Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Nitrogen-containing reactant
Reexamination Certificate
2000-12-22
2002-12-24
Truong, Duc (Department: 1711)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Nitrogen-containing reactant
C528S423000, C528S425000, C528S361000, C528S363000, C528S391000, C528S392000, C525S403000, C525S404000, C525S408000
Reexamination Certificate
active
06498230
ABSTRACT:
BACKGROUND OF THE INVENTION
1. Field of the Invention
This invention relates to a macromolecular solid electrolyte forming a molten salt at room temperature and a polymer to be used therein. More particularly, this invention relates to a macromolecular solid electrolyte exhibiting excellent ion conductivity at low temperatures as of not more than 10° C. and a polymer to be used therein.
2. Description of the Related Art
As an electrolytic material for a fuel cell, for example, a mixture of inorganic compounds which has been thermally molten at an elevated temperature has been heretofore known. Generally, the molten salt which is obtained in a system formed by mixing inorganic compounds, though famed for the lowness of melting point, has a melting point approximating 300° C. For the purpose of enabling the fuel cell to serve as a practical product, the task of remarkably lowering the melting point thereof has been persisting.
Attempts to realize fully satisfactory ion conductivity even at room temperature have been being made and the development of a salt melting at room temperature and to be obtained by the addition of an inorganic salt to a salt of an organic compound has been energetically promoted. U.S. Pat. No. 4,463,072, U.S. Pat. No. 4,463,071, and JP-A-60-136,180 disclose electrolytes using a mixture of an aluminum halide with 1,3-dialkyl imidazol halide or 1,2,3-trialkyl imidazol halide. Though the electrolytes using the compounds as mentioned above melts at room temperature and exhibits high ion conductivity, the aluminum halide encounters a drawback of yielding to decomposition on admitting water even in a very minute amount and the molten salt entails a problem of having the phase condition thereof become unstable on the exposure to change in temperature.
For the purpose of overcoming the problems mentioned above, a macromolecular solid electrolyte containing as an essential component thereof a molten salt polymer which is obtained by reacting an imidazolium derivative selected among 1,3-dialkylimidazolium halide and 1,2,3-trialkylimidazolium halide with a monomer to prepare a molten salt monomer and polymerizing the molten salt monomer has been disclosed in JP-A-10-83,821; and a macromolecular solid electrolyte having impregnated with an imidazolium salt derivative a polyanionic resin to be obtained by introducing a negative charge into a macromolecular acid, a porous macromolecular solid, or a macromolecular thin film has been reported in U.S. Pat. No. 6,025,457.
The macromolecular solid electrolytes disclosed in these official gazettes indeed have high ion conductivity at room temperature (in the neighborhood of 30° C.). They nevertheless are at disadvantage in suffering the ion conductivity to decline conspicuously at lower temperatures such as, for example, of not more than 10° C. and thus rendering fuel cells or lithium secondary cells using the electrolyte difficult to operate effectively at low temperatures. Regarding this point, conventional macromolecular solid electrolytes, while having ion conductivity (log &sgr;, S/cm) of −3 to −4 at 30° C., still entail the same problem of suffering the ion conductivity thereof to decline to −6 at 0° C.
SUMMARY OF THE INVENTION
This invention has been attained in view of the state of affairs mentioned above and, therefore, has an object to provide a macromolecular solid electrolyte which can manifest high ion conductivity even at low temperatures.
Another object of this invention is to provide a polymer which is suitable for the use in such a macromolecular solid electrolyte as mentioned above.
The present inventors have already acquired a knowledge that in the production of a water-soluble graft polymer by the graft polymerization of a monomer component (B) comprising 40 to 100 mol % of (meth)acrylic acid (b1) and 0 to 60 mol % of another monoethylenically unsaturated monomer (b2) to a polyether compound (A) containing not less than 80 mol % of ethylene oxide as a component unit thereof and having a number average molecular weight of not less than 200 at a ratio such that the amount of the monomer component (B) is not less than 25 mass % based on the mass of the polyether compound (A), the reaction by the graft polymerization of the monomer component (B) to the polyether compound (A) in the presence of a polymerization initiator substantially in the absence of a solvent at a temperature of not less than 100° C. results in grafting a monoethylenically unsaturated monomer having (meth) acrylic acid as a main component thereof at a high content to the polyether moiety and thus permits the production of a water-soluble graft polymer having a high graft ratio and that the water-soluble graft polymer thus produced is usable as a dispersing agent for inorganic or organic substances sparingly soluble in water, a water treating agent for preventing the deposition of scale, and a fiber-treating agent such as a dyeing auxiliary and an antistatic agent for fibers and the polymer, when further cross-linked with a cross-linking agent, is usable as an absorbent resin (EP-A-639,592).
The present inventors have further continued a diligent study on various polymers including the water-soluble graft polymers as mentioned above with a view to accomplishing the objects. They have consequently found that when a polymer to be obtained by the reaction of the polymer mentioned above with a specific halogenated nitrogen-containing compound is used in the production of a macromolecular solid electrolyte, the produced macromolecular solid electrolyte shows virtually no decline of ion conductivity even at low temperatures as of not more than 10° C. This invention has been perfected based on this knowledge.
Specifically, the objects mentioned above can be accomplished by a polymer formed of structural units represented by the following formula (1):
wherein R represents a linear or branched alkylene residue of 1 to 4 carbon atoms; X
−
represents a deprotonated residue of an acid; Y
+
represents a cation of a nitrogen-containing compound; Z represents a residue of a monoethylenically unsaturated compound; m represents a number of average addition mols of a branched chain bound to the structural unit, —(RO)—, forming a main chain and is in the range of 2 to 20; n is in the range of 3 to 500; and p is in the range of 0 to 2.
The objects mentioned above can be also accomplished by a polymer which is obtained by the reaction with a cationic nitrogen-containing compound of a polymer (A) to be obtained by polymerizing an acid group-containing monomer to a compound represented by the following formula (2):
R
1
O&Parenopenst;R
2
O)
n
—R
3
(2)
wherein R
1
and R
3
independently represent a hydrogen atom, a group having a carboxylic acid group or a sulfonic acid group, a linear or branched alkyl group of 1 to 4 carbon atoms, or an aryl group of 6 to 10 carbon atoms; R
2
represents a linear or branched alkylene of 1 to 4 carbon atoms; and n is in the range of 3 to 500.
Further, the objects mentioned above can be accomplished by a polymer which is obtained by the reaction with a cationic nitrogen-containing compound of a polymer (A) to be obtained by polymerizing an acid group-containing monomer in the presence of a monoethylenic monomer to a compound represented by the following formula (2):
R
1
O&Parenopenst;R
2
O)
n
—R
3
(2)
wherein R
1
and R
3
independently represent a hydrogen atom, a group having a carboxylic acid group or a sulfonic acid group, a linear or branched alkyl group of 1 to 4 carbon atoms, or an aryl group of 6 to 10 carbon atoms; R
2
represents a linear or branched alkylene of 1 to 4 carbon atoms; and n is in the range of 3 to 500.
This invention relates to (i) a polymer represented by the foregoing formula (1); (ii) a polymer obtained by polymerizing an acid group-containing monomer to a compound represented by the foregoing formula (2) thereby forming a polymer (A) and causing the polymer (A) to react with a cationic nitrogen-containing compound; (iii) a polymer obtained by
Aizawa Ryuji
Aoki Minoru
Ito Shoji
Pan Jinxing
Fish & Richardson P.C.
Nippon Shokubai Co. , Ltd.
Truong Duc
LandOfFree
Polymer and macromolecular solid electrolyte containing the... does not yet have a rating. At this time, there are no reviews or comments for this patent.
If you have personal experience with Polymer and macromolecular solid electrolyte containing the..., we encourage you to share that experience with our LandOfFree.com community. Your opinion is very important and Polymer and macromolecular solid electrolyte containing the... will most certainly appreciate the feedback.
Profile ID: LFUS-PAI-O-2991964