Commercial Liquid Electrolyte Research Articles

Enhanced electrochemical performance of garnet Li7La3Zr2O12 electrolyte by efficient incorporation of LiCl

Garnet-type Ta-doped Li7La3Zr2O12 (LLZO) lithium-ion-conducting ceramic electrolytes has become the promising and critical candidate for developing the high-energy-density all-solid-state lithium batteries, due to the satisfied Li+ conductivity, stability against metallic lithium anode, and the feasible preparation under ambient air. Here, to further increase the lithium-ion conductivity of LLZO comparable to that of the commercial organic liquid electrolytes, lithium chloride (LiCl) is effectively introduced to synthesize the garnet-type ceramic electrolytes with the nominal composition (Li6.5La3Zr1.5Ta0.5O12)1-x–(LiCl)x (x = 0, 5mol%, 10mol%, 15mol%, 20mol%, and 25mol%) via high-temperature calcination process. The cubic structure with highly conductive performance is confirmed from X-ray diffraction measurement as well as Raman spectra analysis. Structural information is observed according to field emission scanning electron microscope equipped with energy dispersive spectrometer and density measurements. Among above investigated ceramic compositions, the prepared (Li6.5La3Zr1.5Ta0.5O12)0.85–(LiCl)0.15 ceramic electrolyte sheet sintered at 1200 °C for 12h presents the room-temperature Li-ion conductivity of 1.22 × 10−3 S·cm−1 by alternating current (AC) impedance analysis along with the corresponding activation energy of 0.262eV through Arrhenius equation calculation. The electronic conductivity measurements are also done by direct-current polarization to confirm the ionic nature for all investigated ceramics. Furthermore, the Li|(Li6.5La3Zr1.5Ta0.5O12)0.85–(LiCl)0.15 |Li symmetric batteries can possess the small interfacial resistance of 92.3 Ω cm2 and stably run for 1000 h at 0.1 mA cm−2 without a short circuit at room temperature. The hybridized lithium-sulfur battery with (Li6.5La3Zr1.5Ta0.5O12)0.85–(LiCl)0.15 electrolyte delivered excellent initial room-temperature discharge capacity of 1204mAh·g−1 and 1152 mAh·g−1 under the current density of 0.1C and 0.2C respectively, large coulombic efficiency, and great cycling stability. Moreover, the lithium-sulfur batteries also can show excellent cycling performances under different current densities and a good capacity recoverability. The above investigation results suggest that the low-melting-point LiCl incorporation in Li6.5La3Zr1.5Ta0.5O12 electrolyte is an effective measurement to synthesize the cubic and dense Li-stuff garnet ceramic sheets for the high-performance rechargeable next-generation solid-state batteries.

GEL POLYMER ELECTROLYTES ELABORATED BY UV-IRRADIATION FOR THE ECO-DESIGN OF LI-ION BATTERIES

This study examines the chemical, thermal, and dielectric properties of gel polymer electrolytes (GPEs) based on poly(ethylene glycol) diacrylate (PEGDA, average Mn=700 g/mol). GPEs were synthesized via a single-step UV-irradiation process, whereby PEGDA was mixed with varying concentrations of a commercial liquid electrolyte (1 M LiPF6 in EC/DEC 50/50 v/v) ranging from 0 to 60 wt%. The results of the infrared analysis indicated that the liquid electrolyte was successfully immobilized within the polymeric matrix. The thermally stable nature of the synthesized GPEs was confirmed across a wide temperature range (-40 to 90°C) through thermal analysis. Furthermore, dielectric measurements were conducted in a frequency range of 0.1 to 106 Hz, with a sinusoidal AC amplitude of 10 mV, from 20 to 100°C. The results demonstrated that the ionic conductivity of GPEs increased with the addition of liquid electrolyte. The GPEs prepared with 60 wt% liquid electrolyte exhibited a conductivity value of approximately 6.6x10-3 S/m at 30°C, which is consistent with the conductivity range reported in the literature.

Flame-retardant in-situ formed gel polymer electrolyte with different valance states of phosphorus structures for high-performance and fire-safety lithium-ion batteries

Lithium-ion batteries (LIBs) have been widely used today owing to portability, high energy storage, and reusability. However, commercial liquid electrolytes in LIBs possess intensive mobility and terrible flammability. Accordingly, leakage, combusting, and even exploding can frequently occur when LIBs work under abuse conditions. Herein, a novel flame-retardant gel polymer electrolyte (GPE) containing + 3 and + 5 phosphorus valence states of phosphorus structures was designed by in-situ thermal polymerization of tri(acryloyloxyethyl) phosphate (TAEP), diethyl vinylphosphonate (DEVP), and pentaerythritol tetraacrylate in electrolytes. After being ignited by fire, this GPE extinguished quickly with a combusting time of only 0.9 s, showing much lower flammability. Besides, the GPE is compatible with graphite anode, LiFePO4 (LFP), and even LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes. The as-assembled LFP and NCM811-based pouch cells (1 Ah-type) with TD-GPE achieved stable cycling, maintaining 88.52 % and 95.2 % of the initial capacities, respectively after 200 and 190 cycles at 0.5C. Moreover, the as-prepared TD-GPE dramatically reduced the fire hazard of NCM811 batteries without sacrificing the electrochemical performance. The thermal abuse test demonstrates that the leakage and combustion of NCM811||TD-GPE||Graphite pouch cell could be significantly suppressed in the test process, indicating that battery safety improves significantly via the combined use of different phosphorus valence structures. This is because the + 5 phosphorus valence of TAEP promoted the formation of carbon layers, and the + 3 phosphorus structure in DEVP captured free radicals by quenching effect. This work paves a different path for designing safe and high-performance GPEs in LIBs based on gaseous-phase and condensed-phase mechanisms.

In-situ electrochemical passivation for constructing high-voltage PEO-based solid-state lithium battery

Polyethylene oxide (PEO) is one of the promising substrates for polymer solid electrolyte. However, when coupled with high energy density nickel-rich layered cathode materials, PEO faces the risk of catalytic decomposition by delithium nickel-rich materials. In this work, the in-situ electrochemical passivation strategy is employed to obtain high voltage PEO-based solid-state lithium battery. Trace commercial liquid electrolyte was added on the surface of LiNi0.8Co0.1Mn0.1O2 (NCM811) electrode, and liquid electrolyte is prior to PEO electrolyte to react with the cathode during charge/discharge process, leading to the formation of cathode-electrolyte interface (CEI) layer. The CEI layer avoids the direct contact between PEO and NCM811, thus effectively prevents PEO from being decomposed by NCM811 under high voltage. As a result, the optimized NCM811||PEO||Li battery displays enhanced electrochemical performance, especially cycling performance. This simple but effective strategy not only simplifies the manufacturing process, but also has instructional guidance for high-voltage PEO-based battery.

A Perspective on the Requirements of Ni‐rich Cathode Surface Modifications for Application in Lithium‐ion Batteries and All‐Solid‐State Lithium‐ion Batteries

AbstractThe increasing adoption of Ni‐rich cathode active materials in commercial liquid electrolyte Lithium‐ion batteries (LIBs) is testament to the improvements in the cathode stability through various surface modification strategies. The development of a deeper understanding of the cathode/electrolyte interface in LIBs has resulted in coatings capable of mitigating both surface and bulk cathode degradation mechanisms. However, due to increasing demands for safe and high energy density cells, a large portion of the research has now shifted towards applying Ni‐rich cathode active materials in inherently safer all‐solid‐state Lithium‐ion batteries (ASSLBs), with the resulting cathode surface modification strategies evolving differently. In this regard, a review outlining the surface modification strategies of Ni‐rich cathode materials applied in both LIB and ASSLB systems is provided. Within, a review of the traditional, advanced and specialized surface modification strategies of each system is discussed, along with a final perspective on the likely future direction of research regarding the design of system‐specific Ni‐rich cathode‐based surface modification strategies.

Practical relevance of charge transfer resistance at the Li metal electrode|electrolyte interface in batteries?

AbstractThe theoretically possible energy and power densities of rechargeable batteries are practically limited by resistances as these lead to overvoltages, particularly pronounced at kinetically harsher conditions, i.e., high currents and/or low temperature. Charge transfer resistance (Rct), being a major type of resistance alongside with Ohmic (RΩ) and mass transport (Rmt), is related with the activation hindrance of electrochemical reactions. Its practical relevance is discussed within this work via analyzing $$\mathrm{Li}\mid \,\, \mid\mathrm{Li}$$ Li ∣ ∣ Li cells with the galvanostatic/constant current (CC) technique. Rct at Li|electrolyte interfaces is shown to be relevantly impacted by electrode–electrolyte interphases; implying the electrolyte type, as well. While solid polymer electrolytes (SPEs), e.g., based on poly(ethylene) oxide (PEO), show negligible Rct, it is evident for commercial liquid electrolytes and readily increase during storage. Given the asymptotic overvoltage vs. current behavior of Rct, obeying Butler-Volmer equation, Rct gets less relevant at enhanced currents, as experimentally validated, finally pointing to the dominance of RΩ and (depending on system) Rmt in the overall resistance. Graphical Abstract

Interconnected Three-Dimensional Porous Alginate-Based Gel Electrolytes for Lithium Metal Batteries.

Lithium batteries have been widely used in our daily lives for their high energy density and long-term stability. However, their safety problems are of paramount concern for consumers, which restricts their scale applications. Gel polymer electrolytes (GPEs) compensate for the defects of liquid leakage and lower ionic conductivity of solid electrolytes, which have attracted a lot of attention. Herein, a 3D interconnected highly porous structural gel electrolyte was prepared with alginate dressing as a host material, poly(ethylene oxide) (PEO), and a commercial liquid electrolyte. With rich polar functional groups and (CH2-CH2-O) segments on the polymer matrix, the transportation of Li+ is faster and uniform; thus, the formations of lithium dendrite were significantly inhibited. The cycle stability of symmetrical Li||Li batteries with modified composite electrolytes (SAA) is greatly improved, and the overpotential remains stable after more than 1000 h. Meanwhile, under the same conditions, the cycle performance of batteries with unmodified electrolytes is inferior and overpotentials are nearly 1 V after 100 h. Additionally, the capacity retention of Li||LiFePO4 with SAA is more than 95% after 200 cycles, while those of the others declined sharply. The alginate dressing-based GPEs can greatly enhance the mechanical and thermal stability of PEO-based GPEs, which provides an environmentally friendly avenue for gel electrolytes' applications in lithium batteries.

Projection Micro Stereolithography of Skin Layered Microporous Polymer Membranes As a Separator for Li-Ion Batteries

Commercial liquid electrolyte lithium-ion batteries (LIBs) traditionally incorporate microporous polymer membranes, or separators, to isolate electrode contact and enable ionic transport. Although they do not actively participate in cell chemistry, well-designed separators can influence cell performance and safety, and thus, are essential components of a cell. Current separator manufacturing processes include "wet" or "dry" mechanical stretching , phase inversion, and evaporation-induced phase separation. However, these processes have limited morphological control of geometry and layered structures. Additive manufacturing techniques have been used to rapidly prototype materials that have both high customizability and fine microstructural control. We investigate hexanediol diacrylate (HDDA) as a polymer system using projection micro-stereolithography, a layer-by-layer photopolymerization technique, to develop separators with controlled microstructures for Li-ion batteries. We successfully fabricate a unique polymer architecture of alternating nanometer thin skin layers and microporous network. The fine control of printing parameters (i.e., printing platform, skin layers, and exposure time), results in tunable porosity and morphology. This unique approach to manufacturing LIB separators provides hierarchical homogeneity for more uniform Li-ion transport. It’s potential as a LIB separator is explored by characterizing its electrolyte wettability, thermal tolerance, electrochemical properties, and mechanical stability. Finally, lithium symmetric cells using the HDDA microporous membranes are evaluated against Celgard 2325 separators. This work provides a promising new route for developing separators using additive manufacturing techniques to enable high performance Li-ion batteries.

An ultra-thin composite electrolyte with vertical aligned Li ion transport pathways for all-solid-state lithium metal battery

All-solid-state lithium metal batteries employing composite electrolytes can fundamentally settle the safety issues of commercial liquid electrolytes. However, the thick thickness and low ionic conductivity as well as unregulated ion transport of current composite electrolytes pose great obstacles in further promoting their applicability and compatibility with Li metal anode. Herein, an ultra-thin composite electrolyte with vertical aligned Li ion transport pathways is rationally designed via filling polyethylene glycol-perfluoropolyether polymer electrolyte into the nanochannels of an alumina template via vacuum infusion and in-situ polymerization. The strong Lewis acid-base effect that existed between ions and composite electrolytes can construct numerous fast channels for Li+ transport. A restrained vertical direction of ion immigration can facilitate the uniform deposition of Li+ on metallic Li anode. The shortened Li ion conductive distance and superior electrolyte/electrode interfaces contribute to the improved electrochemical performance of the assembled solid-state batteries. An ionic conductivity of 1.21 × 10−4 S cm−1 and a transference number of 0.37 at room temperature are achieved for the designed composite electrolytes, which is superior to those of the conventional composite electrolytes reinforced with Al2O3 or garnet nanoparticles. The corresponding Li symmetrical cell can stably work for over 1200 h without short-circuit and the LiFePO4 || Li full cell exhibits a high initial discharge capacity of 164.8 mAh g−1 with capacity retention of 93.7 % after 100 cycles with a coulombic efficiency close to 100 %. This work offers an effective tactic to develop ultra-thin composite electrolytes for high-performance all-solid-state lithium metal batteries.

Effect Of Graphene Oxide on Poly (Methyl Methacrylate)-Grafted Natural Rubber Polymer Electrolytes

Polymer electrolytes (PE) are presently the subject of the majority of research due to their capacity to replace liquid electrolyte that suffer from high flammability and electrolyte leakage and also as a new forms of electrical power production and storage systems. Solid polymer electrolytes (SPE) typically have low ionic conductivity at room temperature because of the high crystallinity of the polymers. Methyl-grafted natural rubber has been studied extensively by a number of researchers due to its advantageous properties such as high flexibility, and ability to solvate inorganic salts to form a polymer-salt complex. Graphene oxide (GO) was used as a nanofiller, ammonium triflate (NH4CF3SO3) served as a dopant salt, and 30 % polymethyl methacrylate grafted natural rubber (MG30) served as the polymer host in the preparation of the nanocomposite polymer electrolyte (CPE) using the solution casting-method. Electrochemical impedance spectroscopy (EIS) was used to analyse the ionic conductivity of the samples, and Fourier-transform infrared spectroscopy (FTIR) was used to analyse the complexation between salt, polymer host and filler while Optical microscope was used to study the surface morphology of the prepared CPE samples. The decrease in peak strength for C=O in the FTIR spectra indicates the interaction between the polymer host and salt The sample containing 15 weight percent NH4CF3SO3 had the highest conductivity, which was 2.05×10-5 S cm-1. This substance has the potential to be used in energy storage devices like batteries and supercapacitors as an alternative to commercial liquid electrolyte.

Suppressing Dendrite Growth with Eco-Friendly Sodium Lignosulfonate Additive in Quasi-Solid-State Li Metal Battery.

The application of lithium metal batteries is limited by the drawbacks of safety problems and Li dendrite formation. Quasi-solid-state electrolytes (QSSEs) are the most promising alternatives to commercial liquid electrolytes due to their high safety and great compatibility with electrodes. However, Li dendrite formation and the slow Li+ diffusion in QSSEs severely hinder uniform Li deposition, thus leading to Li dendrite growth and short circuits. Herein, an eco-friendly and low-cost sodium lignosulfonate (LSS)-assisted PVDF-based QSSE is proposed to induce uniform Li deposition and inhibit Li dendrite growth. Li symmetric cells with 5%-LSS QSSE possess a high Li+ transfer number of 0.79, and they exhibit a long cycle life of 1000 h at a current density/areal capacity of 1 mA cm-2/5 mAh cm-2. Moreover, due to the fast electrochemical dynamics endowed by the improved compatibility of the electrodes and fast Li+ diffusion, the LFP/5%-LSS/Li full cells still maintain a high capacity of 110 mAh g-1 after 250 cycles at 6C. This work provides a novel and promising choice that uses eco-friendly LSS as an additive to PVDF-based QSSE in Li metal batteries.

In situ generated of hybrid interface in poly(1,3-dioxolane) quasi solid electrolyte and extended sulfone cosolvent for lithium-metal batteries

The practical application of lithium metal batteries with high energy density are difficult to apply due to the problem of uncontrolled lithium dendrite growth with commercial liquid electrolytes. Herein, we designed a poly 1,3-dioxolane (PDOL) based quasi solid polymer electrolyte with in-situ polymerization. A small amount of lithium difluoro(oxalato)borate (LiDFOB) provides cationic initiation center for the polymerization of dioxolane (DOL). Sulfolane (SL) were further introduced into the system as a cosolvent and the ionic conductivity was increased to 3.22 × 10-4 S cm-1followed with a high Li+ transfer number of 0.73 at room temperature. Trace amount of SbF3 was introduced to form a robustness inorganic-rich hybrid interface that reduces the decomposition of electrolyte components and retards the formation of lithium dendrites during cycling. The superior rate performance and stable 5C long cycle performance are obtained in LiFePO4||Li full cell owing to the interaction between Li+, SL and PDOL. This work expands the choice of components in quasi solid electrolytes to manufacture qualified LMBs with enhanced performance.

Method for Benchmarking Li Metal Anodes: A Mandatory Step toward Reliable Lithium Metal Batteries

All-solid-state batteries are known to be the new energy storage holy grail that will lead to safer batteries with higher energy density than current Li-ion batteries. The use of a solid electrolyte enables the use of lithium metal as the anode material. However, its composition, its thickness, and the quality/nature of its passivation layer can strongly affect the performance of the battery. For this reason, we propose a simple benchmarking method that evaluates and compares the quality and electrochemical performance of various Li anodes. This method can be easily reproduced, especially concerning the electrochemical evaluation that uses a commercial liquid electrolyte and the widely spread coin-cell format. In total, ~285 coin cells were assembled to benchmark our in-house lithium metal foil (Lithium HQ) with two commercial ones and the results showed the superior performance of our Li metal anode. The performance of the cells seems closely related to the quality and uniformity of the Li surface. In addition, we propose including in the benchmarking method the effect of Li aging in a dry room on the electrochemical performance. This effect is important to consider because the fabrication of all-solid-state batteries is conducted in such an environment.

Scalable wet-slurry fabrication of sheet-type electrodes for sulfide all-solid-state batteries and performance enhancement via optimization of Ni-rich cathode coating layer

All-solid-state Li or Li-ion batteries (ASSLBs) have attracted much attention due to their potential high energy density, high safety, and low manufacturing costs compared to commercial liquid electrolyte Li-ion batteries. However, the rate capacity and cycling performance could not satisfy the practical application. Here, an island-like amorphous Li2O–ZrO2 (LZO) was coated on the surface of LiNi0.88Co0.10Al0.02 (NCA) via a sol-gel method and low-temperature sintering. The electrochemical performance and density functional theory calculation results demonstrate that the LZO coating layer significantly boosts Li-ions transfer. Targeting large-scale production, a sheet-type cathode was prepared by a wet-slurry process with PVDF-HFP as a binder, which exhibits an initial specific capacity of 181.91 mAh·g−1 at 0.13C and 25 °C. Remarkably, the wet-slurry cathode with a high NCA loading of 20 mg cm−2 delivers an initial areal capacity of 2.936 mAh·cm−2 and capacity retention of 69.93% after 1000 cycles at a rate of 0.64C. By employing X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electron microscopy, we reveal that the LZO coating layer and PVDF-HFP binder inhibited the decomposition of sulfide electrolyte and detrimental structure evolution of NCA active material. This work would guide designing high-performance ASSLBs for practical application and commercialization.

Tailoring the Electrochemical Performance of Olivine Phosphate Cathode Materials for Li-Ion Batteries by Strain Engineering: Computational Experiments

The open-circuit voltage (OCV), Li-ion diffusion, and electronic properties of a cathode material can significantly affect the performance of lithium-ion batteries (LIBs). In this work, DFT + U was carried out to investigate the effect of strain engineering in terms of biaxial compressive and tensile strains (BCS and BTS) on the electrochemical properties of olivine-based LiMPO4 (M = Co and Ni). The results show that biaxial compressive strain decreased the average bond lengths of O–Co/Ni and O–P, which means a good improvement in the structural stability of LiCoPO4 (LCP) and LiNiPO4 (LNP). The deployment of BCS and BTS reduced the open-circuit voltage of the LCP and LNP systems. Precisely, imposing a biaxial strain of about ε = ±3.5% for LCP and ε = ±5.5% for LNP reduced the high OCV to values below 4.5 V vs Li/Li+, which is recommended for most commercial liquid electrolyte operation. In addition, it was found that biaxial strain reduces the energy barrier for Li+ diffusion, which promotes Li+ diffusion and increases its mobility in these olivine crystal structures. Further analysis of the electronic structures shows that BTS reduces the material’s band gap and improves electronic conductivity. These results are promising for the commercial utilization of LCP and LNP as potential cathode material in next-generation LIBs like their famous big brother LFP.

Probing Sodium Storage Mechanism in Hollow Carbon Nanospheres Using Liquid Phase Transmission Electron Microscopy.

Carbonaceous materials are promising sodium-ion battery anodes. Improving their performance requires a detailed understanding of the ion transport in these materials, some important aspects of which are still under debate. In this work, nitrogen-doped porous hollow carbon spheres (N-PHCSs) are employed as a model system for operando analysis of sodium storage behavior in a commercial liquid electrolyte at the nanoscale. By combining the ex situ characterization at different states of charge with operando transmission electron microscopy experiments, it is found that a solvated ionic layer forms on the surface of N-PHCSs at the beginning of sodiation, followed by the irreversible shell expansion due to the solid-electrolyte interphase (SEI) formation and subsequent storage of Na(0) within the porous carbon shell. This shows that binding between Na(0) and C creates a Schottky junction making Na deposition inside the spheres more energetically favorable at low current densities. During sodiation, the SEI fills the gap between N-PHCSs, binding spheres together and facilitating the sodium ions' transport toward the current collector and subsequent plating underneath the electrode. The N-PHCSs layer acts as a protective layer between the electrolyte and the current collector, suppressing the possible growth of dendrites at the anode.

Electrode-compatible fluorine-free multifunctional additive regulating solid electrolyte interphase and solvation structure for high-performance lithium-ion batteries

The rapid development and widespread application of lithium-ion batteries (LIBs) have increased demand for high-safety and high-performance LIBs. Accordingly, various additives have been used in commercial liquid electrolytes to severally adjust the solvation structure of lithium ions, control the components of solid electrolyte interphase, or reduce flammability. While it is highly desirable to develop low-cost multifunctional electrolyte additives integrally that address both safety and performance on LIBs, significant challenges remain. Herein, a novel phosphorus-containing organic small molecule, bis(2-methoxyethyl) methylphosphonate (BMOP), was rationally designed to serve as a fluorine-free and multifunctional additive in commercial electrolytes. This novel electrolyte additive is low-toxicity, high-efficiency, low-cost, and electrode-compatible, which shows the significant improvement to both electrochemical performance and fire safety for LIBs through regulating the electrolyte solvation structure, constructing the stable electrode-electrolyte interphase, and suppressing the electrolyte combustion. This work provides a new avenue for developing safer and high-performance LIBs.

Dynamic Networks of Cellulose Nanofibrils Enable Highly Conductive and Strong Polymer Gel Electrolytes for Lithium‐Ion Batteries

AbstractTunable dynamic networks of cellulose nanofibrils (CNFs) are utilized to prepare high‐performance polymer gel electrolytes. By swelling an anisotropically dewatered, but never dried, CNF gel in acidic salt solutions, a highly sparse network is constructed with a fraction of CNFs as low as 0.9%, taking advantage of the very high aspect ratio and the ultra‐thin thickness of the CNFs (micrometers long and 2–4 nm thick). These CNF networks expose high interfacial areas and can accommodate massive amounts of the ionic conductive liquid polyethylene glycol‐based electrolyte into strong homogeneous gel electrolytes. In addition to the reinforced mechanical properties, the presence of the CNFs simultaneously enhances the ionic conductivity due to their excellent strong water‐binding capacity according to computational simulations. This strategy renders the electrolyte a room‐temperature ionic conductivity of 0.61 ± 0.12 mS cm−1 which is one of the highest among polymer gel electrolytes. The electrolyte shows superior performances as a separator for lithium iron phosphate half‐cells in high specific capacity (161 mAh g−1 at 0.1C), excellent rate capability (5C), and cycling stability (94% capacity retention after 300 cycles at 1C) at 60 °C, as well as stable room temperature cycling performance and considerably improved safety compared with commercial liquid electrolyte systems.

Deep eutectic solvent electrolytes based on trifluoroacetamide and LiPF6 for Li-metal batteries

New generation lithium batteries require better performances, improved safety, and sustainability. Better performances can be obtained with lithium anodes and high-voltage cathodes, which in turn pose more pressure on the electrolyte stability, which is mandatory for safety. Deep Eutectic Solvents (DESs) are promising components for safer and more environmentally sustainable electrolytes. We investigate the physico-chemical properties of DESs made with 2,2,2-trifluoroacetamide (TFA) and LiPF6. The best composition is tested against Li metal and two cathode active materials: LiFePO4 (LFP) and high voltage LiNi1-x-yMnxCoyO2 (NMC). We obtain good electrochemical performance in a Li-metal cell with LFP. Accelerated rate calorimetry shows improved thermal stability of the Li|DES|NMC cell with respect to a commercial liquid electrolyte.

Dynamics of polymer electrolyte with LiTFSI via Quasi-Elastic Neutron Scattering

Most lithium batteries offer a wide range of applications. However, safety issues are still an unresolved issue for several applications. To solve the safety issue of Li-ion batteries, solid polymer electrolyte is a promising candidate to replace commercial liquid electrolyte. A 4-arm star poly(ethylene oxide) polymer with LiTFSI salt as an electrolyte was studied. The dynamics of this polymer were explored with the Quasi-Elastic Neutron Scattering technique. Furthermore, the influence of temperature and Li salt concentration on the polymer dynamics was investigated. The dynamics of the polymer ends of the arm show much higher flexibility than the core parts making those types of polymers attractive for further studies in battery research.