

The present article introduces a strategy for controlling oxidation and reduction reactions within polymer electrolyte membrane (PEM) networks as a means of enhancing storage capacity through the complexation of dissociated lithium cations with multifunctional groups of the polymer network. Specifically, co-polymer networks based on polysulfide (PS) and polyoxide (PO) precursors, photo-cured in the presence of succinonitrile (SCN) and lithium bis(trifluoro methane sulfonyl imide) (LiTFSI) salt, exhibited ionic conductivity on the order of mid 10−4 S/cm at ambient temperature in the 30/35/35 (weight %) composition. Lithium titanate (LTO, Li4Ti5O12) electrode was chosen as an anode (i.e., a potential source of Li ions) against lithium iron phosphate (LFP, LiFePO4) cathode in conjunction with polysulfide-co-polyoxide dual polyelectrolyte networks to control viscosity for 3D printability on conformal surfaces of drone and aeronautic vehicles. It was found that the PS-co-PO dual network-based polymer electrolyte containing SCN plasticizer and LiTFSI salt exhibited extra storage capacity (i.e., specific capacity of 44 mAh/g) with the overall specific capacity of 170 mAh/g (i.e., for the combined LTO electrode and PEM) initially that stabilized at 153 mAh/g after 50th cycles with a reasonable capacity retention of over 90% and Coulombic efficiency of over 99%. Of particular interest is the observation of the improved electrochemical performance of the polysulfide-co-polyoxide electrolyte dual-network relative to that of the polyoxide electrolyte single-network.

Anionic Effects on Concentrated Aqueous Lithium Ion Dynamics.

The dynamics, orientational anisotropy, diffusivity, viscosity, and density were measured for concentrated lithium salt solutions, including lithium chloride (LiCl), lithium bromide (LiBr), lithium nitrite (LiNO2), and lithium nitrate (LiNO3), with methyl thiocyanate as an infrared vibrational probe molecule, using two-dimensional infrared spectroscopy (2D IR), nuclear magnetic resonance (NMR) spectroscopy, and viscometry. The 2D IR, NMR, and viscosity results show that LiNO2 exhibits longer correlation times, lower diffusivity, and nearly 4 times greater viscosity compared to those of the other lithium salt solutions of the same concentration, suggesting that nitrite anions may strongly facilitate structure formation via strengthening water-ion network interactions, directly impacting bulk solution properties at sufficiently high concentrations. Additionally, the LiNO2 and LiNO3 solutions show significantly weakened chemical interactions between the lithium cations and the methyl thiocyanate when compared with those of the lithium halide salts.

Ternary Solid Polymer Electrolytes at the Electrochemical Interface: A Computational Study.

Polymer-based solid-like gel electrolytes have emerged as a promising alternative to improve battery performance. However, there is a scarcity of studies on the behavior of these media at the electrochemical interface. In this work, we report classical MD simulations of ternary polymer electrolytes composed of poly(ethylene oxide), a lithium salt [lithium bis(trifluoromethanesulfonyl)imide], and different ionic liquids [1-butyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide and 1-ethyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide] confined between two charged and uncharged graphene-like surfaces. The molecular solvation of Li+ ions and their diffusion as well as the polymer conformational picture were characterized in terms of the radial distribution functions, coordination numbers, number density profiles, orientations, displacement variance, polymer radius of gyration, and polymer end-to-end distance. Our results show that the layering behavior of the ternary electrolyte in the interfacial region leads to a decrease of Li+ mobility in the direction perpendicular to the electrodes and high energy barriers that hinder lithium cations from coming into direct contact with the graphene-like surface. The nature of the ionic liquid and its concentration were found to influence the structural and dynamic properties at the electrode/electrolyte interface, the electrolyte with low amounts of the pyrrolidinium-based ionic liquid being that with the best performance since it favors the migration of Li+ cations toward the negative electrode when compared to the imidazolium-based one.