CN107221699A - A kind of novel high voltage lithium ion battery and energy storage elements based on silicium cathode - Google Patents

A kind of novel high voltage lithium ion battery and energy storage elements based on silicium cathode Download PDF

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CN107221699A
CN107221699A CN201710387222.7A CN201710387222A CN107221699A CN 107221699 A CN107221699 A CN 107221699A CN 201710387222 A CN201710387222 A CN 201710387222A CN 107221699 A CN107221699 A CN 107221699A
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compound
silicon
ion battery
carbon
lithium ion
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陈龙
李海君
栗欢欢
王亚平
徐如玉
江浩斌
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Jiangsu University
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Jiangsu University
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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
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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
    • H01M4/136—Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
    • 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

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

Abstract

The invention discloses a kind of novel high voltage lithium ion battery based on silicium cathode and energy storage elements, the lithium ion battery includes positive pole, negative pole and electrolyte, and positive active material is selected from cobalt phosphate lithium and its compound, and negative electrode active material is selected from silica-base material.The lithium ion battery that the present invention is provided has the characteristics of voltage is high, security is good, specific energy is high.

Description

A kind of novel high voltage lithium ion battery and energy storage elements based on silicium cathode
Technical field
The invention belongs to electrochemical field, and in particular to a kind of novel high voltage lithium ion battery and energy based on silicium cathode Measure memory element.
Background technology
The 21 century mankind must be in face of the energy and two Tough questions of environment, therefore taps a new source of energy and renewable cleaning The energy has profound significance.Electric automobile replaces the fossil fuels such as oil as power using electric energy, with energy-conserving and environment-protective Advantage, receives the concern in the whole world.In the study hotspot related to electric automobile, battery technology is considered as topmost difficulty Close.But current power ion battery systems are in terms of specific energy, specific power, service life, cost, also in the presence of much urgently The problem of solution.Therefore, exploitation design safety is good, specific energy is high, good cycle power lithium-ion battery be it is necessary and Urgent.
Anode material for lithium-ion batteries is one of important component of lithium ion battery, and its research and development is directly influenced Lithium ion battery overall performance.LiCoPO4Crystal has the stable structure of orderly olivine-type as LiFePO4, belongs to Rhombic system, theoretical discharge capacity is 167mAh/g, LiCoPO4Positive electrode, which has, to be had a safety feature, relative to lithium electrode electricity Gesture height (about 4.8V), is expected to turn into high power capacity of new generation, high voltage, the positive electrode of high-energy-density.
In addition, negative material is also to influence the key factor of lithium ion battery overall performance.At present, it is commercially use negative Pole material is mostly graphite cathode material.Such negative material has good charge and discharge platform and structural stability, but in fact Border specific discharge capacity (about 330mAh/g) is close to its theoretical value (372mAh/g), it is impossible to meet lithium ion battery of new generation Demand.Therefore, the negative material for developing, designing novel high-capacity is extremely urgent.Silica-base material is due to the theory ratio with superelevation Capacity (highest 4200mAh/g) and relatively low de- lithium current potential (about 0.4V vs Li/Li+), and the voltage platform of silicon is slightly above stone Ink, is difficult to cause surface to analyse lithium in charging, and more preferably, and silicon rich reserves on earth, cost is relatively low for security performance, thus One of rich potential selection as the carbon-based negative pole upgrading of lithium ion battery.
Therefore, with LiCoPO4As positive electrode, using silica-base material as negative material, design, study, developing new High voltage, high security, cobalt phosphate lithium/silica-base material power lithium-ion battery of high-energy-density have important scientific meaning With commercial application value.
The content of the invention
It is an object of the invention to provide it is a kind of with high voltage, high security, high structural stability based on silicium cathode Novel high voltage lithium ion battery and energy storage elements.
A kind of novel high voltage lithium ion battery based on silicium cathode, comprising be capable of the positive pole of reversible embedding de- lithium, negative pole, every Film and electrolyte, it is characterised in that the positive pole is used as positive active material using cobalt phosphate lithium and its compound；The negative pole with Silica-base material is used as negative electrode binder as negative electrode active material using water based adhesive.
Further, cobalt phosphate lithium compound is at least mixed selected from cobalt phosphate lithium/carbon complex, cobalt phosphate lithium/metal ion One kind in miscellaneous compound, cobalt phosphate lithium/conductive polymer composite.
Further, the carbon in described cobalt phosphate lithium/carbon complex at least includes porous, electrically conductive carbon black (KetjenblackEC600JD), micropore superconduction carbon black (BP2000), carbon nano-fiber (CNFs), ordered mesopore carbon (OMC), many One or several kinds in hole carbon (CMK-3), graphene oxide (GO), graphene (Graphene).
Further, the Doped ions in described cobalt phosphate lithium/metal ion mixing compound at least include：Mg2+, Ca2+, Sr2+, Ba2+, Sc3+, Y3+, Ln3+, Ti4+, Zr4+, Hf4+, V4+, V3+, V2+, Ta3+, Cr3+, Mo3+, W3+, Mn2+, Mn3+, Re3+, Re2+, Fe3+, Fe2+, Ru3+, Os3+, Os2+, Co3+, Co2+, Rh2+, Rh+, Ir2+, Ir+, Ni2+, Ni+, Pd2+, Pd+, Pt+, Cu2+, Cu+, Ag+, Au+, Zn2+, Cd2+, Hg2+, Al3+, Ga3+, In3+, Si4+, Si2+, Ge4+, Ge2+, Sn4+, Sn2+, Pb4+, Pb2+In one Plant or several, wherein Ln3+Represent lanthanide ion：La3+, Ce3+, Pr3+, Nd3+, Sm3+, Eu3+, Gd3+, Tb3+, Dy3+, Ho3+, Er3+, Tm3+, Yb3+, Lu3+。
Further, the conducting polymer in described cobalt phosphate lithium/conductive polymer composite at least includes：Polyaniline (PANi), polypyrrole (PPy), polythiophene (PTh), poly- (3,4- ethene dioxythiophenes)/polystyrolsulfon acid (PEDOT/PSS) etc. One or more in conducting polymer.
Further, silica-base material is at least selected from silicon, silicon-metal compound, silicon-non-metal compound, silico-carbo compound In one kind；Water based adhesive is at least selected from gelatin, sodium alginate, sodium carboxymethylcellulose (CMC)/butadiene-styrene rubber (SBR), poly- One kind in acrylate multiple copolymer.
Further, the metal in described silicon-metal compound at least includes in Fe, Mn, Cu, Mg, Ca, Sn, Ni It is one or more of.
Further, described silicon-non-metal compound at least includes Si/SiOx, Si/TiN compounds, Si/TiB2It is compound Thing, Si/Si3N4One or more in compound.
Further, described silico-carbo compound is at least received including silicon/agraphitic carbon, silicon/porous carbon complex, silicon/carbon Mitron compound, silicon/graphene complex, silicon/carbon black compound, silicon/graphite composite, silicon/carbonaceous mesophase spherules compound In one kind；The porous carbon may be selected from the carbon material containing at least one of macropore, mesoporous, micropore, and the carbon black is selected from second One or more in acetylene black, Ketjen black, the one kind or many of the graphite in native graphite, electrographite, modified graphite Kind.
The present invention provides a kind of method for preparing the high-voltage lithium ion batteries, will contain silicon-based anode active material Electrode matches as negative pole with cobalt phosphate lithium and its compound positive pole.
The energy storage elements being made up of described lithium ion battery, it is characterised in that：The form of the lithium ion battery For one kind in button cell, 18650 batteries, soft-package battery, hard steel housing battery.
Compared with prior art, the high voltage lithium based on silica-base material negative pole and cobalt phosphate lithium positive pole that provides of the present invention from Sub- battery, with the characteristics of security is good, specific capacity is high, specific energy is high.Cobalt phosphate lithium positive electrode has high voltage, high safety Property, high structural stability the characteristics of, be expected to turn into a new generation's 5V high voltages, high power capacity, the positive electrode of high-energy-density.
In addition, silicon based anode material relative to lithium metal voltage platform in 0.4V or so, it is more slightly higher than graphite, it is difficult to cause Lithium is analysed on surface, and security is good；Moreover, silicon and lithium can form Li12Si7、Li13Si4、Li7Si3、Li15Si4、Li22Si5Deng alloy, reason By specific capacity highest (Li22Si5) 4200 MAhs/g can be reached.The use of high power capacity silicon-based anode improves full battery Energy density.In addition, silicon based anode material abundance, cheap, with potential application value.
Brief description of the drawings
Fig. 1 is LiCoPO in embodiment 14The charging and discharging curve of positive pole-full battery of silicon/Carbon anode.
Embodiment
Below in conjunction with the accompanying drawings and specific embodiment the present invention is further illustrated, but protection scope of the present invention is simultaneously Not limited to this.
Novel high voltage lithium ion battery of the present invention based on silicium cathode, including can reversible embedding de- lithium just Pole, negative pole, barrier film and electrolyte, it is characterised in that the positive pole is used as positive active material using cobalt phosphate lithium and its compound； The negative pole is used as negative electrode binder using silica-base material as negative electrode active material using water based adhesive.The lithium ion battery Form be button cell, 18650 batteries, soft-package battery, hard steel housing battery in one kind.
Cobalt phosphate lithium compound at least selected from cobalt phosphate lithium/carbon complex, cobalt phosphate lithium/metal ion mixing compound, One kind in cobalt phosphate lithium/conductive polymer composite.Carbon in described cobalt phosphate lithium/carbon complex at least includes porous lead Electrical carbon black (Ketjenblack EC600JD), micropore superconduction carbon black (BP2000), carbon nano-fiber (CNFs), ordered mesopore carbon (OMC), porous carbon (CMK-3), graphene oxide (GO), graphene (Graphene) etc. have high-specific surface area and excellent conduction One or several kinds in the carbon material of performance.Doped ions in described cobalt phosphate lithium/metal ion mixing compound are extremely Include less：Mg2+, Ca2+, Sr2+, Ba2+, Sc3+, Y3+, Ln3+, Ti4+, Zr4+, Hf4+, V4+, V3+, V2+, Ta3+, Cr3+, Mo3+, W3+, Mn2+, Mn3+, Re3+, Re2+, Fe3+, Fe2+, Ru3+, Os3+, Os2+, Co3+, Co2+, Rh2+, Rh+, Ir2+, Ir+, Ni2+, Ni+, Pd2 +, Pd+, Pt+, Cu2+, Cu+, Ag+, Au+, Zn2+, Cd2+, Hg2+, Al3+, Ga3+, In3+, Si4+, Si2+, Ge4+, Ge2+, Sn4+, Sn2+, Pb4+, Pb2+In one or more, wherein Ln3+Represent lanthanide ion：La3+, Ce3+, Pr3+, Nd3+, Sm3+, Eu3+, Gd3+, Tb3+, Dy3+, Ho3+, Er3+, Tm3+, Yb3+, Lu3+.Conducting polymer in described cobalt phosphate lithium/conductive polymer composite is extremely Include less：Polyaniline (PANi), polypyrrole (PPy), polythiophene (PTh), poly- (3,4- ethene dioxythiophenes)/polystyrolsulfon acid (PEDOT/PSS) one or more in conducting polymer such as.The silica-base material at least selected from silicon, silicon-metal compound, One kind in silicon-non-metal compound, silico-carbo compound；Water based adhesive is at least fine selected from gelatin, sodium alginate, carboxymethyl One kind in plain sodium (the CMC)/butadiene-styrene rubber (SBR) of dimension, polyacrylate multiple copolymer.
Metal in described silicon-metal compound at least includes one kind or several in Fe, Mn, Cu, Mg, Ca, Sn, Ni Kind.Described silicon-non-metal compound at least includes Si/SiOx, Si/TiN compounds, Si/TiB2Compound, Si/Si3N4It is multiple One or more in compound.Described silico-carbo compound at least includes silicon/agraphitic carbon, silicon/porous carbon complex, silicon/carbon Nanotube complex, silicon/graphene complex, silicon/carbon black compound, silicon/graphite composite, silicon/carbonaceous mesophase spherules are combined One kind in thing；The porous carbon may be selected from the carbon material containing at least one of macropore, mesoporous, micropore, and the carbon black is selected from One or more in acetylene black, Ketjen black, one kind in native graphite, electrographite, modified graphite of the graphite or It is a variety of.
Experimental method described in following examples, is conventional method unless otherwise specified；The reagent and material, such as Without specified otherwise, commercially obtain.
Embodiment 1：LiCoPO4The assembling of positive pole-full battery of silicon/Carbon anode and its electrochemical property test
(1) preparation of positive pole
By LiCoPO4：Carbon black：Binding agent=(7.5):(2):(0.5) ratio (mass ratio) mixing, after being well mixed, It is coated on aluminium collector, after vacuum dried, section, obtains anode pole piece.
(2) preparation of negative pole
According to silicon/carbon complex：Carbon black：Binding agent (sodium alginate)=(7.5):(2):(0.5) ratio (mass ratio) Mixing, after being well mixed, is coated on copper current collector, after forced air drying, section, obtains cathode pole piece.
(3) assembling of full battery
Microporous polypropylene membrane Celgard2300 (celgard barrier films Co., Ltd of the U.S.) is inserted between a positive electrode and a negative electrode As barrier film, carbonic ester electrolyte [1M LiPF are added6The DMC (dimethyl carbonate) of (lithium hexafluoro phosphate)/EC (ethene carbonic acid Ester) (volume ratio is 1 to/PC (propene carbonate):1:1) solution.
(4) test of full battery
The full battery of the button of above-mentioned assembling is subjected to charge-discharge test on charge-discharge test instrument, the discharge and recharge of test is interval For 2.0-4.5V.Test temperature is 25 DEG C, and the quality that battery capacity and charging and discharging currents are based on positive electrode is calculated.Figure 1 is the LiCoPO4Charging and discharging curve of the full battery of-silicon/carbon under the conditions of 0.1C, charging platform exists in 4.5V, discharge platform 4.3V or so, initial charge capacity is 165mA h/g, and specific discharge capacity can reach 156mAh/g.
In summary, what the present invention was provided has high voltage, high security, high structure steady based on cobalt phosphate lithium positive electrode Qualitative the characteristics of, it is expected to turn into a new generation's 5V high voltages, high power capacity, the positive electrode of high-energy-density.Silicon-based anode has superelevation Specific capacity and excellent security, and the raw material of silicon-based anode is easy to get, and cost is relatively low, thus the present invention cobalt phosphate lithium just Pole-silicon-based anode battery is expected to as a kind of energy storage device that new security is good and energy density is high, should with good Use prospect.The above is only the preferred embodiments of the present invention, is not intended to limit embodiment of the present invention, and this area is common Technical staff can very easily carry out corresponding flexible or modification, therefore this according to the central scope and spirit of the present invention The protection domain of invention should be defined by the protection domain required by claims.

Claims (10)

1. a kind of novel high voltage lithium ion battery based on silicium cathode, including it is capable of positive pole, negative pole, the barrier film of reversible embedding de- lithium And electrolyte, it is characterised in that the positive pole is used as positive active material using cobalt phosphate lithium and its compound；The negative pole is with silicon Sill is used as negative electrode binder as negative electrode active material using water based adhesive.
2. lithium ion battery according to claim 1, it is characterised in that：Cobalt phosphate lithium compound is at least selected from cobalt phosphate One kind in lithium/carbon complex, cobalt phosphate lithium/metal ion mixing compound, cobalt phosphate lithium/conductive polymer composite.
3. lithium ion battery according to claim 2, it is characterised in that：Carbon in described cobalt phosphate lithium/carbon complex At least include porous, electrically conductive carbon black (Ketjenblack EC600JD), micropore superconduction carbon black (BP2000), carbon nano-fiber (CNFs), one kind in ordered mesopore carbon (OMC), porous carbon (CMK-3), graphene oxide (GO), graphene (Graphene) Or it is several.
4. lithium ion battery according to claim 2, it is characterised in that：Described cobalt phosphate lithium/metal ion mixing is multiple Doped ions in compound at least include：Mg2+, Ca2+, Sr2+, Ba2+, Sc3+, Y3+, Ln3+, Ti4+, Zr4+, Hf4+, V4+, V3+, V2+, Ta3+, Cr3+, Mo3+, W3+, Mn2+, Mn3+, Re3+, Re2+, Fe3+, Fe2+, Ru3+, Os3+, Os2+, Co3+, Co2+, Rh2+, Rh+, Ir2 +, Ir+, Ni2+, Ni+, Pd2+, Pd+, Pt+, Cu2+, Cu+, Ag+, Au+, Zn2+, Cd2+, Hg2+, Al3+, Ga3+, In3+, Si4+, Si2+, Ge4+, Ge2+, Sn4+, Sn2+, Pb4+, Pb2+In one or more, wherein Ln3+Represent lanthanide ion：La3+, Ce3+, Pr3+, Nd3+, Sm3+, Eu3+, Gd3+, Tb3+, Dy3+, Ho3+, Er3+, Tm3+, Yb3+, Lu3+。
5. lithium ion battery according to claim 2, it is characterised in that：Described cobalt phosphate lithium/conducting polymer is combined Conducting polymer in thing at least includes：Polyaniline (PANi), polypyrrole (PPy), polythiophene (PTh), poly- (3,4- ethylene dioxies Thiophene) one or more in the conducting polymer such as/polystyrolsulfon acid (PEDOT/PSS).
6. lithium ion battery according to claim 1, it is characterised in that：The silica-base material is at least selected from silicon, silicon-metal One kind in compound, silicon-non-metal compound, silico-carbo compound；Water based adhesive is at least selected from gelatin, sodium alginate, carboxylic One kind in sodium carboxymethylcellulose pyce (CMC)/butadiene-styrene rubber (SBR), polyacrylate multiple copolymer.
7. lithium ion battery according to claim 6, it is characterised in that：Metal in described silicon-metal compound is extremely Include the one or more in Fe, Mn, Cu, Mg, Ca, Sn, Ni less.
8. lithium ion battery according to claim 6, it is characterised in that：Described silicon-non-metal compound at least includes Si/SiOx, Si/TiN compound, Si/TiB2Compound, Si/Si3N4One or more in compound.
9. lithium ion battery according to claim 6, it is characterised in that：Described silico-carbo compound at least includes silicon/nothing Sizing carbon, silicon/porous carbon complex, silicon/carbon mano-tube composite, silicon/graphene complex, silicon/carbon black compound, silicon/stone One kind in black compound, silicon/carbonaceous mesophase spherules compound；The porous carbon may be selected from containing in macropore, mesoporous, micropore extremely A kind of few carbon material, one or more of the carbon black in acetylene black, Ketjen black, the graphite be selected from native graphite, One or more in electrographite, modified graphite.
10. the energy storage elements being made up of the lithium ion battery any one of claim 1-9, it is characterised in that：Institute The form for stating lithium ion battery is one kind in button cell, 18650 batteries, soft-package battery, hard steel housing battery.
CN201710387222.7A 2017-05-27 2017-05-27 A kind of novel high voltage lithium ion battery and energy storage elements based on silicium cathode Pending CN107221699A (en)

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CN109950483A (en) * 2019-02-25 2019-06-28 安徽瑞达机械有限公司 A kind of lithium ion battery modified phosphate cobalt lithium anode material and preparation method thereof
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Application publication date: 20170929