Inorganic Layers Research Articles

Spin-coated high mobility MoO3 thin film for designing highly efficient lead-free perovskite solar cells

Among the thin film-photovoltaics, perovskite solar cells (PSCs) are one of the most developing topics of research in recent times. Research records reveal that around 26 % efficiency in PSCs has already been achieved so far. However, the commercialization of those PSCs is hindered due to the toxicity of lead (Pb), and the instability of organic cations as well as structural volatility. Several inorganic materials including inorganic hole transport layer (HTL) have recently been proposed and developed to reduce the organic part in the device structure. We fabricate MoO3 thin film materials and conduct a detailed study to realize the potential of MoO3 as a unique HTL for application in PSCs. The synthesis of MoO3 thin film includes several characterization techniques e.g. XRD, FESEM, EDX, UV–Vis, and Hall Effect measurement. We design a MoO3 thin film-based, lead-free PSC structure of FTO/MoO3/PTAA/(FA)2BiCuI6/ZnO/Ag and perform numerical analysis using the SCAPS-1D simulation tool. In the device simulation process, we use the experimentally obtained optoelectrical properties of the MoO3 film and achieve a maximum efficiency of around 22.28 % in a contained lead-free PSC.

Nickel Oxide Hole Injection Layers for Balanced Charge Injection in Quantum Dot Light-Emitting Diodes.

Quantum dot (QD) light-emitting diodes (QLEDs) are promising for next-generation displays, but suffer from carrier imbalance arising from lower hole injection compared to electron injection. A defect engineering strategy is reported to tackle transport limitations in nickel oxide-based inorganic hole-injection layers (HILs) and find that hole injection is able to enhance in high-performance InP QLEDs using the newly designed material. Through optoelectronic simulations, how the electronic properties of NiOx affect hole injection efficiency into an InP QD layer, finding that efficient hole injection depends on lowering the hole injection barrier and enhancing the acceptor density of NiOx is explored. Li doping and oxygen enriching are identified as effective strategies to control intrinsic and extrinsic defects in NiOx, thereby increasing acceptor density, as evidenced by density functional theory calculations and experimental validation. With fine-tuned inorganic HIL, InP QLEDs exhibit a luminance of 45200cdm-2 and an external quantum efficiency of 19.9%, surpassing previous inorganic HIL-based QLEDs. This study provides a path to designing inorganic materials for more efficient and sustainable lighting and display technologies.

Improving Interfacial and Compressive Properties of Polyimide Fiber by Constructing Inorganic Layers on Fiber Surface.

The compressive performance of organic fiber has always been a key problem, limiting its development. In this paper, silicon oxide, alumina, and titanium oxide particles were separately deposited on the surface of high-strength and high-modulus polyimide (PI) fibers to form a structural supporting shell by using a magnetron sputtering method. The theoretical thickness was calculated by thermogravimetric analysis in good agreement with the actual thickness determined from scanning electron microscopy. The mechanics, surface, and interface properties of the measured fibers were analyzed mainly from the aspects of surface energy, interfacial shear strength (IFSS), and compression strength. The results showed that after magnetron sputtering, the inorganic shells were uniformly deposited on the surface of PI fiber, resulting in an increase in the content of inorganic elements as well as the roughness. As a result, the surface energy and IFSS of silica-coated fiber was increased by 174 and 85.6%, respectively, and compression strength was increased by 45.7%. This study provides a new approach for improving the interface property and compression strength of high-strength and high-modulus PI-fiber-reinforced composites.

Interlayer Carrier Dynamics in Two-Dimensional Perovskites Determined by the Length of Conjugated Organic Cations.

Unlocking the restricted interlayer carrier transfer in a two-dimensional perovskite is a crucial means to achieve the harmonization of efficiency and stability in perovskite solar cells. In this work, the effects of conjugated organic molecules on the interlayer carrier dynamics of 2D perovskites were investigated through nonadiabatic molecular dynamics simulations. We found that elongated conjugated organic cations contributed significantly to the accelerated interlayer carrier dynamics, originating from lowered transport barrier and boosted π-p coupling between organic and inorganic layers. Utilizing conjugated molecules of moderate length as spacer cations can yield both superior efficiency and exceptional stability simultaneously. However, conjugated chains that are too long lead to structural instability and stronger carrier recombination. The potential of conjugated chain-like molecules as spacer cations in 2D perovskites has been demonstrated in our work, offering valuable insights for the development of high-performance perovskite solar cells.

Suppressing the damage of deposited Mn(II) ions to graphite anode in lithium‐ion batteries by electrolyte additive agent and positive material coating

AbstractSEM and EDS techniques are carried out to demonstrate the variation of morphology and chemical compound on the surface of graphite anode, which suggest a well‐accepted concept that the manganese ions have serious influence on the reversible capacity fade of graphite anode in lithium ion batteries. Based the main chemical compounds of the inorganic layer on the graphite surface, the evolution steps of graphite structure damaged by Mn ions are derived. Although the amount of deposited manganese ions is small, these play an important role in the catalytic decomposition of the electrolyte. Moreover, Raman analysis shows that the structure of the graphite anode becomes irregular at initial SEI formation cycles and tends to be stable at subsequent cycles. This structure variation is probably generated from the manganese ion deposition and the solid electrolyte interphase (SEI) film formation. According to the capacity tests, the cycling performance of NCM811/graphite lithium‐ion batteries could be improved 50% by FEC additive and B2O3 surface coating. FEC additive maybe benefit graphite forming a stable SEI film in the early stages of cycling to suppress the damage of Mn2+ ions, then improving the cycling performance.

4-Carboxyanilinium dihydrogen phosphate monohydrate, an organophosphate adducts of 4-amino benzoic acid: Structural, vibrational, thermal, and computational studies

4-Carboxyanilinium dihydrogen phosphate monohydrate (4-CAH2PO4·H2O), an organophosphate adduct, was synthesized and characterized by single-crystal X-ray diffraction, Fourier transform infrared (FTIR), Differential scanning calorimetry (DSC) and computational analysis performed using CrystalExplorer 21, Gaussian 09W and Multiwfn 3.7 software. The complex 4-CAH2PO4·H2O crystallized in the triclinic space group, P-1, with two molecules each of 4-carboxyanilinium (4-CA) cations, H2PO4– anions, and water, respectively, in an asymmetric unit. Crystal data for C7H12NO7P: triclinic, space group P-1, a = 8.5238(2) Å, b = 8.9068(2) Å, c = 14.4976(4) Å, α = 106.456(2)°, β = 90.195(2)°, γ = 92.811(2)°, V = 1054.13(5) Å3, Z = 4, T = 293 K, μ(Cu Kα) = 2.587 mm-1, Dcalc = 1.595 g/cm3, 18182 reflections measured (6.358° ≤ 2Θ ≤ 146.396°), 4149 unique (Rint = 0.1018, Rsigma = 0.0521) which were used in all calculations. The final R1 was 0.0584 (I > 2σ(I)) and wR2 was 0.1712 (all data). The organic layer containing 4-CA cations and the inorganic layer containing phosphate anions and water molecules in 4-CAH2PO4·H2O crystals are connected through a three-dimensional network of strong charge-assisted N–H···O and C-OH···O hydrogen bonds. The fingerprint plot of 4-CAH2PO4·H2O obtained indicated that the most prominent interaction corresponds to the short O···H contact, followed by the H···H and H···C contacts. The intermolecular interaction topology of 4-CAH2PO4·H2O has been quantitatively analyzed. The 4-CAH2PO4·H2O complex was optimized by density functional theory (DFT) with B3LYP/6-31G basis set and the theoretical IR vibrational spectra determined. The noncovalent interaction (NCI) and quantum theory of the atom in the molecule (QTAIM) analysis were done using Multiwfn 3.7 software. 4-CAH2PO4·H2O complex structure and its computational analysis are also compared with that of 4-carboxyanilinium dihydrogen phosphate (4-CAH2PO4).

Synergistic effects of organosilicon flame retardant and DOPO-based reactive compatibilizer for high performance PC/PBT composites

PC/PBT alloy is flammable resulting in fire safety hazards in practical applications and the existing flame retardants have a great influence on the mechanical properties, which limits its application range. Therefore, it is an urgent problem to improve the flame retardancy of PC/PBT alloy while taking its mechanical properties into account. Herein, a novel flame retardant and reactive compatibilizer was synthesized by grafting 9,10-dihydro-9-oxa-10-phosphophenanthrene-10-oxide (DOPO) onto ethylene-methyl acrylate-glycidyl methacrylate (EMA-GMA), named as DOPO-EG, to improve the flame retardancy and mechanical properties of PC/PBT alloy simultaneously. Additionally, based on the effective synergistic effect of enhancing the charring and flame retardancy between silicon and phosphorus, the organosilicon flame retardant (RMSi) is introduced and compounded with DOPO-EG to prepare excellent flame retardancy PC/PBT/DOPO-EG/RMSi composites. The results showed that the PC/PBT/DOPO-EG/RMSi composites with 10 wt% DOPO-EG and 8 wt% RMSi (CBE10P10Si8) reached UL-94 V-0 rating and the peak of heat release rate (PHRR) and total heat release rate (THR) of CBE10P10Si8 decreased by 42% and 16% respectively. This is due to the fact that DOPO is cracked into phosphorus radicals to capture and eliminate the active H and OH radicals, inhibiting the chain free radical reaction, and RMSi is enriched on the surface of CBE10P10Si8 to form an inorganic oxygen insulation protective layer during combustion. The impact strength of CBE10P10Si8 increased from 5.8 kJ/m2 to 11.9 kJ/m2. The improvement of impact strength is owing to the existence of DOPO-EG which promotes the formation of the interface layer between PC and PBT phases, resulting in the transfer of stress between the two phases. This work provides a new method for the preparation of PC/PBT alloy with excellent flame retardancy and mechanical properties, and also provides a certain reference value for the research of flame retardancy and toughening modification of polymer composites.

Performance optimization study of lead-free CsSnGeI3 based perovskite solar cell heterostructure with different inorganic electron transport layers: A numerical simulation approach

Perovskite solar cells (PSCs) are considered to be one of the most prominent candidates for its commercialization. The meteoric properties of the PSC have always astounded the researchers. Thus, in this perspective, the germanium-based PSCs are able to increase a sense of curiosity among photovoltaic (PV) researchers due to its superior stability and efficiency. In the present work, different combinations of the lead-free and non-toxic inorganic caesium tin-germanium (CsSnGeI3) based PSC structures have been studied using various electron transport layers (ETLs) (SnS2, TiO2, WS2, MoTe2 and ZnSe) and Mg–CuCrO2 as a hole transport layer due to its meteoric properties. For each ETL, the impact of material parameters including the thickness of the various layers, absorber acceptor density, donor density, absorber defect density, absorber radiative recombination and interfacial defect density are examined to study the cell performance (such as Voc, Jsc, FF, and PCE). Moreover, the role of operating temperature, shunt resistance and series resistance in analysing the cell performance has also been checked towards its practical applicability. The results show ZnSe as the best ETL in comparison to other inorganic ETLs for CsSnGeI3 based absorber with Mg–CuCrO2 as an HTL, used in this work resulting in a good cell performance with a power conversion efficiency (PCE) of 33.24%, Voc ∼ 1.36 V, Jsc ∼ 28.02 mA/cm2 and fill factor (FF) ∼ 86.79%. The proposed simulation work may pave the way for further design and optimization of Sn-based PSCs towards practical applications.

SBP]BF4 Additive Stabilizing Zinc Anode by Simultaneously Regulating the Solvation Shell and Electrode Interface

The zinc anode mainly faces technical problems such as short circuits caused by the growth of dendrite, low coulomb efficiency, and a short cycle life caused by side reactions, which impedes the rapid development of aqueous zinc-ion batteries (AZIBs). Herein, a common ionic liquid, 1,1-Spirobipyrrolidinium tetrafluoroborate ([SBP]BF4), is selected as a new additive for pure ZnSO4 electrolyte. It is found that this additive could regulate the solvation sheath of hydrated Zn2+ ions, promote the ionic mobility of Zn2+, homogenize the flux of Zn2+, avoid side reactions between the electrolyte and electrode, and inhibit the production of zinc dendrites by facilitating the establishment of an inorganic solid electrolyte interphase layer. With the 1% [SBP]BF4-modified electrolyte, the Zn||Zn symmetric cell delivers an extended plating/stripping cycling life of 2000 h at 1 mA cm−2, which is much higher than that of the cell without additives (330 h). As a proof of concept, the Zn‖V2O5 battery using the [SBP]BF4 additive shows excellent cycling stability, maintaining its specific capacity at 97 mAh g−1 after 2000 cycles at 5 A g−1, which is much greater than the 46 mAh g−1 capacity of the non-additive battery. This study offers zinc anode stabilization through high-efficiency electrolyte engineering.

Effectively Inhibiting Charge Injection and Dielectric Loss of High Permittivity Inorganic Materials by Rationally Coating Organic Polymer for Achieving High Output Charge Density

AbstractAlthough high permittivity of inorganic materials (possibly two orders larger than organic polymers) is theoretically considered as ideal triboelectric materials, their high leakage property and low contact potential difference with metal electrodes lead to failure to obtain high triboelectric charge density. Besides, the internal space charge accumulation as a result of their defect levels reduces the output charge density and causes dielectric loss or even dielectric breakdown under charge injection in charge‐excitation triboelectric nanogenerator (CE‐TENG). Herein, this study proposes high permittivity and low dielectric loss inorganic materials as triboelectric layers. In order to prevent charge injection passing through the surface of inorganic materials caused by air breakdown under charge excitation, an organic polymer is coated, which has high permittivity, big polarizability, none charge traps, and large work function difference with metal electrodes. After optimizing the high dielectric inorganic layer and the coated organic polymer layer, the output charge of CE‐TENG based on 1 mm PZT‐5H coated with P(VDF‐TrFE‐CFE) achieves 2.83 mC m−2, 6.5 times of CE‐TENG based on 1 mm PZT‐5H, breaking the historical record for inorganic material TENG. This work clarifies the material selection criteria for CE‐TENG and provides a deeper understanding of charge transfer mechanism of inorganic materials.

Enhanced Conversion Efficiency in MAPbI3 Perovskite Solar Cells through Parameters Optimization via SCAPS-1D Simulation

In this study, various factors affecting the efficiency of the MAPbI3 perovskite solar cell (PSC) were analyzed using the SCAPS-1D simulation program. The basic device analyzed in this study had a structure of ITO/TiO2/MAPbI3/Cu2O/Au. The thickness of each layer (electron transport layer (ETL), perovskite absorption layer (PAL), and hole transport layer (HTL)), PAL defect density and interface defect density were investigated as parameters. The optimized parameters that yielded the highest light conversion efficiency were an ETL (TiO2) thickness of 100 nm, a PAL (MAPbI3) thickness of 1300 nm, an HTL (Cu2O) thickness of 400 nm, a PAL defect density of 1014 cm−3, and an interface defect density of 1013 cm−3 for both absorber/ETL and absorber/HTL interfaces. The optimized PSC exhibited a maximum efficiency of 19.30%. These results obtained in this study are expected to contribute considerably to the optimization and efficiency improvement of perovskite solar cells using inorganic charge-carrier transport layers.

Fluorinated Quasi 2D Perovskite Solar Cells with Improved Stability and Over 19% Efficiency

Abstract2D Ruddlesden–Popper perovskites (RPP) with excellent environmental and structural stability are emerging photovoltaic materials. Here, a benzylamine‐based spacer, namely 3,5‐difluorobenzylamine (DF‐BZA), is developed for stable and efficient quasi‐2D‐RP perovskite solar cells (PSCs). Compared to benzylamine (BZA)‐based quasi‐2D RPP, the DF‐BZA‐based perovskite film exhibited superior film quality with significantly enlarged grain size and improved charge carrier lifetime owing to the fluorine atoms in DF‐BZA. As a result, the optimized (DF‐BZA)2FA3Pb4I13 PSCs achieve a power conversion efficiency (PCE) of 19.24%, while BZA‐based PSCs ((BZA)2FA3Pb4I13) only achieve a PCE of 17.04%. This represents the champion PCE using FA as the A‐site cation in quasi‐2D RPPs with n = 4. Moreover, due to the effective insertion of fluorinated spacers into the inorganic layers, the moisture resistance stability and 85 °C thermal stability of (DF‐BZA)2FA3Pb4I13 are significantly improved. The improvement of photovoltaic performance and stability highlight the great potential of DF‐BZA‐based spacer for high‐performance quasi‐2D RP PSCs.

Understanding the Inorganic‐Rich Feature of Anion‐Derived Solid Electrolyte Interphase

AbstractAnion‐derived solid‐electrolyte interphase (SEI) has received growing attention owing to its appealing properties like fast ion transport and excellent passivation effect. However, a sophisticated understanding of anion‐derived SEI is lacking. To common wisdom, anion‐derived SEI features an inorganic‐rich composition. Herein, it is reveal that the freshly formed anion‐derived SEI consists of a polymer‐rich outer layer and an inorganic inner layer. Then, the organic components dissolve during the discharge process, while the inorganic species with low solubility are retained in the empty SEI husk. The accumulation of empty SEI husks during cycling forms a reacted lithium (Li) layer, which features a much higher content of anion‐derived inorganic species than the newly formed SEI. Therefore, the acknowledged “anion‐derived inorganic‐rich SEI” actually refers to the reacted Li layer instead of the freshly formed SEI. This work provides fruitful insights on the compositional features of anion‐derived SEI.

Dion-Jacobson Type Lead-Free Double Perovskite with Ultra-Narrow Aromatic Interlayer Spacing for Highly Sensitive and Stable X-ray Detection.

The low-toxic and environmentally friendly 2D lead-free perovskite has made significant progress in the exploration of "green" X-ray detectors. However, the gap in detection performance between them and their lead-based analogues remains a matter of concern that cannot be ignored. To reduce this gap, shortening the interlayer spacing to accelerate the migration and collection of X-ray carriers is a promising strategy. Herein, a Dion-Jacobson (DJ) lead-free double perovskite (4-AP)2 AgBiBr8 (1, 4-AP = 4-amidinopyridine) with an ultra-narrow interlayer spacing of 3.0Å, is constructed by utilizing π-conjugated aromatic spacers. Strikingly, the subsequent enhanced carrier transport and increased crystal density lead to X-ray detectors based on bulk single crystals of 1 with a high sensitivity of 1117.3µCGy-1 cm-2 , superior to the vast majority of similar double perovskites. In particular, the tight connection of the inorganic layers by the divalent cations enhances structural rigidity and stability, further endowing 1 detector with ultralow dark current drift (3.06×10-8 nAcm-1 s-1 V-1 , 80V), excellent multiple cycles switching X-ray irradiation stability, as well as long-term environmental stability (maintains over 94% photoresponse after 90 days). This work brings lead-free double perovskites one step closer to realizing efficient practical green applications.

Br-substituent effect on photoluminescence and scintillation properties of (C6H5C2H4NH3)2PbCl4 perovskite-type compounds

The photoluminescence and scintillation properties of n-bromophenethylammonium lead chloride ((n-BrPEA)2PbCl4) (n = 4, 3, and 2) and phenethylammonium lead chloride ((PEA)2PbCl4) have been investigated. All the samples showed broad emission peaks at 400–700 nm upon excitation by UV light or X-ray. The decay time constants of 8–28 ns were obtained which originated from the recombination of self-trapped exciton (STE) within inorganic layers. The afterglow levels at 20 ms after 2 ms of X-ray irradiation of (4-BrPEA)2PbCl4 and (3-BrPEA)2PbCl4 (76 and 55 ppm) were better than (PEA)2PbCl4 (379 ppm). The light yield of (4-BrPEA)2PbCl4 (3100 photons/5.5 MeV-α) was higher than (PEA)2PbCl4 (1400 photons/5.5 MeV-α).

Simulation and Optimization of Lead-Based Perovskite Solar Cells with Cuprous Oxide as a P-type Inorganic Layer

The hole transporting material (HTM) is responsible for selectively transporting holes and blocking electrons which also plays a crucial role in the efficiency and stability of perovskite solar cells (PSCs). Spiro-MeOTAD is the most popular material, which is expensive and can be easily affected by moisture content. There is a need to find an alternative HTM with sufficiently high resistance to moisture content. In this paper, the influence of some parameters with cuprous oxide (Cu2O) as HTM was investigated using a solar cell capacitance simulator (SCAPS). These include the influence of doping concentration and thickness of the absorber layer, the effect of thickness of ETM and HTM as well as electron affinities of ETM and HTM on the performance of the PSCs. From the obtained results, it was found that the concentration of dopant in the absorber layer, the thickness of ETM and HTM and the electron affinity of HTM and ETM affect the performance of the solar cell. The cell performance improves greatly with the reduction of ETM electron affinity and its thickness. Upon optimization of parameters, power conversion efficiency for this device was found to be 20.42% with a current density of 22.26 mAcm-2, voltage of 1.12 V, and fill factor of 82.20%. The optimized device demonstrates an enhancement of 58.80%, 2.25%, 20.40% and 30.23% in PCE, Jsc, FF, and Voc over the initial cell. The results show that Cu2O in lead-based PSC as HTM is an efficient system and an alternative to spiro-MeOTAD.

Endogenous Organic–Inorganic Hybrid Interface for Reversible Zn Electrochemistry

AbstractDespite rechargeable aqueous Zn‐ion batteries (AZIBs) exhibit advantages such as high safety, high specific energy, and low cost, etc, the implementation of Zn anodes is still hampered by insufficient cyclability and grievous side reactions. To improve the cycling stability of the zinc anode, a stable zinc anode/electrolyte interface is needed to suppress dendrite formation and side reactions. Herein, a self‐regulating endogenous organic–inorganic hybrid interface layer (EHI) in situ on the surface of the Zn anode by regulating solvent molecules is constructed. The EHI consists of an organic outer layer containing N─H and ─CH3 and an inorganic inner layer containing ZnO and ZnCO3, which effectively inhibits hydrogen evolution and dendrite growth. Consequently, AZIBs with the EHI achieve a lifespan exceeding 5500 h in 3 mA cm−2, and stripping/plating on copper foils for 600 cycles with an average coulomb efficiency (CE) of 99.47%. This study provides a feasible idea for realizing stable and reversible zinc‐ion batteries.

Internal Ceramic Protective Coating of Hollow‐Core Fibers

To optimize the use of hollow‐core photonic crystal fibers (HC‐PCF), their cores are filled with an atomic gas for an ultra‐enhanced interaction with an incident laser beam in applications such as atomic vapor microcells. One challenge in these gas‐filled HC‐PCFs is to control the physiochemical interactions between the gas medium and the silica inner surface of the fiber core surround. In this work, thus, the processing of ceramic coatings on glass substrates by chemical solution deposition is focused on. Also, the successful implementation of an original coating procedure for a deposition inside hollow‐core fibers with complex microstructures is described. It is indeed possible to form a thin, dense, inorganic, and amorphous layer with a low thickness, low roughness, and high transparency. To obtain such a result, several parameters must be controlled, including the concentration of the solution, the technique and the deposition time, as well as the heat treatment undergone by the fiber. In particular, the selected aluminosilicate coatings, which are nonporous and present a 20–30 nm thickness, demonstrate a considerable improvement of the lifetime properties of the fibers filled with rubidium vapor, without modifying its original guiding properties.

Artificial Hydrophilic Organic and Dendrite-Suppressed Inorganic Hybrid Solid Electrolyte Interface Layer for Highly Stable Zinc Anodes.

Aqueous zinc-ion batteries (AZIBs) have gained significant attentions for their inherent safety and cost-effectiveness. However, challenges, such as dendrite growth and anodic corrosion at the Zn anode, hinder their commercial viability. In this paper, an organic-inorganic coating layer (Nafion-TiO2) was introduced to protect the Zn anode and electrolyte interface. Briefly, Nafion effectively shields against the corrosion from water molecules through the hydrophobic wall of -CF3 and guided zinc deposition from the -SO3 functional group, while TiO2 particles with a higher Young's modulus (151 GPa vs 120 GPa from Zn metal) suppress the zinc dendrite formation. As a result, with the protection of Nafion-TiO2, the symmetrical Zn∥Zn battery shows an improved cycle life of 1,750 h at 0.5 mA cm-2, and the full cell based on Zn∥MnO2 shows a long cycle life over 1,500 cycles at 1 A g-1. Our research offers a novel approach for protecting zinc metal anodes, potentially applicable to other metal anodes such as those in lithium and sodium batteries.

High-Safety Electrolytes with an Anion-Rich Solvation Structure Tuned by Difluorinated Cations for High-Voltage Lithium Metal Batteries.

As next-generation energy storage devices, lithium metal batteries (LMBs) must offer high safety, high-voltage resistance, and a long life span. Electrolyte engineering is a facile strategy to tailor the interfacial chemistry of LMBs. In particular, the solvation structure and derived solid electrolyte interphase (SEI) are crucial for a satisfactory battery performance. Herein, a novel middle-concentrated ionic liquid electrolyte (MCILE) with an anion-rich solvation structure tuned by difluorinated cations is demonstrated to achieve ultrahigh safety, high-voltage stability, and excellent ternary-cathode compatibility. Novel gem-difluorinated cations first synthesized for prestoring fluorine on positively charged species, not only preferentially adsorb in the inner-Helmholtz layers, but also participate in regulating the Li+ solvation structure, resulting in a robust interphase. Moreover, these weak interactions in the Li+ solvation structure including anion-solvent and ionic liquid (IL) cation-solvent pairs are first revealed, which are beneficial for promoting an anion-dominated solvation structure and the desolvation process. Benefiting from the unique anion-rich solvation structure, a stable hetero-SEI structure is obtained. The designed MCILE exhibits compatibility with Li metal anode and the high-voltage ternary cathode at high temperatures (60°C). This work provides a new approach for regulating the solvation structure and electrode interphase chemistry of LMBs via difluorinated IL cations.