CN101859645A - Large power super capacitor power battery - Google Patents
Large power super capacitor power battery Download PDFInfo
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- CN101859645A CN101859645A CN200910049029A CN200910049029A CN101859645A CN 101859645 A CN101859645 A CN 101859645A CN 200910049029 A CN200910049029 A CN 200910049029A CN 200910049029 A CN200910049029 A CN 200910049029A CN 101859645 A CN101859645 A CN 101859645A
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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
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- 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
- Y02E60/13—Energy storage using capacitors
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Abstract
The invention relates to a large power super capacitor power battery capable of being used as a power battery. Titanium-aluminum foil is adopted as cathode, a porous skeleton titanium foil with high specific surface area is prepared, a compact titanium dioxide dielectric layer is formed on the inner surface of a pore canal through high-temperature thermal oxidization, finally a conductive polymer monomer is used for steeping the pore canal to be polymerized and cover the surface of the titanium dioxide so as to form a conductive polymer cathode. By utilizing the high dielectric constant of the titanium dioxide and the high reliability of the conductive polymer cathode, a super capacitor power battery with large capacitance, high voltage, high reliability and super high energy density is realized.
Description
Technical field:
The present invention relates to a kind of ultracapacitor of total solids, can store huge electric energy and can effectively become Vehicular dynamic battery, is to belong to a kind of novel electric power energy storage device.
Background technology:
Because petroleum resources is progressively exhausted, oil crisis causes oil price sharp rising all the time, and internal-combustion engines vehicle produces a large amount of tail gas pollutions again when consuming the petroleum resources of a large amount of costlinesses.Because energy source is extensive, clean environment firendly again, financial crisis in 2008 makes the electric automobile that substitutes petroleum resources face the opportunity of great development.
The new energy sources for automobile technology is one of development in Hi-Tech direction, because existing electric energy energy storage technology weakness very, show that mainly the electric energy reserves are low, the battery energy storage apparatus expensive, the security reliability of heavy-current discharge is relatively poor, causes electric automobile during traveling apart from weak point, need oil electric mixed dynamic to come electric energy supplement to drive the short defective of distance travelled, very cheap in theory electric automobile because the restriction of battery technology, costs an arm and a leg electric automobile and is difficult to popularize rapidly.
Existing electrical power storage battery adopts lead-acid battery, Ni-MH battery and ferric phosphate lithium cell mostly, also has patent report to adopt the electrolysis super capacitor as electrokinetic cell.The lead-acid battery energy density is at 0.04-0.06kWh/kg, and energy density is too low, also can bring heavy metal pollution, can't be applied in automobile power cell.The Ni-MH battery energy density is not high, and generally at 0.08-0.1kWh/kg, once Chong Dian distance travelled is shorter, needs the gasoline engine assistant starting to prolong distance travelled, causes the hybrid vehicle complex structure to involve great expense.And the nickel tenor seldom costs an arm and a leg on the earth, in case extensive practical, cause nickel metal anxiety and spurt in prices, finally make vehicle price expensive and be difficult to popularize.
Chinese patent 200710124145 is introduced ferric phosphate lithium cell, although theoretical energy density can reach 170AH/kg, the LiFePO 4 material electric conductivity is very poor, and the security reliability of high current charge-discharge is difficult to ensure.Because the LiFePO4 energy storage is a chemical reaction, need be when discharging and recharging the conversion of continuous electric energy and chemical energy, lithium ion can run off from electrode when repeated charge, useful life is limited, the disclosed data charging cycle life-span is probably at 2000～3000 times.
Above-mentioned several electrokinetic cell is because number of drawbacks makes the performance of electric automobile be difficult to reach cheap and good-quality requirement.Along with the technological progress of capacitance technology, ultracapacitor has had the big and electrokinetic cell performance of high current charge-discharge rapidly of storage of electrical energy, demonstrates than above-mentioned three kinds of performances that battery is more excellent.Main performance is as follows:
(1) charging rate is fast: owing to do not exist electric energy to transform the chemical reaction of chemical energy, charging can reach more than 95% of its rated capacity in 10 seconds～10 minutes; With to add gasoline the same rapid.
(2) it is long to recycle the life-span, and degree of depth charge and discharge cycles access times can reach 100,000 times～500,000 times, and positive constant is with down, and before vehicle scrapping, battery can not lose efficacy.
(3) large current discharging capability is superpower, and the loss of charge-discharge energy transfer process is very little, big current energy cycle efficieny 〉=90%;
(4) power density height, storing electricity can reach 0.6kWh/kg～3kWh/kg, is equivalent to 1～5 times of ferric phosphate lithium cell;
(5) the product raw material constitute, produce, use, store and disassemble process all less than polluting, and are ideal green environmental protection power supplys; The raw material that uses all is a cheap metal.
(6) non-maintaining: it is simple to discharge and recharge circuit, need not the such charging circuit of rechargeable battery, the coefficient of safety height.
(7) the ultralow temperature characteristic is good, and temperature range is wide-50 ℃～+ 100 ℃;
(8) easy to detect, dump energy can directly be read;
(9) need only burning voltage, the infringement battery does not overcharge.
Ultracapacitor has developed and has been divided into electric chemical super capacitor and super dull and stereotyped electrolytic capacitor.Electric chemical super capacitor comprises electric double layer capacitance and pseudo capacitance, although electric chemical super capacitor can be accomplished 〉=the individual super large capacitor amount of 5000F/, but because must adopt aqueous electrolyte, the summer high temperature leakage current is big, winter severe cold freezes and solidifies the damage electrode, reliability is not high, is difficult to use safely in the north of china in winter severe cold.
Chinese patent CN03114836 reports that a kind of Ni-based electrolysis ultracapacitor as electrokinetic cell, belongs to electric chemical super capacitor, has charging rapidly, and capacitance is big.But owing to be the ultracapacitor that adopts aqueous electrolyte, the aqueous solution will electrochemical decomposition be oxygen when single-unit surpassed 3V, and is withstand voltage very low, has only 0.9V～2.7V, and storage power is very limited; Simultaneously because leakage current is very big during summer high temperature, during electrical power storage self discharge serious, winter low temperature freezes easily down and solidifies and can't use.In Shanghai the practicability of 11 road capacity public transport cars experimentally, it is many to expose fault, poor reliability, it is low to store electric weight, whole battery group is too huge and cause costing an arm and a leg.
Since electrolytical corrosion, the loss gradually of the metal electrode of electrolysis super capacitor, and aging speed is very fast.
Chinese patent CN200710133296 also introduces a kind of water system ruthenium based super capacitor of high-energy-density, because metal Ru is rare precious metals, prepared super capacitor is very expensive, is difficult to be used in a large number
Chinese patent CN200710165636 introduces a kind of ultracapacitor of combination electrode, adopt aluminium, copper, stainless steel or nickel as electrode, need to use liquid electrolyte,, also have electrolyte corrosion and the bigger problem of capacitor equivalent series resistance although capacity is very big.
Because the conductivity of aqueous electrolyte and organic bath is very low, causes the equivalent series resistance (ESR) of capacitor very big, will obviously generate heat when heavy-current discharge, influences useful life.
JP60-37114 in 1985 has introduced a kind of total solids aluminium electrolytic capacitor that contains the polypyrrole conducting polymer that pure pyrroles's polymerization obtains, and equivalent series resistance is very little,
Chinese patent CN02160476 introduces a kind of substituted thiophene conducting polymer of Bayer invention, owing to have very high conductivity, reach 〉=500S/cm, when making, capacitor substitutes liquid electrolyte, can obviously reduce the equivalent series internal resistance of capacitor, so Chinese patent CN031548992 has introduced and adopts the substituted thiophene conducting polymer to come the total solids capacitor of manufacturing property excellence.But polymerization single polymerization monomer 3,4-ethylidene dioxy thiophene is highly stable, need to add oxidant such as p-methyl benzenesulfonic acid iron and come catalytic polymerization,, need to add a large amount of solvents because p-methyl benzenesulfonic acid iron is insoluble to polymerization single polymerization monomer, when the aperture of porous electrode is very little, the solvent of dissolving can make the duct stay a lot of spaces behind the reprocessing heated volatile, reduces the effective area of electrode, therefore need a kind of solvent that do not contain, the conducting polymer of energy polymerisation in bulk.
The alloy that Te Kaiping 5-36576 introduces metallic aluminium and valve metals such as Ti, Zr, Ta prepares the electrochemical capacitor of high-k, shows that the aluminium zircaloy obtains porous zirconium paillon foil electrode through behind the hcl corrosion, has preferable capacitive property.
Chinese patent CN01807047 discloses a kind of employing Titanium material and titanate esters is made the titanium dioxide dielectric layer, at metallic titanium plate coated titanium acid esters, prepare the titanium dioxide dielectric layer through high temperature sintering, and be used to make big capacity titanium electrolytic capacitor, the preparation hell to pay of its titanium dioxide dielectric layer needs high temperature sintering repeatedly just to obtain 500nm compact titanium dioxide dielectric layer.And introduce and to prepare the big electric capacity of titanium dioxide with the aqueous solution, leakage current is very big.
Because the dielectric constant of aluminium oxide has only 8.3, and the dielectric constant of rutile titanium dioxide reaches 90-114, therefore same electrode area, the capacity of super capacitor of employing titanium dioxide dielectric layer improves more than 10 times than the aluminum oxide dielectric layer of aluminium electrode, deficiency at above ultracapacitor and electrokinetic cell, the invention provides a kind of employing titanium dioxide as dielectric layer with high dielectric constant, realize that height is withstand voltage, the super capacitor electrokinetic cell of total solids.
Owing to avoided the use liquid electrolyte, overcome the summer temp rising, the reliability difficult problem that leakage current significantly increases.Simultaneously in the winter time, not having electrolyte coagulation and the problem that lost efficacy, is a kind of high reliability, high-energy ratio, high-tension solid super capacitor electrokinetic cell.
Electrokinetic cell need be stored a large amount of electric energy, and the energy storage formula of super capacitor is as follows:
Q＝1/2*CU
2 (J)
Wherein: C: capacitance F;
U: charge into voltage V
Therefore, charge into voltage to storing electricity to influence specific capacitance bigger, charging voltage is high more, the electric energy that super capacitor stores the more.220V charges into voltage and can Duo more than 5000 times than the electric energy that 3V stores.The ultracapacitor electric energy stored of a 200F/220V is Duoed more than 200 times than the ultracapacitor of 5000F/2.7V.
Summary of the invention:
The present invention is a kind of total solids super capacitor electrokinetic cell that adopts titanium dioxide as dielectric layer.The key of technological invention is the titanium dioxide dielectric layer of high-k of preparation even compact and the negative electrode of low series equivalent resistance.Ultracapacitor need carry out following operation,
At first, the titanium-aluminium alloy paillon foil is corroded in the salt acid tank, the metallic aluminium in the alloy is eroded fully, form the stephanoporate framework titanium foil sheet of high-specific surface area.Then the skeleton titanium foil sheet of porous is carried out electrochemical oxidation, controlled oxidation voltage makes the titanium dioxide oxide-film that forms one deck densification at the surface oxidation in titanium foil sheet duct, and THICKNESS CONTROL is at 200-500nm.POROUS TITANIUM paillon foil after the oxidation immerses in the substituted alkyl dioxy pyrrole monomer after drying, and heating polymerisation in bulk is down covered the total solids ultracapacitor of the fine and close conducting polymer of titanium dioxide dielectric layer as negative electrode fully.
The present invention adopts 3 of general formula (A), and the initator that 4-replaces dioxy pyrroles's conducting polymer monomer and general formula (B) mixes
Wherein: the alkyl of R1=H or C1～C3
The alkyl of R2=C1～C3
Stephanoporate framework titanium foil sheet behind the compound oxide impregnation, polymerisation in bulk is a conductive polymer cathode in the initiation duct after heating, covers the titanium dioxide dielectric layer.The residual fragment of initator forms the doping to conductive compound, has strengthened conductivity.Owing to do not use solvent, no longer need oven dry to reclaim solvent, simplify work flow.Simultaneously, polymerisation in bulk makes the various microchannels of stephanoporate framework titanium foil sheet all can be filled conducting polymer, significantly reduces emptying aperture road area.
Compare with aqueous electrolyte, conducting polymer is an electrolyte that volume is bigger, in case polymerization is fixed in the duct, just can not be out of shape, even the crack of titanium dioxide dielectric layer appearance≤1nm does not influence the insulation property of capacitor yet.If aqueous electrolyte, dielectric layer can puncture cause super capacitor to lose efficacy at once.
Wherein: the alkyl of R3:C1～C8, phenyl, tolyl or benzyl
The alkyl of R4:C1～C8, phenyl, tolyl or benzyl
Because the titanium-aluminium alloy paillon foil is after corrosion, the stephanoporate framework titanium foil sheet of formation can reach 〉=200M
2The high-specific surface area of/g, titanium dioxide has good insulation property simultaneously, and the titanium dioxide dielectric layer of thickness 500nm can long-term safety use under 220V voltage.According to capacitance equation
C＝εS*10
-12/3.6*πd (F)
Wherein: ε: dielectric constant 90-114
S: electrode area cm
2200M
2/ g
D: medium thickness cm 500nm
By this method, be easy to obtain the ultracapacitor of 300F/220V.
For solid super capacitor electrokinetic cell of the present invention better is described, following examples describe in detail,
Embodiment: 1
At the thick 20*20cm of the 0.2mm of a slice titanium aluminum ratio 60/40
2The titanium-aluminium alloy paillon foil, except a bight, 95% is immersed in 10% the hydrochloric acid, keeps corrosion reaction 6-8h at room temperature, up to there not being bubble to produce.Stephanoporate framework titanium foil sheet after will corroding then clear water wash clean, oven dry.Under 1000 ℃ aerobic condition, heat 2h again, form the thick rutile titanium dioxide oxide-film in the 500nm left and right sides at the duct of stephanoporate framework titanium foil sheet inner surface.Behind the cool to room temperature, be immersed in N-methyl-3, in 4-ethylidene dioxy pyrroles and the Lian dibenzyl sulfoxide mixed liquor, be heated to 80 degree, cause N-methyl 3,4-ethylidene dioxy pyrroles polymerisation in bulk, and cover titanium dioxide oxide-film surface, form conductive polymer cathode.
Detect capacitance C=1.33F. puncture voltage: 865V
Embodiment 2:
At the thick 20*20cm of the 0.2mm of a slice titanium aluminum ratio 50/50
2The titanium-aluminium alloy paillon foil, except a bight, 95% is immersed in 10% the hydrochloric acid, keeps corrosion reaction 6-8h at room temperature, up to there not being bubble to produce.Stephanoporate framework titanium foil sheet after will corroding then clear water wash clean, oven dry.Under 1000 ℃ aerobic condition, heat 2h again, form the thick rutile titanium dioxide oxide-film in the 500nm left and right sides at the duct of stephanoporate framework titanium foil sheet inner surface.Behind the cool to room temperature, be immersed in N-methyl-3, in 4-ethylidene dioxy pyrroles and the Lian dibenzyl sulfoxide mixed liquor, be heated to 80 degree, cause N-methyl-3,4-ethylidene dioxy pyrroles polymerisation in bulk, and cover titanium dioxide oxide-film surface, form conductive polymer cathode.
Detect capacitance C=1.41F. puncture voltage: 780V
Embodiment 3:
At the thick 20*20cm of the 0.2mm of a slice titanium aluminum ratio 70/30
2The titanium-aluminium alloy paillon foil, except a bight, 95% is immersed in 10% the hydrochloric acid, keeps corrosion reaction 6-8h at room temperature, up to there not being bubble to produce.Stephanoporate framework titanium foil sheet after will corroding then clear water wash clean, oven dry.Under 1000 ℃ aerobic condition, heat 2h again, form the thick rutile titanium dioxide oxide-film in the 500nm left and right sides at the duct of stephanoporate framework titanium foil sheet inner surface.Behind the cool to room temperature, be immersed in N-methyl-3, in 4-ethylidene dioxy pyrroles and the Lian dibenzyl sulfoxide mixed liquor, be heated to 80 degree, cause N-methyl-3,4-ethylidene dioxy pyrroles polymerisation in bulk, and cover titanium dioxide oxide-film surface, form conductive polymer cathode.
Detect capacitance C=1.06F. puncture voltage: 930V
Embodiment 4:
At the thick 20*20cm of the 0.2mm of a slice titanium aluminum ratio 60/40
2The titanium-aluminium alloy paillon foil, except a bight, 95% is immersed in 10% the hydrochloric acid, keeps corrosion reaction 6-8h at room temperature, up to there not being bubble to produce.Stephanoporate framework titanium foil sheet after will corroding then clear water wash clean, oven dry.Under 1000 ℃ aerobic condition, heat 2h again, form the thick rutile titanium dioxide oxide-film in the 500nm left and right sides at the duct of stephanoporate framework titanium foil sheet inner surface.Behind the cool to room temperature, be immersed in N-methyl 3, in 4-ethylidene dioxy pyrroles and the Lian diphenyl sulfoxide mixed liquor, be heated to 80 degree, cause 3,4-ethylidene dioxy pyrroles polymerisation in bulk, and cover titanium dioxide oxide-film surface, form conductive polymer cathode.
Detect capacitance C=1.12F. puncture voltage: 852V
Embodiment 5:
At the thick 20*20cm of the 0.2mm of a slice titanium aluminum ratio 60/40
2The titanium-aluminium alloy paillon foil, except a bight, 95% is immersed in 10% the hydrochloric acid, keeps corrosion reaction 6-8h at room temperature, up to there not being bubble to produce.Stephanoporate framework titanium foil sheet after will corroding then clear water wash clean, oven dry.Under 910 ℃ aerobic condition, heat 2h again, form the thick rutile titanium dioxide oxide-film in the 500nm left and right sides at the duct of stephanoporate framework titanium foil sheet inner surface.Behind the cool to room temperature, be immersed in N-methyl-3, in 4-ethylidene dioxy pyrroles and the Lian dibenzyl sulfoxide mixed liquor, be heated to 80 degree, cause N-methyl 3,4-ethylidene dioxy pyrroles polymerisation in bulk, and cover titanium dioxide oxide-film surface, form conductive polymer cathode.
Detect capacitance C=1.30F. puncture voltage: 806V
Embodiment 6
The 20*20cm that the 0.2mm of 20 titanium aluminum ratios 60/40 is thick
2The titanium-aluminium alloy paillon foil, except a bight, 95% is immersed in 10% the hydrochloric acid, keeps corrosion reaction 6-8h at room temperature, up to there not being bubble to produce.Stephanoporate framework titanium foil sheet after will corroding then clear water wash clean, oven dry.Under 1000 ℃ aerobic condition, heat 2h again, form the thick rutile titanium dioxide oxide-film in the 500nm left and right sides at the duct of stephanoporate framework titanium foil sheet inner surface.Behind the cool to room temperature, not corrosion bight boring with 20 stephanoporate framework titanium foil sheet, pass closely lamination of back with copper rod, nut is fastening on both sides, all is immersed in N-methyl-3 then except that the bight, in 4-ethylidene dioxy pyrroles and the Lian dibenzyl sulfoxide mixed liquor, be heated to 80 degree, cause N-methyl-3,4-ethylidene dioxy pyrroles polymerisation in bulk, and cover titanium dioxide oxide-film surface, form conductive polymer cathode.
Detect capacitance C=22.6F. puncture voltage: 830V
Embodiment 7:
The super capacitor sheet group parallel connection of embodiment 6 is assembled into power battery pack, and copper rod connects 220V DC power supply anode, and conducting polymer connects negative electrode, with the charged with direct current of 220V/10A, charges into electric weight with the kilowatt-hour meter detection.
Charge into electric energy: 0.13 degree.
Claims (9)
1. one kind with ultracapacitor electrokinetic cell and the manufacturing process thereof of titanium dioxide as dielectric layer, it is characterized in that capacitor anode adopts the titanium-aluminium alloy paillon foil, obtain the porousness skeleton titanium foil sheet of high-specific surface area by chemical corrosion, then porousness skeleton titanium foil sheet is passed through heated oxide, obtain the layer of titanium dioxide dielectric layer at titanium foil inner duct surface oxidation, usefulness conducting polymer monomer dipping duct, and polymerization at last covers titanium dioxide surface becomes capacitor cathode.
2. titanium-aluminium alloy paillon foil according to claim 1, thickness are 0.1～2.0 millimeter, and optimum thickness is 0.2～0.5 millimeter.
3. according to the described conducting polymer monomer of claim 1, be to adopt a kind of substituted alkyl dioxy pyrroles, have general formula
(A) chemical constitution:
Wherein: the alkyl of R1=H or C1～C3
The alkyl of R2=C1～C3.
4. high specific surface area porous property titanium foil sheet according to claim 1 is characterized in that adopting titanium-aluminium alloy paper tinsel plate, erodes the metallic aluminium composition in aqueous hydrochloric acid solution, forms a kind of skeleton titanium foil sheet of inner porous.
5. titanium-aluminium alloy paper tinsel plate according to claim 4 is characterized in that being made up of Titanium and metallic aluminium melting, Titanium weight content 30～90%, and the metallic aluminium weight content is 70～10%.
6. aqueous hydrochloric acid solution according to claim 4 is characterized in that concentration is 0.1～36%.
7. heated oxide method according to claim 1, it is characterized in that the skeleton titanium foil sheet of porous is put into 901～1200 ℃ and the high temperature furnace heated oxide that fills oxygen, the duct inner surface of stephanoporate framework titanium foil sheet is oxidized to one deck rutile titanium dioxide oxide-film.
8. according to the conducting polymer preparation method under the claim 1, it is characterized in that the conducting polymer monomer of general formula (A) is mixed with the radical initiator with general formula (B), after heating, cause the polymerisation in bulk of general formula (A) compound.
Wherein: the alkyl of R3:C1～C8, phenyl, tolyl or benzyl
The alkyl of R4:C1～C8, phenyl, tolyl or benzyl.
9. polymerization according to claim 8, its polymerization temperature are 60～120 degree.
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|---|---|---|---|
| CN200910049029A CN101859645A (en) | 2009-04-09 | 2009-04-09 | Large power super capacitor power battery |
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| CN200910049029A CN101859645A (en) | 2009-04-09 | 2009-04-09 | Large power super capacitor power battery |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103811481A (en) * | 2012-11-12 | 2014-05-21 | 南亚科技股份有限公司 | Semiconductor Device With Rutile Titanium Oxide Dielectric Film |
| CN103915512A (en) * | 2013-01-02 | 2014-07-09 | 南亚科技股份有限公司 | Semiconductor device with rutile titanium oxide dielectric film |
-
2009
- 2009-04-09 CN CN200910049029A patent/CN101859645A/en active Pending
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103811481A (en) * | 2012-11-12 | 2014-05-21 | 南亚科技股份有限公司 | Semiconductor Device With Rutile Titanium Oxide Dielectric Film |
| CN103915512A (en) * | 2013-01-02 | 2014-07-09 | 南亚科技股份有限公司 | Semiconductor device with rutile titanium oxide dielectric film |
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Application publication date: 20101013 |