Electrochemical slurries in semi-solid electrodes and methods of preparing the same

Abstract

Embodiments described herein relate generally to semi-solid slurries made with a mechanically compacted powder, and more particularly methods for preparing semi-solid slurries with a higher solid ratio (e.g., greater than 50% by volume of the slurry) which enables more stable production of batteries with high energy density. Described herein is a method for fabricating a semi-solid electrode and an electrode material. The method involves blending an active material with a conductive material to form an intermediate material, which is then compacted to form a compacted material. This compacted material is subsequently mixed with an electrolyte to form a semi-solid slurry. In some embodiments, the compacted material includes a plurality of agglomerates formed from the electrochemically active material. The method further includes applying the semi-solid slurry onto a current collector material to form a semi-solid electrode.

Description

ELECTROCHEMICAL SLURRIES IN SEMI-SOLID ELECTRODESAND METHODS OF PREPARING THE SAMECross-Reference to Related Applications

[0001] This application claims priority to and the benefit of U.S. Provisional Patent Application No. 63 / 675,708, filed 07 / 25 / 2024, and entitled, “Electrochemical Slurries in SemiSolid Electrodes and Methods of Preparing the Same”, the entire disclosure of which is hereby incorporated by reference herein.Technical Field

[0002] Embodiments described herein relate generally to semi-solid electrode slurries, and methods of producing the same.Background

[0003] Batteries often include solid electrodes, separators, electrolytes, and additional components like packaging, thermal management systems, cell balancing mechanisms, and terminals for electrical current carriers. The electrodes often contain active materials, conductive additives, binders, and other substances.

[0004] Traditional methods for manufacturing batteries involve coating a metallic substrate, such as a current collector, with a slurry made from electrochemically active materials, conductive additives, and binders dissolved in a solvent. This slurry is then dried to evaporate the solvent, and the resulting solid matrix is calendered to a specific thickness. The electrodes are cut, assembled with other components, infused with electrolyte, and the entire assembly is sealed.

[0005] These conventional methods often involve complex and costly manufacturing steps, limiting the potential thicknesses of electrodes produced therefrom. This limitation results in batteries with lower capacity, reduced energy density, and a higher proportion of inactive components to active materials. Additionally, the binders used in traditional electrode formulations can increase tortuosity and decrease the ionic conductivity of the electrode.

[0006] Semi-solid electrodes present a superior battery format as they eliminate the need for a solvent drying process and are cost-effective. However, direct formation of electrodesfrom a semi-solid slurry containing electrolyte and active materials is also limited for increasing the active material ratio due to the stiffness of the slurry. Slurries with higher active material ratios (e.g., greater than 50% by volume of the slurry) are challenging to form because they become too stiff to process effectively.

[0007] Existing technologies have proposed methods to control the stiffness of the slurry by adjusting the amount of conductive additives and mixing conditions. Nevertheless, these approaches do not achieve a sufficiently high active material ratio. Other techniques include increasing the active material ratio by using a softer slurry that can be shaped into an electrode and then mechanically pressing it to redistribute the electrolyte within the electrode. However, these methods face difficulties in controlling the electrolyte redistribution process and effectively utilizing the moved electrolyte.

[0008] Therefore, there is a continuous goal in the development of energy storage systems to simplify manufacturing processes, reduce costs, minimize inactive components in electrodes and finished batteries, and enhance performance.Summary

[0009] Embodiments described herein relate to semi-solid slurries made from a compacted mixture of an active material and a conductive material, and methods for their preparation. The methods described herein enable the production of processable, for example castable, semisolid slurries having a high active material ratio (e.g., greater than 50% by volume of the slurry), thereby resulting in the fabrication of batteries with high energy density (e.g., an electrochemical cell with a cell specific energy density of at least about 250 Wh / kg when discharged at 1C).

[0010] In some aspects, a method includes blending an active material with a conductive material to form an intermediate material, and compacting the intermediate material to form a compacted electrode material. The method further includes mixing the compacted electrode material with an electrolyte to form a semi-solid slurry. The method may further include disposing the semi-solid slurry onto a current collector to form a semi-solid electrode. In some embodiments, the compacting includes passing the intermediate material between a first roller and a second roller separated by a distance, the first roller and the second roller exerting a predetermined pressure onto the intermediate material to form the compacted material.

[0011] In some embodiments, a compacted electrode material includes an electrochemically active material, a portion of which is formed into a plurality of agglomerates, and a conductive material, the conductive material being disposed on and between the plurality of agglomerates. In some embodiments, each of the plurality of agglomerates have a longest dimension of about 10 pm or more. In some embodiments, the compacted electrode material is formed by compacting electrochemically active material and the conductive material.

[0012] In some embodiments, a semi-solid slurry composition includes the electrode compacted material, and about 20% to about 50% by volume of an electrolyte.Brief Description of the Drawings|0013[ FIG. 1 is a schematic illustration of a semi-solid slurry, according to various embodiments.

[0014] FIG. 2 is a flow diagram of a method of forming a semi-solid electrode, according to various embodiments.

[0015] FIG. 3 A shows a picture of a roller press machine, according to various embodiments. FIG. 3B shows a schematic illustration of a roller press machine, according to various embodiments. FIG. 3C shows a picture of a compacted electrode material, according to various embodiments.

[0016] FIGS. 4A-4D show scanning electron microscopy (SEM) images of a comparative uncompacted electrode material and a compacted electrode material subjected to different compacting methods, according to various embodiments.10017 [ FIG. 5 is a plot showing bulk and tap densities (grams per cubic centimeter (g / cc)) of a comparative uncompacted electrode material and a compacted electrode material subjected to different compacting methods, according to various embodiments.

[0018] FIG. 6A shows a plot of conductivity (S / cm) vs. volume fraction of a comparative uncompacted electrode material and a compacted electrode material subjected to different compacting methods, according to various embodiments. FIG. 6B shows a plot of applied force (kN) vs. volume fraction of a comparative uncompacted electrode material and a compacted material subjected to different compacting methods, according to various embodiments.

[0019] FIG. 7 shows an X-ray diffraction (XRD) patterns of a comparative uncompacted electrode material and a compacted electrode material subjected to a compacting method, according to various embodiments.

[0020] FIGS. 8A-8D are photographs of different semi-solid slurry compositions including a comparative uncompacted electrode material and a compacted electrode material subjected to different compacting methods, according to various embodiments.

[0021] FIGS. 9A-9D are photographs of different semi-solid slurry compositions including a comparative uncompacted electrode material with various amounts of electrochemically active material, according to various embodiments.[00221 FIGS. 10A-10D are photographs of different semi-solid slurry compositions including a compacted electrode material with various amounts of electrochemically active material, according to various embodiments.

[0023] FIGS. 11A-11D are photographs of different semi-solid slurry compositions including a compacted electrode material with various amounts of electrochemically active material, according to various embodiments.

[0024] FIG. 12A is a plot showing conductivities (mS / cm) of different semi-solid slurry compositions including a comparative uncompacted electrode material and a compacted electrode material subjected to different compacting methods, according to various embodiments. FIG. 12B is a plot showing yield stresses (kPa) of different semi-solid slurry compositions including a comparative uncompacted electrode material and a compacted electrode material subjected to different compacting methods, according to various embodiments.

[0025] FIG. 13 is a plot showing the effect of compacting methods on average yield stress (kPa) of various semi-solid slurries compositions with different amounts of solid loadings, according to various embodiments.

[0026] FIG. 14 shows a plot of voltage (V) vs. normalized capacity (%) of electrochemical cells made from using a comparative uncompacted electrode material and a compacted electrode material subjected to different compacting methods, according to various embodiments.Detailed Description

[0027] Embodiments described herein relate to semi-solid suspensions (also referred to herein as a “semi-solid slurry”) and a method of preparing the same. The method includes mechanically compacting a blend of an electrochemically active material (also referred to herein as a “active material”) and a conductive material, and then mixing the compacted blend with an electrolyte to form a semi-solid slurry. The mechanical compaction of the active material and conductive additives creates a densified powder that, when made into a slurry, retains its softness. This allows for more stable and efficient battery production, ensuring consistent performance and quality in the final product. In some embodiments, the electrolyte can include a liquid electrolyte.

[0028] Embodiments described herein relate generally to semi-solid electrode slurries, and more particularly to methods for preparing semi-solid slurries for use as electrodes in electrochemical devices such as, for example, batteries. The semi-solid slurries described herein are made from mechanically compacted mixtures of electrochemically active materials and conductive materials.

[0029] Electrochemical devices (e.g., batteries) can be manufactured directly with the semi-solid suspension, thereby avoiding the use of conventional binding agents and the electrode casting step altogether. Some benefits of this approach include, for example: (i) simplified manufacturing with less equipment (i.e., less capital intensive), (ii) the ability to manufacture electrodes of different thicknesses (e.g., by simply changing an extrusion die slot dimension), (iii) processing of thicker (>100 pm) and higher capacity (mAh / cm2) electrodes, thereby decreasing the volume, mass, and cost contributions of inactive components with respect to active material, and (iv) the elimination of binding agents, thereby reducing tortuosity and increasing ionic conductivity of the electrode. Examples of battery architectures utilizing semi-solid suspensions are described in International Patent Publication No. WO 2012 / 024499, entitled “Stationary, Fluid Redox Electrode,” and International Patent Application No. PCT / US11 / 66902, entitled “Semi-Solid Filled Battery and Method of Manufacture,” the disclosures of which are incorporated herein by reference in their entirety.{0030] The semi-solid slurries provided herein are for use in electrodes of electrochemical devices. This disclosure generally describes electrochemical devices such as, for example, lithium ion batteries, however, the compositions, methods and principles described herein are applicable to all devices containing electrochemically active media. Said another way, anyelectrodes and / or devices including at least an active material (source or sink of charge carriers), an electronically conducting additive, and an ionically conducting media (electrolyte) such as, for example, batteries, capacitors, electric double-layer capacitors (e.g., ultracapacitors), pseudo-capacitors, etc., are within the scope of this disclosure.[00311 Consumer electronic batteries have gradually increased in energy density with the progress of lithium-ion battery technology. The stored energy or charge capacity of a manufactured battery is a function of: (1) the inherent charge capacity of the active material (mAh / g), (2) the volume of the electrodes (cm3) (i.e., the product of the electrode thickness, electrode area, and number of layers (stacks)), and (3) the loading of active material in the electrode media (e.g., grams of active material per cm3of electrode media). Therefore, to enhance commercial appeal (e.g., increased energy density and decreased cost), it is generally desirable to increase the areal charge capacity (mAh / cm2) also referred to as “area specific capacity” or “area capacity” herein. The areal charge capacity can be increased, for example, by utilizing active materials that have a higher inherent charge capacity, increasing relative percentage of active charge storing material (i.e., “loading”) in the overall electrode formulation, and / or increasing the relative percentage of electrode material used in any given battery form factor. Said another way, increasing the ratio of active charge storing components (e.g., the electrodes) to inactive components (e.g., the separators and current collectors), increases the overall energy density of the battery by eliminating or reducing components that are not contributing to the overall performance of the battery. One way to increase the areal charge capacity (and reduce the relative percentage of inactive components) is by increasing the amount of active material in the semi-solid slurries. However, forming electrodes directly from a semi-solid slurry that includes electrolyte and active materials encounters challenges when attempting to increase the active material ratio. The stiffness of the slurry restricts the ability to achieve higher ratios of active material (e.g., exceeding 50% by volume of the slurry), making it difficult to process and cast effectively.10032] The semi-solid slurries described herein enable the loading of a larger amount of active material. Compared to semi-solid slurries made from an uncompacted blend of active and conductive materials, the semi-solid slurries obtained according to various embodiments described herein exhibit lower yield stress. This property makes them advantageous for casting, as they maintain softness and ease of processing despite having a high active material ratio (e.g., exceeding 50%), which enhances energy density.

[0033] Some embodiments described herein relate to a semi-solid slurry with greater than about 50%, greater than about 55%, or greater than about 60%, active material by volume. Additionally, in some embodiments, a sufficient quantity of a conductive additive (e.g., carbon black, KETJEN BLACK® carbon particles) can be added to the slurry to improve electrical conductivity and electrochemical performance of the electrode. Furthermore, some embodiments described herein relate to a castable, processable, repeatable, scalable, manufacturing-oriented formulation process.

[0034] As used herein, the term “semi-solid” refers to a material that is a mixture of liquid and solid phases, for example, such as particle suspension, colloidal suspension, emulsion, gel, or micelle.

[0035] As used herein, the term “area specific capacity”, “area capacity”, or “areal capacity” are used interchangeably to define the charge capacity of an electrode or an electrochemical cell per unit area having units of mAh / cm2.

[0036] Exemplary active materials for the positive electrode in a lithium system include the general family of ordered rocksalt compounds LiMCh including those having the a-NaFeCh (so-called “layered compounds”) or orthorhombic-LiMnCh structure type or their derivatives of different crystal symmetry, atomic ordering, or partial substitution for the metals or oxygen. M comprises at least one first-row transition metal but may include non-transition metals including but not limited to Al, Ca, Mg, or Zr. Examples of such compounds include LiCoCh, LiCoCh doped with Mg, LiNiCh, Li(Ni, Co, A1)C>2 (known as “NCA”) and Li(Ni, Mn, Co)Ch (known as “NMC”). Other families of exemplary electroactive materials includes those of spinel structure, such as LiMn2O4 and its derivatives, so-called “layered spinel nanocomposites” in which the structure includes nanoscopic regions having ordered rocksalt and spinel ordering, olivines LiMPO4 and their derivatives, in which M comprises one or more of Mn, Fe, Co, or Ni, partially fluorinated compounds such as LiVPO4F, other “polyanion” compounds as described below, and vanadium oxides VxOy including V2O5 and VeOn.

[0037] In one or more embodiments the active material includes a transition metal polyanion compound, for example as described in U.S. Patent No. 7,338,734, incorporated by reference herein in its entirety. In one or more embodiments the active material includes an alkali metal transition metal oxide or phosphate, and for example, the compound has a composition Ax(M'i-aM"a)y(XD4)z, Ax(M'i-aM"a)y(DXD4)z, or Ax(M'i-aM"a)y(X2D7)z, and have values such that x, plus y(l-a) times a formal valence or valences of M', plus ya times a formalvalence or valence of M", is equal to z times a formal valence of the XD4, X2D7, or DXD4 group; or a compound including a composition (Ai-aM"a)xM'y(XD4)z, (Ai- aM"a)xM'y(DXD4)z(Ai-aM"a)xM'y(X2D7)z and have values such that (l-a)x plus the quantity ax times the formal valence or valences of M" plus y times the formal valence or valences of M' is equal to z times the formal valence of the XD4, X2D7 or DXD4 group. In the compound, A is at least one of an alkali metal and hydrogen, M' is a first-row transition metal, X is at least one of phosphorus, sulfur, arsenic, molybdenum, and tungsten, M" any of a Group IIA, IIIA, IVA, VA, VIA, VIIA, VIIIA, IB, IIB, IIIB, IVB, VB, and VIB metal, D is at least one of oxygen, nitrogen, carbon, or a halogen. The positive electroactive material can be an olivine structure compound LiMPCh, where M is one or more of V, Cr, Mn, Fe, Co, and Ni, in which the compound is optionally doped at the Li, M or O-sites. Deficiencies at the Li-site are compensated by the addition of a metal or metalloid, and deficiencies at the O-site are compensated by the addition of a halogen. In some embodiments, the positive active material includes a thermally stable, transition-metal-doped lithium transition metal phosphate having the olivine structure and having the formula (Lii-xzx)MPC>4, where M is one or more of V, Cr, Mn, Fe, Co, and Ni, and Z is a non-alkali metal dopant such as one or more of Ti, Zr, Nb, Al, or Mg, and x ranges from 0.005 to 0.05.

[0038] In some embodiments, the lithium transition metal phosphate material has an overall composition of Li-x-zMi+zPCh, where M comprises at least one first row transition metal selected from the group consisting of Ti, V, Cr, Mn, Fe, Co and Ni, where x is from 0 to 1 and z can be positive or negative. M includes Fe, z is between about 0.15 and -0.15. The material can exhibit a solid solution over a composition range of 0<x<0.15, or the material can exhibit a stable solid solution over a composition range of x between 0 and at least about 0.05, or the material can exhibit a stable solid solution over a composition range of x between 0 and at least about 0.07 at room temperature (22-25 °C). The material may also exhibit a solid solution in the lithium-poor regime, e.g., where x > 0.8, or x > 0.9, or x > 0.95.

[0039] In some embodiments the redox-active electrode material includes a metal salt that stores an alkali ion by undergoing a displacement or conversion reaction. Examples of such compounds include metal oxides such as CoO, CO3O4, NiO, CuO, MnO, typically used as a negative electrode in a lithium battery, which upon reaction with Li undergo a displacement or conversion reaction to form a mixture of Li2O and the metal constituent in the form of a more reduced oxide or the metallic form. Other examples include metal fluorides such as 1F2, FeF2, FeFs, BiFs, C0F2, and NiF2, which undergo a displacement or conversion reaction to form LiFand the reduced metal constituent. Such fluorides may be used as the positive electrode in a lithium battery. In other embodiments the redox-active electrode material includes carbon monofluoride or its derivatives. In some embodiments the material undergoing displacement or conversion reaction is in the form of particulates having on average dimensions of 100 nanometers or less. In some embodiments the material undergoing displacement or conversion reaction comprises a nanocomposite of the active material mixed with an inactive host.

[0040] In some embodiments, slurry components can be mixed in a batch process (e.g., with a batch mixer), with a specific spatial and / or temporal ordering of component addition, as described in more detail herein. In some embodiments, slurry components can be mixed in a continuous process (e.g. in an extruder), with a specific spatial and / or temporal ordering of component addition.

[0041] In some embodiments, process conditions (temperature; shear rate or rate schedule; component addition sequencing, location, and rate; mixing or residence time; or any combination thereof) can be selected and / or modified to control the electrical, rheological, and / or compositional (e.g., uniformity) properties of the prepared slurry. For example, the process conditions can be selected to produce a prepared slurry having a mixing index of at least about 0.80, at least about 0.90, at least about 0.95, or at least about 0.975.

[0042] FIG. 1 is a schematic diagram of a semi-solid slurry 100 including a compacted electrode material suspended in an electrolyte, according to an embodiment. The compacted electrode material includes an active material 110 and a conductive material 120. A portion of the active material is formed into a plurality of agglomerates 130. The conductive material 120 is disposed on and between the plurality of agglomerates as shown in FIG. 1.

[0043] In some embodiments, the compacted electrode material can be obtained via compacting a blend of the active material 110 and the conductive material 120 using roller press equipment. In some embodiments, the compacted electrode material can be obtained via compacting a blend of the active material 110 and the conductive material 120 using at least one of a die press or a cold isostatic press machine. Any compaction technique that yields a densified powder blend of the active material 110 and the conductive material 120 can be used.

[0044] In some embodiments, the portion of the active material 110 that is formed into of the plurality of agglomerates 130 (i.e., the portion of the active material 110 that is not freely scattered away from the agglomerates 130) is at least at least about 30%, at least about 35%, at least about 40%, at least about 45%, at least about 50%, at least about 55%, at least about 60%,at least about 65%, at least about 70%, at least about 75%, or at least about 80% of the active material.

[0045] In some embodiments, the plurality of agglomerates 130 can have an average longest dimension of at least about 0.1 pm, at least about 0.5 pm, at least about 1 pm, at least about 5 pm, at least about 10 pm, at least about 30 pm, at least about 50 pm, at least about 60 pm, at least about 70 pm, at least about 80 pm, at least about 90 pm, at least about 100 pm, at least about 200 pm, at least about 300 pm, at least about 400 pm, or at least about 500 pm. In some embodiments, the plurality of agglomerates 130 can have an average longest dimension of no more than about 500 pm, no more than about 400 pm, no more than about 300 pm, no more than about 200 pm, no more than about 100 pm, no more than about 90 pm, no more than about 80 pm, no more than about 70 pm, no more than about 60 pm, no more than about 50 pm, no more than about 40 pm, no more than about 30 pm, no more than about 20 pm, no more than about 10 pm, no more than about 5 pm, no more than about 1 pm, no more than about 0.5 pm, or no more than about 0.1 pm. Combinations of the above-referenced dimensions are also possible (e.g., at least about 0.1 pm and no more than about 500 pm or at least about 10 pm and no more than about 100 pm), inclusive of all values and ranges therebetween. In some embodiments, the plurality of agglomerates 130 can have an average longest dimension of about 0.1 pm, about 0.5 pm, about 1 pm, about 5 pm, about 10 pm, about 30 pm, about 50 pm, about 60 pm, about 70 pm, about 80 pm, about 90 pm, about 100 pm, about 200 pm, about 300 pm, about 400 pm, or about 500 pm.

[0046] In some embodiments, the average longest dimension can be determined by intensity average particle size (Z average) as measured by dynamic light scattering. In some embodiments, the average longest dimension can be determined by a number reference particle size measured by dynamic light scattering. In embodiments, the average longest dimension can be determined by transmission electron microscopy.

[0047] The electrochemically active material 110 (referred herein as “an active material”) can be an ion storage material and or any other compound or ion complex that is capable of undergoing Faradaic reaction in order to store energy.

[0048] In some embodiments, the active material 110 can include at least one of silicon, tin, silicon alloys, tin alloys, aluminum, titanium oxide, lithium metal, carbon, lithium- intercalated carbon, lithium nitrides, lithium alloys and lithium alloy forming compounds of silicon, bismuth, boron, gallium, indium, zinc, tin, antimony, aluminum, titanium oxide,molybdenum, germanium, manganese, niobium, vanadium, tantalum, gold, platinum, iron, copper, chromium, nickel, cobalt, zirconium, yttrium, molybdenum oxide, germanium oxide, silicon oxide, or silicon carbide.

[0049] The active material 110 can be a cathode active material or an anode active material. In some embodiments, the anode active material can include graphite, lithium metal (Li), silicon, carbon, lithium-intercalated carbon, lithium nitrides, lithium alloys, lithium alloy forming compounds, or any other anode active material, inclusive of all combinations thereof. In some embodiments, the lithium alloy forming compounds can include silicon, bismuth, boron, gallium, indium, zinc, tin, antimony, aluminum, titanium oxide, molybdenum, germanium, manganese, niobium, vanadium, tantalum, gold, platinum, iron, copper, chromium, nickel, cobalt, zirconium, yttrium, molybdenum oxide, germanium oxide, silicon carbide, and / or silicon-graphite composite. In some embodiments, the cathode active material may include at least one of lithium cobalt oxide (LCO), lithium nickel manganese cobalt oxide (NMC), or lithium iron phosphate (LFP).

[0050] In some embodiments, the compacted electrode material can include between about 50% to about 90% by volume of the active material. In some embodiments, the compacted electrode material can include about 55% to about 90% by volume, about 60% to about 90% by volume, about 65% to about 90% by volume, about 70% to about 90% by volume, about 75% to about 90% by volume, or about 80% to about 90% by volume of the active material, inclusive of all ranges and values therebetween.

[0051] In some embodiments, the semi-solid slurry 100 can include between about 50% to about 80% by volume of active material. In some embodiments, the semi-solid slurry 100 can include at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, at least about 75%, or at least about 80% by volume of active material. In some embodiments, the semi-solid slurry 100 can include no more than about 80%, no more than about 75%, no more than about 70%, no more than about 65%, no more than about 60%, or no more than about 55% by volume of active material. Combinations of the above-referenced volume percentages of active material in the semi-solid slurry 100 are also possible (e.g., at least about 50% and no more than about 80% by volume or at least about 60% and no more than about 70% by volume), inclusive of all values and ranges therebetween. In some embodiments, the semi-solid slurry 100 can include about 50%, about 55%, about 60%, about 65%, about 70%, about 75%, or about 80% by volume of active material.

[0052] In some embodiments, the conductive material 120 can include graphite, activated carbon, conductive carbon, KETJENBLACK® carbon black particles, hard carbon, soft carbon, carbon nanotubes, carbon nanofibers, Nickel-Metal Hydride (NiMH), Nickel Cadmium (NiCd), lithium cobalt oxide, lithium iron phosphate (LFP), or any combination thereof. In some embodiments, the conductive material 120 can include at least one of a metal, a metal carbide, a metal nitride, a metal oxide, an allotrope of carbon, carbon black, graphitic carbon, carbon fibers, carbon microfibers, VGCF, fullerenic carbons, “buckyballs”, CNT’s, MWNT’s, SWNT’s, graphene sheets, aggregates of graphene sheets, materials comprising fullerenic fragments, electronically insulating organic redox compounds rendered electronically active by mixing or blending with an electronically conductive polymer, polyaniline based conductive polymers, polyacetylene based conductive polymers, poly(3,4- ethylenedioxythiophene) (PEDOT), polypyrrole, polythiophene, poly(p-phenylene), poly(triphenylene), polyazulene, polyfluorene, polynaphtalene, polyanthracene, polyfuran, polycarbazole, tetrathiafulvalene-substituted polystyrene, ferrocene-substituted polyethylene, carbazole-substituted polyethylene, polyoxyphenazine, polyacenes, and / or poly(heteroacenes). In some embodiments, the carbon additive can include KETJENBLACK® carbon black particles. In some embodiments, the carbon additive can include carbon nanofibers, CNT’s, SWNT’s, carbon black, and / or MWNT’s.

[0053] In some embodiments, the semi-solid slurry 100 can include between about 0.5% to about 40% by volume of conductive material 120. In some embodiments, the semi-solid slurry 100 can include at least about 0.1%, at least about 0.5%, at least about 1%, at least about 5%, at least about 10%, at least about 15%, at least about 20%, at least about 25%, at least about 30%, or at least about 35% by volume of conductive material 120. In some embodiments, the semi-solid slurry 100 can include no more than about 40%, no more than about 35%, no more than about 30%, no more than about 25%, no more than about 20%, no more than about 15%, no more than about 10%, no more than about 5%, or no more than about 0.5% by volume of conductive material 120. Combinations of the above-referenced volume percentages of conductive material 120 in the semi-solid slurry 100 are also possible (e.g., at least about 0.1% and no more than about 40% by volume or at least about 5% and no more than about 10% by volume), inclusive of all values and ranges therebetween. In some embodiments, the semi-solid slurry 100 can include about 0.5%, about 1%, about 5%, about 10%, about 15%, about 20%, about 25%, about 30%, about 35%, or about 40% by volume of conductive material 120.

[0054] In some embodiments, the semi-solid slurry 100 can include between about 30% to about 50% by volume of electrolyte. In some embodiments, the electrolyte can include a liquid electrolyte. In some embodiments, the electrolyte can include one or more electrolyte solutions. In some embodiments, the one or more electrolyte solutions can include ethylene carbonate (EC), dimethyl carbonate (DMC), gamma-butyrolactone (GBL), Lithium bis(fluorosulfonyl) imide (LiFSI), trioctyl phosphate (TOP), propylene carbonate (PC), dimethoxy ethane (DME), bis(trifluoromethanesulfonyl)imide (TSFI), Lii.4Alo.4Tii.6(P04)3 (LATP), lithium hexafluorophosphate (LiPF6), lithium bis(trifhroromethanesulfonyl)imide (LiTFSI), lithium borate (LiBOB), lithium carbonate (Li2CO3), any other suitable salt, and any combinations thereof. Additional examples of active materials, conductive materials, and electrolyte solutions that can be used to form the semi-solid slurries described herein are described in U.S. Patent No. 9,484,569, entitled, “Electrochemical Slurry Compositions and Methods of Preparing the Same,” (“the ‘569 patent”) and in U.S. Patent No. 9,437,864 entitled, “Asymmetric Battery Having a Semi-Solid Cathode and High Energy Density Anode,” registered September 6, 2016 (“the ‘864 patent), the disclosures of which are incorporated herein by reference in their entirety.

[0055] As used herein, the term “tapped density”, or “tap density” refers to the mass of the unit volume measured after the powder in the container is tapped under specific conditions. The tapped density is generally measured by mechanically tapping a container of powder particles to create a regular vibration, and this rearranges the powder particles. The measurement of tapped density is typically conducted using a tapped density tester. In some embodiments, tap density can be determined in accordance with ASTM B527-22.10056] As used herein, the term “true density” refers to an actual mass of a solid matter per unit volume of a material in an absolutely dense state, i.e., a density after removal of internal pores or voids between particles. That is, true density is the density of the material itself, excluding any pores or voids within or between the particles. Any appropriate gas or liquid displacement method can be employed to determine true density of a powder.10057] In some embodiments, a ratio of a tapped density to a true density of the compacted electrode material is at least about 0.2, at least about 0.3, at least about 0.4, or at least about 0.5. In some embodiments, a ratio of a tapped density to a true density of the compacted electrode material is no more than about 0.8, no more than about 0.7, no more than about 0.6, or no more than about 0.5. Combinations of the above-referenced values are also possible (e.g.,at least about 0.2 and no more than about 0.8 or at least about 0.4 and no more than about 0.7), inclusive of all values and ranges therebetween.

[0058] In some embodiments, it is desirable that semi-solid slurries 100 described herein be “workable” or “castable” in order to facilitate material handling associated with battery manufacturing. For example, if a slurry is too fluid it can be compositionally unstable meaning that homogeneity can be lost under exposure to certain forces, such as gravity (e.g., solids settling) or centrifugal forces. If the slurry is unstable, solid phase density differences, or other attributes, can give rise to separation and / or compositional gradients. In other words, if the slurry is overly fluidic, which may be the result of low solids loadings or a significantly disrupted conductive network, the solids may not be sufficiently bound in place to inhibit particle migration. Alternatively, if an electrochemically active slurry is too solid, the slurry may break up, crumble, and / or segregate into pieces, which can complicate processing and dimensional control. Formulating the slurry within a band of adequate workability can facilitate easier slurry-based battery manufacture. Workability of a slurry can typically be quantified using rheological parameters which can be measured using rheometers. Some examples of different types of rheometers that can be used to quantify slurry workability include strain or stress-controlled rotational, capillary, slit, and extensional rheometers.10059] The “workable” slurries with different solids loadings can be evaluated for flowability and processability. The rheological behavior of the slurries can indicate processability under pressure-driven flows, such as in a single or twin screw extrusion and / or flow through a die. The slurries can be categorized as “suspensions” with different loading levels and a low viscosity liquid medium / matrix. Such suspensions flow behavior can be dependent on size distribution, shape and volume fraction of solid particles, particle-particle and particle-matrix interactions, and matrix rheology. In some embodiments, slurries can be selected based on rheology, which can be used to predict favorable processability of the slurries and / or desired electrochemical performance. The rheology of the “workable” slurries can be governed by the compositional formulation, e.g., different active materials and conductive additives loaded at various concentrations and / or homogeneity of the slurries.

[0060] In some embodiments, the semi-solid slurry 100 can have a yield strength between about 2 kPa and about 150 kPa. In some embodiments, the semi-solid slurry composition can have a yield strength of at least about 2 kPa, at least about 5 kPa, at least about 10 kPa, at least about 15 kPa, at least about 20 kPa, at least about 25 kPa, at least about 30 kPa, at least about 35 kPa, at least about 40 kPa, at least about 45 kPa, at least about 50 kPa, at least about 55 kPa,at least about 60 kPa, at least about 65 kPa, at least about 70 kPa, at least about 75 kPa, at least about 80 kPa, at least about 85 kPa, at least about 90 kPa, at least about 95 kPa, at least about 100 kPa, at least about 105 kPa, at least about 110 kPa, at least about 115 kPa, at least about 120 kPa, at least about 125 kPa, at least about 130 kPa, at least about 135 kPa, or at least about 140 kPa. In some embodiments, the semi-solid slurry composition can have a yield strength of no more than about 150 kPa, no more than about 145 kPa, no more than about 140 kPa, no more than about 135 kPa, no more than about 130 kPa, no more than about 125 kPa, no more than about 120 kPa, no more than about 115 kPa, no more than about 110 kPa, no more than about 105 kPa, no more than about 100 kPa, no more than about 95 kPa, no more than about 90 kPa, no more than about 85 kPa, no more than about 80 kPa, no more than about 75 kPa, no more than about 70 kPa, no more than about 65 kPa, no more than about 60 kPa, no more than about 55 kPa, no more than about 50 kPa, no more than about 45 kPa, no more than about 40 kPa, no more than about 35 kPa, no more than about 30 kPa, no more than about 25 kPa, no more than about 20 kPa, no more than about 15 kPa, no more than about 10 kPa, no more than about 5 kPa, or no more than about 2 kPa. Combinations of the above-referenced yield strengths in the semi-solid slurry composition are also possible (e.g., at least about 2 kPa and no more than about 150 kPa or at least about 50 kPa and no more than about 100 kPa), inclusive of all values and ranges therebetween. In such embodiments, the solid loadings (i.e., the volume fraction of the active material 110 and conductive material 120 with respect to the semi-solid slurry 100) can be at least about 50%, at least about 55%, at least about 60%, at least about 65%, at least about 70%, at least about 75%, at least about 80%, at least about 85%, or at least about 90%.

[0061] In some embodiments, the semi-solid slurry 100 can have an electronic conductivity of at least about 1 mS / cm, at least about 2 mS / cm, at least about 3 mS / cm, at least about 4 mS / cm, at least about 5 mS / cm, at least about 10 mS / cm, at least about 20 mS / cm, at least about 30 mS / cm, at least about 40 mS / cm, at least about 50 mS / cm, at least about 60 mS / cm, least about 70 mS / cm, at least about 80 mS / cm, at least about 90 mS / cm, at least about 100 mS / cm, at least about 110 mS / cm, at least about 120 mS / cm, at least about 130 mS / cm, at least about 140 mS / cm, at least about 150 mS / cm, at least about 200 mS / cm, at least about 250 mS / cm, at least about 300 mS / cm, at least about 350 mS / cm, at least about 400 mS / cm, at least about 450 mS / cm, at least about 500 mS / cm, at least about 550 mS / cm, at least about 600 mS / cm, at least about 650 mS / cm, at least about 700 mS / cm, at least about 750 mS / cm, at least about 800 mS / cm, at least about 850 mS / cm, at least about 900 mS / cm, at least about 950 mS / cm, at leastabout 1,000 mS / cm, at least about 1,500 mS / cm, at least about 2,000 mS / cm, at least about 2,500 mS / cm, or at least about 3,000 mS / cm.

[0062] FIG. 2 shows a flow diagram of a method 10 for preparation of a semi-solid electrode. The method 10 includes blending an active material with a conductive material to form an intermediate material at step 11 and compacting the intermediate material to form a compacted electrode material at step 12. The method 10 can optionally include dry mixing the compacted electrode material at step 13. The method 10 can also include drying the compacted electrode material at step 14. The method 10 further includes mixing the compacted electrode material with an electrolyte to form a semi-solid slurry at step 15 and disposing the semi-solid slurry onto a current collector to form a semi-solid electrode.

[0063] The semi-solid electrode can be a semi-solid anode or a semi-solid cathode. In some embodiments, the compacted electrode material and the semi-solid slurry can be the same or substantially similar to the compacted electrode material and the semi-solid slurry 100 described above in connection with FIG. 1.

[0064] At step 11, the active material and the conductive material are dry -mixed to form the intermediate material. In some embodiments, the active material and the conductive material can be dry-mixed for a pre-determined period of time to ensure homogeneity of the intermediate material. In some embodiments, the intermediate material can be in a powder form. In some embodiments, the mixing at step 11 can be for a time sufficient to coat the active material particles in very fine particles of conductive material. In some embodiments, step 11 can be performed at a temperature higher than the ambient temperature. That is, in some embodiments, a certain amount of heat can be provided to the blending step such that at least one of the active material or the conductive material can be dried.

[0065] In some embodiments, the mixing at step 11 can be for at least about 10 seconds, at least about 20 seconds, at least about 30 seconds, at least about 40 seconds, at least about 50 seconds, at least about 1 minute, at least about 2 minutes, at least about 3 minutes, at least about 4 minutes, at least about 5 minutes, at least about 10 minutes, at least about 20 minutes, at least about 30 minutes, at least about 40 minutes, at least about 50 minutes, at least about 1 hour, at least about 2 hours, at least about 3 hours, at least about 4 hours, at least about 5 hours, at least about 10 hours, at least about 15 hours, or at least about 20 hours. In some embodiments, the mixing at step 11 can be for no more than about 24 hours, no more than about 20 hours, no more than about 15 hours, no more than about 10 hours, no more than about 5 hours, no morethan about 4 hours, no more than about 3 hours, no more than about 2 hours, no more than about 1 hour, no more than about 50 minutes, no more than about 40 minutes, no more than about 30 minutes, no more than about 20 minutes, no more than about 10 minutes, no more than about 5 minutes, no more than about 4 minutes, no more than about 3 minutes, no more than about 2 minutes, no more than about 1 minute, no more than about 50 seconds, no more than about 40 seconds, no more than about 30 seconds, or no more than about 20 seconds. Combinations of the above-referenced mixing durations are also possible (e.g., at least about 10 seconds and no more than about 24 hours or at least about 3 minutes and no more than about 1 hour), inclusive of all values and ranges therebetween. In some embodiments, the mixing at step 11 can be for about 10 seconds, about 20 seconds, about 30 seconds, about 40 seconds, about 50 seconds, about 1 minute, about 2 minutes, about 3 minutes, about 4 minutes, about 5 minutes, about 10 minutes, about 20 minutes, about 30 minutes, about 40 minutes, about 50 minutes, about 1 hour, about 2 hours, about 3 hours, about 4 hours, about 5 hours, about 10 hours, about 15 hours, about 20 hours, or about 24 hours.(0066] In some embodiments, the active material and the conductive material can be mixed together via blade mixing. In some embodiments, the blade mixing can be via a rotating blade. In some embodiments, the blade mixing can be via a fixed blade. In some embodiments, the active material and the conductive material can be directly mixed via a V-blender. In some embodiments, the active material and the conductive material can be mixed via ball milling in a ball mill. In some embodiments, active material and the conductive material can be mixed via roller milling in a roller mill. In some embodiments, the dry -mixing can include milling. In some embodiments, the milling can be at a low enough milling power or milling shear force such that the active material particles are not significantly fractured.

[0067] In some embodiments, compacting (e.g., pressing, pressurizing, densifying, etc.) the intermediate material, at step 12, can include at least one of roller pressing, die pressing, isostatic pressing, and hot pressing. The compacting the intermediate material can lead to the formation of dense compacted electrode material with enhanced mechanical properties by facilitating particle bonding. Accordingly, in some embodiments, the compacted electrode materials include a plurality of agglomerates. Any compaction technique that yields a densified powder blend of an active material 110 and a conductive material 120 (resulting a plurality of agglomerates of active material) can be used at step 12. In some embodiments, the compacting includes exerting a pre-determined amount of pressure on the intermediate material.

[0068] In some embodiments, the pre-determined amount of pressure exerted on the intermediate material can be at least about 200 kPa, at least about 500 kPa, at least about 1,000 kPa, at least about 1,500 kPa, at least about 2,000 kPa, at least about 2,500 kPa, at least about 3,000 kPa, at least about 3,500 kPa, at least about 4,000 kPa, at least about 4,500 kPa, at least about 5,000 kPa, at least about 5,500 kPa, at least about 6,000 kPa, at least about 6,500 kPa, at least about 7,000 kPa, at least about 7,500 kPa, at least about 8,000 kPa, at least about 8,500 kPa, at least about 9,000 kPa, at least about 9,500 kPa, at least about 10,000 kPa, at least about10.500 kPa, at least about 11,000 kPa, at least about 11,500 kPa, at least about 12,000 kPa, at least about 12,500 kPa, at least about 13,000 kPa, at least about 13,500 kPa, or at least about 14,000 kPa. In some embodiments, the pre-determined amount of pressure exerted on the intermediate material can be no more than about 15,000 kPa, no more than about 14,500 kPa, no more than about 14,000 kPa, no more than about 13,500 kPa, no more than about 13,000 kPa, no more than about 12,500 kPa, no more than about 12,000 kPa, no more than about11.500 kPa, no more than about 11,000 kPa, no more than about 10,500 kPa, no more than about 10,000 kPa, no more than about 9,500 kPa, no more than about 9,000 kPa, no more than about 8,500 kPa, no more than about 8,000 kPa, no more than about 7,500 kPa, no more than about 7,000 kPa, no more than about 6,500 kPa, no more than about 6,000 kPa, no more than about 5,500 kPa, no more than about 5,000 kPa, no more than about 4,500 kPa, no more than about 4,000 kPa, no more than about 3,500 kPa, no more than about 3,000 kPa, no more than about 2,500 kPa, no more than about 2,000 kPa, no more than about 1,500 kPa, or no more than about 200 kPa. Combinations of the above-referenced pressure ranges on the intermediate material are also possible (e.g., at least about 200 kPa and no more than about 15,000 kPa), inclusive of all values and ranges therebetween.

[0069] In some embodiments, compaction can be repeated multiple times. After initially compacting the intermediate material, the resulting compacted material can undergo several cycles of compaction. Each cycle may employ the same compaction process or any suitable combination of different compaction processes. For instance, the intermediate material can be first compacted using a roller press, followed by subsequent compaction using a different method such as hot pressing. In some embodiments, the compacting includes passing the intermediate material at least two times between the rollers of the roller press (e.g., about 2 times, about 3 times, about 4 times, about 5 times, about 6 times, about 7 times, about 8 times, about 9 times, about 10 times, or at least about 10 times, inclusive of all values and ranges therebetween).

[0070] In some embodiments, the compacting can include roller pressing. In some embodiments, the roller pressing can employ machines like a roll compactor or roller press, where the intermediate material passes through two counter-rotating rollers. The gap between these rollers can be adjusted to control the compression level of the intermediate material. In some embodiments, the gap is in a range of about 0 pm to about 50 pm, inclusive (e.g., about 1 pm, about 2 pm, about 3 pm, about 4 pm, about 5 pm, about 10 pm, about 15 pm, about 20 pm, about 25 pm, about 30 pm, about 35 pm, about 40 pm, about 45 pm, or about 50 pm, inclusive of all values and ranges therebetween).

[0071] In some embodiments, the compacting can include die pressing (also known as powder compacting). In some embodiments, the die pressing can include the use of equipment such as hydraulic presses or mechanical presses. In such embodiments, the intermediate material can be placed into a die cavity and compressed using a punch to form the desired shape.

[0072] In some embodiments, the compacting can include isostatic pressing that utilizes isostatic presses, either hydraulic or cold isostatic presses (CIP), which apply pressure uniformly in all directions. In such embodiments, the intermediate material can be enclosed in a flexible mold or container and subjected to high-pressure fluids (fluid isostatic pressing) or solids (cold isostatic pressing).

[0073] In some embodiments, the compacting can include hot pressing that employs equipment such as hot presses or sintering furnaces. In some embodiments, the intermediate material can be placed in a mold and heated while pressure is applied. This can allow for the formation of dense materials with enhanced mechanical properties by facilitating particle bonding at elevated temperatures.

[0074] In some embodiments, the compacted electrode material can be obtained via compacting a blend of an active material 110 and a conductive material 120 using a roller press equipment. In some embodiments, the compacted electrode material can be obtained via compacting a blend of an active material 110 and a conductive material 120 using at least one of a die press or a cold isostatic press machine.

[0075] Optional step 13 includes dry mixing the compacted electrode material. In some embodiments, step 13 can include any of the dry mixing processes described above with reference to step 11. Step 13 can be conducted as a batch process using a batch mixer, such asa high shear mixer, planetary mixer, centrifugal planetary mixer, sigma mixer, CAM mixer, and / or roller mixer.

[0076] Optional step 14 can include drying the compacted electrode material such that a moisture level of the compacted electrode material is in a range of about 20 ppm to about 500 ppm, inclusive. In some embodiments, the dried compacted material may have a moisture level of no more than about 500 ppm, no more than about 400 ppm, no more than about 300 ppm, no more than about 200 ppm, no more than about 100 ppm, no more than about 50 ppm, no more than about 40 ppm, no more than about 30 ppm, or no more than about 20 ppm. The drying can encompass various methodologies aimed at reducing the moisture content of the compacted electrode material. The drying may involve employing methods such as air drying, vacuum drying, and / or thermal drying techniques. Air drying utilizes ambient air to gradually remove moisture through natural evaporation, whereas vacuum drying creates a low-pressure environment to expedite moisture removal. Thermal drying methods employ heat, either through convection, conduction, or radiation, to evaporate moisture from the substance. The choice of drying method can depend on factors including the nature of the compacted electrode material, desired moisture levels, and / or efficiency considerations.

[0077] Step 15 includes mixing the compacted electrode material with an electrolyte to form a semi-solid slurry. Some suitable mixing devices that can be used at step 15 can include batch mixers (e.g., C.W. Brabender or BANBURRY® style), continuous compounding devices such as ported single or twin-screw extruders (e.g., Leistritz, Haake), high shear mixers such as blade-style blenders, high speed kneading machines, and / or rotary impellers. In some embodiments, the mixing device can be operable to control the flowability of the slurry regulating the temperature and / or to control the slurry homogeneity by modulating the chemical composition. In some embodiments, the semi-solid slurry can be mixed using a BANBURRY® style batch mixer, a mixing section of a twin screw extruder, a centrifugal planetary mixer, and / or a planetary mixer. In some embodiments, the semi-solid slurry can be sampled and / or monitored after mixing to measure and / or evaluate homogeneity, rheology, conductivity, viscosity, and / or density.

[0078] In some embodiment, the mixing can include adding the electrolyte to the compacted electrode material while the compacted electrode material is dry-mixed. Then, the compacted electrode material and the electrolyte can be mixed together for a certain period of time.

[0079] In some embodiments, some electrolyte loss can be tolerated and used as a control specification, and the amount that can be tolerated generally decreases as electrolyte volume fraction increases and / or mixing index increases. For example, at a mixing index of 0.8, the maximum electrolyte loss can be controlled to less than about 39%, to less than about 33%, or to less than about 27%. At a mixing index of 0.9, the maximum electrolyte loss can be controlled to less than about 5%, to less than about 4%, or to less than about 3%. At mixing indices higher than 0.9, the maximum electrolyte loss can be controlled to less than about 5%, to less than about 4%, or to less than about 3%. Component concentrations can be calculated to determine and / or predict tolerable losses, and vary according to the specific components. In some embodiments, loss tolerances will be higher while in others they will be more restrictive.

[0080] In some embodiments, the composition of the semi-solid slurry and the mixing process can be selected to homogeneously disperse the components of the slurry, achieve a percolating conductive network throughout the slurry and a sufficiently high bulk electrical conductivity. Such properties can correlate to desirable electrochemical performance. Such semi-solid slurries can have a rheological state conducive to processing, which may include transfer, conveyance (e.g., extrusion), dispensing, segmenting or cutting, and post-dispense forming (e.g., press forming, rolling, calendering, etc.), or any combination thereof.[0081 [ In some embodiments, the electrolyte can include an electrolyte with a high boiling temperature, such that a high shear energy can be applied to the mixture during mixing without the electrolyte boiling away. In other words, incorporating an electrolyte with a high boiling point into the mixture can aid in keeping the mixture as a semi-solid during mixing and / or milling, such that it does not dry up and become a solid. In some embodiments, the electrolyte can include ethylene carbonate (EC), propylene carbonate (PC), y-butyrolactone (GBL), or any combination thereof.

[0082] The compositional homogeneity of the semi-solid slurry can be evaluated quantitatively by an experimental method based on measuring statistical variance in the concentration distributions of the components of the slurry suspension. For example, mixing index is a statistical measure, essentially a normalized variance or standard deviation, describing the degree of homogeneity of a composition. (See, e.g., Erol, M, & Kalyon, D.M., Assessment of the Degree of Mixedness of Filled Polymers, Intern. Polymer Processing XX (2005) 3, pps. 228-237). Complete segregation would have a mixing index of zero and a perfectly homogeneous mix a mixing index of one. Alternatively, the homogeneity of the slurry can be described by its compositional uniformity (+x% / -y%), defined herein as the range:(100% - y)*C to (100% + x)*C. All of the values x and y are thus defined by the samples exhibiting maximum positive and negative deviations from the mean value C, thus the compositions of all mixed material samples taken fall within this range.

[0083] The basic process of determining mixing index includes taking a number of equally and appropriately sized material samples from the aggregated mix and conducting compositional analysis on each of the samples. The sampling and analysis can be repeated at different times in the mixing process. The sample size and volume can be based on considerations of length scales over which homogeneity is important, for example, greater than a multiple of both the largest solid particle size and the ultimate mixed state average intraparticle distance at the low end, and 1 / Nth of the total volume where N is the number of samples at the high end. Optionally, the samples can be on the order of the electrode thickness, which is generally much smaller than the length and width of the electrode. Capabilities of certain experimental equipment, such as a thermo-gravimetric analyzer (TGA), can narrow the practical sample volume range further. Sample “dimension” means the cube root of sample volume. For example, a common approach to validating the sampling (number of samples) is that the mean composition of the samples corresponding to a given mixing duration matches the overall portions of material components introduced to the mixer to a specified tolerance. The mixing index at a given mixing time is defined, according to the present embodiments, to be equal to 1- o / oref, where c is the standard deviation in the measured composition (which may be the measured amount of any one or more constituents of the slurry) and Gref is equal to [C(l -C)]1 2, where C is the mean composition of the N samples, so as the variation in sample compositions is reduced, the mixing index approaches unity. It should be understood in the above description that “time” and “duration” are general terms speaking to the progression of the mixing event.

[0084] In some embodiments, the process conditions of step 15 can be selected to produce a prepared a semi-solid slurry having a mixing index of at least about 0.80, at least about 0.90, at least about 0.95, or at least about 0.975.

[0085] In some embodiments, the process conditions of step 15 can be selected to produce a prepared semi-solid slurry having an electronic conductivity of at least about 10'6S / cm, at least about 10'5S / cm, at least about 10'4S / cm, at least about 10'3S / cm, or at least about 10'2S / cm. In some embodiments, the semi-solid slurry has a conductivity in a range of about 1 mS / cm to about 5,000 mS / cm. In some embodiments, the semi-solid slurry has a conductivity in a range of about 4 mS / cm to about 3,000 mS / cm. 1

[0086] In some embodiments, the process conditions of step 15 can be selected to produce a prepared slurry having an apparent viscosity at room temperature of less than about 100,000 Pa-s, less than about 10,000 Pa-s, or less than about 1,000 Pa-s, all at an apparent shear rate of 1,000 s'1. In some embodiments, the process conditions can be selected to produce a prepared slurry having two or more properties as described herein. Examples of systems and methods that can be used for preparing the semi-solid compositions and / or electrodes are described in U.S. Patent No. 9,484,569, (“the ‘569 patent”) filed March 15, 2013, entitled “Electrochemical Slurry Compositions and Methods for Preparing the Same,” the disclosure of which is incorporated herein by reference in their entirety.

[0087] In some embodiments, the semi-solid slurry has a yield strength of no more than about 150 kPa, no more than about 140 kPa, no more than about 130 kPa, no more than about 120 kPa, no more than about 110 kPa, no more than about 100 kPa, no more than about 90 kPa, no more than about 80 kPa, no more than about 70 kPa, no more than about 60 kPa, no more than about 50 kPa, no more than about 40 kPa, no more than about 30 kPa, no more than about 20 kPa, or no more than about 10 kPa.

[0088] In some embodiments, the mixing can be for at least about 5 minutes, at least about 6 minutes, at least about 7 minutes, at least about 8 minutes, at least about 9 minutes, at least about 10 minutes, at least about 11 minutes, at least about 12 minutes, at least about 13 minutes, at least about 14 minutes, at least about 15 minutes, at least about 16 minutes, at least about 17 minutes, at least about 18 minutes, at least about 19 minutes, at least about 20 minutes, at least about 21 minutes, at least about 22 minutes, at least about 23 minutes, at least about 24 minutes, at least about 25 minutes, at least about 26 minutes, at least about 27 minutes, at least about 28 minutes, at least about 29 minutes, or at least about 30 minutes.

[0089] In some embodiments, the mixing can impart a mixing power of at least about 4 kW / kg, at least about 4.5 kW / kg, at least about 5 kW / kg, at least about 5.5 kW / kg, at least about 6 kW / kg, at least about 6.5 kW / kg, at least about 6.7 kW / kg, at least about 7 kW / kg, at least about 7.5 kW / kg, at least about 8 kW / kg, at least about 8.5 kW / kg, at least about 9 kW / kg, or at least about 9.5 kW / kg. In some embodiments, the mixing can impart a mixing power of no more than about 10 kW / kg, no more than about 9.5 kW / kg, no more than about 9 kW / kg, no more than about 8.5 kW / kg, no more than about 8 kW / kg, no more than about 7.5 kW / kg, no more than about 7 kW / kg, no more than about 6.7 kW / kg, no more than about 6.5 kW / kg, no more than about 6 kW / kg, no more than about 5.5 kW / kg, no more than about 5 kW / kg, or no more than about 4.5 kW / kg. Combinations of the above-referenced ranges are also possible(e.g., at least about 4 kW / kg and no more than about 10 kW / kg or at least about 5 kW / kg and no more than about 7 kW / kg), inclusive of all values and ranges therebetween.

[0090] After step 15, the semi-solid slurry can be dispensed onto a current collector to form a semi-solid electrode.

[0091] In some embodiments, the current collector can be an anode current collector or a cathode current collector, depending on which electrode is desired to be formed. In some embodiments, dispensing can include using, for example, a “hanger die” sheet extrusion die, a “winter manifold” sheet extrusion die, a profile-style sheet extrusion die, an arbitrary nozzle operable to apply a continuous stream of material to a substrate, injection into a mold of the correct size and shape (e.g., filling a pocket with material), and / or any other suitable dispensing device. In some embodiments, dispensing the semi-solid slurry onto the current collector can include extruding the slurry through an extrusion die slot (e.g., an extrusion die slot having a width of at least about 100 pm). In some embodiments, the method 10 may include calendering the extruded semi-solid slurry to form a semi-solid electrode having a uniform thickness.

[0092] In some embodiments, prior to dispensing, the semi-solid slurry can be conveyed and / or pressurized, for example, using a piston pump, peristaltic pump, gear / lobe pump, progressing cavity pump, single screw extruder, conveying section of a twin screw extruder, and / or any other suitable conveying device. In some embodiments, the torque and / or power of the conveying device, the pressure at the conveying device exit, the flow rate, and / or the temperature can be measured, monitored and / or controlled during the conveying and / or pressurizing.

[0093] In some embodiments, after dispensing, the semi-solid slurry can be formed into a final electrode. For example, the semi-solid slurry can be calender roll formed, stamped and / or pressed, subjected to vibrational settling, and / or cut into discrete sections. Additionally, in some embodiments, unwanted portions of material can be removed (e.g., masking and cleaning) and optionally recycled back into the slurry manufacturing process.

[0094] FIG. 3A and FIG. 3B illustrate a roller press machine that can be utilized in the method 10 described in FIG. 2, with FIG. 3 A providing a photographic image and FIG. 3B presenting a graphical representation. FIG. 3C shows a photo of a compacted electrode material received from the roller press machine in a densified powder form.{0095] In some embodiments, the roller press machine includes two counter-rotating rollers, R1 and R2, which are spaced apart by a distance D. The distance D can significantlyinfluence the machine's performance characteristics, including pressure distribution, material compression efficiency, and the overall quality of the processed material. In some embodiments, the distance D is zero. In some embodiments, the distance D is about 40 pm. In some embodiments, the distance D is no more than about 50 pm, no more than about 40 pm, no more than about 30 pm, no more than about 20 pm, no more than about 10 pm, no more than about 5 pm, or no more than about 1 pm. In some embodiments, the distance D is about 40 pm. In some embodiments, the distance D is about 50 pm, about 40 pm, about 30 pm, about 20 pm, about 10 pm, about 5 pm, or about 1 pm, inclusive of all values and ranges therebetween. In some embodiments, the rollers can exert a pre-determined amount of pressure on the starting material (e.g., the intermediate material). In some embodiments, the predetermined amount of pressure can be at least about 200 kPa and no more than about 15,000 kPa.

[0096] FIGS. 4A-4D are scanning electron microscopy (SEM) images of a comparative uncompacted electrode material and a compacted electrode material subjected to various compacting methods, according to different embodiments. Each electrode material includes 98 vol% LFP and 2 vol% KETJEN BLACK® carbon black particles. FIG. 4A shows the comparative electrode material without compaction, where particles are distinguishable and loosely distributed, indicating a lack of cohesion. The compacted electrode materials, shown in FIGS. 4B-4D, are obtained using a roller press with different gap settings between its rollers. FIG. 4B illustrates the electrode material compacted once with a roller press having a 40 pm gap, displaying a more cohesive structure with less distinct particles, indicating some degree of compaction. FIG. 4C illustrates the electrode material compacted once with no gap between the rollers, where larger agglomerates and fewer visible gaps suggest a higher degree of compaction. FIG. 4D shows the electrode material compacted twice with no gap between the rollers, exhibiting the highest degree of compaction among the four samples, with large agglomerates and very few individual particles visible. The SEM images demonstrate that the compaction process significantly affects the agglomerate size in the electrode material. As the material undergoes more passes through the roller press or passes through rollers set with smaller gaps, the size of the agglomerates increases due to higher compaction. This indicates that controlling compaction conditions can effectively aid in tuning the microstructure of the electrode material.

[0097] FIG. 5 demonstrates the effect of compaction methods on the bulk and tap densities (grams per cubic centimeter (g / cc)) of both a comparative uncompacted electrode material anda compacted electrode material. The bar graph in FIG. 5 compares the bulk and tap densities of various samples of electrode material processed through a roller press method.

[0098] Bulk density can be defined as the powders apparent density that is related to a volume called the bulk volume, therefore, to determine the value of a bulk density of a specific powder, the bulk volume occupied by that powder has to be measured by a graduated cylinder. Tapped density is generally described in the terms of mass per unit volume that is obtained when voids or air gaps between particles are removed. Across all samples A-D, the tap density is consistently higher than the bulk density, indicating that the powder becomes more compact when tapped.

[0099] Each electrode material sample includes 98 vol% LFP and 2 vol% KETJEN BLACK®. Sample A is the uncompacted comparative electrode material. Sample B is the electrode material compacted once with a roller press having a 40 pm gap. Sample C is the electrode material compacted once with no gap between the rollers. Sample D is the electrode material compacted twice with no gap between the rollers. The graph shown in FIG. 5 reveals that the roller press method significantly increases both bulk and tap densities of the LFP / Ketjen blend, with bulk density nearly doubling, indicating substantial material compaction. A smaller gap and more passes through the roller press result in higher bulk and tap densities, indicating greater compaction. This is supported by SEM images in FIGS. 4A- 4D, which show larger agglomerates due to higher compaction with a smaller gap and more passes. The graph provides quantitative support for the SEM observations, demonstrating the significant impact of the roller press method on the bulk and tap densities of the electrode.

[0100] FIG. 6A presents a plot of conductivity (S / cm) versus volume fraction for both uncompacted and compacted electrode materials subjected to different compaction methods. Samples A, B, C, and D are the same as described in FIG. 5. The data points for Sample A show a positive correlation between volume fraction and conductivity, indicating that even without compaction, increasing the volume fraction enhances conductivity. Sample B, compacted once with a 40 pm gap, exhibits higher conductivity at the same volume fraction compared to Sample A, suggesting that compaction improves conductivity. Sample C, compacted once with no gap, shows further increased conductivity, and Sample D, compacted twice with no gap, exhibits the highest conductivity among all samples. This indicates that multiple passes through the roller press without a gap significantly enhance conductivity. The scatter plot in FIG. 6A demonstrates that the degree of compaction, particularly the number of passes and gap size in the roller press, significantly affects the conductivity of the electrodematerial, with both accessible volume fraction and conductivity increasing from Sample A to Sample D.

[0101] FIG. 6B illustrates the relationship between volume fraction and applied force for samples A, B, C, and D. The plots demonstrate that the compaction process, particularly the number of passes and the gap size in the roller press, significantly impacts the applied force the electrode material can withstand before reaching the percolation threshold of the electrode material. A shift in the percolation threshold by about 10% was observed comparing Sample A to Samples B, C, and D, suggesting that compaction increases percolation threshold. As the degree of compaction increases from Sample A to Sample D, the accessible volume fraction of the electrode material also increases.

[0102] FIG. 7 displays X-ray diffraction (XRD) patterns of a comparative uncompacted electrode material (Sample 1) and a compacted electrode material (Sample 2), both including 98 vol% LFP and 2 vol% KETJEN BLACK® . Sample 2, which has been compacted twice with a roller press with no gap between its rollers, shows no change in LFP crystallinity and fits well to a single phase of LFP. This suggests that the compaction process is non-destructive, and does not affect the crystal structure of the active material.

[0103] FIGS. 8A-8D are photographs depicting various semi-solid slurry compositions made by mixing an electrolyte with different electrode materials. The electrolyte includes lithium bis(fluorosulfonyl)imide dissolved in a solvent mixture of ethylene carbonate and dimethyl carbonate at a volume ratio of 3:7. Each slurry composition includes 49 vol% LFP, 1 vol% KETJEN BLACK®, and 50 vol% electrolyte. FIG. 8A shows a slurry formed from uncompacted electrode material. FIG. 8B shows a slurry made from electrode material compacted once with a roller press having a 40 pm gap. FIG. 8C shows a slurry made from electrode material compacted once with no gap between the rollers. FIG. 8D shows a slurry made from electrode material compacted twice with no gap between the rollers. FIGS. 8A-8D visually demonstrate the changes in texture and consistency of the slurries subjected to different compaction methods. The slurry in FIG. 8A appears less fluid compared to the more compact and fluid-like slurries shown in the subsequent figures.

[0104] FIGS. 9A-9D are photographs depicting different semi-solid slurry compositions made from uncompacted electrode material with varying amounts of electrochemically active material. As the amount of active material increases from 50 vol% in FIG. 9A to 65 vol% in FIG. 9D, castability decreases. Specifically, FIG. 9B shows a slurry with 55 vol% activematerial, and FIG. 9C shows a slurry with 60 vol% active material. Notably, hand-casting was not possible for slurries with more than 50 vol% active material that did not use compacted powders. As the active material percentage increases, the slurry becomes less suitable for casting processes.[0105| FIGS. 10A-10D are photographs of semi-solid slurry compositions made from electrode material compacted once with a roller press machine. FIG. 10A shows a slurry with 50 vol% active material, FIG. 10B shows a slurry with 55 vol% active material, FIG. 10C shows a slurry with 60 vol% active material, and FIG. 10D shows a slurry with 65 vol% active material. These images demonstrate the effect of increasing active material on the physical properties of the slurries, specifically their castability for electrode manufacturing. Handcasting is feasible for slurries prepared with compacted powders up to 60 vol% active material.

[0106] FIGS. 11A-11D are photographs of semi-solid slurry compositions made from electrode material compacted twice with a roller press machine. FIG. 11 A depicts a slurry with 50 vol% active material, FIG. 11B shows a slurry with 55 vol% active material, FIG. 11C shows a slurry with 60 vol% active material, and FIG. 1 ID shows a slurry with 65 vol% active material. These images highlight the impact of increasing active material on the physical properties and castability of the slurries for electrode manufacturing. Hand-casting is possible for slurries with up to 65 vol% active material when compacted powders are used.

[0107] FIGS. 12A and 12B illustrate the impact of various compaction techniques on the electronic conductivity (mS / cm) and yield stress (kPa) of semi-solid slurry compositions, which consist of 49 vol% LFP, 1 vol% KETJEN BLACK®, and 50 vol% electrolyte. Sample A’ represents a semi-solid slurry formed from a comparative electrode material with no compaction. Sample B’ is the slurry formed from an electrode material compacted once using a roller press with a 40 pm gap between the rollers. Sample C’ is formed from an electrode material compacted once with a roller press having no gap between the rollers, and Sample D’ is formed from an electrode material compacted twice with a roller press having no gap between the rollers.

[0108] FIG. 12A is a plot showing the conductivities (S / cm) of various semi-solid slurry compositions, including both uncompacted and compacted electrode materials subjected to different compacting methods. FIG. 12B is a plot displaying the yield stresses (kPa) of these compositions under similar conditions. FIG. 12A illustrates how the degree of compaction influences the electronic conductivity of the semi-solid slurry. The uncompacted material(sample A') exhibits the highest conductivity. Conductivity decreases significantly when the material is compacted once using a roller press with a 40 pm gap (sample B'). However, additional compaction improves the conductivity, as seen in samples C’ and D’. FIG. 12B demonstrates the effect of compaction on the yield stress of the semi-solid slurry. The highest yield stress is observed in the uncompacted material (sample A'). The lowest yield stress occurs when the material is compacted twice with a roller press having no gap (sample D’). Lower yield stress indicates better castability, and the yield stress reduction by 80-95% suggests a substantial improvement in the castability of the semi-solid slurry.

[0109] FIG. 13 is a plot showing the effect of compacting methods on the average yield stress (kPa) of various semi-solid slurry compositions with different amounts of solid loadings (volume fraction of active and conductive material with respect to the slurry), according to various embodiments. For the same solid loading, the semi-solid slurry formed from uncompacted electrode material exhibits higher yield stress. As the total volume of active and conductive material increases in the slurry, yield stress also increases. Among all samples, the semi-solid slurry formed from an electrode material compacted twice with a roller press shows the lowest yield stress. At 55% solid loading, the results for the semi-solid slurries formed from uncompacted electrode material and electrode material compacted once with a roller press show higher yield stresses compared to the semi-solid slurry formed from electrode material compacted twice with a roller press. However, data points beyond 60% solid loading are omitted due to less reliable yield stress measurements at higher loadings.

[0110] FIG. 14 presents a plot of voltage (V) versus normalized capacity (%) for electrochemical cells fabricated using both a comparative uncompacted electrode material and a compacted electrode material subjected to various compacting methods, according to different embodiments. That is, FIG. 14 illustrates how varying levels of powder compaction in battery cells influence their ability to maintain voltage across usage cycles. The cells made using compacted powder demonstrate enhanced accessibility to theoretical capacity, indicating no shutdown of lithium iron phosphate (LFP) through compaction. These findings could hold significant implications for enhancing the efficiency and longevity of such battery cells.

[0111] Various concepts may be embodied as one or more methods, of which at least one example has been provided. The acts performed as part of the method may be ordered in any suitable way. Accordingly, embodiments may be constructed in which acts are performed in an order different than illustrated, which may include performing some acts simultaneously, even though shown as sequential acts in illustrative embodiments. Put differently, it is to beunderstood that such features may not necessarily be limited to a particular order of execution, but rather, any number of threads, processes, services, servers, and / or the like that may execute serially, asynchronously, concurrently, in parallel, simultaneously, synchronously, and / or the like in a manner consistent with the disclosure. As such, some of these features may be mutually contradictory, in that they cannot be simultaneously present in a single embodiment. Similarly, some features are applicable to one aspect of the innovations, and inapplicable to others.

[0112] In addition, the disclosure may include other innovations not presently described. Applicant reserves all rights in such innovations, including the right to embodiment such innovations, file additional applications, continuations, continuations-in-part, divisionals, and / or the like thereof. As such, it should be understood that advantages, embodiments, examples, functional, features, logical, operational, organizational, structural, topological, and / or other aspects of the disclosure are not to be considered limitations on the disclosure as defined by the embodiments or limitations on equivalents to the embodiments. Depending on the particular desires and / or characteristics of an individual and / or enterprise user, database configuration and / or relational model, data type, data transmission and / or network framework, syntax structure, and / or the like, various embodiments of the technology disclosed herein may be implemented in a manner that enables a great deal of flexibility and customization as described herein.10H3I All definitions, as defined and used herein, should be understood to control over dictionary definitions, definitions in documents incorporated by reference, and / or ordinary meanings of the defined terms.

[0114] As used herein, the term “about” generally means plus or minus 10% of the value stated, e.g. about 5 would include 4.5 to 5.5, about 10 would include 9 to 11, about 100 would include 90 to 110. Where a range of values is provided, it is understood that each intervening value, to the tenth of the unit of the lower limit unless the context clearly dictates otherwise, between the upper and lower limit of that range and any other stated or intervening value in that stated range is encompassed within the disclosure. That the upper and lower limits of these smaller ranges can independently be included in the smaller ranges is also encompassed within the disclosure, subject to any specifically excluded limit in the stated range. Where the stated range includes one or both of the limits, ranges excluding either or both of those included limits are also included in the disclosure.

[0115] The phrase “and / or,” as used herein in the specification and in the embodiments, should be understood to mean “either or both” of the elements so conjoined, i.e., elements that are conjunctively present in some cases and disjunctively present in other cases. Multiple elements listed with “and / or” should be construed in the same fashion, i.e., “one or more” of the elements so conjoined. Other elements may optionally be present other than the elements specifically identified by the “and / or” clause, whether related or unrelated to those elements specifically identified. Thus, as a non-limiting example, a reference to “A and / or B”, when used in conjunction with open-ended language such as “comprising” can refer, in one embodiment, to A only (optionally including elements other than B); in another embodiment, to B only (optionally including elements other than A); in yet another embodiment, to both A and B (optionally including other elements); etc.

[0116] As used herein in the specification and in the embodiments, “or” should be understood to have the same meaning as “and / or” as defined above. For example, when separating items in a list, “or” or “and / or” shall be interpreted as being inclusive, i.e., the inclusion of at least one, but also including more than one, of a number or list of elements, and, optionally, additional unlisted items. Only terms clearly indicated to the contrary, such as “only one of’ or “exactly one of,” or, when used in the embodiments, “consisting of,” will refer to the inclusion of exactly one element of a number or list of elements. In general, the term “or” as used herein shall only be interpreted as indicating exclusive alternatives (i.e., “one or the other but not both”) when preceded by terms of exclusivity, such as “either,” “one of,” “only one of,” or “exactly one of.” “Consisting essentially of,” when used in the embodiments, shall have its ordinary meaning as used in the field of patent law.|0117| As used herein in the specification and in the embodiments, the phrase “at least one,” in reference to a list of one or more elements, should be understood to mean at least one element selected from any one or more of the elements in the list of elements, but not necessarily including at least one of each and every element specifically listed within the list of elements and not excluding any combinations of elements in the list of elements. This definition also allows that elements may optionally be present other than the elements specifically identified within the list of elements to which the phrase “at least one” refers, whether related or unrelated to those elements specifically identified. Thus, as a non-limiting example, “at least one of A and B” (or, equivalently, “at least one of A or B,” or, equivalently “at least one of A and / or B”) can refer, in one embodiment, to at least one, optionally including more than one, A, with no B present (and optionally including elements other than B); inanother embodiment, to at least one, optionally including more than one, B, with no A present (and optionally including elements other than A); in yet another embodiment, to at least one, optionally including more than one, A, and at least one, optionally including more than one, B (and optionally including other elements); etc.[0118| In the embodiments, as well as in the specification above, all transitional phrases such as “comprising,” “including,” “carrying,” “having,” “containing,” “involving,” “holding,” “composed of,” and the like are to be understood to be open-ended, i.e., to mean including but not limited to. Only the transitional phrases “consisting of’ and “consisting essentially of’ shall be closed or semi-closed transitional phrases, respectively, as set forth in the United States Patent Office Manual of Patent Examining Procedures, Section 2111.03.[0119| While specific embodiments of the present disclosure have been outlined above, many alternatives, modifications, and variations will be apparent to those skilled in the art. Accordingly, the embodiments set forth herein are intended to be illustrative, not limiting. Various changes may be made without departing from the spirit and scope of the disclosure. Where methods and steps described above indicate certain events occurring in a certain order, those of ordinary skill in the art having the benefit of this disclosure would recognize that the ordering of certain steps may be modified and such modification are in accordance with the variations of the invention. Additionally, certain of the steps may be performed concurrently in a parallel process when possible, as well as performed sequentially as described above. The embodiments have been particularly shown and described, but it will be understood that various changes in form and details may be made.

Claims

Claims1. A method, comprising: blending an active material with a conductive material to form an intermediate material; compacting the intermediate material to form a compacted electrode material; mixing the compacted electrode material with an electrolyte to form a semi-solid slurry; and disposing the semi-solid slurry onto a current collector to form a semi-solid electrode.

2. The method of claim 1, wherein the compacting includes passing the intermediate material between a first roller and a second roller separated by a distance, the first roller and the second roller exerting a pre-determined pressure onto the intermediate material to form the compacted electrode material.

3. The method of claim 2, wherein the distance is in a range of about 0 pm to about 40 pm.

4. The method of claim 2 or 3, wherein the compacting includes passing the intermediate material at least two times between the first roller and the second roller.

5. The method of any one of claims 1-4, wherein a ratio of a tapped density to a true density of the compacted electrode material is in a range of about 0.4 to about 0.7.

6. The method of any one of claims 1-5, wherein the compacting includes exerting pressure on the intermediate material using a die press or a cold isostatic press.

7. The method of any one of claims 1-6, further comprising: prior to mixing the compacted electrode material with the electrolyte, drying the compacted electrode material such that a moisture level of the compacted electrode material is in a range of about 20 ppm to about 500 ppm.

8. The method of any one of claims 1-7, wherein the semi-solid slurry has an electronic conductivity in a range of about 4 mS / cm to about 3000 mS / cm.

9. The method of any one of claims 1-8, wherein the semi-solid slurry has a yield strength of less than 20 kPa.

10. The method of any one of claims 1-9, further comprising: dry mixing the compacted electrode material prior to mixing the compacted electrode material with the electrolyte.

11. The method of claim 10, wherein the dry mixing is performed for a duration of at least about 5 minutes.

12. The method of claim 10 or 11, wherein mixing the compacted electrode material with the electrolyte includes adding the electrolyte to the compacted electrode material while dry mixing the compacted electrode material.

13. The method of any one of claims 1-12, wherein the electrolyte comprises at least one of ethylene carbonate, dimethyl carbonate, gamma-butyrolactone, lithium bis(fluorosulfonyl) imide, trioctyl phosphate, propylene carbonate, dimethoxyethane, bis(trifluoromethanesulfonyl)imide, Lii.4Alo.4Tii.6(P04)3, lithium hexafluorophosphate, lithium bis(trifluoromethanesulfonyl)imide, lithium borate, or lithium carbonate.

14. The method of any one of claims 1-13, wherein the compacted electrode material comprises about 50% to about 90% by volume of an electrochemically active material.

15. The method of claim 14, wherein the compacted electrode material further comprises: a conductive material, the conductive material including at least one of graphite, activated carbon, conductive carbon, KETJEN BLACK® carbon particles, hard carbon, soft carbon, carbon nanotubes, carbon nanofibers, nickel-metal hydride, nickel cadmium, lithium cobalt oxide, or lithium iron phosphate.

16. The method of any one of claims 1-15, wherein the compacted electrode material comprises:an electrochemically active material, a portion of the electrochemically active material formed into a plurality of agglomerates, each of the plurality of agglomerates having a longest dimension of at least about 10 pm; and a conductive material, the conductive material disposed on and between the plurality of agglomerates.

17. The method of any one of claims 1-16, wherein the compacting includes applying a pressure in a range of about 200 kPa to about 15,000 kPa to the intermediate material.

18. The method of any one of claims 1-17, wherein the semi-solid slurry has a mixing index of at least about 0.90.

19. The method of any one of claims 1-18, wherein blending the active material with the conductive material is performed for a duration of at least about 10 minutes.

20. The method of any one of claims 1-19, wherein mixing the compacted electrode material with an electrolyte imparts a mixing power of at least about 4 kW / kg.

21. The method of any one of claims 1-20, wherein disposing the semi-solid slurry onto a current collector comprises extruding the semi-solid slurry through an extrusion die slot having a width of at least about 100 pm.

22. The method of any one of claims 1-21, further comprising: forming an electrochemical cell including the semi-solid electrode.

23. The method of claim 22, wherein the electrochemical cell has a specific energy density of at least about 250 W h / kg when discharged at 1C.

24. A compacted electrode material, comprising: an electrochemically active material, a portion of the electrochemically active material formed into a plurality of agglomerates, each of the plurality of agglomerates having a longest dimension of at least about 10 pm; and a conductive material, the conductive material disposed on and between the plurality of agglomerates.

25. The compacted electrode material of claim 24, wherein a ratio of a tapped density to a true density of the compacted electrode material is in a range of about 0.4 to about 0.7.

26. The compacted electrode material of claim 24 or 25, wherein the portion of the electrochemically active material formed into a plurality of agglomerates includes least about 30% of a total amount of the electrochemically active material.

27. The compacted electrode material of any one of claims 24-26, wherein the electrochemically active material comprises at least one of lithium cobalt oxide, lithium nickel manganese cobalt oxide, or lithium iron phosphate (LFP).

28. The compacted electrode material of any one of claims 24-26, wherein the electrochemically active material comprises at least one of graphite, lithium metal, silicon, carbon, lithium-intercalated carbon, lithium nitrides, lithium alloys, or lithium alloy forming compounds.

29. The compacted electrode material of any one of claims 24-28, wherein the conductive material comprises at least one of graphite, activated carbon, conductive carbon, KETJEN BLACK® carbon particles, hard carbon, soft carbon, carbon nanotubes, carbon nanofibers, nickel-metal hydride, nickel cadmium, lithium cobalt oxide, or lithium iron phosphate.

30. The compacted electrode material of any one of claims 24-29, wherein the compacted electrode material comprises about 50% to about 90% by volume of the electrochemically active material.

31. A semi-solid slurry composition, comprising: the compacted electrode material of any one of claims 24-30; and about 20% to about 50% by volume of an electrolyte.

32. The semi-solid slurry composition of claim 31, wherein the semi-solid slurry composition has a yield strength of less than about 140 kPa.

33. The semi-solid slurry composition of claim 31 or 32, wherein the semi-solid slurry has an electronic conductivity in a range of about 4 mS / cm to about 3,000 mS / cm.

34. The semi-solid slurry composition of any one of claims 31-33, wherein the electrolyte comprises at least one of ethylene carbonate, dimethyl carbonate, gammabutyrolactone, lithium bis(fluorosulfonyl) imide, trioctyl phosphate, propylene carbonate, dimethoxyethane, bis(trifluoromethanesulfonyl)imide, Lii.4Alo.4Tii.6(P04)3, lithium hexafluorophosphate, lithium bis(trifluoromethanesulfonyl)imide, lithium borate, or lithium carbonate.

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