Composite solid-state battery electrolyte, preparation device and preparation method thereof

Abstract

The invention relates to the technical field of chemical batteries, and discloses a composite solid-state battery electrolyte, which comprises a lithium salt, an organic solvent, a polymer and an inorganic active filler, the polymer and the inorganic active filler are cross-linked and compounded, the mass of the inorganic active filler accounts for 7-12% of the total mass of the composite solid-state electrolyte, and the mass of the lithium salt accounts for 1-10% of the total mass of the composite solid-state battery electrolyte. The mass ratio of the lithium salt to the inorganic active filler is (2-3): 20, the ratio of the total mass of the lithium salt and the inorganic active filler to the mass of the organic solvent is (2-5): 10, and the mass of the polymer accounts for 33-42% of the total mass of the composite solid electrolyte. According to the composite solid-state battery electrolyte, the preparation device and the preparation method thereof, in an all-solid-state lithium ion battery, the inorganic active filler and the electrode active material are kept consistent, and the inorganic active filler can accelerate dissociation of lithium salt and improve the ionic conductivity; and the compatibility of the electrode and the electrolyte is improved.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of chemical batteries, in particular to a composite solid-state battery electrolyte, a preparation device and a preparation method thereof. BACKGROUND

[0002] The solid-state electrolyte has the characteristics of high ionic conductivity and good thermal stability. The main materials of the traditional solid-state electrolyte are oxides and sulfides. However, the oxide materials and sulfide materials have some common problems in practical application, such as low ionic conductivity and poor interface stability. In order to solve these problems, a composite solid-state electrolyte is needed. The composite solid-state electrolyte is made by mixing two or more solid-state electrolyte materials, so a mixing device is needed.

[0003] At present, the composite solid-state electrolyte is mainly composed of a polymer electrolyte and an oxide electrolyte. However, this composite solid-state electrolyte has the disadvantage of low room temperature ionic conductivity due to the influence of the polymer electrolyte. The battery capacity may be reduced and the performance such as durability and output may not meet the expectations.

[0004] Therefore, we propose a composite solid-state battery electrolyte, a preparation device and a preparation method thereof. SUMMARY

[0005] In order to make up for the shortcomings of the prior art, the present application provides the following technical scheme: a composite solid-state battery electrolyte, comprising a lithium salt, an organic solvent, a polymer, and an inorganic active filler, the polymer and the inorganic active filler are cross-linked and compounded, the mass of the inorganic active filler accounts for 7-12% of the total mass of the composite solid-state electrolyte, the mass ratio of the lithium salt to the inorganic active filler is 2-3:20, the total mass of the lithium salt and the inorganic active filler to the mass of the organic solvent is 2-5:10, and the mass of the polymer accounts for 33-42% of the total mass of the composite solid-state electrolyte.

[0006] Preferably, the inorganic active filler is a conductive active filler, the conductive active filler is selected from at least one of lithium lanthanum zirconium tantalum oxide, lanthanum zirconium oxide, lithium lanthanum zirconium tantalum oxide, lithium lanthanum zirconium niobium oxide, titanium aluminum lithium phosphate, and lithium lanthanum titanium oxide, the lithium salt is lithium hexafluorophosphate, the organic solvent is 1,3-dioxolan-2-one (EC) and diethyl carbonate (DEC), and the polymer is one or a combination of several of fluorine-based polymer, ether-based polymer, acrylic polymer, and acrylonitrile-based polymer.

[0007] The utility model provides a preparation device of composite solid battery electrolyte for preparing the above-mentioned composite solid battery electrolyte, including preparation bucket, the top of preparation bucket is fixedly installed with drive motor, the inside of preparation bucket is provided with stirring assembly, the output of drive motor is connected with the top of stirring assembly, the top of preparation bucket is provided with the feed inlet of one side at drive motor, the bottom of preparation bucket is provided with discharge pipe, the middle part of discharge pipe is provided with valve, the outside of stirring assembly is provided with scraping assembly.

[0008] Preferably, the output end of the drive motor is fixedly installed with a first bevel gear, the top of the preparation bucket is provided with a rotating rod, the top of the rotating rod is fixedly installed with a second bevel gear, the middle part of the rotating rod is fixedly installed with a fixed sleeve inside the preparation bucket, the outer circumferential surface of the fixed sleeve is provided with a first stirring blade, and the second bevel gear is engaged with the top of the first bevel gear.

[0009] Preferably, the rotating rod is rotatably connected with a rotating sleeve above the fixed sleeve, the rotating sleeve is rotatably connected with the middle part of the top of the preparation bucket, the top of the rotating sleeve is fixedly installed with a third bevel gear above the preparation bucket, the third bevel gear is engaged with the bottom of the first bevel gear, the bottom of the rotating sleeve is fixedly installed with a second stirring blade inside the preparation bucket, and the second stirring blade is wrapped outside the first stirring blade.

[0010] Preferably, the first stirring blade comprises two discs fixedly installed at the upper and lower ends of the fixed sleeve, and a spiral belt integrally arranged on the opposite surfaces of the two discs, the middle part of the fixed sleeve is fixedly installed with the spiral belt through a round rod, the second stirring blade comprises a circular ring fixedly installed with the bottom of the rotating sleeve, and another spiral belt integrally connected with the bottom of the circular ring, the bottom of the second stirring blade spiral belt is integrally provided with another circular ring, the rotation direction of the spiral belt in the second stirring blade is the same as that of the spiral belt in the first stirring blade, and the scraping assembly is fixedly installed with the outer circumferential surface of the circular ring in the second stirring blade.

[0011] Preferably, the bottom of the preparation bucket is fixedly installed with a circulating pump on one side of the discharge pipe, the feed inlet of the circulating pump is fixedly installed with a guide pipe on one side of the discharge pipe through a pipeline, the discharge outlet of the circulating pump is fixedly installed with a guide pipe, the other end of the guide pipe is fixedly installed with the top of the side surface of the preparation bucket, the pipeline provided at the feed inlet of the circulating pump is above the valve, and the diameter of the guide pipe is smaller than that of the discharge pipe.

[0012] Preferably, the scraping assembly comprises a connecting plate fixedly connected with the outer circumferential surface of the annular ring in the second stirring blade, a fixed frame is fixedly installed on the side surface of the connecting plate, a side wall scraper is fixedly installed on the side surface of the fixed frame, the other end of the fixed frame is fixedly installed on the middle part of the side wall scraper, an elastic arc plate is arranged between the fixed frame and the side wall scraper, the fixed frame, the side wall scraper and the elastic arc plate are arranged with the same center, and the distal end of the side wall scraper is in sliding contact with the inner wall of the preparation barrel.

[0013] Preferably, the bottom of the spiral belt of the second stirring blade is fixedly installed with a connecting frame, the bottom of the rotating rod is rotatably connected with a rotating ring below the fixed sleeve, the outer circumferential surface of the rotating ring is fixedly installed with a lower scraper, the bottom of the lower scraper is in sliding contact with the bottom of the inner part of the preparation barrel.

[0014] The preparation method of the composite solid-state battery electrolyte comprises the following steps:

[0015] S1, the organic solvent, lithium salt and inorganic active filler are added into the preparation barrel through the feeding port of the preparation device for mixing and stirring to obtain a mixed solution;

[0016] S2, the polymer is further added into the mixed solution obtained in step S1, and heated and stirred until uniformly mixed to obtain a liquid-phase composite solid-state electrolyte precursor;

[0017] S3, the liquid-phase composite solid-state electrolyte precursor is coated on a tray for sintering, dried and then sintered, the heating rate during sintering is 1-3 ℃ / min, the sintering temperature is 850-900 ℃, and the holding time is 6-12 h.

[0018] Advantages

[0019] Compared with the prior art, the composite solid-state battery electrolyte, the preparation device and the preparation method thereof have the following advantages:

[0020] 1. The composite solid-state battery electrolyte, the preparation device and the preparation method thereof, the composite solid-state battery electrolyte exhibits an ionic conductivity not less than 10-3 S / cm at room temperature, which is equivalent to that of a conventional liquid electrolyte battery, in addition, the solid-state battery using the composite solid-state battery electrolyte has high Li +The solid-state battery shows excellent cycle performance, the inorganic active filler is uniformly dispersed in the composite solid electrolyte, the inorganic active filler is consistent with the electrode active material in the all-solid-state lithium ion battery, and the inorganic active filler can accelerate the dissociation of lithium salt and improve the ionic conductivity, the consistency of the active filler and the positive electrode material is utilized, and the compatibility of the electrode and the electrolyte is improved.

[0021] 2、The composite solid battery electrolyte, preparation device and preparation method thereof, by setting the stirring assembly, the driving motor drives the second bevel gear and the third bevel gear to reverse rotation through the first bevel gear, so that the second bevel gear and the third bevel gear drive the rotating rod and the rotating sleeve to reverse rotation respectively, so that the first stirring blade and the second stirring blade rotate in opposite directions in the inside of the preparation barrel, and then the mixed liquid in the inside of the preparation barrel forms turbulent flow to improve the stirring effect, and the stirring effect is better through the continuous scraping of the side wall scraping plate on the side wall of the preparation barrel, the stirring and mixing efficiency of the various high-performance battery solid electrolyte materials is improved, and the linkage effect is good, only one driving motor needs to be controlled, the control of the present application can be completed, and the operation is greatly simplified.

[0022] 3、The composite solid battery electrolyte, preparation device and preparation method thereof, by coating the fully mixed composite solid electrolyte precursor on the tray for sintering, and optimizing the sintering process of the battery, the grain boundary interface of the solid electrolyte forms a composite grain boundary, and then the formed composite solid electrolyte not only has a wider ion transport channel, but also has a good continuous solid solution interface phase, so that the ion migration is more favorable, and then the obtained composite solid electrolyte shows higher total ionic conductivity. BRIEF DESCRIPTION OF DRAWINGS

[0023] Figure 1 It is a schematic diagram of the overall structure of the present application;

[0024] Figure 2 It is a schematic diagram of the preparation barrel of the present application; Figure 1 It is an enlarged view of A in the present application;

[0025] Figure 3 It is a schematic diagram of the structure of the preparation barrel of the present application;

[0026] Figure 4 It is a schematic diagram of the structure of the first stirring blade of the present application;

[0027] Figure 5 It is a schematic diagram of the structure of the second stirring blade of the present application;

[0028] Figure 6 It is a schematic diagram of the structure of the scraping assembly of the present application;

[0029] Figure 7Structure diagram of the lower scraper of the application;

[0030] Figure 8 Structure diagram of the fixed frame of the application.

[0031] In the figure: 1, preparation barrel; 2, feeding port; 3, discharging pipe; 4, driving motor; 5, first bevel gear; 6, stirring assembly; 601, rotating rod; 602, second bevel gear; 603, fixed sleeve; 604, first stirring blade; 605, rotating sleeve; 606, third bevel gear; 607, second stirring blade; 608, connecting frame; 609, rotating ring; 610, lower scraper; 7, material guide pipe; 8, valve; 9, circulating material pump; 10, scraping assembly; 1001, connecting plate; 1002, fixed frame; 1003, sidewall scraper; 1004, elastic arc plate. DETAILED DESCRIPTION

[0032] The technical solutions in the embodiments of the application will be apparently and completely described below with reference to the accompanying drawings in the embodiments of the application. Obviously, the described embodiments are only part of the embodiments of the application, rather than all the embodiments of the application. Based on the embodiments in the application, all the other embodiments obtained by a person of ordinary skill in the art without creative work fall within the protection scope of the application.

[0033] Please refer to Figures 1 to 8 The composite solid-state battery electrolyte comprises a lithium salt, an organic solvent, a polymer, and an inorganic active filler. The polymer and the inorganic active filler are crosslinked and compounded. The mass of the inorganic active filler accounts for 7-12% of the total mass of the composite solid-state battery electrolyte. The mass ratio of the lithium salt to the inorganic active filler is 2-3:20. The ratio of the total mass of the lithium salt and the inorganic active filler to the mass of the organic solvent is 2-5:10. The mass of the polymer accounts for 33-42% of the total mass of the composite solid-state battery electrolyte.

[0034] As an embodiment of the present application, the inorganic active filler is a conductive active filler selected from at least one of lithium lanthanum zirconium tantalum oxide, lanthanum zirconium oxide, lithium lanthanum zirconium tantalum oxide, lithium lanthanum zirconium niobium oxide, titanium aluminum lithium phosphate, lithium lanthanum titanium oxide, the lithium salt is lithium hexafluorophosphate, the organic solvent is 1,3-dioxolan-2-one (EC) and diethyl carbonate (DEC), the polymer is one or a combination of fluorine-based polymer, ether-based polymer, acrylic polymer and acrylonitrile-based polymer, the composite solid-state electrolyte exhibits an ionic conductivity of not less than 10-3 S / cm at room temperature, which is comparable to that of a conventional liquid electrolyte battery, in addition, the solid-state battery using the composite solid-state electrolyte exhibits excellent cycle performance due to high Li+ transfer number and effective inhibition of lithium dendrites, the inorganic active filler is uniformly dispersed in the composite solid-state electrolyte, the inorganic active filler is consistent with the electrode active material in the all-solid-state lithium ion battery, and the inorganic active filler can accelerate the dissociation of the lithium salt and improve the ionic conductivity, the consistency of the active filler and the positive electrode material improves the compatibility of the electrode and the electrolyte.

[0035] The preparation device of the composite solid-state battery electrolyte comprises a preparation barrel 1, a driving motor 4 fixedly installed at the top of the preparation barrel 1, a stirring assembly 6 arranged in the interior of the preparation barrel 1, and a first conical gear 5 fixedly installed at the output end of the driving motor 4.

[0036] As an embodiment of the present application, the output end of the driving motor 4 is fixedly installed with the first conical gear 5, the top of the preparation barrel 1 is throughly provided with a rotating rod 601, the top of the rotating rod 601 is fixedly installed with a second conical gear 602, the middle of the rotating rod 601 is fixedly installed with a fixed sleeve 603 located in the interior of the preparation barrel 1, the outer circumferential surface of the fixed sleeve 603 is provided with a first stirring blade 604, and the second conical gear 602 is engaged with the top of the first conical gear 5.

[0037] As an embodiment of the present application, the rotating rod 601 is rotatably connected with a rotating sleeve 605 located above the fixed sleeve 603, the rotating sleeve 605 is throughly and rotatably connected with the middle of the top of the preparation barrel 1, the top of the rotating sleeve 605 is fixedly installed with a third conical gear 606 located above the preparation barrel 1, the third conical gear 606 is engaged with the bottom of the first conical gear 5, the bottom of the rotating sleeve 605 is fixedly installed with a second stirring blade 607 located in the interior of the preparation barrel 1, and the second stirring blade 607 is wrapped outside the first stirring blade 604.

[0038] As an embodiment of the present application, the first stirring blade 604 comprises two discs fixedly installed at the upper and lower ends of the fixed sleeve 603, and a spiral belt integrally arranged on the opposite faces of the two discs, the middle part of the fixed sleeve 603 is fixedly installed with the middle part of the spiral belt through a round rod, the second stirring blade 607 comprises a circular ring fixedly installed at the bottom of the rotating sleeve 605, and another spiral belt integrally connected with the bottom of the circular ring, the bottom of the spiral belt of the second stirring blade 607 is integrally provided with another circular ring, the rotating direction of the spiral belt in the second stirring blade 607 is the same as that of the spiral belt in the first stirring blade 604, and the scraping assembly 10 is fixedly installed with the outer circumferential surface of the circular ring in the second stirring blade 607.

[0039] As an embodiment of the present application, the bottom of the preparation barrel 1 is fixedly installed with the circulating material pump 9 located at one side of the discharge pipe 3, the feeding port 2 of the circulating material pump 9 is fixedly installed with the discharge pipe 3 through a conduit, the discharge port of the circulating material pump 9 is fixedly installed with the guide pipe 7, the other end of the guide pipe 7 is fixedly installed with the top of the side of the preparation barrel 1, the conduit of the feeding port 2 of the circulating material pump 9 is arranged above the valve 8, and the diameter of the guide pipe 7 is smaller than that of the discharge pipe 3.

[0040] As an embodiment of the present application, the scraping assembly 10 comprises a connecting plate 1001 fixedly installed with the outer circumferential surface of the circular ring in the second stirring blade 607, a fixed frame 1002 fixedly installed on the side of the connecting plate 1001, a side wall scraping plate 1003 fixedly installed on the side of the connecting plate 1001 and located at the side of the fixed frame 1002, the other end of the fixed frame 1002 is fixedly installed with the middle part of the side wall scraping plate 1003, an elastic arc plate 1004 is arranged between the fixed frame 1002 and the side wall scraping plate 1003, the fixed frame 1002, the side wall scraping plate 1003 and the elastic arc plate 1004 are arranged with the same center, and the end of the side wall scraping plate 1003 is in sliding contact with the inner wall of the preparation barrel 1.

[0041] As one of the embodiments of the present application, the bottom of the spiral belt of the second stirring blade 607 is fixedly provided with a connecting frame 608, the bottom of the rotating rod 601 is rotatably connected with a rotating ring 609 below the fixed sleeve 603, the outer circumferential surface of the rotating ring 609 is fixedly provided with a lower scraper 610, the middle part of the top of the lower scraper 610 is fixedly provided with the bottom of the connecting frame 608, the bottom of the preparation barrel 1 is funnel-shaped, the discharge pipe 3 is located at the lowest part of the bottom of the preparation barrel 1, the bottom of the lower scraper 610 is in sliding contact with the bottom of the inside of the preparation barrel 1, by arranging the stirring assembly 6, the driving motor 4 drives the second bevel gear 602 and the third bevel gear 606 to rotate reversely, so that the rotating rod 601 and the rotating sleeve 605 are driven by the second bevel gear 602 and the third bevel gear 606 to rotate reversely, so that the first stirring blade 604 and the second stirring blade 607 rotate reversely in the inside of the preparation barrel 1, so that the mixed liquid in the inside of the preparation barrel 1 forms a turbulent flow to improve the stirring effect, and the side wall scraper 1003 continuously scrapes the side wall of the preparation barrel 1, so that the stirring effect is better, the stirring and mixing efficiency of the various high-performance battery solid-state electrolyte materials is improved, and the linkage effect is good, only one driving motor 4 needs to be controlled to complete the control of the present application, and the operation is greatly simplified.

[0042] The preparation method of the composite solid-state battery electrolyte comprises the following steps:

[0043] S1, the organic solvent, the lithium salt and the inorganic active filler are added into the preparation barrel 1 through the feeding port 2 of the preparation device for mixing and stirring to obtain a mixed solution;

[0044] S2, the polymer is further added into the mixed solution obtained in step S1, and heated and stirred until the mixed solution is uniform to obtain a liquid-phase composite solid-state electrolyte precursor;

[0045] S3, the liquid-phase composite solid-state electrolyte precursor is coated on a tray for sintering, dried and then sintered, the heating rate during sintering is 1-3 ℃ / min, the sintering temperature is 850-900 ℃, and the holding time is 6-12 h, by coating the fully mixed composite solid-state electrolyte precursor on the tray for sintering and optimizing the sintering process of the battery, the crystal boundary interface of the solid-state electrolyte forms a composite crystal boundary, so that the formed composite solid-state electrolyte not only has a wider ion transport channel, but also has a good continuous solid solution interface phase, so it is more conducive to ion migration, and the obtained composite solid-state electrolyte has higher total ionic conductivity.

[0046] It should be noted that in use, the organic solvent, lithium salt and inorganic active filler are added into the preparation barrel 1 through the feed port 2 of the preparation device, the driving motor 4 drives the second bevel gear 602 and the third bevel gear 606 to rotate reversely through the first bevel gear 5, so that the rotating rod 601 and the rotating sleeve 605 are driven by the second bevel gear 602 and the third bevel gear 606 to rotate reversely, respectively, so that the first stirring blade 604 and the second stirring blade 607 rotate in opposite directions in the interior of the preparation barrel 1, thereby forming a turbulent flow of the mixed liquid in the interior of the preparation barrel 1 to improve the stirring effect, and the side wall scraper 1003 continuously scrapes the side wall of the preparation barrel 1, so that the stirring effect is better, the stirring and mixing efficiency of the various high-performance battery solid electrolyte materials is improved, and the linkage effect is good, so that the control of the present application can be completed by controlling only one driving motor 4, thereby greatly simplifying the operation.

[0047] It should be noted that in this document, the terms "first" and "second" are used only to distinguish one entity or operation from another entity or operation, and do not necessarily require or imply any such actual relationship or order between these entities or operations. Moreover, the terms "include", "contain" or any other variants thereof are intended to cover non-exclusive inclusion, so that the process, method, article or device including a series of elements not only includes those elements, but also includes other elements not explicitly listed or inherent to such process, method, article or device.

[0048] Although embodiments of the present application have been shown and described, it will be understood by those skilled in the art that various changes, modifications, substitutions and alterations can be made thereto without departing from the principles and spirit of the present application, and the scope of the present application is defined by the appended claims and their equivalents.

[0049] Finally, it should be noted that: the above embodiments are only used to illustrate the technical solutions of the present application, and not to limit them; although the present application has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that they can still modify the technical solutions recorded in the foregoing embodiments, or make equivalent substitutions for part or all of the technical features; and these modifications or substitutions do not make the essence of the corresponding technical solutions deviate from the scope of the technical solutions of the embodiments of the present application.

Claims

1. A composite solid-state battery electrolyte, characterized by: The lithium salt, organic solvent, polymer, and inorganic active filler are crosslinked and compounded, the mass of the inorganic active filler accounts for 7-12% of the total mass of the composite solid electrolyte, the mass ratio of the lithium salt to the inorganic active filler is 2-3:20, the ratio of the total mass of the lithium salt and the inorganic active filler to the mass of the organic solvent is 2-5:10, and the mass of the polymer accounts for 33-42% of the total mass of the composite solid electrolyte.

2. The composite solid-state battery electrolyte of claim 1, wherein: The inorganic active filler is an electrically conductive active filler selected from at least one of lithium lanthanum zirconium tantalum oxide, lanthanum zirconium oxide, lithium lanthanum zirconium tantalum oxide, lithium lanthanum zirconium niobium oxide, titanium aluminum lithium phosphate, and lithium lanthanum titanium oxide, the lithium salt is lithium hexafluorophosphate, the organic solvent is 1,3-dioxolan-2-one (EC) and diethyl carbonate (DEC), and the polymer is one or a combination of fluoropolymers, ether polymers, acrylic polymers, and acrylonitrile polymers.

3. A preparation device for preparing the composite solid-state battery electrolyte according to any one of claims 1-2, comprising a preparation barrel (1), characterized in that: The top of the preparation barrel (1) is fixedly provided with a driving motor (4), the inside of the preparation barrel (1) is provided with a stirring assembly (6), the output end of the driving motor (4) is in transmission connection with the top of the stirring assembly (6), the top of the preparation barrel (1) is provided with a feeding port (2) on the side of the driving motor (4), the bottom of the preparation barrel (1) is provided with a discharging pipe (3), the middle part of the discharging pipe (3) is provided with a valve (8), and the outside of the stirring assembly (6) is provided with a scraping assembly (10).

4. The preparation apparatus of the composite solid-state battery electrolyte according to claim 3, characterized in that: The output end of the driving motor (4) is fixedly provided with a first bevel gear (5), the top of the preparation barrel (1) is provided with a rotating rod (601) penetratingly arranged, the top of the rotating rod (601) is fixedly provided with a second bevel gear (602), the middle part of the rotating rod (601) is fixedly provided with a fixed sleeve (603) arranged in the inside of the preparation barrel (1), the outer circumferential surface of the fixed sleeve (603) is provided with first stirring blades (604), and the second bevel gear (602) is in mesh with the top of the first bevel gear (5).

5. The apparatus for preparing a composite solid-state battery electrolyte according to claim 4, characterized by: The rotating rod (601) is rotatably connected with a rotating sleeve (605) arranged above the fixed sleeve (603), the rotating sleeve (605) is penetratingly and rotatably connected with the middle part of the top of the preparation barrel (1), the top of the rotating sleeve (605) is fixedly provided with a third bevel gear (606) arranged above the preparation barrel (1), the third bevel gear (606) is in mesh with the bottom of the first bevel gear (5), the bottom of the rotating sleeve (605) is fixedly provided with second stirring blades (607) arranged in the inside of the preparation barrel (1), and the second stirring blades (607) are wrapped outside the first stirring blades (604).

6. The preparation apparatus of the composite solid-state battery electrolyte according to claim 5, characterized in that: The first stirring blade (604) comprises two discs fixedly installed at the upper and lower ends of a fixed sleeve (603), and a spiral belt integrally arranged on the opposite faces of the two discs, the middle part of the fixed sleeve (603) is fixedly installed with the middle part of the spiral belt through a round rod, the second stirring blade (607) comprises a circular ring fixedly installed at the bottom of a rotating sleeve (605), and another spiral belt integrally connected with the bottom of the circular ring, the bottom of the spiral belt of the second stirring blade (607) is integrally provided with another circular ring, the rotating direction of the spiral belt in the second stirring blade (607) is the same as that of the spiral belt in the first stirring blade (604), and the scraping assembly (10) is fixedly installed with the outer circumferential surface of the circular ring in the second stirring blade (607).

7. The preparation apparatus of the composite solid-state battery electrolyte according to claim 3, characterized in that: The bottom of the preparation barrel (1) is fixedly installed with a circulating material pump (9) located on one side of the discharge pipe (3), the inlet (2) of the circulating material pump (9) is fixedly installed with a guide pipe on one side of the discharge pipe (3), and the outlet of the circulating material pump (9) is fixedly installed with a guide pipe (7), the other end of the guide pipe (7) is fixedly installed with the top of the side of the preparation barrel (1), the guide pipe of the inlet (2) of the circulating material pump (9) is located above the valve (8), and the diameter of the guide pipe (7) is smaller than that of the discharge pipe (3).

8. The apparatus for preparing a composite solid-state battery electrolyte according to claim 6, characterized by: The scraping assembly (10) comprises a connecting plate (1001) fixedly installed with the outer circumferential surface of the circular ring in the second stirring blade (607), a fixed frame (1002) fixedly installed on the side of the connecting plate (1001), and a side wall scraping plate (1003) fixedly installed on the side of the fixed frame (1002), the other end of the fixed frame (1002) is fixedly installed with the middle part of the side wall scraping plate (1003), an elastic arc plate (1004) is arranged between the fixed frame (1002) and the side wall scraping plate (1003), the fixed frame (1002), the side wall scraping plate (1003) and the elastic arc plate (1004) are arranged around the same center, and the distal end of the side wall scraping plate (1003) is in sliding contact with the inner wall of the preparation barrel (1).

9. The apparatus for preparing a composite solid-state battery electrolyte according to claim 6, characterized by: The bottom of the circular ring at the bottom of the spiral belt of the second stirring blade (607) is fixedly installed with a connecting frame (608), the bottom of the rotating rod (601) is rotatably connected with a rotating ring (609) located below the fixed sleeve (603), the outer circumferential surface of the rotating ring (609) is fixedly installed with a lower scraping plate (610), the middle part of the top of the lower scraping plate (610) is fixedly installed with the bottom of the connecting frame (608), the bottom of the preparation barrel (1) is funnel-shaped, the discharge pipe (3) is located at the lowest position of the bottom of the preparation barrel (1), and the bottom of the lower scraping plate (610) is in sliding contact with the bottom of the inner part of the preparation barrel (1).

10. A method for preparing a composite solid-state battery electrolyte according to claim 1, characterized by, The method comprises the following steps: S1, the organic solvent, lithium salt and inorganic active filler in claim 1 are added into the preparation barrel (1) through the inlet (2) of the preparation device in claims 3-9, mixed and stirred to obtain a mixed solution; S2, the polymer is added to the mixed solution obtained in step S1, heated and stirred until mixed uniformly to obtain a liquid-phase composite solid electrolyte precursor; S3, the liquid-phase composite solid electrolyte precursor is coated onto a tray for sintering, dried and then sintered, the heating rate during sintering is 1-3 ℃ / min; the sintering temperature is 850-900 ℃, and the holding time is 6-12 h.

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