2894 results about "All solid state" patented technology

The invention relates to the technical field of solid-state batteries, in particular to oxyhalide solid-state electrolyte as well as a preparation method and application thereof. The method comprises the following steps: taking molten salt LiaMbXc as a raw material, reacting with an oxide AdOf in a molten state, removing steam impurities by utilizing a high-temperature vacuumizing mode, and cooling to prepare the oxyhalide solid electrolyte; according to the invention, the molten salt raw material is molten at high temperature to form the ion melt, and the oxygen element is introduced to replace part of halogen, so that the hardness of the target electrolyte is reduced after cooling, the deformability at room temperature is improved, and the obtained electrolyte is high in conductivity and wide in antioxidant electrochemical window. The prepared oxyhalide solid electrolyte is used for preparing a positive electrode, the adhesion force between the electrolyte and positive electrode material particles, the actual microscopic contact area and the ion migration rate are improved through melt permeation, the problem of a positive electrode interface is effectively relieved, and the electrochemical performance of an all-solid-state battery is improved.

The invention relates to a composite solid electrolyte membrane with high ceramic content and a preparation method and application thereof. The preparation method comprises the following steps: mixing ceramic solid electrolyte particles activated by a silane coupling agent with an in-situ polymerization solution containing a cross-linking agent, an organic monomer, a plasticizer, a lithium salt, an ultraviolet light initiator and a thermal initiator to form solid electrolyte slurry, wherein the ceramic solid electrolyte particles account for 60-90% of the total mass of the composite solid electrolyte membrane; the preparation method comprises the following steps: coating a positive pole piece with solid electrolyte slurry, initiating shallow organic matter monomers and a cross-linking agent to generate in-situ polymerization through an ultraviolet light initiator, covering a negative pole piece for hot pressing treatment, initiating residual organic matter monomers and the cross-linking agent to generate in-situ polymerization through a thermal initiator, and forming a composite electrolyte membrane with high ceramic content. The invention also discloses an all-solid-state battery containing the composite solid electrolyte membrane. The solid-state battery containing the in-situ formed composite solid-state electrolyte membrane has relatively high cycling stability.

The invention discloses a single-ion conductor polymer, a ternary composite binder solution, high-solid-content sulfide electrolyte slurry and a wet film forming method and application thereof, and belongs to the technical field of all-solid-state lithium batteries. The key technical problems in the wet membrane preparation of the sulfide electrolyte are solved through an innovative solvent-binder synergistic system, and the method specifically comprises the steps that 1, through the synergistic effect of a non-polar solvent and a weak-polar solvent, low-viscosity coating of high-solid-content slurry is achieved while the chemical stability of the sulfide electrolyte is guaranteed; 2, a poly (lithium styrenesulfonate-butyl acrylate), styrene butadiene rubber and polyisobutene ternary composite binder is designed, a lithium ion transmission channel is provided through a lithium sulfonate group, a benzene ring structure in the styrene butadiene rubber enhances the mechanical strength, long-chain alkane in the polyisobutene improves the interface adhesive force, and the mechanical strength is improved; the three components cooperate to realize balance of mechanical and electrochemical properties of the electrolyte membrane, so that the prepared electrolyte membrane has low porosity, high ionic conductivity and mechanical strength.

The invention discloses a preparation method and application of a sulfide solid electrolyte membrane based on a gradient polymer / ionic liquid composite binder, and an all-solid-state battery, and belongs to the technical field of all-solid-state batteries. The method comprises the following steps: firstly coating a polymer / ionic liquid / sulfide electrolyte composite layer through a gradient coating process, filling particle gaps under low pressure by utilizing the plasticizing effect of ionic liquid, and reducing the porosity of an interface; and then coating a polymer / sulfide electrolyte surface layer to provide mechanical support and inhibit side reaction of the electrode. According to the design, the electrolyte membrane still keeps high ionic conductivity under the working pressure of a commercial power battery module, and the interface impedance is reduced compared with that of a traditional homogeneous membrane. Through the innovative gradient structure and material combination, the ion transmission bottleneck of the sulfide electrolyte under the low-pressure condition is solved, excellent interface stability and process compatibility are achieved, and a key technical scheme is provided for all-solid-state battery industrialization.

The invention relates to a solid electrolyte coated silicon-carbon negative electrode material and a preparation method thereof, an all-solid-state battery and an electric device, and belongs to the technical field of methods or devices for directly converting chemical energy into electric energy. The solid electrolyte coated silicon-carbon negative electrode material comprises a silicon-carbon negative electrode material and a solid electrolyte coating layer arranged on the surface of the silicon-carbon negative electrode material, the solid electrolyte coating layer comprises at least one of sulfide electrolyte and halide electrolyte; the silicon-carbon negative electrode material comprises an inner core and a carbon coating layer arranged on the surface of the inner core, the inner core comprises a porous carbon matrix and a silicon-based material positioned in pores of the porous carbon matrix. The solid-state electrolyte coated silicon-carbon negative electrode material enables an all-solid-state battery to have high ionic conductivity and first efficiency and excellent cycling stability.

The invention belongs to the technical field of design and preparation of solid electrolyte materials, and particularly relates to a LiBH4-based composite solid electrolyte material and a preparation method thereof.The LiBH4-based composite solid electrolyte material is obtained by performing high-energy ball milling on a mixture of LiBH4 and one or two metal halides MX2 in a certain molar ratio in an argon atmosphere; m is Mg, Zn, Ni or Bi; x is F, Cl, Br or I. According to the LiBH4 composite solid electrolyte prepared by the preparation method disclosed by the invention, the ionic conductivity at room temperature is improved to 10 <-4 > S cm <-1 > or above, and the ion diffusion activation energy is only 0.16 eV; the process is simple, the preparation time is short, the repeatability is high, no pollution is caused to the environment, and the industrial production requirement is met, so that the all-solid-state lithium ion battery electrolyte is expected to realize commercialized application.

The invention relates to the technical field of all-solid-state batteries, in particular to a halide sulfide double-layer coated positive electrode material and a preparation method and application thereof. The halide sulfide double-layer coated positive electrode material comprises a positive electrode material substrate, and a halide electrolyte coating layer and a sulfide electrolyte coating layer which sequentially coat the positive electrode material substrate. The halide electrolyte coating layer is located in the middle layer, compatibility with a positive electrode interface can be achieved by means of high oxidation resistance of the halide electrolyte coating layer, and the problem of the positive electrode interface occurring in sulfide electrolyte oxygenolysis is solved. The sulfide electrolyte coating layer is located on the outermost layer, air stability is excellent, processing in a dry environment can be met, and the problems that halide electrolyte is poor in chemical stability, cannot be processed and manufactured in an external environment and is high in density are solved. The halide sulfide double-layer coated positive electrode material has high interface stability and good chemical stability.

The invention discloses a composite coated graphite negative electrode material, a preparation method thereof and a lithium ion solid-state battery, and belongs to the technical field of lithium ion solid-state batteries, the composite coated graphite negative electrode material comprises a graphite matrix and a composite coating layer, and the composite coating layer comprises an inner layer amorphous lithium chloride and an outer layer nanocrystalline LiF / Li3N composite phase. Mixing graphite, lithium chloride containing crystal water and ammonium fluoride to obtain a mixed material; placing the mixed material in a microwave reaction cavity, heating the mixed material to 600-700 DEG C at the microwave power of 800-1200 W in an H2 / Ar mixed atmosphere, and keeping the temperature for 20-60 minutes; and cooling the sintered mixed material, grinding, and sieving with a 100-300 mesh sieve to obtain the composite coated graphite negative electrode material with a coating layer thickness of 10-50 nm. The invention provides an innovative amorphous LiCl / nanocrystalline LiF-Li3N gradient coating layer design, the performance of the lithium ion battery is remarkably improved by optimizing an ion migration path, enhancing the interface stability and reducing the process cost, and a new engineering way is provided for realizing high magnification and long cycle performance of the sulfide all-solid-state battery.

The invention provides a surface-modified sulfide electrolyte and a preparation method thereof, and an all-solid-state battery, the surface-modified sulfide electrolyte comprises a sulfide electrolyte and a modification layer coated on the surface of the sulfide electrolyte, the chemical general formula of the modification layer is LiaMbNcXd, 0 < = a < = 3, 0 < = b < = 1, 0 < = c < = 1, 0 < = d < = 6, and 0 < = c < = 1. M is at least one element of magnesium, aluminum, calcium, iron, zirconium, niobium, tantalum, tungsten, gadolinium, yttrium, indium, hafnium, lanthanum and ytterbium, and X is at least one element of oxygen, sulfur, fluorine, chlorine, bromine and iodine. According to the surface-modified sulfide electrolyte, the modification layer with high ionic conductivity and high oxidation potential is coated outside the sulfide electrolyte, so that when the surface-modified sulfide electrolyte is applied to a positive electrode of an all-solid-state battery, the modification layer can improve the oxidation potential of the electrolyte on the premise of not reducing the ionic conductivity of the electrolyte; the effects of improving the interface stability between the positive electrode active material and the sulfide electrolyte and further improving the cycle performance of the battery are achieved.

The invention belongs to the technical field of solid-state batteries, and provides a lithium-sulfur-phosphorus-chlorine-bromine solid-state electrolyte, a preparation method thereof and an all-solid-state battery. The preparation method comprises the following steps: mixing lithium sulfide and phosphorus sulfide, and carrying out ball milling to obtain a lithium-sulfur-phosphorus ternary mixture; in protective gas, the lithium-sulfur-phosphorus ternary mixture, lithium chloride and lithium bromide are mixed and then subjected to ball milling, and a lithium-sulfur-phosphorus-chlorine-bromine mixture is obtained; and carrying out heat treatment on the lithium-sulfur-phosphorus-chlorine-bromine mixture in protective gas to obtain the lithium-sulfur-phosphorus-chlorine-bromine solid electrolyte. The lithium-sulfur-phosphorus-chlorine-bromine solid electrolyte provided by the invention not only improves the electrochemical stability, but also maintains the high ionic conductivity characteristic.

The invention discloses a solid electrolyte, a preparation method thereof and an all-solid-state battery, and belongs to the technical field of solid electrolytes. According to the preparation method, a nano inert oxide and a solid electrolyte raw material are compounded through mechanical grinding, and the solid electrolyte with a core-shell structure is prepared; the device comprises an inner core, an interface layer and a shell from inside to outside, the inner core is a solid electrolyte matrix, the interface layer is a transition layer generated by reaction of the solid electrolyte matrix and a nano inert oxide, and the shell is a nano inert oxide layer. The material combines the advantages of high moisture resistance and wide electrochemical window of the nano inert oxide and the characteristics of high ionic conductivity and excellent mechanical property of the solid electrolyte, and the comprehensive performance of the material is remarkably improved through the synergistic effect of the components. The composite structure design not only solves the problem of performance limitation of a single material system, but also realizes collaborative optimization of ionic conductivity, environmental adaptability and electrochemical stability while ensuring the material stability.

The invention discloses an oxyhalide solid electrolyte, a preparation method thereof and an all-solid-state battery, and relates to the technical field of batteries. The solid electrolyte is LiaMbNcXdOe, M and N are the same elements or different elements, and M and N are at least one of Zn, Ba, Al, In, Y, Cr, Ti, Zr, Hf, Nb, Ta, La, Ce, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb and Lu; x is at least one of F, Cl, Br and I. The oxyhalide solid electrolyte with high ionic conductivity and cost advantage is prepared by selecting high-valence metal oxide, halide and lithium halide through a ball milling method and combining annealing and hot pressing processes, and the oxyhalide solid electrolyte can show good electrochemical performance when being applied to all-solid-state lithium metal batteries.

The invention discloses a mixed ion conductor layer for a lithium metal negative electrode, a preparation method of the mixed ion conductor layer and an all-solid-state battery, and belongs to the technical field of sulfide all-solid-state batteries. The preparation method comprises the following steps: synthesizing a sulfide electrolyte 70 (0.75 Li2S-0.25 P2S5)-30LiI through a liquid phase, introducing graphene oxide and a lithium salt precursor 2, 5-dihydroxy-1, 4-benzene diphosphate in the electrolyte preparation process, and carrying out heat treatment and pressing to obtain a mixed ion conductor layer; the graphene oxide can isolate the sulfide electrolyte layer from the lithium metal negative electrode, interface reaction is avoided, and a special porous and interlayer structure provides a transverse growth space for lithium metal deposition. And meanwhile, the lithium diphosphate-based MOF among the graphene layers ensures the rapid movement of lithium ions, enhances the bulk diffusion of lithium at the negative electrode end, reduces the local current density, plays a role in dredging the distribution of the lithium ions, and remarkably prolongs the cycle life of the sulfide all-solid-state battery.

The invention discloses an all-solid-state composite dry conductive agent and a preparation method thereof, and belongs to the technical field of batteries. The all-solid-state composite dry conductive agent is prepared by the following steps: uniformly mixing carbon nanotubes, high-dispersion carbon black and graphene to obtain a primary mixture; then preparing a uniformly dispersed glue solution from the composite dispersant and water; and then adding the primary mixture into the glue solution, uniformly mixing, sanding, homogenizing, drying and crushing to obtain the product, the high-dispersion carbon black is obtained by oxidizing carbon black to form active groups such as carboxyl and hydroxyl on the surface of the carbon black, halogenating acyl and then reacting with lithium 2, 5-diaminobenzene sulfonate. The preparation method comprises the following steps: grafting histidine ester into carboxymethyl cellulose by using propylene glycol diglycidyl ester as a cross-linking agent, then introducing allyl-1, 3-sultone, then copolymerizing with lithium 2-acrylamido-2-methylpropanesulfonate and 3-aminobenzoic acid allyl ester protected by fluorenylmethoxycarbonyl, and then deprotecting to obtain the composite dispersant.

The invention provides a solid-state battery and a preparation method thereof, and particularly relates to the technical field of solid-state batteries. The solid-state battery is composed of a plurality of laminated units, the laminated unit comprises a positive pole piece, an all-solid-state electrolyte membrane and a negative pole piece which are sequentially stacked according to a sandwich structure; among the positive pole piece, the all-solid-state electrolyte membrane and the negative pole piece, convex structures and concave structures which are uniformly arranged are distributed on any two mutually contacted surfaces of the positive pole piece, the all-solid-state electrolyte membrane and the negative pole piece. When the components of the solid-state battery are overlapped, the convex structures and the concave structures on the surfaces of the solid-state battery can be mutually engaged to form a stable micro-embedded structure, the interface bonding strength between the positive electrode and the electrolyte and between the negative electrode and the electrolyte is greatly enhanced through physical embedding, and the problem of unstable bonding in the prior art is solved. Meanwhile, the uniform concave-convex structure ensures the controllability and consistency of the interface contact area, effectively reduces and stabilizes the interface impedance, improves the performance consistency of the pole piece, and further improves the production yield and the overall performance stability of the battery.

The invention discloses a modified silicon negative electrode material and a preparation method and application thereof, belongs to the technical field of all-solid-state batteries, and can compensate the active lithium loss of the whole battery, improve the cycle performance of the battery and relieve the volume change through negative electrode pre-lithiation. The method comprises the following steps: pressing silicon powder into blocks under a certain pressure; coating the blocky silicon and the cut lithium foil according to a certain proportion, grinding and mixing to obtain a precursor I; under the protection of inert gas, the precursor I is heated for the first time, and a powder precursor II is obtained; and grinding the precursor II, pressing the precursor II into blocks, heating the blocks in a vacuum or inert atmosphere to a preset temperature, and grinding the blocks to obtain the lithium-silicon alloy. The preparation process is simple, the silicon negative electrodes with different pre-lithiation degrees can be prepared by controlling the lithium addition amount, the cycling stability of the battery is improved, and the volume expansion of the electrode is relieved.

The invention relates to a doped modified argyrodite type solid electrolyte and a preparation method thereof, and belongs to the technical field of all-solid-state battery materials. The chemical formula of the electrolyte is Li < 5.5 + 2x + 2y > P < 1-x-y > Y < x > Bi < y > S < 4.5-1.5 x-1.5 y > O < 1.5 x + 1.5 y > Cl < 1.5 >, x is greater than or equal to 0.01 and less than or equal to 0.04, and y is greater than or equal to 0.01 and less than or equal to 0.04; the yttrium element and the bismuth element are doped at the P site of the argyrodite type electrolyte, and the oxygen element is doped at the S site of the argyrodite type electrolyte. After the argyrodite type electrolyte is in contact with metal lithium, an interface protection layer rich in lithium oxide can be formed in situ at an interface in a circulating process, so that lithium can be uniformly deposited, the generation of interface side reaction is inhibited, the interface stability of the argyrodite type electrolyte to a lithium metal negative electrode is improved, and the polarization voltage of a symmetrical battery is reduced; and the cycling stability of the all-solid-state lithium metal battery is enhanced.

The utility model provides an all-solid-state battery capable of preventing short circuit, and belongs to the technical field of all-solid-state batteries. The all-solid-state battery comprises a solid electrolyte layer, positive plates and negative plates, the positive plates and the negative plates are alternately stacked, the solid electrolyte layer is arranged between the positive plates and the negative plates, an insulating frame layer is further arranged between the positive plates and the negative plates, and the insulating frame layer is of a hollow quadrilateral frame structure. The inner frame is smaller than the positive plate, and the outer frame is larger than the positive plate. The lithium ion battery can prevent the structural integrity of the electrolyte layer from being damaged by the shearing effect generated by the edge of the pole piece under high voltage, so that the battery is short-circuited due to contact of the positive and negative pole pieces, the yield of the lithium ion battery is obviously improved, the short-circuit rate of the battery is reduced, and the cycle performance of the battery is improved.

A method for synergistically preparing lithium sulfide by vacuum molten salt based on hydrogen sulfide-lithium salt reaction belongs to the technical field of battery materials, and comprises the following steps: placing a lithium salt solid in a reactor, introducing a molten salt medium on the surface of the lithium salt or in a reaction system, introducing purified hydrogen sulfide gas under a vacuum auxiliary condition, controlling the reaction temperature to be 200-500 DEG C, and reacting for 1-2 hours; and adjusting the flow rate of hydrogen sulfide to be 50-1000mL / min and the retention time to be 5-180min, continuously exhausting gas to discharge water vapor in the reaction process, stopping introducing hydrogen sulfide gas after the reaction is finished, cooling the system to room temperature under the protection of inert gas, taking out the product, washing to remove residual fused salt, and carrying out vacuum drying to obtain the high-purity lithium sulfide. The prepared lithium sulfide has high purity (greater than or equal to 99.90%), low defect density and an excellent crystal structure, and can be widely applied to lithium-sulfur batteries, all-solid-state batteries and novel energy storage technologies, so that the energy density is improved, the cycle life is prolonged, and the energy consumption is reduced.

The invention discloses a high-performance lithium-rich manganese oxide positive electrode material, a preparation method thereof and application of the high-performance lithium-rich manganese oxide positive electrode material to an all-solid-state battery. The lithium-rich manganese oxide positive electrode material coats / composites a lithium-rich manganese positive electrode base material and a lithium ion conductor or a conductive agent in situ through a freeze-drying method. In-situ coating / compounding of a lithium ion conductor or a conductive agent on the lithium-rich manganese oxide positive electrode material is realized through freeze drying, the interface impedance is effectively reduced, the interface stability is improved, and the lithium ion and electron transmission efficiency is improved. The lithium-rich manganese oxide positive electrode material prepared by the invention can inhibit the release and side reaction of lattice oxygen in the cycle process, and improve the structural stability and cycle life of the material; meanwhile, the freeze-drying method can maintain the nano dispersity and uniformity of the material, full solid-solid contact between the lithium-rich manganese material and a lithium ion conductor or a conductive agent is realized, and the high specific capacity of the lithium-rich manganese positive electrode material in all-solid-state battery application is ensured. The prepared lithium-rich manganese-based all-solid-state battery has the reversible specific capacity as high as 273 mAh / g, the bottleneck that the capacity release of the lithium-rich manganese oxide positive electrode material in an all-solid-state battery system is limited is broken through, the strategy provides a new design thought and technical path for the construction of the high-specific-energy all-solid-state battery positive electrode material, the adopted process is simple and controllable, and the method is suitable for industrial production. The method is suitable for large-scale preparation.

The invention discloses a polycrystalline positive electrode material for a sulfide all-solid-state battery, a preparation method of the polycrystalline positive electrode material and a secondary battery, the surface of a high-nickel polycrystalline positive electrode material is coated with a conductive polymer in a surface coating manner, and an inorganic electrolyte is dispersed in the conductive polymer. According to the polycrystal positive electrode material for the sulfide all-solid-state battery, the stress generated by expansion of the high-nickel polycrystal positive electrode material is effectively relieved by utilizing the elasticity of the conductive polymer, the mechanical strength and durability of the material are enhanced, and the problem that the high-nickel polycrystal positive electrode material is easy to crack in the circulating process is effectively solved. In addition, the interfacial compatibility between the high-nickel polycrystalline positive electrode material subjected to coating modification treatment and the electrolyte is improved, the coated conductive polymer also has excellent electronic conductivity, the inorganic electrolyte can realize lithium ion transmission on a polymer chain segment, and the combined action of the two can improve the internal grain boundary conductivity of the polycrystal, so that the rate performance is improved.

The present application relates to a kind of full solid-state lithium ion membrane reactor with symmetrical structure and its application, the reactor is in situ construction on the both sides of solid-state lithium ion conductor film with Pt and / or Ni as catalyst, with single-walled carbon nanotube etc. Conductive material is used as current collector gas diffusion electrode, the reactor can work in nitrogen hydrogen mixture atmosphere, integration is high, scale is flexible.The present application changes the working mode of traditional reactor using liquid electrolyte, replaces inefficient nitrogen and proton mass transfer with efficient lithium ion mass transfer, couples lithium-mediated nitrogen reduction and hydrogen oxidation reaction to synthesize ammonia, and the maximum working current density is increased to 1000mA / cm 2 , and can work at 40mA / cm 2 Current density for a long time, with innovation and broad industrial application prospect.

Solid electrolyte compositions and solid-state batteries are disclosed, which comprise a solid electrolyte layer including a sulfide-containing solid-state electrolyte material and a compound of Chemical Formula 1. The sulfide-containing solid-state electrolyte material includes but is not limited to Li6PS5Cl (“LPSC”), an LPS-based glass or glass ceramic of formula xLi2S·yP2S5, wherein x+y=1, or an argyrodite-based sulfide-based solid electrolyte or formula Li6PS5X, wherein X═Cl, Br, or I) or Li6-yPS5-yCl1+y, where y is <1. In some aspects, the compound of Chemical Formula 1 is sodium 3-mercapto-1-propanesulfonate (3M1P).

The invention relates to the technical field of battery detection, and discloses an all-solid-state battery health state detection method based on electrochemical impedance spectroscopy. The method comprises the following steps: applying a dynamic mechanical modulation signal to a selected area on the surface of the all-solid-state battery, and simultaneously performing broadband electrochemical impedance spectroscopy measurement to obtain a time domain impedance signal; a multi-harmonic analysis is performed on the time-domain impedance signal to obtain at least one zero-order response, one-order response, and high-order harmonic response, and the state of health of the battery is evaluated based on these responses. According to the method, the zero-order response is associated with the conventional impedance, the first-order response is associated with the interface flexibility, and the high-order harmonic response is associated with the structural defect, so that the technical problems that different physical recession modes are difficult to distinguish and early mechanical structural risks cannot be effectively identified in the prior art are solved; the early failure risk of the battery can be identified, the local defect can be spatially positioned, and the accuracy, depth and foresight of health state assessment are improved.

The invention discloses an isostatic pressing device of an all-solid-state battery and a preparation method of the all-solid-state battery, the isostatic pressing device of the all-solid-state battery comprises a shell with an opening at the upper end and an upper cover, an isostatic pressing cavity is formed in the shell, the upper cover covers the upper end of the shell, a cylinder is arranged in the isostatic pressing cavity, and the upper cover covers the upper end of the shell. An all-solid-state battery and a conductive connecting piece used for being electrically connected with a tab of the all-solid-state battery are placed in the cylinder body, the cylinder body comprises a left half part, an insulating parting strip and a right half part, the left half part, the insulating parting strip and the right half part are sequentially connected, the left half part is electrically connected with the upper cover, and the insulating parting strip is electrically connected with the conductive connecting piece. The left half part is electrically connected with the shell, the right half part is electrically connected with the shell, an insulating sealing ring is arranged between the shell and the upper cover, and a tab of the all-solid-state battery is electrically connected with the left half part or the right half part through the conductive connecting piece; the device has the advantages that the isostatic pressing function and the in-situ formation function are achieved, the preparation process is shortened, and the production efficiency is improved.

The invention belongs to the technical field of all-solid-state sulfide lithium metal batteries, and relates to a lithium battery electrode containing an interface self-repairing coating as well as a preparation method and application of the lithium battery electrode. The electrode comprises a lithium metal negative electrode substrate and the interface self-repairing coating coated on the surface of the lithium metal negative electrode substrate, the interface self-repairing coating is internally provided with a dynamic reversible network, and the dynamic reversible network is constructed by disulfide bonds and hydrogen bonds. A layer of interface self-repairing coating is formed on the surface of a lithium metal negative electrode substrate to serve as a physical isolation barrier, metal lithium and sulfide electrolyte are isolated and prevented from being directly subjected to reduction reaction, and coating microcracks generated by volume change in lithium metal circulation can be repaired, so that the possibility of interface exposure caused by coating breakage is reduced, and the service life of the lithium metal negative electrode is prolonged. Meanwhile, good interface contact can be kept, the synergistic effect of stable interface impedance, lithium dendrite inhibition and long-term cycle performance improvement is achieved, and the long-term cycle stability of the all-solid-state lithium battery is improved.

The invention relates to the technical field of solid-state lithium ion batteries, in particular to a composite solid-state electrolyte diaphragm, a preparation method and an all-solid-state battery. According to the invention, a 3D ion / electron channel is constructed through a cellulose skeleton, an oxide electrolyte nanowire directional arrangement technology is adopted, and an in-situ interface lithium fluoride repairing layer is adopted, so that the industrialization bottleneck that high ion conduction-mechanical strength-interface stability is difficult to collaboratively optimize in the prior art is broken through; the common problems of insufficient bulk phase and interface ion conductivity, poor mechanical strength, poor compatibility with a high-nickel positive electrode / silicon carbon negative electrode and the like of a solid-state battery are effectively solved. The mass energy density of the prepared all-solid-state battery can reach 360 Wh / kg, the capacity retention ratio can still be maintained at 80% or above after 1100 times of circulation, and the all-solid-state battery successfully passes 190 DEG C thermal runaway and acupuncture tests and shows excellent safety performance and wide industrial application prospects.

The invention belongs to the technical field of lithium ion battery positive electrode material preparation, and relates to a manganese-based positive electrode of an all-solid-state battery system, a preparation method and application of the manganese-based positive electrode, the general formula of the manganese-based positive electrode is Li < 1 + x > NiyCoyMn3yOz, the preparation method comprises the following steps: S1, grinding and mixing a lithium-rich manganese original material and lithium phosphate in an inert gas protective atmosphere to obtain a precursor mixture; s2, performing high-energy mechanical ball milling on the precursor mixture; s3, collecting the powder subjected to high-energy mechanical ball milling in an inert gas protective atmosphere to obtain a manganese-based positive electrode material; the manganese-based positive electrode material disclosed by the invention realizes mixed arrangement of part of cations and a double-phase synergistic heterostructure, and has high energy density and voltage, and a halide and sulfide-based all-solid-state battery assembled by using the manganese-based positive electrode material shows good cycling stability and rate capability.

The invention discloses a composite positive electrode, a preparation method thereof and an all-solid-state battery. The composite positive electrode comprises a composite solid electrolyte and a positive electrode active material. The composite solid electrolyte comprises a first solid electrolyte and a second solid electrolyte, wherein the molecular structural formula of the first solid electrolyte is Li < 2 + > (4-a) < x > Zr < 1-x > A < x > Cl < 6-by > By; the second solid electrolyte is selected from one or more of sulfide solid electrolytes; the selection of the metal element A and the non-metal element B meets the condition that XIC * x + (1-x) * 1.687 is less than 1.6; and [(6-by) * 3.16 + y * Xp] / [(6-by + y) * (XIC * x + (1-x) * 1.687)] > = 1.9; wherein the valence state of the metal element A is + a, and the valence state of the non-metal element B is-b; xIC represents the electronegativity of the metal element A, and Xp represents the electronegativity of the non-metal element B. According to the invention, the material forming the composite positive electrode is selected based on the electronegativity of the contained elements, so that the stability and the electrical performance are improved.

The invention discloses a high-entropy oxide composite negative electrode material as well as a preparation method and application thereof, and relates to the technical field of all-solid-state lithium battery negative electrode materials, and the high-entropy oxide composite negative electrode material comprises a metal element and an oxygen element, the high-entropy oxide composite negative electrode material comprises a metal element and an oxygen element, wherein the metal elements are at least five of a chromium element, an iron element, a nickel element, a manganese element, a molybdenum element, a copper element and a cerium element; the molar ratio of the metal element to the oxygen element is 3: 4; the high-entropy oxide composite negative electrode material is of a spinel structure. According to the prepared high-entropy oxide composite negative electrode material, the problems that a traditional negative electrode material is unstable in structure, poor in interface contact and short in cycle life are solved, the electrochemical performance is improved, and an all-solid-state lithium battery prepared from the high-entropy oxide composite negative electrode material shows high reversible specific capacity and excellent cycle stability.