WO2013050283A1 - Cellules lithium-ion présentant des propriétés améliorées - Google Patents

Cellules lithium-ion présentant des propriétés améliorées Download PDF

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Publication number
WO2013050283A1
WO2013050283A1 PCT/EP2012/069010 EP2012069010W WO2013050283A1 WO 2013050283 A1 WO2013050283 A1 WO 2013050283A1 EP 2012069010 W EP2012069010 W EP 2012069010W WO 2013050283 A1 WO2013050283 A1 WO 2013050283A1
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WIPO (PCT)
Prior art keywords
lithium
carbonate
solvent
cell according
ion cell
Prior art date
Application number
PCT/EP2012/069010
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German (de)
English (en)
Inventor
David ENSLING
Original Assignee
Varta Microbattery Gmbh
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Varta Microbattery Gmbh filed Critical Varta Microbattery Gmbh
Publication of WO2013050283A1 publication Critical patent/WO2013050283A1/fr

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Classifications

    • 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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • 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
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0568—Liquid materials characterised by the solutes
    • 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
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0569—Liquid materials characterised by the solvents
    • 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
    • H01M10/04—Construction or manufacture in general
    • H01M10/0422—Cells or battery with cylindrical casing
    • H01M10/0427—Button cells
    • 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
    • H01M10/04—Construction or manufacture in general
    • H01M10/0431—Cells with wound or folded electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H01M2300/0028—Organic electrolyte characterised by the solvent
    • H01M2300/0037—Mixture of solvents
    • H01M2300/004—Three solvents
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H01M2300/0028—Organic electrolyte characterised by the solvent
    • H01M2300/0037—Mixture of solvents
    • H01M2300/0042—Four or more solvents
    • 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

Definitions

  • the present invention relates to a lithium-ion cell having at least one negative and at least one positive electrode, which are connected to one another via an ion-conducting electrolyte, wherein the electrolyte comprises a solvent and a conductive salt component dissolved therein.
  • battery originally meant several galvanic cells connected in series, but today also individual galvanic cells are often referred to as "battery.”
  • an energy-supplying chemical reaction takes place, which consists of two electrically coupled but spatially separated partial reactions
  • a partial reaction taking place at a comparatively lower redox potential takes place at the negative electrode, one with a comparatively higher redox potential at the positive electrode
  • electrons are released at the negative electrode by an oxidation process, resulting in an electron current via an external consumer to the positive one Electrode, from which a corresponding amount of electrons is taken in.
  • a reduction process takes place.
  • a lonenstr om inside the cell.
  • electrochemically active components for lithium-ion batteries are basically all materials in question, which can absorb lithium ions and release again.
  • the state of the art in this regard for the negative electrode in particular carbon-based particles such as graphitic carbon or for the intercalation of lithium capable non-graphitic carbon materials.
  • metallic and semi-metallic materials which can be alloyed with lithium.
  • the elements tin, antimony and silicon are able to form intermetallic phases with lithium.
  • the active materials industrially used at this time mainly include lithium cobalt oxide (L1CO 2), LiMn 2 O 4 spinel (LiMn 2 O 4 ), lithium iron phosphate (LiFePO 4 ), and derivatives such as LiNii / 3 Mni / 3 Coi / 302 or LiMnP0 4 . All electrochemically active materials are usually contained in the form of particles in the electrodes.
  • Electrode binders and current conductors should be mentioned in the first place. Via current conductors, the transport of the electrons from and to the electrodes takes place. Electrode binders ensure the mechanical stability of the electrodes as well as the mutual contacting of the particles of the electrochemically active material and their connection to the current conductors. To improve the electrical connection of the electrochemically active particles to the current conductor conductivity-enhancing additives contribute, which are also subsumed under the collective term "electrochemically inactive components.” All electrochemically inactive components should be at least in the potential range of the respective electrode electrochemically stable and a chemically inert character have compared to common electrolyte solutions. Common electrolyte solutions include solutions of lithium salts such as lithium hexafluorophosphate (LiPF 6 ) in organic solvents such as ethers or esters of carbonic acid.
  • LiPF 6 lithium hexafluorophosphate
  • This topcoat is referred to as "Solid Electrolyte Interphase” (SEI) and is usually composed primarily of electrolyte decomposition products and a certain amount of lithium, which is accordingly no longer available for further charge / discharge reactions
  • SEI Solid Electrolyte Interphase
  • the SEI is ideally However, it is also an obstacle for the extremely small lithium ions, but this is an obstacle during charging and discharging processes.
  • Another important feature of the SEI is that it prevents further direct contact of the electrolyte solution with the electrochemically active components in the anode, thereby protecting it from further decomposition.
  • EP 0 683 537 B1 describes lithium-ion cells which have a negative electrode comprising a carbon material having a degree of crystallinity of more than 80%, wherein the electrolyte used is a mixture of two organic solvents (ethylene carbonate and dimethyl carbonate) and a Lithium salt is used.
  • the electrolyte contains as an additive vinylene carbonate or a vinyl carbonate derivative, which is added to selectively form an SEI during the formation.
  • a better stability of the cells at higher temperatures, in particular at 60 ° C, should be ensured.
  • Lithium-ion cells according to the invention like the generic lithium-ion cells mentioned at the beginning, have at least one negative and at least one positive electrode, which are connected via an ionic lead.
  • electrolyte which electrolyte comprises a solvent and a conductive salt component dissolved therein.
  • the solvent contains at least one, preferably at least two, carbonates from the group comprising diethyl carbonate (DEC), dimethyl carbonate (DMC), ethyl methyl carbonate (EMC) and propylene carbonate (PC) in addition to ethylene carbonate (EC). includes.
  • DEC diethyl carbonate
  • DMC dimethyl carbonate
  • EMC ethyl methyl carbonate
  • PC propylene carbonate
  • EC ethylene carbonate
  • EC, DEC, DMC, EMC and PC belong to the organic carbonates (acyclic and cyclic carbonic acid esters) and are highly volatile, polar solvents, which are characterized among other things by their low toxicity.
  • the solvent comprises at least three of said carbonates, in particular the components EC, DEC and EMC or it consists of said components.
  • the electrolyte of a lithium ion cell according to the invention may additionally comprise at least one co-solvent from the group comprising butylene carbonate (BC), dipropyl carbonate (DPC), methyl propyl carbonate (MPC) and ethyl propyl carbonate (EPC).
  • the proportion of the cosolvent optionally is preferably below 10%, based on the total weight of all components of the electrolyte which are liquid at room temperature and normal pressure.
  • the electrolyte contains the components EC and DEC and / or DMC and / or EMC and / or PC and optionally the co-solvent in the following proportions:
  • DEC Between 5 and 85%, preferably between 5 and 80%, more preferably between 10 and 60%, DEC between 5 and 85%, preferably between 5 and 80%, particularly preferably between 10 and 60%, DMC
  • EMC EMC
  • the stated percentages represent preferred ranges for the individual components, regardless of the combination in which the components are actually present in the solvent. Incidentally, the percentages are in each case percent by weight, based on the total weight of all components of the electrolyte which are liquid at room temperature and normal pressure. In the electrolyte, the respective proportions add up to 100%.
  • the solvent has the three components EC, DEC and EMC in each case in the same proportions, ie in a ratio of 1: 1: 1.
  • mixtures which, in addition to EC, comprise at least one, preferably at least two components from the group comprising DEC, DMC, EMC and PC, in particular the said preferred mixtures, are particularly suitable as electrolyte components of lithium-ion cells, in particular if they are in the proportions indicated.
  • the cycle behavior of a secondary lithium-ion cell according to the invention in a temperature range between -20 ° C and 60 ° C can be significantly improved. Especially at an elevated temperature of 60 ° C, significant improvements were observed.
  • the conductive salt component dissolved in the solvent is particularly preferably a mixture of at least two lithium salts, in particular a mixture which contains, in addition to a fluorinated lithium phosphate (lithium fluorophosphate), at least one further lithium salt, preferably a lithium borate and / or a lithium alkylsulfonylimide.
  • a fluorinated lithium phosphate lithium fluorophosphate
  • at least one further lithium salt preferably a lithium borate and / or a lithium alkylsulfonylimide.
  • the lithium fluorophosphate is particularly preferably lithium hexafluorophosphate (LiPF 6 ).
  • the at least one further lithium salt is preferably selected from the group comprising lithium bis (oxalato) borate (LiBOB), lithium difluoro (oxalato) borate (LiFOB), lithium (fluorosulfonyl) (nonafluorobutanesulfonyl) imide (LiFNFSI), lithium (trifluoromethanesulfonyl) imide (LiTFSI) and mixtures selected from the lithium salts mentioned.
  • the conductive salt component is a mixture which, in addition to a lithium fluorophosphate, in particular LiPF 6 , as further lithium salt (s) lithium bis (oxalato) borate (LiBOB) and / or lithium difluoro (oxalato) borate ( LiFOB).
  • a lithium fluorophosphate in particular LiPF 6
  • LiBOB lithium bis (oxalato) borate
  • LiFOB lithium difluoro (oxalato) borate
  • the cycle stability and also the current-carrying capacity of the lithium-ion cells according to the invention could in some cases be drastically increased. This is especially true for the combination of lithium hexafluorophosphate with LiBOB. It is believed that these positive effects are due to the formation of a particularly stable SEI on the surface of the active materials.
  • the lithium fluorophosphate in a molar concentration between 0.1 and 4.0 M, preferably between 0.5 and 2 , 0 M, in particular between 0.8 and 1, 4 M to add.
  • a molar concentration between 0.01 and 1.0 M, preferably between 0.05 and 0.5 M, in particular between 0.1 and 0.3 M has proven to be particularly advantageous.
  • the weight ratio of the lithium fluorophosphate to the at least one further conductive salt in the conductive salt component should, in preferred embodiments, be in a range between 20: 1 and 4: 1, especially about 10: 1, to achieve the above effects.
  • the electrolyte of a lithium-ion cell according to the invention comprises at least one additive, in particular from the group with vinylene carbonate (VC), cyclohexylbenzene (CHB), biphenyl (BP), diphenyl ether (DPE), toluene (TOL), xylene (XYL), 1,3-propane sultone (PS), propensultone (PRS), butane sultone (BS), propylmethane sulfonate (PMS), thiophene (TP) and succinic anhydride (BSA).
  • VC vinylene carbonate
  • CHB cyclohexylbenzene
  • BP biphenyl
  • DPE diphenyl ether
  • TOL toluene
  • XYL 1,3-propane sultone
  • PS propensultone
  • BS butane sultone
  • PMS propylmethane sulfonate
  • the electrolyte contains the components EC and DEC and / or DMC and / or EMC and / or PC and optionally the co-solvent and / or the at least one additive in the following proportions:
  • DEC DEC
  • DMC Between 5 and 85%, preferably between 5 and 80%, particularly preferably between 10 and 60%, DMC between 5 and 85%, preferably between 5 and 80%, more preferably between 10 and 60%, EMC
  • the percentages given are representative of the individual components, regardless of the combination of the components actually present in the solvent.
  • the percentages here are also percentages by weight, based on the total weight of all components of the electrolyte which are liquid at room temperature and normal pressure. In the electrolyte, the respective proportions add up to 100%.
  • the carbonate additive VC can significantly improve the performance of a lithium-ion cell. Due to the low dissociation energies of the carbonate-carbon bond in the VC, it competes with electrolytic solvents during SEI formation, it reacts preferentially with electrochemical active materials. As a consequence, the chemical composition and probably also the morphology of the SEI is likely to change. This has a particularly positive effect on the safety properties of the lithium-ion cell according to the invention, since the decomposition of the electrolyte can be at least partially prevented.
  • the VC is added in amounts of at most between 0.1 and 2 wt .-%, based on the total mass of the electrolyte, since it can otherwise lead to increased gassing of the cell.
  • at least one further stabilizing additive may also be added to the electrolyte.
  • PS, PRS, PMS and / or BS are preferably used according to the invention for this purpose.
  • CHB, XYL, TOL, DPE and BP are preferably added to the electrolyte of a lithium-ion cell according to the invention as an overcharge additive, in particular in a proportion of 1 to 5% by weight, based on the total mass of the electrolyte. If a cell according to the invention is overloaded, these additives prevent or slow down a decomposition reaction and heat generation.
  • a lithium-ion cell according to the invention is, in particular, a cell in which the at least one negative and the at least one positive electrode are formed as flat layers and are constituents of an electrode-separator composite which is present as a coil.
  • the lithium-ion cell according to the invention is housed in a button cell housing, particularly preferably in a housing, as described in DE 10 2009 008 859 A1.
  • a button cell housing particularly preferably in a housing, as described in DE 10 2009 008 859 A1.
  • the content of this document is hereby incorporated by reference into the content of this specification.
  • the electrolyte contained 1 M LiPF 6 as conductive salt component
  • the electrolyte contained a mixture of EC and DEC in the weight ratio 4: 5 (EC: DEC)
  • the electrolyte contained 2% by weight BS, 2% by weight CHB and 0.5% by weight VC
  • Electrolyte 1 (according to the invention)
  • the conductive salt component contained 0.9 M LiPF 6 and 0.1 M LiBOB
  • the electrolyte contained a mixture of EC, DEC and EMC in the weight ratio 1: 1: 1 (EC: DEC: EMC)
  • the electrolyte contained 5 wt .-% PC
  • the electrolyte contained 3 wt .-% PS, 0.5 wt .-% VC and 0.1 wt .-% TP
  • Electrolyte 2 (according to the invention)
  • the conductive salt component contained 0.9 M LiPF 6 and 0.1 M LiBOB
  • the electrolyte contained a mixture of EC, DEC and EMC in the weight ratio 1: 1: 1 (EC: DEC: EMC)
  • the electrolyte contained 5 wt .-% PC
  • the electrolyte contained 3 wt .-% PS, 1, 5 wt .-% CHB, 0.5 wt .-% VC, 2 wt .-% TP and 0.5 wt .-% BP
  • Cells with the reference electrolyte and the electrolytes 1 and 2 were cycled at 60 ° C in the voltage range between 3.0 and 4.2V.
  • the charge / discharge rate was 1 C / 1 C in cccv mode (cv limit C / 50).
  • the observed drop in the discharge capacity is shown in FIG. It can be clearly seen that the cells with the electrolyte 1 and 2 have a significantly higher cycle stability compared to the cells with the reference electrolyte.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)

Abstract

L'invention concerne une cellule lithium-ion comprenant au moins une électrode négative et au moins une électrode positive, qui sont interconnectées par l'intermédiaire d'un électrolyte conducteur d'ions, ledit électrolyte comprenant un solvant et un composant sel conducteur dissous dedans et ledit solvant contenant, outre du carbonate d'éthylène, au moins deux carbonates du groupe comprenant carbonate de diéthyle, carbonate de diméthyle, éthylméthylcarbonate et carbonate de propylène ainsi qu'éventuellement également au moins un cosolvant du groupe comprenant carbonate de butylène, carbonate de dipropyle, méthylpropylcarbonate et éthylpropylcarbonate.
PCT/EP2012/069010 2011-10-05 2012-09-26 Cellules lithium-ion présentant des propriétés améliorées WO2013050283A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102011084009A DE102011084009A1 (de) 2011-10-05 2011-10-05 Lithium-Ionen-Zellen mit verbesserten Eigenschaften
DE102011084009.5 2011-10-05

Publications (1)

Publication Number Publication Date
WO2013050283A1 true WO2013050283A1 (fr) 2013-04-11

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