Electrolytes For Batteries Research Articles

Comparison of trifluoromethyl- and pentafluoroethyl-substituted dicyanoimidazolide lithium salts–their association and electrochemical properties in oligo(ethylene glycols) of different chain length

In this paper, the effect of the length of solvent molecules on the properties of electrolytes was investigated. It was investigated in the model electrolytes consisting of either lithium 4,5-dicyano-2-(trifluoromethyl)imidazolide (LiTDI) or 4,5-dicyano-2-(pentafluoroethyl)imidazolide (LiPDI) dissolved in diglyme and tetraglyme. Such systems were chosen for several reasons. LiTDI is a promising salt for electrolytes for lithium-ion batteries, while LiPDI has a very similar structure, allowing for an assessment of the impact of a difference on electrolyte properties. The solvents were chosen on the basis of the number of oxygen atoms, which for diglyme is insufficient to fulfil lithium’s coordination sphere and is more than enough for this purpose for tetraglyme. This work is a continuation of the study for triglyme. In this work, conductivity, viscosity, lithium transference number, thermal properties and degree of ionic association (as well as solvent-ion interactions) were measured to determine the impact of individual factors. The ionic association’s degree was obtained from FTIR measurements of the samples as well as estimated with Fuoss-Kraus formalism. The conductivity of the samples for those salts depends mostly on the solvent viscosity, while the position of conductivity maxima depends mostly on the length of the solvent molecule. Transference numbers are more dependent on the ionic association and, thus, salt being used.

In-Situ Cross-linked F- and P-Containing Solid Polymer Electrolyte for Long-Cycling and High-Safety Lithium Metal Batteries with Various Cathode Materials.

The practical application of lithium metal batteries (LMBs) has been hindered by limited cycle-life and safety concerns. To solve these problems, we develop a novel fluorinated phosphate cross-linker for gel polymer electrolyte in high-voltage LMBs, achieving superior electrochemical performance and high safety simultaneously. The fluorinated phosphate cross-linked gel polymer electrolyte (FP-GPE) by in-situ polymerization method not only demonstrates high oxidation stability but also exhibits excellent compatibility with lithium metal anode. LMBs utilizing FP-GPE realize stable cycling even at a high cut-off voltage of 4.6 V (vs Li/Li+) with various high-voltage cathode materials. The LiNi0.6Co0.2Mn0.2O2|FP-GPE|Li battery exhibits an ultralong cycle-life of 1200 cycles with an impressive capacity retention of 80.1%. Furthermore, the FP-GPE-based batteries display excellent electrochemical performance even at practical conditions, such as high cathode mass loading (20.84 mg cm-2), ultrathin Li (20 μm), and a wide temperature range of -25 to 80 ℃. Moreover, the first reported solid-state 18650 cylindrical LMBs have been successfully fabricated and demonstrate exceptional safety under mechanical abuse. Additionally, the industry-level 18650 cylindrical LiMn2O4|FP-GPE|Li4Ti5O12 cells demonstrate a remarkable cycle-life of 1400 cycles. Therefore, the impressive electrochemical performance and high safety in practical batteries demonstrate a substantial potential of well-designed FP-GPE for large-scale industrial applications.

Electrolyte Leakage in Cylindrical Lithium-Ion Batteries Subjected to Temperature Cycling

In transportation and operation, lithium-ion batteries can be exposed to environments where the temperature exceeds 75 °C, compromising seal integrity and leading to electrolyte leakage and safety issues. Standards introduced by regulatory bodies require temperature testing, including temperature cycling tests. This study examines cylindrical battery electrolyte leakage due to temperature cycling between 25 °C and 80 °C through capacity tests, electrochemical impedance spectroscopy, computed tomography scans, and thermal analysis. Different thermal expansions among battery cap elements were identified as the cause of leakage. The thermal test parameters and requirements in the UN Manual of Tests and Criteria Section 38.3 were reviewed, revealing the 72 °C upper-temperature limit and the 24 h storage period after temperature cycling fail to effectively qualify lithium-ion batteries for real-world applications.

Water and Salt Concentration-Dependent Electrochemical Performance of Hydrogel Electrolytes in Zinc-Ion Batteries.

Zinc-ion batteries (ZIBs) are promising energy storage devices with safe, nonflammable electrolytes and abundant, low-cost electrode materials. Their practical applications are hampered by various water-related undesirable reactions, such as the hydrogen evolution reaction (HER), corrosion of zinc metal, and water-induced decay of cathode materials. Polymer hydrogel electrolytes were used to control these reactions. However, salt, water, and polymeric backbones intervene in polymer hydrogels, and currently, there are no systematic studies on how salt and water concentrations synergistically affect polymer hydrogels' electrochemical performance. Here, we used an in situ polymerization method to synthesize polyacrylamide (PAM) hydrogels with varied Zn(ClO4)2 (0.5 to 2.0 mol kg-1) and water (40 to 90 wt %) concentrations. Their electrochemical performances in Zn||Ti half-cells, Zn||Zn symmetrical cells, and Zn||V2O5 full cells have been comprehensively evaluated. Although the ionic conductivity of electrolytes increases with the salt concentration, a high salt concentration of 2.0 mol kg-1 with more Zn2+ solvated H2O would induce more severe HER and Zn corrosion at the electrolyte/electrode interfaces. A narrow window of the water concentration at 70-80 wt % is optimal to balance needs for achieving a high ionic conductivity and restricting water-related undesirable reactions. The chemically more active water counts roughly 64.1-73.1 wt % of the total water in electrolytes. PAM hydrogel electrolyte with 1.0 mol kg-1 Zn(ClO4)2 and 80 wt % water enables 1200 h of stable cycling in a Zn||Zn symmetric cell and 99.24% of Coulombic efficiency in a Zn||Ti half-cell. Due to the water-induced decay of V2O5, the electrolyte with 70 wt % water delivers the best performance in a Zn||V2O5 full cell, which can retain 73.7% of its initial capacity after 400 charge/discharge cycles. Our results show that achieving precise control of salt and water concentrations of hydrogel electrolytes in their optimal windows to reduce the fraction of chemically more active water while retaining high ionic conductivity is essential to enabling high-performance ZIBs.

Carbonate Ester-Based Electrolyte Enabling Rechargeable Zn Battery to Achieve High Voltage and High Zn Utilization.

Owing to the high H2O activity, the aqueous electrolyte in the Zn battery exhibits a narrow electrochemical window and inevitable hydrogen evolution reaction, limiting the anode utilization ratio and performance at high voltage. Carbonate ester, the well-developed electrolyte solvent in Li-ion batteries, exhibits aprotic properties and high anodic stability. However, its use in Zn metal batteries is limited due to the low solubility of Zn salts in carbonate esters. Herein, we propose a carbonate ester-based electrolyte (EC:DMC:EMC = 1:1:1 wt %), which contains a new Zn salt (Zn(BHFip)2) characterized by low cost, easy synthesis, and excellent aprotic solvent solubility. The BHFip- anion assists in forming Zn2+ conductive SEI on the anode and decomposes at high voltage to generate a protective CEI layer on the cathode. The Zn//Zn symmetric cell using such electrolyte achieves a remarkable Zn utilization ratio of 91% for 125 h, which has rarely been reported before. Furthermore, the Zn//LiMn2O4 full cell with an average operation voltage of 1.7 V demonstrates reliable cycling for 135 cycles with an N/P ratio of 1:1. In addition, the Zn//LiNi0.5Mn1.5O4 full cell exhibits a high discharge median voltage exceeding 2.2 V for 280 cycles, with the high voltage plateau (above 2 V) constituting 82% of the total capacity.

Electrochemical Removal of HF from Carbonate-based LiPF6-containing Li-ion Battery Electrolytes

Due to the hydrolytic instability of LiPF6 in carbonate-based solvents, HF is a typical impurity in Li-ion battery electrolytes. HF significantly influences the performance of Li-ion batteries, for example by impacting the formation of the solid electrolyte interphase at the anode and by affecting transition metal dissolution at the cathode. Additionally, HF complicates studying fundamental interfacial electrochemistry of Li-ion battery electrolytes, such as direct anion reduction, because it is electrocatalytically relatively unstable, resulting in a LiF passivation layer. Methods to selectively remove ppm levels of HF from LiPF6-containing carbonate-based electrolytes are limited. We introduce and benchmark a simple yet efficient electrochemical method to selectively remove ppm amounts of HF from LiPF6-containing carbonate-based electrolytes. The basic idea is the application of a suitable potential to a high surface-area metallic electrode upon which only HF reacts (electrocatalytically) while all other electrolyte components are unaffected under the respective conditions.

Investigation of sulphate hydride anti-perovskite as solid electrolyte

Over the last decade, anti-perovskites have drawn significant attention as potential solid-electrolytes for solid-state batteries. Due to the increase in consumption of lithium, there has been a push towards next generation batteries, including sodium-ion batteries. The first representative of the material class of sulphate hydride anti-perovskites, Na3SO4H, was synthesized by solid-state methods as a possible electrolyte for sodium solid-state batteries. Structural characterization confirms the results reported in literature with P4/nmm space group Thermal measurements (DSC and TGA) reveal the stability of the material up to 633 K with H2 release beginning shortly after. Here were report the first electrochemical measurements of this new sulphate hydride anti-perovskite with room temperature conductivity of 4.0 × 10−7 S/cm. Similarly, the electronic conductivity was also measured by Direct Current (DC) experiments to understand a non-linear Arrhenius plot of the conductivity. From the EIS and DC measurements, it is suggested that the electronic and ionic conductivities of this material fall in the same range at room temperature. Upon heating, the material becomes a mainly ionic conductor, explaining the change in the activation energy values in the Arrhenius plot (0.83 eV at low T and 0.24 eV at high T). Solid-state NMR hints at defects in the structure that correspond to Na1 and Hb-c-d dynamics.

The Influence of Cathode Degradation Products on the Anode Interface in Lithium-Ion Batteries.

Degradation of cathode materials in lithium-ion batteries results in the presence of transition metal ions in the electrolyte, and these ions are known to play a major role in capacity fade and cell failure. Yet, while it is known that transition metal ions migrate from the metal oxide cathode and deposit on the graphite anode, their specific influence on anode reactions and structures, such as the solid electrolyte interphase (SEI), is still quite poorly understood due to the complexity in studying this interface in operational cells. In this work we combine operando electrochemical atomic force microscopy (EC-AFM), electrochemical quartz crystal microbalance (EQCM), and electrochemical impedance spectroscopy (EIS) measurements to probe the influence of a range of transition metal ions on the morphological, mechanical, chemical, and electrical properties of the SEI. By adding representative concentrations of Ni2+, Mn2+, and Co2+ ions into a commercially relevant battery electrolyte, the impacts of each on the formation and stability of the anode interface layer is revealed; all are shown to pose a threat to battery performance and stability. Mn2+, in particular, is shown to induce a thick, soft, and unstable SEI layer, which is known to cause severe degradation of batteries, while Co2+ and Ni2+ significantly impact interfacial conductivity. When transition metal ions are mixed, SEI degradation is amplified, suggesting a synergistic effect on the cell stability. Hence, by uncovering the roles these cathode degradation products play in operational batteries, we have provided a foundation upon which strategies to mitigate or eliminate these degradation products can be developed.

Studi Pengaruh Elektrolit Nacl terhadap Baterai Elektroda Pb- Pb02 berbasis PV Sebagai Charging

Research has been conducted on the study of the effect of NaCl electrolyte on Pb-PbO2 electrode batteries. So far, H2SO4 battery electrolyte can have a negative impact, one of which can irritate the skin, it will even become toxic when inhaled by humans. For this reason, I tried to replace the use of the H2SO4 electrolyte with NaCl electrolyte so that a voltage of 6.73 volts was obtained while the H2SO4 electrolyte reached a voltage of 12 volts with an electrolyte that was more environmentally friendly. Furthermore, the NaCl electrolyte will be developed to increase the voltage yield equal to the H2SO4 electrolyte.

Revitalization of Diluent Amide-Based Electrolyte for Building High-Voltage Lithium-Metal Batteries.

Hitherto, highly concentrated electrolyte is the overarching strategy for revitalizing the usage of amide - in lithium-metal batteries (LMBs), which simultaneously mitigates the reactivity of amide toward Li and regulates uniform Li deposition via forming anion-solvated coordinate structure. However, it is undeniable that this would bring the cost burden for practical electrolyte preparation, which stimulates further electrolyte design toward tailoring anion-abundant Li+ solvation structure in stable amide electrolytes under a low salt content. Herein, a distinct method is conceived to design anions-enriched Li+ solvation structure in dilute amide-electrolyte (1m Li-salt concentration) with the aid of integrating perfluoropolyethers (PFPE-MC) with anion-solvating ability and B/F-involved additives. The optimized electrolyte based on N,N-Dimethyltrifluoroacetamide (FDMAC) exhibits outstanding compatibility with Li and NCM622 cathode, facilitates uniform Li deposition along with robust solid electrolyte interphase (SEI) formation. Accordingly, both the lab-level LMB coin cell and practical pouch cell based on this dilute FDMAC electrolyte deliver remarkable performances with improved capacity and cyclability. This work pioneers the feasibility of diluted amide as electrolyte in LMB, and provides an innovativestrategy for highly stable Li deposition via manipulating solvation structure within diluent electrolyte, impelling the electrolyte engineering development for practical high-energy LMBs.

NaSbF4 nanoparticles as solid-state electrolytes in sodium-iodine batteries: sodium ion transport via conversion reaction and shuttle effect retarded by fluoride

Na-I2 batteries have emerged as an appealing energy storage technology owing to high energy density and cost-effectiveness. However, the practical application of Na-I2 batteries faces the dissolution of iodide/polyiodide in the electrolyte during the charge/discharge process. Herein, we immobilize I2 by utilization of NaSbF4 (NSF)-based solid-state electrolyte (SSE). Impressively, the Na+ transport in NSF nanoparticles (NPs) is via the conversion reaction of NaSbF4 + NaF ↔ Na2SbF5, which is different from the acknowledged Na+ diffusion mechanism via vacancies in inorganic SSEs. To improve the interfacial compatibility, a composite polymer electrolyte (CPE) is fabricated based on NSF, poly (vinylidene fluoride - hexafuoro -propylene) (PVDF-HFP) and NaClO4, giving rise to stable Na stripping/plating in Na|Na symmetric cell. Especially, the quasi-solid-state Na|NSF CPE |I2 full cell shows an outstanding electrochemical behavior, which is associated with the partial reduction of ClO4− → Cl− and the stabilization of I+ by F− or Cl− in the charge/discharge process. The resultant I+-F- or I+-Cl- intermediate can promote the multi-electron transfer of 2I− → I2 → 2I+, leading to enhanced capacity and mitigated shuttle effect of iodide. Meanwhile, the formation of I+-F- in turn weakens the interaction of Na⋯F in NSF, which is beneficial for Na+ transport.

Mixture electrolyte suppressing water-induced parasitic reactions on Zn anode by tuning multilayer solvating structure

Though aqueous zinc ion batteries have been identified as a feasible option for energy storage, there are still some challenges that block the development of aqueous zinc ion battery, especially the issues from zinc metal anode. Tuning solvating structure of Zn2+ and adjusting the electrolyte in recent years is considered to be a simple but potential strategy to improve stability of zinc anode. In this work, a mixture electrolyte was obtained by dessolving LiTFSI/TEGDME Li-O2 battery electrolyte into 2 M aqueous ZnSO4 solution to tune solvating structure and adjust the striping/plating process of anode. Molecular spectrum and X-ray based method clarified that the mixture electrolyte plays dual functions to protect anode during electrochemical process. From one aspect, TEGDME partially replaced water and reconstructed a new multilayer solvating shell with TFSI-, which is beneficial for fast dendrite-free deposition. From the other aspect, surface spectrum also revealed that due to the participation of Li+ and TFSI-, a surface layer with ZnOHS framework and ZnF2 fillings formed on anode which further inhibit the dendrite growth and stabilize anode. This work combines the method of tuning solvation structure and construct SEI together and opens a new view designing new electrolytes for aqueous Zn-ion battery.

Influence of Zr aggregation on Li-ion conductivity of amorphous solid-state electrolyte Li-La-Zr-O.

In our study, we investigated the influence of the local structure of amorphous Li-La-Zr-O (a-LLZO) on Li-ion conductivity using abinitio molecular dynamics (AIMD). A-LLZO has shown promising properties in inhibiting the growth of lithium dendrites, making it a potential candidate for solid electrolytes in all-solid-state lithium batteries. The low Li-ion conductivity of a-LLZO is currently limiting its practical applications. Our findings revealed that the homogeneous distribution of Zr-O polyhedra within the pristine structure of a-LLZO contributes to enhanced Li-ion conductivity. By reducing the interconnections among Zr-O polyhedra, the AIMD-simulated a-LLZO sample achieved a Li-ion conductivity of 5.78 × 10-4 S/cm at room temperature, which is slightly lower than that of cubic LLZO (c-LLZO) with a Li-ion conductivity of 1.63 × 10-3 S/cm. Furthermore, we discovered that Li-ion conductivity can be influenced by adjusting the elemental ratios within a-LLZO. This suggests that fine-tuning the composition of a-LLZO can potentially further enhance its Li-ion conductivity and optimize its performance as a solid electrolyte in lithium batteries.

Mof-derived ionic conductor enhancing the performance of polymer electrolyte for solid-state lithium batteries

The solid-state electrolyte is an important component of solid-state batteries and significantly influences the performance of batteries. However, pure solid-state polymer electrolyte has challenges such as low ionic conductivity, weak mechanical strength and poor ability to inhibit lithium dendrites. Therefore, a unique nano porous structural material based on a metal–organic framework (MOF) was proposed as a filler to enhance the polymer electrolyte, which is lithium ionic liquid (Li-IL) immersed into the MIL-125 framework to transform MIL-125 from an inert conductor to an efficient ionic conductor to obtain MIL-125-Li. MIL-125-Li not only has Lewis acid nature, but also provides a more definite and continuous transport pathway for the rapid migration of Li+. The composite polymer electrolytes (CPEs), containing 15 wt% of MIL-125-Li, exhibit an ionic conductivity of 3.9 × 10-4 S cm−1 at 28 °C. Furthermore, the CPEs demonstrate excellent interfacial stability with the lithium metal electrode, effectively inhibiting the growth of lithium dendrites. The assembled symmetric Li/PL-15 % MIL-125/Li battery can be stably cycled for more than 700 h at 0.1 mA cm−2 at 28 °C. Applying the composite polymer electrolyte to LiFePO4/Li batteries, the discharge specific capacity achieves ∼130 mAh g-l with a capacity retention rate of 83.9 % after cycling for 500 cycles at 0.5C. This simple modification method provides a novel design idea for all solid-state lithium batteries with excellent electrochemical performance.

Enhancement of ionic conductivity and electrochemical stability of PVA/HPMC/PANI/CuSO4 gel polymer for rechargeable batteries electrolytes

Gel polymer electrolytes (GPEs) have drawn a lot of interest due to their special qualities, which include high conductivity that is comparable to liquid electrolytes, excellent mechanical stability, and high flexibility. Using the solution casting approach, we have synthesized copper ion conducting gel polymer electrolyte (GPE) films made of polyvinyl alcohol (PVA) as the polymer host. An ionic salt, copper sulphate (CuSO4), and a plasticizing solvent, PANI/ [BMIM] [BF4] polyionic liquid, were employed. The structural, electrical, and electrochemical properties of the GPE films were carefully examined. The significant XRD crystalline peak decreased and disappeared upon the addition of PANI/[BMIM] [BF4] polyionic liquid, suggesting that PIL is a useful plasticizer for the PVA/HPMC polymers.The conductivity of GPE films was determined by electrochemical impedance spectroscopy measurements. The sample containing 20% CuSO4 salt has the highest room temperature conductivity (σ = 5.11 × 10−3 S/cm). The measurements of transference numbers show that ions are primarily responsible for the transport of these electrolytes. It seems that the working voltage range is high enough to be used as an electrolyte in batteries, based on the results of using linear sweep voltammetry (LSV) and cyclic voltammetry to evaluate the electrochemical stability of the GPE films.

A new iron battery technology: Charge-discharge mechanism of ferrous chloride and ferric oxide electrolyte in all solid-state iron-graphite batteries

This study investigates a Fe/SSE/GF battery. Iron (Fe) as cathode material contains higher electrical capacity and competitive advantages. The solid-state electrolyte (SSE) material is sodium silicate powder mixed with iron compound powders. There are four types of iron compounds: 1) iron oxide, 2) chlorinated/Na-rich iron oxide, 3) Cl-rich iron oxide, 4) ferrous chloride, which are compared with sodium silicate powder. The negative electrode material is graphite film (GF). According to experiments, converting iron into iron oxide or ferric chloride can enhance battery capacity (beyond 200 mAh/g) and cycle life. The reliability of the Fe/SSE/GF battery was assessed by substituting sodium silicate powder with an iron compound electrolyte and adding binder (Polyvinyl Alcohol, PVA) into powder to enhance the performance of Fe/SSE/GF. This experimental research is not only innovative but also represents a significant milestone in the field of solid-state energy storage.

Synthesis and Properties of Polyvinylidene Fluoride-Hexafluoropropylene Copolymer/Li6PS5Cl Gel Composite Electrolyte for Lithium Solid-State Batteries.

Gel electrolytes for lithium-ion batteries continue to replace the organic liquid electrolytes in conventional batteries due to their advantages of being less prone to leakage and non-explosive and possessing a high modulus of elasticity. However, the development of gel electrolytes has been hindered by their generally low ionic conductivity at room temperature and high interfacial impedance with electrodes. In this paper, a poly (vinylidene fluoride)-hexafluoropropylene copolymer (PVdF-HFP) with a flexible structure, Li6PS5Cl (LPSCl) powder of the sulfur-silver-germanium ore type, and lithium perchlorate salt (LiClO4) were prepared into sulfide gel composite electrolyte films (GCEs) via a thermosetting process. The experimental results showed that the gel composite electrolyte with 1% LPSCl in the PVdF-HFP matrix exhibited an ionic conductivity as high as 1.27 × 10-3 S·cm-1 at 25 °C and a lithium ion transference number of 0.63. The assembled LiFePO4||GCEs||Li batteries have excellent rate (130 mAh·g-1 at 1 C and 54 mAh·g-1 at 5 C) and cycling (capacity retention was 93% after 100 cycles at 0.1 C and 80% after 150 cycles at 0.2 C) performance. This work provides new methods and strategies for the design and fabrication of solid-state batteries with high ionic conductivity and high specific energy.

Research Progress on the Composite Methods of Composite Electrolytes for Solid-State Lithium Batteries.

In the current challenging energy storage and conversion landscape, solid-state lithium metal batteries with high energy conversion efficiency, high energy density, and high safety stand out. Due to the limitations of material properties, it is difficult to achieve the ideal requirements of solid electrolytes with a single-phase electrolyte. A composite solid electrolyte is composed of two or more different materials. Composite electrolytes can simultaneously offer the advantages of multiple materials. Through different composite methods, the merits of various materials can be incorporated into the most essential part of the battery in a specific form. Currently, more and more researchers are focusing on composite methods for combining components in composite electrolytes. The ion transport capacity, interface stability, machinability, and safety of electrolytes can be significantly improved by selecting appropriate composite methods. This review summarizes the composite methods used for the components of composite electrolytes, such as filler blending, embedded framework, and multilayer bonding. It also discusses the future development trends of all-solid-state lithium batteries (ASSLBs).

Reevaluate low-concentration ether-based electrolytes for lithium metal batteries

Ether is regarded as an exceptional solvent in liquid electrolytes for lithium (Li) metal batteries due to its outstanding compatibility with Li metal anode. Low salt concentration in ether-based electrolytes (LCEEs) is highly favorable to reducing the cost of future Li metal batteries. Nevertheless, LCEEs have been reported to exhibit poor anodic stability (as low as 4.0 V vs. Li/Li+), therefore considered unsuitable for practical batteries using LiNixMnyCozO2 as cathodes and charge up to 4.4 V. Here, using 1.0 M lithium bis(fluorosulfonyl)imide (LiFSI) in 1,2-dimethoxyethane (DME) as the baseline, we demonstrate the intrinsic anodic stability window of LCEE to be above 4.5 V. We revealed the true failure mechanism of LCEE to be various electrochemical reactions with different working electrodes (WEs). We further provide electrolyte and electrode design rules to prevent LCEE decomposition, as well as electrode and packaging materials corrosion at high voltage. This study highlights the importance of previously overlooked battery component compatibility in electrolyte development and offers valuable insights into battery engineering considerations toward high-energy and cost-effective Li metal batteries.

Electrolyte Design for High-Voltage Lithium-Metal Batteries with Synthetic Sulfonamide-Based Solvent and Electrochemically Active Additives.

Considering practical viability, Li-metal battery electrolytes should be formulated by tuning solvent composition similar to electrolyte systems for Li-ion batteries to enable the facile salt-dissociation, ion-conduction, and introduction of sacrificial additives for building stable electrode-electrolyte interfaces. Although 1,2-dimethoxyethane with a high-donor number enables the implementation of ionic compounds as effective interface modifiers, its ubiquitous usage is limited by its low-oxidation durability and high-volatility. Regulation of the solvation structure and construction of well-structured interfacial layers ensure the potential strength of electrolytes in both Li-metal and LiNi0.8 Co0.1 Mn0.1 O2 (NCM811). This study reports the build-up of multilayer solid-electrolyte interphase by utilizing different electron-accepting tendencies of lithium difluoro(bisoxalato) phosphate (LiDFBP), lithium nitrate, and synthetic 1-((trifluoromethyl)sulfonyl)piperidine. Furthermore, a well-structured cathode-electrolyte interface from LiDFBP effectively addresses the issues with NCM811. The developed electrolyte based on a framework of highly- and weakly-solvating solvents with interface modifiers enables the operation of Li|NCM811 cells with a high areal capacity cathode (4.3 mAh cm-2 ) at 4.4V versus Li/Li+ .