Continuous secondary particle production and product thereof

Abstract

Continuous production of agglomerated particles may be accomplished with the mixing of primary particles and an agglomeration binder or solution in a continuous kneader. The continuous kneader may mix the primary particles and the agglomeration solution as they are conveyed along the length of the continuous kneader from a first end to a second end to produce agglomerated secondary particles, wherein internal temperature along the length of the continuous kneader is maintained at a temperature below about 500°C. The shearing forces or shear gap within the continuous kneader may be adjusted to produce size-controlled agglomerated particles.

Description

CONTINUOUS SECONDARY PARTICLE PRODUCTION AND PRODUCTTHEREOFINCORPORATION BY REFERENCE TO ANY PRIORITY APPLICATIONS

[0001] This PCT application claims priority to U.S. Provisional Application 63 / 609208. filed December 12, 2023, the entirety of which is incorporated herein for any and all purposes.BACKGROUND OF THE INVENTION

[0002] A battery cell generally consists of an anode, a cathode, a liquid electrolyte, a separator, and one or more current collectors. For lithium ion batteries, the anode and cathode materials may be optimized for the insertion (lithiation) or removal (delithiation) of lithium ions. Similarly, in a sodium ion battery the anode and cathode materials may be optimized for the movement of sodium ions from the anode to the cathode (during cell discharge) or from the cathode to the anode (during cell charging).

[0003] Carbon is a useful material in a battery anode in a lithium batten' as it is lightweight and allows for efficient intercalation of the lithium ions. Graphite is particularly useful as it allows the intercalation of lithium ions in the two-dimensional carbon sheets that make up the graphite material. Graphite has an exceptional ability to limit swelling upon lithiation or lithium intercalation, which results in reduced harm to the battery. This is a significant advantage in producing batteries that are sustainable and reusable for extended charge and discharge cycles.

[0004] Natural graphite may be obtained from natural sources and ore deposits. Natural graphite forms under intense heat and pressure over millions of years. On the other hand, synthetic graphite may be synthesized as the byproduct of various chemical processes. For example, synthetic graphite may be synthesized from petroleum, coal, or other synthetic or natural carbon materials. Synthetic graphite is desirable for lithium ion batteries due to its purity, performance, and consistency. As an anode material, synthetic graphite enables better cycling stability, faster charging, higher quality consistency, and fast production scalability.

[0005] Anode materials containing graphite or graphitizable carbons have previously been processed in batch methods. While batch processes have been useful in maintaining the consistency of anode materials, batch processes may be more expensiveand less efficient due to their cyclical nature. Additionally, most methods for agglomerating secondary anode particles involve high temperatures exceeding 500°C.

[0006] Thus, there is a need to create a process for the production of anode materials in a continuous process that is a lower temperature process and produces anode materials with the same quality and electrochemical characteristics as anode materials that are produced via batch processes.SUMMARY

[0007] The systems and methods disclosed herein provide a continuous process for the synthesis of anode materials. The processes disclosed herein are environmentally friendly, cost-effective, and more efficient than previous methods.

[0008] In some aspects, the techniques described herein relate to a method for continuously synthesizing agglomerated secondary particles, the method including: providing a continuous kneader having a first end and a second end; providing primary particles including a graphitizable material into the first end of the continuous kneader; providing an agglomeration solution into the first end of the continuous kneader; and mixing the primary particles and the agglomeration solution as they are conveyed along a length of the continuous kneader from the first end to the second end to produce the agglomerated secondary' particles; wherein internal temperature along the length of the continuous kneader is maintained at a temperature below about 500°C.

[0009] In some aspects, the techniques described herein relate to a method, wherein the agglomeration solution is an aqueous agglomeration solution that includes non- graphitizable lignin, sugar, or plant-derived carbohydrate molecules.

[0010] In some aspects, the techniques described herein relate to a method, wherein the continuous kneader is a single barrel, tri-stroke continuous kneader.

[0011] In some aspects, the techniques described herein relate to a method, wherein internal temperature along the length of the continuous kneader is maintained at a temperature below about 300°C.

[0012] In some aspects, the techniques described herein relate to a method, wherein internal temperature along the length of the continuous kneader is maintained within about 50°C of the softening point of the agglomeration solution.

[0013] In some aspects, the techniques described herein relate to a method, wherein a length to diameter ratio of a mixing shaft of the continuous kneader is greater than about 10: 1.

[0014] In some aspects, the techniques described herein relate to a method, wherein a length to diameter ratio of a mixing shaft of the continuous kneader is greater than about 20: 1.

[0015] In some aspects, the techniques described herein relate to a method, wherein the primary7particles include graphitizable soft carbon particles having a D50 less than about 100 pm.

[0016] In some aspects, the techniques described herein relate to a method, wherein the primary particles are selected from a group consisting of micronized petroleum coke powder, polyvinyl chloride, mesophase pitch, pitch coke, and coal coke; wherein the primary7particles have a D50 less than about 20pm.

[0017] In some aspects, the primary7particles are selected from a group consisting of micronized petroleum coke powder, polyvinyl chloride, mesophase pitch, pitch coke, and coal coke; wherein the primary particles have a bi-modal particle size distribution.

[0018] In some aspects, where the bi-modal particle size distribution is a combination of a first set of primary particles with a D50 greater than 5pm but less than about 20pm and a second set of primary^ particles with a D50 less than about 5 pm.

[0019] In some aspects, the primary7particles with a D50 less than about 5pm are derived from fine byproduct of mechanical processing of petroleum coke powder, polyvinyl chloride, mesophase pitch, pitch coke, and coal coke.

[0020] In some aspects, the techniques described herein relate to a method, wherein the agglomeration solution includes between about 5 wt% and about 15 wt% of the total feed mass conveyed along the length of the continuous kneader.

[0021] In some aspects, the techniques described herein relate to a method, wherein the agglomerated secondary particles have a D50 between about 50 pm and about 500 pm.

[0022] In some aspects, the techniques described herein relate to a method, wherein the agglomerated secondary particles have a D50 greater than about 1 mm and the method additional includes milling the agglomerated secondary particles to size control the secondary particles to between about 10-30 pm.

[0023] In some aspects, the techniques described herein relate to a method, wherein at least one of the primary particles and the agglomeration solution are heated before being provided into the first end of the continuous kneader.

[0024] In some aspects, the techniques described herein relate to a method, further including removing the agglomerated secondary particles from the second end of the continuous kneader and calcining the agglomerated secondary' particles in a rotary kiln at a temperature between about 800 and about 1350°C to produce calcined secondary particles.

[0025] In some aspects, the techniques described herein relate to a method, further including passing the calcined secondary particles into a continuously classifying grinding mill and reducing the D50 of the calcined particles to less than about 30 pm.

[0026] In some aspects, the techniques described herein relate to a method, further including graphitizing the calcined particles at temperatures greater than about 2500°C after reducing the D50 of the calcined particles to produce a graphitized anode material.

[0027] In some aspects, the disclosure relates to agglomerated secondary particles produced according to the techniques described herein.

[0028] In some aspects, the techniques described herein relate to agglomerated secondary particles, wherein the secondary particles are comprised of at least 2 to about 100 primary particles agglomerated together.

[0029] In some aspects, the techniques described herein relate to agglomerated secondary particles, wherein the agglomerated secondary particles have a D50 greater than about 300 pm.

[0030] In some aspects, the techniques described herein relate to a method for continuously producing agglomerated secondary- particles, the method including: providing a continuous kneader having a first end and a second end; providing primary particles included of graphitizable carbons into an inlet between the first end and the second end of the continuous kneader; providing an agglomeration binder into one or more inlets between the first end and the second end of the continuous kneader; and conveying the primary particles and the agglomeration binder through one or more high shear sections followed by one or more low shear sections along a length of the continuous kneader to produce the secondary particles.

[0031] In some aspects, the techniques described herein relate to a method, wherein the one or more high shear sections have a shear gap of less than about 4 mm and the one or more low shear sections have a shear gap of more than about 4 mm.

[0032] In some aspects, the techniques described herein relate to a method, wherein the agglomeration binder has a D50 greater than about 2000 pm and is selected from a group consisting of plant based polymer, petroleum pitch, and coal tar pitch.

[0033] In some aspects, the techniques described herein relate to a method, wherein the continuous kneader is a tri-stroke continuous kneader.

[0034] In some aspects, the techniques described herein relate to a method, wherein the continuous kneader is configured such that a shear gap is adjustable in the one or more high shear sections and the one or more low shear sections.

[0035] In some aspects, the techniques described herein relate to a method, wherein the agglomeration binder is micronized high temperature petroleum pitch with a particle size D50 between about 2 pm and 5 pm.

[0036] In some aspects, the techniques described herein relate to a method, wherein the agglomeration binder has a softening point above about 100 degrees Celsius.

[0037] In some aspects, the techniques described herein relate to a method for continuously producing size-controlled secondary particles, the method including: providing a continuous kneader having a first end and a second end; providing a plurality of flights connected to a central rotating rod within the continuous kneader; providing one or more stationary kneading bolts along an interior wall of the continuous kneader; providing primary particles including a graphitizable material into the first end of the continuous kneader; providing an agglomeration solution containing binder molecules into the first end of the continuous kneader; and mixing the primary particles and the agglomeration solution as they are conveyed along a length of the continuous kneader from the first end to the second end to produce the secondary particles having a D50 exceeding about 300 pm; wherein internal temperature along the length of the continuous kneader is maintained at a temperature below about 500°C.

[0038] In some aspects, the techniques described herein relate to a method, additionally including milling the agglomerated secondary particles in a rotary7kiln to reduce a size of the agglomerated secondary particles to a D50 below about 200 pm.

[0039] In some aspects, the techniques described herein relate to a method, wherein the agglomerated secondary particles have a binder to particle mass ratio of about 5: 100 to about 20: 100.

[0040] In some aspects, the techniques described herein relate to a method, wherein a shear gap between the plurality7of flights and the one or more stationary kneading bolts varies along the length of the continuous kneader.

[0041] In some aspects, the techniques described herein relate to a method, additionally including discharging the mixture of primary particles and the agglomeration solution at the second end of the continuous kneader, wherein the ratio of secondary particles to primary particles is at least 100: 1.

[0042] In some aspects the techniques described herein relate to a battery containing a graphitized anode material.

[0043] In some aspects the techniques described herein relate to a battery containing a graphitized anode material comprised of graphitized secondary particles.BRIEF DESCRIPTION OF THE DRAWINGS

[0044] Figure 1 is an SEM image showing a secondary anode material produced in accordance with embodiments herein.

[0045] Figure 2 illustrates an example of a continuous kneader.

[0046] Figure 3 illustrates a view' of an internal structure of a continuous kneader.

[0047] Figure 4 illustrates various configurations for screw' flights for a continuous kneader.

[0048] Figure 5 illustrates the rotation, strokes, and material flow' of a tri-stroke kneader.

[0049] Figure 6 illustrates a shearing mechanism of a continuous kneader.

[0050] Figure 7 illustrates a general process for the production of agglomerated particles.DETAILED DESCRIPTION

[0051] The systems and methods disclosed herein allow for the production of secondary anode materials in a continuous manner. In some embodiments the materials are synthesized using continuous compounding equipment. The embodiments described herein afford much higher operational efficiency, lower temperature requirements, and significantly higher throughput per machine or system.

[0052] Secondary anode materials generally comprise one or more primary particles that are agglomerated together via an agglomeration solution. The agglomeration of primary particles, resulting in secondary anode materials, produces many benefits. One reason for agglomerating graphite in battery anodes is this allows for more efficient storage of lithium, sodium, or other ions, which can improve the overall capacity and energy density of the battery7. Agglomerating graphite or graphitizable materials in battery anodescan improve the performance and manufacturability of the batteries, making them more suitable for a wide range of applications.

[0053] Agglomerated particles generally have a larger total volume than primary particles, as they are comprised of two or more primary particles. As the generally spherical volume of the agglomerated particles increases, the surface area to volume ratio decreases, which can provide desirable electrochemical characteristics. The agglomerated particles possess desirable charge and discharge characteristics and have high purity according to the processes disclosed herein. These electrochemical characteristics are achieved by producing agglomerated particles according to methods disclosed herein. The methods and product disclosed herein allow for the production of agglomerated particles and battery active materials that are carbon friendly, cost-effective, and reduce the number of pre- and post- granulation steps.

[0054] Agglomerated particles may be produced continuously or intermittently by providing primary particles and an agglomeration solution into one or more ports of a continuous kneader and removing secondary’ particles continuously or intermittently from an exit port of the continuous kneader. Through the continuous or semi-continuous addition and / or removal of secondary' particles the process may be optimized for output size and throughput, reducing costs and increasing the output of a single production line.

[0055] Figure 1 is an SEM image of sample secondary anode particles produced in accordance with embodiments disclosed herein. The SEM image shows a scale of 10 microns with an SED at 5 kilovolts and a working distance (WD) of 1 1.9 mm. The image generally shows one or more primary' particles that have been agglomerated together into one or more generally spherical secondary particles. The size of the particles may vary', but they may be configured on the order of 10 to 30 microns, as discussed further below.

[0056] Figure 2 illustrates a sample continuous kneader 200 that may be used in some embodiments herein. The continuous kneader 200 generally contains a first end 220 and a second end 222. The first end 220 may be comprised of a first portion of the kneader and the second end 222 may be comprised of a second portion of the kneader. In one or more embodiments the material may be provided in the first end 220 through various ports and removed from the second end 222 through one or more removal ports. In embodiments herein the material is generally conveyed from the first end 220 of the continuous kneader 200 to the second end 222 of the kneader. The material is generally conveyed along an internal screw (discussed further with regard to Figures 3 and 4) thatmay simultaneously mix, convey, shear, and agglomerate material within the cylindrical barrel of the continuous kneader.

[0057] The powder particles may be provided from one or more hoppers or containers, such as hoppers 206 and 208. The hoppers 206 and 208 may provide different sizes of primary particles or they may provide primary' particles heated or pre-conditioned. In some embodiments there is only a single hopper, such as 206. that provides a single type of primary particle to the powder chute 224 provided near the first end 220 of the continuous kneader 200. In some embodiments the powder may be directly fed into the powder chute 224. In some embodiments the hoppers may convey the material into the continuous kneader at a predetermined rate in order to provide a suitable ratio of primary particle to agglomeration solution. The primary particles may be conveyed into the continuous kneader at a suitable continuous or semi-continuous rate with one or more conveyer mechanisms, such as conveyer belts, rotating screws, nozzles, gates, pneumatic transport, etc. The fill level of the hoppers may also be maintained in order to provide a continuous flow of material. In some embodiments the primary particles a maintained or replenished in the hopper at a minimum of 10% fill.

[0058] The primary particles may be provided in a bimodal particle distribution, including a first set of primary' particles and a second set of primary' particles. Hopper 206 may be filled with or configured to dispense primary particles with a first particular size distribution (a first set of particles) and hopper 208 may be filled with or configured to dispense primary particles with a second particle size distribution that is different from the first particle size distribution (a second set of particles). In some embodiments the D50 of the first size distribution and the D50 of the second size distribution may differ from each other by at least 5 pm. In some embodiments the D50 of the first size distribution and the D50 of the second size distribution may differ from each other by at least about 1 pm, at least about 2 pm, at least about 3 pm, at least about 10 pm, at least about 15 pm, or any value or range between the aforementioned values. As another non-limiting example, the D50 of the first primary particles may be about 10-20 pm and the D50 of the second primary particles may be in the range of about 1-5 pm. As a further non-limiting example the D50 of the first primary’ particles may be greater than 10 pm but less than 20 pm and the D50 of the second primary' particles may be less than 5 pm. The primary particles in hopper 206 and the primary' particles in hopper 208 may be homogeneously mixed prior to or during conveyance into the first end 220 of the continuous kneader.

[0059] In further embodiments a predefined, bimodal mixture of primary particles may be provided in hopper 206 and / or hopper 208 or each set of particle sizes may be provided in respective hoppers, 206 and 208. The bimodal mixture may be a homogeneous mixture. The bimodal particle size in each set of primary particles may differ in D50 particle size range by at least 2 pm or more. A first set of particles may have a D50 in the range of about 5 pm to 20 pm and a second set of particles may have a D50 less than about 5 pm. As another example, a first set of particles may have a D50 in the range of about 6 pm to 20 pm and a second set of particles may have a D50 less than about 4 pm. The ratio of the first set of particles and the second set of particles may be about 50:50, 40:60, 60:40, 30:70, 70:30, or any ratio in between (e.g. 35:65). The second set of particles (having a D50 less than about 5 pm or less than about 3 pm) may be a fine or ultra-fine byproduct of mechanical processing of petroleum coke powder, polyvinyl chloride, mesophase pitch, pitch coke, and coal coke. Sieving may be performed prior to providing the primary particles in hoppers 206 and / or 208 in order to size control the primary particles, as discussed herein. For example, the primary particles may be sent through a size controlling mesh.

[0060] The powder or primary particles may be provided in the hoppers 206 and 208 along with an agglomeration binder. The agglomeration binder may be a solid material at room temperature. The agglomeration material or binder that is provided may be heated and melted (for example in the continuous kneader barrel) to become an agglomeration solution that mixes with the primary particles in the continuous kneader. In some embodiments hopper 206 and hopper 208 are provided as loss-in-weight hoppers. The loss-in-weight hoppers may be employed as gravimetric feeders that directly measure the primary particle and / or agglomeration binder weight to achieve and maintain a predetermined feed rate or predetermined ratio between the constituents. The feed rate may be measured in units of weight per time (e.g. kg / h), and the setpoint may be programmed by the operator in a feeder control (not shown). The feeder control may be a microprocessor or processor configured to regulate the feeding of the particles into the mixing portion of the continuous kneader. In some embodiments, gravimetric feeding may be preferred, as it can be more precise than volumetric feeding. For example, gravimetric feeding allows for more precision in the amount of material dispensed and the significant figures associated therewith. The loss-in-weight hoppers may be calibrated prior to having particles provided in them. The amount of pitch binder added to the barrel 232 may be from about 3 wt% pitch binder to about 25 wt%, about 5 wt% binder to about 20 wt% binder, about 5 wt% binderto about 15 wt% binder, about 7 wt% binder to about 12 wt% binder, or any value or range of values in between. The total combination of binder and primary particles comprises 100 wt%. For example, where pitch is provided at about 10 wt% then primary particles are provided at about 90 wt%. It is generally advantageous to provide binder at greater than 3 wt%, as agglomeration generally will not occur below about 3 wt%. However, it may be possible to reduce the wt% of the binder to below 3 wt%.

[0061] The primary particles provided from the hopper may be size controlled. In some embodiments the primary particles may have a single size distribution or one or more size distributions and be provided with a D50 between about 1 pm and about 20 pm, about 2 pm and about 17 pm, between about 4 pm and about 15 pm, between about 5 pm and about 10 pm or any value or range of values in between. In some embodiments the primary particles may be provided with a D50 less than about 50 pm, less than about 30 pm, less than about 20 pm, less than about 15 pm, less than about 10 pm, less than about 8 pm, or any value or set of values in between.

[0062] Where the agglomeration binder is provided in granular form it may be micronized and / or size controlled. In some embodiments the binder such as pitch is a micronized pitch having a D50 between about 0.1 pm and about 10 pm, about 1 pm and about 7 pm, about 2 pm and about 5pm or any range of values in between. In some embodiments the micronized pitch has a bimodal D50 distribution, similar to the distribution discussed above.

[0063] In some embodiments the powder particles are provided dry at room temperature. The powder particles may be heated prior to being fed into the powder chute 224 or heated while being conveyed in the powder chute 224. In some embodiments the powder chute 224 may contain a mixing mechanism to premix the primary particles and / or binder particles prior to being provided into the first end 220 of the continuous kneader. The mixing in the powder chute 224 may be a light mixing without significant shearing force.

[0064] In some embodiments the primary’ particles may be provided as micronized petroleum coke powder, polyvinyl chloride, mesophase pitch, pitch coke, or coal coke. In some embodiments petroleum needle coke is provided as primary particles and is in micronized form. The primary’ particles may have a D50 between about 1 pm and about 50pm, about 1 pm and about 40pm, about 1 pm and about 30pm. about 5 pm and about 20pm, about 5 pm and about 10pm. The primary particles may have a D50 less than about 100 pm, less than about 50 pm, less than about 30 pm, less than about 20 pm, lessthan about 10 pm or any value in between. The primary particles may be provided in a bi- modal particle size distribution, as discussed herein. As one example, the primary particles may be provided in two different groups, the groups having a difference in the D50 particle size distribution of at least 1 pm.

[0065] One or more agglomeration solutions may be fed from first tank 202 and second tank 204 into one or more ports, such as first port 226 and second port 228, in the region of the first end 220 of the continuous kneader. In some embodiments only a single agglomeration solution may be provided from a single tank, such as first tank 202, so that a second tank 204 is not required. In some embodiments the first tank 202 and the second tank 204 are dispensed with entirely and the primary particles and agglomeration binder are provided in micronized or granular form, as discussed above. In some embodiments the first tank and / or second tank may be modified to dispense a micronized agglomeration binder. The first tank 202 and second tank 204 may hold an agglomeration solution or a binder solution, which may be used interchangeably herein. The fill level of the tank maybe maintained or replenished to ensure a continuous fill level for a continuous kneading. In some embodiments different concentrations of agglomeration solution are provided from first tank 202 and second tank 204. In some embodiments the agglomeration solution is heated prior to being injected or pumped into a region of the first end 220 of the continuous kneader. In some embodiments, the binder may be liquified pitch. In some embodiments, the heating may advantageously allow for additional dissolution of particles in the agglomeration solution. The solution may be heated between about 60 degrees and 100 degrees, between 70 degrees and 90 degrees, or between 75 degrees and 85 degrees. In some embodiments the piping or conduit between the first tank 202 and second tank 204 and the first port 228 and second port 226 is heated.

[0066] The first port 228 and / or second port 226 may be positioned relative to the entrance of the primary particles into the continuous kneader 200. For example, the first port 228 and / or second port 226 may provide an agglomeration solution into the mixing shaft of the continuous kneader such that the agglomeration solution is provided into the mixing shaft of the continuous kneader about 15 cm up from the powder chute 224. The agglomeration solution may additionally or alternatively be injected into the mixing shaft of the continuous kneader at one or more ports along the length of the mixing shaft, from the first end 220 to the second end 222 of the continuous kneader 200. In some embodiments the continuous kneader is provided with two or more, three or more, four ormore, or five or more ports equally spaced along the length of the kneader for injecting an agglomeration solution or material.

[0067] The solution may be controlled by a control processor, nozzle, or valve in order to prevent clogging of material within the continuous kneader due to a high agglomeration solution to primary particle ratio. In some embodiments a mass flow meter may be used in order to control the injection of agglomeration solution into the mixing shaft of the continuous kneader 200. In some embodiments, pump mass flow curves may be calibrated before and during a test trial to control the amount of agglomeration solution and to provide an accurate solution to particle ratio. The solution to particle ratio may be controlled to reduce variances and prevent clogging. In some embodiments the solution to particle ratio is advantageously’ maintained within less than 3% of the desired ratio, within less than 2% of the desired ratio, within less than 1% of the desired ratio, within less than 0.5% of the desired ratio of any value in between. In a preferred embodiment the solution to particle ratio is maintained within 1% of the desired ratio.

[0068] The agglomeration solution may be provided through the first port 228 or second port 226 such that the agglomeration solution constitutes about 5% to about 15% by mass of the total mixed material. In some embodiments the mass of agglomeration solution constitutes at least about 5%, at least about 7%, at least about 10%, at least about 12%, at least about 15%. at least about 20% or any range in between (i.e. about 10- about 12%) of the total mass of the mixed material provided into the continuous kneader 200.

[0069] The agglomeration solution may be an aqueous solution, organic solution, or mixture of solvents. The agglomeration solution may have one or more solutes provided. The agglomeration solution generally provides hard carbon forming or non- graphitizable materials that adhere to graphitic or graphite-forming primary particles. In some embodiments the agglomeration solution comprises non-graphitizable lignin, sugar, or plant-derived carbohydrate molecules that may' act as binder molecules. The lignin may be provided as ammonium lignosulfonate, sodium ligninsulfonate, soda lignin, or dealkaline lignin. The lignin is provided in a form that can be dissolved or homogeneous in an aqueous solution. Ammonium lignosulfonate may be selected for its ability to dissolve in an aqueous solution. In some embodiments the aqueous solution may be a basic solution in order to facilitate dissolution of lignin molecules.

[0070] The form of the agglomeration solution may include, without limitation, homogeneous or heterogeneous solutions comprising agglomeration particles dissolved or dispersed in a solvent, an aqueous (water) solution, an alkaline aqueous solution, a misciblesolution, an immiscible solution, a semi-organic solution, a semi-aqueous solution, an acidic aqueous solution, a fluid or viscous solution, or a substantially aqueous solution.

[0071] The material provided in the solution may be non-graphitizable organic molecules. The organic molecules may be selected from a group consisting of ammonium lignosulfonate, sodium ligninsulfonate, soda lignin, dealkaline lignin, sucrose, ribose, riboside, glucose, glucoside, mannose, mannoside, galactose, galactoside, talitol, taloside, rhamnitol, rhamnoside, maltose, maltoside, lactoside, lactoside tetraacetate, 2,3-desoxy- 2,3-dehydrolactoside, 2,3-desoxy-2,3-dehydrolactoside pentaacetate, 2,3-desoxylactoside, glucouronate, N-acetylglucosamine, fructose, sorbose, 2-deoxygalactose, 2-deoxy glucose, maltulose, lactulose, palatinose, leucrose, trehalose, gentiobiose, isomaltose, maltulose, turanose. lactose, mannitol, sorbitol, dulcitol, xylitol, 1 -aminosorbitol, isomaltitol, cellobiitol, lactitol, maltitol, and fructose.

[0072] The agglomeration solution may be an aqueous solution containing lignin, sugar, or plant-derived carbohydrate molecules with about 1%- about 50% solids byweight. about 3%- about 20% solids by weight, about 3%- about 15% solids by weight, about 8%- about 15% solids by weight, at least about 3% solids by weight, at least about 5% solids by weight, at least about 8% solids by weight, at least about 10% solids by weight, at least about 15% solids by weight, at least about 20% solids by weight, at least about 30% solids by weight. In some embodiments the lignin, sugar, or plant-derived carbohydrate molecules are dissolved or dispersed in the aqueous water solution. The lignin, sugar, or plant-derived carbohydrate molecules may functionally act as binder molecules in the aqueous solution. In one embodiment components of the agglomeration solution are heated to make an agglomeration solution containing between about 8% to about 25% solids by weight. In some embodiments an aqueous agglomeration solution may have a concentration between about 0. 1 wt% and about 40 wt%, between about 1 wt% and about 30 wt%, between about 1 wt% and about 20 wt%, between about 2 wt% and about 18 wt%, between about 2 wt% and about 15 wt%, between about 2 wt% and about 12 wt%, or between about 8 wt% and about 10 wt%.

[0073] In some embodiments the agglomeration solution is provided as pitch. The pitch may be petroleum, coal tar, or pitch derived from plants (such as pine tar). Tar and coal tar may sometimes be used interchangeably. The pitch may be a high softening point and high purity- petroleum pitch. The pitch may be solid at room temperature as a viscoelastic polymer and when subjected to heat the pitch generally becomes less viscous. The pitch may have a softening point in the range of about 50°C to about 250°C or about100°C to about 200°C with less than about 5% mesophase. In some embodiments the pitch has less than about 3% mesophase, less than about 2% mesophase, less than about 1% mesophase, or any range in between these values (i.e. about 2- about 3%). In some embodiments the pitch may be a high softening point pitch with a softening point below about 300°C. In some embodiments the pitch may be a medium softening point pitch with a softening point below about 150°C. In some embodiments the softening point of the pitch may be below about 100°C. In some embodiments the pitch may have a softening point around 70°C. In some embodiments the pitch may have a softening between any of the aforementioned values (i.e. about 100°C to about 150°C).

[0074] The pitch may be provided in the form of granular isotropic petroleum pitch with a D50 between about 3000 pm and 1 cm. The isotropic petroleum pitch may have a high softening point and high purity. In some embodiments the softening point of the granular isotropic petroleum pitch is in the range of about 150°C to about 200°C. In some embodiments the pitch may be a micronized isotropic petroleum pitch, with a D50 size between about 2 and about 5 m. The micronized pitch may be a high purity, high melting point pitch as well.

[0075] One or more pumps 212 may be used to pneumatically pump the agglomeration solution into the continuous kneader. The one or more pumps 212 may be any pump known in the art. In general, the pumps push or inject the agglomeration solution into the continuous kneader at a predetermined rate or in a predetermined ratio in order to provide a suitable ratio of agglomeration solution to primary particles. The predetermined rate of inj ection may be controlled by software known in the art and through mechanical means such as nozzles, valves, gates, etc. The agglomeration solution may be sprayed into the first end 220 of the continuous kneader as a mist or droplets or it may be injected into the continuous kneader as a stream. The first tank 202 and the second tank 204 may also be configured to provide a predetermined ratio or concentration of agglomeration particles (such as non-graphitizable particles mentioned above) with or in the agglomeration solution. In some embodiments the agglomeration solution may be gravity fed so that no pumping is required.

[0076] In some embodiments the agglomeration solution comprises about 3 to about 50% of the total feed mass conveyed along the length of the continuous kneader, preferably between about 5% and about 15% of the total feed mass. Where the agglomeration solution or agglomeration binder is more than 50% of the total feed mass this generally results in clogging due to a high liquid to powder ratio.

[0077] The continuous kneader may be driven by one or more motor, such as motor 230. The motor 230 may be configured to actuate the internal mixing mechanism of the continuous kneader in order to provide a suitable mixture of materials. For example, the motor 230 may provide a rotation force on an internal screw (discussed further with regards to Figures 2 and 3) to convey material from the first end 220 of the continuous kneader to a second end 222 of the continuous kneader such that the material can be discharged from a discharge port 214. The motor may be a 75 horse power (HP) motor with a 300 revolution per minute (RPM) maximum. In some embodiments the motor is controlled within a max RPM of about 200 with a 150 pounds per hour overall feed rate. In some embodiments the motor is controlled within a max RPM of about 120 with a 75 pounds per hour overall feed rate. The torque of the motor may be controlled in order to prevent fluctuations in mixing speeds. In some embodiments the torque of the motor is steady state with fluctuations of < about 10% of a set limit, such as a limit of 200 RPM. In some embodiments the fluctuations may be below about 5%, below about 3%, below about 2%, or any value in between. The conveyance of the material of primary particles and agglomeration solution may be substantially continuous. In some embodiments the material is conveyed in a reciprocating fashion, such that the material is substantially conveyed forward along the screw with reciprocating oscillations.

[0078] The continuous kneader may have one or more exhaust ports 210, which may facilitate the release of gases during the mixing process. For example, in some embodiments the agglomeration solution may have volatile components that are converted to gas during the continuous kneading, such as at temperatures exceeding about 100 degrees Celsius. The exhaust ports may be provided with various filters in order to allow- the escape of gases from the continuous kneader and prevent the escape of solid particles, such as primary or secondary particles. In some embodiments the venting of gases from the exhaust port 210 may be facilitated by one or more gas scrubbers in order to prevent the release of noxious gases into the atmosphere.

[0079] The continuous kneader has a mixing shaft, such as a barrel 232, which extends from the first end 220 to the second end 222 of the continuous kneader. The barrel 232 houses an internal mixing mechanism, such as a screw7. The barrel 232 may be generally cylindrical, but other shapes may be envisioned by a person having ordinary7skill in the art. The barrel 232 may contain one or more hinges 234 which may be used to view and access the inside of the barrel. The hinges 234 may be used to replace brokencomponents, modify the amount or position of flights on the internal screw, or retrieve samples of mixed material for testing of the material’s properties.

[0080] The diameter of the barrel 232 may be optimized in order to accurately mix and size control the primary particles mixed with the agglomeration solution. In some embodiments the the length to diameter ratio of the barrel of the continuous kneader is greater than about 10: 1, greater than about 20: 1, greater than about 30: 1, greater than about 40: 1. or any of the values between (i.e. about 27: 1). In some embodiments the length to diameter of the continuous kneader barrel 232 may be between about 10: 1 and 40: 1, between about 15:1 and 35:1, between about 20: 1 and 30: 1, or any range between the ranges. In a preferred embodiment the length to diameter ratio of the barrel between about 25: 1 and 30: 1. Having a length to diameter ratio greater than 15: 1 is advantageous as it provides a longer section of shearing per unit of material (comprising of primary particles and agglomeration binder) while still providing adequate throughput .

[0081] The mixing portion of the continuous kneader may be temperature controlled via a temperature control system 216. The temperature control system may facilitate temperature control through any known software. In some embodiments the temperature control system may be configured to provide a constant temperature profile along a mixing portion, from the first end 220 to the second end 222, in the barrel 232. In some embodiments the temperature control system may be configured to provide a temperature variation or gradient along one or more zones between the first end 220 to the second end 222. In some embodiments the continuous kneader 200 has at least 3 heating zones, at least 5 heating zones, or at least 7 heating zones. Within the temperature zones there may be a heating and cooling section such that there are at least 6, at least 10, or at least 14 heating and cooling sections. The heating and cooling sections may be configurable in a temperature range of from -20°C to 350°C, but the zones may be configured between a temperature of from about 100°C to about 350°C.

[0082] The temperature may be configured to increase or decrease the temperature of the first end 220 or the second end 222 based upon one or more sensors or feedback mechanisms that measure the temperature of the mixed components. The feedback mechanism may be contact or non-contact sensors. In some embodiments the temperature feedback mechanism is a thermal infrared sensor, and the temperature may be sensed through one or more windows in barrel 232.

[0083] The temperature in the first end 220 or the second end 222, or any section between the first end 220 and the second end 222, may be controlled to be belowabout 600°C. below about 500°C, below about 400°C, below about 300°C, below about 250°C, or any of the values between (i.e. between about 300°C and about 400°C). A reduced temperature (for example below about 500°C) advantageously reduces the energy requirements for the continuous kneader. The temperature along the mixing portion of the continuous kneader may also be controlled between about 100°C and about 500°C, between about 150°C and 450°C. between about 200°C and 400°C, or between about 250°C and about 350°C. Where the agglomeration solution has a melting point the temperature along the length of the continuous kneader may be controlled within within about 50°C of the softening point of the agglomeration solution. In some embodiments one or more zones along the first end 220 and the second end 222 may be controlled such that the temperature is within about 40°C of the softening point of the agglomeration solution, about 30°C of the softening point of the agglomeration solution, about 20°C of the softening point of the agglomeration solution, about 10°C of the softening point of the agglomeration solution, or any range of values between (i.e. within about 30°C to about 40°C of the softening point).

[0084] The temperature may be controlled to provide expansion and contraction zones along one or more sections of the continuous kneader 200. In some embodiments a first zone located in the first end 220 may be configured as a preheating zone or a premelting zone. The first zone may be the first section of the mixing shaft, such that it is the first section of the continuous kneader along a single axis of a mixing shaft. The first zone may be configured about 50°C cooler than one or more zones that are downstream of the first zone, where downstream is the conveyance direction from the first end 220 to the discharge port 214 along a single, central mixing axis. In some embodiments the first zone in the first end 220 may be configured below the softening point of the agglomeration binder or solution such that melting of the agglomeration binder does not occur in the first zone. In some embodiments there are about 7 melting zones where the first zone is controlled to a temperature more than 25°C outside of the softening point of the agglomeration binder or binder and the remaining 6 zones are controlled to a temperature within 25°C of the softening point of the agglomeration binder. For example, the first zone may be controlled significantly below the softening point of the agglomeration binder (for example below 100°C) and the second through sixth zones may be controlled within 25 °C of the softening point of the agglomeration binder.

[0085] The temperature of the continuous kneader may be controlled with any number of temperature control mechanisms known in the art, including electrical or thermal materials. In some embodiments the barrel 232 or internal volume of the barrel 232 istemperature controlled with one or more thermal coils or Peltier elements. In some embodiments the barrel 232 or internal volume of the barrel 232 is temperature controlled via a heated fluid circulated through the outer casing of barrel 232. In some embodiments the temperature of the barrel is controlled via heated sand on the exterior or in the thickness of barrel 232. In some embodiments the heated material or fluid may be circulated through thermal control port 218. In some embodiments the circuitry for the temperature control system may be provided in thermal control port 218.

[0086] As discussed earlier the material containing secondary particles are discharged from the continuous kneader through discharge port 214. The discharge port 214 may convey material directly or indirectly to an apparatus for size controlling or heating the secondary particles. For example, the discharge port 214 may be connected to a hose, conveyor, belt, tube, vessel, or other apparatus. In some embodiments the secondary particles are discharged from the discharge port 214 into a controlled environment. For example, the air temperature, pressure, composition, or humidity may be controlled in order to prevent contamination or other reactions that may occur. For example, the air may have a reduced oxygen content or reduced water content. The flow out of the discharge port may have a sheath or conveyance tube to facilitate negative pressure or reduce pressure in order to create a vacuum to suck material out of the discharge port into a size controlling apparatus or calcination vessel, as well as reduce interaction of the discharged material with potential environmental or atmospheric contaminants, etc.

[0087] Figure 3 illustrates a view of internal structure of a continuous kneader 300. The continuous kneader 300 may have substantially the same systematic configuration as the continuous kneader 200 discussed above. Thus, continuous kneader 300 may be seen as a cutaway of continuous kneader 200. The continuous kneader may be opened by unlocking one or more hinges, such as the hinges 234 discussed above, that are connected to or in communication with the barrel casing 306.

[0088] The continuous kneader 300 has a rod 302 extending along the length of the mixing portion of the continuous kneader. The rod is generally located within a central portion of the barrel casing 306 for symmetrical rotation. The rod 302 is connected to one or more motors, such as the motor 230 discussed with regard to continuous kneader 200 above. The rod 302 is rotated by the one or more rotors to turn the flights 314 of the rod 302. The flights 314 of the rod 302 are generally in a helical configuration and the rod 302 in combination with the flights 314 may be termed a “screw / ' although the generally helical configuration of the flights 314 themselves may be termed a “screw.” The rotation of theflights 314 may exert a forward advancement of the mixing material toward the discharge port of the continuous kneader, such as the discharge port 214 discussed above.

[0089] The mixing material may have a residence time along the length of the mixing portion of less than 5 minutes, less than 3 minutes, less than 2 minutes, less than 1 minute, less than about 30 seconds, or any range of values between. In some embodiments the mixing time is about 1 minute. Thus, the primary particles mixed with an agglomeration solution are generally conveyed along the generally helical flights 314 in a continuous manner for about a minute before being discharged from the continuous kneader 300. The residence time may be increased by placing a restriction on the discharge of the continuous kneader. The restriction on the discharge port may be a mechanical discharge mechanism. Examples could include a gate, flap, bar, reduced discharge nozzle diameter, or any other restriction mechanism known in the art.

[0090] The inner side of the barrel casing 306 is provided with one or more or a plurality7of kneading bolts 304. A kneading bolt 304 may also be termed a “pin."’ The kneading bolts generally work in coordination with the flights 314 in order to provide mixing and / or shearing forces on the material provided into the continuous kneader 300. As discussed more with regard to the figures below, the kneading bolts are provided adjacent to the rotating flights 314 with a configurable gap between the flights 314 and the kneading bolts 304. The gap may be configured on a per kneading bolt basis or on a per mixing section basis. The gap may vary between about 0.5 mm and about 10 mm. This advantageously tailors the shearing force in each section, as discussed further herein.

[0091] The continuous kneader 300 may have one or more kneading sections, such as first section 308, second section 310, and third section 312. Although only three sections are depicted here, a person having ordinary7skill in the art would understand that the sections may not be limited, and more than three sections may be desirable in order to provide optimal mixing and / or shearing on the primary7particles and agglomeration solution. The number of flights 314 or the number of kneading bolts 304 may be varied from section to section in order to vary the mixing and / or shearing action. As one example, the first section 308 may be configured as a high shearing zone, second section 310 may be configured as a low shearing zone, and third section 312 may be configured as a high shearing zone. Many other configurations may be envisioned such as a high, high, low configuration, a low. low, high configuration, a high, medium, low configuration, a low, medium, high configuration, etc. A low shearing zone or section may be provided merely as a conveyance zone where material is generally mixed and conveyed without highshearing forces. As discussed further below, the shearing force is generally dictated by the shear gap between the kneading bolts 304 and the flights 314.

[0092] The length of the mixing portion including the rod 302 and flights 314 may be varied based upon the desired final product. In some embodiments the shaft of the continuous kneader has a length to diameter ratio of about 30: 1. The diameter is generally measured as the diameter of the cylindrical portion of the shaft, such as the diameter of the barrel casing 306 when the barrel casing is closed. In some embodiments the diameter of the barrel casing 306 is about 60 mm. In some embodiments the diameter of the mixing shaft, such as barrel casing 306, is at least 20 mm, at least 40 mm, at least 60 mm, at least 80 mm, at least 100 mm, at least 120 mm, at least 200 mm, at least 400 mm, at least 1000 mm, or any range of values between (i.e. 60-80 mm). In some embodiments the barrel casing is about 60 to about 100 mm in diameter.

[0093] Figure 4 illustrates various configurations of screw flights 314 that may be used in the continuous kneading process of the present invention. The screw flight configurations shown in Figure 4 may be used in various zones or sections of the continuous kneading apparatus. First mixer 402 has fewer screw flights 314 than second mixer 404. and second mixer 404 has fewer screw flights 314 than third mixer 406. First mixer 402 may be used for high dispersive mixing and low distributive mixing, second mixer 404 may be used for medium dispersive mixing and medium distributive mixing, and third mixer 406 may be used for high distributive and low dispersive mixing. Third mixer 406 provides less free mixing volume than first mixer 402, which can increase the amount of mixing force to which the mixed material is subjected. In some embodiments increasing the number of flights increases the amount of shear force per length of the continuous kneader.

[0094] Figure 5 illustrates rotation, strokes, and material flow of a tri-stroke continuous kneading according to some embodiments herein. As with Figure 3, Figure 5 depicts several kneading bolts 304 that work in coordination with the flights 314 in order to provide mixing and / or shearing forces on the material provided into the continuous kneader 500. The kneading bolts are provided adjacent to the rotating flights 314 with a configurable shear gap between the flights 314 and the kneading bolts 304, The gap may vary between about 0.5 mm and about 10 mm. As shown in Figure 3, the kneading bolts 304 may be provided on the inner surface of the barrel casing 306. However, the kneading bolts may be provided in other positions, where appropriate, to provide a shear gap between the kneading bolts 304 and the flights 314. For example, a person having ordinary skill inthe art could envision a configuration where the kneading bolts and flights are swapped with each other.

[0095] Due the helical nature of the flights 314 the mixed material is generally conveyed in a product flow direction 510. The flights 314 are attached to a central spinning axis and rotate in a rotation direction 512. The kneader may be a reciprocal kneader, as shown here, with a stroke 508. The stroke 508 enables multiple paths between the flights 314 and the kneading bolts 304. For example, a first path 502 is depicted with a unique path for shearing mixing material between the flights 314 and the kneading bolts 304. After one or more flights 314 pass one or more kneading bolts 304 the continuous kneader may initiate a forward or backward stroke 508 in order to produce a new path, such as second path 504. This general process may continue with third path 506. Thus, the tri-stroke continuous kneader may produce a shear gap (a gap between a kneading bolt 304 and a flight 314) on either side of the kneading bolts 304, effectively using the shearing space within the barrel 232. Through the reciprocating nature of the continuous kneader the bolts may advantageously mix and shear material in several ways. The continuous kneader may be configured with a shear gap larger on one side of the kneading bolt 304 than on the other side of the kneading bolt 304.

[0096] Figure 6 depicts a shearing mechanism of a continuous kneader. As discussed previously, a shear gap 602 may be produced between one or more flights 314 and one or more kneading bolts 304. The kneading bolts 304 and flights 314 may be the same as those depicted in Figures 3-5. The shear gap 602 generally produces shear forces on the mixing material. A Shear forces occur when two objects slide past each other in opposite directions. The shear gap represents the distance or gap between the surfaces causing shear stress. The shear gap 602 is depicted in Figure 6 as the distance between two lines, bounded by arrows, that represent the general distance between the flights 314 and the kneading bolts 304. As with Figure 5, a rotation direction 512, stroke 508, and material flow direction 510 interplay throughout the mixing process. The general reciprocating or oscillating nature of the stroke 508 can be opposite of the general product flow direction 510, but the mixed product nonetheless continues to flow in the product flow direction 510 as it is advanced forward through the general helical nature of the flights 314 that are rotated in a rotation direction 512.

[0097] The distance of the shear gap 602 may be relatively constant as the flight advances from a first flight position 606 to a second flight position 608. The shear gap 602 varies as the flight advances from a first flight position 606 to a second flight position 608.In some embodiments the length of the flights 314 may vary to increase the length that the flight 314 extends along the kneading bolt 304 (such as to increase the amount of elevated shear force).

[0098] The kneaded material is subjected to shear forces as it is sent in a direction 604 of the shear gap 602 where the material will be sheared by the relative movement of the kneading bolts 304 and the flights 314 in opposite directions. As shown in Figure 6, only some of the material may be sent through the shear gap 602 and some of the material will be excluded from a particular shear gap 602 and deflect in a direction opposite of the direction 604. In some embodiments the shear gap generally decreases along the length of the continuous kneader. For example, a first section in the first end 220 may have a shear gap in excess of 10 mm, a second section may have a shear gap of about 10 mm, a third section may have a shear gap of about 8 mm, a third section may have a shear gap of about 5 mm, a fourth section may have a shear gap of about 3 mm, and so on. In some embodiments various sections from the first end 220 to the second end 222 may each have low shear sections and high shear sections. A first section may have shear gaps of >10mm (high) / 6 mm (low), a second section with 10 mm (high) / 4 mm (low), a third section with 8 mm (high) / 3 mm (low), a fourth section with 6 mm (high) / 2 mm (low), a fifth section with 4 mm (high) / 1 mm (low), a sixth section with 3 mm (high) / 0.5 mm (low), a seventh section with 2 mm (high) / 0. 1 mm low, or any combination of the previous values. In some embodiments sections may be interspersed with other sections, such as a fifth section may be interspersed with fourth sections. In some embodiments the order of sections may be varied, interspersing higher shear sections with lower shear sections. In some embodiments the shear sections may be reversed, with a seventh section in first end 220 and a first section in second end 222. The expansion and contraction temperature zones mentioned previously may be paired with one or more high shear or low shear sections.

[0099] The shear gap 602 may be configured between about 0.1 mm and 10 mm, between about 0.5 mm and 7 mm, between about 1 mm and 5 mm, between about 2 mm and 4 mm. or any value in between. In some embodiments the shear gap 602 may be less than about 15 mm. less than about 10 mm, less than about 7 mm. or any value in between the stated values. In some embodiments the continuous kneader may have one or more high shear sections with a shear gap of less than about 4 mm and the one or more low shear sections with a shear gap of more than about 4 mm. This advantageously may provide one or more conveyance zones with a wider shear gap and one or more shear zones with a narrower shear gap.

[0100] Although the embodiments discussed above relate to a single barrel apparatus with a first end 220 and a second end 222, it should be understood that a person having skill in the art may implement variations of the process. A person having skill in the art would appreciate that the continuous kneader may have converging or diverging barrels that converge or diverge from a single barrel. The continuous kneader may also have multiple discharge ports for discharging material from various stages or sections of the continuous kneader. Thus, the effective length of the continuous kneader may be varied by opening or closing discharge ports at predetermined distances along the length of the continuous kneader.

[0101] Figure 7 depicts a general process for the production of agglomerated particles. 710 comprises providing a continuous kneader having a first end and a second end. 720 comprises providing primary particles comprising a graphitizable material into the first end of the continuous kneader. 730 comprises providing an agglomeration solution into the first end of the continuous kneader. 740 comprises mixing the primary particles and the agglomeration solution as they are conveyed along the length of the continuous kneader from the first end to the second end to produce agglomerated secondary particles, wherein internal temperature along the length of the continuous kneader is maintained at a temperature below about 500°C. Although not depicted, 740 may be subsequently followed by calcination and graphitization, as discussed in embodiments herein, to produce an anode material.

[0102] The material produced according to embodiments herein may be incorporated into a batter . For example, after the secondary particles have been discharged from the continuous kneader they may be calcined and then graphitized to produce anode materials. The anode materials may then be incorporated with binders or additives in a wet or dry process and applied to a current collector of a battery. The battery may be a rechargeable battery or single use battery.

[0103] In some aspects, the disclosure relates to a batten,' containing the graphitized anode material produced according to embodiments disclosed herein. The battery anode materials disclosed herein may be incorporated into various consumer or commercial devices. Examples include but are not limited to personal electronic devices, electric cars or mobility devices, battery energy storage devices, electric tools, electric bicycles, electric toys, or any other electrically powered device. The anode material may be coated onto a current collector with one or more binders or conductive additives.Post Continuous Kneading

[0104] The discharged particles may be size controlled by varying mixing parameters, such as mixing speed, shear gap, mixing shaft length, residence time, etc. In some embodiments a mixture of primary particles and secondary particles (comprising two or more primary particles) are discharged from the discharge port. In some embodiments the ratio of secondary’ particles to primary particles discharged ranges from 1: 1 to 10,000: 1 or any value in between.

[0105] In some embodiments the discharged material is primarily comprised of granulated secondary' particles. For example, the discharged material may have a ratio of secondary' particles to primary particles of at least about 100:1. In some embodiments the ratio of secondary particles to primary particles is at least about 10: 1, at least about 50: 1, at least about 200: 1, at least about 500: 1, at least about 1,000: 1, or any value in between.

[0106] In some embodiments the discharged material is primarily comprised of granulated micro or macro (e.g. +1 mm) secondary particles. The granulated particles may be composed of at least two primary particles agglomerated or bound together or in a range of 2 to about 100 primary particles bound together. In some embodiments the granulated particles are comprised of 2 to about 50 primary particles bound together, about 3 to about 30 primary particles bound together, about 3 to about 15 primary particles bound together, about 3 to about 7 primary particles bound together, or any value in these ranges (i.e. about 4 particles). In some embodiments the micro granulated particles are comprised of 2 to about 10 particles bound together. The secondary particles discharged from the second end of the continuous kneader may have a Mohr’s hardness of more than about 2. In some embodiments macro-granulated secondary particles or briquettes may be released from discharge port. The macro-granulated particles have a D50 of more than about 1 mm to about 25 mm. In some embodiments the macrogranulated secondary particles may have a D50 particle size between about 25 mm and about 50 mm.

[0107] The target size of the secondary’ particles may be controlled to a D50 in a range of about 10pm to about 100pm, about 100pm to about 2000pm. about 2mm to about 25mm, or any range of values between. Preferably the secondary particles are controlled in a microgranulation range to have a D50 within a range of 50pm to 500pm.

[0108] The discharged particles, comprised of secondary particles and a minority portion of ungranulated primary particles, are subjected to calcination after continuous kneading. The primary’ particles may be calcined together with the secondaryparticles and subsequently removed or sieved and separated from the secondary particles after calcination. However, in some embodiments the primary particles may sieved or separated prior to calcination or after graphitization. Advantageously, primary particles that are separated from the secondary particles may be reused and inserted back into the hoppers (206 or 206), first end of the continuous kneader (220), or additional ports along the length of the continuous kneader. Reusing non-agglomerated primary particles is beneficial as it reduces waste and lowers cost of the synthesized battery anode materials. Similarly, where oversized secondary particles are sieved or separated from size-selected secondary particles these may also be broken up and / or recycled for additional reuse.

[0109] The material discharged from the discharge port 214 may be fed through a conveying mechanism directly to a calcination apparatus. In some embodiments the secondary particles are not cooled to room temperature prior to being conveyed to the calcination apparatus. The calcination process may calcine the secondary particles, harden non-graphitizing material in the agglomeration solution or binder, and / or remove volatile content. The calcination apparatus may be a rotary kiln. The rotary kiln may be configured to subject the secondary particles to mechanical and thermal agitation and change the size of the granules. The size of the secondary particles may be reduced in the rotary kiln. For example, macro-granulated secondary particles may be size controlled to sub-macro secondary- particles having a particle size below about 1 mm. The secondary particles may be further size controlled to a particle size below about 750 pm, below about 600 pm, below about 500 pm, below about 400 pm, or between about 250 pm and about 500 pm. The calcination temperature can be controlled between 800°C and 1350°C, between 900°C and 1200°C, between 1050°C and 1150°C, or any value in between. In some embodiments the calcination temperature is about 1100°C. The residence time of the secondary particles in the calcination apparatus is around 30 minutes to 5 hours. During the calcination nongraphitizing carbon particles are crystallized and low boiling point impurities and volatile compounds are removed from the secondary particles. The calcined secondary particles may be cooled below oxidation temperature before discharge from the calcination apparatus.

[0110] After calcination, the secondary particles may be passed into a continuous classifying grinding mill for particle sizing. The classifying grinding mill is able to remove any particles that are below the optimal size (such as below 5 pm) and also to reduce the size of any oversized particle that was not size controlled during calcination, etc. The classifier speed and airflow may be adjusted depending on the powder properties toachieve target size. Oversized particles exceeding about 25 pm are further downsized and separated for recycle. The resulting granules that have passed through sizing may have a target D50 size of about 10- about 10pm, more preferably about 12- about 17pm, with a normal size distribution.

[0111] Following calcination and particle sizing, the secondary particles may be directly fed or conveyed into a continuous powder flow graphitization process. In a continuous powder flow graphitization process the soft-carbon species are atomically rearrange into a graphitic structure. The temperatures in the graphitization process may be greater than about 2000°C, greater than about 2500°C, greater about 2800°C, greater than about 3000°C, greater than about 3500°C, or any value in between (i.e. between about 2000 °C and 3500°C). The residence of the secondary particles in the continuous flow graphitization process can be controlled from about 1 to about 30 hours, about 3 to about 25 hours, about 5 to about 20 hours, or about 8 to about 12 hours. In some embodiments about 10 hours is a time sufficient to convert or grow' graphite layers having a proper order for high lithium-ion intercalation potential.

[0112] The graphitized secondary particles may be cooled to room temperature and incorporated into an anode of an electrochemical cell. In some embodiments the anode materials are incorporated onto an anode current collector in a dry or wet process w ith one or more binders. The electrochemical cell may be a lithium-ion electrochemical cell. Thus, the process may be used to continuously process raw materials including primary particles in an agglomeration solution into final lithium-ion grade synthetic graphite to be used as an anode active material.

[0113] In some embodiments the hard carbon content of the anode active material is between about 0.01 wt% and about 5%, between about 0.1 wt% and about 4 wt%; between about 0.2 wt% and about 4 wt%, between about 0.3 wt% and about 4 wt%, between about 0.5 wt% and about 2.5 wt%, between about 0.5 wt% and about 3.25 wt%, or between about 0.5 wt% and about 3 wt%. In a preferred embodiment the hard carbon content is between about 0.3 wt% and about 2.5 wt% or preferably about 1 wt% to about 1.5 wt%. In some embodiments the hard carbon content in the anode active material may be stated in terms of minimum hard carbon content such as at least about 0. 1 wt%, at least about 0.2 wt%, at least about 0.3 wt%, at least about 0.4 wt%, at least about 0.5 wt%, at least about 1 wt%, at least about 2 wt%, or at least about 3 wt%. In a preferred embodiment the hard carbon content is at least 0.3 wt%. In embodiments disclosed herein the hard carbon content is substantially derived from the agglomeration solution / material and theprimary particles are substantially free of non-graphitizable hard carbons. In various embodiments all of the hard carbon is derived from the agglomeration solution composed of plant-derived carbon materials.

[0114] The ratio of soft carbon to hard carbon in the anode active material may vary', for reasons discussed above. It may be desirable to have more or less hard carbon depending upon the charge / discharge characteristics of the powder or the desired size of the secondary’ particles. The soft carbon / hard carbon weight ratio may be about 60:40, about 65:35, about 70:30, about 75:25, about 80:20, about 85: 15, about 90: 10, about 95:5, about 97:3, about 98:2, about 99: 1, about 99.9:0.9 or any number in between. In the preferred embodiment the weight ratio of soft carbon to hard carbon is about 97.5:2.5.

[0115] In some embodiments the pre and post continuous kneading steps are aligned with the throughput of continuous kneading to enable a fully continuous process flow. In some embodiments, multiple rate-limiting operational units are required to maintain full utilization of the rate maximizing step. Storage can be included between process steps to allow for eventual equipment planned and unplanned downtime. Intermediate process storage between unit operations can be determined by those skilled in the art.Definitions

[0116] “Graphitizable’7used herein should be interpreted as a person having ordinary skill in the art would understand the term, but generally refers to a material that is capable of being converted to graphite through heating, such as pyrolysis at temperatures exceeding 1000 degrees Celsius. Graphitizable materials may be referred to as soft carbon. Graphitizable materials may be composed almost entirely of the element carbon or may be substantially composed of the element carbon. Graphitizing carbons are generally soft and non-porous. Some examples of graphitizable materials are micronized petroleum coke powder, polyvinyl chloride, mesophase pitch, pitch coke, or coal coke. Graphitizable materials that have been graphitized may be termed artificial graphite.

[0117] “Non-graphitizable” used herein should be interpreted as a person having ordinary skill in the art would understand the term but generally refers to a material that is not capable of being converted to graphite through heating. In some instances non- graphitizable materials may be referred to as chars, charcoal, or hard carbons. Some non- exhaustive examples of non-graphitizable carbons are glassy carbon and polyvinylidene chloride (PVDC). While not being bound to any theory, it is theorized that cross-linkingbetween the basic structural units of the non-graphitizable material prevents conversion of the material to graphite during pyrolysis.

[0118] '‘Shear gap” used herein should be interpreted as a person having ordinary skill in the art would understand the term but generally refers the distance or gap between two surfaces causing shear stress. Shear forces occur when two objects slide past each other in opposite directions or the relative motion between the two is in opposite directions.

[0119] “Solution” used herein should be interpreted as a person having ordinary skill in the art would understand the term but generally refers to a formulation in a liquid state having one or more solvents and may additionally have one or more solutes.

[0120] The term “mesophase” herein should be interpreted as a person having ordinary skill in the art would understand the term but generally refers to nematic liquid crystal structure which can be graphitizable.

[0121] The term “micronized pitch” or “micronized isotropic petroleum pitch” herein should be interpreted as a person having ordinary skill in the art would understand the term but generally refers to isotropic micronized particles of pitch. Micronized pitch is similar to viscoelastic pitch, but it has been micronized and is in a granular form. Micronized pitch has a relatively high softening point, such as above 100 degrees Celsius, which allows for micronization. Micronized pitch is produced by mechanical attrition of a hardened pitch material.

[0122] The term “conveyance zone” as used herein refers to a mixing zone that primarily conveys mixed material forward in a product flow direction. A conveyance zone generally has a shear gap greater than 4 mm.

[0123] A “tri-stroke continuous kneader” should be interpreted as a person having ordinary skill in the art would understand the term, but generally refers to a continuous kneader with a central rotating screw, stationary kneading bolts along the interior casing of the kneader, and a reciprocating stroke that produces three kneading paths between the screw flights and the kneading bolts.EXAMPLES

[0124] The following Examples are intended to be exemplary in nature and are not intended to limit the scope of the application in any way.Example 1

[0125] Preparation: Two loss weight hoppers, previously calibrated, were loaded with materials. One with petroleum needle coke, micronized to a D50 between 5and 10pm, and the other with micronized isotropic petroleum pitch, with a D50 size between 2 and 5 pm. These feeders fed directly into a chute dropping into the entry port of continuous mixer. The continuous reciprocal mixer had a 60mm diameter, and a 28: 1 L:D ratio, indicating the length is 28 times larger than the diameter. The system utilized a 75 HP motor with a 300 rpm maximum. Heating / cooling zones were located down the length with 14 in total across 7 temperature zones.

[0126] The elements were configured with expansion and contracting zones, and consistent heat was applied through the shaft. The first heating zone was ~50°C cooler than the rest, to allow a longer conveyance zone before melting occurred. The zones were set from 200 to 300°C through the testing. The system tested can range from -20°C to 350°C.

[0127] Mixing occurred at 120 rpm, with an overall mass feed of 130 pounds per hour or 59 kilograms per hour. The ratio of pitch binder to primary particle coke was varied from 5 wt% pitch binder, to over 25wt% or 5: 100 to more than 25: 100. Different torque zones were observed based on the level of granulation occurring during the mixing. Residence times of the mixed material were roughly 60 seconds. Agglomerated particles discharge from the end of the kneader were in the range of 50pm to 500pm.

[0128] The agglomerated particles then treated through a calcination thermal process in a rotary kiln to remove volatile content and harden the binder. The rotary kiln subjected the particles to mechanical and thermal agitation to change the size of the granules. Calcination occurred around 1 100°C from 0.5 to 5.0 hours. The calcination crystalized the carbon and removed volatile carbon compounds and low boiling point impurities. The resulting secondary' particles that were reduced in size in rotary calcination were cooled below oxidation temperature before discharge.

[0129] After calcination, the particles are passed into a continuously classifying grinding mill for final sizing. This removed any particles that are below the required size, and also reduced the size of any oversized particles that may have remained. Oversized particles were further doyvnsized and separated for recycle. The classifier speed and airflow may be adjusted depending on the powder properties to achieve target size. The resulting granules that have passed through sizing, with a target D50 size after sizing of 12-17pm, and a normal size distribution.

[0130] The resulting particles were directly fed into a continuous powder flow graphitization process. In this process, temperatures greater than 2800°C were utilized to convert the soft-carbon species to atomically re-arrange into a graphitic structure.Residence times were controlled from 1 to 30 hours, with a typical 10 hour time sufficient to grow graphite layers with proper order for high lithium ion intercalation potential.Example 2

[0131] Preparation: Two loss -in- weight hoppers, previously calibrated, were loaded with materials. One with petroleum needle coke, micronized to a D50 between 5 and 10pm, and the other with granular isotropic petroleum pitch, with a D50 size of ~3000pm, that is generally granular with a wide particle size distribution having a top size of 1 cm. These feeders fed directly into a shoot dropping into the entry port of continuous mixer. The continuous reciprocal mixer had a 60 mm diameter and a 28: 1 L:D ratio. Indicating the length is 28 times larger than the diameter. This system utilized a 75 HP motor with a 300 RPM maximum. Heating / cooling zones were located down the length with 14 in total across 7 temperature zones. The elements were configured with expansion and contracting zones, and consistent heat was applied through the shaft. The first heating zone was ~50°C cooler than the rest, to allow a longer conveyance zone before melting occurred. The zones were set from 280 to 350°C through the testing.

[0132] High shear internal elements were utilized at the inlet of the reciprocal kneader. This results in close clearance between the pins and kneading elements, typically of < 1mm during each of the tri-strokes per rotation. This section can break friable coke quickly into much smaller pieces, before full heating and melting begins. The configuration was such that clearances would alternate from <lmm to ~4mm and up 10mm, down the length of the kneader before the final discharge chute.

[0133] Other parameters were the same as in Example 1, and the material was finished in the same manner as Example 1 for final graphitization.Example 3

[0134] Preparation: One loss weight hopper, previously calibrated, was loaded with petroleum needle coke, micronized to a D50 between 5 and 10pm. A recirculating liquid pump and heated vessel was loaded with a lignin agglomeration solution. The powder w as fed directly into a chute dropping into the entry port of continuous mixer.

[0135] The liquid was injected into the kneader, at least 15 cm further up the kneader than the powder feed. The solution was injected into one, or several areas, along the length of the kneader. Solution feed was closely controlled in order to prevent clogging from a high liquid to pow der ratio.

[0136] The continuous reciprocal mixer had a 60 mm diameter and a 28: 1 L:D ratio, indicating the length is 28 times larger than the diameter. The system utilized a 75HP motor with a 300 rpm maximum. Heating / cooling zones are located down the length with 14 in total across 7 temperature zones. The elements were configured with expansion and contracting zones, and consistent heat was applied through the shaft. The zones were set from 140 to 200°C through the testing. The lignin solution was heated to 80°C during mixing, with insulated lines into the kneader. The kneader was operated at 120 rpm with a feed rate of 75 pounds or 34 kilograms per hour total. The binder was fed at 5 to 15% by mass. Pump mass flow curves were calibrated before and during the trial for control.

[0137] Other parameters were the same as in Example 1, and the material was finished in the same manner as Example 1 for final graphitization.Additional Embodiments

[0138] It should be appreciated that all combinations of the foregoing concepts and additional concepts discussed in greater detail below (provided such concepts are not mutually inconsistent) are contemplated as being part of the inventive subject matter disclosed herein. In particular, all combinations of claimed subject matter appearing at the end of this disclosure are contemplated as being part of the inventive subject matter disclosed herein. It should also be appreciated that terminology explicitly employed herein that also may appear in any disclosure incorporated by reference should be accorded a meaning most consistent with the particular concepts disclosed herein.

[0139] Reference throughout the specification to “one example’; “another example”, “an example”, and so forth, means that a particular element (e.g., feature, structure, and / or characteristic) described in connection with the example is included in at least one example described herein, and may or may not be present in other examples. In addition, it is to be understood that the described elements for any example may be combined in any suitable manner in the various examples unless the context clearly dictates otherwise.

[0140] It is to be understood that the ranges provided herein include the stated range and any value or sub-range within the stated range, as if such value or sub-range were explicitly recited. For example, a range from about 2 nm to about 20 nm should be interpreted to include not only the explicitly recited limits of from about 2 nm to about 20 nm, but also to include individual values, such as about 3.5 nm, about 8 nm, about 18.2 nm, etc., and sub-ranges, such as from about 5 nm to about 10 nm, etc. Furthermore, when “about” and / or “substantially” are / is utilized to describe a value, this is meant to encompass minor variations (up to + / - 10%) from the stated value.

[0141] While several examples have been described in detail, it is to be understood that the disclosed examples may be modified. Therefore, the foregoing description is to be considered non-limiting.

[0142] While certain examples have been described, these examples have been presented by way of example only, and are not intended to limit the scope of the disclosure. Indeed, the novel methods and systems described herein may be embodied in a variety’ of other forms. Furthermore, various omissions, substitutions and changes in the systems and methods described herein may be made without departing from the spirit of the disclosure. The accompanying claims and their equivalents are intended to cover such forms or modifications as would fall within the scope and spirit of the disclosure.

[0143] Features, materials, characteristics, or groups described in conjunction with a particular aspect, or example are to be understood to be applicable to any other aspect or example described in this section or elsewhere in this specification unless incompatible therewith. All of the features disclosed in this specification (including any accompanying claims, abstract and drawings), and / or all of the steps of any method or process so disclosed, may be combined in any combination, except combinations where at least some of such features and / or steps are mutually exclusive. The protection is not restricted to the details of any foregoing examples. The protection extends to any novel one, or any novel combination, of the features disclosed in this specification (including any accompanying claims, abstract and drawings), or to any novel one, or any novel combination, of the steps of any method or process so disclosed.

[0144] Furthermore, certain features that are described in this disclosure in the context of separate implementations can also be implemented in combination in a single implementation. Conversely, various features that are described in the context of a single implementation can also be implemented in multiple implementations separately or in any suitable sub-combination. Moreover, although features may be described above as acting in certain combinations, one or more features from a claimed combination can, in some cases, be excised from the combination, and the combination may be claimed as a subcombination or variation of a sub-combination.

[0145] Moreover, while operations may be depicted in the drawings or described in the specification in a particular order, such operations need not be performed in the particular order shown or in sequential order, or that all operations be performed, to achieve desirable results, unless provided otherwise herein. Other operations that are not depicted or described can be incorporated in the example methods and processes. Forexample, one or more additional operations can be performed before, after, simultaneously, or between any of the described operations. Further, the operations may be rearranged or reordered in other implementations. Those skilled in the art will appreciate that in some examples, the actual steps taken in the processes illustrated and / or disclosed may differ from those shown in the figures. Depending on the example, certain of the steps described above may be removed or others may be added. Furthermore, the features and attributes of the specific examples disclosed above may be combined in different ways to form additional examples, all of which fall within the scope of the present disclosure.

[0146] For purposes of this disclosure, certain aspects, advantages, and novel features are described herein. Not necessarily all such advantages may be achieved in accordance with any particular example. Thus, for example, those skilled in the art will recognize that the disclosure may be embodied or carried out in a manner that achieves one advantage or a group of advantages as taught herein without necessarily achieving other advantages as may be taught or suggested herein.

[0147] Conditional language, such as "can." “could / ’ “might,” or “may,” unless specifically stated otherwise, or otherwise understood within the context as used, is generally intended to convey that certain examples include, while other examples do not include, certain features, elements, and / or steps. Thus, such conditional language is not generally intended to imply that features, elements, and / or steps are in any way required for one or more examples.

[0148] Conjunctive language such as the phrase “at least one of X, Y, and Z,” unless specifically stated otherwise, is otherwise understood with the context as used in general to convey that an item, term, etc. may be either X, Y, or Z. Thus, such conjunctive language is not generally intended to imply that certain examples require the presence of at least one of X, at least one of Y, and at least one of Z.

[0149] Language of degree used herein, such as the terms “approximately,” “about,” “generally,” and “substantially” represent a value, amount, or characteristic close to the stated value, amount, or characteristic that still performs a desired function or achieves a desired result.

[0150] The scope of the present disclosure is not intended to be limited by the specific disclosures of preferred examples in this section or elsewhere in this specification and may be defined by claims as presented in this section or elsewhere in this specification or as presented in the future. The language of the claims is to be interpreted broadly based on the language employed in the claims and not limited to the examples described in thepresent specification or during the prosecution of the application, which examples are to be construed as non-exclusive.

[0151] Although the foregoing invention has been described in terms of certain preferred embodiments, other embodiments will be apparent to those of ordinary skill in the art. Additionally, other combinations, omissions, substitutions, and modifications will be apparent to the skilled artisan, in view of the disclosure herein. Accordingly, the present invention is not intended to be limited by the recitation of the preferred embodiments but is instead to be defined by reference to the appended claims.

[0152] The terminology7used in the description presented herein is not intended to be interpreted in any limited or restrictive manner and unless otherwise indicated refers to the ordinary meaning as would be understood by one of ordinary skill in the art in view of the specification. Furthermore, embodiments may comprise, consist of, consist essentially of, several novel features, no single one of which is solely responsible for its desirable attributes or is believed to be essential to practicing the embodiments herein described. As used herein, the section headings are for organizational purposes only and are not to be construed as limiting the described subject matter in any way. When definitions of terms in incorporated references appear to differ from the definitions provided in the present teachings, the definition provided in the present teachings shall control. It will be appreciated that there is an implied “about” prior to the temperatures, concentrations, times, etc. discussed in the present teachings, such that slight and insubstantial deviations are within the scope of the present teachings herein unless provided otherwise herein.

[0153] Although this disclosure is in the context of certain embodiments and examples, those of ordinary skill in the art will understand that the present disclosure extends beyond the specifically disclosed embodiments to other alternative embodiments and / or uses of the embodiments and obvious modifications and equivalents thereof. In addition, while several variations of the embodiments have been shown and described in detail, other modifications, which are within the scope of this disclosure, will be readily apparent to those of ordinary skill in the art based upon this disclosure. It is also contemplated that various combinations or sub-combinations of the specific features and aspects of the embodiments may be made and still fall within the scope of the disclosure. It should be understood that various features and aspects of the disclosed embodiments can be combined with, or substituted for, one another in order to form varying modes or embodiments of the disclosure. Thus, it is intended that the scope of the present disclosureherein disclosed should not be limited by the particular disclosed embodiments described above.

Claims

WHAT IS CLAIMED IS:

1. A method for continuously synthesizing agglomerated secondary7particles, the method comprising: providing a continuous kneader having a first end and a second end; providing primary7particles comprising a graphitizable material into the first end of the continuous kneader; providing an agglomeration solution into the first end of the continuous kneader; and mixing the primary7particles and the agglomeration solution as they are conveyed along a length of the continuous kneader from the first end to the second end to produce the agglomerated secondary7particles; wherein internal temperature along the length of the continuous kneader is maintained at a temperature below about 500°C.

2. The method of Claim 1, wherein the agglomeration solution is an aqueous agglomeration solution that comprises non-graphitizable lignin, sugar, or plant-derived carbohydrate molecules.

3. The method of Claims 1 or 2, wherein the continuous kneader is a single barrel, tri-stroke continuous kneader.

4. The method of any one of Claims 1-3, wherein internal temperature along the length of the continuous kneader is maintained at a temperature below about 300°C.

5. The method of any one of Claims 1-4, wherein internal temperature along the length of the continuous kneader is maintained within about 50°C of the softening point of the agglomeration solution.

6. The method of any one of Claims 1-5, wherein a length to diameter ratio of a mixing shaft of the continuous kneader is greater than about 10: 1.

7. The method of any one of Claims 1-6, wherein the primary particles have a bi- modal particle size distribution with a first set of primary particles having a D50 greater than 5pm but less than about 20pm and a second set of primary particles with a D50 less than about 5 pm.

8. The method of any one of Claims 1-7, wherein the primary7particles comprise graphitizable soft carbon particles having a D50 less than about 100pm.

9. The method of any one of Claims 1 -8, wherein the primary particles are selected from a group consisting of micronized petroleum coke powder, polyvinyl chloride, mesophase pitch, pitch coke, and coal coke; wherein the primary particles have a Dso less than about 20pm.

10. The method of any one of Claims 1 -9, wherein the agglomeration solution comprises between about 5 wt% and about 15 wt% of the total feed mass conveyed along the length of the continuous kneader.

11. The method of any one of Claims 1-10, wherein the agglomerated secondary7particles have a Dso between about 50 pm and about 500 pm.

12. The method of any one of Claims 1-10, wherein the agglomerated secondary particles have a Dso greater than about 1 mm and the method additional comprises milling the agglomerated secondary particles to size control the secondary particles to between about 10-30 pm.

13. The method of any one of Claims 1-12, wherein at least one of the primary particles and the agglomeration solution are heated before being provided into the first end of the continuous kneader.

14. The method of any one of Claims 1-13, further comprising removing the agglomerated secondary particles from the second end of the continuous kneader and calcining the agglomerated secondary particles in a rotary kiln at a temperature between about 800 and about 1350°C to produce calcined secondary particles.

15. The method of Claim 14, further comprising passing the calcined secondary particles into a continuously classifying grinding mill and reducing the Dso of the calcined particles to less than about 30 pm.

16. The method of Claim 15, further comprising graphitizing the calcined particles at temperatures greater than about 2500°C after reducing the Dso of the calcined particles to produce a graphitized anode material.

17. Agglomerated secondary particles produced according to the process of Claim 1.

18. The agglomerated secondary particles of Claim 17, wherein the secondary particles are comprised of at least 2 to about 100 primary particles agglomerated together.

19. The agglomerated secondary particles of Claim 17, wherein the agglomerated secondary particles have a D50 greater than about 300 pm.

20. A method for continuously producing agglomerated secondary particles, the method comprising: providing a continuous kneader having a first end and a second end; providing primary particles comprised of graphitizable carbons into an inlet between the first end and the second end of the continuous kneader; providing an agglomeration binder into one or more inlets between the first end and the second end of the continuous kneader; and conveying the primary particles and the agglomeration binder through one or more high shear sections followed by one or more low shear sections along a length of the continuous kneader to produce the agglomerated secondary particles.

21. The method of Claim 20, wherein the one or more high shear sections have a shear gap of less than about 4 mm and the one or more low shear sections have a shear gap of more than about 4 mm.

22. The method of Claims 20 or 21. wherein the agglomeration binder has a D50 greater than about 2000 pm and is selected from a group consisting of plant based polymer, petroleum pitch, and coal tar pitch.

23. The method of any one of Claims 20-22, wherein the continuous kneader is a tri-stroke continuous kneader.

24. The method of any one of Claims 20-22. wherein the continuous kneader is configured such that a shear gap is adjustable in the one or more high shear sections and the one or more low shear sections.

25. The method of any one of Claims 20-24, wherein the agglomeration binder is micronized high temperature petroleum pitch with a particle size D50 between about 2 pm and 5 pm and wherein the primary particles have a bi-modal particle size distribution.

26. The method of any one of Claims 20-25, wherein the agglomeration binder has a softening point above about 100 degrees Celsius.

27. A method for continuously producing size-controlled secondary particles, the method comprising: providing a continuous kneader having a first end and a second end;providing a plurality of flights connected to a central rotating rod within the continuous kneader; providing one or more stationary kneading bolts along an interior wall of the continuous kneader; providing primary particles comprising a graphitizable material into the first end of the continuous kneader; providing an agglomeration solution containing binder molecules into the first end of the continuous kneader; and mixing the primary' particles and the agglomeration solution as they are conveyed along a length of the continuous kneader from the first end to the second end to produce the secondary’ particles having a D50 exceeding about 300 pm; wherein internal temperature along the length of the continuous kneader is maintained at a temperature below about 500°C.

28. The method of Claim 27, additionally comprising milling the agglomerated secondary' particles in a rotary kiln to reduce a size of the agglomerated secondary particles to a D50 below about 200 pm.

29. The method of Claims 27-28, wherein the agglomerated secondary particles have a binder to particle mass ratio of about 5:100 to about 20: 100.

30. The method of Claims 27-29, wherein a shear gap between the plurality of flights and the one or more stationary’ kneading bolts varies along the length of the continuous kneader.

31. The method of Claims 27-30, additionally comprising discharging a mixture of primary' particles and the agglomeration solution at the second end of the continuous kneader, wherein the ratio of secondary particles to primary particles is at least 100: 1.

32. A battery containing the graphitized anode material made by the method ofClaim 16.

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