CN106410194A - Composite lithium battery and preparation method thereof - Google Patents
Composite lithium battery and preparation method thereof Download PDFInfo
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- CN106410194A CN106410194A CN201611053752.XA CN201611053752A CN106410194A CN 106410194 A CN106410194 A CN 106410194A CN 201611053752 A CN201611053752 A CN 201611053752A CN 106410194 A CN106410194 A CN 106410194A
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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
- 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
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/581—Chalcogenides or intercalation compounds thereof
- H01M4/5815—Sulfides
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
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- 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
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Abstract
The invention discloses a composite lithium battery and a preparation method thereof. The composite lithium battery comprises an anode, a cathode, electrolyte and a diaphragm, wherein the anode comprises an anode active substance; the anode active substance is prepared from elemental sulfur and ferric phosphate or sulfide and lithium iron phosphate in a compounded manner; and the cathode is a lithium metal cathode or a composite cathode of metallic lithium and carbon. As the advantages of high specific volume of sulfur and high security and long service life of a lithium iron phosphate material are utilized, the defect that a conventional lithium iron phosphate ion battery is low in discharge energy density can be avoided, the defects that a lithium sulfur battery is low in security and poor in circulation property can be also avoided, and comprehensive properties of energy density, security and circulation service life of the battery can be improved.
Description
Technical field
The invention belongs to field of lithium, it is related to a kind of composite lithium ion battery and preparation method thereof.
Background technology
The energy is the important substance basis that the national economic development and living standards of the people improve, and is also to directly affect economic sending out
One key factor of exhibition.Due to the increasingly deficient of the non-renewable energy resources such as oil, natural gas, coal and using these energy
The increasingly serious problem of environmental pollution being brought, countries in the world all are stepping up to explore the new energy or new sustainable development energy
Source utilizes technology, and battery is exactly one.Meanwhile, for convenience as wind energy, solar energy, tide energy, geothermal energy etc. cleaning, safety,
Regenerative resource ground uses, and needs to be converted into electric energy, that is, needs to carry out energy stores using the electrochemical power source of high power capacity.
With the exploitation of the progress of electronic technology, the requirement of lower power and portable set, electrochemical cell is largely used to the people
With consumption, industry and military field.Meanwhile, electrical equipment increases to electrochmical power source to what battery capacity and power characteristic required
Popularization also functions to certain facilitation.
In numerous energy storage devices, lithium ion battery can provide highest energy density, and has voltage stabilization, self discharge
The advantages of little, life-span length and memory-less effect, it is widely used in the aspects such as Aero-Space, portable equipment, electric tool.Lithium ion
The energy density of battery can reach 150 Wh kg-1, still cannot meet the demand to energy sustainable growth for the modern society, study carefully
Its reason, basic challenge is the positive pole of battery and the restriction of negative material specific capacity.At present, anode material for lithium-ion batteries
Mainly adopt transition metal oxide or phosphate, negative pole mainly adopts graphite, because the reaction principle of these materials is deintercalation
Reaction, positive electrode specific capacity is about 150 200 mAh g-1, specific capacity about 370 mAhg of negative pole graphite-1, limit lithium
The capacity of ion battery and energy density, even if optimisation technique, its energy density maximum can lift 30%, much cannot meet
The endurance of electric automobile 800 km.Meanwhile, the lifting of energy density increased the security risk of lithium ion battery.In order to protect
The security of card battery, the low but safe ferric phosphate lithium cell of energy density becomes main electrokinetic cell.
In order to meet the demand to energy density such as electric automobile, intelligent grid of sustainable development, it is new that people start exploitation
The battery of type electrochemical system.Based on conversion reaction and with the electrode material of more polyion and electron reaction, good choosing can be become
Select.Recently, lithium air and lithium-sulfur cell are because of its energy density height (respectively 3500 Wh kg-1With 2500 Wh kg-1) obtain
Extensive concern, becomes the representative of model electrochemical system battery.The negative pole of lithium-air battery is lithium metal, and positive pole is from environment
Absorb oxygen, in air electrode internal oxidation reduction.However, because the technology of lithium-air battery key component not yet breaks through, making
Obtain its chargeable performance and cycle performance faces enormous challenge.Compared with lithium-air battery, positive pole and negative material are respectively
The lithium-sulfur cell institute facing challenges of elemental sulfur and lithium metal are then smaller, are considered easily practical.Its theoretical energy
Density is up to 2600 Whkg-1, 5 times of about current commercial cells, the theoretical specific capacity of positive pole and negative material is respectively
1672mAh g-1With 3860 mAh g-1, the conversion reaction based on elemental sulfur of the high power capacity of elemental sulfur, sulphur atom can be with
Two lithium atom reactions generate Li2S.Not only theoretical specific capacity is high for elemental sulfur, and rich reserves, environmental friendliness, low cost.
Although lithium-sulfur cell has very big advantage in specific energy density, poor cycle performance, security limit
Its practical application.Show that sulfur-based positive electrode material is primarily present following problem from the research of lithium-sulfur cell cyclic process and mechanism:
(1)Elemental sulfur is electronics and ion insulator at room temperature(Room-temperature conductivity is 5 × 10-30S/cm), need to add greatly
Amount conductive agent, improves electronic conductivity and the ionic conductivity of positive pole;
(2)Elemental sulfur can form readily soluble polysulfide in discharge process, is dissolved in the loss that electrolyte causes active material, causes
Its cycle performance is made to be deteriorated, many sulphions are diffused into negative pole and directly occur self discharge to react with negative pole, are formed " shuttle effect ", cause
Battery efficiency is made to be deteriorated;
(3)Battery discharge insoluble end-product Li2S2And Li2S deposits in positive electrode surface, causes positive electrode surface to be passivated, has a strong impact on
The electrochemical reaction of battery;
For these problems, research staff is modified to lithium-sulfur cell, has obtained to a certain degree solving.But make a general survey of current changing
Property technology be all around synthesizing sulfur-bearing anode composite, by the improvement of the microstructure of anode composite material, to obtain reach overcome,
Improve the purpose of chemical property.But due to the loss of active material cannot be avoided completely, fundamentally respectively take shortcoming.This is
Though lithium-sulfur cell have passed through the research and development of many decades, but still is not reaching to the basic reason of industrialization.
Content of the invention
The purpose of the present invention is to overcome the defect that in existing lithium battery, active material easily loses, and provides a kind of alleviation lithium sulphur
The drawbacks of battery security is low, cycle performance is poor, lifting battery is comprehensive in specific energy density, security, cycle life
Energy.
For reaching above-mentioned purpose, the invention provides a kind of composite lithium ion battery, including positive pole, negative pole, electrolyte and barrier film,
Wherein, this positive pole comprises positive active material, and this positive active material is combined or sulfide and phosphoric acid with ferric phosphate by elemental sulfur
Iron lithium is combined and is prepared from, and this negative pole selects the composite negative pole of lithium an- ode or lithium metal and carbon.
In described combination electrode, the weight/mass percentage composition of sulphur or sulfide is 5% ~ 40%.
Described sulfide is lithium sulfide.
Described electrolyte is ethers electrolyte.
Described electrolyte comprises 1.0M LiTFSI/DME(1,2- dimethoxy):DOL(1,3- dioxolanes),
Wherein, the mixed volume of LiTFSI/DME and DOL is than for 1:1.
Described electrolyte also comprises 0.2M LiNO3.
Described barrier film selects microporous polypropylene membrane.
The composite preparation process of described anode composite is combined for physics, and it comprises:Weigh respectively elemental sulfur or sulfide,
LiFePO4;Grind or ball milling mixing is uniform.
Described simple substance sulfur materials are crystal or noncrystal;Described LiFePO 4 material is nano material, or nanometer is made
Grain material.
Present invention also offers a kind of preparation method according to above-mentioned composite lithium ion battery, the method comprises:
Step 1, weighs elemental sulfur or sulfide, LiFePO4 respectively;
Step 2, elemental sulfur or sulfide, LiFePO4 mixing are ground or ball milling are made the two uniformly mix, obtain positive-active
Material;
Step 3, positive active material is made anode, forms composite lithium ion battery with negative pole, barrier film and electrolyte.
Present invention firstly provides LiFePO4 (olivine-type)/sulphur composite electrochemical new system, it is one kind has two sections
The novel battery system of different flash-over characteristic platforms.By by elemental sulfur in lithium-sulfur cell or sulfide and lithium ion battery
Lithium iron phosphate positive material is combined, and builds a kind of new composite lithium ion battery.This system has worked in coordination with lithium-ion battery lithium iron phosphate
" dissolution/precipitation " energy storage mechnism of sulfur materials in " intercalation/deintercalation " mechanism of positive electrode and lithium-sulfur cell, to lift compound storage
Energy system is for the purpose of specific energy density, safety-type, the combination property of cycle performance.The present invention utilizes height ratio capacity and the phosphorus of sulphur
The high safety of sour iron lithium material, long circulating characteristic, using the two mixing as positive electrode, the NEW TYPE OF COMPOSITE lithium battery developed can
To realize the controllable adjustment from high security, long-life to high specific energy, it is more suitable for power vehicle for battery high specific energy and Gao An
The demand of full performance.Blended anode material preparation method in this composite lithium ion battery simple it is easy to industrialized production.
Brief description
Fig. 1 is raw material selected by the embodiment of the present invention 1 and prepared NEW TYPE OF COMPOSITE lithium battery blended anode material
SEM (ESEM) figure of material, wherein, A is simple substance sulfur materials, and B is LFPO positive electrode, and C is blended anode material.
Fig. 2 is cyclic voltammetric (CV) curve of the NEW TYPE OF COMPOSITE lithium battery prepared by the embodiment of the present invention 1.
Fig. 3 is the charging and discharging curve of the NEW TYPE OF COMPOSITE lithium battery prepared by the embodiment of the present invention 1.
Fig. 4 is the charging and discharging curve of the NEW TYPE OF COMPOSITE lithium battery prepared by the embodiment of the present invention 2.
Fig. 5 is the charging and discharging curve of the NEW TYPE OF COMPOSITE lithium battery prepared by the embodiment of the present invention 3.
Fig. 6 is the charging and discharging curve of the NEW TYPE OF COMPOSITE lithium battery prepared by the embodiment of the present invention 4.
Specific embodiment
The invention will be further described to pass through specific embodiment below in conjunction with accompanying drawing, and these embodiments are merely to illustrate
The present invention, is not limiting the scope of the invention.
Embodiment 1:
Step 1, according to stoichiometric proportion precise elemental sulfur and LFPO(LiFePO4)Positive electrode, wherein sulphur account for 30%.Step
Rapid 2, load weighted material is put into grinding half an hour, obtains mixing material sample, the positive pole as NEW TYPE OF COMPOSITE lithium battery is lived
Property material.Step 3, positive active material is made anode, with negative pole, barrier film and electrolyte composition complex lithium electricity
Pond.
Elemental sulfur(A in Fig. 1), LFPO positive electrode(B in Fig. 1)And the blended anode being obtained by the present embodiment
Material(C in Fig. 1)SEM(ESEM)Figure is as shown in figure 1, the pattern base of as can be seen from the figure simple substance sulfur materials itself
This is not destroyed, and LFPO positive electrode particle is attached to elemental sulfur material surface.
The cyclic voltammetric of the blended anode material being obtained by the present embodiment(CV)Curve map is as shown in Fig. 2 can from figure
Clearly to tell the redox peaks of elemental sulfur positive electrode and the redox peaks of LFPO positive electrode, sulfur materials are described
All play respective electrical property with LiFePO 4 material it is shown that respective charge-discharge characteristics, show the mixing of bi-material
Do not affect its basic structure and property.
The charging and discharging curve of the composite lithium ion battery being obtained by the present embodiment is as shown in figure 3, can clearly divide from figure
Discern the charge and discharge platform of elemental sulfur positive electrode and the charge and discharge platform of LFPO positive electrode, charge specific capacity is
451.5mAh/g, specific discharge capacity is 418.1mAh/g, and efficiency is 92.6%.
Embodiment 2:
Step 1, according to stoichiometric proportion precise elemental sulfur and LFPO positive electrode, wherein sulphur accounts for 20%.Step 2, will weigh
Grinding half an hour put into by good material, obtains mixing material sample, as the cathode active material of NEW TYPE OF COMPOSITE lithium battery.
Step 3, positive active material is made anode, forms composite lithium ion battery with negative pole, barrier film and electrolyte.
The charging and discharging curve of the NEW TYPE OF COMPOSITE lithium battery being obtained by the present embodiment is as shown in figure 4, can be clear from figure
Tell the charge and discharge platform of elemental sulfur positive electrode and the charge and discharge platform of LFPO positive electrode, charge specific capacity is
320.2mAh/g, specific discharge capacity is 336.8mAh/g, and efficiency is 105.2%.
Embodiment 3:
Step 1, according to stoichiometric proportion precise lithium sulfide and LFPO positive electrode, wherein lithium sulfide accounts for 30%.Step 2, will
Grinding half an hour put into by load weighted material, obtains mixing material sample, as the positive active material of NEW TYPE OF COMPOSITE lithium battery
Material.Step 3, positive active material is made anode, forms composite lithium ion battery with negative pole, barrier film and electrolyte.
The charging and discharging curve of the NEW TYPE OF COMPOSITE lithium battery being obtained by the present embodiment is as shown in figure 5, its charge ratio after testing
Capacity is 471.9mAh/g, and specific discharge capacity is 439.4mAh/g, and efficiency is 93.1%.
Embodiment 4:
Step 1, according to stoichiometric proportion precise lithium sulfide and LFPO positive electrode, wherein lithium sulfide accounts for 20%.Step 2, will
Grinding half an hour put into by load weighted material, obtains mixing material sample, as the positive active material of NEW TYPE OF COMPOSITE lithium battery
Material.Step 3, positive active material is made anode, forms composite lithium ion battery with negative pole, barrier film and electrolyte.
The charging and discharging curve of the NEW TYPE OF COMPOSITE lithium battery being obtained by the present embodiment is as shown in fig. 6, its charge ratio after testing
Capacity is 396.8mAh/g, and specific discharge capacity is 390.1mAh/g, and efficiency is 98.3%.
In sum, the present invention utilizes the height ratio capacity of sulphur and the high safety of LiFePO 4 material, long circulating characteristic, by two
Person mixes as positive electrode, and the NEW TYPE OF COMPOSITE lithium battery developed can be realized from high security, long-life to high specific energy
Controllable adjustment, is more suitable for the demand for battery high specific energy and high safety performance for the power vehicle.And, in this composite lithium ion battery
Blended anode material preparation method simple it is easy to industrialized production.
Although present disclosure has been made to be discussed in detail by above preferred embodiment, but it should be appreciated that above-mentioned
Description is not considered as limitation of the present invention.After those skilled in the art have read the above, for the present invention's
Multiple modifications and substitutions all will be apparent from.Therefore, protection scope of the present invention should be limited to the appended claims.
Claims (10)
1. a kind of composite lithium ion battery, including positive pole, negative pole, electrolyte and barrier film it is characterised in that this positive pole comprises positive-active
Material, this positive active material is combined with ferric phosphate by elemental sulfur or sulfide is combined with LiFePO4 and is prepared from, this negative pole
Select the composite negative pole of lithium an- ode or lithium metal and carbon.
2. composite lithium ion battery as claimed in claim 1 it is characterised in that in described combination electrode sulphur or sulfide quality
Percentage composition is 5% ~ 40%.
3. composite lithium ion battery as claimed in claim 1 is it is characterised in that described sulfide is lithium sulfide.
4. composite lithium ion battery as claimed in claim 1 is it is characterised in that described electrolyte is ethers electrolyte.
5. composite lithium ion battery as claimed in claim 4 is it is characterised in that described electrolyte comprises 1.0M LiTFSI/DME:
DOL, wherein, the mixed volume of LiTFSI/DME and DOL is than for 1:1.
6. composite lithium ion battery as claimed in claim 5 is it is characterised in that described electrolyte also comprises 0.2M LiNO3.
7. composite lithium ion battery as claimed in claim 1 is it is characterised in that described barrier film selects microporous polypropylene membrane.
8. composite lithium ion battery as claimed in claim 1 is it is characterised in that the preparation method of described composite cathode active material
It is combined for physics, it comprises:Weigh elemental sulfur or sulfide, LiFePO4 respectively;Grind or ball milling mixing is uniform.
9. composite lithium ion battery as claimed in claim 1 is it is characterised in that simple substance sulfur materials are crystal or noncrystal;Ferric phosphate
Lithium material is nano material.
10. a kind of preparation method of composite lithium ion battery according to claim 1 is it is characterised in that the method comprises:
Step 1, weighs elemental sulfur or sulfide, LiFePO4 respectively;
Step 2, elemental sulfur or sulfide, LiFePO4 mixing are ground or ball milling are made the two uniformly mix, obtain positive-active
Material;
Step 3, positive active material is made anode, forms composite lithium ion battery with negative pole, barrier film and electrolyte.
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CN201611053752.XA CN106410194A (en) | 2016-11-25 | 2016-11-25 | Composite lithium battery and preparation method thereof |
PCT/CN2017/108595 WO2018095202A1 (en) | 2016-11-25 | 2017-10-31 | Composite lithium battery and preparation method therefor |
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Cited By (6)
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CN107342412A (en) * | 2017-07-07 | 2017-11-10 | 江西省科学院应用化学研究所 | A kind of preparation method of nanoparticle phosphotungstate/sulphur positive electrode |
WO2018095202A1 (en) * | 2016-11-25 | 2018-05-31 | 上海空间电源研究所 | Composite lithium battery and preparation method therefor |
CN108987725A (en) * | 2018-08-21 | 2018-12-11 | 南开大学 | A kind of anode composite material of lithium sulfur battery and preparation method thereof |
CN109148854A (en) * | 2018-08-21 | 2019-01-04 | 南开大学 | The lithium sulfur battery anode material and preparation method of carbon doping phosphoric acid ferrimanganic lithium sulfur loaded |
CN109167034A (en) * | 2018-08-21 | 2019-01-08 | 南开大学 | Using ternary material as lithium-sulfur battery composite cathode material of carrier and preparation method thereof |
CN116207370A (en) * | 2023-05-06 | 2023-06-02 | 江苏天合储能有限公司 | High-performance SEI film and preparation method thereof |
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CN114824648A (en) * | 2022-03-18 | 2022-07-29 | 扬州大学 | PW 12 @ PDADMAC/WMCNT modified polypropylene diaphragm and application thereof in lithium-sulfur battery |
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Cited By (7)
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WO2018095202A1 (en) * | 2016-11-25 | 2018-05-31 | 上海空间电源研究所 | Composite lithium battery and preparation method therefor |
CN107342412A (en) * | 2017-07-07 | 2017-11-10 | 江西省科学院应用化学研究所 | A kind of preparation method of nanoparticle phosphotungstate/sulphur positive electrode |
CN108987725A (en) * | 2018-08-21 | 2018-12-11 | 南开大学 | A kind of anode composite material of lithium sulfur battery and preparation method thereof |
CN109148854A (en) * | 2018-08-21 | 2019-01-04 | 南开大学 | The lithium sulfur battery anode material and preparation method of carbon doping phosphoric acid ferrimanganic lithium sulfur loaded |
CN109167034A (en) * | 2018-08-21 | 2019-01-08 | 南开大学 | Using ternary material as lithium-sulfur battery composite cathode material of carrier and preparation method thereof |
WO2020037948A1 (en) * | 2018-08-21 | 2020-02-27 | 南开大学 | Lithium-sulfur battery composite anode material using ternary material as carrier and preparation method for lithium-sulfur battery composite anode material |
CN116207370A (en) * | 2023-05-06 | 2023-06-02 | 江苏天合储能有限公司 | High-performance SEI film and preparation method thereof |
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Application publication date: 20170215 |