High-shear dynamic mixing reaction device for preparing flexible particles and dynamic processing technology

Abstract

The application discloses a high-shear dynamic mixing reaction device for preparing flexible particles and a dynamic processing technology, relates to the technical field of battery raw material preparation, and is characterized in that the technology adopts a pulsating stress dynamic processing method to prepare flexible particle materials for batteries in a compact space on the basis of an existing chemical formula, the performance obtained from a material formula and the performance obtained from the pulsating stress dynamic processing are complementary to each other to form an organic whole, the reaction device comprises a cylinder body, a feeding port is formed in the top of the cylinder body, and a discharging port is formed in the bottom of the cylinder body, a kneading and overturning mixing mechanism is arranged, the rotation of a stirring shaft is used as the driving force of a sliding block, the sliding block reciprocatingly slides in a fixed sleeve, upward and downward pressure is provided for materials in the cylinder body, the setting of triangular fins on a baffle can provide better shearing force for moderately rotating material particles, the materials are continuously kneaded, rubbed and overturned, tend to be circular, and can make carbon coating more uniform.

Description

Technical Field

[0001] This invention relates to the field of battery raw material preparation technology, specifically to a high-shear dynamic mixing reaction device and dynamic processing technology for preparing flexible particles. Background Technology

[0002] Traditional high-temperature solid-state methods generally use chemical formulas to manufacture electrode materials. Since the materials being processed are in a static state during the preparation process, and are heated under the action of moving equipment, the mechanical parameters of the materials being processed (such as elastic modulus E) do not change significantly during the preparation process. At the same time, the carbon coating is also formed under static conditions through the relationship between time and viscosity. The static materials in the preparation process do not have the conditions for mutual mixing. Therefore, the consistency of the synthesized product is relatively poor.

[0003] During the operation of battery materials, lithium ions carrying electrons shuttle through the material during the transmission process. When lithium ions flow into the material, it expands, and when they flow out of the material, it contracts. The expansion and contraction of the material creates flow stress, which is diffusion stress. As lithium ions flow in and out, the diffusion stress cycles and forms fatigue stress. This fatigue stress is the main factor causing battery particle damage and failure.

[0004] To achieve better conductivity, the coated carbon needs to be formed in an orderly manner with a high degree of graphitization. However, in the subsequent sintering process, the sintering temperature is determined by the electrical properties of the battery material, which is generally around 700℃. It is difficult to reach the sintering temperature required for needle coke (which has a significantly higher degree of order and graphitization than ordinary coke) of about 1450℃. Therefore, the degree of graphitization will inevitably decrease.

[0005] In existing technologies, firstly, high-energy-consuming sand mills are used to crush raw materials into nanoparticles through the impact force of grinding balls for several hours. Generally, the particle diameter (d50) can reach about 500 nanometers. If the particle diameter (d50) is further reduced to less than 500 nanometers, the energy consumption will increase exponentially, and the morphology cannot be guaranteed to be spherical. Secondly, the material is transported by dynamic equipment and synthesized in a static form at an appropriate temperature for several hours. This process is mainly based on chemical reaction synthesis, which has little improvement on the orderliness and mechanical properties of the coated carbon in the material. Finally, the material is then subjected to high-temperature sintering and lattice shaping in a static form for several hours. Although the purpose of heating is sintering and lattice shaping, the heat transfer of the material will take up a lot of time, resulting in unnecessary energy consumption.

[0006] In addition, current dynamic mixing reactors are highly targeted. For certain reactions in the preparation of battery nanomaterials that are sensitive to stirring intensity, over-stirring can easily occur, leading to side reactions or a decline in product quality. Therefore, additional mixing devices are usually required, which increases equipment costs.

[0007] Therefore, in view of this, the present invention proposes a high-shear dynamic mixing reaction device and dynamic processing technology for preparing flexible particles to make up for and improve the deficiencies of the prior art. Summary of the Invention

[0008] To address the aforementioned technical problems, this invention proposes a high-shear dynamic mixing reaction device and dynamic processing technology for preparing flexible particles. This addresses the issues in existing technologies, such as the high diffusion stress of lithium ions during material shuttle, which reduces battery life, low orderliness of coated carbon, low consistency (insufficient uniformity) of prepared products, and low applicability of the device.

[0009] To achieve the above objectives, the technical solution adopted by this invention is as follows: a high-shear dynamic mixing reaction device and dynamic processing technology for preparing flexible particles, comprising a cylinder, wherein a feed inlet is provided at the top of the cylinder, a discharge outlet is provided at the bottom of the cylinder, a jacket is fixedly connected to the outer wall of the bottom of the cylinder, a spiral guide plate is fixedly connected to the inner wall of the jacket, and the side of the spiral guide plate away from the jacket is fixedly connected to the outer wall of the cylinder, and further comprising:

[0010] The kneading and mixing mechanism is used to provide reciprocating pressure and high shear mixing to the material inside the cylinder;

[0011] An adaptive gas distribution mechanism is used to automatically adjust the gas distribution range to adapt to the mixing of different types of flexible particles in the device.

[0012] Preferably, the kneading and mixing mechanism includes a stirring shaft rotatably connected to the top of the cylinder, the bottom end of the stirring shaft extending to the bottom of the cylinder, a motor fixedly connected to the top of the cylinder, the top of the stirring shaft penetrating the top of the cylinder and fixedly connected to the output end of the motor, a pair of protrusions fixedly connected to the middle of the stirring shaft, a stirrer slidably connected to the outer walls of the stirring shaft and the protrusions, a telescopic sleeve fixedly connected to the top of the stirrer, and the inner wall of the telescopic sleeve slidably sleeved on the outer wall of the stirring shaft.

[0013] Preferably, the kneading and mixing mechanism further includes a pair of sliders fixedly connected to the top of the telescopic sleeve. The outer wall of the telescopic sleeve is slidably sleeved with a fixed sleeve. The inner wall of the fixed sleeve is provided with a reciprocating threaded groove. The outer walls of the pair of sliders are slidably connected to the reciprocating threaded groove. A support frame is fixedly connected to the top of the fixed sleeve. The top of the support frame is fixedly connected to the top inner wall of the cylinder. Multiple baffles are fixedly connected at equal intervals to the inner wall of the cylinder. Several triangular fins are fixedly connected to both sides of each baffle.

[0014] Preferably, the adaptive gas distribution mechanism includes a turntable fixedly connected to the bottom of the stirring shaft. Multiple limiting sleeves are fixedly connected at equal intervals to the outer wall of the turntable. Sliding rods are slidably connected to the inner walls of the multiple limiting sleeves. Rotating blades are fixedly connected to the side of the multiple sliding rods away from the turntable. A spring is fixedly connected to the side of the sliding rods near the turntable. The side of the springs away from the sliding rods is fixedly connected to the inner wall of the turntable.

[0015] Preferably, the adaptive gas distribution mechanism further includes a gas distributor fixedly connected to the inner wall of the bottom of the cylinder. The gas distributor has several exhaust ports at its top and bottom. A gas inlet pipe is fixedly connected to the top of the gas distributor. The side of the gas inlet pipe away from the gas distributor is fixedly inserted through the outer wall of the cylinder and the jacket.

[0016] Preferably, the gas distributor is flower-shaped, with the top exhaust ports evenly distributed on the upper surface of the gas distributor and the bottom exhaust ports concentrated on the lower surface of the middle part of the gas distributor.

[0017] Preferably, the length of the fixed sleeve is set to one-third of the height of the cylinder.

[0018] Preferably, the triangular fins are arranged alternately on both sides of the baffle.

[0019] Preferably, the jacket has a heat transfer medium inlet at the bottom and a heat transfer medium outlet at the top.

[0020] A high-shear dynamic mixing reaction apparatus and dynamic processing technology for preparing flexible particles includes the following steps:

[0021] Step 1: High-shear mixing and strengthening process: The rotating device consists of two stationary rings and two rotating rings interlocked. The stationary rings have multiple small holes, and the rotating rings have cutters on their surfaces. The material enters the inner cavity of the rotating device from the center. Under the centrifugal force of the rotating device, it flows radially out through the small holes on the first stationary ring and flows out through the small holes on the second stationary ring. The rotating outer ring rotates in the narrow channel formed between the two stationary rings and forms a vertical shear with the material that flows radially out of the small holes on the first stationary ring and radially enters the second stationary ring. This process crushes and tears the material that is mainly subjected to high-speed shear, which can break through the bottleneck of 500nm particle diameter. However, the morphology of the processed particles is irregular.

[0022] Step 2: Dynamic synthesis and dynamic sintering process: Based on the original static temperature change synthesis principle, under temperature change conditions, dynamic synthesis and sintering with the combined action of rheological stress and rheological shear stress is added to accelerate thermochemical reaction and material mixing. Through the dynamic mixing reaction device, the material is subjected to pressure, shear force and friction in the cylinder, and is constantly kneaded and turned.

[0023] I. Rheological Process: The chemical reaction synthesis is carried out in a stirred cylinder. The reaction process is a highly efficient plug flow reaction. In this dynamic synthesis reactor, the volumetric flow rate of the material processed in the unit reaction space (cubic meters) is no more than 0.3 cubic meters per unit reaction time (hour). The material is mixed more than 100 times, which greatly improves the consistency of the material after the synthesis reaction.

[0024] II. Superplastic stage: In the latter half of the rheological process, under the dynamic action of pulsating stress at an appropriate temperature, the material undergoes particle deformation due to diffusion of grain boundary slip and dislocation grain boundary slip. When the strain rate reaches a suitable level, the material exhibits fine grain superplasticity.

[0025] Third, although dynamic sintering supplements some synthesis reactions, it also provides sintering function for lattice shaping. For high-temperature solid-state sintering, it saves sintering time, facilitates thorough sintering of materials, and reduces energy consumption.

[0026] IV. Carbon Coating Process: A dynamic stirring method with pulsating stress is adopted. Under the action of shear stress generated by stirring, cycloalkanes and polar aromatics can be removed quickly.

[0027] Condition 1: At the same temperature, the viscosity is reduced by stirring. The decrease in viscosity is conducive to the formation of mesophase microspheres, which provides a good foundation for the formation of coated carbon to develop in an ordered direction.

[0028] Condition 2: Within a suitable temperature range, more intermediate phases are generated by stirring. The more intermediate phases are generated in the coated carbon, the higher the degree of order of the coated carbon formed in the later sintering, and the higher the degree of graphitization.

[0029] Condition 3: Within a suitable temperature range, more and better intermediate phases are generated through time and agitation.

[0030] Compared with the prior art, the beneficial effects of the present invention are:

[0031] 1. When materials are dynamically mixed, the kneading and mixing mechanism uses the rotation of the stirring shaft as the driving force for the slider, which slides back and forth in the fixed sleeve. The slider eventually drives the agitator to move up and down synchronously, providing upward and downward pressure to the material in the cylinder. The agitator continuously squeezes the material and impacts the baffle for shearing and mixing. The triangular fins on the baffle provide better shearing force to the moderately rotating material particles, enhancing the shearing force. The material in the cylinder is subjected to effective pressure, shearing force and friction, and is constantly kneaded and turned over. After repeated kneading by the equipment, the particles deform and the grain boundaries slip. The elastic modulus of the material decreases, the strain rate sensitivity index m increases, and the flexibility increases. Under the same charge and discharge conditions, the probability of particle breakage failure can be greatly reduced. Furthermore, the strip or sheet-like material caused by high shear will gradually become round after kneading, which can make the carbon coating more uniform. With the temperature control of the jacket, a carbon shell is uniformly formed on the outer wall of the material particles.

[0032] 2. By setting up triangular fins and a gas distributor, the triangular fins not only increase the shear force of the material, but their staggered arrangement on both sides of the baffle increases the density of triangular fins on the baffle surface, which can accelerate the diffusion of heat from the jacket into the cylinder, improving the heat conduction effect. Combined with the use of a stirrer, the temperature of the material reaction is more uniform, and the response rate of the jacket to the temperature control inside the cylinder is improved. In addition, the flower-shaped gas distributor can avoid the baffle range and increase the airflow coverage area at the bottom of the cylinder. With the gas distributor's top and bottom ventilation, the material in the dead corner at the bottom of the cylinder can be concentrated and mixed into the middle of the cylinder, making the material suspension orderly and further enhancing the carbon coating effect.

[0033] 3. Through the adaptive gas distribution mechanism, when the rotating shaft is moderately agitated, the spring stretches under centrifugal force, causing the rotating blades to lengthen. This automatically expands the diameter range of the spiraling gas distribution, helping to disperse the gas more widely within the cylinder. The expanded gas distribution range also increases the contact area between the gas and the material, resulting in more uniform spacing between material particles and improved mass transfer efficiency. When the rotating shaft agitates at low speed, the rotating blades shorten. For some reactions sensitive to agitation intensity, low-speed agitation reduces the gas distribution range, preventing side reactions or product quality degradation caused by over-aggregation, thus helping to maintain... The system maintains the stability and controllability of the reaction system. Simultaneously, the length of the rotating blades is automatically adjusted according to the rotational speed of the stirring shaft. This allows for both moderate stirring during the preparation of battery raw materials to prevent particle agglomeration and low-speed stirring to avoid side reactions or product quality degradation caused by excessive stirring, thus increasing the applicability of the device. Furthermore, during the preparation process, the materials are subjected to shear strain under shear stress. The shear strain multiplied by the time the material endures the shear strain equals the shear strength. The greater the shear strength, the better the material mixes. With over 100 mixing cycles, the consistency of the synthesized material after the reaction is significantly improved. Attached Figure Description

[0034] Figure 1 This is a schematic diagram of the overall structure of a preferred embodiment of the present invention;

[0035] Figure 2 This is a three-dimensional sectional view of the cylindrical body shown in this invention;

[0036] Figure 3 As shown in this invention Figure 2 An enlarged 3D structural diagram at point A in the middle;

[0037] Figure 4 This is a schematic diagram of the structure of the gas distributor connection shown in this invention;

[0038] Figure 5 This is a schematic diagram of the structure of the telescopic sleeve connection shown in the present invention;

[0039] Figure 6 This is a schematic diagram of the structure of the triangular fin connection shown in this invention;

[0040] Figure 7 This is a schematic diagram of the slider connection structure shown in the present invention;

[0041] Figure 8 This is a schematic diagram of the structure of the convex strip connection shown in this invention;

[0042] Figure 9 This is a schematic diagram of the structure of the sliding rod connection shown in the present invention;

[0043] Figure 10 As shown in this invention Figure 9 Enlarged structural diagram at point B;

[0044] Figure 11 This is a schematic diagram of the morphology of the processed particles as shown in this invention;

[0045] Figure 12 These are TEM images of the particles after dynamic synthesis and dynamic sintering as shown in this invention.

[0046] Figure 13 This is a schematic diagram of the E(τ) and F(τ) functions of the rheological reaction shown in this invention;

[0047] Figure 14 This is a schematic diagram of the grain superplastic strain rate sensitivity index as shown in this invention;

[0048] Figure 15 This is a schematic diagram of the shear strain rate and shear stress curves shown in this invention;

[0049] Figure 16 This is a schematic diagram of the viscosity-time curves shown in this invention;

[0050] Figure 17 This is a schematic diagram of the yield and viscosity curves of the intermediate phase shown in this invention;

[0051] Figure 18 This is a schematic diagram of the yield and time curves of the carbon microspheres MCMB shown in this invention.

[0052] The numbers on the map are:

[0053] 1. Cylinder body; 2. Inlet; 3. Outlet; 4. Jacket; 5. Spiral guide plate;

[0054] 6. Kneading and mixing mechanism; 61. Support frame; 62. Fixed sleeve; 63. Telescopic sleeve; 64. Agitator; 65. Baffle; 66. Triangular fin; 67. Agitator shaft; 68. Reciprocating threaded groove; 69. Slider; 610. Raised bar;

[0055] 7. Adaptive gas distribution mechanism; 71. Rotating vane; 72. Gas inlet pipe; 73. Gas distributor; 74. Exhaust port; 75. Limiting sleeve; 76. Turntable; 77. Sliding rod; 78. Spring. Detailed Implementation

[0056] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. 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 skilled in the art without creative effort are within the scope of protection of the present invention.

[0057] Embodiment 1 of the present invention

[0058] Please refer to Figures 1 to 10 As shown:

[0059] To address the problems mentioned in the technical solutions, this application provides a high-shear dynamic mixing reaction apparatus for preparing flexible particles, including a cylinder 1, a feed inlet 2 at the top of the cylinder 1, a discharge outlet 3 at the bottom of the cylinder 1, a jacket 4 fixedly connected to the outer wall of the bottom of the cylinder 1, a spiral guide plate 5 fixedly connected to the inner wall of the jacket 4, and the side of the spiral guide plate 5 away from the jacket 4 fixedly connected to the outer wall of the cylinder 1, and further including:

[0060] The kneading and mixing mechanism 6 is used to provide reciprocating pressure and high shear mixing to the material inside the cylinder 1;

[0061] The adaptive gas distribution mechanism 7 is used to automatically adjust the gas distribution range to adapt to the mixing of different types of flexible particles in the device;

[0062] The kneading and mixing mechanism 6 includes a stirring shaft 67 rotatably connected to the top of the cylinder 1. The bottom end of the stirring shaft 67 extends to the bottom of the cylinder 1. A motor is fixedly connected to the top of the cylinder 1. The top of the stirring shaft 67 passes through the top of the cylinder 1 and is fixedly connected to the output end of the motor. A pair of protrusions 610 are fixedly connected to the middle of the stirring shaft 67. The outer walls of the stirring shaft 67 and the protrusions 610 are slidably connected to a stirrer 64. A telescopic sleeve 63 is fixedly connected to the top of the stirrer 64. The inner wall of the telescopic sleeve 63 is slidably sleeved on the outer wall of the stirring shaft 67.

[0063] The kneading and mixing mechanism 6 also includes a pair of sliders 69 fixedly connected to the top of the telescopic sleeve 63. The outer wall of the telescopic sleeve 63 is slidably sleeved with a fixed sleeve 62. The inner wall of the fixed sleeve 62 is provided with a reciprocating threaded groove 68. The outer walls of the pair of sliders 69 are slidably connected in the reciprocating threaded groove 68. The top of the fixed sleeve 62 is fixedly connected with a support frame 61. The top of the support frame 61 is fixedly connected to the top inner wall of the cylinder 1. Multiple baffles 65 are fixedly connected at equal intervals on the inner wall of the cylinder 1. Several triangular fins 66 are fixedly connected to both sides of the baffles 65.

[0064] The length of the fixed sleeve 62 is set to one-third of the height of the cylinder 1;

[0065] The triangular fins 66 are arranged alternately on both sides of the baffle 65;

[0066] The jacket 4 has a heat transfer medium inlet at the bottom and a heat transfer medium outlet at the top.

[0067] Wherein: the fixed sleeve 62 is used to ensure the reciprocating motion of the stirrer 64, and the triangular fins 66 are used to conduct heat from the jacket 4 to the cylinder 1.

[0068] The effects achieved by this embodiment are as follows: In the prior art, most stirring devices are fixed to the shaft, which may result in insufficient uniformity of material mixing and insufficient shear and friction forces on the material, leading to insufficient roundness of the strip or sheet-like material, thus affecting the uniformity of carbon coating. Compared with the prior art, through the implementation of this embodiment, the kneading and mixing mechanism 6 can use the rotation of the stirring shaft 67 as the driving force for the slider 69, causing the slider 69 to slide back and forth within the fixed sleeve 62. The slider 69 ultimately drives the stirrer 64 to move up and down synchronously, providing upward and downward pressure to the material in the cylinder 1, and the stirrer 64 continuously... The extruded material impacts the baffle 65 for shearing and mixing. The triangular fins 66 on the baffle 65 provide better shearing force to the moderately rotating material particles, enhancing the shearing intensity. This allows the material to withstand effective pressure, shearing force, and friction within the cylinder 1, continuously being kneaded and turned, gradually becoming more rounded, resulting in more uniform carbon coating. Simultaneously, during the above preparation process, the material is subjected to shear strain under shear stress. The shear strain multiplied by the time the material endures the shear strain equals the shear strength. The greater the shear strength, the better the material is mixed. This mixing process exceeds 100 times, significantly improving the consistency of the material after the synthesis reaction.

[0069] Further examples: Please refer to Figures 2 to 4 , Figures 8 to 10 As shown:

[0070] The adaptive gas distribution mechanism 7 includes a turntable 76 fixedly connected to the bottom of the stirring shaft 67. Multiple limiting sleeves 75 are fixedly connected at equal intervals on the outer wall of the turntable 76. Sliding rods 77 are slidably connected to the inner walls of the multiple limiting sleeves 75. Rotating blades 71 are fixedly connected to the side of the multiple sliding rods 77 away from the turntable 76. Springs 78 are fixedly connected to the side of the sliding rods 77 close to the turntable 76. The side of the springs 78 away from the sliding rods 77 is fixedly connected to the inner wall of the turntable 76.

[0071] The adaptive gas distribution mechanism 7 also includes a gas distributor 73 fixedly connected to the inner wall of the bottom of the cylinder 1. The gas distributor 73 has several exhaust ports 74 at its top and bottom. A gas inlet pipe 72 is fixedly connected to the top of the gas distributor 73. The side of the gas inlet pipe 72 away from the gas distributor 73 is fixedly inserted through the outer wall of the cylinder 1 and the jacket 4.

[0072] The gas distributor 73 is flower-shaped, with top exhaust ports 74 evenly distributed on the upper surface of the gas distributor 73, and bottom exhaust ports 74 concentrated on the lower surface of the middle part of the gas distributor 73.

[0073] Among them, the number of exhaust ports 74 on the gas distributor 73 is more at the top than at the bottom, and the baffles 65 are all located in the flower-shaped recess of the gas distributor 73.

[0074] The effects achieved by this embodiment are as follows: In the prior art, dynamic mixing reactors are highly targeted. For certain reactions in the preparation of battery nanomaterials that are sensitive to stirring intensity, over-stirring can easily occur, leading to side reactions or a decrease in product quality. Therefore, additional mixing devices are usually required, increasing equipment costs. Compared with the prior art, this embodiment, by setting an adaptive gas distribution mechanism 7, can automatically adjust the length of the rotating blade 71 according to the rotation speed of the stirring shaft 67. This allows for moderate stirring during the preparation of battery materials to prevent particle agglomeration, while also allowing for low-speed stirring to avoid side reactions or a decrease in product quality caused by excessive stirring, thus increasing the applicability of the device. At the same time, since the material is subjected to shear strain under shear stress during the above preparation process, the shear strain multiplied by the time the material is subjected to shear strain equals the shear strength. The greater the shear strength, the better the material is mixed. With more than 100 mixing cycles, the consistency of the material after the synthesis reaction is greatly improved.

[0075] Embodiment 2 of the present invention

[0076] A high-shear dynamic mixing reaction apparatus and dynamic processing technology for preparing flexible particles includes the following steps:

[0077] Step 1: High-shear mixing and strengthening process: The rotating device consists of two stationary rings and two rotating rings interlocked. The stationary rings have multiple small holes, and the rotating rings have cutters on their surfaces. The material enters the inner cavity of the rotating device from the center. Under the centrifugal force of the rotating device, it flows radially out through the small holes on the first stationary ring and flows out through the small holes on the second stationary ring. The rotating outer ring rotates in the narrow channel formed between the two stationary rings and forms a vertical shear with the material that flows radially out of the small holes on the first stationary ring and radially enters the second stationary ring. This process crushes and tears the material that is mainly subjected to high-speed shear, which can break through the bottleneck of 500nm particle diameter. However, the morphology of the processed particles is irregular.

[0078] like Figure 11 The diagram shows the morphology of the processed particles.

[0079] Step 2: Dynamic Synthesis and Dynamic Sintering Process: Based on the original static temperature change synthesis principle, dynamic synthesis and sintering with the combined action of rheological stress and rheological shear stress are added under temperature change conditions to accelerate thermochemical reaction and material mixing. The morphology of the processed particles is irregular, which has a negative impact on the compaction density and electrochemical performance of the battery products. However, combined with the subsequent dynamic synthesis process, through the dynamic mixing reaction device, the material is subjected to pressure, shear force and friction in the cylinder 1, and is constantly kneaded and turned. During the dynamic synthesis and kneading process, the morphology of the material particles will also become closer to the spherical shape, just like kneading coal balls.

[0080] like Figure 12 The image shown is a TEM image of the particles after dynamic synthesis and dynamic sintering.

[0081] I. Rheological Process: The chemical synthesis reaction takes place in a stirred cylinder 1. This reaction process is a highly efficient plug flow reaction, and its E(τ) and F(τ) functions are as follows: Figure 13 The curves of the functions of the plug flow reactor shown are given, where E(τ) is the residence time distribution density function and F(τ) is the cumulative residence time distribution function.

[0082] II. Superplastic Stage: In the latter half of the rheological process, under the dynamic action of pulsating stress at an appropriate temperature, accompanied by diffuse grain boundary slip and dislocation grain boundary slip, the material deforms. When the strain rate reaches a suitable level, the material exhibits fine-grained superplasticity. Its grain superplastic strain rate sensitivity index is as follows: Figure 14 As shown in the figure; where V is the deformation rate; m is the strain rate sensitivity index, G is the maximum point, and D is the steady point;

[0083] The strain rate sensitivity index (m) is used to measure the superplasticity of a material, and it is described using the single maximum velocity jump method as follows:

[0084]

[0085] Where σ and ε are the true stress and the true strain rate, respectively;

[0086] Grain boundary sliding (GBS) is the main deformation mechanism of superplastic deformation. GBS operates in polycrystalline materials under four important prerequisites: first, it requires very small grain size, usually less than 15 μm; second, the deformation temperature should be relatively high, at 160 °C or above; third, the strain rate ε < 0.3 1 / S; and fourth, the stress on the material should be greater than 3 MPa. These four prerequisites control the degree of dynamic change of pulsating stress (compressive stress), adjust the elastic modulus of the material, and change the material's flexibility. With the strain rate sensitivity index m as the indicative parameter, it has rapidly evolved into the basic principle for designing superplastic materials.

[0087] The slip of crystals in this dynamic synthesis reactor means that the volumetric flow rate of the material processed per unit reaction time (hour) and per unit reaction space (cubic meter) is no greater than 0.3 cubic meters.

[0088] III. Although dynamic sintering supplements some synthesis reactions, it also provides sintering functions for lattice shaping. For high-temperature solid-state sintering, it saves sintering time, facilitates thorough sintering of materials, and reduces energy consumption. Table 1 shows the curve relationship between strain rate sensitivity index, elastic modulus, and diffusion stress. Table 2 shows the cycle life test results. Table 3 shows the comparison results of discharge rate and discharge time. Table 4 shows the test results of discharge temperature at the discharge rate. Table 5 shows the test results of impact parameters (safety).

[0089] Table 1. Relationship between strain rate sensitivity index and elastic modulus and diffused stress.

[0090]

[0091] Among them, the measured elastic modulus and strain rate sensitivity index of the cathode material in working condition 1, and the data of the cathode material in working condition 2 are from the literature;

[0092] Table 2 Cycle life test

[0093]

[0094] Table 3 Comparison of Discharge Rate and Discharge Time

[0095]

[0096] Table 4 Discharge Temperature at High Rate

[0097]

[0098] Table 5 Impact Parameters (Safety)

[0099]

[0100] IV. Carbon Coating Process: A dynamic stirring method with pulsating stress is adopted. Under the action of shear stress generated by stirring, cycloalkanes and polar aromatics can be removed quickly.

[0101] Condition 1: At the same temperature, stirring generates shear stress and shear strain to reduce viscosity. The decrease in viscosity is conducive to the formation of mesophase microspheres, providing a good foundation for the formation of coated carbon to develop in an ordered direction.

[0102] Example 1

[0103] Equal temperature

[0104]

[0105] like Figure 15 The figure shows a schematic diagram of shear strain rate and shear stress curves;

[0106] Example 2

[0107] The relationship between time and viscosity of a certain medium-temperature coal tar pitch is as follows:

[0108]

[0109] like Figure 16 The figure shown is a schematic diagram of viscosity-time curves;

[0110] As can be seen from the data table, in the dynamic synthesis reactor, at the same temperature, the shorter the residence time of the organic CH compound from melting into a liquid phase to forming an intermediate phase, the better for reducing viscosity. At 390℃, if the residence time of the liquid phase organic CH compound is reduced from 3h to 0.1h, the viscosity decreases from 0.716 to 0.315 Pa*s, a decrease of 2.27 times.

[0111] Condition 2: Within a suitable temperature range, more intermediate phases are generated by stirring. The more intermediate phases are generated in the coated carbon, the higher the degree of order of the coated carbon formed in the later sintering, and the higher the degree of graphitization.

[0112] like Figure 17 The figure shows a schematic diagram of the mesophase yield and viscosity curves. It can be seen from the figure that the lower the viscosity, the higher the mesophase yield.

[0113] Condition 3: Within a suitable temperature range, more and better intermediate phases are generated through time and agitation;

[0114] like Figure 18 The figure shows a schematic diagram of the yield and time curve of carbon microspheres MCMB. It can be seen from the figure that the longer the time, the higher the yield of carbon microspheres.

[0115] The complete usage steps and working principle of the above embodiments are as follows:

[0116] In the initial state: the stirring shaft 67 is stationary, the slider 69 is located at the bottom of the reciprocating threaded groove 68, the spring 78 is in a naturally relaxed state, and the sliding rod 77 is retracted into the inner wall of the limiting sleeve 75.

[0117] Work process:

[0118] In operation, the operator first feeds the highly sheared nano-sized material particles into the cylinder 1 through the feed inlet 2. Simultaneously, the gas distributor 73 is activated to blow air, suspending the material particles within the cylinder 1. Meanwhile, the heating medium is discharged from the heat transfer medium inlet into the jacket 4, spiraling upwards through the spiral guide plate 5 to fill the jacket 4, thus heating the inside of the cylinder 1. Next, the motor is started, driving the stirring shaft 67 to rotate. Under the limiting action of the protruding strip 610, the stirrer 64 and the telescopic sleeve 63 move with the stirring shaft. 67. Due to the support frame 61 being sleeved on the outer wall of the telescopic sleeve 63, and the slider 69 being slidably connected within the reciprocating threaded groove 68, the rotation of the telescopic sleeve 63 drives the slider 69 to rotate synchronously. The rotating slider 69 spirals upward along the groove of the reciprocating threaded groove 68, thereby driving the telescopic sleeve 63 and the agitator 64 upward together until the slider 69 reaches the top of the fixed sleeve 62. Due to the reciprocating nature of the reciprocating threaded groove 68, the slider 69 can move upward along the reciprocating threaded groove. The grooves of the groove 68 move downwards and back in a continuous manner, causing the agitator 64 to reciprocate up and down during rotation. Since the length of the fixed sleeve 62 is set to one-third of the height of the cylinder 1, the reciprocating movement range of the agitator 64 is the middle of the cylinder 1, which is the position where the gas distributor 73 blows and concentrates the material. This is beneficial for the agitator 64 to continuously tumble the suspended material up and down, increasing the friction and pressure on the material. At the same time, with the triangular fins 66, the tips of the triangular fins 66 face outwards, which can provide better shearing force for the moderately rotating material particles. The material is continuously kneaded and turned inside the cylinder 1, gradually becoming more rounded, thereby improving the uniformity of mixing, so that the material particles can be better and more evenly carbonized. In addition, the triangular fins 66 are arranged alternately on both sides of the baffle 65, which increases the density of the triangular fins 66 on the surface of the baffle 65, improving the heat conduction effect of the baffle 65, thereby improving the response rate of the jacket 4 to the internal temperature control of the cylinder 1.

[0119] Please refer to the above work process. Figures 1 to 2 , Figures 5 to 8 .

[0120] Furthermore, the flower-shaped gas distributor 73 can avoid the area of ​​the baffle 65, ensuring that the gas blown out by the gas distributor 73 effectively covers the bottom area of ​​the cylinder 1. The gas distributor 73 can also vent from both the top and bottom. The gas blown downwards from the exhaust port 74 can agitate the small amount of material falling to the bottom of the cylinder 1, giving the material particles a pushing force, causing the material to move upwards along the arc of the bottom of the cylinder 1. Combined with the upward blowing from the top exhaust port 74, the material is concentrated and mixed into the middle of the cylinder 1, thereby reducing mixing dead zones. Simultaneously, as the stirring shaft 67 rotates, the bottom turntable 76 also rotates. When the mixture inside the cylinder 1 is undergoing a carbon coating process, high-speed stirring is required to reduce the viscosity between material particles. At this time, the turntable 76, rotating at high speed with the stirring shaft 67, generates centrifugal force. The rotating blade 71 drives the sliding rod 77 to slide out from the limiting sleeve 75, stretching... Spring 78 moves the rotating blade 71 away from the limiting sleeve 75, which is equivalent to increasing the length of the rotating blade 71 and increasing its rotation diameter. In conjunction with the gas distributor 73 continuously discharging gas upward, the rotating blade 71 can agitate the vertically upward gas to form a spiral upward gas. The increase in the rotation diameter of the rotating blade 71 expands the diameter range of the spiral upward gas, thereby increasing the contact area between the gas and the material, making the spacing between material particles more uniform, and thus improving the mass transfer efficiency. When the reaction in the cylinder 1 is sensitive to the stirring intensity, the stirring shaft 67 needs to stir at a low speed. At this time, almost no centrifugal force is generated. Therefore, the spring force of spring 78 can reset the sliding rod 77, so that the rotation diameter of the rotating blade 71 is reduced, avoiding side reactions or product quality degradation caused by excessive stirring. In this way, the length of the rotating blade 71 can be adaptively adjusted to increase the adaptability of the device to mixing different materials.

[0121] Please refer to the above work process. Figures 2 to 4 , Figures 8 to 10 .

[0122] The circuits and instrument controls involved in this invention are all existing technologies and will not be described in detail here.

[0123] Although embodiments of the invention 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 to these embodiments without departing from the principles and spirit of the invention, the scope of which is defined by the appended claims and their equivalents.

Claims

1. A high-shear dynamic mixing reaction apparatus for preparing flexible particles, comprising a cylindrical body (1), wherein a feed inlet (2) is provided at the top of the cylindrical body (1), a discharge outlet (3) is provided at the bottom of the cylindrical body (1), a jacket (4) is fixedly connected to the outer wall of the bottom of the cylindrical body (1), a spiral guide plate (5) is fixedly connected to the inner wall of the jacket (4), and the side of the spiral guide plate (5) away from the jacket (4) is fixedly connected to the outer wall of the cylindrical body (1), characterized in that, It also includes: The kneading and mixing mechanism (6) is used to provide reciprocating pressure and high shear mixing to the material inside the cylinder (1); An adaptive gas distribution mechanism (7) is used to automatically adjust the gas distribution range to adapt to the mixing of different types of flexible particles in the device; The kneading and mixing mechanism (6) includes a stirring shaft (67) rotatably connected to the top of the cylinder (1). The bottom end of the stirring shaft (67) extends to the bottom of the cylinder (1). A motor is fixedly connected to the top of the cylinder (1). The top of the stirring shaft (67) passes through the top of the cylinder (1) and is fixedly connected to the output end of the motor. A pair of protrusions (610) are fixedly connected to the middle of the stirring shaft (67). A stirrer (64) is slidably connected to the outer walls of the stirring shaft (67) and the protrusions (610). A telescopic sleeve (63) is fixedly connected to the top of the stirrer (64). The inner wall of the telescopic sleeve (63) is slidably sleeved on the outer wall of the stirring shaft (67). The kneading and mixing mechanism (6) also includes a pair of sliders (69) fixedly connected to the top of the telescopic sleeve (63). The outer wall of the telescopic sleeve (63) is slidably sleeved with a fixed sleeve (62). The inner wall of the fixed sleeve (62) is provided with a reciprocating thread groove (68). The outer walls of the pair of sliders (69) are slidably connected in the reciprocating thread groove (68). The top of the fixed sleeve (62) is fixedly connected with a support frame (61). The top of the support frame (61) is fixedly connected to the top inner wall of the cylinder (1). The inner wall of the cylinder (1) is fixedly connected with multiple baffles (65) at equal intervals. Several triangular fins (66) are fixedly connected to both sides of the baffles (65). The adaptive gas distribution mechanism (7) includes a turntable (76) fixedly connected to the bottom of the stirring shaft (67). Multiple limiting sleeves (75) are fixedly connected at equal intervals on the outer wall of the turntable (76). Sliding rods (77) are slidably connected to the inner walls of the multiple limiting sleeves (75). Rotating blades (71) are fixedly connected to the side of the multiple sliding rods (77) away from the turntable (76). A spring (78) is fixedly connected to the side of the sliding rod (77) close to the turntable (76). The side of the spring (78) away from the sliding rod (77) is fixedly connected to the inner wall of the turntable (76). The adaptive gas distribution mechanism (7) also includes a gas distributor (73) fixedly connected to the inner wall of the bottom of the cylinder (1). The gas distributor (73) has several exhaust ports (74) at the top and bottom. The top of the gas distributor (73) is fixedly connected to a gas inlet pipe (72). The side of the gas inlet pipe (72) away from the gas distributor (73) is fixedly inserted through the outer wall of the cylinder (1) and the jacket (4).

2. The high-shear dynamic mixing reaction apparatus for preparing flexible particles according to claim 1, characterized in that, The gas distributor (73) is flower-shaped, with the top exhaust port (74) evenly distributed on the upper surface of the gas distributor (73) and the bottom exhaust port (74) concentrated on the lower surface of the middle part of the gas distributor (73).

3. The high-shear dynamic mixing reaction apparatus for preparing flexible particles according to claim 1, characterized in that, The length of the fixed sleeve (62) is set to one-third of the height of the cylinder (1).

4. The high-shear dynamic mixing reaction apparatus for preparing flexible particles according to claim 1, characterized in that, The triangular fins (66) are arranged alternately on both sides of the baffle (65).

5. The high-shear dynamic mixing reaction apparatus for preparing flexible particles according to claim 1, characterized in that, The jacket (4) has a heat transfer medium inlet at the bottom and a heat transfer medium outlet at the top.

6. A high-shear dynamic processing method for preparing flexible particles, wherein the process is implemented using the high-shear dynamic mixing and reaction apparatus for preparing flexible particles according to any one of claims 1-5, characterized in that, The process includes the following steps: Step 1: High-shear mixing and strengthening process: The rotating device consists of two stationary rings and two rotating rings interlocked. The stationary rings have multiple small holes, and the rotating rings have cutters on their surfaces. The material enters the inner cavity of the rotating device from the center. Under the centrifugal force of the rotating device, it flows radially out through the small holes on the first stationary ring and flows out through the small holes on the second stationary ring. The rotating outer ring rotates in the narrow channel formed between the two stationary rings and forms a vertical shear with the material that flows radially out of the small holes on the first stationary ring and radially enters the second stationary ring. This process crushes and tears the material that is mainly subjected to high-speed shear, which can break through the bottleneck of 500nm particle diameter. However, the morphology of the processed particles is irregular. Step 2: Dynamic synthesis and dynamic sintering process: Based on the original static temperature change synthesis principle, under the temperature change condition, dynamic synthesis and sintering with the combined action of rheological stress and rheological shear stress is added to accelerate thermochemical reaction and material mixing. Through the dynamic mixing reaction device, the material is subjected to pressure, shear force and friction in the cylinder (1) and is constantly rubbed and turned over.

1. Rheological process: The chemical reaction synthesis is carried out in a cylinder (1) with stirring function. The reaction process is a highly efficient piston reaction. In this dynamic synthesis reactor, the volume flow rate of the material processed in the unit reaction space is no more than 0.3 cubic meters per unit reaction time. The material is mixed more than 100 times, which greatly improves the consistency of the material after the synthesis reaction. II. Superplastic stage: In the latter half of the rheological process, under the dynamic action of pulsating stress at an appropriate temperature, the material undergoes particle deformation due to diffusion of grain boundary slip and dislocation grain boundary slip. When the strain rate reaches a suitable level, the material exhibits fine grain superplasticity, with crystal size less than 15 μm. In addition, the deformation temperature is relatively high, at 160℃ and above, the strain rate ε < 0.3 1 / S, and the stress on the material is greater than 3 MPa. Third, although dynamic sintering supplements some synthesis reactions, it also provides sintering function for lattice shaping. For high-temperature solid-state sintering, it saves sintering time, facilitates thorough sintering of materials, and reduces energy consumption. IV. Carbon Coating Process: A dynamic stirring method with pulsating stress is adopted. Under the action of shear stress generated by stirring, cycloalkanes and polar aromatics can be removed quickly. Condition 1: At the same temperature, the viscosity is reduced by stirring. The decrease in viscosity is conducive to the formation of mesophase microspheres, which provides a good foundation for the formation of coated carbon to develop in an ordered direction. Condition 2: Within a suitable temperature range, more intermediate phases are generated by stirring. The more intermediate phases are generated in the coated carbon, the higher the degree of order of the coated carbon formed in the later sintering, and the higher the degree of graphitization. Condition 3: Within a suitable temperature range, more and better intermediate phases are generated through time and agitation.

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