USH723H - Lithium electrochemical cell containing diethylcarbonate as an electrolyte solvent additive - Google Patents
Lithium electrochemical cell containing diethylcarbonate as an electrolyte solvent additive Download PDFInfo
- Publication number
- USH723H USH723H US07/215,664 US21566488A USH723H US H723 H USH723 H US H723H US 21566488 A US21566488 A US 21566488A US H723 H USH723 H US H723H
- Authority
- US
- United States
- Prior art keywords
- lithium
- electrochemical cell
- diethylcarbonate
- electrolyte
- coo
- Prior art date
- Legal status (The legal status 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 status listed.)
- Abandoned
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Images
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
- H01M10/056—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
- H01M10/05—Accumulators with non-aqueous electrolyte
-
- 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
-
- 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
Definitions
- This invention relates in general to a lithium electrochemical cell and in particular, to a lithium electrochemical cell including lithium as the anode, the lithium intercalating compound Li x CoO 2 (0 ⁇ x ⁇ 1) as the cathode, and a solution of a lithium salt in a mixed organic solvent of methyl formate (MF) and diethylcarbonate (DEC) as the electrolyte.
- a lithium electrochemical cell including lithium as the anode, the lithium intercalating compound Li x CoO 2 (0 ⁇ x ⁇ 1) as the cathode, and a solution of a lithium salt in a mixed organic solvent of methyl formate (MF) and diethylcarbonate (DEC) as the electrolyte.
- MF methyl formate
- DEC diethylcarbonate
- Li x CoO 2 (0 ⁇ x ⁇ 1) is particularly attractive for battery applications because of its inherently high energy content.
- the known Li x CoO 2 cathode material/solvent combinations are susceptible to oxidation during charge and reduction during discharge that results in losses in cell capacity and cycle-life.
- both the cathode and anode are subject to reaction with the solvent and electrolyte. This can result in poor lithium cyclability and structural rearrangement of the active material which may limit rechargeability.
- the general object of this invention is to provide an improved lithium electrochemical cell including Li x CoO 2 (0 ⁇ x ⁇ 1) as the cathode active material.
- a more particular object of the invention is to provide an intercalating solvent system for Li x CoO 2 (0 ⁇ x ⁇ 1) that produces higher energy lithium cells also characterized by increased resistance to solvent oxidation and improved lithium cycling efficiencies.
- the solution can be, for example, 1 to 2 mol dm -3 LiAsF 6 in the mixed organic solvent.
- LiAsF 6 as the electrolyte salt
- other electrolyte salts can be used such as the soluble salts of light metals, for example, tetrafluoroborates, tetrachloroaluminates, perchlorates, hexafluorophosphates, and halides of lithium.
- the mass percent of the DEC in the mixed organic solvent can vary from 10 to 100 mass percent.
- the instant invention identifies and demonstrates that the addition of DEC to ester containing electrolytes, such as LiAsF 6 in MF, results in significant improvements in the electrolytes resistance to electrochemical oxidation and improved lithium cycling efficiencies.
- these electrolytes containing the DEC additives are used in Li/Li x CoO 2 electrochemical cells, there is significant improvements in the cell cycling behavior over cells without the DEC additive.
- the drawing compares cycling results obtained for additions of DEC and dimethylcarbonate (DMC) to LiAsF 6 in MF electrolyte in a Li/Li x CoO 2 electrochemical cell.
- DEC dimethylcarbonate
- the drawing shows the dramatic improvement in cycling behavior for the electrolyte containing DEC as opposed to DMC.
- the Li/Li x CoO 2 cells are cycled between either 4.3 V to 3.5 V or 4.3 V to 2.5 V where the charging rate is 0.5 mAcm 2 , the discharge rate is 2 0 mAcm 2 , and the temperature is 25° C.
- the Li x CoO 2 cathodes include a mixture of 80 weight percent Li x CoO 2 , 10 weight percent carbon diluent, and 10 weight percent Teflon binder. The cathode mixture is roll pressed onto aluminum substrates and sintered in a vacuum oven at 280° C. for 1 hour.
- the cycling is performed on identically prepared cells consisting of flag electrodes sealed in a glass pressure vessel where Celgard 2400 is used as separators and a glass fiber wick for drawing electrolyte in between the electrode.
- DMC homologues of DEC
- DMC has been utilized in lithium cells and are known to be sufficiently stable towards lithium.
- DMC and DEC show structural similarities, they behave very differently in the presence of lithium, both chemically and electrochemically.
- DMC produces a high cycling efficiency of 80 percent as compared to DEC which is 0 percent. This is due to the reactive nature of DEC with lithium as opposed to the more stable DMC solvent.
- DMC is more stable with lithium, its addition to the LiAsF 6 -MF electrolyte does not result in the improved results observed with DEC.
- DEC as a solvent additive in electrolytes for use in either primary, rechargeable, or reserve electrochemical cells is not considered to be limited to the instance where lithium is the anode. That is, other light metals or composites may be applicable as the anode such as sodium, potassium and aluminum, or any conductively doped polymeric material or similar compound.
- the positive electrode or cathode may be any oxide, sulfide or combinations of titanium, vanadium, chromium, manganese, iron, cobalt, nickel, copper, zinc, zirconium, niobium, molybdenum, hafnium, tantalum, or tungsten or any conductively doped polymeric material or similar compound.
Abstract
An electrochemical cell comprising lithium as the anode, the lithium intelating compound Lix CoO2 (O<X<1) as the cathode, and a solution of a lithium salt in a mixed organic solvent of methylformate and diethylcarbonate as the electrolyte.
Description
The invention described herein may be manufactured, used, and licensed by or for the Government for governmental purposes without the payment to us of any royalty thereon.
This invention relates in general to a lithium electrochemical cell and in particular, to a lithium electrochemical cell including lithium as the anode, the lithium intercalating compound Lix CoO2 (0<x<1) as the cathode, and a solution of a lithium salt in a mixed organic solvent of methyl formate (MF) and diethylcarbonate (DEC) as the electrolyte.
This application is copending with U.S. patent application Ser. No. 125,642, filed Nov. 1, 1987, now U.S. Pat. No. 4,786,499 for "Lithium Electrochemical Cell Including Aprotic Solvent-Dialkyl Carbonate Solvent Mixture" and assigned to a common assignee. In that application, there is described and claimed a lithium electrochemical cell including lithium as the anode, non-stoichiometric (NS)-V6 O13 as the cathode, and a solution of a lithium salt in a mixed organic solvent of methyl formate and diethylcarbonate as the electrolyte.
Another lithium intercalating compound, to wit, Lix CoO2 (0<x<1) is particularly attractive for battery applications because of its inherently high energy content. However, the known Lix CoO2 cathode material/solvent combinations are susceptible to oxidation during charge and reduction during discharge that results in losses in cell capacity and cycle-life. In addition to oxidation and reduction of the electrolyte, both the cathode and anode are subject to reaction with the solvent and electrolyte. This can result in poor lithium cyclability and structural rearrangement of the active material which may limit rechargeability.
The general object of this invention is to provide an improved lithium electrochemical cell including Lix CoO2 (0<x<1) as the cathode active material. A more particular object of the invention is to provide an intercalating solvent system for Lix CoO2 (0<x<1) that produces higher energy lithium cells also characterized by increased resistance to solvent oxidation and improved lithium cycling efficiencies.
It has now been found that the aforementioned objects can be attained by employing a system including lithium as the anode, Lix CoO2 (0<x<1) as the cathode, and a solution of a lithium salt in a mixed organic solvent of MF and DEC as the electrolyte.
The solution can be, for example, 1 to 2 mol dm-3 LiAsF6 in the mixed organic solvent. Though the use of LiAsF6 as the electrolyte salt is preferred, other electrolyte salts can be used such as the soluble salts of light metals, for example, tetrafluoroborates, tetrachloroaluminates, perchlorates, hexafluorophosphates, and halides of lithium.
The mass percent of the DEC in the mixed organic solvent can vary from 10 to 100 mass percent. The instant invention identifies and demonstrates that the addition of DEC to ester containing electrolytes, such as LiAsF6 in MF, results in significant improvements in the electrolytes resistance to electrochemical oxidation and improved lithium cycling efficiencies. In addition, when these electrolytes containing the DEC additives are used in Li/Lix CoO2 electrochemical cells, there is significant improvements in the cell cycling behavior over cells without the DEC additive.
The drawing compares cycling results obtained for additions of DEC and dimethylcarbonate (DMC) to LiAsF6 in MF electrolyte in a Li/Lix CoO2 electrochemical cell.
The drawing shows the dramatic improvement in cycling behavior for the electrolyte containing DEC as opposed to DMC. The Li/Lix CoO2 cells are cycled between either 4.3 V to 3.5 V or 4.3 V to 2.5 V where the charging rate is 0.5 mAcm2, the discharge rate is 2 0 mAcm2, and the temperature is 25° C. The Lix CoO2 cathodes include a mixture of 80 weight percent Lix CoO2, 10 weight percent carbon diluent, and 10 weight percent Teflon binder. The cathode mixture is roll pressed onto aluminum substrates and sintered in a vacuum oven at 280° C. for 1 hour. The cycling is performed on identically prepared cells consisting of flag electrodes sealed in a glass pressure vessel where Celgard 2400 is used as separators and a glass fiber wick for drawing electrolyte in between the electrode.
Interestingly, homologues of DEC such as DMC have been utilized in lithium cells and are known to be sufficiently stable towards lithium. However, although DMC and DEC show structural similarities, they behave very differently in the presence of lithium, both chemically and electrochemically. DMC produces a high cycling efficiency of 80 percent as compared to DEC which is 0 percent. This is due to the reactive nature of DEC with lithium as opposed to the more stable DMC solvent. However, even though DMC is more stable with lithium, its addition to the LiAsF6 -MF electrolyte does not result in the improved results observed with DEC. Therefore, where the successful use of DMC as a solvent in lithium cells may imply the possible use of a similar solvent such as DEC, this is not made obvious due to the lack of lithium stability of the neat DEC electrolyte, thus precluding such applications. Furthermore, one would not find obvious the discovery that a mixture of the unstable solvent DEC with another solvent would produce an improved mixture suitably stable for use in a lithium cell. It is only through its addition to other ester electrolytes that the use of DEC in lithium cells is possible.
The use of DEC as a solvent additive in electrolytes for use in either primary, rechargeable, or reserve electrochemical cells is not considered to be limited to the instance where lithium is the anode. That is, other light metals or composites may be applicable as the anode such as sodium, potassium and aluminum, or any conductively doped polymeric material or similar compound. Moreover, the positive electrode or cathode, may be any oxide, sulfide or combinations of titanium, vanadium, chromium, manganese, iron, cobalt, nickel, copper, zinc, zirconium, niobium, molybdenum, hafnium, tantalum, or tungsten or any conductively doped polymeric material or similar compound.
We wish it to be understood that we do not desire to be limited to the exact details as described for obvious modifications will occur to a person skilled in the art.
Claims (5)
1. An electrochemical cell comprising lithium as the anode, the lithium intercalating compound Lix CoO2 (0<x<1) as the cathode, and a solution of a lithium salt in a mixed organic solvent of methylformate and diethylcarbonate as the electrolyte.
2. An electrochemical cell according to claim 1 wherein the mass percent of the diethylcarbonate in the mixed organic solvent of methylformate and diethylcarbonate can vary from about 10 to 100 mass percent in the electrolyte.
3. An electrochemical cell according to claim 2 wherein the solution of lithium salt is 1-2 mol dm-3 LiAsF6 in methylformate.
4. An electrochemical cell according to claim 1 wherein the Lix CoO2 cathode consists of a mixture of about 80 weight percent Lix CoO2, about 10 weight percent carbon diluent and about 10 weight percent Teflon binder roll pressed onto aluminum substrates and sintered in a vacuum oven at 280° C. for 1 hour.
5. An electrochemical cell according to claim 4 wherein the mass percent of the diethylcarbonate in the mixed organic solvent of methylformate and diethylcarbonate can vary from about 10 to 100 mass percent in the electrolyte and wherein the solution of lithium salt is 1-2 mol dm-3 LiAsF6 in methylformate.
Priority Applications (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US07/215,664 USH723H (en) | 1988-07-06 | 1988-07-06 | Lithium electrochemical cell containing diethylcarbonate as an electrolyte solvent additive |
CA000599186A CA1306001C (en) | 1988-07-06 | 1989-04-19 | Lithium electrochemical cell containing diethylcarbonate asan electrolyte solvent additive |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US07/215,664 USH723H (en) | 1988-07-06 | 1988-07-06 | Lithium electrochemical cell containing diethylcarbonate as an electrolyte solvent additive |
Publications (1)
Publication Number | Publication Date |
---|---|
USH723H true USH723H (en) | 1990-01-02 |
Family
ID=22803877
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
US07/215,664 Abandoned USH723H (en) | 1988-07-06 | 1988-07-06 | Lithium electrochemical cell containing diethylcarbonate as an electrolyte solvent additive |
Country Status (2)
Country | Link |
---|---|
US (1) | USH723H (en) |
CA (1) | CA1306001C (en) |
Cited By (16)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US5147739A (en) * | 1990-08-01 | 1992-09-15 | Honeywell Inc. | High energy electrochemical cell having composite solid-state anode |
US5284721A (en) * | 1990-08-01 | 1994-02-08 | Alliant Techsystems Inc. | High energy electrochemical cell employing solid-state anode |
US20060093917A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20060093923A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20060093872A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20060093913A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20060093873A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Lithium-ion battery |
US20060093871A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Lithium-ion battery |
US20080020279A1 (en) * | 2004-10-29 | 2008-01-24 | Medtronic, Inc. | Lithium-ion battery |
US20080020278A1 (en) * | 2004-10-29 | 2008-01-24 | Medtronic, Inc. | Lithium-ion battery |
US20090274849A1 (en) * | 2008-04-30 | 2009-11-05 | Medtronic, Inc. | Formation process for lithium-ion batteries |
US7635541B2 (en) | 2004-10-29 | 2009-12-22 | Medtronic, Inc. | Method for charging lithium-ion battery |
US7927742B2 (en) | 2004-10-29 | 2011-04-19 | Medtronic, Inc. | Negative-limited lithium-ion battery |
US9077022B2 (en) | 2004-10-29 | 2015-07-07 | Medtronic, Inc. | Lithium-ion battery |
US9287580B2 (en) | 2011-07-27 | 2016-03-15 | Medtronic, Inc. | Battery with auxiliary electrode |
US9587321B2 (en) | 2011-12-09 | 2017-03-07 | Medtronic Inc. | Auxiliary electrode for lithium-ion battery |
-
1988
- 1988-07-06 US US07/215,664 patent/USH723H/en not_active Abandoned
-
1989
- 1989-04-19 CA CA000599186A patent/CA1306001C/en not_active Expired - Fee Related
Cited By (47)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US5147739A (en) * | 1990-08-01 | 1992-09-15 | Honeywell Inc. | High energy electrochemical cell having composite solid-state anode |
US5284721A (en) * | 1990-08-01 | 1994-02-08 | Alliant Techsystems Inc. | High energy electrochemical cell employing solid-state anode |
US20100009245A1 (en) * | 2004-10-29 | 2010-01-14 | Medtronic,Inc. | Lithium-ion battery |
US7883790B2 (en) | 2004-10-29 | 2011-02-08 | Medtronic, Inc. | Method of preventing over-discharge of battery |
US20060093916A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Lithium-ion battery |
US7662509B2 (en) | 2004-10-29 | 2010-02-16 | Medtronic, Inc. | Lithium-ion battery |
US20060093918A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Lithium-ion battery |
US20060093913A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20060093873A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Lithium-ion battery |
US20060093871A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Lithium-ion battery |
US20060093921A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Lithium-ion battery |
US20080020279A1 (en) * | 2004-10-29 | 2008-01-24 | Medtronic, Inc. | Lithium-ion battery |
US20080020278A1 (en) * | 2004-10-29 | 2008-01-24 | Medtronic, Inc. | Lithium-ion battery |
US7337010B2 (en) | 2004-10-29 | 2008-02-26 | Medtronic, Inc. | Medical device having lithium-ion battery |
US7563541B2 (en) | 2004-10-29 | 2009-07-21 | Medtronic, Inc. | Lithium-ion battery |
US20090208845A1 (en) * | 2004-10-29 | 2009-08-20 | Medtronic, Inc. | Lithium-ion battery |
US7582387B2 (en) | 2004-10-29 | 2009-09-01 | Medtronic, Inc. | Lithium-ion battery |
US7682745B2 (en) | 2004-10-29 | 2010-03-23 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20090286158A1 (en) * | 2004-10-29 | 2009-11-19 | Medtronic, Inc. | Lithium-ion battery |
US20100076523A1 (en) * | 2004-10-29 | 2010-03-25 | Medtronic, Inc. | Method of preventing over-discharge of battery |
US7641992B2 (en) | 2004-10-29 | 2010-01-05 | Medtronic, Inc. | Medical device having lithium-ion battery |
US7642013B2 (en) | 2004-10-29 | 2010-01-05 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20060093917A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20100015528A1 (en) * | 2004-10-29 | 2010-01-21 | Medtronic, Inc. | Lithium-ion battery |
US20060093872A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Medical device having lithium-ion battery |
US9077022B2 (en) | 2004-10-29 | 2015-07-07 | Medtronic, Inc. | Lithium-ion battery |
US7635541B2 (en) | 2004-10-29 | 2009-12-22 | Medtronic, Inc. | Method for charging lithium-ion battery |
US7740985B2 (en) | 2004-10-29 | 2010-06-22 | Medtronic, Inc. | Lithium-ion battery |
US7794869B2 (en) | 2004-10-29 | 2010-09-14 | Medtronic, Inc. | Lithium-ion battery |
US20100239908A1 (en) * | 2004-10-29 | 2010-09-23 | Medtronic, Inc. | Lithium-ion battery |
US7803481B2 (en) | 2004-10-29 | 2010-09-28 | Medtronic, Inc, | Lithium-ion battery |
US7807299B2 (en) | 2004-10-29 | 2010-10-05 | Medtronic, Inc. | Lithium-ion battery |
US7811705B2 (en) | 2004-10-29 | 2010-10-12 | Medtronic, Inc. | Lithium-ion battery |
US7858236B2 (en) | 2004-10-29 | 2010-12-28 | Medtronic, Inc. | Lithium-ion battery |
US7875389B2 (en) | 2004-10-29 | 2011-01-25 | Medtronic, Inc. | Lithium-ion battery |
US7879495B2 (en) | 2004-10-29 | 2011-02-01 | Medtronic, Inc. | Medical device having lithium-ion battery |
US20060093923A1 (en) * | 2004-10-29 | 2006-05-04 | Medtronic, Inc. | Medical device having lithium-ion battery |
US7927742B2 (en) | 2004-10-29 | 2011-04-19 | Medtronic, Inc. | Negative-limited lithium-ion battery |
US7931987B2 (en) | 2004-10-29 | 2011-04-26 | Medtronic, Inc. | Lithium-ion battery |
US8105714B2 (en) | 2004-10-29 | 2012-01-31 | Medtronic, Inc. | Lithium-ion battery |
US9065145B2 (en) | 2004-10-29 | 2015-06-23 | Medtronic, Inc. | Lithium-ion battery |
US8980453B2 (en) | 2008-04-30 | 2015-03-17 | Medtronic, Inc. | Formation process for lithium-ion batteries |
US9899710B2 (en) | 2008-04-30 | 2018-02-20 | Medtronic, Inc. | Charging process for lithium-ion batteries |
US20090274849A1 (en) * | 2008-04-30 | 2009-11-05 | Medtronic, Inc. | Formation process for lithium-ion batteries |
US10615463B2 (en) | 2008-04-30 | 2020-04-07 | Medtronic, Inc. | Formation process for lithium-ion batteries with improved tolerace to overdischarge conditions |
US9287580B2 (en) | 2011-07-27 | 2016-03-15 | Medtronic, Inc. | Battery with auxiliary electrode |
US9587321B2 (en) | 2011-12-09 | 2017-03-07 | Medtronic Inc. | Auxiliary electrode for lithium-ion battery |
Also Published As
Publication number | Publication date |
---|---|
CA1306001C (en) | 1992-08-04 |
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