DK170284B1 - Adhesive compsn. contg. high and low mol. wt. polyacrylic acid - and solvent, esp. for laminated separator for alkaline electrolyte cell - Google Patents
Adhesive compsn. contg. high and low mol. wt. polyacrylic acid - and solvent, esp. for laminated separator for alkaline electrolyte cell Download PDFInfo
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- DK170284B1 DK170284B1 DK622187A DK622187A DK170284B1 DK 170284 B1 DK170284 B1 DK 170284B1 DK 622187 A DK622187 A DK 622187A DK 622187 A DK622187 A DK 622187A DK 170284 B1 DK170284 B1 DK 170284B1
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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
- 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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Abstract
Description
i DK 170284 B1in DK 170284 B1
Den foreliggende opfindelse angår polyacrylsyreklæbemidler til sammenføjning af separatormaterialer anvendt i elektrokemi ske elementer, samt anvendelse af et klæbemiddel ifølge opfindelsen til laminering af et absorberende, ikke-vævet materialelag til et barrieremateriale til 5 dannelse af en separator for et element med alkalisk elektrolyt eller til sammenføjning af spiralvi kl ingerne af et spiral vi kl et separatorrør indbefattet i et elektrokemisk element.The present invention relates to polyacrylic acid adhesives for joining separator materials used in electrochemical elements, and to use an adhesive according to the invention for laminating an absorbent, nonwoven material layer to a barrier material to form a separator for an alkaline electrolyte element or for joining. of the spiral veins of a spiral we of a separator tube included in an electrochemical element.
Klæbemidlet ifølge opfindelsen er specielt anvendeligt til brug sammen med de absorberende materialer eller barrierematerialer, som an-10 vendes i elektrokemi ske elementer.The adhesive of the invention is particularly useful for use with the absorbent or barrier materials used in electrochemical elements.
Kombinationer af absorberende papir eller ikke-vævet stof og barrierematerialer har været anvendt i nogen tid i elektrokemiske elementer, navnlig elementer med alkalisk elektrolyt. For at lette håndtering og indføring i elementet under elementmontage lamineres disse materialer 15 ofte sammen ved hjælp af klæbemidler eller varmeforseglingsteknikker.Combinations of absorbent paper or nonwoven fabric and barrier materials have been used for some time in electrochemical elements, in particular elements with alkaline electrolyte. To facilitate handling and insertion into the element during element assembly, these materials are often laminated together by means of adhesives or heat sealing techniques.
I cylindriske elementer, navnlig elementer med alkalisk elektrolyt anvendes ofte spiralviklede rør af absorptions- eller barrieremateriale, som holdes i form ved hjælp af et klæbemiddel, der er påført for at låse spiralernes overlappende dele.In cylindrical elements, in particular elements with alkaline electrolyte, helically wound tubes of absorbent or barrier material are often used which are held in shape by an adhesive applied to lock the overlapping parts of the spirals.
20 Brugen af klæbemiddel eller varmeforsegling bevirker sædvanligvis en blokering af porerne i det absorberende materiale eller barrierematerialet. Dette bevirker igen forøgelse af den elektriske modstand og/-eller et fald i materialets elektrolytabsorptionskapacitet og en forringelse af materialets befugtningsegenskaber. Som resultat forringes ele-25 mentsystemets ydelse.The use of adhesive or heat seal usually causes a blockage of the pores in the absorbent or barrier material. This in turn causes an increase in electrical resistance and / or a decrease in the electrolyte absorption capacity of the material and a deterioration of the wetting properties of the material. As a result, the performance of the element system is degraded.
Der har været gjort forsøg på at anvende klæbemidler, som er kompatible med alkaliske elektrokemi ske systemer, og som ikke fører til uønsket blokering af absorptions- eller barrierematerialernes porer. Sådanne klæbemidler har involveret brug af geldannelsesmidl er baseret på 30 langkædede polyacrylsyrer, se f.eks. US-PS nr. 3.894.889. Disse har imidlertid alvorlige praktiske ulemper. De lider af ekstremt høj viskositet og dårlige flydeegenskaber, således at det er nødvendigt at anvende specielle belægnings- og lamineringsmaskiner til påføring af klæbemidlerne og specielt udstyr til at bringe klæbemidlet fra en opbe-35 varingstank til klæbemiddelbelægningshovedet. På grund af den høje viskositet og de dårlige flydeegenskaber er hastigheden, hvormed disse klæbemidler påføres, lav, hvilket reducerer gennemløbet under lamineringsoperationen og derved øger generalomkostningerne og signifikant DK 170284 B1 2 øger prisen på det færdige element.Attempts have been made to use adhesives which are compatible with alkaline electrochemical systems and which do not lead to undesirable blocking of the pores of the absorption or barrier materials. Such adhesives have involved the use of gelling agent based on 30 long chain polyacrylic acids, see e.g. U.S. Patent No. 3,894,889. However, these have serious practical disadvantages. They suffer from extremely high viscosity and poor flow properties so that it is necessary to use special coating and laminating machines for applying the adhesives and special equipment to bring the adhesive from a storage tank to the adhesive coating head. Due to the high viscosity and the poor flow properties, the rate at which these adhesives are applied is low, reducing the throughput during the lamination operation, thereby increasing the overall cost and significantly increasing the price of the finished element.
US patent nr. 4.109.066 omhandler en semi-permeabel membran til bly(syre) batterier. Den semi-permeable membran har en mi kroporøs struktur, som omfatter en første polymer og en anden polymer, der er 5 intimt blandet deri, hvor den første polymer er valgt blandt polyacryl-syre, méthacrylsyre eller blandinger deraf, og den anden polymer er opløselig i vand og er valgt blandt polyvinyl pyrrol idon, polyvinyl al kohol og copolymer indeholdende vinyl pyrrol idon eller vinyl alkolhol -sekvenser eller blandinger af disse polymerer. US-4.109.066 nævner ikke 10 en komponent med lav molekylvægt, der falder inden for det i den foreliggende ansøgnings krav 1 angivne molekylvægtområde og omhandler ikke at denne komponent har i det væsentlige lineære kæder. En komponent med høj molekylvægt er beskrevet, idet det foretrukne interval fra 50.000 til 1 mi 11 inon klart ligger uden for molekyl vægtinterval!et for kompo-15 nenten med høj molekylvægt ifølge det foreliggende krav 1. Der er intetsteds i US-4.109.066 omtalt, at komponenten med høj molekylvægt omfatter forgrenede kæder.U.S. Patent No. 4,109,066 discloses a semi-permeable membrane for lead (acid) batteries. The semi-permeable membrane has a body-corrosive structure comprising a first polymer and a second polymer intimately mixed therein, the first polymer being selected from polyacrylic acid, methacrylic acid or mixtures thereof, and the second polymer being soluble. in water and is selected from polyvinyl pyrrolidone, polyvinylalcohol and copolymer containing vinyl pyrroleon or vinylalcohol sequences or mixtures of these polymers. US-4,109,066 does not mention a low molecular weight component which falls within the molecular weight range specified in claim 1 of the present application and does not disclose that this component has substantially linear chains. A high molecular weight component is disclosed, the preferred range of from 50,000 to 1 ml of 11 inon being clearly outside the molecular weight range of the high molecular weight component of the present claim 1. There is nowhere in US-4,109,066 disclosed that the high molecular weight component comprises branched chains.
Den foreliggende opfindelse har som formål at tilvejebringe et polyacrylklæbemiddel til sammenføjning af separatormaterialer anvendt i 20 elektrokemi ske elementer med lav viskositet, som kan anvendes på absorberende eller porøse materialer anvendt i omgivelser med alkalisk elektrolyt uden at bevirke poreblokering. Det har vist sig, at et klæbemiddel system med fremragende egenskaber kan dannes ud fra en blanding af en langkædet polyacrylsyre og en kortkædet polyacrylsyre.The present invention has for its object to provide a polyacrylic adhesive for joining separator materials used in low-viscosity electrochemical elements which can be applied to absorbent or porous materials used in alkaline electrolyte environments without causing pore blocking. It has been found that an adhesive system with excellent properties can be formed from a mixture of a long chain polyacrylic acid and a short chain polyacrylic acid.
25 Opfindelsen tilvejebringer et klæbemiddel af forholdsvis lav viskositet, som kan påføres med simpelt apparatur og ved højt gennemløb. Klæbemidlet ifølge opfindelsen har bedre elektrokemi ske egenskaber end konventionelle lamineringsklæbemidler og varmebindingsteknikker og svækker ikke elementabsorptionsmidlets og separatorkomponenternes absorp-30 ti onskapacitet eller befugtningsegenskaber, men kan endda forbedre be-fugtningsegenskaberne for laminerede separatorer til elementer med alkalisk elektrolyt.The invention provides a relatively low viscosity adhesive which can be applied with simple apparatus and at high throughput. The adhesive according to the invention has better electrochemical properties than conventional laminating adhesives and heat bonding techniques and does not impair the absorbent capacity or wetting properties of the element absorbent and separator components, but can even improve the wetting properties of laminated electrolyte separators for elements with alkaline electrolytes.
Opfindelsen angår et polyacrylsyreklæbemiddel til sammenføjning af separatormaterialer anvendt i elektrokemi ske elementer, hvilket er ejen-35 dommeligt ved, at det omfatter en blanding af en første komponent, som er mindst én polyacrylsyre med høj molekylvægt, og en anden komponent, som er mindst én polyacrylsyre med lav molekylvægt, i et opløsningsmiddel, hvor polyacrylsyren af den første komponent har en molekylvægt i DK 170284 B1 3 intervallet fra 1,25 millioner til 5 millioner og omfatter molekyler med forgrenede kæder, polyacrylsyren af den anden komponent har en molekylvægt i intervallet fra 2.000 til 500.000 og omfatter molekyler med i det væsentlige lineære kæder og forholdet mellem mængden af polyacrylsyre 5 med høj molekylvægt og mængden af polyacrylsyre med lav molekylvægt ligger i området 1:0,4 til 1:1,2 dele efter vægt.The invention relates to a polyacrylic acid adhesive for joining separator materials used in electrochemical elements, which is characterized in that it comprises a mixture of a first component which is at least one high molecular weight polyacrylic acid and a second component which is at least one low molecular weight polyacrylic acid, in a solvent wherein the polyacrylic acid of the first component has a molecular weight in the range of 1.25 million to 5 million and comprises branched chain molecules, the polyacrylic acid of the second component has a molecular weight in the range of 2,000 to 500,000 and comprises molecules with substantially linear chains and the ratio of the amount of high molecular weight polyacrylic acid 5 to the low molecular weight polyacrylic acid ranges from 1: 0.4 to 1: 1.2 parts by weight.
Kombinationen af langkædede og kortkædede polyacrylsyrer giver et klæbemiddel system med fremragende gel danne!sesegenskaber i kombination med lav viskositet. Den langkædede polyacrylsyre indeholder fortrinsvis 10 forgrenede kæder, mens den kortkædede polyacrylsyre indeholder i det væsentlige lineære eller kun svagt forgrenede kæder. Forgrenede langkædede polyacrylsyrer har fremragende gel dannelse og klæbeegenskaber i vandige eller alkaliske opløsninger men høj viskositet. De mindre i det væsentlige lineære molekyler af kortkædet polyacrylsyre befinder sig mellem de 15 langkædede molekyler og reducerer interferencen mellem disse, idet de i realiteten virker som et molekylært smøremiddel med det resultat, at blandingens viskositet reduceres markant uden, at den langkædede poly-acrylsyres geldannelses- og klæbeegenskaber svækkes.The combination of long chain and short chain polyacrylic acids provides an adhesive system with excellent gel forming properties in combination with low viscosity. The long-chain polyacrylic acid preferably contains 10 branched chains, while the short-chain polyacrylic acid contains substantially linear or only slightly branched chains. Branched long chain polyacrylic acids have excellent gel formation and adhesive properties in aqueous or alkaline solutions but high viscosity. The less substantially linear molecules of short-chain polyacrylic acid are located between the 15 long-chain molecules and reduce their interference, in effect acting as a molecular lubricant, with the result that the viscosity of the mixture is significantly reduced without the gel formation of the long-chain polyacrylic acid. - and adhesive properties are impaired.
Den langkædede polyacrylsyre har typisk en molekylvægt i interval-20 let fra 1.250.000 til 5.000.000, fortrinsvis ca. 3.000.000. Lavere molekylvægte giver utilstrækkelige geldannelses- og klæbeegenskaber, mens højere molekylvægte bevirker, at der ikke let dannes egnede opløsninger.The long chain polyacrylic acid typically has a molecular weight in the range of from 1,250,000 to 5,000,000, preferably about 3,000,000. Lower molecular weights provide insufficient gelling and adhesive properties, while higher molecular weights do not easily form suitable solutions.
Den kortkædede polyacrylsyre har fortrinsvis en molekylvægt i intervallet fra 2.000 til 500.000, fortrinsvis ca. 250.000. Polyacrylsyrer 25 med håndgribeligt højere eller lavere molekylvægte reducerer ikke den samlede viskositet håndgribeligt.The short-chain polyacrylic acid preferably has a molecular weight in the range of 2,000 to 500,000, preferably approx. 250,000. Polyacrylic acids 25 with tangibly higher or lower molecular weights do not tangibly reduce the overall viscosity.
Langkædede polyacrylsyrer, som er egnet til brug ifølge opfindelsen, indbefatter "Carbopol" (varemærke) rækken, navnlig produktet Carbo-pol 941 opadtil. Carbopol 934 har vist sig specielt egnet.Long-chain polyacrylic acids suitable for use in the invention include the "Carbopol" (trademark) row, in particular the product Carbo-pol 941 upwards. Carbopol 934 has proved particularly suitable.
30 Komponenterne i klæbemiddel systemet ifølge opfindelsen kan være dispergeret i et vandigt opløsningsmiddel eller i et passende polært organisk opløsningsmiddel, for eksempel methanol eller ethanol. Organiske opløsningsmiddel systemer er sædvanligvis at foretrække på grund af bedre kompatibilitet med de i alkalisk elektrokemi ske elementer anvendte ab-35 sorptions- og barrierematerialer. Disse danner helt gelerede dispersioner og befugter ikke hurtigt cellulosematerialet og får det til at kvælde, således som det forekommer ved anvendelse af vand.The components of the adhesive system of the invention may be dispersed in an aqueous solvent or in a suitable polar organic solvent, for example methanol or ethanol. Organic solvent systems are usually preferred due to better compatibility with the absorption and barrier materials used in alkaline electrochemical elements. These form completely gelled dispersions and do not rapidly moisten the cellulose material and cause it to swell as it occurs when using water.
Klæbemiddel bl andingen, almindeligvis beskrevet som en "dispersion", DK 170284 B1 4 kan varieres betragteligt i viskositet og flydeegenskåber ved variation af forholdet mellem mængderne af langkædede og kortkædede polyacrylsyrer og/eller deres molekylvægte for at tilpasse dem efter den påføringsteknik, som skal benyttes til påføring af klæbemidlet.Adhesive admixture, commonly described as a "dispersion", can be considerably varied in viscosity and flow characteristics by varying the ratio of the amounts of long-chain and short-chain polyacrylic acids and / or their molecular weights to adapt to the application technique to be used. for applying the adhesive.
5 Et typisk anvendeligt lamineringssystem omfatter et "Meyer" bjælke applikationshoved med en sammenklemning af de laminerede materialer, mens de endnu er våde, efterfulgt af tørring, for eksempel ved hjælp af en luftstrøm. Brugen af opløsningsmiddel letter tørring ved lavere temperaturer, hvilket kan være vigtigt ved nogle elementseparatorsystemer 10 for at undgå beskadigelse af separatormaterialerne.A typical usable lamination system comprises a "Meyer" beam application head with a squeeze of the laminated materials while still wet, followed by drying, for example by means of an air stream. The use of solvent facilitates drying at lower temperatures, which may be important in some element separator systems 10 to avoid damage to the separator materials.
Opfindelsen beskrives nu yderligere i forbindelse med fremstilling af laminerede separatorer, som er egnet til brug i cylindriske alkaliske manganelementer.The invention is now further described in connection with the manufacture of laminated separators suitable for use in cylindrical alkaline manganese elements.
Separatoren omfatter et ikke-vævet materialelag, navnlig ikke-vævet 15 nylon lamineret til en regenereret cellulosefilm af høj renhed og i batteri kvalitet.The separator comprises a nonwoven material layer, in particular non-woven 15 nylon laminated for a high purity and battery-quality regenerated cellulose film.
Sådanne laminater er blevet fremstillet under anvendelse af forskellige klæbemiddel systemer til dannelse af en binding mellem de to laminatmaterialer herunder: 20 vandbaserede acrylharpikser, acrylcopolymerer, PVA, natriumsil icatbaserede klæbemidler, og varmebundne klæbemidler.Such laminates have been prepared using various adhesive systems to form a bond between the two laminate materials including: 20 water-based acrylic resins, acrylic copolymers, PVA, sodium silicate-based adhesives, and heat-bonded adhesives.
25 Laminater fremstillet ved hjælp af disse klæbemiddel systemer er blevet vurderet med hensyn til deres våde ionresistens, befugtningsegen-skaber og tilbøjelighed til at delaminere. Alle disse klæbemiddel systemer fandtes at være utilstrækkelige, navnlig på grund af dårlig bindestyrke eller på grund af en stor stigning i separatorens våde ion-30 resistens.25 Laminates made using these adhesive systems have been assessed for their wet ion resistance, wetting properties and propensity to delaminate. All of these adhesive systems were found to be inadequate, particularly due to poor bond strength or due to a large increase in the wet ion resistance of the separator.
Et klæbemiddel omfattende en dispersion af Carbopol 934 (en langkædet forgrenet polyacrylsyre med molekylvægt på ca. 3.000.000) i methanol har vist sig at være et passende klæbemiddel til brug i et sådant separatorsystem med hensyn til alle elektrokemi ske egenskaber og 35 befugtningsegenskaber. Det kan imidlertid ikke let anvendes i praksis på * grund af dets meget høje viskositet.An adhesive comprising a dispersion of Carbopol 934 (a long chain branched polyacrylic acid having a molecular weight of about 3,000,000) in methanol has been found to be a suitable adhesive for use in such a separator system in all electrochemical and wetting properties. However, it cannot easily be used in practice due to its very high viscosity.
Tilsætningen af en polyacrylsyre med forholdsvis lav molekylvægt (fortrinsvis ca. 250.000) til Carbopol-dispersionen resulterer i et DK 170284 B1 5 overraskende og betydeligt fald i viskositet og en markant forbedring i flydeegenskaber uden nogen svækkelse af de elektrokemi ske egenskaber og befugtningsegenskaberne i sammenligning med en separator dannet ved hjælp af Carbopol 934 uden tilsat polyacrylsyre med lav molekylvægt. På 5 grund af reduktionen i viskositet og de forbedrede flydeegenskaber kan klæbemiddel systemet omfattende langkædede og kortkædede polyacrylsyrer anvendes til fremstilling af laminerede elementseparatorer ved hjælp af konventionelle belægnings- og lamineringsteknikker med forholdsvis højt gennemløb.The addition of a relatively low molecular weight polyacrylic acid (preferably about 250,000) to the Carbopol dispersion results in a surprising and significant decrease in viscosity and a marked improvement in flow properties without any impairment of the electrochemical and wetting properties in comparison with a separator formed by Carbopol 934 without the addition of low molecular weight polyacrylic acid. Due to the reduction in viscosity and the improved flow properties, the adhesive system comprising long-chain and short-chain polyacrylic acids can be used to prepare laminated element separators by conventional, relatively high throughput coating and lamination techniques.
10 De forbedrede flydeegenskaber illustreres i den følgende tabel.10 The improved flow properties are illustrated in the following table.
DK 170284 B1 6DK 170284 B1 6
Brookfield viskositet (målt ved 20 opm og 20eC) e.p.s.Brookfield viscosity (measured at 20 rpm and 20 ° C) e.p.s.
® 5% Carbopol 934 i methanol 11.200 5% Carbopol 934, 2% polyacryl- syre (PAA) i methanol 5.900 5% Carbopol 934, 4% PAA 4.200 5% Carbopol 934, 6% PAA 3.800® 5% Carbopol 934 in methanol 11,200 5% Carbopol 934, 2% polyacrylic acid (PAA) in methanol 5,900 5% Carbopol 934, 4% PAA 4,200 5% Carbopol 934, 6% PAA 3,800
Sammenlignelige resultater opnås ved anvendelse af andre forgrenede 15 langkædede polyacrylsyrer af Carbopol-type i kombination med andre korte lineære polyacrylsyrer. Forhold op til 6 dele PAA til 5 dele Carbopol 934 er blevet testet. Ved denne værdi iagttoges et svagt tab af klæbestyrke.Comparable results are obtained using other branched 15 long-chain Carbopol-type polyacrylic acids in combination with other short linear polyacrylic acids. Ratios up to 6 parts PAA to 5 parts Carbopol 934 have been tested. At this value, a slight loss of adhesive strength was observed.
Claims (7)
Applications Claiming Priority (4)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| GB8607793 | 1986-03-27 | ||
| GB8607793A GB2188326B (en) | 1986-03-27 | 1986-03-27 | Adhesive |
| US8700409 | 1987-02-23 | ||
| PCT/US1987/000409 WO1987005918A1 (en) | 1986-03-27 | 1987-02-23 | Polyacrylic acid adhesive and cell separator therefrom |
Publications (3)
| Publication Number | Publication Date |
|---|---|
| DK622187A DK622187A (en) | 1987-11-26 |
| DK622187D0 DK622187D0 (en) | 1987-11-26 |
| DK170284B1 true DK170284B1 (en) | 1995-07-24 |
Family
ID=26290556
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| DK622187A DK170284B1 (en) | 1986-03-27 | 1987-11-26 | Adhesive compsn. contg. high and low mol. wt. polyacrylic acid - and solvent, esp. for laminated separator for alkaline electrolyte cell |
Country Status (1)
| Country | Link |
|---|---|
| DK (1) | DK170284B1 (en) |
-
1987
- 1987-11-26 DK DK622187A patent/DK170284B1/en not_active IP Right Cessation
Also Published As
| Publication number | Publication date |
|---|---|
| DK622187A (en) | 1987-11-26 |
| DK622187D0 (en) | 1987-11-26 |
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