CN112133955B - Cell structure of solid-state battery and preparation method thereof - Google Patents
Cell structure of solid-state battery and preparation method thereofDownload PDFInfo
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- CN112133955B CN112133955BCN202011043360.1ACN202011043360ACN112133955BCN 112133955 BCN112133955 BCN 112133955BCN 202011043360 ACN202011043360 ACN 202011043360ACN 112133955 BCN112133955 BCN 112133955B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
- H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
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Abstract
Translated fromChinese
Description
Technical Field
The invention belongs to the technical field of battery cells, and relates to a cell structure of a solid-state battery and a preparation method thereof.
Background
A solid-state battery, also known as an all solid-state lithium battery, is an energy storage device that, relative to a liquid-state lithium battery, contains no liquid in its structure and all materials are present in solid form. Specifically, the lithium ion battery consists of a positive electrode material, a negative electrode material and an electrolyte, and the liquid lithium battery consists of the positive electrode material, the negative electrode material, the electrolyte and a diaphragm. The solid-state battery adopts non-flammable solid-state battery electrolyte to replace flammable organic liquid electrolyte, so that the safety of a battery system is greatly improved, the high-energy anode and cathode can be better adapted, the weight of the system is reduced, and the synchronous improvement of energy density is realized. Among various new battery systems, solid-state batteries are the next-generation technology closest to the industry, which has become a consensus of the industry and the scientific community.
In order to solve the problems of increased conduction path and limited conduction of electrons in thick electrodes in solid-state batteries, more conductive carbon is added into a positive electrode coating to solve the problems. However, this method has significant drawbacks: (1) the conductive carbon is nano powder particles, is difficult to uniformly disperse in the anode slurry, and is easy to form agglomeration particularly when the content is increased, so that a conductive network cannot be well constructed, and the electronic conductivity is reduced. (2) Solid electrolytes such as sulfide electrolytes used in solid-state batteries are unstable at high pressure, and particularly, when in contact with conductive carbon, they are more likely to undergo decomposition reaction at high pressure to cause a decrease in the ionic conductivity of the sulfide electrolyte; when more conductive carbon is added to the positive electrode sheet, it causes rapid deterioration of the contact section of the solid electrolyte and the conductive carbon, and rather, the battery performance is significantly degraded. (3) The increase of the conductive carbon content inevitably occupies the proportion of other substances in the positive pole piece: a reduction in the proportion of the positive electrode active material leads to a reduction in the energy that can be emitted, which in turn leads to a reduction in the overall energy density of the battery; the decrease of the content of the solid electrolyte can cause that an ion conductive network in the positive pole piece can not be well constructed, and the ion conduction limited energy can not be normally exerted.
CN108695548A discloses a stacked all-solid-state battery including a plurality of all-solid-state batteries each having: a positive electrode layer having a positive electrode current collector and a positive electrode active material layer containing a positive electrode active material formed on the positive electrode current collector; a negative electrode layer having a negative electrode current collector and a negative electrode active material layer containing a negative electrode active material formed on the negative electrode current collector; and a solid electrolyte layer which is disposed between the positive electrode active material layer and the negative electrode active material layer and contains a solid electrolyte having lithium ion conductivity.
CN108695558A discloses an all-solid battery cell, which comprises a positive electrode current collector, an integrated electrode and a negative electrode current collector, wherein the integrated electrode is located between the positive electrode current collector and the negative electrode current collector.
CN104919628A discloses an all-solid battery comprising a negative electrode layer, a positive electrode layer, a solid electrolyte layer disposed between the positive electrode layer and the negative electrode layer, a negative electrode current collector connected to the negative electrode layer, the negative electrode current collector containing a sulfide solid electrolyte, the negative electrode current collector containing a metal that reacts with the sulfide solid electrolyte, and a positive electrode current collector connected to the positive electrode layer, with a sulfur compound-containing layer being present between the negative electrode layer and the negative electrode current collector.
In the conventional method, in order to solve the problems of increased conduction path and limited conduction of electrons in a thick electrode in a solid-state battery, more conductive carbon is added into a positive electrode coating at present, but the method has obvious defects, and in order to better solve the technical problems, optimization and improvement of the structure of the existing solid-state battery are urgently needed.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a cell structure of a solid-state battery and a preparation method thereof.
In order to achieve the purpose, the invention adopts the following technical scheme:
the invention provides a cell structure of a solid-state battery, which comprises a positive pole piece, an electrolyte layer and a negative pole piece which are sequentially stacked, wherein the positive pole piece comprises a positive coating and a positive current collector which are sequentially stacked from the surface of the electrolyte layer, and the negative pole piece comprises a negative coating and a negative current collector which are sequentially stacked from the surface of the electrolyte layer.
The battery core structure also comprises a positive electrode porous electric conductor and/or a negative electrode porous electric conductor.
The positive porous conductor comprises a positive porous layer clamped between a positive pole piece and an electrolyte layer and at least one positive protruding part vertically fixed on the positive porous layer, and the positive protruding part penetrates through the positive coating and is inserted into the positive current collector.
The negative porous conductor comprises a negative porous layer clamped between the negative pole piece and the electrolyte layer, and at least one negative protruding part vertically fixed on the negative porous layer, wherein the negative protruding part penetrates through the negative coating and is inserted into the negative current collector.
In the traditional method, in order to solve the problems of increase of conduction paths and limited conduction of electrons in a thick electrode in a solid-state battery, more conductive carbon is added in a positive electrode coating to solve the problems. However, the method has obvious defects, most obviously, the conductive carbon is nano powder particles, and is difficult to uniformly disperse in the anode slurry, and particularly, when the content is increased, the conductive carbon is easy to form agglomeration, so that a conductive network cannot be well constructed, and the electronic conductivity is reduced. According to the invention, the positive porous conductor and/or the negative porous conductor are arranged, so that the cell structure of the all-solid-state battery is optimized, the electronic conduction network in the pole piece is optimized, the transmission path of electrons in the pole piece is reduced, the polarization phenomenon caused by limited electronic conduction in the positive pole piece is reduced on the premise of not increasing the content of conductive carbon in the pole piece, and the problem of easy agglomeration when the content of the conductive carbon is increased is solved.
Further, the present invention embeds a positive porous conductor composed of a positive porous layer and a positive protruding portion between the positive coating and the electrolyte layer, and/or embeds a negative porous conductor composed of a negative porous layer and a negative protruding portion between the negative coating and the electrolyte layer, the positive porous conductor and the negative porous conductor are collectively called porous conductors, and the porous conductors mainly function as: (1) the protruding part in the porous electric conductor penetrates through the coating and is directly contacted with the current collector; the material of the porous electric conductor is a good conductor of electrons, so that the current collector and the porous electric conductor have almost the same potential, and electrons can be rapidly transferred between the current collector and the porous electric conductor; (2) run through by many protruding portions in the coating, can make coating and protruding portion fully contact, be favorable to the electron in the coating to transmit to the mass flow body fast more in, and then reduce the polarization phenomenon because of electron conduction is smooth and easy to lead to.
It should be noted that there are three different parallel technical solutions in the present invention, specifically including:
firstly, the cell structure only comprises a positive porous conductor between a positive pole piece and an electrolyte layer, and does not comprise a negative porous conductor;
secondly, the cell structure only comprises a negative porous conductor between the negative pole piece and the electrolyte layer, and does not comprise a positive porous conductor;
and thirdly, the battery cell structure simultaneously comprises a positive porous conductor and a negative porous conductor.
In a preferred embodiment of the present invention, the material of the positive electrode porous conductor and the negative electrode porous conductor is stainless steel.
Preferably, the porous structures of the positive electrode porous layer and the negative electrode porous layer are diamond-shaped grid structures.
In a preferred embodiment of the present invention, the thickness of the positive electrode porous layer and the negative electrode porous layer is 10 to 100 μm, and may be, for example, 10 μm, 20 μm, 40 μm, 50 μm, 60 μm, 70 μm, 80 μm, 90 μm or 100 μm, and is not limited to the above-mentioned values, and other values not mentioned in the above-mentioned range are also applicable.
Preferably, the thickness of the positive electrode porous layer is the same as or different from that of the negative electrode porous layer.
Preferably, the pore diameters of the positive electrode porous layer and the negative electrode porous layer are 0.355 to 12.5mm, and may be, for example, 0.3mm, 0.5mm, 1mm, 1.5mm, 2mm, 2.5mm, 3mm, 3.5mm, 4mm, 4.5mm, 5mm, 5.5mm, 6mm, 6.5mm, 7mm, 7.5mm, 8mm, 8.5mm, 9mm, 9.5mm, 10mm, 10.5mm, 11mm, 11.5mm, 12mm, or 12.5mm, and are not limited to the values listed, and other values not listed in the range of the values are also applicable.
Preferably, the pore diameter of the positive electrode porous layer is the same as or different from that of the negative electrode porous layer.
Preferably, the mesh number of the positive electrode porous layer and the negative electrode porous layer is 2 to 50 mesh, for example, 2 mesh, 5 mesh, 10 mesh, 15 mesh, 20 mesh, 25 mesh, 30 mesh, 35 mesh, 40 mesh, 45 mesh or 50 mesh, and is not limited to the above-mentioned numerical values, and other non-mentioned numerical values in this numerical value range are also applicable.
Preferably, the mesh number of the positive electrode porous layer is the same as or different from that of the negative electrode porous layer.
In the invention, the positive porous layer and the negative porous layer are both porous structures, so that the electrolyte layer can respectively penetrate through the through holes on the positive porous layer/the negative porous layer to be directly contacted with the positive pole piece/the negative pole piece after being compacted by external pressure, and the ion transmission path between the pole piece and the electrolyte layer is not influenced.
In a preferred embodiment of the present invention, the length of the positive electrode protrusion is 1 to 5 μm greater than the thickness of the positive electrode coating layer, and may be, for example, 1.0 μm, 1.5 μm, 2.0 μm, 2.5 μm, 3.0 μm, 3.5 μm, 4.0 μm, 4.5 μm or 5.0 μm, and is not limited to the above-mentioned values, and other values not listed in the above-mentioned range of values are also applicable.
Preferably, the length of the negative electrode protrusion is 1 to 5 μm greater than the thickness of the negative electrode coating, and may be, for example, 1.0 μm, 1.5 μm, 2.0 μm, 2.5 μm, 3.0 μm, 3.5 μm, 4.0 μm, 4.5 μm, or 5.0 μm, and is not limited to the values listed, and other values not listed in the range of the values are also applicable.
Preferably, the length of the positive electrode protrusion is the same as or different from that of the negative electrode protrusion.
In a preferred embodiment of the present invention, the positive electrode protrusions are arranged on the positive electrode porous layer in a matrix form, and the negative electrode protrusions are arranged on the negative electrode porous layer in a matrix form.
Preferably, the positive and negative protrusions are arranged at a density of 2 to 50 per square inch, for example, 2, 5, 10, 15, 20, 25, 30, 35, 40, 45, or 50 per square inch, and are not limited to the values listed, and other values not listed in this range are also applicable.
Preferably, the arrangement density of the positive electrode protrusions is the same as or different from that of the negative electrode protrusions.
In a preferred embodiment of the present invention, the distance between two adjacent positive electrode protrusions is 0.355 to 12.5mm, for example, 0.355mm, 0.5mm, 1mm, 1.5mm, 2mm, 2.5mm, 3mm, 3.5mm, 4mm, 4.5mm, 5mm, 5.5mm, 6mm, 6.5mm, 7mm, 7.5mm, 8mm, 8.5mm, 9mm, 9.5mm, 10mm, 10.5mm, 11mm, 11.5mm, 12mm, or 12.5mm, and is not limited to the values listed, and other values not listed in the range of the values are also applicable.
Preferably, the distance between two adjacent negative electrode protrusions is 0.355 to 12.5mm, for example, 0.355mm, 0.5mm, 1mm, 1.5mm, 2mm, 2.5mm, 3mm, 3.5mm, 4mm, 4.5mm, 5mm, 5.5mm, 6mm, 6.5mm, 7mm, 7.5mm, 8mm, 8.5mm, 9mm, 9.5mm, 10mm, 10.5mm, 11mm, 11.5mm, 12mm, or 12.5mm, and is not limited to the enumerated values, and other non-enumerated values in the numerical range are also applicable.
Preferably, the distance between two adjacent positive electrode protrusions is the same as or different from the distance between two adjacent negative electrode protrusions.
In the present invention, the positive/negative porous conductors (collectively referred to as porous conductors) should have the following characteristics: (1) a good conductor of electrons, so that the electrons can be rapidly transferred between the current collector and the porous conductor; (2) the porous conductor has high mechanical strength, so that the porous conductor can be penetrated into the positive electrode coating or the negative electrode coating under the action of external pressure, and the porous conductor is preferably made of metal; (3) the porous electrical conductor should have good machinability; (4) the porous conductor is made of a material which is stable in electrochemistry and can stably exist with an electrolyte, so the material of the porous conductor is more preferably stainless steel; (5) the length of the protruding part in the porous electric conductor should be larger than the thickness of the pole piece coating, so that the protruding part can penetrate into the positive current collector and be in contact with the current collector.
In a preferred embodiment of the present invention, the thickness of the positive electrode current collector is 6 to 15 μm, and may be, for example, 6 μm, 7 μm, 8 μm, 9 μm, 10 μm, 11 μm, 12 μm, 13 μm, 14 μm or 15 μm, and is not limited to the above-mentioned values, and other values not listed in the above-mentioned range are also applicable.
Preferably, the thickness of the positive electrode coating is 50 to 150 μm, for example, 50 μm, 60 μm, 70 μm, 80 μm, 90 μm, 100 μm, 110 μm, 120 μm, 130 μm, 140 μm or 150 μm, and is not limited to the values listed, and other values not listed in the range of the values are also applicable.
Preferably, the thickness of the negative electrode coating is 15 to 80 μm, for example, 15 μm, 20 μm, 25 μm, 30 μm, 35 μm, 40 μm, 45 μm, 50 μm, 55 μm, 60 μm, 65 μm, 70 μm, 75 μm or 80 μm, and is not limited to the values listed, and other values not listed in the range of the values are also applicable.
Preferably, the thickness of the negative electrode current collector is 6 to 15 μm, and may be, for example, 6 μm, 7 μm, 8 μm, 9 μm, 10 μm, 11 μm, 12 μm, 13 μm, 14 μm or 15 μm, and is not limited to the above-mentioned values, and other values not listed in the above-mentioned range are also applicable.
In a second aspect, the invention provides a method for preparing the battery cell structure of the first aspect, where the battery cell structure is prepared by any one of the following preparation methods:
the preparation method comprises the following steps: the positive pole piece is pressed towards the free end of the positive protruding part, and the free end of the positive protruding part penetrates through the positive coating and is inserted into the positive current collector; the electrolyte layer is superposed on the plane side of the positive porous layer, and the electrolyte layer is embedded into the pores of the positive porous layer after pressurization; stacking the negative pole piece on the surface of one side of the electrolyte layer, which is far away from the positive pole piece, and preparing a battery core structure comprising a positive porous conductor;
the second preparation method comprises the following steps: the negative pole piece is pressed into the free end of the negative protruding part, and the free end of the negative protruding part penetrates through the negative coating and is inserted into the negative current collector; the electrolyte layer is superposed on the plane side of the negative porous layer, and the electrolyte layer is embedded into the pores of the negative porous layer after pressurization; stacking the positive pole piece on the surface of one side of the electrolyte layer, which is far away from the negative pole piece, and preparing a battery core structure comprising a negative pole porous conductor;
the preparation method comprises the following steps: the positive pole piece is pressed towards the free end of the positive protruding part, and the free end of the positive protruding part penetrates through the positive coating and is inserted into the positive current collector; the negative pole piece is pressed into the free end of the negative protruding part, and the free end of the negative protruding part penetrates through the negative coating and is inserted into the negative current collector; and respectively superposing the plane side of the anode porous layer and the plane layer of the cathode porous layer on the surfaces of the two sides of the electrolyte layer, and pressurizing to obtain the battery core structure comprising the anode porous conductor and the cathode porous conductor.
In a preferred embodiment of the present invention, the pressure applied to press the positive electrode tab into the positive electrode protrusion is 450 to 550MPa, for example, 450MPa, 460MPa, 470MPa, 480MPa, 490MPa, 500MPa, 510MPa, 520MPa, 530MPa, 540MPa or 550MPa, and is not limited to the above-mentioned values, and other values not shown in the above-mentioned numerical range are also applicable.
Preferably, the pressure applied to press the negative electrode tab into the negative electrode protrusion is 450 to 550MPa, for example, 450MPa, 460MPa, 470MPa, 480MPa, 490MPa, 500MPa, 510MPa, 520MPa, 530MPa, 540MPa or 550MPa, and is not limited to the above-mentioned values, and other values not mentioned in the above-mentioned range are also applicable.
In a preferred embodiment of the present invention, the pressurizing pressure is 150 to 250MPa, and may be, for example, 150MPa, 160MPa, 170MPa, 180MPa, 190MPa, 200MPa, 210MPa, 220MPa, 230MPa, 240MPa or 250MPa, and is not limited to the above-mentioned values, and other values not listed in the above-mentioned range are also applicable.
It should be noted that the cell structure provided by the present invention has three optional structural forms (that is, only includes the positive porous conductor, only includes the negative porous conductor, and includes both the positive porous conductor and the negative porous conductor), and correspondingly, the preparation methods of different structural forms are also different, taking the preparation of the cell structure including both the positive porous conductor and the negative porous conductor as an example, the preparation method of the cell structure is as follows:
(1) the free end of the positive electrode protruding part faces the positive electrode piece, and the positive electrode piece is pressed into the positive electrode protruding part through an external pressure of 450-550 MPa, so that the positive electrode protruding part penetrates through the positive electrode coating and is inserted into the positive electrode current collector;
(2) superposing the electrolyte layer on the plane side of the porous layer of the positive electrode, applying an external pressure of 150-250 MPa, and embedding the electrolyte layer into pores of the porous layer of the positive electrode;
(3) the free end of the negative electrode protruding portion faces the negative electrode plate, and the negative electrode plate is pressed into the negative electrode protruding portion through an external pressure of 450-550 MPa, so that the negative electrode protruding portion penetrates through the negative electrode coating and is inserted into the negative electrode current collector;
(4) and (3) superposing the negative pole piece embedded with the negative porous conductor in the step (3) on one side of the electrolyte layer obtained in the step (2), enabling the plane side of the negative porous layer to be tightly attached to the surface of the solid electrolyte, applying an external pressure of 150-250 MPa, and embedding the electrolyte layer into pores of the negative porous layer to prepare the cell structure comprising the positive porous conductor and the negative porous conductor.
Compared with the prior art, the invention has the beneficial effects that:
the invention optimizes the cell structure of the all-solid-state battery by arranging the positive porous electric conductor and/or the negative porous electric conductor, optimizes the electronic conduction network in the pole piece, reduces the transmission path of electrons in the pole piece and reduces the polarization phenomenon caused by limited electronic conduction in the positive pole piece on the premise of not increasing the content of conductive carbon in the pole piece.
Drawings
Fig. 1 is a schematic diagram of a cell structure provided inembodiment 1 of the present invention;
fig. 2 is a schematic diagram of a cell structure provided inembodiment 2 of the present invention;
fig. 3 is a schematic diagram of a cell structure provided inembodiment 3 of the present invention;
fig. 4 is a graph of first cycle voltage-gram capacity of all-solid-state batteries provided in example 7 of the present invention, comparative example 1 and comparative example 2;
fig. 5 is a graph showing a cycle-capacity relationship of all-solid batteries provided in example 7 of the present invention, comparative example 1 and comparative example 2;
wherein, 1-positive electrode current collector; 2-positive coating; 3-an electrolyte layer; 4-coating the negative electrode; 5-negative current collector; 6-a porous layer of positive electrode; 7-positive electrode tab; 8-a negative porous layer; 9-negative electrode tab.
Detailed Description
It is to be understood that in the description of the present invention, the terms "center", "longitudinal", "lateral", "up", "down", "front", "back", "left", "right", "vertical", "horizontal", "top", "bottom", "inner", "outer", etc., indicate orientations or positional relationships based on those shown in the drawings, and are used only for convenience in describing the present invention and for simplicity in description, and do not indicate or imply that the device or element being referred to must have a particular orientation, be constructed and operated in a particular orientation, and thus, should not be taken as limiting the present invention. Furthermore, the terms "first", "second", etc. are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first," "second," etc. may explicitly or implicitly include one or more of that feature. In the description of the present invention, "a plurality" means two or more unless otherwise specified.
It should be noted that, in the description of the present invention, unless otherwise explicitly specified or limited, the terms "disposed," "connected" and "connected" are to be construed broadly, and may be, for example, fixedly connected, detachably connected, or integrally connected; can be mechanically or electrically connected; they may be connected directly or indirectly through intervening media, or they may be interconnected between two elements. The specific meaning of the above terms in the present invention can be understood by those of ordinary skill in the art through specific situations.
The technical scheme of the invention is further explained by the specific implementation mode in combination with the attached drawings.
Example 1
The embodiment provides a cell structure of a solid-state battery as shown in fig. 1, where the cell structure includes a positive electrode plate, anelectrolyte layer 3, and a negative electrode plate, which are sequentially stacked. A positive porous conductor is arranged between the positive pole piece and theelectrolyte layer 3, the positive porous conductor is partially embedded into the positive pole piece, and the positive porous conductor is made of stainless steel.
The positive pole piece comprises apositive pole coating 2 and a positive polecurrent collector 1 which are sequentially stacked on the surface of anelectrolyte layer 3, and the negative pole piece comprises anegative pole coating 4 and a negative polecurrent collector 5 which are sequentially stacked on the surface of theelectrolyte layer 3. The thickness of the positive electrodecurrent collector 1 was 6 μm, the thickness of thepositive electrode coating 2 was 50 μm, the thickness of thenegative electrode coating 4 was 15 μm, and the thickness of the negative electrodecurrent collector 5 was 6 μm. The positive porous conductor comprises a positiveporous layer 6 clamped between the positive pole piece and theelectrolyte layer 3 and at least one positive protruding part 7 vertically fixed on the positiveporous layer 6, wherein the positive protruding part 7 penetrates through thepositive coating 2 and then is inserted into the positivecurrent collector 1.
The thickness of theporous layer 6 of the positive electrode is 10 μm, and the porous structure is a diamond grid structure. The aperture is 0.355 mm. The length of the positive electrode protrusion 7 is 1 μm greater than the thickness of thepositive electrode coating 2. The positive electrode protruding parts 7 are arranged on the positive electrodeporous layer 6 in a matrix mode, the arrangement density of the positive electrode protruding parts 7 is 2 per square inch, and the distance between every two adjacent positive electrode protruding parts 7 is 12.5 mm.
The embodiment also provides a preparation method of the battery cell structure, and the preparation method comprises the following steps:
(1) the positive pole piece is pressed in towards the free end of the positiveprotruding part 9 under the external pressure of 450MPa, and the free end of the positiveprotruding part 9 penetrates through thepositive coating 2 and is inserted into the positivecurrent collector 1;
(2) theelectrolyte layer 3 is superposed on the plane side of the positive electrodeporous layer 6, and theelectrolyte layer 3 is embedded into the pores of the positive electrodeporous layer 6 after external pressure of 150MPa is applied;
(3) and the negative pole piece is stacked on the surface of one side of theelectrolyte layer 3 away from the positive pole piece, and the battery core structure comprising the positive porous conductor is prepared.
Example 2
The embodiment provides a cell structure of a solid-state battery as shown in fig. 1, where the cell structure includes a positive electrode plate, anelectrolyte layer 3, and a negative electrode plate, which are sequentially stacked. A positive porous conductor is arranged between the positive pole piece and theelectrolyte layer 3, the positive porous conductor is partially embedded into the positive pole piece, and the positive porous conductor is made of stainless steel.
The positive pole piece comprises apositive pole coating 2 and a positive polecurrent collector 1 which are sequentially stacked on the surface of anelectrolyte layer 3, and the negative pole piece comprises anegative pole coating 4 and a negative polecurrent collector 5 which are sequentially stacked on the surface of theelectrolyte layer 3. The thickness of the positive electrodecurrent collector 1 was 8 μm, the thickness of thepositive electrode coating 2 was 70 μm, the thickness of thenegative electrode coating 4 was 30 μm, and the thickness of the negative electrodecurrent collector 5 was 8 μm. The positive porous conductor comprises a positiveporous layer 6 clamped between the positive pole piece and theelectrolyte layer 3 and at least one positive protruding part 7 vertically fixed on the positiveporous layer 6, wherein the positive protruding part 7 penetrates through thepositive coating 2 and then is inserted into the positivecurrent collector 1.
The thickness of theporous layer 6 of the positive electrode is 100 μm, and the porous structure is a diamond grid structure. The aperture is 12.5 mm. The length of the positive electrode tab 7 is 5 μm greater than the thickness of thepositive electrode coating 2. The positive electrode protruding parts 7 are arranged on the positive electrodeporous layer 6 in a matrix manner, the arrangement density of the positive electrode protruding parts 7 is 50 per square inch, and the distance between every two adjacent positive electrode protruding parts 7 is 0.355 mm.
The embodiment also provides a preparation method of the battery cell structure, and the preparation method comprises the following steps:
(1) the positive pole piece is pressed in towards the free end of the positiveprotruding part 9 under the external pressure of 550MPa, and the free end of the positiveprotruding part 9 penetrates through thepositive coating 2 and is inserted into the positivecurrent collector 1;
(2) theelectrolyte layer 3 is superposed on the plane side of the positive electrodeporous layer 6, and theelectrolyte layer 3 is embedded into the pores of the positive electrodeporous layer 6 after external pressure of 250MPa is applied;
(3) and the negative pole piece is stacked on the surface of one side of theelectrolyte layer 3 away from the positive pole piece, and the battery core structure comprising the positive porous conductor is prepared.
Example 3
The embodiment provides a cell structure of a solid-state battery as shown in fig. 2, where the cell structure includes a positive electrode plate, anelectrolyte layer 3, and a negative electrode plate, which are sequentially stacked. A negative porous conductor is arranged between the negative pole piece and theelectrolyte layer 3, the negative porous conductor is partially embedded into the negative pole piece, and the negative porous conductor is made of stainless steel.
The positive pole piece comprises apositive pole coating 2 and a positive polecurrent collector 1 which are sequentially stacked on the surface of anelectrolyte layer 3, and the negative pole piece comprises anegative pole coating 4 and a negative polecurrent collector 5 which are sequentially stacked on the surface of theelectrolyte layer 3. The thickness of the positive electrodecurrent collector 1 was 10 μm, the thickness of thepositive electrode coating 2 was 90 μm, the thickness of thenegative electrode coating 4 was 45 μm, and the thickness of the negative electrodecurrent collector 5 was 10 μm. The negative porous conductor comprises a negativeporous layer 8 sandwiched between the negative pole piece and theelectrolyte layer 3, and at least one negativeprotruding part 9 vertically fixed on the negativeporous layer 8, wherein the negativeprotruding part 9 penetrates through thenegative coating 4 and then is inserted into the negativecurrent collector 5.
The thickness of the negative electrodeporous layer 8 is 10 μm, and the porous structure is a diamond grid structure. The pore diameter of the negative electrodeporous layer 8 was 0.355 mm. The length of thenegative electrode protrusion 9 is 1 μm greater than the thickness of thenegative electrode coating 4. The negativeelectrode protruding parts 9 are arranged on the negative electrodeporous layer 8 in a matrix mode, the arrangement density of the negativeelectrode protruding parts 9 is 2 per square inch, and the distance between every two adjacent negativeelectrode protruding parts 9 is 12.5 mm.
The embodiment also provides a preparation method of the battery cell structure, and the preparation method comprises the following steps:
(1) the negative pole piece is pressed in towards the free end of the negative protruding part 7 under the external pressure of 500MPa, and the free end of the negative protruding part 7 penetrates through thenegative coating 4 and is inserted into the negativecurrent collector 5;
(2) theelectrolyte layer 3 is superposed on the plane side of the negative electrodeporous layer 8, and theelectrolyte layer 3 is embedded into the pores of the negative electrodeporous layer 8 after external pressure of 200MPa is applied;
(3) and the positive pole piece is stacked on the surface of one side of theelectrolyte layer 3 away from the negative pole piece, and the battery core structure comprising the negative pole porous conductor is prepared.
Example 4
The embodiment provides a cell structure of a solid-state battery as shown in fig. 2, where the cell structure includes a positive electrode plate, anelectrolyte layer 3, and a negative electrode plate, which are sequentially stacked. A negative porous conductor is arranged between the negative pole piece and theelectrolyte layer 3, the negative porous conductor is partially embedded into the negative pole piece, and the negative porous conductor is made of stainless steel.
The positive pole piece comprises apositive pole coating 2 and a positive polecurrent collector 1 which are sequentially stacked on the surface of anelectrolyte layer 3, and the negative pole piece comprises anegative pole coating 4 and a negative polecurrent collector 5 which are sequentially stacked on the surface of theelectrolyte layer 3. The thickness of the positive electrodecurrent collector 1 was 12 μm, the thickness of thepositive electrode coating 2 was 110 μm, the thickness of thenegative electrode coating 4 was 60 μm, and the thickness of the negative electrodecurrent collector 5 was 12 μm. The negative porous conductor comprises a negativeporous layer 8 sandwiched between the negative pole piece and theelectrolyte layer 3, and at least one negativeprotruding part 9 vertically fixed on the negativeporous layer 8, wherein the negativeprotruding part 9 penetrates through thenegative coating 4 and then is inserted into the negativecurrent collector 5.
The thickness of the negative electrodeporous layer 8 is 100 μm, and the porous structure is a diamond grid structure. The pore diameter of the negative electrodeporous layer 8 was 12.5 mm. The length of thenegative electrode protrusion 9 is 5 μm greater than the thickness of thenegative electrode coating 4. The negativeelectrode protruding parts 9 are arranged on the negative electrodeporous layer 8 in a matrix manner, the arrangement density of the negativeelectrode protruding parts 9 is 50 per square inch, and the distance between every two adjacent negativeelectrode protruding parts 9 is 0.355 mm.
The embodiment also provides a preparation method of the battery cell structure, and the preparation method comprises the following steps:
(1) the negative pole piece is pressed in towards the free end of the negative protruding part 7 under the external pressure of 450MPa, and the free end of the negative protruding part 7 penetrates through thenegative coating 4 and is inserted into the negativecurrent collector 5;
(2) theelectrolyte layer 3 is superposed on the plane side of the negative electrodeporous layer 8, and theelectrolyte layer 3 is embedded into the pores of the negative electrodeporous layer 8 after external pressure of 150MPa is applied;
(3) and the positive pole piece is stacked on the surface of one side of theelectrolyte layer 3 away from the negative pole piece, and the battery core structure comprising the negative pole porous conductor is prepared.
Example 5
The embodiment provides a cell structure of a solid-state battery as shown in fig. 3, where the cell structure includes a positive electrode plate, anelectrolyte layer 3, and a negative electrode plate, which are sequentially stacked. A positive porous conductor is arranged between the positive pole piece and theelectrolyte layer 3, a negative porous conductor is arranged between the negative pole piece and theelectrolyte layer 3, the positive porous conductor is partially embedded into the positive pole piece, the negative porous conductor is partially embedded into the negative pole piece, and the positive porous conductor and the negative porous conductor are both made of stainless steel.
The positive pole piece comprises apositive pole coating 2 and a positive polecurrent collector 1 which are sequentially stacked on the surface of anelectrolyte layer 3, and the negative pole piece comprises anegative pole coating 4 and a negative polecurrent collector 5 which are sequentially stacked on the surface of theelectrolyte layer 3. The thickness of the positive electrodecurrent collector 1 was 14 μm, the thickness of thepositive electrode coating 2 was 130 μm, the thickness of thenegative electrode coating 4 was 75 μm, and the thickness of the negative electrodecurrent collector 5 was 14 μm. The positive porous conductor comprises a positiveporous layer 6 clamped between the positive pole piece and theelectrolyte layer 3 and at least one positive protruding part 7 vertically fixed on the positiveporous layer 6, wherein the positive protruding part 7 penetrates through thepositive coating 2 and then is inserted into the positivecurrent collector 1. The negative porous conductor comprises a negativeporous layer 8 sandwiched between the negative pole piece and theelectrolyte layer 3, and at least one negativeprotruding part 9 vertically fixed on the negativeporous layer 8, wherein the negativeprotruding part 9 penetrates through thenegative coating 4 and then is inserted into the negativecurrent collector 5.
The thickness of the positive electrodeporous layer 6 and the negative electrodeporous layer 8 was 50 μm, and the porous structures of the positive electrodeporous layer 6 and the negative electrodeporous layer 8 were diamond-mesh structures. The pore diameters of the positive electrodeporous layer 6 and the negative electrodeporous layer 8 were 5.5 mm. The length of the positive electrode tab 7 is 4.5 μm greater than the thickness of thepositive electrode coating 2, and the length of thenegative electrode tab 9 is 4.5 μm greater than the thickness of thenegative electrode coating 4. The positive electrode tabs 7 are arranged in a matrix on the positive electrodeporous layer 6, and thenegative electrode tabs 9 are arranged in a matrix on the negative electrodeporous layer 8. The arrangement density of the positive electrode protruding parts 7 and the negativeelectrode protruding parts 9 is 30 per square inch, the distance between two adjacent positive electrode protruding parts 7 is 5.5mm, and the distance between two adjacent negativeelectrode protruding parts 9 is 5.5 mm.
The embodiment also provides a preparation method of the battery cell structure, and the preparation method comprises the following steps:
(1) the positive pole piece is pressed in towards the free end of the positiveprotruding part 9 under the external pressure of 500MPa, and the free end of the positiveprotruding part 9 penetrates through thepositive coating 2 and is inserted into the positivecurrent collector 1;
(2) the negative pole piece is pressed in towards the free end of the negative protruding part 7 under the external pressure of 500MPa, and the free end of the negative protruding part 7 penetrates through thenegative coating 4 and is inserted into the negativecurrent collector 5;
(3) the plane side of the positiveporous layer 6 and the plane layer of the negativeporous layer 8 are respectively superposed on the surfaces of the two sides of theelectrolyte layer 3, and after external pressure of 200MPa is applied, the surfaces of the two sides of theelectrolyte layer 3 are respectively partially embedded into the positiveporous layer 6 and the negativeporous layer 8, so that the battery core structure comprising the positive porous conductor and the negative porous conductor is prepared.
Example 6
The embodiment provides a cell structure of a solid-state battery as shown in fig. 3, where the cell structure includes a positive electrode plate, anelectrolyte layer 3, and a negative electrode plate, which are sequentially stacked. A positive porous conductor is arranged between the positive pole piece and theelectrolyte layer 3, a negative porous conductor is arranged between the negative pole piece and theelectrolyte layer 3, the positive porous conductor is partially embedded into the positive pole piece, the negative porous conductor is partially embedded into the negative pole piece, and the positive porous conductor and the negative porous conductor are both made of stainless steel.
The positive pole piece comprises apositive pole coating 2 and a positive polecurrent collector 1 which are sequentially stacked on the surface of anelectrolyte layer 3, and the negative pole piece comprises anegative pole coating 4 and a negative polecurrent collector 5 which are sequentially stacked on the surface of theelectrolyte layer 3. The thickness of the positive electrodecurrent collector 1 was 15 μm, the thickness of thepositive electrode coating 2 was 150 μm, the thickness of thenegative electrode coating 4 was 80 μm, and the thickness of the negative electrodecurrent collector 5 was 15 μm. The positive porous conductor comprises a positiveporous layer 6 clamped between the positive pole piece and theelectrolyte layer 3 and at least one positive protruding part 7 vertically fixed on the positiveporous layer 6, wherein the positive protruding part 7 penetrates through thepositive coating 2 and then is inserted into the positivecurrent collector 1. The negative porous conductor comprises a negativeporous layer 8 sandwiched between the negative pole piece and theelectrolyte layer 3, and at least one negativeprotruding part 9 vertically fixed on the negativeporous layer 8, wherein the negativeprotruding part 9 penetrates through thenegative coating 4 and then is inserted into the negativecurrent collector 5.
The thickness of the positive electrodeporous layer 6 is 70 μm, the thickness of the negative electrodeporous layer 8 is 30 μm, and the porous structures of the positive electrodeporous layer 6 and the negative electrodeporous layer 8 are diamond grid structures. The pore diameter of the positive electrodeporous layer 6 was 10.5mm, and the pore diameter of the negative electrodeporous layer 8 was 8.5 mm. The length of the positive electrode tab 7 is 5 μm greater than the thickness of thepositive electrode coating 2, and the length of thenegative electrode tab 9 is 3 μm greater than the thickness of thenegative electrode coating 4. The positive electrode tabs 7 are arranged in a matrix on the positive electrodeporous layer 6, and thenegative electrode tabs 9 are arranged in a matrix on the negative electrodeporous layer 8. The arrangement density of the positive electrode protrusions 7 is 15 per square inch, the arrangement density of thenegative electrode protrusions 9 is 20 per square inch, the distance between two adjacent positive electrode protrusions 7 is 10.5mm, and the distance between two adjacentnegative electrode protrusions 9 is 8.5 mm.
The embodiment also provides a preparation method of the battery cell structure, and the preparation method comprises the following steps:
(1) the positive pole piece is pressed in towards the free end of the positiveprotruding part 9 under the external pressure of 550MPa, and the free end of the positiveprotruding part 9 penetrates through thepositive coating 2 and is inserted into the positivecurrent collector 1;
(2) the negative pole piece is pressed in towards the free end of the negative protruding part 7 under the external pressure of 550MPa, and the free end of the negative protruding part 7 penetrates through thenegative coating 4 and is inserted into the negativecurrent collector 5;
(3) the plane side of the positiveporous layer 6 and the plane layer of the negativeporous layer 8 are respectively superposed on the surfaces of the two sides of theelectrolyte layer 3, and after external pressure of 250MPa is applied, the surfaces of the two sides of theelectrolyte layer 3 are respectively partially embedded into the positiveporous layer 6 and the negativeporous layer 8, so that the cell structure comprising the positive porous conductor and the negative porous conductor is prepared.
Example 7
The present embodiment provides a solid-state battery, wherein the cell structure provided inembodiment 1 is the cell structure provided inembodiment 1, stainless steel is used as a positivecurrent collector 1, and the positive slurry component includes: a binder, a conductive agent, a sulfide solid electrolyte and a positive electrode active material. The surface capacity is 6.8mAh/cm2The thickness of the positiveelectrode coating layer 2 was 120 μm, and the content of conductive carbon therein was 1.5%.
Comparative example 1
This comparative example provides a solid-state battery in which the component contents, coating thickness and surface capacity of the positive electrode tab and the negative electrode tab, and the thickness and component of theelectrolyte layer 3 were exactly the same as those of example 7. The difference from example 7 is that no positive porous conductor was added between theelectrolyte layer 3 and the positive electrode tab, and no negative porous conductor was added between theelectrolyte layer 3 and the negative electrode tab. A full cell was assembled using the same process flow as in example 7.
Comparative example 2
This comparative example provides a solid-state battery in which the conductive carbon content was increased to 5% on the premise of ensuring the same surface capacity as that of the positive electrode sheet in example 7; theelectrolyte layer 3, the negative pole piece and the assembly process are kept unchanged, and the positive porous conductor and the negative porous conductor are also omitted, so that the all-solid-state battery is manufactured and assembled.
The all-solid-state batteries prepared in example 7, comparative example 1, and comparative example 2 were subjected to cycle testing using a charge and discharge apparatus. The first cycle voltage-gram capacity data is shown in fig. 4, and the cycle-capacity graph is shown in fig. 5.
As can be seen from FIG. 4, example 7 obtained by the method of the present invention has the highest capacity performance in the first week, which is related to the optimized structure designed by the present invention, and the function of optimizing the electronic conductive network inside the pole piece is achieved by embedding a layer of porous conductor with protrusions in the coating layer of the pole piece, so that the polarization phenomenon in the positive pole piece is reduced. As can be seen from fig. 5, the battery of comparative example 2 has significantly inferior cycle performance to that of example 7, because the sulfide electrolyte is unstable under high pressure, and particularly, when it is in contact with conductive carbon, it is more likely to undergo decomposition reaction under high pressure, resulting in a decrease in the ionic conductivity of the sulfide electrolyte; when more conductive carbon is added to the positive electrode sheet, it causes rapid deterioration of the contact section of the solid electrolyte and the conductive carbon, and rather, the battery performance is significantly degraded. The method can remarkably optimize the electronic conductive network in the positive pole piece, does not introduce more conductive carbon, and effectively improves the cycle performance of the battery.
The applicant declares that the above description is only a specific embodiment of the present invention, but the scope of the present invention is not limited thereto, and it should be understood by those skilled in the art that any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are within the scope and disclosure of the present invention.
Claims (18)
1. The cell structure of the solid-state battery is characterized by comprising a positive pole piece, an electrolyte layer and a negative pole piece which are sequentially stacked, wherein the positive pole piece comprises a positive coating and a positive current collector which are sequentially stacked from the surface of the electrolyte layer, and the negative pole piece comprises a negative coating and a negative current collector which are sequentially stacked from the surface of the electrolyte layer;
the battery cell structure also comprises a positive electrode porous electric conductor and/or a negative electrode porous electric conductor;
the positive porous conductor comprises a positive porous layer clamped between a positive pole piece and an electrolyte layer and at least one positive protruding part vertically fixed on the positive porous layer, and the positive protruding part penetrates through the positive coating and is inserted into the positive current collector;
the negative porous conductor comprises a negative porous layer clamped between the negative pole piece and the electrolyte layer and at least one negative protruding part vertically fixed on the negative porous layer, and the negative protruding part penetrates through the negative coating and is inserted into the negative current collector;
the battery cell structure is prepared by any one of the following preparation methods:
the preparation method comprises the following steps: the positive pole piece is pressed towards the free end of the positive protruding part, and the free end of the positive protruding part penetrates through the positive coating and is inserted into the positive current collector; the electrolyte layer is superposed on the plane side of the positive porous layer, and the electrolyte layer is embedded into the pores of the positive porous layer after pressurization; stacking the negative pole piece on the surface of one side of the electrolyte layer, which is far away from the positive pole piece, and preparing a battery core structure comprising a positive porous conductor;
the second preparation method comprises the following steps: the negative pole piece is pressed into the free end of the negative protruding part, and the free end of the negative protruding part penetrates through the negative coating and is inserted into the negative current collector; the electrolyte layer is superposed on the plane side of the negative porous layer, and the electrolyte layer is embedded into the pores of the negative porous layer after pressurization; stacking the positive pole piece on the surface of one side of the electrolyte layer, which is far away from the negative pole piece, and preparing a battery core structure comprising a negative pole porous conductor;
the preparation method comprises the following steps: the positive pole piece is pressed towards the free end of the positive protruding part, and the free end of the positive protruding part penetrates through the positive coating and is inserted into the positive current collector; the negative pole piece is pressed into the free end of the negative protruding part, and the free end of the negative protruding part penetrates through the negative coating and is inserted into the negative current collector; and respectively superposing the plane side of the anode porous layer and the plane layer of the cathode porous layer on the surfaces of the two sides of the electrolyte layer, and pressurizing to obtain the battery core structure comprising the anode porous conductor and the cathode porous conductor.
2. The cell structure of claim 1, wherein the positive porous conductor and the negative porous conductor are made of stainless steel.
3. The cell structure of claim 1, wherein the porous structures of the positive and negative porous layers are diamond-shaped lattice structures.
4. The cell structure of claim 1 or 2, wherein the thickness of the positive electrode porous layer and the negative electrode porous layer is 10-100 μm.
5. The cell structure of claim 1, wherein the thickness of the positive porous layer is the same as or different from the thickness of the negative porous layer.
6. The cell structure of claim 1, wherein the pore diameter of the positive electrode porous layer and the negative electrode porous layer is 0.355-12.5 mm.
7. The cell structure of claim 1, wherein the pore size of the positive porous layer is the same as or different from the pore size of the negative porous layer.
8. The cell structure of claim 1, wherein the mesh number of the positive electrode porous layer and the negative electrode porous layer is 2-50 meshes.
9. The cell structure of claim 1, wherein the mesh number of the positive porous layer is the same as or different from the mesh number of the negative porous layer.
10. The cell structure of claim 1, wherein the length of the positive electrode protrusion is 1-5 μm greater than the thickness of the positive electrode coating;
the length of the negative electrode protruding part is 1-5 mu m greater than the thickness of the negative electrode coating;
the length of the positive electrode protruding part is the same as or different from that of the negative electrode protruding part.
11. The cell structure of claim 1, wherein the positive protrusions are arranged in a matrix on the positive porous layer and the negative protrusions are arranged in a matrix on the negative porous layer.
12. The cell structure of claim 1, wherein the positive protrusions and the negative protrusions are arranged at a density of 2-50 protrusions per square inch.
13. The cell structure of claim 1, wherein the positive protrusions are arranged at a density that is the same as or different from the density of the negative protrusions.
14. The battery cell structure of claim 1, wherein the distance between two adjacent positive electrode protrusions is 0.355-12.5 mm;
the distance between two adjacent negative electrode protruding parts is 0.355-12.5 mm;
the distance between two adjacent positive electrode protrusions is the same as or different from the distance between two adjacent negative electrode protrusions.
15. The cell structure of claim 1, wherein the thickness of the positive current collector is 6-15 μm;
the thickness of the positive coating is 50-150 mu m;
the thickness of the negative electrode coating is 15-80 μm;
the thickness of the negative current collector is 6-15 mu m.
16. The battery cell structure of claim 1, wherein the applied pressure of the positive pole piece pressed into the positive protruding part is 450-550 MPa.
17. The cell structure of claim 1, wherein the applied pressure of the negative pole piece pressed into the negative pole protrusion is 450-550 MPa.
18. The cell structure of claim 1, wherein the pressure applied is 150-250 MPa.
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| CP01 | Change in the name or title of a patent holder | Address after:No.8899 Xincheng Avenue, Jintan District, Changzhou City, Jiangsu Province Patentee after:SVOLT Energy Technology Co.,Ltd. Address before:No.8899 Xincheng Avenue, Jintan District, Changzhou City, Jiangsu Province Patentee before:SVOLT Energy Technology Co.,Ltd. |