CN102439771B - Porous conductive active composite electrode used in lithium ion battery - Google Patents
Porous conductive active composite electrode used in lithium ion battery Download PDFInfo
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- CN102439771B CN102439771B CN201180001321.8A CN201180001321A CN102439771B CN 102439771 B CN102439771 B CN 102439771B CN 201180001321 A CN201180001321 A CN 201180001321A CN 102439771 B CN102439771 B CN 102439771B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1391—Processes of manufacture of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/621—Binders
- H01M4/622—Binders being polymers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
- H01M4/625—Carbon or graphite
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
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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
Abstract
Active composite materials are diffused in a conductive porous matrix, and the conductive porous matrix is formed on a current collector to form a composite lithium ion battery electrode. The active composite materials comprise nanocluster active materials diffused on a conductive skeleton structure, the conductive skeleton structure comprises a conductive polymer or a conductive fibril. The active materials are metal base materials comprising one or more elements, such as tin, aluminum, silicon, titanium; or carbon base materials comprising one or more carbon materials, such as graphite, carbon fiber, carbon nanotube; or a combination of the metal base materials and the carbon base materials. The particle size of the active material is between 1 nanometer to 10 micrometers. By an in-situ polymerization method or a chemical graft method, the active materials are diffused in the conductive skeleton. The conductive porous matrix comprises a conductive polymer adhesive and a lithium ion diffusion channel generated by a pore forming agent, and conductive particles.
Description
[technical field]
The present invention relates to the electrode of lithium ion battery, particularly comprise the electrode of active composite material; This active composite material is dispersed in conductivity porous matrix; In this conductivity porous matrix, there is passage to spread for lithium ion.
[background technology]
Lithium ion battery is for multiple portable electric appts, as mobile phone and laptop computer.Although lithium ion battery is enough competent at for portable electric appts, Come demand does not comprise for the battery of electric motor car than the higher capacitance of those existing battery needs.There is the whole bag of tricks for improving the specific capacity of lithium ion battery material, such as the open text 2011/0114254,2008/0237536,2010/0021819,2010/0119942,2010/0143798,2010/0285365,2010/0062338 of United States Patent (USP), and loose structure anode and the composite anode in International Publication WO 2008/021961 and European patent 1 207 572, described.Although these anodes can improve battery performance, but still have and need to seek to improve lithium ion cell electrode performance and take into account the technology that processing procedure is simple, low-cost and can produce in batches simultaneously, with can supply future the demand of electric motor car and portable electric appts on a large scale.
[summary of the invention]
The present invention relates to composite lithium ion cell electrode, it is dispersed in a conductivity porous matrix containing an active composite material, and this conductivity porous matrix is formed on a collector.This active composite material is dispersed in a conducting matrix grain structure containing the active material of nanocluster.This active material is atomic tin, aluminium, silicon, titanium and carbon, and its particle size is between about 1 nanometer to 10 micron.Conductivity skeleton comprises at least one conducting polymer or a Dao electricity Xian Silk.By in-situ polymerization or chemical graft method, active material is dispersed on conducting matrix grain.
Conductivity porous matrix comprises an electric conductive polymer adhesive and lithium ion diffusion admittance; This passage is formed by pore creating material during in active composite material is blended in conductivity porous matrix.This conductivity porous matrix also comprises electroconductive particle.
[accompanying drawing explanation]
Fig. 1 is the schematic diagram of the composite lithium ion cell electrode of one embodiment of the invention.
Fig. 2 is the schematic diagram for the active composite material of Fig. 1 electrode.
[embodiment]
Referring to Fig. 1, show composite lithium ion cell electrode 10 of the present invention.In the embodiment shown in fig. 1, electrode comprises collector 20 (current collector), its normally conductive metal sheet as copper.Be placed on collector 20 is that an active composite material 30 is dispersed in a conductivity porous matrix 40.This active composite material comprises particulate active material 32, as shown in Figure 2, is dispersed in conductivity skeleton structure 34.Active material 32 has particulate structure, and its granular size scope is between about 1 nanometer is to about 10 microns.When this electrode is used as anode, particle comprises that metal_based material is as tin, aluminium, silicon, titanium, or carbon-based material is as graphite, carbon fiber, CNT (carbon nano-tube) (CNT), or combinations thereof.In anode, these materials provide super embedding medium (intercalation media) in the charging stage for lithium ion.At discharge regime, lithium ion moves to negative electrode from anode.Due to the embedding at lithium ion with the change in volume causing during deviating from, at the charging and discharging week after date repeating, solid metal active material can produce fragmentation (being cleaved into less particle).Using the benefit of nanometer particle active material is to avoid this problem, also can provide a larger surface area for embedding lithium (lithium intercalation).
Conductivity skeleton 34 comprises at least one conducting polymer or a conduction fibril (conductive filament), and by situ aggregation method or chemical graft process (will in following discussion), active material 32 be dispersed on this conductivity skeleton.By this way active material is separated on conductivity skeleton, can avoid active material conglomerate in porous, electrically conductive matrix 40, so the present invention has increased the feasibility that batch production is manufactured.
The conducting polymer of conductivity skeleton 34 comprises pyrroles (pyrrole), aniline (aniline), thiophene (thiofuran); Or conduction fibril also can be used as skeleton 34 as CNT (carbon nano-tube) or carbon nano-fiber.As can see from Figure 2, skeleton 34 and the structure tool microchannel that the active material 32 disperseing forms, provide lithium ion diffusion admittance to active material 32.Lithium ion embeds to be increased, thereby the capacitance of battery is just improved by this active composite material 30.During charging and discharging, when lithium ion embeds and deviates from, microchannel also contributes to provide space for the expansion of active material particles and contraction.
Active composite material 30 is dispersed in conductivity porous matrix 40, as shown in Figure 1.Conductivity porous matrix 40 comprises an electric conductive polymer adhesive (polymeric binder) and lithium ion diffusion admittance 42, this passage in active composite material is blended in conductivity porous matrix during by pore-creating material production (will discuss below).Electric conductive polymer adhesive can be a kind of improved pyrroles, aniline or thiophene, or other suitable electric conductive polymers, and tool conductance is higher than the material of 10S/cm.Lithium ion passage 42 provides lithium by electrode surface, to be moved to the path of inner active material 32.In addition, during charging and discharging, when lithium ion embeds and deviates from, passage 42 contributes to provide space for the expansion of whole active electrode and contraction.At an embodiment, the cumulative volume of passage is less than 5% of electrode.
In order to increase the conductivity of porous matrix 40, at least one electroconductive particle is comprised in conductivity porous matrix as particle 50 or 60.In the embodiment of Fig. 1, particle 50 is graphite, and particle 60 is carbon black (carbon black).But, also can select other electroconductive particles to be used in porous matrix 40.
A typical method of making electrode 10 is described below.The formation of active composite material 30 comprises from a kind of suitable precursor solution (precursor solution) if Precipitation active material 32 tin, aluminium, silicon or titanium precursor body salt (nitrate, carbonate etc.) is as tin, aluminium, silicon or titanium.Precursor solution is mixed in additive as sulfonate (sulfonate), imines (imine) and nitride (nitride).Then the precursor powder that dehydrates and be precipitated, its particle size is approximately 1-100 micron.Then, in the air lower than 1000 ℃ or inert environments, this sediment is heat-treated, produce reduction/calcined powder, after grinding, particle size can be reduced in the scope that is less than 100 microns, preferably in the scope of 1 nanometer to 10 micron.The method tool meets cost benefit, transreplication and can be mass feasibility.
For active material 32 is dispersed in skeleton structure 34, can choice for use several method.One of them method is carbon fiber, CNT (carbon nano-tube) and/or carbon-point are carried out to surface treatment, and a carboxyl of generation (COOH) to be tied up on carbon back skeleton.Active material particulate mixes with additive, as APTES (aminopropyltriethoxywerene werene), APTMS (APTES) or APPA (2-amino-5-phosphine-3-penetenoic acid), then through rinsing and dry after form the active material powder having activated.In order to form carboxyl in carbon skeleton structure, by carbon skeleton structure and a reagent mix, as EDC (N-(3-dimethylamino-propyl)-N '-ethyl-carbodiimide hydrochloride) or NHS (N-hydroxy-succinamide sulfonate sodium).This has the carbon skeleton structure of carboxyl and the solution of this activating activities material powder to carry out chemical action through mixing, and this active material is combined on this carbon back skeleton.
At another, active material is dispersed in the embodiment on skeleton, has used situ aggregation method.Particulate tin, aluminium, silicon or titanium mix with an additive, as sulfonic acid, sodium salt or sulfonate.This mixture is added to one containing polymer solution, as pyrroles, aniline, thiophene.Add again an additive as ferric trichloride or ammonium sulfate.In a deoxidation solution, at the temperature of about 10 ℃, polymerization reaction take place.The active composite material producing is exactly that active material is dispersed on a stephanoporate framework.
First atomic active material is dispersed on skeleton to prepare an active material compound, then active material compound is incorporated to conductivity porous matrix, so active material particles can conglomerate, and thereby improves the area for embedding lithium.In order to set up conductivity porous matrix, by a conducting polymer, obtain an adhesive as pyrroles, aniline or thiophene surface modification (surface-modified); By this active material compound, conductive polymer adhesive and a pore creating material (its can be pore-creating material and/or expanded material as carbonate, (NH
4)
2cO
3or C
2h
4n
4o
2), and other electroconductive particle mixes as particle 50 and/or 60 (graphite, carbon black).By this mixture apply collector 20 as copper sheet on, through bleed and solvent evaporation after, leave active material compound and electroconductive particle and be dispersed in porous, electrically conductive matrix; Pore-creating material forms hole, hole And and produces continuous interconnection duct in matrix, is provided as the passage that lithium ion moves.
Although described each embodiment of the present invention, be not limited in these embodiment.Various variations and change will be understood by those skilled in the art.These variations and change comprise within the scope of the appended claims.
Claims (15)
1. a composite lithium ion cell electrode, comprises
One active composite material is dispersed in a conductivity porous matrix, and this conductivity porous matrix is formed on a collector; This active composite material comprises that an active material is dispersed in a conductivity skeleton structure, the atomic granular size of active material is less than 10 microns, comprise following at least one material: a metal_based material, comprise one or more elements, described element comprises tin, aluminium, silicon or titanium; Or a carbon-based material, comprises one or more carbon materials, and described carbon material comprises graphite, carbon fiber or carbon nano-tube; Or the composition of this metal_based material and this carbon-based material; Conductivity skeleton comprises at least one conducting polymer or a conduction fibril; By a situ aggregation method or a chemical graft process, described active material is dispersed on described conductivity skeleton by chemical action;
Described conductivity porous matrix comprises an electric conductive polymer adhesive and lithium ion diffusion admittance, its passage in active composite material is blended in conductivity porous matrix during by pore creating material, formed, described conductivity porous matrix also comprises the conducting particles of particulate.
2. composite lithium ion cell electrode as claimed in claim 1, wherein said collector is a copper sheet.
3. composite lithium ion cell electrode as claimed in claim 1, wherein said conducting particles is carbon black and/or graphite.
4. composite lithium ion cell electrode as claimed in claim 1, wherein said conductivity skeleton is a carbon fiber and/or CNT (carbon nano-tube).
5. composite lithium ion cell electrode as claimed in claim 1, wherein said conductivity skeleton is electric conductive polymer.
6. composite lithium ion cell electrode as claimed in claim 1, wherein said electrode is anode.
7. composite lithium ion cell electrode as claimed in claim 1, wherein said electric conductive polymer adhesive comprises polypyrrole, polyaniline or polythiophene.
8. composite lithium ion cell electrode as claimed in claim 1, wherein said pore creating material comprises at least one pore-creating material or expanded material.
9. make a method for composite lithium ion cell electrode claimed in claim 1, comprising:
From the precursor solution of a kind of tin, aluminium, silicon or titanium precursor body salt or its mixture, mix with following one or more additives: sulfonate, imines and nitride; Precipitation Metal Substrate active material sediment;
Sediment dehydrates and the precursor powder that is precipitated, and its particle size is 1-100 micron;
Then, in the air lower than 1000 ° of C or inert environments, this sediment is heat-treated, obtain the active material powder of reduction calcining;
After further grinding, active material particulate size is reduced;
Active material is dispersed on a conductivity skeleton by a situ aggregation method or a chemical graft process, by chemical action, forms active composite material.
10. a method claimed in claim 9, wherein active material particulate size is less than the scope of 10 microns more than 1 nanometer.
11. 1 kinds of methods of making composite lithium ion cell electrode claimed in claim 1, comprising: framework material and a reagent are reacted, form carboxyl on this framework material, this framework material comprises carbon fiber, CNT (carbon nano-tube) or carbon-point; Active material particulate mixes with one or more additives for activating activities material, to form an active material having activated; Then this has the framework material of carboxyl and the solution of this activating activities material powder and produces chemical effect through mixing, and this active material is combined on this framework material.
12. 1 kinds of methods of making composite lithium ion cell electrode claimed in claim 1, comprising: mixed active particles of material is in the polymeric solution of a conducting polymer, to disperse this active material on conductivity skeleton.
13. methods as claimed in claim 12, wherein said conducting polymer comprises polypyrrole, polyaniline or polythiophene.
14. 1 kinds of methods of making composite lithium ion cell electrode claimed in claim 1, comprising: active material is dispersed on a conductivity skeleton by a situ aggregation method or a chemical graft process, by chemical action, forms active composite material; Described active composite material is added in a mixture, and this mixture comprises a conductive polymer adhesive, by a conducting polymer, through surface modification, obtains this conductive polymer adhesive; This mixture also comprises a pore creating material, and its material is pore-creating material or expanded material or its combination; This mixture also comprises conducting particles; This mixture is applied on collector, and to form a porous, electrically conductive matrix, active composite material and conducting particles are dispersed in wherein.
15. methods as claimed in claim 14, wherein said conducting polymer comprises polypyrrole, polyaniline or polythiophene.
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| PCT/CN2011/078672 WO2013026190A1 (en) | 2011-08-19 | 2011-08-19 | Porous conductive active composite electrode for lithium ion batteries |
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| Publication Number | Publication Date |
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| CN102439771A CN102439771A (en) | 2012-05-02 |
| CN102439771B true CN102439771B (en) | 2014-04-09 |
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| CN201180001321.8A Expired - Fee Related CN102439771B (en) | 2011-08-19 | 2011-08-19 | Porous conductive active composite electrode used in lithium ion battery |
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| Country | Link |
|---|---|
| CN (1) | CN102439771B (en) |
| HK (1) | HK1173558A1 (en) |
| WO (1) | WO2013026190A1 (en) |
Families Citing this family (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US9431651B2 (en) | 2013-08-30 | 2016-08-30 | Hong Kong Applied Science and Technology Research Institute Company Limited | Composite material for a lithium ion battery anode and a method of producing the same |
| CN103904299B (en) * | 2014-03-24 | 2015-10-28 | 宁德新能源科技有限公司 | Lithium rechargeable battery and cathode pole piece thereof |
| JP5999399B2 (en) * | 2014-09-08 | 2016-09-28 | Jsr株式会社 | Binder composition for lithium ion secondary battery electrode, slurry for lithium ion secondary battery electrode, lithium ion secondary battery electrode, and lithium ion secondary battery |
| CN106861762B (en) * | 2015-12-12 | 2019-03-22 | 中国科学院大连化学物理研究所 | The synthesis of metal oxide nano cluster and nano-cluster and the application in water oxygen |
| CN108666568A (en) * | 2017-04-01 | 2018-10-16 | 清华大学 | Anode of lithium ion battery |
| CN109473633B (en) * | 2017-09-07 | 2021-06-11 | 上海杉杉科技有限公司 | Nano silicon-based composite fiber negative electrode material of lithium ion battery and preparation method of nano silicon-based composite fiber negative electrode material |
| CN109205743B (en) * | 2018-11-02 | 2021-04-13 | 南京工业大学 | Preparation method and application of carbon nanotube composite titanium oxide porous carbon material |
| CN109509877B (en) * | 2018-11-30 | 2020-12-11 | 清华大学深圳研究生院 | Carbon-coated porous metal coating current collector, preparation method and lithium battery |
| CN109950464A (en) * | 2019-02-01 | 2019-06-28 | 湖北锂诺新能源科技有限公司 | A kind of porous silicon-carbon cathode pole piece and preparation method thereof |
| KR102203515B1 (en) * | 2020-02-28 | 2021-01-14 | 서울대학교산학협력단 | Method of preparing electrodes for lithium secondary battery |
| CN113278820B (en) * | 2021-05-21 | 2022-06-17 | 中南大学 | Electrode material for lithium extraction in salt lake, preparation method of electrode material and electrode for lithium extraction in salt lake |
| CN116741993A (en) * | 2022-03-03 | 2023-09-12 | 比亚迪股份有限公司 | Electrode plate, preparation method thereof and lithium battery |
| CN115312777A (en) * | 2022-09-07 | 2022-11-08 | 湖北亿纬动力有限公司 | Low-tortuosity thick electrode and preparation method and application thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101009368A (en) * | 2001-03-20 | 2007-08-01 | 爱克索里奥克斯公司 | Mesoporous network electrode for electrochemical cell |
| CN101499522A (en) * | 2008-01-28 | 2009-08-05 | 财团法人工业技术研究院 | Anode material of lithium battery and its production method, lithium secondary battery employing the same |
| CN101894940A (en) * | 2010-08-03 | 2010-11-24 | 哈尔滨工业大学 | Porous silicon-based cathode for lithium battery and preparation method thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US8936874B2 (en) * | 2008-06-04 | 2015-01-20 | Nanotek Instruments, Inc. | Conductive nanocomposite-based electrodes for lithium batteries |
| CA2638410A1 (en) * | 2008-07-28 | 2010-01-28 | Hydro-Quebec | Composite electrode material |
-
2011
- 2011-08-19 WO PCT/CN2011/078672 patent/WO2013026190A1/en active Application Filing
- 2011-08-19 CN CN201180001321.8A patent/CN102439771B/en not_active Expired - Fee Related
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101009368A (en) * | 2001-03-20 | 2007-08-01 | 爱克索里奥克斯公司 | Mesoporous network electrode for electrochemical cell |
| CN101499522A (en) * | 2008-01-28 | 2009-08-05 | 财团法人工业技术研究院 | Anode material of lithium battery and its production method, lithium secondary battery employing the same |
| CN101894940A (en) * | 2010-08-03 | 2010-11-24 | 哈尔滨工业大学 | Porous silicon-based cathode for lithium battery and preparation method thereof |
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| CN102439771A (en) | 2012-05-02 |
| WO2013026190A1 (en) | 2013-02-28 |
| HK1173558A1 (en) | 2013-05-16 |
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