EP3081671B1 - Scandium concentrate production method - Google Patents

Scandium concentrate production method Download PDF

Info

Publication number
EP3081671B1
EP3081671B1 EP15740883.2A EP15740883A EP3081671B1 EP 3081671 B1 EP3081671 B1 EP 3081671B1 EP 15740883 A EP15740883 A EP 15740883A EP 3081671 B1 EP3081671 B1 EP 3081671B1
Authority
EP
European Patent Office
Prior art keywords
scandium
aluminum
electrolysis
potential
alloy
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.)
Not-in-force
Application number
EP15740883.2A
Other languages
German (de)
English (en)
French (fr)
Other versions
EP3081671A1 (en
EP3081671A4 (en
Inventor
Jun-Ichi Takahashi
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.)
Sumitomo Metal Mining Co Ltd
Original Assignee
Sumitomo Metal Mining Co Ltd
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 Sumitomo Metal Mining Co Ltd filed Critical Sumitomo Metal Mining Co Ltd
Publication of EP3081671A1 publication Critical patent/EP3081671A1/en
Publication of EP3081671A4 publication Critical patent/EP3081671A4/en
Application granted granted Critical
Publication of EP3081671B1 publication Critical patent/EP3081671B1/en
Not-in-force legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Images

Classifications

    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C21/00Alloys based on aluminium
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B59/00Obtaining rare earth metals
    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25CPROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C3/00Electrolytic production, recovery or refining of metals by electrolysis of melts
    • C25C3/06Electrolytic production, recovery or refining of metals by electrolysis of melts of aluminium
    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25CPROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C3/00Electrolytic production, recovery or refining of metals by electrolysis of melts
    • C25C3/34Electrolytic production, recovery or refining of metals by electrolysis of melts of metals not provided for in groups C25C3/02 - C25C3/32

Definitions

  • the present invention relates to a scandium concentrate production method, and in more detail, relates to a method of reusing an alloy containing scandium and aluminum as aluminum and scandium concentrates.
  • Aluminum scandium alloys containing aluminum and scandium have a characteristic of being light weight and high strength, and in addition to sports articles, have been used in fields requiring shock resistance. Additionally, in the future, applications as a structural material for aircraft, electric vehicles, high-speed rail, etc. are also expected. However, since the production volume of scandium is very small, scandium is extremely high cost. For this reason, it is not easy to broadly apply scandium industrially.
  • Patent Document 1 Japanese Unexamined Patent Application, Publication No. 2003-171724
  • the scandium quality of these disposed articles, etc. is far higher than the scandium quality of nickel oxide ores, etc., and recovering scandium from the disposed articles, etc. and reusing is expected to be an effective means.
  • an element contained in Al-Sc alloy is aluminum, and the content of scandium is a very small amount comparing with the content of aluminum; therefore, it is not possible to effectively recover scandium concentrate by simply melting Al-Sc alloy.
  • the present invention has been made in order to solve the above such problems, and the object thereof is to effectively recover scandium concentrate from Al-Sc alloy.
  • the Al-Sc alloy in structures, etc. is widely used by concentrating to 0.1 to 1% Sc.
  • the Sc concentration of the Al-Sc master alloy is 1 to 2%.
  • the present invention has an object of efficiently recovering scandium concentration of a degree that can be used as is as an Al-Sc master alloy from scrap articles of Al-Sc alloy having a Sc concentration on the order of 0.1 to 1%.
  • the present inventors found that the above-mentioned object could be achieved by bringing chlorine into contact with an alloy containing aluminum and scandium, and melting, followed by subjecting the molten mixture to electrolysis at predetermined conditions, thereby arriving at completion of the present invention.
  • the present invention provides the following matters.
  • a first aspect of the present invention is a scandium concentrate production method, including: a molted mixture generation step of generating a molten mixture of aluminum chloride and scandium chloride by bringing chlorine into contact with an alloy containing aluminum and scandium, and melting; a first electrolysis step of subjecting the molten mixture to first electrolysis at a potential between the metalation potential of aluminum and the metalation potential of scandium to generate molten aluminum; and a second electrolysis step of subjecting the molten mixture, after the molten aluminum generation step, to second electrolysis at a potential capable of recovering scandium to generate a scandium concentrate.
  • the molten mixture generation step is a step of melting the alloy brought into contact with the chlorine into a melt of a chloride-based salt or eutectic salt having a melting point or eutectic temperature higher than 500°C.
  • This scandium concentrate can be used as is as a high-quality Al-Sc master alloy.
  • FIG. 1 is a schematic view showing a scandium concentrate production method according to the present invention.
  • the present method includes: a molten mixture generation step S1 of generating a molten mixture of aluminum chloride and scandium chloride by bringing chlorine into contact with an alloy containing aluminum and scandium and melting; a first electrolysis step of subjecting the molten mixture to first electrolysis at a potential between the metalation potential of aluminum and the metalation potential of scandium; and a second electrolysis step of subjecting the molten mixture, after the molten aluminum generation step S2, to second electrolysis at a potential capable of recovering scandium to generate a scandium concentrate.
  • the molten mixture generation step S1 brings chlorine gas into contact with an Al-Sc alloy serving as a raw material (disposed articles, manufacturing defect articles, etc.), to obtain a mixture of aluminum chloride and scandium chloride.
  • the contact temperature with chlorine gas is not particularly limited.
  • the present invention uses a molten salt electrolysis method to melt an ionic solid by bringing to high temperature, and then electrolyzing this.
  • the molten salt In the view of the melting point of aluminum being 660.5°C, and heating the molten salt to a temperature higher than this melting point, it is necessary for the molten salt to have a melting point or eutectic temperature higher than 500°C.
  • the vapor pressure of the chloride increases by the activity of the salt rising accompanying an increase in temperature, when the melting point or eutectic temperature is remarkably low compared to the melting point of aluminum, due to heating up to a temperature higher than the melting point of aluminum upon electrolysis, and thus the volatilization of salt will occur.
  • the salt composition gradually changes by way of this volatilization, and the electrolytic voltage continually changes accompanying this; therefore, it is difficult to appropriately control electrolysis. For this reason, it is not preferable to use a molten salt having a melting point or eutectic temperature that is remarkably low compared to the melting point of aluminum.
  • the eutectic temperature of the LiCl-KCl eutectic salt is 350°C, and it is not preferable because the eutectic temperature is remarkably low compared to the melting point of aluminum.
  • molten salt having a melting point or eutectic temperature close to the melting point of aluminum, in the point of not requiring to heat more than necessary upon electrolysis.
  • the molten salt requires there to be a difference of at least 0.8 V between the metalation potential of aluminum and the metalation potential of scandium.
  • the electrolytic potentials of elements differ according to the type and composition of molten salt. Due to aluminum and scandium coexisting, the present invention configures so that only aluminum is generated in the first electrolysis, and scandium is first generated in the second electrolysis; therefore, the molten salt requires to have at least a certain difference between the metalation potential of aluminum and the metalation potential of scandium. A greater difference is preferable, it is more preferably at least 1.0 V, and even more preferably at least 1.2 V.
  • the metalation potential of Al 3+ is -1.04 V
  • the metalation potential of Sc 3+ is -1.83 V.
  • the difference between the two is about 0.8 V, and thus is sufficient to suppress both aluminum and scandium generating in the first electrolysis.
  • detailed data for the metalation potential is not known, even if the type of metal element constituting the salt differs, a great difference in the metalation potentials will not arise so long as being chloride-based salts.
  • the heating temperature of the molten salt is sufficient so long as an extent able to sufficiently melt the Al-Sc alloy.
  • the liquidus temperature of the Al-Sc alloy will differ according to the scandium concentration contained in the Al-Sc alloy.
  • the liquidus temperature of the Al-Sc alloy is determined by referencing a published phase diagram of Al-Sc alloy. For example, in the case of the scandium concentration being on the order of 0.2 to 0.4%, the liquidus temperature of the Al-Sc alloy is on the order of 660°C, which is the eutectic temperature.
  • the liquidus temperature rises as the scandium concentration contained in the Al-Sc alloy increases, and the liquidus temperature in the case of the scandium concentration being 1% is about 730°C, and the liquidus temperature in the case of being 2% exceeds 800°C.
  • the above-mentioned mixture i.e. mixture of aluminum chloride and scandium chloride
  • the first electrolysis step S2 subjects the molten mixture obtained in the molten mixture generation step S1 to the first electrolysis at a potential between the metalation potential of aluminum and the metalation potential of scandium to generate molten aluminum.
  • the type of electrode is not particularly limited, for example, establishing silver as the reference electrode, graphite as the anode, and nickel as the cathode can be exemplified.
  • the potential in the first electrolysis is required to be between the metalation potential of aluminum and the metalation potential of scandium, and in more detail, no more than the metalation potential of aluminum and at least the metalation potential of scandium. If not in this range, it is not preferable because not only molten aluminum, but also scandium can also generate at the cathode.
  • the potential in the first electrolysis is preferably closer to the metalation potential of aluminum, and specifically, is preferably within the range of -1.50 V to -1.04 V, and is more preferably within the range of -1.30 V to -1.10 V.
  • the temperature of the molten salt is not particularly limited so long as higher than the melting point of aluminum.
  • the first electrolysis it is preferable to store the aluminum in a storage container along with molten salt in advance.
  • the interior of the storage container is heated up to a temperature higher than the melting point of aluminum; therefore, the stored aluminum is used as an aluminum electrode (cathode) through the above-mentioned nickel.
  • new aluminum produced in the electrolysis of the Al-Sc alloy melts into the aluminum that had already melted. As a result thereof, the concentration of scandium contained in the molten salt rises.
  • the second electrolysis step S3 subjects the molten mixture to the second electrolysis at a potential capable of recovering scandium, after the molten aluminum generation step S2. By doing this, the liquid scandium dissolves in the liquid aluminum obtained in the first electrolysis, and a scandium concentrate is generated.
  • the type of electrode is not particularly limited, and the same one as the electrode used in the first electrolysis can be used.
  • the potential in the second electrolysis is required to be capable of recovering scandium, and be no more than the metalation potential of scandium. If not in this range, it is not preferable because liquid scandium will not dissolve in the liquid aluminum obtained in the first electrolysis at the cathode.
  • the potential in the second electrolysis is sufficient so long as no more than -1.83 V, when considering the stability of the operation, it is preferably no more than -2.0 V.
  • the amount of aluminum stored in advance inside the storage container can be arbitrarily set according to the target scandium quality for the scandium concentrate.
  • the temperature of the molten salt is not particularly limited so long as higher than the temperature of the liquidus of the Al-Sc alloy contained in the molten salt; however, based on the stability of the operation, etc., it is preferably at least 5°C higher than the temperature of the liquidus of the Al-Sc alloy, and more preferably at least 10°C higher.
  • the scandium concentrate of the present invention may be reused as is as a high-grade Al-Sc master alloy, or may be reused after remelting and making into a master alloy.
  • by recovering scandium from a scandium concentrate by a known method such as solvent extraction it is possible to very efficiently recover scandium compared to a case of recovering from nickel oxide ore.
  • FIG. 2 is a schematic view illustrating the configuration of the electrolysis apparatus 1 used in the present Examples.
  • the electrolysis apparatus 1 includes: a quartz container 2 that encloses the Al-Sc alloy along with molten salt; a quartz tube 3 with one side open, and accommodating the quartz container 2 from this opening; a rubber stopper 4 that seals this quartz tube 3; a reference electrode (silver) 5, anode (graphite) 6 and cathode (nickel) 7 inserted inside of the quartz container 2; a gas substitution unit 8 that substitutes the inside of the quartz tube 3 with argon gas; a thermocouple 9 that is inserted inside of the quartz container 2; an electric furnace 10 that keeps the temperature inside of the quartz tube 3 at a predetermined temperature; and an insulation board 11 that keeps the adiabaticity of the inside of the quartz tube 3.
  • the reference electrode (silver) 5, the anode (graphite) 6 and the cathode (nickel) 7 were immersed to the positions shown in FIG. 2 , and the first electrolysis was performed while holding at the potential of -1.25 V for the potential of the Ag + /Ag reference electrode 5.
  • Aluminum was thereby recovered from the bottom of the quartz container 2 through the cathode 7.
  • the inside of the quartz tube 3 was heated to 880°C, and the second electrolysis was performed.
  • the inside of the quartz tube 3 was cooled to room temperature. Then, the salt 12 (mixture of aluminum and NaCl-KCl eutectic salt) and scandium concentrate 13 that solidified from cooling were retrieved.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Mechanical Engineering (AREA)
  • Electrochemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Environmental & Geological Engineering (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Geology (AREA)
  • Manufacturing & Machinery (AREA)
  • Electrolytic Production Of Metals (AREA)
  • Manufacture And Refinement Of Metals (AREA)
EP15740883.2A 2014-01-27 2015-01-23 Scandium concentrate production method Not-in-force EP3081671B1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2014012667A JP5907188B2 (ja) 2014-01-27 2014-01-27 スカンジウム濃縮物の製造方法
PCT/JP2015/051828 WO2015111698A1 (ja) 2014-01-27 2015-01-23 スカンジウム濃縮物の製造方法

Publications (3)

Publication Number Publication Date
EP3081671A1 EP3081671A1 (en) 2016-10-19
EP3081671A4 EP3081671A4 (en) 2016-12-21
EP3081671B1 true EP3081671B1 (en) 2017-08-02

Family

ID=53681495

Family Applications (1)

Application Number Title Priority Date Filing Date
EP15740883.2A Not-in-force EP3081671B1 (en) 2014-01-27 2015-01-23 Scandium concentrate production method

Country Status (3)

Country Link
EP (1) EP3081671B1 (ja)
JP (1) JP5907188B2 (ja)
WO (1) WO2015111698A1 (ja)

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
TR201704220A2 (tr) * 2017-03-21 2018-03-21 Minertek Mineral Teknolojileri Madencilik Sanayi Ve Ticaret Anonim Sirketi (NH4)2NaScF6 formundaki skandiyum bileşiğinden elde edilen ScF3 bileşiğine, CaCl2 ve/veya MgCl2 bileşiklerinin ilavesiyle oluşturulan, skandiyum tuz karışımlarından elektroliz yöntemi vasıtasıyla skandiyum metali ve Al-Sc alaşımlarının üretim metodu
CN107630234B (zh) * 2017-09-18 2019-09-17 江西理工大学 一种利用氯盐氧化物体系熔盐电解制备铝钪中间合金的方法
JP7361058B2 (ja) * 2018-03-15 2023-10-13 エフイーエー マテリアルズ エルエルシー アルミニウム-スカンジウム合金の製造方法
CN115011805A (zh) * 2022-01-19 2022-09-06 昆明理工大学 一种从冶炼渣中回收钪和铝的方法

Family Cites Families (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2874039A (en) * 1954-06-17 1959-02-17 Pechiney Prod Chimiques Sa Extraction of scandium from its ores
US6808695B1 (en) * 2000-05-22 2004-10-26 Toth Aluminum Corporation Process for continuously producing aluminum from clays
JP4224532B2 (ja) 2001-12-07 2009-02-18 青森県 Al−Sc母合金の製造法およびその方法によって得られたAl−Sc母合金
JP5094031B2 (ja) * 2006-03-23 2012-12-12 大平洋金属株式会社 スカンジウム含有合金の製造方法
JP5472897B2 (ja) * 2008-12-09 2014-04-16 株式会社東芝 画像処理装置
JP2012136766A (ja) * 2010-12-28 2012-07-19 Kyoto Univ 電気分解による金属の製造方法

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
None *

Also Published As

Publication number Publication date
EP3081671A1 (en) 2016-10-19
JP2015140446A (ja) 2015-08-03
JP5907188B2 (ja) 2016-04-26
EP3081671A4 (en) 2016-12-21
WO2015111698A1 (ja) 2015-07-30

Similar Documents

Publication Publication Date Title
EP3081671B1 (en) Scandium concentrate production method
KR102289555B1 (ko) 전해 환원에 의한 금속의 생성방법 및 장치
JP5504515B2 (ja) 希土類金属の回収方法
Fray et al. Aspects of the application of electrochemistry to the extraction of titanium and its applications
Kong et al. Electrochemical deoxidation of titanium scrap in MgCl2-HoCl3 system
JP5445725B1 (ja) Al−Sc合金の製造方法
RU2463387C2 (ru) Получение вольфрама и вольфрамовых сплавов из соединений, содержащих вольфрам, электрохимическим способом
EP3081670B1 (en) Scandium concentrate production method
CN106868550A (zh) 一种熔融盐中电解废钛制备高纯钛的方法
Abbasalizadeh et al. Rare earth extraction from NdFeB magnets and rare earth oxides using aluminum chloride/fluoride molten salts
Lee et al. Thermodynamics of fluoride-based molten fluxes for extraction of magnesium through the low temperature solid oxide membrane (LT-SOM) process
US20230392273A1 (en) Method for manufacturing recycled aluminum, manufacturing equipment, manufacturing system, recycled aluminum, and processed aluminum product
EP3078757B1 (en) Scandium chloride and scandium chloride production method
Selivanov et al. The effect of the nickel sulphide alloys structure on their electrochemical oxidation parameters
EP3081659B1 (en) Scandium concentrate recovery method
Natsui et al. Molten Oxide Electrolysis Using Copper-Containing Carbon-Saturated Molten Iron Anode
JP6234160B2 (ja) 希土類金属の製造方法
Haarberg et al. Electrodeposition of Lead from Chloride Melts
JP2012162764A (ja) 希土類元素の回収方法及び回収システム
Abbasalizadeh et al. Novel reactive anode for electrochemical extraction of rare earth metals from rare earth oxides
Kuznetsov Anodic Processes during the Electrowinning of Niobium from Chloride-Fluoride Melts and the Influence of Oxide Ions on Them
Kamimura et al. Thermodynamic Effect of NaCl and KCl Addition on the Equilibrium Between Molten ZnCl 2-Based Salt and Liquid Zn–Cd Alloy
Qin et al. Direct electroreduction of indium and tin oxides in molten salts
Sokhanvaran et al. Advances in Electrometallurgy for Sustainable Metal Production
Kuznetsov et al. Oxygen species in a niobium-containing fluoride melt.

Legal Events

Date Code Title Description
PUAI Public reference made under article 153(3) epc to a published international application that has entered the european phase

Free format text: ORIGINAL CODE: 0009012

17P Request for examination filed

Effective date: 20160711

AK Designated contracting states

Kind code of ref document: A1

Designated state(s): AL AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HR HU IE IS IT LI LT LU LV MC MK MT NL NO PL PT RO RS SE SI SK SM TR

AX Request for extension of the european patent

Extension state: BA ME

RIN1 Information on inventor provided before grant (corrected)

Inventor name: TAKAHASHI, JUN-ICHI

A4 Supplementary search report drawn up and despatched

Effective date: 20161123

RIC1 Information provided on ipc code assigned before grant

Ipc: C25C 3/34 20060101ALI20161117BHEP

Ipc: C22C 21/00 20060101ALI20161117BHEP

Ipc: C22B 59/00 20060101AFI20161117BHEP

Ipc: C25C 3/06 20060101ALI20161117BHEP

REG Reference to a national code

Ref country code: DE

Ref legal event code: R079

Ref document number: 602015003909

Country of ref document: DE

Free format text: PREVIOUS MAIN CLASS: C25C0003360000

Ipc: C22B0059000000

GRAP Despatch of communication of intention to grant a patent

Free format text: ORIGINAL CODE: EPIDOSNIGR1

STAA Information on the status of an ep patent application or granted ep patent

Free format text: STATUS: GRANT OF PATENT IS INTENDED

RIC1 Information provided on ipc code assigned before grant

Ipc: C25C 3/06 20060101ALI20170217BHEP

Ipc: C22B 59/00 20060101AFI20170217BHEP

Ipc: C22C 21/00 20060101ALI20170217BHEP

Ipc: C25C 3/34 20060101ALI20170217BHEP

INTG Intention to grant announced

Effective date: 20170314

DAX Request for extension of the european patent (deleted)
GRAS Grant fee paid

Free format text: ORIGINAL CODE: EPIDOSNIGR3

GRAA (expected) grant

Free format text: ORIGINAL CODE: 0009210

STAA Information on the status of an ep patent application or granted ep patent

Free format text: STATUS: THE PATENT HAS BEEN GRANTED

AK Designated contracting states

Kind code of ref document: B1

Designated state(s): AL AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HR HU IE IS IT LI LT LU LV MC MK MT NL NO PL PT RO RS SE SI SK SM TR

REG Reference to a national code

Ref country code: CH

Ref legal event code: EP

Ref country code: AT

Ref legal event code: REF

Ref document number: 914560

Country of ref document: AT

Kind code of ref document: T

Effective date: 20170815

REG Reference to a national code

Ref country code: IE

Ref legal event code: FG4D

REG Reference to a national code

Ref country code: DE

Ref legal event code: R096

Ref document number: 602015003909

Country of ref document: DE

REG Reference to a national code

Ref country code: NL

Ref legal event code: MP

Effective date: 20170802

REG Reference to a national code

Ref country code: AT

Ref legal event code: MK05

Ref document number: 914560

Country of ref document: AT

Kind code of ref document: T

Effective date: 20170802

REG Reference to a national code

Ref country code: LT

Ref legal event code: MG4D

REG Reference to a national code

Ref country code: FR

Ref legal event code: PLFP

Year of fee payment: 4

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: HR

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: FI

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: NO

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20171102

Ref country code: AT

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: NL

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: LT

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: SE

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: PL

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: LV

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: RS

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: GR

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20171103

Ref country code: ES

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: IS

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20171202

Ref country code: BG

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20171102

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: DK

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: CZ

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

REG Reference to a national code

Ref country code: DE

Ref legal event code: R097

Ref document number: 602015003909

Country of ref document: DE

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: IT

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: SM

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: EE

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: SK

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

PLBE No opposition filed within time limit

Free format text: ORIGINAL CODE: 0009261

STAA Information on the status of an ep patent application or granted ep patent

Free format text: STATUS: NO OPPOSITION FILED WITHIN TIME LIMIT

26N No opposition filed

Effective date: 20180503

REG Reference to a national code

Ref country code: DE

Ref legal event code: R119

Ref document number: 602015003909

Country of ref document: DE

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: SI

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

REG Reference to a national code

Ref country code: CH

Ref legal event code: PL

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: DE

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20180801

Ref country code: LU

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20180123

REG Reference to a national code

Ref country code: IE

Ref legal event code: MM4A

REG Reference to a national code

Ref country code: BE

Ref legal event code: MM

Effective date: 20180131

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: LI

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20180131

Ref country code: CH

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20180131

Ref country code: BE

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20180131

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: IE

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20180123

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: MC

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: MT

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20180123

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: TR

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: PT

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: RO

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: MK

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20170802

Ref country code: CY

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

Ref country code: HU

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT; INVALID AB INITIO

Effective date: 20150123

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: AL

Free format text: LAPSE BECAUSE OF FAILURE TO SUBMIT A TRANSLATION OF THE DESCRIPTION OR TO PAY THE FEE WITHIN THE PRESCRIBED TIME-LIMIT

Effective date: 20170802

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: GB

Payment date: 20211206

Year of fee payment: 8

Ref country code: FR

Payment date: 20211217

Year of fee payment: 8

GBPC Gb: european patent ceased through non-payment of renewal fee

Effective date: 20230123

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: GB

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20230123

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: FR

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20230131