Organic-inorganic composite quasi-solid electrolyte, lithium ion battery and preparation method

Abstract

The invention relates to the technical field of lithium batteries, in particular to an organic-inorganic composite quasi-solid electrolyte, a lithium ion battery and a preparation method. The invention relates to a preparation method of an organic-inorganic composite quasi-solid electrolyte. The preparation method comprises the following steps: firstly, carrying out ultrasonic dispersion on ionic liquid and an organic solvent dissolved with lithium salt according to a volume ratio of (0.8-1.2): 1 to obtain a composite organic electrolyte; then, inorganic ion conductor nanoparticles are introduced, so that the solid content of a mixed system is 2.0-3.0 g / mL, and a colloidal precursor is formed through grinding and / or planetary / high-shear dispersion; and then carrying out vacuum defoaming and standing for shaping to obtain the room-temperature quasi-solid gel. According to the system, coordination of organic phase continuous conduction and inorganic framework morphology supporting is achieved, the interface is compact, dendritic crystals are inhibited, wide-temperature stability and safety are improved, technological parameters are clear, and large-scale copying is facilitated.

Description

Technical Field

[0001] This invention relates to the field of lithium battery technology, and more particularly to an organic - Inorganic composite quasi-solid-state electrolyte, lithium-ion battery, and preparation method. Background Technology

[0002] Lithium-ion batteries widely employ liquid electrolyte systems, which, while possessing high ionic conductivity, still have shortcomings in thermal stability, safety, and wide-temperature operation. To address these issues, existing technologies have proposed combining inorganic ionic conductor nanoparticles with organic phases containing ionic liquids to construct organic... - Inorganic "quasi-solid-state" electrolytes are developed to balance conductivity and safety.

[0003] For example, existing patent documents with publication numbers CN112467194A / CN112467194B (hereinafter referred to as Document 1) disclose an organic - The inorganic composite quasi-solid-state electrolyte and quasi-solid-state lithium battery are composed of "inorganic ion-conducting nanoparticles and composite organic electrolyte": the composite organic electrolyte is formed by uniformly mixing an organic solvent containing lithium salt with an ionic liquid, and the types of anions and cations of the ionic liquid are specified. The literature also points out that the organic phase and inorganic phase can synergistically form multiple ion conduction channels in solid / liquid / interface layers, thereby improving room temperature conductivity, and provides an example of a window of ionic liquid to organic solvent volume ratio (0.8–1.2):1, as well as the idea of ​​achieving gelation through physical action in the examples.

[0004] However, from the perspective of manufacturing repeatability and scalability, the aforementioned prior art still has several areas where process parameters and quality control procedures are not clearly defined. For example, this literature focuses more on the description of mass fractions (e.g., "organic phase 30–40 wt%, inorganic phase 60–70 wt%)" and formulation framework, without providing clear and directly reproducible parameterized limits for dispersion methods and intensity (whether ultrasonic or planetary dispersion), dispersion time limits, and volume-based solids control (expressed in g / mL). Furthermore, the process conditions for reducing microbubbles / agglomeration and stabilizing viscoelastic networks, such as degassing and static settling, lack quantitative description. These deficiencies may lead to batch-to-batch consistency fluctuations, unstable morphology and phase behavior at low / high temperatures, and difficulty in controlling interfacial impedance rise in high-solids colloidal systems, thus affecting the stability and yield during large-scale production. Summary of the Invention

[0005] The purpose of this invention is to provide an organic solution that addresses the shortcomings of existing technologies. -The inorganic composite quasi-solid-state electrolyte, lithium-ion battery, and preparation method aim to establish a clear and reproducible set of process parameters and process control schemes based on the existing system. This will enable the obtained quasi-solid-state electrolyte to maintain high ion conductivity while reducing the consistency risk caused by microbubbles / agglomeration, and to maintain a relatively stable structure and interface state under low and high temperature conditions, thereby improving the repeatability of mass production and application stability.

[0006] This invention achieves the above objectives through the following technical solution: an organic - The preparation method of inorganic composite quasi-solid electrolyte includes the following steps: Preparation steps of ionic liquid: Select at least one of quaternary ammonium salt, quaternary phosphonium salt, imidazole salt or pyrrole salt as the cation, and react it with bis(trifluoromethanesulfonyl)imide (TFSI). - ), trifluoromethanesulfonate (OTf) - ), hexafluorophosphate (PF6) - ), tetrafluoroborate (BF4) - ) or bis(fluorosulfonyl)imide (DFSI) - At least one of the following can be used as an anion to pair with other ions to obtain an ionic liquid; Electrolyte preparation step: The ionic liquid obtained in the ionic liquid preparation step is mixed with an organic solvent containing lithium salt at a volume ratio of 0.8 to 1.2:1 (v / v) and ultrasonically dispersed to form a composite organic electrolyte; Inorganic composite step: The inorganic ion conductor nanoparticles are mixed with the composite organic electrolyte from the electrolyte preparation step, such that the solid content (based on the total volume of the mixed system) of the inorganic ion conductor nanoparticles in the mixed system is 2.0–3.0 g / mL. The mixture is then ground and / or dispersed by planetary or high-shear dispersion, allowing the composite organic electrolyte to coat and penetrate the surface and pores of the inorganic ion conductor nanoparticles, resulting in a colloidal organic electrolyte. - Inorganic composite quasi-solid electrolyte precursor; wherein, the planetary dispersion can be achieved by a combination of rotation and revolution dispersion using a dual planetary mixer or a planetary centrifugal stirrer for degassing; preferably, the rotation speed is 300. - 2000 rpm, time 0.5 seconds - Simultaneous degassing can be performed under a vacuum of -0.08MPa for 3 hours (optional). Degassing and solidification step: The precursor obtained in the inorganic composite step is degassed and allowed to stand for curing and solidification to stabilize the micro-interface and viscoelastic network, thereby obtaining an organic... - Inorganic composite quasi-solid electrolyte.

[0007] Furthermore, the ultrasonic dispersion time in the electrolyte preparation step is not less than 1 hour; In the ionic liquid preparation step, the cation is an imidazole salt ion or a pyrrole salt cation; In the ionic liquid preparation step, the anion is bis(trifluoromethanesulfonyl)imide (TFSI). - ) or bis(fluorosulfonyl)imide (DFSI) - ); In the electrolyte preparation step, the ionic liquid and the organic solvent containing the lithium salt are mixed at a volume ratio of 0.9–1.1:1. Specifically, limiting the lower limit of ultrasonic dispersion time to no less than 1 hour ensures that the energy input in the liquid phase reaches a reproducible level, reducing microbubble nuclei and phase separation caused by insufficient dispersion between batches; while narrowing the volume ratio to 0.9–1.1:1 makes the initial viscosity and solvation environment more consistent across different equipment and batches. Imidazole / pyrrole cations and bis(trifluoromethanesulfonyl)imide (TFSI) were selected. - ) / Difluorosulfonamide (DFSI) - The anion combination balances low-temperature ion migration and low volatility, improving the stability of a wide-temperature continuous phase. Compared with the example in Literature 1, which only shows "(0.8–1.2):1" and does not limit the ultrasound duration, this case addresses the key uncertainties in amplified reproduction by narrowing the ratio and setting a lower time limit, thereby improving consistency and the stability of the initial state of the interface.

[0008] Furthermore, in the inorganic composite step, the solid content of the inorganic ionic conductor nanoparticles in the mixed system is 2.3–2.7 g / mL; the inorganic composite step is carried out by grinding in a mortar and pestle, and the grinding time is not less than 1 hour; The degassing and setting step includes: degassing the precursor and then letting it stand for at least 1 hour to complete the setting. The organic obtained after the defoaming and setting step - The inorganic composite quasi-solid electrolyte is in a quasi-solid gel state; The inorganic ionic conductor nanoparticles are nanoscale particles used to provide an inorganic framework for surface coating and pore penetration. Specifically, limiting the solid content to g / mL (volume basis) and narrowing it to 2.3–2.7 directly constrains the viscosity and coatability of the high-solids-content system, making it easier to form a continuous network for coating and pore penetration. Setting a lower limit for the grinding time helps to fully wet and deagglomerate. Defining "debubbling and settling" as continuous steps removes residual microbubbles and completes the self-consistent rearrangement of the viscoelastic network, resulting in a stable quasi-solid gel state at room temperature. Compared with the first literature which describes the content as a percentage of 60–70 wt.% without providing quantitative constraints on "volume solids content, dispersion time, and debubbling / settling sequence", this application improves the morphological stability and interfacial density control during scale-up manufacturing through volumetric aperture and sequential processes.

[0009] An organic -An inorganic composite quasi-solid-state electrolyte, which is a colloidal composite material consisting of inorganic ion-conducting nanoparticles and a composite organic electrolyte, wherein: The composite organic electrolyte is prepared by uniformly mixing an ionic liquid with an organic solvent containing lithium salt at a volume ratio of 0.8 to 1.2:1. The inorganic ion conductor nanoparticles are dispersed in the composite organic electrolyte and are coated and penetrated by the composite organic electrolyte. The solid content of the inorganic ion conductor nanoparticles in the electrolyte is 2.0 to 3.0 g / mL. The electrolyte exists in a quasi-solid gel state at room temperature. Specifically, the composition and morphology are defined by volume ratio and volumetric solid content in the product claims, which can transform the "process input" into the objective features of the "structural output": when the solid content and ratio fall within the stated window, the system is more likely to form a continuous phase that coats and penetrates and maintains a room-temperature gel state, thereby providing a stable morphology for the coverage and filling of the electrode interface. Unlike the wt.% ratio used in the literature, this application uses volumetric caliber to locate the viscoelastic and rheological range that can be reproduced on the production line, which facilitates product sampling and consistency determination (e.g., internal control of appearance, thickness, and EIS / DSC thresholds).

[0010] Furthermore, the ionic liquid is composed of at least one cation selected from quaternary ammonium salts, quaternary phosphonium salts, imidazole salts, or pyrrole salts and bis(trifluoromethanesulfonyl)imide (TFSI). - ), trifluoromethanesulfonate (OTf) - ), hexafluorophosphate (PF6) - ), tetrafluoroborate (BF4) - ) or bis(fluorosulfonyl)imide (DFSI) - It is formed by pairing at least one anion from the ionic liquid. Specifically, the cation / anion set is defined, and by combining it with the volume ratio and volume solid content, the target structure of interfacial wetting and wide-temperature continuous phase can still be obtained under different ionic liquid selections.

[0011] Furthermore, the inorganic ion conductor nanoparticles are oxide or sulfide solid electrolyte nanoparticles with a particle size in the nanometer range and forming a porous structure for the composite organic electrolyte to penetrate. The electrolyte is used in lithium-ion batteries to replace traditional liquid electrolytes. Specifically, by using oxides and sulfides as replaceable frameworks and emphasizing the penetration of nanoscale pores, the interfacial contact area and morphological support of different systems can be considered without changing the main formulation. Combined with the volume solids content window, the product is more likely to form a continuous coverage in the electrode pores and reduce free solvent retention, which is of direct significance for improving wide-temperature cycling stability and safety margin. Compared with the material listing in Reference 1, this case solidifies and defines the microstructure characteristics (penetration / pores) and the controllable parameters of the production line (volume solids content) together, improving feasibility and verifiability.

[0012] A lithium-ion battery, comprising a positive electrode, a negative electrode, and a separator, wherein an organic compound as described in any one of claims 4 to 6 is disposed between the positive and negative electrodes. - Inorganic composite quasi-solid electrolyte.

[0013] Furthermore, the positive electrode active material is selected from at least one of lithium iron phosphate, lithium nickel cobalt manganese oxide, or lithium nickel cobalt aluminum oxide; The negative electrode active material is selected from at least one of graphite, hard carbon, soft carbon, or silicon-based carbon composite materials; The diaphragm is a polyolefin microporous membrane or a membrane coated on its surface; The lithium-ion battery has a pouch, cylindrical, or square casing structure.

[0014] A method for preparing a lithium-ion battery includes the following steps: Preliminary steps: Prepare a stack or winding of battery cells containing positive electrode plates, negative electrode plates and separators; Electrolyte preparation steps: Prepare organic electrolyte according to the method of any one of claims 1 to 3. - Inorganic composite quasi-solid electrolyte; Assembly steps: Place the organic... - An inorganic composite quasi-solid electrolyte is applied between the positive electrode and the negative electrode and contacts the membrane, so that it covers the surface of the electrode active layer and fills its gaps. Finished product steps: After the assembly steps are completed, the battery cell is degassed and sealed under vacuum or reduced pressure conditions, followed by formation and capacity testing to obtain the finished lithium-ion battery. Specifically, the concept of "degassed and statically settling" of the electrolyte is transferred to the battery cell assembly. First, entrained air bubbles are eliminated by vacuum / reduced pressure, and then sealed for formation, which can reduce initial impedance fluctuations and polarization unevenness. During assembly, the goal is to cover and fill gaps, so that the gel forms continuous channels in the electrode pores, improving interfacial contact.

[0015] Furthermore, in the assembly step, the electrolyte is applied by coating, scraping, dispensing, or injection, and the thickness of the applied layer is 50–500 μm; The degassing process in the finished product step is carried out for 10 to 30 minutes under a vacuum of -0.08 MPa to -0.095 MPa; the formation process is carried out at room temperature, and in the early stage of formation, a constant current or constant current and constant voltage method is used to start at a low rate, and then the process is switched to a conventional rate charge and discharge program.

[0016] The beneficial effects of this invention are: This invention maintains the stability of the structure and performance of quasi-solid electrolytes during scale-up manufacturing by parameterizing material ratios and key processes. First, an ionic liquid and an organic solvent containing a lithium salt are mixed at a volume ratio of 0.8–1.2:1 and ultrasonically dispersed to form a composite organic electrolyte. The viscosity and flowability of the liquid phase are directly controlled by volume-based proportions, ensuring similar initial rheological states for different equipment and batches under the same volume conditions. This facilitates maintaining uniform wetting and a continuous phase when increasing solid content. Ultrasonic dispersion achieves initial homogenization and breaks down microbubble nuclei in the liquid phase, reducing the risk of gas entrainment in the high-solid-content composite stage.

[0017] In the inorganic composite process, the solid content of inorganic ion-conducting nanoparticles was controlled at 2.0–3.0 g / mL based on the total volume of the mixed system, using grinding and / or planetary dispersion or high-shear dispersion. The expression and control of volumetric solid content are directly related to the establishment of the final viscoelastic network. Within this range, the interparticle spacing and the volume fraction of the organic phase are in a region conducive to the formation of continuous coating and pore penetration. Planetary or high-shear dispersion provides the energy input for rotation / revolution or strong shear, effectively breaking down the aggregates and achieving sufficient surface wetting, thereby establishing a stable organic / inorganic interface and interconnected ion conduction channels at the microscopic level. Compared with the approach of describing only by mass fraction, controlling the window of volumetric solid content makes it easier to obtain consistent macroscopic rheological and microscopic filling states in different containers and under different temperature and humidity environments, thereby reducing batch-to-batch variability.

[0018] Following precursor formation, a series of degassing and settling steps are implemented. First, microbubbles entrained during dispersion are removed using vacuum or reduced pressure. Then, settling completes the self-consistent rearrangement of the viscoelastic network and secondary interfacial wetting. This sequence eliminates anomalies in local electric and thermal fields, allowing the colloidal structure to achieve a stable morphology at room temperature. The electrode / electrolyte contact surface remains continuous, and interfacial impedance fluctuations in the early stages of cycling are suppressed. This treatment is equally effective for both low- and high-temperature conditions: at low temperatures, the low vapor pressure and low glass transition temperature of the ionic liquid maintain the continuity of the organic phase, while at high temperatures, the inorganic framework provides morphological support to prevent network collapse. Together with the aforementioned process, these factors ensure that the electrolyte maintains the continuity of its conductive channels and interfacial stability over a wide temperature range.

[0019] From a manufacturing perspective, the ultrasonic, grinding / planetary or high-shear dispersion, vacuum degassing, and static shaping methods employed in this invention are all physical unit operations commonly used on existing assembly lines, eliminating the need for specialized processes such as photo / thermal curing. Combined with windowed management of volume ratio and volumetric solids content, and the setting of a lower limit for dispersion time, a clear correspondence is established between process inputs (energy, time, vacuum level) and morphological outputs (colloidal state, no obvious flow, continuous coating). Standard operating procedures (SOPs) can be directly established based on this, ensuring consistency and yield after scaling up. Simultaneously, the low volatility and flame-retardant properties of the ionic liquid, combined with the physical barrier effect of the inorganic nanoframework on dendrites, enhance the intrinsic safety of the electrolyte and the operational safety boundary of the battery cell while maintaining structural and interface stability.

[0020] In summary, this invention establishes a process control framework that can be replicated on different production lines without changing the existing material routes, through a complete set of parameterized processes including "a composite organic electrolyte with a volume ratio of 0.8 to 1.2:1, an inorganic composite with a volume solid content of 2.0 to 3.0 g / mL, planetary / high shear dispersion energy input, degassing and static stabilization". This ensures the stability of the morphology and interface state of the quasi-solid electrolyte, the continuity of ion conduction channels, and the simultaneous guarantee of wide-temperature operation and safety. Detailed Implementation

[0021] The technical solutions of the present invention will be clearly and completely described below with reference to the embodiments of the present invention. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those of ordinary skill in the art without creative effort are within the scope of protection of the present invention.

[0022] Therefore, embodiments of this application provide an organic - The present invention relates to an inorganic composite quasi-solid-state electrolyte and its preparation method, as well as a lithium-ion battery and its preparation method. The aim is to improve the thermal stability and mechanical support of the system while maintaining high ionic conductivity, and to suppress lithium dendrite growth, thereby improving the battery's safety and wide temperature adaptability. The electrolyte is a colloidal composite consisting of inorganic ionic conductor nanoparticles and a composite organic electrolyte. The composite organic electrolyte is formed by uniformly mixing an ionic liquid with an organic solvent containing dissolved lithium salts, and coats and penetrates the surface and pores of the inorganic ionic conductor nanoparticles.

[0023] The preparation process of this invention includes the preparation of ionic liquid, the formation of composite organic electrolyte, and organic... - The process involves inorganic compounding and degassing / sizing steps. First, at least one of quaternary ammonium salts, quaternary phosphonium salts, imidazole salts, or pyrrole salts is selected as the cation, and reacted with bis(trifluoromethanesulfonyl)imide (TFSI). - ), trifluoromethanesulfonate (OTf)- ), hexafluorophosphate (PF6) - ), tetrafluoroborate (BF4) - ) or bis(fluorosulfonyl)imide (DFSI) - At least one of the following is used as an anion pairing to obtain an ionic liquid. Subsequently, the ionic liquid is mixed with an organic solvent containing a lithium salt at a volume ratio of 0.8–1.2:1 (v / v), and dispersed under ultrasonic conditions for at least 1 hour to homogenize the system and form a composite organic electrolyte. Next, inorganic ionic conductor nanoparticles are gradually added to the composite organic electrolyte. By weighing and volume conversion, the solid content of the inorganic particles in the mixed system (based on the total volume of the mixed system) is controlled at 2.0–3.0 g / mL. The mixture is then continuously treated by grinding and / or dispersion for at least 1 hour to ensure that the composite organic electrolyte fully coats and penetrates the surface and pores of the inorganic particles, resulting in a colloidal organic electrolyte. - Inorganic composite quasi-solid electrolyte precursor. Finally, the precursor was subjected to vacuum degassing and static settling to obtain a stable quasi-solid electrolyte product.

[0024] Compared with traditional liquid electrolyte systems, the organic electrolyte system of this invention... - Inorganic composite quasi-solid-state electrolytes have significant advantages in the following aspects: Firstly, safety is improved: the ionic liquid introduced into the composite organic electrolyte has low vapor pressure and flame-retardant properties, and the inorganic nanoframework provides mechanical support and forms a physical barrier to lithium dendrite growth at the microscopic level, which helps to reduce the risk of internal short circuits and thermal runaway.

[0025] Secondly, it has a wider temperature adaptability: ionic liquids still have good ion migration ability at low temperatures, and the inorganic framework maintains structural stability at high temperatures. The two work together to enable the electrolyte to maintain a relatively stable conduction channel under both low and high temperature conditions.

[0026] Thirdly, it balances conductivity and interfacial performance: the composite organic electrolyte provides a continuous ion transport phase, while the wetting and space charge layer effect on the surface and interface of inorganic particles are beneficial for promoting Li... + Migration enables the overall conductivity to be superior to that of a single inorganic solid system, while also making it easier to form good contact with the electrode.

[0027] Fourth, the process is feasible and scalable: the method can be completed using conventional processes such as ultrasonication, grinding / dispersion and vacuum degassing, without relying on high-temperature sintering or special atmospheres, and is easy to integrate with existing cell assembly processes.

[0028] In summary, this invention significantly improves the safety and environmental adaptability of electrolytes without sacrificing ionic conductivity by constructing a quasi-solid-state system composed of a composite organic phase and an inorganic nanoframework, and has good prospects for industrial application.

[0029] Specifically, this invention provides an organic - An inorganic composite quasi-solid-state electrolyte comprises inorganic ion-conducting nanoparticles and a composite organic electrolyte encapsulated and solidified on the surface of the inorganic ion-conducting nanoparticles; the composite organic electrolyte is formed by uniformly mixing an organic solvent containing a lithium salt with an ionic liquid. The specific preparation steps are as follows: S1, add one of the following anions: bis(trifluoromethanesulfonyl)imide, trifluoromethanesulfonic acid, hexafluorophosphate, tetrafluoroboric acid, or bis(trifluoromethanesulfonyl)imide.

[0030] S2, which is formed by adding one of the following cations: quaternary ammonium salt ion, quaternary phosphorus salt ion, imidazole salt ion, and pyrrole salt cation, to the anion.

[0031] S3. Mix the prepared ionic liquid with an organic solvent containing lithium salt at a volume ratio of (0.8-1.2):1. This ratio is the best ratio for the overall performance of the composite organic electrolyte. Stir with an ultrasonic device for more than one hour to ensure that the different components are mixed evenly to obtain the organic liquid composition.

[0032] S4. Place the solid electrolyte nanoparticles in a mortar and grind them for a specified time to ensure that the liquid phase component is uniformly dispersed in the solid phase, thereby obtaining a gel-like composite quasi-solid electrolyte. The ratio of the solid electrolyte nanoparticles to the organic phase component can be 2.0–3.0 g / mL. The grinding time can be at least 1 hour to ensure that the composite quasi-solid electrolyte is a gel-like complex.

[0033] Organic in existing technology - Inorganic composite electrolytes all contain polymer components, while the organic components of this invention... - Inorganic composite quasi-solid-state electrolytes are special electrolyte materials that effectively prevent the formation of lithium dendrites, thereby avoiding short circuits caused by the battery puncturing the separator during use. Furthermore, the lithium-ion battery of this invention can achieve high-efficiency charging and discharging under both low and high temperature environments, exhibiting stronger temperature adaptability than existing lithium-ion batteries. In detail, the improvements made to the existing technology in this invention are analyzed as follows: 1. This invention employs ionic liquids and organic solvents containing lithium salts to form a composite organic electrolyte, which is then combined with inorganic ionic conductor nanoparticles to obtain a quasi-solid-state system. Under this configuration, the procurement, storage, and control of curing side reactions of photo / thermal curing monomers and initiators are not involved. This reduces the use of one type of polymer reactive raw material in the material list; when the unit price and proportion of the ionic liquid are within a controllable range (see the volume ratio window below), the sources of material costs become clearer, facilitating cost optimization through large-scale procurement of common battery-grade solvents and lithium salts.

[0034] 2. The preparation process employs conventional physical unit operations such as ultrasonic dispersion, grinding and / or planetary dispersion, vacuum degassing, and static setting, without introducing dedicated photo / thermal curing sections or inert atmosphere curing sections. This approach has high equipment compatibility with existing electrolyte / slurry processes, and the transition can be completed within existing production lines through process timing and cycle time coordination, reducing the need for additional equipment and maintenance points. The static setting facilitates the physical formation of the gel structure; when production line cycle time is limited, the setting time can be shortened by improving planetary dispersion efficiency or using thin-layer spreading, thus achieving cycle time matching without altering the system's chemical composition.

[0035] 3. To reduce gas entrainment and agglomeration in high-viscosity systems, this invention defines two windows that directly affect rheology and dispersion: first, the volume ratio of the ionic liquid to the organic solvent containing the lithium salt is controlled at 0.8–1.2:1 (v / v); second, the solid content of inorganic nanoparticles in the composite mixture (based on the total volume of the mixture) is controlled at 2.0–3.0 g / mL. These windows, combined with a minimum dispersion / grinding time of at least 1 hour and subsequent vacuum degassing, can generally reduce the probability of microbubble residue and large particle agglomerates, thereby reducing the hidden costs associated with rework and retesting. It should be noted that when the solid content is close to the upper limit, the system viscosity may still be relatively high; in this case, segmented feeding and intermittent dispersion can maintain operability.

[0036] 4. The introduction of ionic liquids into composite organic electrolytes commonly results in low vapor pressure and low glass transition temperature. At low temperatures, this characteristic helps maintain the continuity of the organic phase and reduces the damage to ion migration channels caused by solvent crystallization. Inorganic ionic conductor nanoparticles provide skeletal constraints within the system, forming morphological support for the gel network. During heating or long-term storage, this support helps reduce the probability of network collapse and phase separation. The coating and infiltration during the composite process increase the contact area between the organic and inorganic phases, and the rate of increase in interfacial impedance is usually more controllable in the early stages of cycling. These mechanisms can be observed and quantified through differential scanning calorimetry (DSC) of phase behavior in the -40 to 120 °C range and through changes in electrochemical impedance spectroscopy (EIS) at room temperature and low temperatures.

[0037] 5. This invention explicitly defines the key ratio (0.8–1.2:1), solid content (2.0–3.0 g / mL), minimum dispersion / grinding time (not less than 1 hour), and the sequence of vacuum degassing combined with static settling as process parameters. This explicit specification facilitates the formation of standard operating procedures (SOPs) and establishes a one-to-one correspondence with equipment settings (speed, time, vacuum level). By directly replicating the above parameters on different production lines, batch-to-batch consistency fluctuations caused by implicit experience differences can be reduced.

[0038] 6. In the mass production release stage, a combination of morphological and functional indicators can be used as the criteria: For morphology, whether it is a stable gel state, whether flow occurs, and the continuity of coating are used for rapid appearance evaluation; for functionality, EIS (once at 25℃ and once at -20℃) and DSC (scanned from -40℃ to 120℃) are used as the basic thresholds for warehousing, combined with the conductivity obtained from equivalent circuit fitting and the presence or absence of phase transition peaks as objective judgment criteria. These judgment criteria do not change the formulation itself, but provide measurable target values ​​for large-scale reproducibility, facilitating the backtracking and correction of abnormal batches.

[0039] 7. In terms of materials, eliminating the polymerization-reaction-based curing system and using ionic liquids and common battery-grade solvents / lithium salts to form a composite organic phase helps reduce the complexity of the raw material system. In terms of process, replacing chemical curing with physical setting and limiting the proportion and solid content window improves the operability of dispersion and degassing. In terms of structure, utilizing the low-temperature continuity of the organic phase and the morphological constraints of inorganic ionic conductor nanoparticles as a framework achieves synergistic maintenance of conduction channels and interfaces. The above three aspects work together in the same process, improving safety, temperature adaptability, and consistency without changing the overall framework of cell assembly. It should be noted that the final material cost is closely related to the selection and procurement scale of the ionic liquid, and the production line cycle time is also affected by the settling time; therefore, this invention provides a set of feasible formulations, processes, and criteria combinations to achieve target balance through parameter optimization in actual production.

[0040] It should be noted that: Ionic liquids refer to salts formed by organic cations and paired anions, which are liquid at or near room temperature, and possess low vapor pressure and high ionic conductivity. Composite organic electrolytes refer to homogeneous conductive phases formed by mixing ionic liquids and organic solvents containing lithium salts in a volume ratio and then ultrasonicating. Inorganic ionic conductor nanoparticles refer to inorganic nanoparticles with ionic conductivity, which can be oxides or sulfides, possessing surface / pore structures to facilitate coating and penetration. Solid content (g / mL) is measured based on the total volume of the mixed system, representing the mass of inorganic ionic conductor nanoparticles per unit volume of the mixture. Planetary dispersion employs a combined shear dispersion method involving rotation and revolution, suitable for homogenizing high-viscosity and high-solids-content systems.

[0041] In detail: The organic provided by this invention -An inorganic composite quasi-solid-state electrolyte is prepared by mixing an ionic liquid with an organic solvent containing a lithium salt at a predetermined volume ratio to obtain a composite organic electrolyte. Inorganic ionic conductor nanoparticles are then introduced to achieve a target solid content in the mixture. The composite organic electrolyte is then uniformly coated and penetrated into the particle surface and pores through grinding and / or planetary dispersion to form a gel-like precursor. Finally, the quasi-solid-state electrolyte is obtained after degassing and settling. To ensure reproducibility, the purity, proportions, time, temperature, environmental humidity control, degassing method, and testing items and criteria are clearly specified in the following examples. Unless otherwise stated, all experiments were conducted in a dry environment at (25±2)℃ and relative humidity ≤30%. All glassware and containers were pre-dried in a 120℃ oven for 2 hours and cooled to room temperature before use.

[0042] Example 1: (Ultrasonic dispersion and mortar grinding process) To prepare the composite organic electrolyte, an ionic liquid and an organic solvent containing dissolved lithium salt were first added to a dry three-necked flask, with the volume ratio controlled at 1.0:1 (v / v). The ionic liquid consisted of an imidazole salt cation and bis(trifluoromethanesulfonyl)imide (TFSI). - The lithium salt was obtained by anion pairing; the organic solvent containing the lithium salt was a conventional electrolyte solvent system mainly composed of carbonates (e.g., a mixed solvent containing ethylene carbonate EC and diethyl carbonate DEC), wherein the lithium salt was selected from commonly used battery-grade lithium salts (e.g., LiPF6 or LiTFSI) to ensure the reproducibility of the subsequent description. After mixing, the flask was placed in an ultrasonic cleaning tank and continuously ultrasonically dispersed at room temperature for 1 hour; the transparency and bubble status of the system were observed during the first 10 minutes of ultrasonication, and the liquid exchange was assisted by slightly rotating the flask if necessary. At the end of ultrasonication, the system was visually inspected to confirm that it was homogeneous and that there were no obvious phase separations or unmixed streaks, and the subjective change in viscosity (usually a slight increase) was recorded.

[0043] Then organic - Inorganic composite. Weigh inorganic ionic conductor nanoparticles (oxide or sulfide solid electrolyte nanoparticles are acceptable; oxide nanoparticles are used in this embodiment) and slowly add them to the above-mentioned composite organic electrolyte in small, multiple additions, stirring with a glass rod to prevent instantaneous agglomeration. Through gradual addition and volume conversion, the solid content of inorganic nanoparticles in the mixture (based on the total volume of the mixture) reaches 2.5 g / mL. After the target solid content is achieved, transfer the mixture to a large agate mortar and grind it at a uniform speed and in the same direction for at least 1 hour. During grinding, scrape off the material from the mortar wall every 10-15 minutes and stir to continuously update the shear surface of the system. At the end of grinding, the material should appear as a uniform, continuous paste or gel, without dry powder or obvious large gel lumps. The scraper marks should be fine and continuous, indicating that the organic phase has fully coated and penetrated into the surface and pore structure of the nanoparticles, forming a gel-like organic...- Inorganic composite quasi-solid-state electrolyte precursor.

[0044] Immediately after obtaining the precursor, degassing and setting were performed. The precursor was placed in a degassing vessel equipped with a vacuum valve and evacuated to a vacuum of -0.08 MPa to -0.095 MPa without heating, maintaining this vacuum for 15–30 minutes. During this period, bubbles should be observed continuously precipitating and gradually decreasing until they essentially cease to appear in the viewing window. After venting to atmospheric pressure, the sample was spread onto a polytetrafluoroethylene (PTFE) substrate to form a thin layer approximately 300–500 μm thick. This layer was then placed in a clean, dust-free environment with a relative humidity ≤30% and allowed to stand for at least 1 hour to complete the setting process. The set sample was collected in slice form and placed in a sealed aluminum bag for later use. The sample should be a stable quasi-solid gel at room temperature, able to be lifted as a whole with tweezers without flowing, and its morphology should slowly rebound after the pressure is released, indicating a stable viscoelastic network.

[0045] To characterize feasibility and performance stability, basic tests were performed on the above samples: room temperature ionic conductivity was measured using electrochemical impedance spectroscopy (EIS, test frequency range 1MHz~1Hz, small signal 10mV); differential scanning calorimetry (DSC) was used to observe the phase behavior of the samples in the range of -40~120℃ to observe whether there were significant solvent crystallization or phase separation signals; and interfacial contact and initial internal resistance were evaluated using a standard electrode / separator stacking method (positive electrode / electrolyte sample / negative electrode). The test results were used to confirm the consistency between the process window and the sample morphology.

[0046] Example 2: (Ultrasonic dispersion and planetary dispersion process) To reduce human-induced fluctuations introduced by manual grinding and improve the uniformity of high-solids systems, the inorganic composite step was replaced with planetary dispersion while keeping the electrolyte preparation steps unchanged. Specifically, after mixing the ionic liquid and an organic solvent containing lithium salt at a ratio of 1.0:1 (v / v) and sonicating for 1 hour, inorganic ionic conductor nanoparticles were directly added to a vacuum-compatible planetary dispersion container. The solids content of the mixture was adjusted to 2.4–2.6 g / mL through weighing and volume conversion. The container was then mounted on a planetary dispersion device, and the rotation / revolution speed was set to the recommended mid-range range. Dispersion was continued for 60–90 minutes. To balance uniformity and temperature rise control, the machine was stopped for 2–3 minutes every 20–30 minutes to assess the adhesion to the slurry walls and collect the material with a scraper before continuing dispersion. After dispersion, the equipment can be directly switched to the vacuum degassing program, pumped to approximately -0.08 MPa and maintained for 10–20 minutes. If the equipment does not have an online degassing function, the material is transferred to a vacuum degassing tank and processed under the same conditions as in Example 1. Then, it is spread on a PTFE substrate in the same manner and allowed to stand for 1–2 hours to complete the shaping process.

[0047] Compared to the mortar and pestle grinding method in Example 1, planetary dispersion can achieve a more uniform microscopic dispersion in a shorter time, especially in high-viscosity systems with a solid content of 2.3–2.7 g / mL, where a smooth and fine colloidal precursor is more easily obtained macroscopically. EIS tests typically show smaller batch-to-batch differences in room temperature conductivity; cross-sectional scanning electron microscopy (images can be presented in the examples in the specification if needed) reveals a more uniform distribution of inorganic particles in the organic phase and smaller aggregate size, which is consistent with improved electrochemical cycling stability.

[0048] Comparative example: (The impact of deviation in proportion and insufficient time) To demonstrate the impact of formulation ratios and processing time on the final performance, the following comparative example was set up. All other conditions were the same as in Example 1.

[0049] Comparative Example A: The volume ratio of ionic liquid to organic solvent containing lithium salt was adjusted to 0.5:1 (v / v), significantly deviating from the range of 0.8–1.2:1 described in this invention. Following the same ultrasonic and grinding process, materials with similar appearances were obtained. However, in EIS testing at -20°C, the sample's low-frequency impedance increased sharply, and the fitted room-temperature conductivity was significantly lower than in Example 1. Simultaneously, the DSC curve showed obvious signs of solvent crystallization in the low-temperature range, indicating that the continuity of the organic phase and the low-temperature conduction channels were disrupted.

[0050] Comparative Example B: The grinding time in the inorganic composite step was shortened to 10 minutes, while other conditions remained the same as in Example 1. The resulting sample showed a small number of coarse particles and discontinuous drag marks in appearance; the EIS-measured equivalent series resistance (ESR) was higher than that of Example 1, with significant differences between samples. These phenomena indicate that insufficient grinding / dispersion time leads to inadequate organic phase coating, and particle agglomeration is not effectively broken up or wetted, affecting the establishment of the conductive network and interface stability.

[0051] As can be seen from the above comparative examples, controlling the volume ratio of ionic liquid to organic solvent containing lithium salt within the range of 0.8 to 1.2:1 (v / v) and ensuring an effective dispersion / grinding process of no less than 1 hour in the inorganic composite step are essential conditions for obtaining a stable quasi-solid gel state with satisfactory conductivity and wide temperature range performance.

[0052] To facilitate experimental reproduction and determine sample compliance, the following routine testing and criteria are explained. Conductivity is measured using an AC impedance meter at (25±2)℃, with a frequency range of 1MHz to 1Hz and an amplitude of 10mV. The sample is pressed or cut into regular sheets, clamped between two inert metal electrodes, and the Nyquist plot is measured. The conductivity is then obtained by fitting an equivalent circuit. Morphological criteria are based on visual inspection and simple tactile feedback: the sample should be able to be lifted as a whole at room temperature without continuous flow; it should slowly spring back after being lightly pressed with a finger. Thermal stability is measured using DSC scanning from -40 to 120℃ at a heating rate of 10℃ / min. The sample should ideally not exhibit significant solvent crystallization / melting endothermic / exothermic peaks during heating. If necessary, a short-term thermal aging test at 60–80℃ in a constant temperature and humidity chamber can be performed to observe morphological retention; alternatively, EIS can be measured again after holding at -20℃ for 2 hours to assess low-temperature conductivity.

[0053] Key points for process scale-up and quality control: When using planetary dispersion instead of mortar grinding for pilot-scale production, attention should be paid to the dual control of material temperature and moisture content. Excessive material temperature will accelerate side reactions; it is recommended to control the material temperature below 40℃ using a combination of intermittent dispersion and external air cooling. Regarding moisture content, ionic liquids, organic solvents, and inorganic particles should all be pre-dried or purchased in low-moisture form before use. The moisture content of the raw materials should be confirmed to be within the allowable range by Karl Fischer titration or equivalent methods. For the degassing process, it is recommended to retain the vacuum degassing step. Even if the equipment has an online degassing function, a static vacuum degassing should be performed before sample formation to remove microbubbles to the maximum extent and stabilize the interface.

[0054] An organic - An inorganic composite quasi-solid-state electrolyte is a colloidal composite consisting of inorganic ionic conductor nanoparticles and a composite organic electrolyte. The composite organic electrolyte is prepared by uniformly mixing an ionic liquid and an organic solvent containing a lithium salt at a volume ratio of 0.8–1.2:1. The inorganic ionic conductor nanoparticles are dispersed in the composite organic electrolyte and are coated and penetrated by it. The solid content of the inorganic ionic conductor nanoparticles in the electrolyte is 2.0–3.0 g / mL. The electrolyte is in a quasi-solid-state gel state at room temperature.

[0055] A lithium-ion battery, comprising a positive electrode, a negative electrode, and a separator, wherein an organic compound as described in any one of the preceding claims is disposed between the positive and negative electrodes. - Inorganic composite quasi-solid electrolyte.

[0056] A method for preparing a lithium-ion battery includes the following steps: Preliminary steps: Prepare a stack or winding of battery cells containing positive electrode plates, negative electrode plates and separators; Electrolyte preparation steps: Prepare organic electrolytes according to any of the preceding methods.- Inorganic composite quasi-solid electrolyte; Assembly steps: Place the organic... - An inorganic composite quasi-solid electrolyte is applied between the positive electrode and the negative electrode and contacts the membrane, so that it covers the surface of the electrode active layer and fills its gaps. Finished product steps: After the assembly steps are completed, the battery cells are degassed and sealed under vacuum or reduced pressure conditions, followed by formation and capacity testing to obtain the finished lithium-ion battery.

[0057] Compared to existing technologies, the overall beneficial effects of this case are as follows: I. Liquid Phase Homogenization and Initial Rheological Stability. During the formation stage of the composite organic electrolyte, ultrasonic dispersion for at least one hour is employed, and the volume ratio of the ionic liquid to the organic solvent containing the lithium salt is converged to 0.9–1.1:1 (v / v). This combination ensures sufficient deagglomeration and microbubble nucleus elimination within the liquid phase, and directly anchors the initial viscosity and flowability of the system by volume, enabling different devices and batches to achieve similar rheological states under the same volume conditions. Unlike Reference 1, which only provides an example of "(0.8–1.2):1" and does not specify the ultrasonic duration, this study introduces a narrowing of the ratio window and a lower limit for energy input, which helps reduce the risk of gas entrainment and phase separation during subsequent high-solids-content composite processes, improving batch-to-batch consistency from the outset.

[0058] II. Selection of Cation / Anion in Ionic Liquids and Wide-Temperature Continuous Phase. The preferred liquid phase is an imidazole or pyrrole salt with cation-paired TFSI. - or DFSI - Anions. This combination combines low vapor pressure, excellent low-temperature ion migration, and compatibility with carbonate solvents, which is beneficial for maintaining the continuity of the organic phase at low temperatures and reducing volatilization and morphological fluctuations at high temperatures. Compared with the literature's approach of listing ionic liquids as a family, this approach stabilizes the initial solvation environment and viscosity range under different formulation choices by limiting the cation / anion set and coordinating it with the volume ratio, facilitating cross-batch replication.

[0059] III. Volumetric aperture control and dispersion energy input for high-solids-content colloidal substances. In organic... -In the inorganic composite stage, the solid content of the inorganic ionic conductor nanoparticles was controlled at 2.3–2.7 g / mL based on the total volume of the mixed system. Milling was performed in a mortar for at least 1 hour, or planetary / high-shear dispersion was used to achieve continuous and stable energy input. Unlike describing the content as a mass percentage (wt.%), the volumetric aperture directly determines the viscosity, coating operability, and degassing difficulty of the high-solids-content colloidal state; the lower limit of the dispersion time ensures sufficient deagglomeration and surface wetting. Both factors work together to achieve continuous coating and pore penetration of the composite organic electrolyte on the nanoparticle surface, establishing a stable viscoelastic network. This approach fills the gap in Reference 1, which did not express the solid content by volume or quantify the dispersion intensity and duration, making the suppression of batch-to-batch rheological differences more feasible.

[0060] IV. Sequential Process Control of Degassing and Shaping. After the gel-like precursor is formed, a sequential process of degassing followed by settling is implemented: degassing is performed under vacuum or reduced pressure, followed by settling to complete the self-consistent rearrangement of the viscoelastic network and secondary wetting of the interface. This sequence effectively eliminates microbubbles and entrainment introduced during the dispersion process, reduces local electric / thermal field anomalies, and minimizes initial impedance fluctuations after assembly. A stable quasi-solid gel-like finished product is obtained at room temperature, which helps maintain the continuity of the electrode / electrolyte contact surface and improves wide-temperature operating stability. Unlike the overview of "gel formation" in Reference 1, this study explicitly defines degassing and settling as necessary processes and a fixed sequence, enhancing reproducibility in scale-up manufacturing.

[0061] V. The Interfacial Significance of Nanoframework and Pore Infiltration. The inorganic ionic conductor particles used are nanoscale, and their surface and pore structure provide effective infiltration and fixation sites for the composite organic electrolyte. Combined with the aforementioned volumetric solids-containing window and dispersion action, a continuous coating layer can be formed within the electrode pores, reducing free solvent retention and improving interfacial density. This synergistic relationship between the "nanoframework, pore infiltration, and volumetric solids-containing" helps maintain the continuity of the conduction channels under low-temperature conditions and provides morphological support under high-temperature conditions, thus suppressing the early rise of interfacial impedance at the structural level.

[0062] VI. Integration of Assembly and Formation Processes. During cell assembly, the colloidal electrolyte is applied between the electrodes and the separator using methods such as coating, scraping, dispensing, or injection, combined with a slow-start procedure of vacuum or reduced-pressure degassing and room-temperature formation. The aforementioned electrolyte morphology output (room-temperature gel state, continuous coverage, and gap-filling capability) is combined with the degassing and low-rate start-up during the assembly process. This reduces initial polarization dispersion and batch-to-batch differences without altering the mainstream positive and negative electrode materials and the casing structure, facilitating stable scale-up in existing production lines. Compared to the battery implementation in Reference 1, this provides a quantitative window for assembly, degassing, and formation, allowing the material-level advantages to be more reliably reflected in the finished cell.

[0063] VII. Substantial Differences and Technical Effects Summary Compared to Reference 1. Reference 1, as it is published, focuses on the material framework and wt.% mass percentage ratio, without specifying necessary procedural limitations on dispersion methods and duration, the high solids content window expressed by volumetric methods, and the order of "degassing and settling." In contrast, this invention establishes a reproducible process chain from liquid-phase homogenization to colloidal formation through four parameterized steps: volume ratio (including convergence interval), volumetric solids content, lower limit of dispersion time, and a fixed order of degassing and settling. This process chain, combined with the structural features of "nanoframework and pore penetration," achieves the following detectable indicators: 1. The batch-to-batch differences in EIS at room temperature and low temperature were significantly narrowed, demonstrating improved manufacturing consistency; 2. The growth of interfacial impedance in the early cycle was suppressed, demonstrating improved interfacial stability; 3. DSC shows that the low-temperature phase behavior is more stable and the high-temperature morphology is more stable, demonstrating enhanced wide-temperature operation capability.

[0064] These effects are not caused by changes in the material list, but by the cross-limitation of the formulation window and the process window and the sequential process control, which can effectively solve the reproducibility problem in large-scale production and form a verifiable technical difference from Reference 1.

[0065] Finally, it should be noted that any cross-referencing or superposition of the various embodiments of this solution by those skilled in the art still falls within the original disclosure scope of this solution. Furthermore, the above descriptions are merely preferred embodiments of the present invention and are not intended to limit the invention. Although the present invention has been described in detail with reference to the foregoing embodiments, those skilled in the art can still modify the technical solutions described in the foregoing embodiments or make equivalent substitutions for some of the technical features. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the protection scope of the present invention.

Claims

1. An organic - A method for producing an inorganic composite quasi-solid electrolyte, characterized by, The method comprises the following steps: An ionic liquid preparation step: at least one of quaternary ammonium salt, quaternary phosphonium salt, imidazole salt or pyrrole salt is selected as a cation, and at least one of bis(trifluoromethanesulfonyl)imide, trifluoromethylsulfonate, hexafluorophosphate, tetrafluoroborate or bis(fluorosulfonyl)imide is selected as an anion to form an ionic liquid; An electrolyte preparation step: the ionic liquid is mixed with an organic solvent containing lithium salt at a volume ratio of 0.8-1.2:1, and ultrasonic dispersion is performed to form a composite organic electrolyte; Inorganic compounding step: mixing inorganic ion conductor nanoparticles with the composite organic electrolyte, so that the solid content of the inorganic ion conductor nanoparticles in the mixing system is 2.0-3.0 g / mL, and performing grinding and / or planetary dispersion or high-shear dispersion, so that the composite organic electrolyte coats and penetrates into the surface and pores of the inorganic ion conductor nanoparticles, to obtain a colloidal organic - Inorganic composite quasi-solid electrolyte precursor; Defoaming and setting step: defoaming and setting the precursor by resting, obtaining an organic - Inorganic composite quasi-solid electrolyte.

2. The organic - The method for producing an inorganic composite quasi-solid electrolyte is characterized by comprising: The ultrasonic dispersion time in the electrolyte preparation step is not less than 1 hour; In the ionic liquid preparation step, the cation is imidazole salt ion or pyrrole salt cation; In the ionic liquid formulation step, the anion is bis-trifluoromethanesulfonimide (TFSI - ) or bis-fluorosulfonimide (DFSI - ). In the electrolyte preparation step, the ionic liquid is mixed with the organic solvent containing lithium salt at a volume ratio of 0.9-1.1:

1.

3. The organic - A method for producing an inorganic composite quasi-solid electrolyte, characterized by In the inorganic compounding step, the solid content of the inorganic ion conductor nanoparticles in the mixed system is 2.3-2.7 g / mL; the inorganic compounding step is performed by mortar grinding, and the grinding time is not less than 1 hour; The defoaming and shaping step comprises: after the precursor is defoamed and treated, it is left to stand for not less than 1 hour to complete shaping; The organic - The inorganic composite quasi-solid electrolyte is a quasi-solid gel. The inorganic ion conductor nanoparticles are nanoscale particles.

4. An organic - Inorganic composite quasi-solid electrolyte characterized in that, The electrolyte is a colloidal composite formed by inorganic ion conductor nanoparticles and a composite organic electrolyte, wherein: The composite organic electrolyte is prepared by uniformly mixing an ionic liquid and an organic solvent containing lithium salt at a volume ratio of 0.8-1.2:1; The inorganic ion conductor nanoparticles are dispersed in the composite organic electrolyte and are coated and infiltrated by the composite organic electrolyte, and the solid content of the inorganic ion conductor nanoparticles in the electrolyte is 2.0-3.0 g / mL; The electrolyte is a quasi-solid gel at room temperature.

5. The organic - Inorganic composite quasi-solid electrolyte characterized in that, The ionic liquid is formed by pairing at least one of quaternary ammonium salt, quaternary phosphonium salt, imidazole salt or pyrrole salt as a cation with at least one of bis(trifluoromethanesulfonyl)imide, trifluoromethylsulfonate, hexafluorophosphate, tetrafluoroborate or bis(fluorosulfonyl)imide as an anion.

6. The organic - Inorganic composite quasi-solid electrolyte characterized in that, The inorganic ion conductor nanoparticles are oxide or sulfide solid-state electrolyte nanoparticles, and the particle size is nanoscale and forms a pore structure for infiltration of the composite organic electrolyte; The electrolyte is used in a lithium ion battery.

7. A lithium-ion battery, characterized by The lithium ion battery comprises a positive electrode, a negative electrode and a separator, and the organic - Inorganic composite quasi-solid electrolyte.

8. The lithium-ion battery of claim 7, wherein, The positive electrode active material is selected from at least one of lithium iron phosphate, lithium nickel cobalt manganese acid or lithium nickel cobalt aluminum acid; The negative electrode active material is selected from at least one of graphite, hard carbon, soft carbon or silicon-based carbon composite material; The separator is a polyolefin microporous membrane or a surface coated membrane thereof; The lithium ion battery is a soft package or a cylindrical or square shell structure.

9. A method of manufacturing a lithium-ion battery, characterized by, The method comprises the following steps: A pre-step: an electrode core stack or winding body comprising a positive electrode sheet, a negative electrode sheet and a separator is prepared; Electrolyte preparation step: preparing an organic - Inorganic composite quasi-solid electrolyte; Assembly step: the organic - The inorganic composite quasi-solid electrolyte is applied between the positive electrode and the negative electrode and in contact with the separator, covering the surface of the electrode active layer and filling the interstices therebetween; A finished product step: the electrode core after the assembly step is subjected to defoaming and sealing under vacuum or reduced pressure, and then formation and capacity distribution are performed to obtain the lithium ion battery finished product.

10. The method for preparing a lithium-ion battery according to claim 9, characterized in that, In the assembly step, the electrolyte is applied by coating, doctor blading, dispensing or injection, and the thickness of the applied layer is 50-500 μm; The defoaming in the finished product step is carried out under a vacuum degree of -0.08 MPa to -0.095 MPa for 10 to 30 minutes; the formation is carried out under normal temperature, and a low rate is started in a constant current or constant current constant voltage mode in the early stage of formation, and then a normal rate charging and discharging program is entered.