CN109980291B - Battery cell of cylindrical lithium-sulfur battery and preparation method and application thereof - Google Patents

Battery cell of cylindrical lithium-sulfur battery and preparation method and application thereof Download PDF

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CN109980291B
CN109980291B CN201910254869.1A CN201910254869A CN109980291B CN 109980291 B CN109980291 B CN 109980291B CN 201910254869 A CN201910254869 A CN 201910254869A CN 109980291 B CN109980291 B CN 109980291B
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electrode
cylindrical
lithium
battery
sulfur
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CN109980291A (en
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夏阳
李姣姣
张文魁
陈安琪
黄辉
甘永平
张俊
梁初
贺馨平
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Zhejiang University of Technology ZJUT
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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
    • 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
    • H01M4/04—Processes of manufacture in general
    • H01M4/043—Processes of manufacture in general involving compressing or compaction
    • H01M4/0433—Molding
    • 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
    • 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
    • H01M4/134—Electrodes based on metals, Si or alloys
    • 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
    • H01M4/139—Processes of manufacture
    • 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
    • H01M4/139—Processes of manufacture
    • H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
    • 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
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The invention relates to a cell structure design of a cylindrical lithium-sulfur battery, a preparation method and application thereof, belonging to the field of lithium-sulfur battery design and manufacture, wherein the cell comprises a positive electrode, a negative electrode, a diaphragm sleeve and a cylindrical battery shell, one electrode of the positive electrode and the negative electrode is cylindrical, the other electrode is in a honeycomb briquette shape, a lead is arranged in the cylindrical electrode, the diaphragm sleeve is sleeved outside the cylindrical electrode, the battery shell is coated outside the honeycomb briquette shape electrode, the diaphragm sleeve is embedded into a through hole of the honeycomb briquette shape electrode, and the top of the battery shell is provided with a cap seal; the positive electrode is a sulfur-containing conductive composite material, and the negative electrode is a lithium band, lithium powder or a lithium mesh. Compared with the existing lithium sulfur battery with a laminated structure or a winding structure, the battery core has the advantages of remarkably improving the energy density of the lithium sulfur battery, improving the conductivity of the lithium sulfur battery, improving the structural stability of the lithium sulfur battery, enhancing the electrochemical reaction activity of the lithium sulfur battery, inhibiting the shuttle effect of polysulfide and improving the utilization rate of materials of the lithium sulfur battery.

Description

Battery cell of cylindrical lithium-sulfur battery and preparation method and application thereof
Technical Field
The invention relates to a cell structure design of a cylindrical lithium-sulfur battery, a preparation method and application thereof, belonging to the field of design and manufacture of lithium-sulfur batteries.
Background
Lithium-sulfur (Li-S) batteries have attracted attention because of their high theoretical energy density (2600Wh/kg), low cost, environmental friendliness, good safety, and the like, and are considered to be a new type of high energy density lithium secondary batteries with great potential. However, in the existing liquid electrolyte system, the Li-S battery still has the following problems: (1) elemental sulfur (S)8) Has poor electronic insulation (5 multiplied by 10)- 30S/cm, 25 ℃), so that the sulfur electrode material has low utilization rate, poor reaction activity and low high-rate performance; (2) elemental sulfur (S)8) And the discharge product lithium sulfide (Li)2S) has a large difference in density and polarity (S)8: nonpolar, [ rho ] 2.03g/cm3；Li2S: polarity, p 1.67g/cm3) Before and after charge and discharge reactions, the sulfur electrode not only generates larger volume change, but also the interface compatibility of the carrier material and the active substance is changed, so that the interface instability and the structural damage of the sulfur electrode are caused; (3) lithium polysulfide (Li) as discharge intermediate for sulfur electrodes2SxX is more than or equal to 4 and less than or equal to 8) has higher solubility in an organic electrolyte system to generate Li2SxThe shuttle effect causes corrosion of a lithium cathode and loss of a sulfur anode, resulting in low charging and discharging efficiency and poor cycle stability. Obviously, for the commercial application of Li-S batteries, the core work is to optimize and rationally design the Li-S battery structure and improve the structural stability and electrochemical activity of the sulfur electrode material.
Currently, Li-S batteries are primarily of a stacked or rolled configuration, however, due to their large electrode contact area, barrier layers or special adsorbents are needed to inhibit or mitigate polysulfide shuttling problems and lithium metal corrosion problems. The present invention therefore proposes a novel Li-S battery structure: one pole is designed and processed into a cylindrical electrode, the other pole is processed into a honeycomb briquette-shaped electrode, and the cylindrical electrode and the honeycomb briquette-shaped electrode are nested with each other to construct a cylindrical Li-S battery. The design can improve the material utilization rate of the Li-S battery, reduce the shuttle effect of polysulfide and improve the structural stability of the electrode, thereby having obvious advantages compared with the existing Li-S battery structure.
Disclosure of Invention
The invention provides a cylindrical lithium-sulfur battery cell which can improve the material utilization rate of a Li-S battery, reduce polysulfide shuttling effect and improve the stability of an electrode structure, and simultaneously provides a preparation method and application of the cell, so that the cylindrical lithium-sulfur battery cell has wide application prospect.
The technical scheme adopted by the invention for solving the technical problems is as follows:
one of the positive electrode and the negative electrode is cylindrical, the other electrode is honeycomb-shaped, a lead is arranged in the cylindrical electrode, a diaphragm sleeve is sleeved outside the cylindrical electrode, a battery shell is wrapped outside the honeycomb-shaped electrode, the cylindrical electrode sleeved with the diaphragm sleeve is embedded into a through hole of the honeycomb-shaped electrode, the number of the cylindrical electrodes is the same as that of the through holes of the honeycomb-shaped electrode, one cylindrical electrode is embedded into one through hole, and a cap is arranged at the top of the battery shell for sealing;
the positive electrode is a sulfur-containing conductive composite material, and the negative electrode is a lithium band, lithium powder or a lithium mesh.
Preferably, the positive electrode is at least one of a sulfur/carbon composite, a sulfur/conductive polymer composite, and a sulfur/metal oxide composite.
Preferably, the membrane sleeve is a porous tube with a sealed bottom, so as to prevent the short circuit phenomenon caused by the contact of the positive electrode and the negative electrode, and the membrane sleeve is made of a PP (polypropylene) membrane, a PE (polyethylene) membrane, a PP/PE mixed membrane, a glass fiber membrane, a PTFE (polytetrafluoroethylene) membrane, a PVDF (polyvinylidene fluoride) membrane, an organic-inorganic composite membrane or porous ceramic.
Preferably, the outer diameter of the cylindrical electrode fitted with the membrane sleeve is matched with the inner diameter of the through hole of the honeycomb briquette-shaped electrode fitted with the cylindrical electrode.
Preferably, the lead is a spiral metal wire, the metal wire is spirally raised close to the inner wall of the cylindrical electrode, the thread pitch of the metal wire is 6-10 mm, and the line width of the metal wire is 1.0-1.5 mm.
Preferably, when the cylindrical electrode is a positive electrode, the lead is aluminum, nickel, or stainless steel; when the cylindrical electrode is a negative electrode, the lead is copper, nickel or platinum.
Preferably, the diameter of the cylindrical electrode is 10 to 20mm, and the height is 60 to 70 mm.
Preferably, the cap is coated with insulating glue.
A preparation method of a battery core of a cylindrical lithium-sulfur battery is based on a cylindrical mold and a honeycomb briquette-shaped mold, and comprises the following steps:
s1, presetting one electrode of the positive electrode and the negative electrode of the battery as a cylindrical electrode and presetting the other electrode as a honeycomb briquette-shaped electrode;
s2, placing the material of the cylindrical electrode and the spiral lead in a cylindrical mould, compacting to prepare the cylindrical electrode with the lead, and embedding the cylindrical electrode into a diaphragm pipe sleeve;
s3, placing the material of the honeycomb briquette shaped electrode in a honeycomb briquette shaped die, compacting the honeycomb briquette shaped electrode to form the honeycomb briquette shaped electrode, and coating a battery shell outside the honeycomb briquette shaped electrode;
s4, placing the cylindrical electrode with the membrane sleeve prepared in the step S2 in a through hole of the honeycomb briquette-shaped electrode, then injecting electrolyte liquid, sealing the cover cap, and secondarily isolating the cylindrical electrode with the insulating glue, thus obtaining the cylindrical lithium-sulfur battery.
A cylindrical lithium-sulfur battery cell is used for cylindrical batteries of 18650, 21700 and 26650 types.
The invention has the beneficial effects that:
1. compared with the existing lithium sulfur battery with a laminated structure or a winding structure, the battery core of the lithium sulfur battery has the advantages of obviously improving the energy density of the lithium sulfur battery, improving the conductivity of the lithium sulfur battery, improving the structural stability of the lithium sulfur battery, enhancing the electrochemical reaction activity of the lithium sulfur battery, inhibiting the shuttle effect of polysulfide and improving the utilization rate of materials of the lithium sulfur battery;
2. the preparation method of the battery core of the lithium-sulfur battery has the advantages of simple process, low cost, easy popularization and wide application prospect.
Drawings
Fig. 1 is a schematic structural diagram of a cell of a cylindrical lithium-sulfur battery prepared in example 1 of the present invention;
FIG. 2 is a cross-sectional view of FIG. 1;
FIG. 3 is a top view of example 3 of the present invention;
FIG. 4 is a schematic structural view of a cylindrical electrode prepared in example 2 of the present invention;
fig. 5 is a charge-discharge capacity-voltage curve of a cylindrical lithium-sulfur battery cell prepared in example 1 of the present invention at 0.1C;
fig. 6 is a charge-discharge cycle curve of a battery cell of a cylindrical lithium-sulfur battery prepared in example 1 of the present invention at 0.5C.
In the figure: 1-positive electrode; 2-a membrane sleeve; 3-a negative electrode; 4-a battery housing; 5-a lead; 6-capping; 7-insulating glue.
Detailed Description
The technical solution of the present invention is further illustrated by the following embodiments in conjunction with the accompanying drawings.
Example 1:
a preparation method of a battery core of a cylindrical lithium-sulfur battery is based on a cylindrical mold and a honeycomb briquette-shaped mold, and comprises the following steps:
s1, presetting the positive electrode 1 of the battery as a cylindrical electrode and presetting the negative electrode 3 as a honeycomb briquette-shaped electrode;
s2, pressing quantitative sulfur-carbon composite material powder and the spiral aluminum wire 5 into a cylindrical electrode through a specific cylindrical die, wherein the diameter of the cylindrical electrode is 10mm, the height of the cylindrical electrode is 60mm, the pressure of the die is 30Mpa, maintaining the pressure for 15min, and then putting the cylindrical electrode into a porous PP diaphragm sleeve 2 with the thickness of 0.1 mm;
s3, pressing the lithium metal powder into a honeycomb briquette electrode in a specific honeycomb briquette mold, wherein the diameter of a through hole in the honeycomb briquette electrode is 10.2mm (the same as the outer diameter of a diaphragm sleeve), the outer diameter is 15mm, the height is 60mm, the pressure of the mold is 10MPa, keeping the pressure for 10min, and then coating the battery shell 4 outside the honeycomb briquette electrode;
s4, embedding the sulfur-carbon cylindrical electrode sleeved with the porous PP diaphragm sleeve 2 into a through hole in the honeycomb coal-shaped metal lithium electrode, injecting liquid, sealing the cap 6, coating insulating glue 7, and performing secondary isolation to obtain the battery core of the cylindrical lithium-sulfur battery, as shown in the attached drawing 1.
FIG. 5 is a charge-discharge capacity-voltage curve of the cell at a current density of 0.1C; fig. 6 is a graph of the charge-discharge cycle at 0.5C current density for this cell.
Example 2:
a preparation method of a battery core of a cylindrical lithium-sulfur battery is based on a cylindrical mold and a honeycomb briquette-shaped mold, and comprises the following steps:
s1, presetting the positive electrode 1 of the battery as a cylindrical electrode and presetting the negative electrode 3 as a honeycomb briquette-shaped electrode;
s2, pressing a certain amount of sulfur/conductive polymer composite powder and a spiral aluminum wire 5 into a cylindrical electrode with a diameter of 15mm, a height of 60mm and a pressure of 20MPa through a specific cylindrical die, maintaining the pressure for 10min, as shown in figure 4, wherein the spiral diameter of the spiral aluminum wire 5 is 14mm, the thread pitch is 8mm, the line width is 1.2mm, and then putting the cylindrical electrode into porous Al with a thickness of 0.1mm2O3In the diaphragm casing 2;
s3, pressing the lithium metal powder into a honeycomb briquette electrode in a specific honeycomb briquette mold, wherein the diameter of a through hole in the honeycomb briquette electrode is 15.2mm (the same as the outer diameter of a diaphragm sleeve), the outer diameter is 20mm, the height is 60mm, the pressure of the mold is 5MPa, keeping the pressure for 7min, and then coating the battery shell 4 on the outer part of the mold;
s4, sheathing porous Al2O3And (3) embedding the sulfur/conductive polymer cylindrical electrode of the diaphragm sleeve 2 into a straight-through hole in the honeycomb-coal-shaped metal lithium electrode, injecting liquid, sealing the cap 6, coating insulating glue 7, and performing secondary isolation to obtain the battery core of the cylindrical lithium-sulfur battery.
Example 3:
a preparation method of a battery core of a cylindrical lithium-sulfur battery is based on a cylindrical mold and a honeycomb briquette-shaped mold, and comprises the following steps:
s1, presetting the battery cathode 3 as a cylindrical electrode and the anode 1 as a honeycomb briquette electrode;
s2, pressing quantitative lithium metal powder and the spiral copper wire 5 into a cylindrical electrode through a specific cylindrical die, wherein the diameter of the cylindrical electrode is 10mm, the height of the cylindrical electrode is 65mm, the pressure of the die is 10MPa, maintaining the pressure for 10min, and then putting the cylindrical electrode into a porous PP/PE diaphragm sleeve 2 with the thickness of 0.15 mm;
s3, pressing the sulfur-carbon composite material into a honeycomb briquette electrode in a specific honeycomb briquette mold, wherein the diameter of a through hole in the honeycomb briquette electrode is 10.2mm (the same as the outer diameter of a diaphragm sleeve), the outer diameter is 15mm, the height is 65mm, pressing is carried out under the pressure of 30MPa, and the pressure is maintained for 5 min;
s4, inserting the metal lithium cylindrical electrode sleeved with the porous PP/PE diaphragm sleeve 2 into a through hole in the sulfur-carbon honeycomb-coal-shaped electrode, wherein the top view is as shown in figure 3, and after liquid injection, the cap 6 is sealed and coated with insulating glue 7 for secondary isolation to obtain the battery cell of the cylindrical lithium-sulfur battery.
The above-described embodiments are merely preferred embodiments of the present invention, which is not intended to be limiting in any way, and other variations and modifications are possible without departing from the scope of the invention as set forth in the appended claims.

Claims (8)

1. A battery core of a cylindrical lithium-sulfur battery comprises a positive electrode, a negative electrode, a diaphragm sleeve and a battery shell, and is characterized in that,
one of the positive electrode and the negative electrode is cylindrical, the other electrode is honeycomb-shaped, a lead is arranged in the cylindrical electrode, a diaphragm sleeve is sleeved outside the cylindrical electrode, a battery shell is wrapped outside the honeycomb-shaped electrode, the cylindrical electrode sleeved with the diaphragm sleeve is embedded into a through hole of the honeycomb-shaped electrode, the number of the cylindrical electrodes is the same as that of the through holes of the honeycomb-shaped electrode, one cylindrical electrode is embedded into one through hole, and a cap is arranged at the top of the battery shell for sealing;
the positive electrode is a sulfur-containing conductive composite material, and the negative electrode is a lithium belt, lithium powder or a lithium net;
the membrane sleeve is a porous pipe with a sealed bottom, and is made of a PP (polypropylene) membrane, a PE (polyethylene) membrane, a PP/PE mixed membrane, a glass fiber membrane, a PTFE (polytetrafluoroethylene) membrane, a PVDF (polyvinylidene fluoride) membrane, an organic-inorganic composite membrane or porous ceramic;
the lead wire is a spiral metal wire, the metal wire is tightly attached to the inner wall of the cylindrical electrode and spirally rises to a vertex, the thread pitch is 6-10 mm, and the line width is 1.0-1.5 mm.
2. The cell of a cylindrical lithium sulfur battery according to claim 1, wherein the positive electrode is at least one of a sulfur/carbon composite, a sulfur/conductive polymer composite, and a sulfur/metal oxide composite.
3. The battery cell of the cylindrical lithium-sulfur battery of claim 1, wherein the outer diameter of the cylindrical electrode sleeved with the membrane sleeve is matched with the inner diameter of the through hole of the honeycomb briquette-shaped electrode embedded with the cylindrical electrode.
4. The cylindrical lithium-sulfur battery cell of claim 1, wherein when the cylindrical electrode is a positive electrode, the lead is aluminum, nickel or stainless steel; when the cylindrical electrode is a negative electrode, the lead is copper, nickel or platinum.
5. The battery cell of the cylindrical lithium-sulfur battery of claim 1, wherein the cylindrical electrode has a diameter of 10-20 mm and a height of 60-70 mm.
6. The battery cell of the cylindrical lithium-sulfur battery of claim 1, wherein the cap is coated with an insulating glue.
7. A preparation method of a battery cell of a cylindrical lithium-sulfur battery as claimed in any one of claims 1 to 6, based on a cylindrical mold, a honeycomb briquette-shaped mold and a spiral lead, wherein the method comprises the following steps:
s1, presetting one electrode of the positive electrode and the negative electrode of the battery as a cylindrical electrode and the other electrode as a honeycomb briquette-shaped electrode, wherein the number of the cylindrical electrodes is the same as that of the through holes of the honeycomb briquette-shaped electrode;
s2, placing the material of the cylindrical electrode and the spiral lead in a cylindrical mould, compacting to obtain the cylindrical electrode with the spiral lead, and embedding the cylindrical electrode in a diaphragm tube sleeve;
s3, placing the material of the honeycomb briquette shaped electrode in a honeycomb briquette shaped die, compacting the honeycomb briquette shaped electrode to form the honeycomb briquette shaped electrode, and coating a battery shell outside the honeycomb briquette shaped electrode;
s4, placing the cylindrical electrode with the membrane sleeve prepared in the step S2 in a through hole of the honeycomb briquette-shaped electrode, injecting electrolyte, sealing a cap, and secondarily isolating by using insulating glue to obtain the cylindrical lithium-sulfur battery.
8. A battery core of the cylindrical lithium-sulfur battery as claimed in any one of claims 1 to 6 is used for cylindrical batteries of 18650, 21700 and 26650 types.
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CN206480700U (en) * 2017-01-20 2017-09-08 江南山 A kind of multitube lithium-sulfur cell
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JPH1040901A (en) * 1996-07-22 1998-02-13 Kao Corp Nonaqueous secondary battery
CN202454617U (en) * 2012-03-06 2012-09-26 华太电池（天津）有限公司 Alkaline battery
CN106784623A (en) * 2017-01-20 2017-05-31 江南山 A kind of multitube lithium-sulfur cell

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