CN101662034A - Method for preparing electrolyte of all-vanadium redox flow batteries - Google Patents
Method for preparing electrolyte of all-vanadium redox flow batteries Download PDFInfo
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- CN101662034A CN101662034A CN200910307744A CN200910307744A CN101662034A CN 101662034 A CN101662034 A CN 101662034A CN 200910307744 A CN200910307744 A CN 200910307744A CN 200910307744 A CN200910307744 A CN 200910307744A CN 101662034 A CN101662034 A CN 101662034A
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- vanadium
- electrolyte
- redox flow
- vanadium redox
- flow battery
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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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- 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
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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Abstract
The invention relates to a method for preparing electrolyte of all-vanadium redox flow batteries and belongs to the field of battery electrolyte. A technical problem solved by the invention is providing a method for preparing electrolyte of all-vanadium redox flow batteries, and aqueous migration can be avoided while preparing the electrolyte by the method. The method for preparing electrolyte ofall-vanadium redox flow batteries comprises the following steps: heating VOSO4 to 40-60 DEG C; then charging sulfur-free reducing gas to prepare the electrolyte of the all-vanadium redox flow batteries. The method helps solve the technical problem of great errors in precision and purity of the electrolyte due to the aqueous migration of a diaphragm in the conventional electrolysis process, simplify preparation process of the electrolyte of the vanadium redox batteries, shorten preparation time, improve work efficiency, adequately utilize all vanadium raw materials, avoid waste of 1/3 vanadiumin electrolyte preparation by the conventional electrolysis process, save production cost and avoid waste of resources, and has wide application prospect.
Description
Technical field
The present invention relates to a kind of method for preparing all-vanadium redox flow battery electrolyte, belong to the battery electrolyte field.
Background technology
Present full vanadium ion fluid cell electrolyte mainly adopts the electrochemical process preparation, and its preparation method is: electrolysis in battery makes electrolyte with vanadic sulfate solution or vanadic oxide solution.Electrochemical process prepares electrolyte and has following defective:
1, electrochemical process prepares electrolyte and need carry out in barrier film, but the research of barrier film also is in the improvement stage at present, substantially all there is the problem of water migration in barrier film, causes during preparation electrolyte the precision and the purity error of the electrolyte that electrolysis goes out bigger in these barrier films easily, influences battery performance.
2, electrolysis concentration easily produces crystallization during greater than the solution of 1.8mol/L and stops up barrier film.
If trivalent vanadium and tetravalence vanadium ratio are not 1: 1 in 3 prepared electrolyte, the current potential that makes vanadium cell is inconsistent and cause efficiency for charge-discharge low, also can add the big flood migration and make the volume capacity of electrolyte at battery the two poles of the earth inconsistent.
Because vanadium raw materials has 1/3 as anode, there is 2/3 vanadium raw materials to carry out electrolysis when 4, electrochemical process prepares electrolyte, 1/2 waste liquid is arranged after the electrolysis, can cause 1/3 vanadium raw materials waste.
Therefore, preparation how to prevent during all-vanadium redox flow battery electrolyte the sealing transport phenomena generation, reduce cost, reduce the wasting of resources and become the technical barrier that this area presses for solution at present.
Summary of the invention
Technical problem to be solved by this invention provides a kind of method for preparing all-vanadium redox flow battery electrolyte, can prevent the generation of sealing transport phenomena when adopting this method to prepare electrolyte.
The method that the present invention prepares all-vanadium redox flow battery electrolyte is with VOSO
4Solution is heated to 40～60 ℃, feeds the not reducibility gas of sulfur-bearing then, makes all-vanadium redox flow battery electrolyte.
Wherein, the reducibility gas of above-mentioned not sulfur-bearing can be a reducibility gas commonly used, as: hydrogen and/or carbon monoxide.
Further, the reducibility gas of above-mentioned not sulfur-bearing is preferably hydrogen.The reaction response time with hydrogen is fast, and hydrogen can decompose by ammonia and make, and preparation time is short, and reaction condition is not harsh, can not endanger health of operators, and fail safe is higher.
Wherein, above-mentioned VOSO
4Concentration is preferably 1.5～1.7mol/L.
Wherein, when feeding the excessive velocities of hydrogen, local overheating produces turbulent, relatively more dangerous easily; It is slow excessively to feed hydrogen rate, and then reaction is abundant inadequately, subsequent reactions can not be carried out smoothly, because the reaction liberated heat of follow-up reaction needed front.When preparation total V density when being the all-vanadium redox flow battery electrolyte of 1.5～1.7mol/L, if prepare 4 valency vanadium and 3 valency vanadium concentration equate substantially be | C
4 valency vanadium-C
3 valency vanadium|/(C
4 valency vanadium+ C
3 valency vanadiumThe all-vanadium redox flow battery electrolyte of)≤0.1, then every liter of VOSO
4The amount that solution feeds hydrogen is 8.96 * 10
-3～2.528 * 10
-3Nm
3/ h, the hydrogen time that feeds can decide according to total vanadium amount size, as: when total vanadium amount is 1.4～1.7mol, feeds hydrogen and can make electrolyte after 0.45～0.6 hour.C
4 valency vanadium, C
3 valency vanadiumBe respectively the molar concentration of 4 valency vanadium, 3 valency vanadium.If preparation is the all-vanadium redox flow battery electrolyte of 3 valency vanadium, then every liter of VOSO entirely
4The amount that solution feeds hydrogen is 1.792 * 10
-2～5.056 * 10
-2Nm
3/ h, the hydrogen time that feeds can decide according to total vanadium amount size, as: when total vanadium amount is 1.4～1.7mol, feeds hydrogen and can make electrolyte after 0.45～0.6 hour.The electrolyte for preparing other concentration if desired, then the feeding amount of hydrogen can be according to VOSO
4The concrete concentration of solution is suitably regulated, and avoids producing local overheating and turbulent getting final product.
Wherein, above-mentioned VOSO
4Solution can directly adopt commercially available VOSO
4Solution also can directly prepare.In order to reduce production costs preferred directly preparation VOSO
4Solution.VOSO
4Solution can adopt following method to make:
To H
2SO
4The adding mol ratio is 1: 1～1.5 V in the solution
2O
5And V
2O
3, make VOSO
4Solution.V
2O
5And V
2O
3Add H
2SO
4In the time of in the solution, reaction meeting heat release, making part 3 valency vanadium is 4 valency vanadium by airborne dioxygen oxidation, so V
2O
3Mole can be a little more than V
2O
5Work as V
2O
5And V
2O
3Mol ratio be 1: 1.5 o'clock, with H
2SO
4Have micro-3 valency vanadium in the reaction gained solution, but its content is less, can ignore.Further, better for the electrolyte property that makes preparation, make the most approaching, the above-mentioned V of molar concentration of 3 valency vanadium and 4 valency vanadium in the gained electrolyte
2O
3, V
2O
5Mol ratio be preferably 1: 1.
Wherein, above-mentioned H
2SO
4Solution concentration is too high then bumping can to take place, and influences handling safety, if H
2SO
4Solution concentration is crossed to hang down and was then reacted slow, influences production efficiency.Above-mentioned H
2SO
4The concentrated sulfuric acid of solution preferred specific gravity 1.84 and water 1: 2 by volume～3 is mixed with and forms.
Wherein, above-mentioned H
2SO
4Solution is crossed at most can cause the wasting of resources, increases cost, above-mentioned H
2SO
4With V
2O
5Weight ratio be preferably 256～570: 115; Wherein, described H
2SO
4Weight be the weight of the concentrated sulfuric acid of proportion 1.84.
The method that the present invention prepares all-vanadium redox flow battery electrolyte has solved that traditional electrolysis process exists because electrolyte precision and purity that the water migration of barrier film causes have the very technical barrier of mistake, simplified preparation technology's program of electrolyte of vanadium redox battery, shortened preparation time, improved operating efficiency, utilize all vanadium raw materials fully, overcome the waste of the vanadium of 1/3 when the traditional electrical solution prepares electrolyte, saved production cost, avoided the wasting of resources, had broad application prospects.
Embodiment
The method that the present invention prepares all-vanadium redox flow battery electrolyte is with VOSO
4Solution is heated to 40～60 ℃, feeds the not reducibility gas of sulfur-bearing then, makes all-vanadium redox flow battery electrolyte.
Wherein, the reducibility gas of above-mentioned not sulfur-bearing can be a reducibility gas commonly used, as: hydrogen and/or carbon monoxide.
Further, the reducibility gas of above-mentioned not sulfur-bearing is preferably hydrogen.The reaction response time with hydrogen is fast, and hydrogen can decompose by ammonia and make, and preparation time is short, and reaction condition is not harsh, can not endanger health of operators, and fail safe is higher.
Wherein, above-mentioned VOSO
4Concentration is preferably 1.5～1.7mol/L.
Wherein, when feeding the excessive velocities of hydrogen, local overheating produces turbulent, relatively more dangerous easily; It is slow excessively to feed hydrogen rate, and then reaction is abundant inadequately, subsequent reactions can not be carried out smoothly, because the reaction liberated heat of follow-up reaction needed front.When preparation total V density when being the all-vanadium redox flow battery electrolyte of 1.5～1.7mol/L, if prepare 4 valency vanadium and 3 valency vanadium concentration equate substantially be | C
4 valency vanadium-C
3 valency vanadium|/(C
4 valency vanadium+ C
3 valency vanadiumThe all-vanadium redox flow battery electrolyte of)≤0.1, then every liter of VOSO
4The amount that solution feeds hydrogen is 8.96 * 10
-3～2.528 * 10
-3Nm
3/ h, the hydrogen time that feeds can decide according to total vanadium amount size, as: when total vanadium amount is 1.4～1.7mol, feeds hydrogen and can make electrolyte after 0.45～0.6 hour.C
4 valency vanadium, C
3 valency vanadiumBe respectively the molar concentration of 4 valency vanadium, 3 valency vanadium.If preparation is the all-vanadium redox flow battery electrolyte of 3 valency vanadium, then every liter of VOSO entirely
4The amount that solution feeds hydrogen is 1.792 * 10
-2～5.056 * 10
-2Nm
3/ h, the hydrogen time that feeds can decide according to total vanadium amount size, as: when total vanadium amount is 1.4～1.7mol, feeds hydrogen and can make electrolyte after 0.45～0.6 hour.The electrolyte for preparing other concentration if desired, then the feeding amount of hydrogen can be according to VOSO
4The concrete concentration of solution is suitably regulated, and avoids producing local overheating and turbulent getting final product.
Wherein, above-mentioned VOSO
4Solution can directly adopt commercially available VOSO
4Solution also can directly prepare.In order to reduce production costs preferred directly preparation VOSO
4Solution.VOSO
4Solution can adopt following method to make:
To H
2SO
4The adding mol ratio is 1: 1～1.5 V in the solution
2O
5And V
2O
3, make VOSO
4Solution.V
2O
5And V
2O
3Add H
2SO
4In the time of in the solution, reaction meeting heat release, making part 3 valency vanadium is 4 valency vanadium by airborne dioxygen oxidation, so V
2O
3Mole can be a little more than V
2O
5Work as V
2O
5And V
2O
3Mol ratio be 1: 1.5 o'clock, with H
2SO
4Have micro-3 valency vanadium in the reaction gained solution, but its content is less, can ignore.Further, better for the electrolyte property that makes preparation, make the most approaching, the above-mentioned V of molar concentration of 3 valency vanadium and 4 valency vanadium in the gained electrolyte
2O
3, V
2O
5Mol ratio be preferably 1: 1.
Wherein, above-mentioned H
2SO
4Solution concentration is too high then bumping can to take place, and influences handling safety, if H
2SO
4Solution concentration is crossed to hang down and was then reacted slow, influences production efficiency.Above-mentioned H
2SO
4The concentrated sulfuric acid of solution preferred specific gravity 1.84 and water 1: 2 by volume～3 is mixed with and forms.
Wherein, above-mentioned H
2SO
4Solution is crossed at most can cause the wasting of resources, increases cost, above-mentioned H
2SO
4With V
2O
5Weight ratio be preferably 256～570: 115; Wherein, described H
2SO
4Weight be the weight of the concentrated sulfuric acid of proportion 1.84.
Below in conjunction with embodiment the specific embodiment of the present invention is further described, does not therefore limit the present invention among the described scope of embodiments.
Implementing example 1 adopts the inventive method to prepare all-vanadium redox flow battery electrolyte
1, raw material:
V
2O
3: V
2O
3Content is more than 90%;
V
2O
5: analyze pure;
H
2SO
4: analyze pure, d=1.84;
H
2: the hydrogen that ammonia obtains after decomposing and the mist of nitrogen.
2, electrolyte preparation process:
Take by weighing 59.92 gram V
2O
3, 72.72 gram V
2O
5, the 372.4 gram concentrated sulfuric acids, and get an amount of distilled water, obtain the sulfuric acid solution of the vanadic sulfate of the blue look of 1L after the reaction.Test: sulfuric acid concentration 2.2mol/L, the concentration of 4 valency vanadium is 1.6mol/L in the vanadic sulfate.
In solution, feed hydrogen, the superficial gas velocity 2.0m/s of hydrogen, the amount of feeding is 4.213 * 10
-2Nm
3/ h feeds 0.5h.Superficial gas velocity (m/s)=amount (Nm
3/ h) * [reaction temperature (℃)+273]/273/ conversion zone sectional area/3600, the conversion zone sectional area is the pipe of feeding hydrogen or the sectional area of pipeline, its unit is m
2
Gained electrolyte is measured, and the result is: 3 valency vanadium concentration 1.6mol/L, the concentration 3.0mol/L of sulfuric acid.
Implementing example 2 adopts the inventive method to prepare all-vanadium redox flow battery electrolyte
1, raw material:
V
2O
3: V
2O
3Content is more than 90%;
V
2O
5: analyze pure;
H
2SO
4: analyze pure, d=1.84;
H
2: the hydrogen that ammonia obtains after decomposing and the mist of nitrogen.
2, electrolyte preparation process:
Take by weighing 59.92 gram V
2O
3, 72.72 gram V
2O
5, the 418.72 gram concentrated sulfuric acids, and get an amount of distilled water, obtain the sulfuric acid solution of the vanadic sulfate of the blue look of 1L after the reaction.Test: sulfuric acid concentration 2.6mol/L, the concentration of 4 valency vanadium is 1.6mol/L in the vanadic sulfate.
In solution, feed hydrogen, the superficial gas velocity 0.427m/s of hydrogen, the amount of feeding is 9.0 * 10
-3Nm
3/ h feeds 0.5h.
Gained electrolyte is measured, and the result is: 3 valency vanadium concentration 0.82mol/L, 4 valency vanadium concentration 0.78mol/L, the concentration 3.0mol/L of sulfuric acid.
Implementing example 3 adopts the inventive method to prepare all-vanadium redox flow battery electrolyte
1, raw material:
V
2O
3: V
2O
3Content is more than 90%;
V
2O
5: analyze pure;
H
2SO
4: analyze pure, d=1.84;
H
2And CO: the hydrogen that ammonia obtains after decomposing and the mist of nitrogen, the volume ratio of hydrogen and carbon monoxide is 1: 1.
2, electrolyte preparation process:
Take by weighing 59.92 gram V
2O
3, 72.72 gram V
2O
5, the 372.4 gram concentrated sulfuric acids, and get an amount of distilled water, obtain the sulfuric acid solution of the vanadic sulfate of the blue look of 1L after the reaction.Test: sulfuric acid concentration 2.2mol/L, the concentration of 4 valency vanadium is 1.6mol/L in the vanadic sulfate.
Feed hydrogen and carbon monoxide in solution, the superficial gas velocity 0.214m/s of hydrogen, the superficial gas velocity of carbon monoxide are 0.214m/s, and the amount of feeding is 9.0 * 10
-3Nm
3/ h feeds 0.5h.
Gained electrolyte is measured, and the result is: 3 valency vanadium concentration 1.6mol/L, the concentration 3.0mol/L of sulfuric acid.
Implementing example 4 adopts the inventive method to prepare all-vanadium redox flow battery electrolyte
1, raw material:
V
2O
3: V
2O
3Content is more than 90%;
V
2O
5: analyze pure;
H
2SO
4: analyze pure, d=1.84;
H
2And CO: the hydrogen that ammonia obtains after decomposing and the mist of nitrogen; The volume ratio of hydrogen and carbon monoxide is 1: 1.
2, electrolyte preparation process:
Take by weighing 59.92 gram V
2O
3, 72.72 gram V
2O
5, the 418.72 gram concentrated sulfuric acids, and get an amount of distilled water, obtain the sulfuric acid solution of the vanadic sulfate of the blue look of 1L after the reaction.Test: sulfuric acid concentration 2.6mol/L, the concentration of 4 valency vanadium of vanadic sulfate is 1.6mol/L.
In solution, feed hydrogen and carbon monoxide, the superficial gas velocity 0.214m/s of hydrogen, the superficial gas velocity 0.214m/s of carbon monoxide, the amount of feeding is 9.0 * 10
-3Nm
3/ h feeds 0.5h.
Gained electrolyte is measured, and the result is: 3 valency vanadium concentration 0.83mol/L, 4 valency vanadium concentration 0.77mol/L, the concentration 3.0mol/L of sulfuric acid.
Claims (10)
1. prepare the method for all-vanadium redox flow battery electrolyte, it is characterized in that: VOSO
4Solution is heated to 40～60 ℃, feeds the not reducibility gas of sulfur-bearing then, makes all-vanadium redox flow battery electrolyte.
2. the method for preparing all-vanadium redox flow battery electrolyte according to claim 1 is characterized in that: the reducibility gas of described not sulfur-bearing is hydrogen and/or carbon monoxide.
3. the method for preparing all-vanadium redox flow battery electrolyte according to claim 2 is characterized in that: the reducibility gas of described not sulfur-bearing is a hydrogen.
4. the method for preparing all-vanadium redox flow battery electrolyte according to claim 3 is characterized in that: described VOSO
4Concentration is 1.5～1.7mol/L.
5. the method for preparing all-vanadium redox flow battery electrolyte according to claim 4 is characterized in that: every liter of VOSO
4The amount that solution feeds hydrogen is 8.96 * 10
-3～2.528 * 10
-3Nm
3/ h makes 4 valency vanadium and 3 valency vanadium | C
4 valency vanadium-C
3 valency vanadium|/(C
4 valency vanadium+ C
3 valency vanadiumThe all-vanadium redox flow battery electrolyte of)≤0.1.
6. the method for preparing all-vanadium redox flow battery electrolyte according to claim 4 is characterized in that: every liter of VOSO
4The amount that solution feeds hydrogen is 1.792 * 10
-2～5.056 * 10
-2Nm
3/ h, making is the all-vanadium redox flow battery electrolyte of 3 valency vanadium entirely.
7. according to claim 5 or the 6 described methods that prepare all-vanadium redox flow battery electrolyte, it is characterized in that: when total vanadium amount was 1.4～1.7mol, the time that feeds hydrogen was 0.45～0.6 hour.
8. according to each described method for preparing all-vanadium redox flow battery electrolyte of claim 1～7, it is characterized in that described VOSO
4Solution adopts following method to make:
To H
2SO
4The adding mol ratio is 1: 1～1.5 V in the solution
2O
5And V
2O
3, make VOSO
4Solution.
9. the method for preparing all-vanadium redox flow battery electrolyte according to claim 8 is characterized in that: described H
2SO
4Solution is that the concentrated sulfuric acid of proportion 1.84 and water 1: 2 by volume～3 are mixed with and form; Described H
2SO
4With V
2O
5Weight ratio be 256～570: 115; Wherein, described H
2SO
4Weight be the weight of the concentrated sulfuric acid of proportion 1.84.
10. the method for preparing all-vanadium redox flow battery electrolyte according to claim 9 is characterized in that: described V
2O
3, V
2O
5Mol ratio be 1: 1.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2009103077447A CN101662034B (en) | 2009-09-25 | 2009-09-25 | Method for preparing electrolyte of all-vanadium redox flow batteries |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2009103077447A CN101662034B (en) | 2009-09-25 | 2009-09-25 | Method for preparing electrolyte of all-vanadium redox flow batteries |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN101662034A true CN101662034A (en) | 2010-03-03 |
| CN101662034B CN101662034B (en) | 2011-08-03 |
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ID=41789910
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN2009103077447A Expired - Fee Related CN101662034B (en) | 2009-09-25 | 2009-09-25 | Method for preparing electrolyte of all-vanadium redox flow batteries |
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|---|---|
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103151549A (en) * | 2013-01-31 | 2013-06-12 | 四川省川威集团有限公司 | Preparation method of high-purity vanadium battery electrolyte based on extraction-and-reverse-extraction system |
| WO2019206121A1 (en) * | 2018-04-27 | 2019-10-31 | 江苏泛宇能源有限公司 | Manufacturing method and device of flow battery electrolyte |
-
2009
- 2009-09-25 CN CN2009103077447A patent/CN101662034B/en not_active Expired - Fee Related
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103151549A (en) * | 2013-01-31 | 2013-06-12 | 四川省川威集团有限公司 | Preparation method of high-purity vanadium battery electrolyte based on extraction-and-reverse-extraction system |
| WO2019206121A1 (en) * | 2018-04-27 | 2019-10-31 | 江苏泛宇能源有限公司 | Manufacturing method and device of flow battery electrolyte |
| CN110416585A (en) * | 2018-04-27 | 2019-11-05 | 江苏泛宇能源有限公司 | The preparation method and preparation facilities of fluid cell electrolyte |
| CN110416585B (en) * | 2018-04-27 | 2020-10-23 | 江苏泛宇能源有限公司 | Preparation method and preparation device of flow battery electrolyte |
Also Published As
| Publication number | Publication date |
|---|---|
| CN101662034B (en) | 2011-08-03 |
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