GB2084789A - Galvanic cell - Google Patents
Galvanic cell Download PDFInfo
- Publication number
- GB2084789A GB2084789A GB8125181A GB8125181A GB2084789A GB 2084789 A GB2084789 A GB 2084789A GB 8125181 A GB8125181 A GB 8125181A GB 8125181 A GB8125181 A GB 8125181A GB 2084789 A GB2084789 A GB 2084789A
- Authority
- GB
- United Kingdom
- Prior art keywords
- electrolyte
- galvanic cell
- cell according
- dimethyl ether
- cell
- 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.)
- Granted
Links
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical compound COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 claims abstract description 30
- 239000003792 electrolyte Substances 0.000 claims abstract description 28
- WDXYVJKNSMILOQ-UHFFFAOYSA-N 1,3,2-dioxathiolane 2-oxide Chemical compound O=S1OCCO1 WDXYVJKNSMILOQ-UHFFFAOYSA-N 0.000 claims abstract description 17
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 claims abstract description 17
- 150000003839 salts Chemical class 0.000 claims abstract description 11
- 239000000203 mixture Substances 0.000 claims abstract description 9
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 7
- 229910019923 CrOx Inorganic materials 0.000 claims abstract description 6
- 229910001540 lithium hexafluoroarsenate(V) Inorganic materials 0.000 claims abstract description 6
- 229910001290 LiPF6 Inorganic materials 0.000 claims abstract description 5
- 239000011255 nonaqueous electrolyte Substances 0.000 claims abstract description 4
- XMFOQHDPRMAJNU-UHFFFAOYSA-N lead(II,IV) oxide Inorganic materials O1[Pb]O[Pb]11O[Pb]O1 XMFOQHDPRMAJNU-UHFFFAOYSA-N 0.000 claims abstract description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 7
- 239000002808 molecular sieve Substances 0.000 claims description 2
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 2
- 238000004821 distillation Methods 0.000 claims 2
- 239000002904 solvent Substances 0.000 abstract description 12
- 238000009835 boiling Methods 0.000 abstract description 11
- WMWLMWRWZQELOS-UHFFFAOYSA-N bismuth(iii) oxide Chemical compound O=[Bi]O[Bi]=O WMWLMWRWZQELOS-UHFFFAOYSA-N 0.000 abstract description 5
- 239000007772 electrode material Substances 0.000 abstract description 3
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 abstract description 3
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 abstract 1
- 229910001486 lithium perchlorate Inorganic materials 0.000 abstract 1
- 239000007774 positive electrode material Substances 0.000 abstract 1
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 5
- 239000008151 electrolyte solution Substances 0.000 description 4
- 229940021013 electrolyte solution Drugs 0.000 description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 3
- 238000001035 drying Methods 0.000 description 3
- 238000007710 freezing Methods 0.000 description 3
- 230000008014 freezing Effects 0.000 description 3
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- AMXOYNBUYSYVKV-UHFFFAOYSA-M lithium bromide Chemical compound [Li+].[Br-] AMXOYNBUYSYVKV-UHFFFAOYSA-M 0.000 description 2
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 2
- 239000004033 plastic Substances 0.000 description 2
- 229920003023 plastic Polymers 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- JBYHSSAVUBIJMK-UHFFFAOYSA-N 1,4-oxathiane Chemical compound C1CSCCO1 JBYHSSAVUBIJMK-UHFFFAOYSA-N 0.000 description 1
- GUXJXWKCUUWCLX-UHFFFAOYSA-N 2-methyl-2-oxazoline Chemical compound CC1=NCCO1 GUXJXWKCUUWCLX-UHFFFAOYSA-N 0.000 description 1
- 229910000552 LiCF3SO3 Inorganic materials 0.000 description 1
- -1 Lilo4 Inorganic materials 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 101100230509 Neurospora crassa (strain ATCC 24698 / 74-OR23-1A / CBS 708.71 / DSM 1257 / FGSC 987) hat-1 gene Proteins 0.000 description 1
- WGLPBDUCMAPZCE-UHFFFAOYSA-N Trioxochromium Chemical group O=[Cr](=O)=O WGLPBDUCMAPZCE-UHFFFAOYSA-N 0.000 description 1
- 229910000423 chromium oxide Inorganic materials 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- BDUPRNVPXOHWIL-UHFFFAOYSA-N dimethyl sulfite Chemical compound COS(=O)OC BDUPRNVPXOHWIL-UHFFFAOYSA-N 0.000 description 1
- 239000002001 electrolyte material Substances 0.000 description 1
- 239000002360 explosive Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 230000009183 running Effects 0.000 description 1
- YLQBMQCUIZJEEH-UHFFFAOYSA-N tetrahydrofuran Natural products C=1C=COC=1 YLQBMQCUIZJEEH-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/14—Cells with non-aqueous electrolyte
- H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/14—Cells with non-aqueous electrolyte
- H01M6/16—Cells with non-aqueous electrolyte with organic electrolyte
- H01M6/162—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte
- H01M6/164—Cells with non-aqueous electrolyte with organic electrolyte characterised by the electrolyte by the solvent
-
- 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
Landscapes
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Secondary Cells (AREA)
- Primary Cells (AREA)
Abstract
The invention provides a galvanic cell comprising a negative lithium electrode, a non-aqueous electrolyte and a reducible positive electrode, wherein the electrolyte is a solution of a conducting salt in a mixture of diglycol dimethyl ether and ethylene sulphite. Preferably a 1 molar solution of one of the salts LiPF6, LiClO4 and LiAsF6 in a mixture of diglycol dimethyl ether and ethylene sulphite is used as the electrolyte. The high boiling points of the solvent components (160 DEG C and 173 DEG C) ensure, on account of the low vapour pressure, that the cell is safe to handle. The electrolyte conductivity is almost 10<2> OMEGA <-1>.cm<-1>. The stability of the electrolyte with respect to the electrode materials is manifested in the good storability of the cell. CrOx, Bi2O3, Pb3O4 and MnO2 are suitable as positive electrode materials.
Description
SPECIFICATION
Galvanic cell
The invention relates to a galvanic cell of the type comprising a negative lithium electrode, a non-aqueous electrolyte, and a reducible positive electrode.
Galvanic cells of the type referred to above and in particular with positive electrodes, whose reducible consituent is chromium oxide, CrOx (where x = 2 to 2.9), or bismuth trioxide, Bi203, or managanese dioxide, are, on account of their voltage behaviour, a suitable replacementof cells of the known Leclanché type in instrument batteries. One form of such Li/CrO,, Li/Bi2 03,
Li/Pb304 or Li/MnO2 cells is the handy button-type cell. By stacking these cells on top of one another and encasing them in a shrinkdown plastics tubing, batteries are obtained whose discharge voltages are a multiple of approximately 1.5 V, corresponding to a Li/Bi203 cell, or a multiple of approximately 3 V, corresponding to the CrOx cell.
Galvanic cells of the type referred to are known from German Offenlegungsschriften (DE-A) 25 16 704, 27 26 380 and 25 35 468. These cells are characterised in general by a constant voltage state and good storability, which require mutually compatible electrolyte and electrode materials. Solutions of various salts in mixtures of the solvents propylene carbonate and 1,2dimethoxyethane, and also with tetrahydrofuran as an additional mixture component, are disclosed as cell electrolyte in the specifications.
Of these solvents dimethoxyethane has a relatively low boiling point of 84.8 C, which is disadvantageous insofar as explosive vapour mixtures can be formed during handling and processing. In the case of propylene carbonate there is alos a disadvantageous tendency to undergo a degree of polymerisation, especially at elevated temperatures, and this results in deposits being formed on the lithium electrode.
An object of the invention is to provide a cell of the type referred to wherein the electrolyte comprises only solvents having a boiling point of more than 100 C and the electrolyte has such a good electrical conductivity that the cell can aslo withstand pulse loads with relatively high currents. Such pulse loads with relatively high currents occur for example when a dial or an alarm device is to be actuated in an electronic clock, which actuation is associated with a very much larger current input than the normal continuous load current.
In accordance with the present invention, there is provided a galvanic cell comprising a negative lithium electrode, a non-aqueous electrolyte and a reducible positive electrode, wherein the electrolyte is a solution of a conducting salt in a mixture of diglycol dimethyl ether and ethylene sulphite.
The conducting salt is preferably present in the electrolyte at a concentration of approximately 1M.
The conductivity of approximately 1 molar solutions of any one of the salts LiAsF6, Lilo4, LiBF4, LiPF6, LiCF3SO3 and LiBr in either diglycol dimethyl ether or in ethylene sulphite is approximately about 4 X 10 - 32- 1 X cm-1. It has surprisingly been found that this conductivity is roughly doubled if the individual solvents are replaced by a mixture thereof.
Conductivity values for some examples of electrolyte solutions for cells according to the invention are given in Table 1 below. The solutions were as follow: 1. 10 ml diglycol dimethyl ether + 10 ml ethylene sulphite + 2.0 g Lilo4 2. 5 ml diglycol dimethyl ether + 15 ml ethylene sulphite + 4.0 g LiAsF6 3. 10 ml diglycol dimethyl ether + 10 ml ethylene sulphite + 3.0 g LiBF4 4. 5 ml diglycol dimethyl ether + 15 ml ethylene sulphite + 4.0 g LIPS, 5. 6 ml dimethoxyethane + 14 ml propylene carbonate + 2.0 g Lilo4 Electrolyte No. 5 is the known electrolyte mentioned above and serves as a comparison.
TABLE 1
Conductivity
Electrolyte Water content (# X cm) - > c 103 No. ppm at 22 C 1 18.3 9.8 2 22.2 9.5 3 50.7 7.2 4 26.3 9.2 5 13.0 11.3
Referring to Table 1 all the conductivity values found are similar. Larger differences are found however in the water contents, which are partly derived from the solvents and partly from the
conducting salts, these involving varying degrees of difficulty in drying.
An inherent advantage of the invention is shown by electrolytes Nos. 1 to 4 to be the fact that
the good conductivity values are achieved with mixtures of solvents which, unlike propylene
carbonate, do not tend to polymerise, and which are liquid over a very wide temperature range
and have high boiling points, especially compared with dimethoxyethane.
The freezing points and boiling points of the solvents are as follows:
Diglycol dimethyl ether
Freezing point: - 68"C Boiling point: 1 60 C Ethylene sulphite
Freezing point: - 11 'C Boiling point: 1 73'C The dangers inherent in solvents of low boiling points are thereby obviated by the present
invention. Furthermore, the losses as a result of diffusion through plastics cell seals is less in the case of high boiling liquids than in the case of the more readily volatile solvents, especially at higher temperatures.
Moreover, the electrolyte solutions according to Examples 1 to 4 can be cooled to temperatures not exceeding - 1 5'C without crystals separating out.
It was found that other electrolyte solvents with boiling points above 1 00 C, including dimethyl formamide (153"C), dimethyl sulphite (126"C), 2-methyl-2-oxazoline (1 10'C), 1
methyl-2-pyrrolidone (205 C), and 1 ,4-thioxane (147"C), are not resistant to lithium or have too low conductivities and are thus unsuitable for electrolyte solutions in cells according to the
invention.
LiPF6, LiAsF6 and Lilo4 are preferred as conducting salts in cells according to the invention, preferably in a concentration of 1 mole/l. Before use they are preferably dried as follows in a drying gun under a vacuum:
LiPF6 72 hat 1 20 C LiAsF6 72 h at 90 C Lilo4 72 h at 205 C The electrolyte solvents according to the invention are preferably distilled under reduced pressure for the purposes of purification. A first runnings and a residue of 20% by volume are in each case discarded. The subsequent drying of diglycol dimethyl ether is carried out with active aluminium oxide and of ethylene sulphite with a 4 A molecular sieve.Prior treatment of a small proportion of the ethylene sulphite with Al203 may however be advantageous because traces of SO2 are thereby formed, and the S02 forms in the cell a passivating covering layer on the lithium electrode and thereby contributes to improving the storage properties of the cell.
Diglycol dimethyl ether and ethylene sulphite are preferably mixed in a volume ratio of about
1:1 to 1:3 in the electrolyte solution for cells according to the invention.
In electrical tests involving the experimental Li/CrOx cells of dimensions 11.6 X 3.6 mm, which were provided with electrolytes Nos. 1 to 5 described above, pulse loads were applied which were comparable to the loads during operation of the "backlight" of a LCD clock. The pulse currents each of 10 seconds' duration were amplified in the sequence 2.3 mA/cm2, 3.5 mA/cm2 and 4.7 mA/cm2. The cells were subjected to this treatment in the following stages:
(a) new state
(b) after 50% capacity discharge
(c) after 90% capacity discharge.
The drawing shows in a diagram the minimal voltages U(V), which were established at the end of a pulse, and the d.c. resistances Rj (#) calculated from the voltage drop, produced for the three aforementioned discharge states (a), (b) and (c). Compared with the known electrolyte
No. 5, the electrolyte Nos. 1 to 4 do not show any significant reduction in conductivity, which generally runs in parallel with an increase in boiling point and to this extent would be expected, or at least do not exhibit a reduction of such an amount as to influence the discharge behaviour of the cell. Thus, the advantages of the electrolyte for cells according to the invention, which are namely the low vapour pressure and the stability with respect to the electrode materials, are not offset by disadvantages in other respects.
It was even found that cells with the electrolytes Nos. 1 and 2 behaved, after 3 months' storage at 60 C, more favourably than a comparison cell with the known electrolyte No. 5 since their internal resistances (d.c. resistances Rj) had risen much less compared with the values in the new state, and also the impedance, measured at 1000 Hz, was clearly lower with electrolytes Nos. 1 and 2.
This fact can be seen from Table 2.
TABLE 2
Electrolyte No.
1 2 5
Impedance (1000 Hz) 90 64 174 d.c. resistance at 10 seconds 2.3 mA/cm2 391 350 410 at 10 seconds 3.5 mA/cm2 300 261 379 at 10 seconds 4.7 mA/cm2 250 219 332
Claims (11)
1. A galvanic cell comprising a negative lithium electrode, a non-aqueous electrolyte and a reducible positive electrode, wherein the electrolyte is a solution of a conducting salt in a mixture of diglycol dimethyl ether and ethylene sulphite.
2. A galvanic cell according to claim 1, wherein the said conducting salt of the electrolyte is
LiPF6, Lilo4 or LiAsF6.
3. A galvanic cell according to claim 2, wherein said conducting salt is present in the electrolyte at a concentration of 0.5 to 1.5 M.
4. A galvanic cell according to any preceding claim, wherein the diglycol dimethyl ether and ethylene sulphite are present in a volume ratio of 0.8:1 to 1:3 preferably 0.9:1 to 1:3.
5. A galvanic cell according to any preceding claim, wherein the positive electrode is of CrOx (where x is 2 to 2.9), By202, Pb304 or Mono2.
6. A galvanic cell according to any preceding claim, wherein the diglycol dimethyl ether and the ethylene sulphite have been distilled under reduced pressure.
7. A galvanic cell according to claim 6, wherein the diglycol dimethyl ether has been dried, after the distillation, with active aluminium oxide.
8. A galvanic cell according to claim 6 or 7, wherein the ethylene sulphite has been dried, after the distillation, with a molecular sieve.
9. A galvanic cell according to any preceding claim, wherein at least a portion of the ethylene sulphite has been treated with Awl203.
10. A galvanic cell according to claim 1, wherein the electrolyte is substantially as described herein as electrolyte No. 1, 2, 3 or 4.
11. A galvanic cell according to claim 10, being a Li/CrOx cell.
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE3033589 | 1980-09-06 |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| GB2084789A true GB2084789A (en) | 1982-04-15 |
| GB2084789B GB2084789B (en) | 1983-11-23 |
Family
ID=6111282
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| GB8125181A Expired GB2084789B (en) | 1980-09-06 | 1981-08-18 | Galvanic cell |
Country Status (3)
| Country | Link |
|---|---|
| JP (1) | JPS5776764A (en) |
| FR (1) | FR2490020A1 (en) |
| GB (1) | GB2084789B (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0289706A2 (en) * | 1987-05-02 | 1988-11-09 | VARTA Batterie Aktiengesellschaft | Galvanic primary cell with a negative lithium electrode |
Family Cites Families (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3468716A (en) * | 1965-10-24 | 1969-09-23 | Electrochimica Corp | Organic electrolyte electrochemical system |
| US3578500A (en) * | 1968-07-08 | 1971-05-11 | American Cyanamid Co | Nonaqueous electro-chemical current producing cell having soluble cathode depolarizer |
| CA970028A (en) * | 1971-02-03 | 1975-06-24 | Bruce H. Garth | High energy density battery |
| FR2127399A5 (en) * | 1971-03-05 | 1972-10-13 | Accumulateurs Fixes | |
| US3778310A (en) * | 1972-05-01 | 1973-12-11 | Du Pont | High energy density battery having unsaturated heterocyclic solvent containing electrolyte |
| JPS5244418B2 (en) * | 1973-05-31 | 1977-11-08 | ||
| FR2344135A1 (en) * | 1976-03-09 | 1977-10-07 | Accumulateurs Fixes | SPECIFIC HIGH ENERGY ELECTROCHEMICAL GENERATORS |
-
1981
- 1981-06-17 FR FR8111967A patent/FR2490020A1/en active Granted
- 1981-08-18 GB GB8125181A patent/GB2084789B/en not_active Expired
- 1981-09-04 JP JP56138675A patent/JPS5776764A/en active Granted
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0289706A2 (en) * | 1987-05-02 | 1988-11-09 | VARTA Batterie Aktiengesellschaft | Galvanic primary cell with a negative lithium electrode |
| EP0289706A3 (en) * | 1987-05-02 | 1991-05-15 | VARTA Batterie Aktiengesellschaft | Galvanic primary cell with a negative lithium electrode |
Also Published As
| Publication number | Publication date |
|---|---|
| GB2084789B (en) | 1983-11-23 |
| JPS5776764A (en) | 1982-05-13 |
| FR2490020A1 (en) | 1982-03-12 |
| FR2490020B1 (en) | 1985-03-22 |
| JPH0353746B2 (en) | 1991-08-16 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PCNP | Patent ceased through non-payment of renewal fee |
Effective date: 19980818 |