CN103280339A - Method for preparing cerium oxide electrode of supercapacitor - Google Patents

Method for preparing cerium oxide electrode of supercapacitor Download PDF

Info

Publication number
CN103280339A
CN103280339A CN2013101276550A CN201310127655A CN103280339A CN 103280339 A CN103280339 A CN 103280339A CN 2013101276550 A CN2013101276550 A CN 2013101276550A CN 201310127655 A CN201310127655 A CN 201310127655A CN 103280339 A CN103280339 A CN 103280339A
Authority
CN
China
Prior art keywords
cerium oxide
oxide electrode
mixture
electrode
current collector
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
CN2013101276550A
Other languages
Chinese (zh)
Inventor
朱明原
史涛涛
聂林才
殷利民
薄伟强
胡业旻
李瑛�
金红明
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
University of Shanghai for Science and Technology
Original Assignee
University of Shanghai for Science and Technology
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by University of Shanghai for Science and Technology filed Critical University of Shanghai for Science and Technology
Priority to CN2013101276550A priority Critical patent/CN103280339A/en
Publication of CN103280339A publication Critical patent/CN103280339A/en
Pending legal-status Critical Current

Links

Images

Classifications

    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/13Energy storage using capacitors

Landscapes

  • Battery Electrode And Active Subsutance (AREA)

Abstract

The invention relates to a method for preparing a cerium oxide electrode of a supercapacitor. The method comprises the following steps: a) mixing and stirring ceria powder of which the particle size is less than 1 mum, conductive agent and binder according to a certain proportion, wherein the content of the conductive agent is 10-20 wt% of the total mass of the mixture, and the content of the binder is 10-20 wt% of the total mass of the mixture; and b) coating the mixture on a current collector, and drying to obtain the cerium oxide electrode.

Description

一种用于超级电容器的氧化铈电极的制备方法A kind of preparation method for the cerium oxide electrode of supercapacitor

技术领域 technical field

本发明涉及一种用于超级电容器的氧化铈电极的制备方法,属于化学工业及材料科学与工程技术领域。  The invention relates to a method for preparing a cerium oxide electrode used in a supercapacitor, and belongs to the technical fields of chemical industry and material science and engineering. the

背景技术 Background technique

超级电容器是一种拥有高能量密度,高功率和高循环性能的储能装置,和电池配套使用具有广阔的应用前景。现在已经广泛应用于航空航天、信息技术等各种需要瞬间大功率放电的领域。超级电容器分为双电层电容器和赝电容器,其中赝电容器比双电层电容器具有更高的比容量,因此更具有发展潜力。赝电容的电极材料主要是过渡金属氧化物,如氧化钌、氧化镍、氧化钴和氧化锰等。目前,赝电容电容器研究比较成功的是氧化钌/H2SO4,体系,但氧化钌价格高昂,且H2SO4溶液对电极集流体的要求较高,从而限制了其广泛应用。所以寻找低成本,高性能的电极材料势在必行。二氧化铈是一种很好的电极材料,它具有良好的电化学氧化还原性和较低的成本。Li等制备的二氧化铈和石墨烯的复合电极材料具有280Fg-1的比容量。集流体的应用也对电极材料的性能产生较大的影响,泡沫镍由于具有多孔的三维结构和高比表面积,是一种优秀的电极集流体材料。本专利利用泡沫镍等做集流体,氧化铈做活性材料,制备具有良好电化学性能的电极材料。  Supercapacitor is an energy storage device with high energy density, high power and high cycle performance, and it has broad application prospects when used in conjunction with batteries. Now it has been widely used in aerospace, information technology and other fields that require instantaneous high-power discharge. Supercapacitors are divided into electric double layer capacitors and pseudocapacitors, among which pseudocapacitors have higher specific capacity than electric double layer capacitors, so they have more development potential. The electrode materials of pseudocapacitors are mainly transition metal oxides, such as ruthenium oxide, nickel oxide, cobalt oxide, and manganese oxide. At present, the more successful research on pseudocapacitive capacitors is the ruthenium oxide/H 2 SO 4 system, but the price of ruthenium oxide is high, and the H 2 SO 4 solution has high requirements on the electrode collector, which limits its wide application. Therefore, it is imperative to find low-cost, high-performance electrode materials. Ceria is a good electrode material, which has good electrochemical redox properties and low cost. The composite electrode material of ceria and graphene prepared by Li et al. has a specific capacity of 280Fg -1 . The application of the current collector also has a great impact on the performance of the electrode material. Nickel foam is an excellent electrode current collector material due to its porous three-dimensional structure and high specific surface area. In this patent, nickel foam is used as a current collector, and cerium oxide is used as an active material to prepare an electrode material with good electrochemical performance.

发明内容 Contents of the invention

本发明的目的在于提供一种用于超级电容器的氧化铈电极的制备方法,以获得具有高比容量的超级电容器电极材料。  The object of the present invention is to provide a method for preparing a cerium oxide electrode for a supercapacitor, so as to obtain a supercapacitor electrode material with a high specific capacity. the

为达到上述目的,本发明采用如下技术方案:  To achieve the above object, the present invention adopts the following technical solutions:

一种用于超级电容器的氧化铈电极的制备方法,具有以下步骤:  A preparation method for a cerium oxide electrode for a supercapacitor, comprising the following steps:

a)将粒径小于1μm的二氧化铈粉末、导电剂和粘结剂按一定比例进行混合搅拌,其中导电剂含量为混合物总质量的10~20wt%,粘结剂含量为混合物总质量的10~20wt%; a) Mix and stir the ceria powder with a particle size of less than 1 μm, the conductive agent and the binder in a certain proportion, wherein the content of the conductive agent is 10-20wt% of the total mass of the mixture, and the content of the binder is 10% of the total mass of the mixture ~20wt%;

b)将混合物涂到集流体上,干燥后得到氧化铈电极。 b) The mixture is coated on the current collector and dried to obtain a cerium oxide electrode.

所述步骤b)或为:将步骤a)的混合物研磨,然后压成0.5~2μm厚的薄膜,将薄膜用10-50MPa的压力压在集流体上,得到氧化铈电极。  The step b) may be: grind the mixture in step a), and then press it into a film with a thickness of 0.5-2 μm, and press the film on the current collector with a pressure of 10-50 MPa to obtain a cerium oxide electrode. the

所述的导电剂为乙炔黑、碳纳米管、碳纳米微球中的一种或几种;粘结剂为聚偏氟乙烯或聚四氟乙烯溶解在二甲基乙酰胺或二甲基亚砜有机溶液中形成的溶液;集流体为泡沫镍,不锈钢网、镍片、钛片或石墨片。  The conductive agent is one or more of acetylene black, carbon nanotubes, and carbon nanospheres; the binder is polyvinylidene fluoride or polytetrafluoroethylene dissolved in dimethylacetamide or dimethylmethylene The solution formed in the sulfone organic solution; the current collector is nickel foam, stainless steel mesh, nickel sheet, titanium sheet or graphite sheet. the

与现有技术相比,本发明具有如下的突出的实质性特点和显著地进步:  Compared with the prior art, the present invention has the following prominent substantive features and remarkable progress:

a)泡沫镍集流体具有三维网状结构,提高了活性物质与电解液间的接触面积,从而提高了电极的比容量。 a) The nickel foam current collector has a three-dimensional network structure, which increases the contact area between the active material and the electrolyte, thereby increasing the specific capacity of the electrode.

b)与直接在集流体上沉积薄膜所得到的电极相比,本发明所制得的电极活性物质与集流体间的结合力更强,有利于延长电极的使用寿命;单位面积的活性物质负载质量更大,有利于提高电极的功率。  b) Compared with the electrode obtained by directly depositing a thin film on the current collector, the binding force between the electrode active material and the current collector prepared by the present invention is stronger, which is beneficial to prolong the service life of the electrode; the active material loading per unit area Larger mass is beneficial to increase the power of the electrode. the

附图说明 Description of drawings

图1是本发明实施例一和实施例二所制得电极的循环伏安测试图。  Fig. 1 is a cyclic voltammetry test chart of electrodes prepared in Example 1 and Example 2 of the present invention. the

图2是本发明实施例三中电极在碱性电解质液中测试的循环伏安性能图。  Fig. 2 is a diagram of the cyclic voltammetry performance of the electrode tested in the alkaline electrolyte solution in Example 3 of the present invention. the

图3是本发明实施例三中电极在中性电解质液中测试的循环伏安性能图。  Fig. 3 is a diagram of the cyclic voltammetry performance of the electrode tested in a neutral electrolyte solution in Example 3 of the present invention. the

具体实施方式Detailed ways

下面结合实施例对本发明的技术方案做进一步说明。  The technical solutions of the present invention will be further described below in conjunction with the embodiments. the

实施例一Embodiment one

将粒径小于1μm的氧化铈粉末、乙炔黑和聚偏氟乙烯(PVDF)按照质量比为80:10:10进行混合,将混合物置于磁力搅拌器上室温搅拌12小时后涂在大小为1×2cm的泡沫镍片上,然后置于真空干燥箱中120℃干燥12h,最终得到泡沫镍集流体氧化铈电极。 Mix cerium oxide powder with a particle size of less than 1 μm, acetylene black and polyvinylidene fluoride (PVDF) at a mass ratio of 80:10:10, place the mixture on a magnetic stirrer at room temperature and stir for 12 hours, and then spread it on a surface of size 1 ×2cm foamed nickel sheet, and then placed in a vacuum drying oven at 120 ° C for 12 hours to obtain a foamed nickel current collector cerium oxide electrode.

用0.1M Na2SO4做电解质溶液,饱和甘汞电极作为参比电极,铂为对电极对上述制得的电极进行循环伏安测试,如图1所示。扫描速率为10 mV s-1时,测得的比容为57 F g-1。  0.1M Na 2 SO 4 was used as the electrolyte solution, a saturated calomel electrode was used as the reference electrode, and platinum was used as the counter electrode to conduct cyclic voltammetry tests on the electrodes prepared above, as shown in Figure 1 . At a scan rate of 10 mV s -1 , the measured specific volume is 57 F g -1 .

实施例二Embodiment two

将粒径小于1μm的氧化铈粉末、乙炔黑和聚偏氟乙烯(PVDF)按照质量比为80:10:10进行混合,将混合物置于磁力搅拌器上室温搅拌12小时后涂在大小为1×1cm的石墨片上,然后置于真空干燥箱中120℃干燥12h,最终得到石墨集流体氧化铈电极。 Mix cerium oxide powder with a particle size of less than 1 μm, acetylene black and polyvinylidene fluoride (PVDF) at a mass ratio of 80:10:10, place the mixture on a magnetic stirrer at room temperature and stir for 12 hours, and then spread it on a surface of size 1 ×1cm graphite sheet, and then dried in a vacuum oven at 120°C for 12h to finally obtain a graphite current collector cerium oxide electrode.

用0.1M Na2SO4做电解质溶液,饱和甘汞电极作为参比电极,铂为对电极对上述制得的电极进行循环伏安测试,如图1所示。扫描速率为10 mV s-1时,测得的比容为7 F g-1。  0.1M Na 2 SO 4 was used as the electrolyte solution, a saturated calomel electrode was used as the reference electrode, and platinum was used as the counter electrode to conduct cyclic voltammetry tests on the electrodes prepared above, as shown in Figure 1 . At a scan rate of 10 mV s -1 , the measured specific volume is 7 F g -1 .

实施例三Embodiment three

将粒径小于1μm的氧化铈粉末、乙炔黑和聚四氟乙烯(PTFE)按照质量比为70:15:15进行混合,将混合物研磨后压成厚度为2μm左右的薄膜,待薄膜干燥后压在泡沫镍集流体上,得到氧化铈电极。 Mix cerium oxide powder with a particle size of less than 1 μm, acetylene black and polytetrafluoroethylene (PTFE) at a mass ratio of 70:15:15, grind the mixture and press it into a film with a thickness of about 2 μm, and press it after the film is dry. On the foamed nickel current collector, a cerium oxide electrode is obtained.

将所制得的氧化铈电极在碱性电解液中进行电化学性能测试。循环伏安测试中以饱和甘汞电极作为参比电极,铂为对电极,描速率为5 mV s-1,测试电压范围为0-0.4 V,如图2所示。在2M KOH、2M NaOH、2M LiOH电解液中进行循环伏安测试,得到的比容分别为241 F g-1 、152 F g-1 、87 F g-1。  The prepared cerium oxide electrode was tested for electrochemical performance in alkaline electrolyte. In the cyclic voltammetry test, a saturated calomel electrode was used as the reference electrode, platinum was used as the counter electrode, the scanning rate was 5 mV s -1 , and the test voltage range was 0-0.4 V, as shown in Figure 2. Cyclic voltammetry tests were performed in 2M KOH, 2M NaOH, and 2M LiOH electrolytes, and the obtained specific volumes were 241 F g -1 , 152 F g -1 , and 87 F g -1 , respectively.

将所制得的氧化铈电极在中性电解液中进行电化学性能测试。循环伏安测试中以饱和甘汞电极作为参比电极,铂为对电极,描速率为5 mV s-1,测试电压范围为0.5-0.9 V,如图3所示。在0.1M Na2SO4、0.1M K2SO4、0.1M (NH4)2SO4电解液中进行循环伏安测试,得到的比容分别为89 F g-1、61 F g-1、10 F g-1。  The prepared cerium oxide electrode was tested for electrochemical performance in neutral electrolyte. In the cyclic voltammetry test, a saturated calomel electrode was used as the reference electrode, platinum was used as the counter electrode, the scanning rate was 5 mV s -1 , and the test voltage range was 0.5-0.9 V, as shown in Figure 3. The cyclic voltammetry test was carried out in 0.1M Na 2 SO 4 , 0.1M K 2 SO 4 , 0.1M (NH 4 ) 2 SO 4 electrolytes, and the obtained specific volumes were 89 F g -1 , 61 F g -1 , 10 F g -1 .

Claims (3)

1.一种用于超级电容器的氧化铈电极的制备方法,其特征在于,具有以下步骤:  1. A preparation method for a cerium oxide electrode for supercapacitor, characterized in that, has the following steps: a)将粒径小于1μm的二氧化铈粉末、导电剂和粘结剂按一定比例进行混合搅拌,其中导电剂含量为混合物总质量的10~20wt%,粘结剂含量为混合物总质量的10~20wt%; a) Mix and stir the ceria powder with a particle size of less than 1 μm, the conductive agent and the binder in a certain proportion, wherein the content of the conductive agent is 10-20wt% of the total mass of the mixture, and the content of the binder is 10% of the total mass of the mixture ~20wt%; b)将混合物涂到集流体上,干燥后得到氧化铈电极。 b) The mixture is coated on the current collector and dried to obtain a cerium oxide electrode. 2.根据权利要求1所述的一种用于超级电容器的氧化铈电极的制备方法,其特征在于,所述步骤b)或为:将步骤a)的混合物研磨,然后压成0.5~2μm厚的薄膜,将薄膜用10-50MPa的压力压在集流体上,得到氧化铈电极。 2. A method for preparing a cerium oxide electrode for a supercapacitor according to claim 1, characterized in that the step b) is: grinding the mixture in step a), and then pressing it into a thickness of 0.5-2 μm The film is pressed on the current collector with a pressure of 10-50 MPa to obtain a cerium oxide electrode. 3.根据权利要求1或2所述的一种用于超级电容器的氧化铈电极的制备方法,其特征在于,所述的导电剂为乙炔黑、碳纳米管、碳纳米微球中的一种或几种;粘结剂为聚偏氟乙烯或聚四氟乙烯溶解在二甲基乙酰胺或二甲基亚砜有机溶液中形成的溶液;集流体为泡沫镍,不锈钢网、镍片、钛片或石墨片。 3. a kind of preparation method for the cerium oxide electrode of supercapacitor according to claim 1 and 2, is characterized in that, described conductive agent is a kind of in acetylene black, carbon nanotube, carbon nano microsphere or several kinds; the binder is a solution formed by dissolving polyvinylidene fluoride or polytetrafluoroethylene in dimethylacetamide or dimethyl sulfoxide organic solution; the current collector is nickel foam, stainless steel mesh, nickel sheet, titanium flakes or graphite flakes.
CN2013101276550A 2013-04-12 2013-04-12 Method for preparing cerium oxide electrode of supercapacitor Pending CN103280339A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN2013101276550A CN103280339A (en) 2013-04-12 2013-04-12 Method for preparing cerium oxide electrode of supercapacitor

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN2013101276550A CN103280339A (en) 2013-04-12 2013-04-12 Method for preparing cerium oxide electrode of supercapacitor

Publications (1)

Publication Number Publication Date
CN103280339A true CN103280339A (en) 2013-09-04

Family

ID=49062829

Family Applications (1)

Application Number Title Priority Date Filing Date
CN2013101276550A Pending CN103280339A (en) 2013-04-12 2013-04-12 Method for preparing cerium oxide electrode of supercapacitor

Country Status (1)

Country Link
CN (1) CN103280339A (en)

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN105116036A (en) * 2015-08-13 2015-12-02 东北大学 Preparation and usage method for cerium (IV) ion selectivity electrodes
CN106531454A (en) * 2016-12-29 2017-03-22 铜陵市胜美达电子制造有限公司 Ageing-resistant cobaltosic oxide nanowire carbon aerogel composite supercapacitor positive electrode material and preparation method thereof
CN107093521A (en) * 2017-05-08 2017-08-25 华北电力大学(保定) A kind of Ce/C composites, its preparation method and its application
CN108447702A (en) * 2018-03-06 2018-08-24 常州大学 Preparation of a rGO-CeO2/PorousPANI ternary composite electrode material with high cycle life
CN115472445A (en) * 2022-09-29 2022-12-13 贵州民族大学 A kind of method that utilizes ceria to prepare supercapacitor electrode material

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1796990A (en) * 2004-12-20 2006-07-05 西北师范大学 Method for fabricating electrode of Nano ceric oxide selective membrane
CN1813323A (en) * 2003-04-28 2006-08-02 昭和电工株式会社 Valve acting metal sintered body, production method therefor and solid electrolytic capacitor
CN101076913A (en) * 2004-01-12 2007-11-21 燃料电池能有限公司 Fused carbonate fuel battery cathode with mixed oxide coatings
CN101383418A (en) * 2007-08-31 2009-03-11 丹麦技术大学 Electrodes based on ceria and stainless steel
CN102299311A (en) * 2011-07-20 2011-12-28 彩虹集团公司 Cathode active material and preparation method thereof and lithium ion secondary battery prepared by cathode active material

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1813323A (en) * 2003-04-28 2006-08-02 昭和电工株式会社 Valve acting metal sintered body, production method therefor and solid electrolytic capacitor
CN101076913A (en) * 2004-01-12 2007-11-21 燃料电池能有限公司 Fused carbonate fuel battery cathode with mixed oxide coatings
CN1796990A (en) * 2004-12-20 2006-07-05 西北师范大学 Method for fabricating electrode of Nano ceric oxide selective membrane
CN101383418A (en) * 2007-08-31 2009-03-11 丹麦技术大学 Electrodes based on ceria and stainless steel
CN102299311A (en) * 2011-07-20 2011-12-28 彩虹集团公司 Cathode active material and preparation method thereof and lithium ion secondary battery prepared by cathode active material

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN105116036A (en) * 2015-08-13 2015-12-02 东北大学 Preparation and usage method for cerium (IV) ion selectivity electrodes
CN106531454A (en) * 2016-12-29 2017-03-22 铜陵市胜美达电子制造有限公司 Ageing-resistant cobaltosic oxide nanowire carbon aerogel composite supercapacitor positive electrode material and preparation method thereof
CN107093521A (en) * 2017-05-08 2017-08-25 华北电力大学(保定) A kind of Ce/C composites, its preparation method and its application
CN108447702A (en) * 2018-03-06 2018-08-24 常州大学 Preparation of a rGO-CeO2/PorousPANI ternary composite electrode material with high cycle life
CN115472445A (en) * 2022-09-29 2022-12-13 贵州民族大学 A kind of method that utilizes ceria to prepare supercapacitor electrode material
CN115472445B (en) * 2022-09-29 2024-03-29 贵州民族大学 A method for preparing supercapacitor electrode materials using cerium dioxide

Similar Documents

Publication Publication Date Title
Wu et al. Fe3O4-based core/shell nanocomposites for high-performance electrochemical supercapacitors
CN103295798B (en) A kind of porous complex carbon material and application thereof
Chen et al. Facilely synthesized porous NiCo2O4 flowerlike nanostructure for high-rate supercapacitors
Han et al. High energy density sodium-ion capacitors through co-intercalation mechanism in diglyme-based electrolyte system
JP2014501028A (en) Composite electrode material, manufacturing method thereof, and application
EP3913706A1 (en) Pre-lithiated negative electrode and preparation method therefor, and lithium ion battery and supercapacitor having pre-lithiated negative electrode
CN101546651A (en) Nano graphite sheet/manganese dioxide doped composite material and preparation method thereof
Shi et al. 3D mesoporous hemp-activated carbon/Ni3S2 in preparation of a binder-free Ni foam for a high performance all-solid-state asymmetric supercapacitor
CN106024408B (en) A kind of ruthenium-oxide-vulcanization carbon/carbon-copper composite material, using and a kind of electrode slice of ultracapacitor
CN108597891B (en) Silica @ metal oxide/graphene aerogel dual-load dual-coating composite material and preparation method and application thereof
CN101060038A (en) Expanded graphite/metal oxide composite material and preparation method thereof
CN105513829A (en) Carbon nanotube/carbon fiber composite material and carbon-base/manganese oxide composite electrode material
CN111883366A (en) A kind of polypyrrole nanosphere@titanium carbide composite material and its preparation method and application
CN103280339A (en) Method for preparing cerium oxide electrode of supercapacitor
CN106206051B (en) A kind of graphene modified activated carbon and its application
CN105244474A (en) High-specific capacity lithium-sulfur secondary battery composite cathode and preparation method thereof
CN103839695A (en) Graphene electrode plate, and preparation method and application thereof
Liu et al. Hexadecyl trimethyl ammonium bromide assisted growth of NiCo 2 O 4@ reduced graphene oxide/nickel foam nanoneedle arrays with enhanced performance for supercapacitor electrodes
CN114408919A (en) Coconut shell material-based porous carbon material subjected to high-temperature thermal shock carbonization and KOH activation, and preparation method and application thereof
CN116666641A (en) Multi-element nano carbon conductive precoat modified current collector and preparation method and application thereof
CN107910201A (en) A kind of preparation method of laminar composite
CN102856080B (en) A kind of super capacitor material based on nano porous metal conducting polymer and preparation method thereof
CN110491684B (en) Acicular flower cobalt-nickel double metal hydroxide composite material and its preparation method and application
CN114171711B (en) Electrode preparation method of water-based zinc ion battery, electrode and battery
CN105513835B (en) A kind of preparation method and application of nickel hydroxide/graphene flexible electrode material

Legal Events

Date Code Title Description
C06 Publication
PB01 Publication
C10 Entry into substantive examination
SE01 Entry into force of request for substantive examination
C02 Deemed withdrawal of patent application after publication (patent law 2001)
WD01 Invention patent application deemed withdrawn after publication

Application publication date: 20130904