High-shear dynamic mixing reaction device for preparing flexible particles and dynamic treatment process

Abstract

The invention discloses a high-shear dynamic mixing reaction device for preparing flexible particles and a dynamic treatment process, and relates to the technical field of preparation of battery raw materials, and the process is characterized in that a flexible particle material for a battery is prepared in a compact space by adopting a pulsating stress dynamic processing method on the basis of an existing chemical formula. Performance obtained by a material formula and performance obtained by pulsating stress dynamic processing are mutually complemented to form an organic whole, the reaction device comprises a barrel, a feeding port is formed in the top of the barrel, a discharging port is formed in the bottom of the barrel, and a kneading and turning mixing mechanism is arranged, rotation of a stirring shaft is used as driving force of a sliding block, so that the material formula and the pulsating stress dynamic processing are combined, and the material formula and the pulsating stress dynamic processing are combined. The sliding block slides in the fixed sleeve in a reciprocating mode, upward and downward pressure is provided for materials in the barrel, the triangular fins are arranged on the baffles in a matched mode, the tips of the triangular fins can provide better shearing force for material particles rotating moderately, the materials are continuously kneaded and turned over and tend to be round, and carbon coating can be more uniform.

Description

Technical Field

[0001] The invention relates to the technical field of battery raw material preparation, and in particular to a high-shear dynamic mixing reaction device and a dynamic processing process for preparing flexible particles. Background Art

[0002] The traditional high-temperature solid-phase method generally uses chemical formulas to manufacture electrode materials. During the preparation process, the processed material is in a static state and is heated by the moving equipment. Therefore, the mechanical parameters of the processed material itself (such as elastic modulus E, etc.) do not change significantly during the preparation process. At the same time, the coated carbon is also formed by the corresponding relationship between time and viscosity under static conditions. The static materials in the preparation process do not have the conditions for mutual mixing. Therefore, after synthesis, the consistency of the product is relatively poor.

[0003] When the battery material is in working state, lithium ions carry electrons and shuttle through the material during the transmission process. When lithium ions flow into the material, it expands, and when lithium ions flow out of the material, it contracts. The expansion and contraction of the material causes flow stress, which is diffusion stress. Diffusion stress forms fatigue stress as lithium ions flow in and out. This fatigue stress is the main factor for the failure of battery particles.

[0004] In order to obtain better conductivity, the coated carbon is required to be formed in an orderly manner and the degree of graphitization is as high as possible. However, in the subsequent sintering process, the sintering temperature is determined by the electrical properties of the battery material, which is generally around 700°C. It is difficult to reach the sintering temperature of about 1450°C required for needle coke (the degree of order and graphitization is significantly higher than that of ordinary coke), so the degree of graphitization is bound to decrease.

[0005] In the prior art, firstly, a sand mill with high energy consumption is used to crush the raw materials into nanoparticles through the impact force of the grinding balls for several hours, and 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 and for several hours. This process is mainly based on chemical reaction synthesis, and the orderliness and mechanical properties of the coated carbon of the material are slightly improved. Finally, the material is sintered at high temperature and lattice-shaped in a static form for several hours. During the heating process, although the purpose is sintering and lattice-shaped, the heat transfer of the material will take up a lot of time, resulting in unnecessary energy consumption.

[0006] In addition, the current dynamic mixing reactors are highly targeted. For certain reactions that are sensitive to stirring intensity during the preparation of battery nanomaterials, excessive stirring is prone to occur, resulting in side reactions or deterioration in product quality. Therefore, additional mixing devices are usually required, increasing equipment costs.

[0007] In view of this, the present invention proposes a high shear dynamic mixing reaction device and a dynamic treatment process for preparing flexible particles to make up for and improve the deficiencies of the prior art. Summary of the invention

[0008] In order to solve the above technical problems, the present invention proposes a high-shear dynamic mixing reaction device and a dynamic treatment process for preparing flexible particles, so as to solve the problems in the prior art that the diffusion stress of lithium ions when shuttling in the material is relatively large, thereby reducing the service life of the battery, the order of the coated carbon is low, the consistency of the prepared products is low (insufficient uniformity), and the applicability of the device is low.

[0009] To achieve the above purpose, the technical solution adopted by the present invention is: a high shear dynamic mixing reaction device and a dynamic treatment process for preparing flexible particles, comprising a cylinder, a feed port is provided at the top of the cylinder, a discharge port 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 also includes:

[0010] The kneading and mixing mechanism is used to provide up and down reciprocating pressure and high shear stirring for the materials in the cylinder;

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

[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 extends to the bottom position of the cylinder, the top of the cylinder is fixedly connected to a motor, the top of the stirring shaft passes through the top of the cylinder and is fixedly connected to the output end of the motor, a pair of convex strips are fixedly connected to the middle of the stirring shaft, the outer walls of the stirring shaft and the convex strips are slidably connected to an agitator, the top of the agitator is fixedly connected to a telescopic sleeve, and the inner wall of the telescopic sleeve is slidably sleeved on the outer wall of the stirring shaft.

[0013] Preferably, the kneading and mixing mechanism also includes a pair of sliding blocks 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 thread groove, the outer walls of the pair of sliding blocks are slidably connected in the reciprocating thread groove, the top of the fixed sleeve is fixedly connected to a support frame, the top of the support frame is fixedly connected to the top inner wall of the cylinder, a plurality of baffles are equidistantly fixedly connected to the inner wall of the cylinder, and a plurality of triangular fins are fixedly connected to both sides of the baffle.

[0014] Preferably, the adaptive gas distribution mechanism includes a turntable fixedly connected to the bottom of the stirring shaft, a plurality of limit sleeves are equidistantly fixedly connected to the outer wall of the turntable, a plurality of inner walls of the limit sleeves are slidably connected to sliding rods, a plurality of sliding rods are fixedly connected to rotating blades on the side away from the turntable, a spring is fixedly connected to the side of the sliding rod close to the turntable, and a side of the spring away from the sliding rod is fixedly connected to the inner wall of the turntable.

[0015] Preferably, the adaptive gas distribution mechanism also includes a gas distributor fixedly connected to the inner wall of the bottom of the cylinder, a plurality of exhaust ports are provided at the top and bottom of the gas distributor, a gas inlet pipe is fixedly connected to the top of the gas distributor, and the side of the gas inlet pipe away from the gas distributor is fixedly passed through the outer wall of the cylinder and the jacket.

[0016] Preferably, the gas distributor is in a flower shape, the exhaust ports at the top are evenly distributed on the upper surface of the gas distributor, and the exhaust ports at the bottom are concentrated on the middle lower surface of the gas distributor.

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

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

[0019] Preferably, a heat carrier inlet is provided at the bottom of the jacket, and a heat carrier outlet is provided at the top of the jacket.

[0020] A high shear dynamic mixing reaction device and a dynamic treatment process for preparing flexible particles include the following steps:

[0021] Step 1: High shear mixing and strengthening process: The rotating equipment is composed of two stationary rings and two moving rings that are staggered and sleeved. There are multiple small holes on the stationary rings, and cutters are provided on the surface of the moving rings. The material enters the inner cavity of the rotating equipment from the center. Under the centrifugal action of the rotating equipment, it flows out radially through the small holes on the first stationary ring and flows out toward the small holes of the second stationary ring. The outer moving ring rotates in the narrow channel formed between the two stationary rings and forms vertical shear with the material that flows out radially from the small holes of the first stationary ring and enters the second stationary ring radially, thereby crushing and tearing the material that is mainly subjected to high-speed shearing, which can break through the bottleneck of particle diameter of 500nm, but 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 the condition of temperature change, dynamic synthesis and sintering with the combined effect of rheological stress and rheological shear stress, accelerating thermochemical reaction and material mixing are added. Through the dynamic mixing reactor, the material is subjected to pressure, shear force and friction in the cylinder, and is constantly kneaded and turned over;

[0023] 1. Rheological link: Chemical reaction synthesis is carried out in a tubular container with stirring function. The reaction process is an efficient piston (plug flow) reaction. The volume flow rate of the material processed in this dynamic synthesis reactor per unit reaction time (hour) and per unit reaction space (cubic meter) is no more than 0.3 cubic meters. The material is mixed more than 100 times, which greatly improves the consistency of the material after the synthesis reaction;

[0024] 2. Superplasticity: In the second half of the rheological process, the material is subjected to the dynamic action of pulsating stress at an appropriate temperature, accompanied by diffusion grain boundary sliding and dislocation grain boundary sliding, which causes particle deformation. When the strain rate reaches an appropriate level, the material exhibits fine grain superplasticity.

[0025] 3. Although dynamic sintering will supplement some synthesis reactions, it also provides sintering function for lattice shaping. For high-temperature solid-state sintering, it saves sintering time, facilitates the burning of materials, and reduces energy consumption;

[0026] 4. Carbon coating: The pulsating stress dynamic stirring method is adopted. The shear stress generated by the stirring can quickly remove cycloalkanes and polar aromatics.

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

[0028] Condition 2: More intermediate phases are generated by stirring within an appropriate temperature range, because in the formed coated carbon, the more intermediate phases are contained in the formation process, the higher the order of the coated carbon formed by the later sintering, and the higher the graphitization degree;

[0029] Condition three: within the appropriate temperature range, more and better mesophases are generated through time and stirring.

[0030] Compared with the prior art, the present invention has the following beneficial effects:

[0031] 1. When the material is dynamically mixed, the kneading and mixing mechanism is set up, and the rotation of the stirring shaft is used as the driving force of the slider, so that the slider slides back and forth in the fixed sleeve. The slider finally drives the agitator to reciprocate up and down synchronously, providing upward and downward pressure for the material in the cylinder, and the agitator continuously squeezes the material to hit the baffle for shearing and stirring. The triangular fins on the baffle are set up, and the tip can provide better shear force for the moderately rotating material particles, enhance the shear force, so that the material is subjected to effective pressure, shear force and friction in the cylinder, and is constantly kneaded and turned over. After repeated kneading of the granular material by the equipment, the particle deformation and grain boundary slip are caused, the elastic modulus of the material is reduced, the strain rate sensitivity index m is increased, and the flexibility is increased. Under the same charge and discharge conditions, the probability of particle fracture failure can be greatly reduced, and the strip or sheet material caused by high shear will gradually tend to be round after kneading, which can make the carbon coating more uniform, and cooperate with the temperature control of the jacket to make the outer wall of the material particle evenly form a carbon shell;

[0032] 2. Through the setting of triangular fins and gas distributors, the triangular fins not only increase the shear force of the material, but also the staggered arrangement on both sides of the baffle increases the density of the triangular fins distributed on the baffle surface, which can accelerate the diffusion of heat in the jacket into the cylinder, improve the heat conduction effect, and use the agitator to make the temperature more uniform during the material reaction process, while improving the response rate of the jacket to the temperature control inside the cylinder. 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 upper and lower ventilation settings of the gas distributor, the materials in the dead corners at the bottom of the cylinder can be concentrated and mixed into the middle of the cylinder for mixing, so that the suspended materials become orderly, further enhancing the effect of carbon coating;

[0033] 3. Through the setting of the adaptive gas distribution mechanism, when the shaft is stirred moderately, under the action of centrifugal force, the spring stretches to extend the rotating blades, so that the gas distributor automatically expands the diameter range of the gas spiral rise, which helps the gas to be more widely dispersed in the cylinder, and the expanded gas distribution range increases the contact area between the gas and the material, making the spacing between the material particles more uniform, thereby improving the mass transfer efficiency. When the shaft is stirred at a low speed, the rotating blades are shortened. For some reactions that are sensitive to stirring intensity, low-speed stirring can reduce the gas distribution range to avoid side reactions or product quality degradation caused by excessive stirring, which helps to maintain The stability and controllability of the reaction system are maintained. At the same time, the length of the rotating blade is automatically adjusted according to the rotation speed of the stirring shaft, so that in the process of preparing battery raw materials, nanomaterials can be prepared by moderate stirring to prevent particle agglomeration, and low-speed stirring can be performed to avoid side reactions or product quality degradation caused by excessive stirring, thereby increasing the applicability of the device; at the same time, since in the above preparation process, the material is subjected to shear strain under shear stress, the shear strain multiplied by the time the material is subjected to shear strain is equal to the shear strength. The greater the shear strength, the better the material mixing. The mixing number exceeds 100 times, which greatly improves the consistency of the material after the synthesis reaction. BRIEF DESCRIPTION OF THE DRAWINGS

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

[0035] Figure 2 It is a three-dimensional cross-sectional view of the cylinder shown in the present invention;

[0036] Figure 3 The present invention shows Figure 2 A schematic diagram of the enlarged three-dimensional structure in the middle;

[0037] Figure 4 It is a structural schematic diagram of the gas distributor connection shown in the present invention;

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

[0039] Figure 6 It is a structural schematic diagram of the triangular fin connection shown in the present invention;

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

[0041] Figure 8 It is a structural schematic diagram of the convex strip connection shown in the present invention;

[0042] Fig. 9 It is a structural schematic diagram of the connection of the sliding rod shown in the present invention;

[0043] Fig.10 The present invention shows Fig. 9 The enlarged structural diagram at B in the middle;

[0044] Fig.11 It is a schematic diagram of the morphology of particles after processing shown in the present invention;

[0045] Fig.12 This is a TEM morphology of particles after dynamic synthesis and dynamic sintering shown in the present invention;

[0046] Fig.13 Schematic diagram of the E(τ) function and the F(τ) function of the rheological link reaction shown in the present invention;

[0047] Fig.14 It is a schematic diagram of the superplastic strain rate sensitivity index of grains shown in the present invention;

[0048] Fig.15 It is a schematic diagram of shear strain rate and shear stress curve shown in the present invention;

[0049] Fig.16 It is a schematic diagram of viscosity and time curve shown in the present invention;

[0050] Fig.17 This is a schematic diagram of the mesophase yield and viscosity curve shown in the present invention;

[0051] Fig.18 It is a schematic diagram of the yield and time curve of carbon microspheres MCMB shown in the present invention.

[0052] The numbers in the figure are:

[0053] 1. Cylinder; 2. Feed inlet; 3. Discharge 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 thread groove; 69. Sliding block; 610. Raised strip;

[0055] 7. Adaptive gas distribution mechanism; 71. Rotating blades; 72. Gas inlet pipe; 73. Gas distributor; 74. Exhaust port; 75. Limit sleeve; 76. Turntable; 77. Sliding rod; 78. Spring. DETAILED DESCRIPTION

[0056] The following will be combined with the drawings in the embodiments of the present invention to clearly and completely describe the technical solutions in the embodiments of the present invention. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work 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] In order to solve the problems mentioned in the technical solution, the embodiment of the present application provides a high shear dynamic mixing reaction device for preparing flexible particles, including a cylinder 1, a feed port 2 is opened at the top of the cylinder 1, a discharge port 3 is opened at the bottom of the cylinder 1, a jacket 4 is fixedly connected to the outer wall of the bottom of the cylinder 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 cylinder 1, and also includes:

[0060] The kneading and mixing mechanism 6 is used to provide up and down reciprocating pressure and high shear stirring for the material in the cylinder 1;

[0061] An adaptive gas distribution mechanism 7, used to automatically adjust the gas distribution range to adapt the device to mix different types of flexible particles;

[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 position of the cylinder 1, the top of the cylinder 1 is fixedly connected to a motor, 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 convex strips 610 are fixedly connected to the middle of the stirring shaft 67, the outer walls of the stirring shaft 67 and the convex strips 610 are slidably connected to a stirrer 64, the top of the stirrer 64 is fixedly connected to a telescopic sleeve 63, and 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 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, a plurality of baffles 65 are equidistantly fixedly connected to the inner wall of the cylinder 1, and a plurality of triangular fins 66 are fixedly connected to both sides of the baffle 65;

[0064] The length of the fixed sleeve 62 is set to be 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] A heat medium inlet is provided at the bottom of the jacket 4, and a heat medium outlet is provided at the top of the jacket 4;

[0067] Among them: the fixed sleeve 62 is used to ensure the reciprocating motion of the stirrer 64, and the triangular fins 66 are used to conduct the heat in 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, insufficient shear force and friction force on the material, resulting in insufficient roundness of the strip or sheet material, thereby affecting the uniformity of the coated carbon. Compared with the prior art, through the implementation of this embodiment, the kneading and mixing mechanism 6 is set to use the rotation of the stirring shaft 67 as the driving force of the slider 69, so that the slider 69 slides back and forth in the fixed sleeve 62, and the slider 69 finally drives the agitator 64 to reciprocate up and down synchronously, providing upward and downward pressure for the material in the cylinder 1, and the agitator 64 continuously The extruded material hits the baffle 65 for shearing and stirring. The triangular fins 66 on the baffle 65 are arranged so that the tip thereof can provide better shearing force for the moderately rotating material particles, thereby enhancing the shearing force, so that the material is subjected to effective pressure, shearing force and friction in the cylinder 1, and is constantly kneaded and turned over, and will gradually tend to be round, which can make the carbon coating more uniform. At the same time, since in the above-mentioned preparation process, the material is subjected to shear strain under shear stress, the shear strain multiplied by the time the material is subjected to the shear strain is equal to the shear strength. The greater the shear strength, the better the material mixing. The mixing times here exceed 100 times, which greatly improves the consistency of the material after the synthesis reaction.

[0069] For 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, a plurality of limit sleeves 75 are fixedly connected to the outer wall of the turntable 76 at equal intervals, a plurality of limit sleeves 75 are slidably connected to the inner walls of the plurality of limit sleeves 75, a plurality of sliding rods 77 are fixedly connected to the rotating blades 71 on the side away from the turntable 76, a spring 78 is fixedly connected to the side of the sliding rod 77 close to the turntable 76, and a side of the spring 78 away from the sliding rod 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, and a plurality of exhaust ports 74 are provided at the top and bottom of the gas distributor 73. The top of the gas distributor 73 is fixedly connected to a gas inlet pipe 72, and the side of the gas inlet pipe 72 away from the gas distributor 73 is fixedly penetrated through the outer wall of the cylinder 1 and the jacket 4;

[0072] The gas distributor 73 is in a flower shape, the top exhaust ports 74 are evenly distributed on the upper surface of the gas distributor 73, and the bottom exhaust ports 74 are concentrated on the middle lower surface of the gas distributor 73;

[0073] The number of exhaust ports 74 arranged on the gas distributor 73 is greater at the top than at the bottom, and the baffles 65 are all located at the concave positions of the gas distributor 73 .

[0074] The effects achieved by this embodiment are as follows: In the prior art, the dynamic mixing reactor is highly targeted. For some reactions that are sensitive to stirring intensity during the preparation of battery nanomaterials, excessive stirring is prone to occur, resulting in side reactions or reduced product quality. Therefore, an additional mixing device is usually required, which increases the equipment cost. Compared with the prior art, through the implementation of this embodiment, an adaptive gas distribution mechanism 7 is set to automatically adjust the length of the rotating blade 71 according to the rotation speed of the stirring shaft 67, so that during the preparation of battery raw materials, both moderate stirring and preparation of nanomaterials can be performed to prevent particle agglomeration, and low-speed stirring can be performed to avoid side reactions or reduced product quality caused by excessive stirring, thereby increasing the applicability of the device; at the same time, since in the above-mentioned preparation process, the material is subjected to shear strain under shear stress, the shear strain multiplied by the time the material is subjected to shear strain is equal to the shear strength. The greater the shear strength, the better the material mixing. The mixing times here exceed 100 times, which greatly improves the consistency of the material after the synthesis reaction.

[0075] Embodiment 2 of the present invention

[0076] A high shear dynamic mixing reaction device and a dynamic treatment process for preparing flexible particles include the following steps:

[0077] Step 1: High shear mixing and strengthening process: The rotating equipment is composed of two stationary rings and two moving rings that are staggered and sleeved. There are multiple small holes on the stationary rings, and cutters are provided on the surface of the moving rings. The material enters the inner cavity of the rotating equipment from the center. Under the centrifugal action of the rotating equipment, it flows out radially through the small holes on the first stationary ring and flows out toward the small holes of the second stationary ring. The outer moving ring rotates in the narrow channel formed between the two stationary rings and forms vertical shear with the material that flows out radially from the small holes of the first stationary ring and enters the second stationary ring radially, thereby crushing and tearing the material that is mainly subjected to high-speed shearing, which can break through the bottleneck of particle diameter of 500nm, but the morphology of the processed particles is irregular;

[0078] like Fig.11 Shown is a schematic diagram of the particle morphology after processing;

[0079] Step 2: Dynamic synthesis and dynamic sintering process: Based on the original static temperature change synthesis principle, under the condition of temperature change, dynamic synthesis and sintering with the combined effect of rheological stress and rheological shear stress, accelerating thermochemical reaction and material mixing are added. The morphology of the processed particles is in an irregular shape, which has a negative impact on the compaction density and electrochemical performance of the later battery products. However, combined with the subsequent dynamic synthesis process, the material is subjected to pressure, shear force and friction in the cylinder 1 through a dynamic mixing reactor, and is constantly kneaded and turned over. During the dynamic synthesis kneading process, the morphology of the material particles will be close to a spherical morphology, just like kneading coal balls;

[0080] like Fig.12 Shown are the TEM morphologies of particles after dynamic synthesis and dynamic sintering;

[0081] 1. Rheological link: Chemical reaction synthesis is carried out in a tubular container with stirring function. The reaction process is an efficient piston (plug flow) reaction. The E(τ) function and F(τ) function of the reaction are as follows: Fig.13 The function curve of the plug flow reactor shown in , where E(τ) is the residence time distribution density function and F(τ) is the cumulative residence time distribution function;

[0082] 2. Superplasticity: In the second half of the rheological process, the material is subjected to the dynamic action of pulsating stress at an appropriate temperature, accompanied by diffusion grain boundary sliding and dislocation grain boundary sliding, which causes particle deformation. When the strain rate reaches an appropriate level, the material exhibits fine grain superplasticity. The grain superplasticity strain rate sensitivity index is as follows: Fig.14 As shown; Among them, V is the deformation speed; m is the strain rate sensitivity index, G is the maximum point, and D is the stable point;

[0083] The index for measuring the superplasticity of materials is the strain rate sensitivity index (m), which is described by the single maximum method of velocity jump as follows:

[0084]

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

[0086] Grain boundary sliding (GBS) is the main deformation mechanism of superplastic deformation. There are four important prerequisites for GBS to operate in polycrystalline materials. First, it requires a very small grain size, usually less than 15μm. Second, the deformation temperature should be relatively high, at or above 160℃, the strain rate ε&<0.3(1 / S), and the stress on the material is greater than 3Mpa. These four prerequisites control the dynamic change of pulsating stress (extrusion stress), adjust the elastic modulus of the material, change the flexibility of the material, and use the strain rate sensitivity index m as a signature parameter, which quickly evolved into the basic principle for designing materials with superplasticity.

[0087] The crystal slip in this dynamic synthesis reactor is not more than 0.3 cubic meters of volume flow rate of the material processed in the unit reaction time (hour) and unit reaction space (cubic meters);

[0088] 3. Although dynamic sintering will supplement some synthesis reactions, it also provides a sintering function for lattice shaping. For high-temperature solid-state sintering, it saves sintering time, is conducive to the burn-through of materials, and reduces energy consumption. The following Table 1 shows the curve relationship between the strain rate sensitivity index and the elastic modulus and diffusion stress, Table 2 shows the cycle life test results, Table 3 shows the discharge rate and discharge time comparison results, Table 4 shows the test results of the discharge temperature under the rate, and Table 5 shows the test results of the impact parameters (safety).

[0089] Table 1 Curve relationship between strain rate sensitivity index, elastic modulus and diffusion stress

[0090] project symbol unit Condition 1 Condition 2 Elastic modulus E Mpa 488.9 2880 Strain rate sensitivity index (extrusion stress) m 2.31 0.99 Charge state SOC 0.4 0.4 Strain 1 ε 1 ％ 2.78 2.78 Diffusion stress 1 σ1 Mpa 32.27 49.67

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

[0092] Table 2 Cycle life test

[0093]

[0094] Table 3 Comparison of discharge rate and discharge time

[0095]

[0096] Table 4 Discharge temperature at rate

[0097] project symbol unit Ratio Crate 1 2 3 4 5 Conversion rate Crate1 0.897149 1.75833255 2.619516 3.480699 4.341882686 Discharge temperature trc ℃ 30.72377 38.8283436 48.30387 58.82817 69.65091755 Discharge temperature trc1 ℃ 29.96891 36.7360189 44.31569 51.73361 57.79292669 Discharge temperature difference △trc ℃ 0.754859 2.09232474 3.988179 7.09456 11.85799086

[0098] Table 5 Impact parameters (safety)

[0099]

[0100] 4. Carbon coating: The pulsating stress dynamic stirring method is adopted. The shear stress generated by the stirring can quickly remove cycloalkanes and polar aromatics.

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

[0102] Example 1

[0103] Temperature is equal

[0104] Working conditions Shear rate temperature Viscosity symbol Y t μ unit 1 / s ℃ P*s Material stillness ① 0 44.53675 15.5355 Material Flow ② 15 44.53675 5.276951 Provides a temperature rise of ~25.56°C ① / ② 1 2.944029

[0105] like Fig.15 Shown is a schematic diagram of shear strain rate and shear stress curve;

[0106] Example 2

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

[0108] project unit Condition 1 Condition 2 time τ h 0.1 3 Viscosity η390 10-1Pa*s Calculate viscosity η390 10-1Pa*s 3.148798 7.1606 Viscosity ratio ξη 0.439739

[0109] like Fig.16 Shown is a schematic diagram of viscosity and time curve;

[0110] It can be seen from the data table that the shorter the residence time of the organic CH compound from melting to liquid phase to generating intermediate phase in the dynamic synthesis reactor at the same temperature, the more conducive to reducing the viscosity. At 390°C, if the residence time of the liquid organic CH compound is reduced from 3h to 0.1h, the viscosity will drop from 0.716 to 0.315Pa*s, a decrease of 2.27 times.

[0111] Condition 2: More intermediate phases are generated by stirring within an appropriate temperature range, because in the formed coated carbon, the more intermediate phases are contained in the formation process, the higher the order of the coated carbon formed by the later sintering, and the higher the graphitization degree;

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

[0113] Condition three: within the appropriate temperature range, more and better mesophases are generated through time and agitation;

[0114] like Fig.18 Shown is a schematic diagram of the MCMB yield and time curve of carbon microspheres. 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 embodiment are as follows:

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

[0117] Working process:

[0118] When in use, the staff first puts the highly sheared nano-scale material particles from the feed port 2 into the cylinder 1, and at the same time starts the gas distributor 73 to blow air to blow the material particles to suspend in the inner cavity of the cylinder 1, and discharges the heating medium from the heat carrier inlet into the jacket 4, and the spiral guide plate 5 spirally rises to fill the jacket 4, and the cylinder 1 is heated. Then the motor is started to drive the stirring shaft 67 to rotate. Under the limiting effect of the convex strip 610, the stirrer 64 and the telescopic sleeve 63 move along with the stirring shaft. 67 rotates synchronously. Since the support frame 61 is sleeved on the outer wall of the telescopic sleeve 63, and the slider 69 is slidably connected to the reciprocating thread groove 68, the rotation of the telescopic sleeve 63 can drive the slider 69 to rotate synchronously. The rotating slider 69 can rise along the hole groove of the reciprocating thread groove 68, and then the telescopic sleeve 63 and the agitator 64 are driven upward by the slider 69 until the slider 69 reaches the top of the fixed sleeve 62. Due to the reciprocating nature of the reciprocating thread groove 68, the slider 69 can move along the reciprocating thread groove 68. The holes of the groove 68 are turned back and moved downward, and in this way, the stirrer 64 can also perform up and down reciprocating motion during the rotation process. Since the length of the fixed sleeve 62 is set to one-third of the height of the cylinder 1, the reciprocating range of the stirrer 64 is the middle part of the cylinder 1, which is the position where the gas distributor 73 blows and concentrates the material, which is conducive to the stirrer 64 to continuously flip the suspended material up and down, increase the friction and pressure on the material, and at the same time, with the setting of the triangular fins 66, the tip of the triangular fins 66 facing outward can provide better shear force for the moderately rotating material particles. The material is constantly kneaded and turned over in the cylinder 1, gradually tending to be round, thereby improving the uniformity of mixing, so that the material particles are better and more evenly carbon-coated. In addition, by staggering the triangular fins 66 on both sides of the baffle 65, the density of the triangular fins 66 distributed on the surface of the baffle 65 is increased, the heat conduction effect of the baffle 65 is improved, and the response rate of the jacket 4 to the temperature control inside the cylinder 1 is improved;

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

[0120] Furthermore, the flower-shaped gas distributor 73 can avoid the range of the baffle 65, ensuring that the gas blown out by the gas distributor 73 effectively covers the range at the bottom of the cylinder 1, and the gas distributor 73 can exhaust gas from both the top and the bottom. The gas blown downward from the exhaust port 74 can blow a small amount of material that falls on the bottom of the cylinder 1, giving the material particles a thrust, so that the material moves upward along the curvature of the bottom of the cylinder 1, and cooperates with the top exhaust port 74 to blow air upward, so that the material is concentrated and mixed into the middle part of the cylinder 1 for mixing, thereby reducing the mixing dead angle. At the same time, during the rotation of the stirring shaft 67, the bottom turntable 76 also rotates as a whole. When the mixed material inside the cylinder 1 is a carbon coating process, high-speed stirring is required because it is necessary to reduce the viscosity between the material particles. At this time, the turntable 76 rotating at high speed with the stirring shaft 67 will generate centrifugal force, and the rotating blade 71 drives the sliding rod 77 to slide out of the limit sleeve 75, stretching The spring 78 moves the rotating blade 71 in the direction away from the limiting sleeve 75, which is equivalent to increasing the length of the rotating blade 71, thereby increasing its rotating diameter. In cooperation with the gas distributor 73 to continuously discharge gas upward, the rotating blade 71 can stir the vertically upward gas to form a spiral upward gas, and the increase in the rotating diameter of the rotating blade 71 expands the diameter range of the gas spiral rise, thereby increasing the contact area between the gas and the material, making the spacing between the material particles more uniform, thereby improving the mass transfer efficiency. When the cylinder 1 is carrying out some reactions that are sensitive to stirring intensity, the stirring shaft 67 needs to stir at a low speed, and almost no centrifugal force is generated at this time. Therefore, the elastic force of the spring 78 can reset the sliding rod 77, so that the rotating diameter of the rotating blade 71 is reduced, avoiding side reactions or a decrease in product quality caused by excessive stirring. In this way, the length of the rotating blade 71 is adaptively controlled to increase the adaptability of the device to mix different materials.

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

[0122] The circuits and instrument controls involved in the present invention are all prior art and will not be described in detail here.

[0123] Although embodiments of the present invention have been shown and described, it will be appreciated by those skilled in the art that various changes, modifications, substitutions and variations may be made to the embodiments without departing from the principles and spirit of the present invention, and that the scope of the present invention is defined by the appended claims and their equivalents.

Claims

1. A high shear dynamic mixing reaction device for preparing flexible particles, comprising a barrel (1), a feed inlet (2) is provided at the top of the barrel (1), a discharge outlet (3) is provided at the bottom of the barrel (1), a jacket (4) is fixedly connected to the outer wall of the bottom of the barrel (1), a spiral guide plate (5) is fixedly connected to the inner wall of the jacket (4), and a side of the spiral guide plate (5) away from the jacket (4) is fixedly connected to the outer wall of the barrel (1), characterized in that: Also included are: The kneading and mixing mechanism (6) is used to provide up and down reciprocating pressure and high shear stirring for the material in the cylinder (1); The adaptive gas distribution mechanism (7) is used to automatically adjust the gas distribution range to adapt the device to mix different types of flexible particles.

2. The high shear dynamic mixing reaction device for preparing flexible particles according to claim 1, characterized in that: The kneading and mixing mechanism (6) comprises 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 position of the cylinder (1), the top of the cylinder (1) is fixedly connected to a motor, 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 convex strips (610) are fixedly connected to the middle of the stirring shaft (67), the outer walls of the stirring shaft (67) and the convex strips (610) are slidably connected to an agitator (64), the top of the agitator (64) is fixedly connected to a telescopic sleeve (63), and the inner wall of the telescopic sleeve (63) is slidably sleeved on the outer wall of the stirring shaft (67).

3. The high shear dynamic mixing reaction device for preparing flexible particles according to claim 2, characterized in that: 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 to 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 equidistantly fixedly connected to a plurality of baffles (65); and a plurality of triangular fins (66) are fixedly connected to both sides of the baffle (65).

4. The high shear dynamic mixing reaction device for preparing flexible particles according to claim 2, characterized in that: The adaptive gas distribution mechanism (7) comprises a turntable (76) fixedly connected to the bottom of the stirring shaft (67); a plurality of limit sleeves (75) are fixedly connected to the outer wall of the turntable (76) at equal intervals; the inner walls of the plurality of limit sleeves (75) are slidably connected to sliding rods (77); the sides of the plurality of sliding rods (77) away from the turntable (76) are fixedly connected to rotating blades (71); the side of the sliding rod (77) close to the turntable (76) is fixedly connected to a spring (78); the side of the spring (78) away from the sliding rod (77) is fixedly connected to the inner wall of the turntable (76).

5. The high shear dynamic mixing reaction device for preparing flexible particles according to claim 1, characterized in that: The adaptive gas distribution mechanism (7) further comprises a gas distributor (73) fixedly connected to the inner wall of the bottom of the cylinder (1), a plurality of exhaust ports (74) are provided at the top and bottom of the gas distributor (73), a gas inlet pipe (72) is fixedly connected to the top of the gas distributor (73), and a side of the gas inlet pipe (72) away from the gas distributor (73) is fixedly penetrated through the outer wall of the cylinder (1) and the jacket (4).

6. The high shear dynamic mixing reaction device for preparing flexible particles according to claim 5, characterized in that: The gas distributor (73) is in a flower shape, the exhaust ports (74) at the top are evenly distributed on the upper surface of the gas distributor (73), and the exhaust ports (74) at the bottom are concentrated on the middle lower surface of the gas distributor (73).

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

8. The high shear dynamic mixing reaction device for preparing flexible particles according to claim 3, characterized in that: The triangular fins (66) are arranged alternately on both sides of the baffle (65).

9. The high shear dynamic mixing reaction device for preparing flexible particles according to claim 1, characterized in that: A heat carrier medium inlet is provided at the bottom of the jacket (4), and a heat carrier medium outlet is provided at the top of the jacket (4).

10. A high shear dynamic treatment process for preparing flexible particles, the process being implemented using the high shear dynamic mixing reaction device for preparing flexible particles according to claims 1-9, the process comprising the following steps: Step 1: High shear mixing and strengthening process: The rotating equipment is composed of two stationary rings and two moving rings that are staggered and sleeved. There are multiple small holes on the stationary rings, and cutters are provided on the surface of the moving rings. The material enters the inner cavity of the rotating equipment from the center. Under the centrifugal action of the rotating equipment, it flows out radially through the small holes on the first stationary ring and flows out toward the small holes of the second stationary ring. The outer moving ring rotates in the narrow channel formed between the two stationary rings and forms vertical shear with the material that flows out radially from the small holes of the first stationary ring and enters the second stationary ring radially, thereby crushing and tearing the material that is mainly subjected to high-speed shearing, which can break through the bottleneck of particle diameter of 500nm, but 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 condition of temperature change, dynamic synthesis and sintering with the combined effect of rheological stress and rheological shear stress to accelerate the thermochemical reaction and material mixing are added. Through the dynamic mixing reactor, the material is subjected to pressure, shear force and friction force in the cylinder (1), and is constantly kneaded and turned over; 1. Rheological link: Chemical reaction synthesis is carried out in a tubular container with stirring function. The reaction process is an 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; 2. Superplasticity: In the second half of the rheological process, the material is subjected to the dynamic action of pulsating stress at an appropriate temperature, accompanied by diffusion grain boundary sliding and dislocation grain boundary sliding, which causes particle deformation. When the strain rate reaches an appropriate level, the material exhibits fine grain superplasticity, and the crystal size is less than 15μm. Secondly, the deformation temperature is relatively high, at 160℃ and above, the strain rate E&<0.3(1 / S), and the stress on the material is greater than 3Mpa.

3. Although dynamic sintering will supplement some synthesis reactions, it also provides sintering function for lattice shaping. For high-temperature solid-state sintering, it saves sintering time, facilitates the burning of materials, and reduces energy consumption; 4. Carbon coating: The pulsating stress dynamic stirring method is adopted. The shear stress generated by the stirring can quickly remove cycloalkanes and polar aromatics. Condition 1: At the same temperature, the viscosity is reduced by stirring. The decrease in viscosity is conducive to the formation of mesophase globules, which provides a good foundation for the formation of coated carbon to develop in an orderly direction. Condition 2: More intermediate phases are generated by stirring within an appropriate temperature range, because in the formed coated carbon, the more intermediate phases are contained in the formation process, the higher the order of the coated carbon formed by the later sintering, and the higher the graphitization degree; Condition three: within the appropriate temperature range, more and better mesophases are generated through time and stirring.

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