Sulfide solid electrolyte synthesis apparatus and method

Abstract

This invention provides a sulfide solid electrolyte synthesis apparatus and method, relating to the field of solid-state battery production technology. The synthesis apparatus includes: a sample feeding module, a bead feeding module, a ball milling module, a sieving module, a powder scraping module, and a sintering module. The sample feeding module and the bead feeding module are located upstream of the ball milling module, the sieving module and the powder scraping module are located downstream of the ball milling module, and the sintering module is located downstream of the sieving module, used for sintering the solid powder sieved by the sieving module. Through quantitative closed-loop feeding, scraping of residue from the tank wall, sieving, and direct transmission of sintering, the preparation efficiency, batch consistency, and environmental safety are significantly improved, reducing manual intervention within the glove box and eliminating moisture absorption and impurity introduction. This synthesis apparatus supports high-throughput synthesis with adjustable multi-parameter parameters, providing stable, clean, and controllable hardware support for the industrial-scale expansion of sulfide electrolytes.

Description

Technical Field

[0001] This invention relates to the field of solid-state battery production technology, and in particular to a sulfide solid electrolyte synthesis apparatus and method. Background Technology

[0002] Sulfide-based solid-state electrolytes (SSEs) are key materials for achieving high-safety, high-energy-density all-solid-state lithium / sodium batteries. Typical examples include Li6PS5Cl (LPSCl) and Li... 10 GeP2S 12 (LGPS) and its derivatives can achieve approximately 10 at room temperature. - ³ to 10 - With a lithium-ion conductivity on the order of 2S / cm, combined with good mechanical plasticity and positive electrode interface wettability, it is considered one of the most industrially promising solid electrolyte systems.

[0003] However, the large-scale preparation of sulfide electrolytes has long been limited by the low throughput, high environmental sensitivity and uncontrollable nature of the synthesis process, which seriously restricts its transition from the laboratory to the production line. The existing mainstream synthesis methods mainly include high-energy mechanical ball milling and liquid-phase solvothermal methods. Both of them have insurmountable industrialization obstacles: First, although high-energy mechanical ball milling does not require solvents, has high product purity and easy structure control, the process is highly dependent on manual intervention. Specifically, (1) the clamping, sealing, positioning and unloading of the ball milling jar all need to be completed manually by the operator in the glove box. The operation of a single batch is time-consuming and there are human error and exposure risks; (2) the addition of materials (precursor powder) and the addition of beads (grinding media) cannot achieve precise quantitative and synchronous coupling, resulting in large batch composition deviation and poor repeatability; (3) after ball milling, a large amount of active powder adheres to the inner wall of the jar. The recovery rate of traditional pouring or vibration methods is low and impurities are easily introduced, resulting in material waste and cross-contamination; (4) the ball milling product needs to be manually sieved to separate the powder and the ball milling beads, which is inefficient and difficult to adapt to continuous processes. The aforementioned defects directly result in the method being unable to support high-throughput material screening with multiple components and parameters, and it is also difficult to scale up to kilogram-level stable production. Second, although liquid-phase methods (such as solution combustion method and sol-gel method) can achieve a certain degree of automation, they face a double bottleneck: (1) Anhydrous organic solvents (such as toluene, THF) and strongly reducing precursors (such as thioacetamide) must be used, which is not only costly and highly toxic, but also the residual carbon / organic matter significantly inhibits ion migration, resulting in the conductivity of the obtained electrolyte generally being lower than 10. -³ S / cm; (2) Subsequent high-temperature solvent removal and carbonization side reactions are difficult to avoid, the heat treatment window is narrow, and sulfur volatilization and phase decomposition are easily triggered, further deteriorating the electrochemical performance. In addition, this route involves a large amount of waste liquid treatment, which does not conform to the industrial policy orientation of green manufacturing and low-carbon development. More seriously, neither of the two methods has solved the extreme sensitivity of sulfide materials to trace moisture (H2O<1ppm) and oxygen - any small environmental fluctuation (such as glove box dew point> H2S release can be triggered by 60°C or brief opening of the hatch, which not only endangers operational safety but also leads to the formation of insulating impurities such as LiOH / Li2CO3 in the product, significantly reducing the actual ionic conductivity and interface stability.

[0004] Therefore, existing technologies lack an integrated synthesis equipment that can operate fully automatically, at high throughput, and in a closed loop under ultra-dry and inert conditions, and integrates quantitative feeding, efficient grinding, in-situ tank cleaning, precise sieving, and controlled sintering. There is an urgent need to develop a dedicated synthesis equipment for sulfide solid electrolytes to meet industrialization needs, so as to systematically solve common technical bottlenecks such as high reliance on manual labor, poor batch consistency, low material recovery rate, fragmented processes, high energy consumption, and difficulty in environmental control, and provide a reliable material preparation platform for the engineering application of all-solid-state batteries. Summary of the Invention

[0005] The purpose of this invention is to provide a sulfide solid electrolyte synthesis equipment and method to achieve high-throughput continuous preparation of sulfide solid electrolytes from raw material feeding, ball milling, sieving, recovery of residual powder from tank walls to sintering, thus overcoming the industrialization bottlenecks of traditional manual ball milling and liquid phase methods, such as low efficiency, high environmental sensitivity, insufficient product conductivity, and inability to scale up the process.

[0006] In a first aspect, the sulfide solid electrolyte synthesis equipment provided by the present invention includes: a sample addition module, a bead addition module, a ball milling module, a sieving module, a powder scraping module, and a sintering module; The sample addition module and the bead addition module are both located upstream of the ball milling module. The sample addition module is used to quantitatively add solid powder into the ball milling jar, and the bead addition module is used to quantitatively input ball milling beads into the ball milling jar. The sieving module and the powder scraping module are both located downstream of the ball milling module. The sieving module is used to sieve solid powder and grinding beads, and the powder scraping module is used to scrape off the solid powder adhering to the inner wall of the ball milling jar. The sintering module is located downstream of the sieving module and is used to sinter the solid powder that passes through the sieving module.

[0007] In conjunction with the first aspect, the present invention provides a first possible implementation of the first aspect, wherein the sample feeding module includes: a material rack and a vibrating material feeding device; The material rack is provided with multiple circumferentially spaced holding positions, each of which is used to hold the ball mill jar; The vibratory feeding device is rotatably connected to the material rack, and the feeding port of the vibratory feeding device corresponds one by one to each of the holding positions.

[0008] In conjunction with the first aspect, the present invention provides a second possible implementation of the first aspect, wherein the ball milling module includes: a ball milling base, a first rotary driving device, a second rotary driving device, and a pressing device; The ball mill base is mounted on the first rotary drive device, and the first rotary drive device is used to drive the ball mill base to rotate. The ball milling stand is provided with multiple ball milling stations, and each ball milling station is equipped with a corresponding second rotary drive device. The second rotary drive device is used to drive the ball milling jar installed at the corresponding ball milling station to rotate. The pressing device is located beside the ball mill base, and the pressing device is used to press the ball mill jar into the ball mill station.

[0009] In conjunction with the first aspect, the present invention provides a third possible implementation of the first aspect, wherein the sieving module includes: a clamping member, a flipping drive member, a sieving device, and a vibration motor; The clamping member is used to clamp the ball mill jar, and the clamping member is installed on the movable end of the flipping drive member; The screening device is located below the clamping member, and the vibration motor is connected to the screening device.

[0010] In conjunction with the third possible implementation of the first aspect, the present invention provides a fourth possible implementation of the first aspect, wherein the vibration motor is connected to the flipping drive in a transmission manner.

[0011] In conjunction with the first aspect, the present invention provides a fifth possible implementation of the first aspect, wherein the powder scraping module includes: a rotating clamp, a powder scraping head holder, and a three-axis module; The rotating clamp is used to hold the grinding jar and drive the grinding jar to rotate; The scraper head holder is installed on the movable end of the three-axis module, and the scraper head holder is used to connect the scraper paddle.

[0012] In conjunction with the fifth possible implementation of the first aspect, the present invention provides a sixth possible implementation of the first aspect, wherein the scraper head frame is equipped with a scraper drive device for driving the scraper paddle to rotate and / or vibrate.

[0013] In conjunction with the first aspect, the present invention provides a seventh possible implementation of the first aspect, wherein the bead-adding module includes a hopper, a material inlet opening and closing device, and a technical sensor; The bottom of the hopper is provided with a discharge port, and the discharge port opening and closing device and the technical sensor are both installed at the discharge port.

[0014] In conjunction with the first aspect, the present invention provides an eighth possible embodiment of the first aspect, wherein the sulfide solid electrolyte synthesis apparatus further includes a switch cover module for opening and closing the cover of the ball mill jar.

[0015] Secondly, the sulfide solid electrolyte synthesis method provided by the present invention uses the sulfide solid electrolyte synthesis equipment described in the first aspect, and includes the following steps: The sample addition module is controlled to quantitatively add solid powder into the ball mill jar; The bead-adding module is controlled to quantitatively input grinding beads into the grinding jar; The ball milling module is started and the solid powder is ball milled in the ball milling jar. The robotic arm is controlled to pour the solid powder and grinding beads in the ball mill jar into the sieving module, and the solid powder adhering to the inner wall of the ball mill jar is scraped off by the powder scraping module; The sintering module is started to sinter the solid powder that is sieved by the sieving module.

[0016] The embodiments of this invention bring the following beneficial effects: By constructing a fully enclosed, modular sulfide solid electrolyte synthesis equipment integrating sample addition, bead addition, ball milling, sieving, powder scraping, and sintering, the preparation efficiency, process consistency, and environmental safety of sulfide electrolyte materials are significantly improved. Each module is arranged in series according to process logic and supports dew point ≤ It operates continuously in an ultra-dry inert atmosphere at 60℃, effectively avoiding the safety risk of H2S generation when sulfide raw materials come into contact with moisture, reducing the reliance on manual intervention, and especially solving the problem that traditional high-energy ball mills require frequent exposure to the glove box during the clamping, fixing, and opening of the ball mill jar, which is cumbersome and prone to introducing impurities.

[0017] Furthermore, the sample addition module and the bead addition module enable quantitative, synchronous, and closed feeding of powder and milling beads; the sieving module and the powder scraping module work together to efficiently separate the ball milling products and recover residues from the tank walls, ensuring material yield and batch-to-batch repeatability; the sintering module directly connects to the sieved powder, avoiding contamination and moisture absorption caused by intermediate transfer. The entire system supports high-throughput synthesis and screening with adjustable parameters for multiple batches, providing a stable, clean, and scalable hardware foundation for the rapid iterative optimization of the composition, process, and performance of sulfide solid electrolytes, thus effectively responding to the core needs of industrialization for improved synthesis efficiency, reduced energy consumption, and controllable purity.

[0018] To make the above-mentioned objects, features and advantages of the present invention more apparent and understandable, preferred embodiments are described below in detail with reference to the accompanying drawings. Attached Figure Description

[0019] To more clearly illustrate the technical solutions in the specific embodiments or related technologies of the present invention, the drawings used in the description of the specific embodiments or related technologies will be briefly introduced below. Obviously, the drawings described below are some embodiments of the present invention. For those skilled in the art, other drawings can be obtained from these drawings without creative effort.

[0020] Figure 1 This is a schematic diagram of a sulfide solid electrolyte synthesis apparatus provided in an embodiment of the present invention; Figure 2 A schematic diagram of the sample feeding module of the sulfide solid electrolyte synthesis apparatus provided in an embodiment of the present invention; Figure 3 A schematic diagram of the ball mill module of the sulfide solid electrolyte synthesis equipment provided in an embodiment of the present invention; Figure 4 This is a schematic diagram of the internal structure of the ball mill module in the sulfide solid electrolyte synthesis equipment provided in an embodiment of the present invention. Figure 5 A schematic diagram of the sieving module of the sulfide solid electrolyte synthesis equipment provided in an embodiment of the present invention; Figure 6 This is a schematic diagram of the powder scraping module of the sulfide solid electrolyte synthesis equipment provided in an embodiment of the present invention.

[0021] Icons: 100-Sample feeding module; 101-Container position; 110-Material rack; 120-Vibrating feeding device; 200-Ball mill module; 210-Ball mill seat; 220-First rotary drive device; 230-Second rotary drive device; 240-Pressure fitting device; 300-Sieving module; 310-Clamping device; 320-Tilting drive device; 330-Sieving device; 340-Vibration motor; 400-Powder scraper module; 410-Rotating clamp; 420-Powder scraper head rack; 430-Triaxial module; 500-Sintering module; 600-Opening and closing cover module. Detailed Implementation

[0022] The technical solution of the present invention will now be clearly and completely described with reference to the accompanying drawings. Obviously, the described embodiments are only some, not all, of the embodiments of the present invention. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0023] In the description of this invention, it should be noted that the terms "center," "upper," "lower," "left," "right," "vertical," "horizontal," "inner," and "outer," etc., indicate the orientation or positional relationship based on the orientation or positional relationship shown in the accompanying drawings. They are used only for the convenience of describing the invention and for simplifying the description, and do not indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation. Therefore, they should not be construed as limitations on the invention. Furthermore, the terms "first," "second," and "third" are used only to describe differences in name and should not be construed as indicating or implying relative importance. Physical quantities in formulas, unless otherwise specified, should be understood as basic quantities in the International System of Units (SI), or derived quantities derived from basic quantities through mathematical operations such as multiplication, division, differentiation, or integration.

[0024] In the description of this invention, it should be noted that, unless otherwise explicitly specified and limited, the terms "installation," "connection," and "linking" should be interpreted broadly. For example, they can refer to a fixed connection, a detachable connection, or an integral connection; they can refer to a mechanical connection or an electrical connection; they can refer to a direct connection or an indirect connection through an intermediate medium; and they can refer to the internal connection of two components. Those skilled in the art can understand the specific meaning of the above terms in this invention based on the specific circumstances.

[0025] like Figure 1As shown, the sulfide solid electrolyte synthesis equipment provided in this embodiment of the invention includes: a sample addition module 100, a bead addition module, a ball milling module 200, a sieving module 300, a powder scraping module 400, and a sintering module 500; the sample addition module 100 and the bead addition module are both located upstream of the ball milling module 200. The sample addition module 100 is used to quantitatively add solid powder into the ball milling jar, and the bead addition module is used to quantitatively input ball milling beads into the ball milling jar; the sieving module 300 and the powder scraping module 400 are both located downstream of the ball milling module 200. The sieving module 300 is used to sieve the solid powder and the ball milling beads, and the powder scraping module 400 is used to scrape off the solid powder adhering to the inner wall of the ball milling jar; the sintering module 500 is located downstream of the sieving module 300 and is used to sinter the solid powder sieved by the sieving module 300.

[0026] Among them, the sulfide solid electrolyte synthesis equipment is integrated into the dew point ≤ Inside a 60℃ ultra-dry inert atmosphere glove box, the overall dimensions of the equipment are 8.2 meters long × 1.3 meters wide × 2.1 meters high. It consists of a sample feeding module 100, a bead feeding module, a ball milling module 200, a sieving module 300, a powder scraping module 400, and a sintering module 500 arranged sequentially along the process flow direction. The sample feeding module 100 and the bead feeding module are located upstream of the ball milling module 200, respectively responsible for the quantitative and closed feeding of solid powder and grinding beads. The ball milling module 200 completes the parallel mechanical activation of multiple tanks. The sieving module 300 and the powder scraping module 400... Located downstream of the ball milling module 200, the sintering module 500 separates the powder from the milling beads in the ball milling product and actively recovers the residual powder on the inner wall of the ball milling jar. Located downstream of the sieving module 300, the sintering module 500 directly receives the pure powder after sieving and performs controlled heat treatment. The modules work together with the robotic arm through standardized interfaces. The entire system operates in a closed loop under a sealed inert atmosphere, avoiding the risk of materials being exposed to environmental moisture and oxygen throughout the process, thereby preventing the hydrolysis of sulfide raw materials to produce H2S and insulating impurities such as LiOH / Li2CO3.

[0027] like Figure 1 and Figure 2 As shown, the sample feeding module 100 includes: a material rack 110 and a vibrating feeding device 120; the material rack 110 is provided with a plurality of circumferentially spaced holding positions 101, each holding position 101 being used to place a ball mill jar; the vibrating feeding device 120 is rotatably connected to the material rack 110, and the feeding port of the vibrating feeding device 120 corresponds to each holding position 101.

[0028] In an optional embodiment, the material rack 110 has a horizontal turntable structure with 10 holding positions 101 spaced circumferentially along its upper edge. Each holding position 101 is equipped with a weighing balance for placing and monitoring the mass of the ball mill jar in real time. The vibrating feeding device 120 is vertically raised and lowered by a top rod and driven to rotate by a motor, and integrates a vibration motor as an excitation source. The vibrating feeding device 120 is rotatably connected to the central axis of the material rack 110, so that its feeding port can be aligned sequentially with each holding position 101. During the sample addition process, the empty ball mill jar is first placed on the balance of any holding position 101 and tare and zeroed. Then, the control system retrieves the corresponding hopper according to the preset formula, controls the opening of the feeding port by adjusting the lifting position of the top rod, controls the stirring intensity of the stirring rod by adjusting the motor speed, and adjusts the feeding flow rate by adjusting the frequency of the vibration motor. Combined with the real-time reading feedback of the balance, the above three parameters are dynamically closed-loop adjusted to finally achieve a single solid powder sample addition accuracy of ±0.5mg. Alternatively, the rack 110 can also be designed as a linear slide rail array, which, together with a multi-station translation mechanism, enables the switching of the holding position.

[0029] like Figure 1 , Figure 3 and Figure 4 As shown, the ball milling module 200 includes: a ball milling base 210, a first rotary drive device 220, a second rotary drive device 230, and a pressing device 240; the ball milling base 210 is mounted on the first rotary drive device 220, which drives the ball milling base 210 to rotate; the ball milling base 210 has multiple ball milling stations, and each ball milling station is correspondingly equipped with a second rotary drive device 230, which drives the ball milling jar installed at the corresponding ball milling station to rotate; the pressing device 240 is located beside the ball milling base 210 and is used to press the ball milling jar into the ball milling station.

[0030] The ball mill base 210 is a four-station disc structure, installed at the output end of the first rotary drive device 220. Driven by the first rotary drive device 220, it rotates intermittently around its vertical axis, allowing each ball milling station to sequentially enter the clamping, grinding, and unloading positions. Each ball milling station is equipped with an independent second rotary drive device 230, whose output end is connected to the drive interface at the bottom of the ball mill jar, used to drive the ball mill jar to rotate at high speed around its own axis. The pressing device 240 is located beside the ball mill base 210 and includes two sets of electric push rods: one set drives the Y-shaped push rod to descend, causing the spring-loaded top ball inside the station to retract and make room; the other set drives the circular push rod to descend, pressing the ball mill jar to a preset height. At this time, the Y-shaped push rod rises, and the top ball pops out under the spring's reset action and is locked into the U-shaped grooves on both sides of the ball mill jar, completing the radial and axial degree of freedom constraints. The circular push rod then rises, realizing automatic clamping of a single jar. The pressing device 240 also integrates a photoelectric sensor to detect whether the ball mill jar is in place. Optionally, the annular and circular pressure rods in the pressing device 240 can be replaced with pneumatic rotary pressing cylinders; the ball mill jar locking method can also be replaced with top rod locking or threaded engagement, but it needs to be adapted to the automated execution logic.

[0031] like Figure 1 and Figure 5 As shown, the sieving module 300 includes: a clamping member 310, a tilting drive member 320, a sieving device 330, and a vibration motor 340; the clamping member 310 is used to clamp the ball mill jar, and the clamping member 310 is installed on the movable end of the tilting drive member 320; the sieving device 330 is located below the clamping member 310, and the vibration motor 340 is connected to the sieving device 330.

[0032] The clamping component 310 is a parallel electric gripper structure, installed on the movable end of the tilting drive component 320, used to clamp the ball mill jar after the lid opening operation. The tilting drive component 320 is a servo-electric tilting mechanism that can drive the clamping component 310 to tilt around the horizontal axis to the tilting angle. The sieving device 330 is a funnel structure with a built-in filter screen. The filter screen aperture is adapted to the ball milling bead particle size, and the bottom opening of the funnel faces the crucible below. The vibration motor 340 is fixed to the outer wall of the funnel, providing vertical excitation force. During operation, the robotic arm hands the opened ball mill jar to the clamping component 310 for clamping, the tilting drive component 320 drives it to tilt, and at the same time, the vibration motor 340 starts, causing the powder in the jar to accelerate away from the jar wall under the assistance of vibration and fall into the crucible through the filter screen, while the ball milling beads are trapped above the filter screen. Optionally, the sieving device 330 can be replaced with a double-layer vibrating filter screen structure, or high-pressure inert gas can be used to purge and assist powder falling, but an additional air source and pressure stabilization unit are required.

[0033] Furthermore, the vibration motor 340 is connected to the tilting drive 320 via a transmission connection. The output shaft of the vibration motor 340 is rigidly connected to the housing of the tilting drive 320 via a coupling. This allows the vibration energy generated by the vibration motor 340 during operation to be transmitted through the housing of the tilting drive 320 to the clamping member 310 and the ball mill jar it is clamped. This simultaneously stimulates the micro-vibration of the jar during the tilting process, significantly improving the efficiency of removing the adhering powder. This transmission connection method avoids the need for an additional jar vibration mechanism, simplifies the structure, and enhances the efficiency of vibration energy utilization.

[0034] like Figure 1 and Figure 6 As shown, the scraper module 400 includes: a rotary clamp 410, a scraper head holder 420, and a three-axis module 430; the rotary clamp 410 is used to clamp the ball mill jar and drive the ball mill jar to rotate; the scraper head holder 420 is installed on the movable end of the three-axis module 430, and the scraper head holder 420 is used to connect the scraper paddle. The rotary clamp 410 is a rotary electric gripper with a servo motor, used to clamp the ball mill jar and drive it to rotate at a low and uniform speed around its own axis; the scraper head rack 420 is a double-layer bracket structure, with the upper layer storing unused scraper blades and the lower layer storing used scraper blades; the scraper head rack 420 is installed on the movable end of the three-axis module 430, which consists of three-way linear motors and guide rails, and can drive the scraper head rack 420 to be precisely positioned in three-dimensional space; during operation, the three-axis module 430 moves the scraper head rack 420 to the scraper blade pick-up and drop position, the lifting module descends to allow the quick-change head to align with the scraper blade, and the quick-change head completes the gripping through the pneumatic steel ball locking mechanism, then the three-axis module 430 returns to the origin, the lifting module rises to the designated height, the rotary clamp 410 moves the ball mill jar to directly below the scraper blade, the lifting module descends to allow the scraper blade to be inserted into the jar, and the scraping operation is started. Optionally, the scraper head rack 420 can be replaced with a single-layer or multi-layer rack, and the scraper blade after use can be separately set up for recycling; the quick-change head can also be replaced with a conical clamp type, threaded locking type or pneumatic / hydraulic tensioning type structure.

[0035] Furthermore, the scraper head holder 420 is equipped with a scraper drive mechanism, which drives the scraper blade to rotate and / or vibrate. A vibration motor is fixed to the quick-change head, driving the scraper blade to vibrate axially at high frequency and small amplitude. The quick-change head has two limit pins that engage with the grooves on the scraper blade handle to prevent relative slippage during rotation and vibration. During scraping, the rotating clamp 410 drives the ball mill jar to rotate at low speed, and the scraper blade rotates and vibrates synchronously, efficiently stripping powder adhering to the jar wall under the combined action of multiple motions. In addition, the transmission method of the scraper drive mechanism can be replaced with gear transmission.

[0036] Furthermore, the ball-feeding module includes a hopper, a feed inlet opening / closing device, and technical sensors. The bottom of the hopper has a discharge port, where the opening / closing device and technical sensors are installed. A through-beam photoelectric sensor is installed at the hopper discharge port to detect whether the grinding balls pass through and perform initial screening and counting. The grinding balls fall through the discharge port into a rotary buffer position. The rotary table has 18 buffer slots, driven by a stepper motor. When a buffer slot reaches the discharge position, a proximity switch below it detects whether the grinding balls slide out smoothly. The grinding balls are guided by a chute at the discharge port and accurately fall into the grinding jar below. The entire process is coordinated by a PLC controller based on a preset grinding ball quantity command, coordinating the electric actuator, rotary table positioning, and sensor feedback to achieve quantitative, synchronous, and impact-free feeding of the grinding balls. Additionally, the counting sensor can be replaced with an image recognition sensor or a weight sensing feedback system.

[0037] Furthermore, the sulfide solid electrolyte synthesis equipment also includes a cover switching module 600, which is used to open and close the cover of the ball mill jar. The cover switching module 600 includes a gripper assembly, a lifting device, and a torque feedback motor. The gripper assembly adopts an adaptive envelope structure, compatible with the outer contours of ball mill jar covers of different specifications. The lifting device drives the gripper assembly to move vertically, completing the entire process of gripping, lifting, rotating to loosen / tighten, and pressing back the cover. The torque feedback motor monitors the tightening torque in real time, ensuring sealing reliability and avoiding excessive torque damage to the jar threads. The entire cover opening and closing operation is completed within the inert atmosphere of the glove box, eliminating the risk of environmental intrusion during the opening process. This module, in conjunction with the robotic arm, constitutes a key guarantee for the closed feeding, closed grinding, and closed transfer of the ball mill jar.

[0038] The sulfide solid electrolyte synthesis method provided in this embodiment of the invention uses the sulfide solid electrolyte synthesis equipment described in the above embodiments, and includes the following steps: Step S001: Control the sample addition module 100 to quantitatively add solid powder to multiple ball mill jars respectively. The type and mass of the sample added to each jar are independently set according to the preset formula, and the sample addition accuracy is controlled within ±0.5 mg. S002: The ball bead feeding module controls the quantitative input of grinding balls into each grinding jar. The input quantity is set according to the ball-to-material ratio parameter and is verified by both photoelectric sensor and proximity switch. S003: Control the switch cover module 600 to complete the sealing and closing of each grinding jar; control the robotic arm to transfer the sealed jar to the grinding station of the grinding module 200, where the clamping device 240 automatically completes the clamping; control the grinding module 200 to start, and each grinding jar synchronously performs high-energy grinding under the drive of the independent second rotary drive device 230; S004: After ball milling, the control switch cover module 600 opens the cover; the control robotic arm transfers the opened ball mill jar to the screening module 300, where it is clamped by the clamping member 310 and then tilted by the flipping drive member 320, while the vibration motor 340 is started simultaneously to excite the screening; after the tilting is completed, the control robotic arm transfers the empty jar to the powder scraping module 400, where it is clamped by the rotating clamp 410 and rotated at low speed. The three-axis module 430 drives the scraper to insert into the jar, and the powder scraping drive member is started, driving the scraper to rotate and vibrate to scrape off the residual powder on the inner wall; S005: Control the robotic arm to collect all the powder after scraping and recovery into the same crucible, and then place the crucible into the sintering module 500; control the opening of the furnace door of the sintering module 500, the robotic arm to send the crucible into the furnace chamber, and after the furnace door is closed, execute the entire process of heating-holding-cooling according to the preset program. The sintering atmosphere is continuously supplied with high-purity argon gas, and the dew point is maintained at ≤ 60℃; After sintering, the robotic arm removes the crucible and transfers it to the subsequent characterization process; The entire process operates in a fully automated closed loop under an ultra-dry inert atmosphere, requiring no manual intervention for tank loading and unloading, powder transfer, or atmosphere maintenance. This effectively avoids the release of H2S and the generation of side reaction impurities caused by moisture and oxygen, ensuring the phase purity, ionic conductivity, and batch consistency of the obtained sulfide solid electrolyte.

[0039] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention, and not to limit them; although the present invention has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some or all of the technical features; and these modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the scope of the technical solutions of the embodiments of the present invention.

Claims

1. A sulfide solid electrolyte synthesis apparatus, characterized in that, include: Sample addition module (100), bead addition module, ball milling module (200), sieving module (300), powder scraping module (400) and sintering module (500); The sample addition module (100) and the bead addition module are both located upstream of the ball milling module (200). The sample addition module (100) is used to quantitatively add solid powder into the ball milling jar, and the bead addition module is used to quantitatively input ball milling beads into the ball milling jar. The sieving module (300) and the powder scraping module (400) are both located downstream of the ball milling module (200). The sieving module (300) is used to sieve solid powder and grinding beads, and the powder scraping module (400) is used to scrape off the solid powder adhering to the inner wall of the ball milling jar. The sintering module (500) is located downstream of the sieving module (300) and is used to sinter the solid powder that passes through the sieving module (300).

2. The sulfide solid electrolyte synthesis apparatus according to claim 1, characterized in that, The sample feeding module (100) includes: a material rack (110) and a vibrating material feeding device (120); The material rack (110) is provided with a plurality of circumferentially spaced holding positions (101), each of which is used to hold the ball mill jar; The vibrating discharge device (120) is rotatably connected to the material rack (110), and the discharge port of the vibrating discharge device (120) corresponds to each of the holding positions (101).

3. The sulfide solid electrolyte synthesis apparatus according to claim 1, characterized in that, The ball mill module (200) includes: a ball mill base (210), a first rotary drive device (220), a second rotary drive device (230), and a press-fit device (240). The ball mill base (210) is mounted on the first rotary drive device (220), and the first rotary drive device (220) is used to drive the ball mill base (210) to rotate; The ball milling stand (210) is provided with multiple ball milling stations, and each ball milling station is equipped with a corresponding second rotary drive device (230). The second rotary drive device (230) is used to drive the ball milling jar installed at the corresponding ball milling station to rotate. The pressing device (240) is located beside the ball mill base (210), and the pressing device (240) is used to press the ball mill jar into the ball milling station.

4. The sulfide solid electrolyte synthesis apparatus according to claim 1, characterized in that, The sieving module (300) includes: a clamping member (310), a tilting drive member (320), a sieving device (330), and a vibration motor (340). The clamping member (310) is used to clamp the ball mill jar, and the clamping member (310) is mounted on the movable end of the flipping drive member (320); The screening device (330) is located below the clamping member (310), and the vibration motor (340) is connected to the screening device (330).

5. The sulfide solid electrolyte synthesis apparatus according to claim 4, characterized in that, The vibration motor (340) is connected to the flipping drive (320) in a transmission connection.

6. The sulfide solid electrolyte synthesis apparatus according to claim 1, characterized in that, The powder scraping module (400) includes: a rotating clamp (410), a powder scraping head rack (420), and a three-axis module (430). The rotating clamp (410) is used to clamp the grinding jar and drive the grinding jar to rotate; The scraper head holder (420) is installed on the movable end of the three-axis module (430), and the scraper head holder (420) is used to connect the scraper paddle.

7. The sulfide solid electrolyte synthesis apparatus according to claim 6, characterized in that, The scraper head holder (420) is equipped with a scraper drive mechanism, which is used to drive the scraper paddle to rotate and / or vibrate.

8. The sulfide solid electrolyte synthesis apparatus according to claim 1, characterized in that, The bead-adding module includes a hopper, a material inlet opening and closing device, and technical sensors; The bottom of the hopper is provided with a discharge port, and the discharge port opening and closing device and the technical sensor are both installed at the discharge port.

9. The sulfide solid electrolyte synthesis apparatus according to claim 1, characterized in that, The sulfide solid electrolyte synthesis equipment also includes a switch cover module (600) for opening and closing the cover of the ball mill jar.

10. A method for synthesizing a sulfide solid electrolyte, characterized in that, The method for synthesizing sulfide solid electrolytes uses the sulfide solid electrolyte synthesis equipment described in any one of claims 1-9, and includes the following steps: The sample addition module (100) is controlled to quantitatively add solid powder into the ball mill jar; The bead-adding module is controlled to quantitatively input grinding beads into the grinding jar; The ball milling module (200) is started and the solid powder is ball milled in the ball milling jar. The robotic arm is controlled to pour the solid powder and grinding balls in the ball mill jar into the sieving module (300), and the solid powder adhering to the inner wall of the ball mill jar is scraped off by the powder scraping module (400); The sintering module (500) is started to sinter the solid powder sieved by the sieving module (300).

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