EP1892728A1 - Process of producing the radioisotope TL-201 - Google Patents

Process of producing the radioisotope TL-201 Download PDF

Info

Publication number
EP1892728A1
EP1892728A1 EP06119491A EP06119491A EP1892728A1 EP 1892728 A1 EP1892728 A1 EP 1892728A1 EP 06119491 A EP06119491 A EP 06119491A EP 06119491 A EP06119491 A EP 06119491A EP 1892728 A1 EP1892728 A1 EP 1892728A1
Authority
EP
European Patent Office
Prior art keywords
liquid
target material
solution
ion exchange
solid target
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.)
Granted
Application number
EP06119491A
Other languages
German (de)
French (fr)
Other versions
EP1892728B1 (en
EP1892728B9 (en
Inventor
Wuu-Jyh Lin
Ting-Shien Duh
Ying-Ming c/o Atomic En. Council-Inst. of Nucl. Energy Tsai
Sun-Rong Huang
Chien-Hsin Lu
Mao-Hsung Chang
Jenn-Tzong Chen
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.)
Institute of Nuclear Energy Research
Original Assignee
Institute of Nuclear Energy Research
Atomic Energy Council
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 Institute of Nuclear Energy Research, Atomic Energy Council filed Critical Institute of Nuclear Energy Research
Priority to EP20060119491 priority Critical patent/EP1892728B9/en
Publication of EP1892728A1 publication Critical patent/EP1892728A1/en
Publication of EP1892728B1 publication Critical patent/EP1892728B1/en
Application granted granted Critical
Publication of EP1892728B9 publication Critical patent/EP1892728B9/en
Not-in-force legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Images

Classifications

    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/001—Recovery of specific isotopes from irradiated targets
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G4/00—Radioactive sources
    • G21G4/04—Radioactive sources other than neutron sources
    • G21G4/06—Radioactive sources other than neutron sources characterised by constructional features
    • G21G4/08—Radioactive sources other than neutron sources characterised by constructional features specially adapted for medical application
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/001—Recovery of specific isotopes from irradiated targets
    • G21G2001/0078—Thallium

Definitions

  • the present invention relates to producing T1-201; more particularly, it relates to quickly filtering out a high-purity T1-201 liquid.
  • T1-201 thallous chloride ( 201 TlCl 2 )can be absorbed by heart muscle to be gathered at the heart muscle. Therefore, T1-201 can be used in a myocardial image for diagnosing heart disease; and can be applied in other medical diagnoses, like a tumor image. Hence, T1-201 is the most commonly used radioisotope in division of nuclear medicine.
  • T1-201 is directly washed out. But the T1-201 directly washed out quite often contains impurities so that its purity is not good. Hence, the prior art does not fulfill users' requests on actual use.
  • the main purpose of the present invention is to form a T1-203 solid target material through electroplating, irradiate the T1-203 solid target material with a proton beam, dissolve the T1-203 solid target material to process through a first chemical separation and a second chemical separation, and quickly filter out a high-purity Tl-201 liquid.
  • the present invention is a radioisotope T1-201 production process, where a T1-203 solid target material is obtained from a plated target material of T1-203 through electroplating; the T1-203 solid target material is irradiated with a proton beam by using a cyclotron; the T1-203 solid target material is dissolved with a strong acid liquid to obtain a Pb-201 solution and a T1-203 solution; ammonia and water are added for a precipitation to separate a T1-201 liquid and a Pb-201 liquid out; hydrochloric acid is added for a first ion exchange with a resin while impurities are filtered out; the Pb-201 liquid is taken out to be decayed into a T1-201 liquid; and a hydrochloric acid (HC1) having sulfur dioxide (SO 2 ) is added to the T1-201 liquid to obtain a T1-201 liquid having a high purity through a second ion exchange by using a resin.
  • HC1 hydrochloric acid having sulfur dioxide (SO
  • FIG. 1 is a plot view showing a process flow of a preferred embodiment according to the present invention.
  • the present invention is a radioisotope T1-201 production process, comprising electroplating 1, irradiating 2, processing a first chemical separation 3, decaying 4 and processing a second chemical separation 5, where the first chemical separation 3 comprises dissolving 31, processing a precipitation 32 and processing a first ion exchange 33; and the second chemical separation 5 is a second ion exchange.
  • the first chemical separation 3 comprises dissolving 31, processing a precipitation 32 and processing a first ion exchange 33; and the second chemical separation 5 is a second ion exchange.
  • FIG.2 is a detailed view showing a flow chart of the preferred embodiment. As shown in the figure, when producing a radioisotope T1-201 according to the present invention, the following steps are processed:
  • the present invention is a radioisotope T1-201 production process, where a T1-203 solid target material is formed through an electroplating; the T1-203 solid target material is irradiated with a proton beam; the T1-203 solid target material is dissolved to be processed through a first chemical separation and a second chemical separation; and a T1-201 liquid is quickly filtered out, which has a high purity.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Medicines That Contain Protein Lipid Enzymes And Other Medicines (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Nuclear Medicine (AREA)

Abstract

The radioisotope T1-201 is produced. The process includes electroplating, irradiating, dissolving, precipitating, ion exchanging, decaying and filtering. The T1-201 obtained is a liquid having a high purity.

Description

    Field of the invention
  • The present invention relates to producing T1-201; more particularly, it relates to quickly filtering out a high-purity T1-201 liquid.
    • Description of the Related Art
  • T1-201 thallous chloride (201TlCl2)can be absorbed by heart muscle to be gathered at the heart muscle. Therefore, T1-201 can be used in a myocardial image for diagnosing heart disease; and can be applied in other medical diagnoses, like a tumor image. Hence, T1-201 is the most commonly used radioisotope in division of nuclear medicine.
  • To produce a T1-201, as revealed in "Production of T1-201 and Pb203 via Proton Induced Nuclear Reaction on Natural Thallium," by Qaim S. M., Weinreich R. and Ollig H., International Journal of Applied Radiation and Isotopes, 30 (1979) pp.85-95, T1-201 is directly washed out. But the T1-201 directly washed out quite often contains impurities so that its purity is not good. Hence, the prior art does not fulfill users' requests on actual use.
    • Summary of the invention
  • The main purpose of the present invention is to form a T1-203 solid target material through electroplating, irradiate the T1-203 solid target material with a proton beam, dissolve the T1-203 solid target material to process through a first chemical separation and a second chemical separation, and quickly filter out a high-purity Tl-201 liquid.
  • To achieve the above purpose, the present invention is a radioisotope T1-201 production process, where a T1-203 solid target material is obtained from a plated target material of T1-203 through electroplating; the T1-203 solid target material is irradiated with a proton beam by using a cyclotron; the T1-203 solid target material is dissolved with a strong acid liquid to obtain a Pb-201 solution and a T1-203 solution; ammonia and water are added for a precipitation to separate a T1-201 liquid and a Pb-201 liquid out; hydrochloric acid is added for a first ion exchange with a resin while impurities are filtered out; the Pb-201 liquid is taken out to be decayed into a T1-201 liquid; and a hydrochloric acid (HC1) having sulfur dioxide (SO2) is added to the T1-201 liquid to obtain a T1-201 liquid having a high purity through a second ion exchange by using a resin. Accordingly, a novel radioisotope T1-201 production process is obtained.
    • Brief description of the drawing
  • The present invention will be better understood from the following detailed description of the preferred embodiment according to the present invention, taken in conjunction with the accompanying drawings, in which
    • FIG.1
    is the plot view showing the process flow of the preferred embodiment according to the present invention; and
    FIG.2
    is the detailed view showing the flow chart of the preferred embodiment.
    Description of a preferred embodiment
  • The following description of the preferred embodiment is provided to understand the features and the structures of the present invention.
  • FIG. 1 is a plot view showing a process flow of a preferred embodiment according to the present invention. As shown in the figure, the present invention is a radioisotope T1-201 production process, comprising electroplating 1, irradiating 2, processing a first chemical separation 3, decaying 4 and processing a second chemical separation 5, where the first chemical separation 3 comprises dissolving 31, processing a precipitation 32 and processing a first ion exchange 33; and the second chemical separation 5 is a second ion exchange. Thus, a novel radioisotope T1-201 production process is obtained for acquiring a T1-201 liquid having a high purity.
  • FIG.2 is a detailed view showing a flow chart of the preferred embodiment. As shown in the figure, when producing a radioisotope T1-201 according to the present invention, the following steps are processed:
    1. (a) Electroplating 1: A T1-203 solid target material 12 is obtained from a plated target material 11 of T1-203 through electroplating.
    2. (b) Irradiating 2: The T1-203 solid target material 12 is irradiated with a proton beam by using a cyclotron 21, where an irradiation energy of the cyclotron 21 is located between fifteen mega electron volts (MeV) and forty MeV.
    3. (c) Processing a first chemical separation: The first chemical separation 3 comprises the following steps:
      • (c1) Dissolving 31: After the irradiating, the T1-203 solid target material 12 is dissolved with a strong acid liquid 34 to obtain a Pb-201 solution 35 and a Tl-203 solution 36, where the strong acid liquid 34 is a solution of nitric acid having ferric iron (HNO3/Fe3/H2O).
      • (c2) Processing a precipitation 32: Ammonia (NH3) and water 321 are added to the Pb-201 solution 35 and the Tl-203 solution 36 for a precipitation to separate out a T1-201 liquid 37 and a Pb-201 liquid 38; and
      • (c3) Processing a first ion exchange 33: Hydrochloric acid (HCl) 331 is added to the Tl-201 liquid 37 and the Pb-201 liquid 38 for a first ion exchange by using a resin 332 with impurities filtered out;
    4. (d) Decaying 4: The Pb-201 liquid is taken out to be decayed into a T1-201 liquid 41.
    5. (e) Processing a second chemical separation: And a second chemical separation 5 is processed, which is a second ion exchange 51.
      • (e1) Processing a second ion exchange 51: An HCl acid having sulfur dioxide (SO2) 511 is added to the T1-201 liquid 41 to obtain a T1-201 liquid 52 having a high purity through a second ion exchange by using a resin 512.
  • Thus, a novel radioisotope T1-201 production process is obtained.
  • To sum up, the present invention is a radioisotope T1-201 production process, where a T1-203 solid target material is formed through an electroplating; the T1-203 solid target material is irradiated with a proton beam; the T1-203 solid target material is dissolved to be processed through a first chemical separation and a second chemical separation; and a T1-201 liquid is quickly filtered out, which has a high purity.
  • The preferred embodiment herein disclosed is not intended to unnecessarily limit the scope of the invention. Therefore, simple modifications or variations belonging to the equivalent of the scope of the claims and the instructions disclosed herein for a patent are all within the scope of the present invention.

Claims (8)

  1. Process of producing the radioisotope Tl-201, comprising steps of:
    (a) Electroplating: wherein a Tl-203 solid target material is obtained from a plated target material of Tl-203 through electroplating;
    (b) Irradiating: wherein said Tl-203 solid target material is irradiated with a proton beam by using a cyclotron;
    (c) Processing a first chemical separation: wherein said T1-203 solid target material is dissolved with a strong acid liquid to be separated into a T1-201 liquid and a Pb-201 liquid with impurities filtered out;
    (d) Decaying: wherein said Pb-201 liquid is obtained to be decayed into a Tl-201 liquid; and
    (e) Processing a second chemical separation: wherein a T1-201 liquid having a high purity is obtained through filtering.
  2. The process according to claim 1, wherein an irradiation energy of said cyclotron in step (b) is located between 15 mega electron volts (MeV) and 40 MeV.
  3. The process according to claim 1, wherein said step (c) comprises steps of:
    (c1) Dissolving: wherein, after said irradiating, said Tl-203 solid target material is dissolved with a strong acid liquid to obtain a Pb-201 solution and a Tl-203 solution;
    (c2) Processing a precipitation: wherein ammonia (NH3) and water are applied to said Pb-201 solution and said T1-203 solution for a precipitation to obtain a Tl-201 liquid and a Pb-201 liquid; and
    (c3) Processing a first ion exchange: wherein hydrochloric acid (HC1) is applied to said T1-201 liquid and said Pb-201 liquid for an ion exchange by using a resin with impurities filtered out.
  4. The process according to claim 3, wherein said strong acid liquid used in step (c1) is a solution of nitric acid having ferric iron (HNO3/Fe3/H2O).
  5. The process according to claim 1,
    wherein step (e) is a second ion exchange; and
    wherein an HC1 having sulfur dioxide (SO2) is applied to said T1-201 liquid to obtain a T1-201 liquid having a high purity through a second ion exchange by using a resin.
  6. Process of producing the radioisotope T1-201, comprising steps of:
    (a) Electroplating: wherein a T1-203 solid target material is obtained from a plated target material of T1-203 through electroplating;
    (b) Irradiating: wherein said T1-203 solid target material is irradiated with a proton beam by using a cyclotron;
    (c1) Dissolving: wherein, after said irradiating, said T1-203 solid target material is dissolved with a strong acid liquid to obtain a Pb-201 solution and a Tl-203 solution;
    (c2) Processing a precipitation: wherein NH3 and water are applied to said Pb-201 solution and said T1-203 solution for a precipitation to obtain a T1-201 liquid and a Pb-201 liquid;
    (c3) Processing a first ion exchange: wherein HCl is applied to said T1-201 liquid and said Pb-201 liquid for an ion exchange by using a resin with impurities filtered out;
    (d) Decaying: wherein said Pb-201 liquid is obtained to be decayed into a Tl-201 liquid; and
    (e1) Processes a second ion exchange: wherein an HCl having SO2 is applied to said T1-201 liquid to obtain a T1-201 liquid having a high purity through an second ion exchange by using a resin.
  7. The process according to claim 6, wherein an irradiation energy of said cyclotron in step (b) is located between 15MeV and 40 MeV.
  8. The process according to claim 6, wherein said strong acid liquid used in step (c1) is HNO3/Fe3/H2O.
EP20060119491 2006-08-24 2006-08-24 Process of producing the radioisotope Tl-201 Not-in-force EP1892728B9 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP20060119491 EP1892728B9 (en) 2006-08-24 2006-08-24 Process of producing the radioisotope Tl-201

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
EP20060119491 EP1892728B9 (en) 2006-08-24 2006-08-24 Process of producing the radioisotope Tl-201

Publications (3)

Publication Number Publication Date
EP1892728A1 true EP1892728A1 (en) 2008-02-27
EP1892728B1 EP1892728B1 (en) 2013-12-04
EP1892728B9 EP1892728B9 (en) 2014-04-09

Family

ID=37607072

Family Applications (1)

Application Number Title Priority Date Filing Date
EP20060119491 Not-in-force EP1892728B9 (en) 2006-08-24 2006-08-24 Process of producing the radioisotope Tl-201

Country Status (1)

Country Link
EP (1) EP1892728B9 (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1916669B1 (en) * 2006-10-25 2014-12-24 Atomic Energy Council - Institute of Nuclear Energy Research Separation Device for Radioisotope Tl-201

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3993538A (en) 1976-01-27 1976-11-23 The United States Of America As Represented By The United States Energy Research And Development Administration Production of high purity radiothallium
US4297166A (en) 1978-02-20 1981-10-27 Nihon Medi-Physics, Co., Ltd. Thallium-carrying target material and its production

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3993538A (en) 1976-01-27 1976-11-23 The United States Of America As Represented By The United States Energy Research And Development Administration Production of high purity radiothallium
US4297166A (en) 1978-02-20 1981-10-27 Nihon Medi-Physics, Co., Ltd. Thallium-carrying target material and its production

Non-Patent Citations (3)

* Cited by examiner, † Cited by third party
Title
LAMBRECHT R M ET AL: "TARGET PREPARATION AND RECOVERY OF ENRICHED ISOTOPES FOR MEDICAL RADIONUCLIDE PRODUCTION", NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH, SECTION - A: ACCELERATORS, SPECTROMETERS, DETECTORS AND ASSOCIATED EQUIPMENT, ELSEVIER, AMSTERDAM, NL, vol. A282, no. 1, 1 October 1989 (1989-10-01), pages 296 - 300, XP000067682, ISSN: 0168-9002 *
QAIM S M ET AL: "Production of <201>Tl and <203>Pb via proton induced nuclear reactions on natural thallium", INTERNATIONAL JOURNAL OF APPLIED RADIATION AND ISOTOPES UK, vol. 30, no. 2, February 1979 (1979-02-01), pages 85 - 95, XP002415296, ISSN: 0020-708X *
QAIM S. M.; WEINREICH R.; OLLIG H.: "Production of Tl-201 and Pb203 via Proton Induced Nuclear Reaction on Natural Thallium", INTERNATIONAL JOURNAL OF APPLIED RADIATION AND ISOTOPES, vol. 30, 1979, pages 85 - 95

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1916669B1 (en) * 2006-10-25 2014-12-24 Atomic Energy Council - Institute of Nuclear Energy Research Separation Device for Radioisotope Tl-201

Also Published As

Publication number Publication date
EP1892728B1 (en) 2013-12-04
EP1892728B9 (en) 2014-04-09

Similar Documents

Publication Publication Date Title
KR102570211B1 (en) Separation of target tree combinations
US6490330B1 (en) Production of high specific activity copper -67
US6337055B1 (en) Inorganic sorbent for molybdenum-99 extraction from irradiated uranium solutions and its method of use
EP1076905B1 (en) Production of palladium-103
ES2553743T3 (en) Purification process for Mo-99
CA2576907A1 (en) Method of separating and purifying cesium-131 from barium carbonate
EP1892728A1 (en) Process of producing the radioisotope TL-201
US5167938A (en) Process for strontium-82 separation
KR100858265B1 (en) Process for the recovery of a radioisotope from an irradiated target
US7578982B1 (en) Radioisotope TI-201 production process
EP4136661A2 (en) Technetium-99m generator for enriched molybdenum
WO2004059661A1 (en) Rubidium-82 generator based on sodium nonatitanate support, and separation methods for the recovery of the recovery of strontium-82 from irradiated targets
JP4571109B2 (en) Production process of radioisotope thallium-201
US7578935B2 (en) Separation device of radioisotope Tl-201
RU2695635C1 (en) Method of producing radionuclide lutetium-177
TW200800372A (en) Process for producing radioisotope Tl-201
TWI320058B (en)
TWI574728B (en) Method for making carrier-free radioactive isotopic gallium-67
CN1053017C (en) Method for extracting palladium metal
JP4936304B2 (en) Recovery method for recovering thallium-203 isotope from thallium-201 radioisotope residue
CN115198120B (en) From containing 176 Yb 3+ Recovery and enrichment in leacheate 176 Yb 2 O 3 Is a method of (2)
EP1916669A1 (en) Separation Device for Radioisotope Tl-201
JP4674727B2 (en) Separation apparatus for radioisotope thallium-201
JP5916084B2 (en) Purified Mo solution preparation method for preparation and purified Mo solution preparation apparatus for preparation
CN116646104A (en) Separation and preparation from waste Sr-90 radioactive source 90 Method of Y nuclides

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

AK Designated contracting states

Kind code of ref document: A1

Designated state(s): AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HU IE IS IT LI LT LU LV MC NL PL PT RO SE SI SK TR

AX Request for extension of the european patent

Extension state: AL BA HR MK YU

17P Request for examination filed

Effective date: 20080331

17Q First examination report despatched

Effective date: 20080618

AKX Designation fees paid

Designated state(s): AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HU IE IS IT LI LT LU LV MC NL PL PT RO SE SI SK TR

REG Reference to a national code

Ref country code: DE

Ref legal event code: R079

Ref document number: 602006039480

Country of ref document: DE

Free format text: PREVIOUS MAIN CLASS: G21G0004080000

Ipc: G21G0001000000

RIC1 Information provided on ipc code assigned before grant

Ipc: G21G 1/00 20060101AFI20120910BHEP

GRAP Despatch of communication of intention to grant a patent

Free format text: ORIGINAL CODE: EPIDOSNIGR1

INTG Intention to grant announced

Effective date: 20130628

RAP1 Party data changed (applicant data changed or rights of an application transferred)

Owner name: ATOMIC ENERGY COUNCIL - INSTITUTE OF NUCLEAR ENERG

GRAS Grant fee paid

Free format text: ORIGINAL CODE: EPIDOSNIGR3

GRAA (expected) grant

Free format text: ORIGINAL CODE: 0009210

AK Designated contracting states

Kind code of ref document: B1

Designated state(s): AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HU IE IS IT LI LT LU LV MC NL PL PT RO SE SI SK TR

REG Reference to a national code

Ref country code: GB

Ref legal event code: FG4D

REG Reference to a national code

Ref country code: CH

Ref legal event code: EP

REG Reference to a national code

Ref country code: AT

Ref legal event code: REF

Ref document number: 643813

Country of ref document: AT

Kind code of ref document: T

Effective date: 20140115

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: 602006039480

Country of ref document: DE

Effective date: 20140130

REG Reference to a national code

Ref country code: NL

Ref legal event code: VDEP

Effective date: 20131204

REG Reference to a national code

Ref country code: AT

Ref legal event code: MK05

Ref document number: 643813

Country of ref document: AT

Kind code of ref document: T

Effective date: 20131204

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

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: 20131204

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: 20131204

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: 20131204

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: 20131204

REG Reference to a national code

Ref country code: LT

Ref legal event code: MG4D

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

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: 20131204

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: 20131204

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: 20131204

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

Ref country code: BE

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: 20131204

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: 20131204

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: 20140404

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

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: 20131204

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: 20131204

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: 20131204

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: 20140404

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: 20131204

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: 20131204

REG Reference to a national code

Ref country code: DE

Ref legal event code: R097

Ref document number: 602006039480

Country of ref document: DE

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

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: 20131204

26N No opposition filed

Effective date: 20140905

REG Reference to a national code

Ref country code: DE

Ref legal event code: R097

Ref document number: 602006039480

Country of ref document: DE

Effective date: 20140905

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: 20131204

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

Ref country code: LU

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: 20140824

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: 20131204

REG Reference to a national code

Ref country code: CH

Ref legal event code: PL

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

Effective date: 20140824

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: 20140831

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: 20131204

Ref country code: CH

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

Effective date: 20140831

REG Reference to a national code

Ref country code: IE

Ref legal event code: MM4A

REG Reference to a national code

Ref country code: FR

Ref legal event code: ST

Effective date: 20150430

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: 20140824

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: 20140824

Ref country code: FR

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

Effective date: 20140901

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

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: 20131204

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

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: 20140305

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

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: 20060824

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: 20131204

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

Ref country code: DE

Payment date: 20180426

Year of fee payment: 13

REG Reference to a national code

Ref country code: DE

Ref legal event code: R119

Ref document number: 602006039480

Country of ref document: DE

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: 20200303