WO1999050855A1 - Medizinische radioaktive ruthenium-strahlenquellen hoher dosisleistung und verfahren zur herstellung dieser - Google Patents
Medizinische radioaktive ruthenium-strahlenquellen hoher dosisleistung und verfahren zur herstellung dieser Download PDFInfo
- Publication number
- WO1999050855A1 WO1999050855A1 PCT/EP1999/002159 EP9902159W WO9950855A1 WO 1999050855 A1 WO1999050855 A1 WO 1999050855A1 EP 9902159 W EP9902159 W EP 9902159W WO 9950855 A1 WO9950855 A1 WO 9950855A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- ruthenium
- carrier
- gold
- layers
- radioactive
- Prior art date
Links
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
- C25D3/00—Electroplating: Baths therefor
- C25D3/02—Electroplating: Baths therefor from solutions
- C25D3/50—Electroplating: Baths therefor from solutions of platinum group metals
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
- C25D5/00—Electroplating characterised by the process; Pretreatment or after-treatment of workpieces
- C25D5/10—Electroplating with more than one layer of the same or of different metals
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25D—PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
- C25D5/00—Electroplating characterised by the process; Pretreatment or after-treatment of workpieces
- C25D5/60—Electroplating characterised by the structure or texture of the layers
- C25D5/623—Porosity of the layers
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61N—ELECTROTHERAPY; MAGNETOTHERAPY; RADIATION THERAPY; ULTRASOUND THERAPY
- A61N5/00—Radiation therapy
- A61N5/10—X-ray therapy; Gamma-ray therapy; Particle-irradiation therapy
- A61N5/1001—X-ray therapy; Gamma-ray therapy; Particle-irradiation therapy using radiation sources introduced into or applied onto the body; brachytherapy
- A61N2005/1019—Sources therefor
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61N—ELECTROTHERAPY; MAGNETOTHERAPY; RADIATION THERAPY; ULTRASOUND THERAPY
- A61N5/00—Radiation therapy
- A61N5/10—X-ray therapy; Gamma-ray therapy; Particle-irradiation therapy
- A61N5/1001—X-ray therapy; Gamma-ray therapy; Particle-irradiation therapy using radiation sources introduced into or applied onto the body; brachytherapy
- A61N5/1002—Intraluminal radiation therapy
Definitions
- the invention relates to radioactive ruthenium radiation sources with a dose rate of at least 1.5 Gy / min at a distance of 2 mm (water), which consist of an activity carrier and an enclosure of the carrier from a body-compatible material, with a multi-layer system of metals on the carrier and / or alloys are electroplated, in which at least two layers consist of ruthenium-106, and inactive intermediate layers of other metals or alloys are present between the radioactive ruthenium layers.
- the activity carrier is made with a body-compatible material, e.g. a metal or plastic.
- the activity carrier can be enclosed by filling it into a capsule and then closing it, or by means of electrodeposition of a cover layer, e.g. made of hard gold.
- Electrolytes but is halogen-free, contains at least 1.5 g / 1 sulphate ions and has a pH of at most 4.
- Ruthenium radiation sources for ophthalmology on the market are made by electrolytic deposition of ruthenium made from commercially available radioactive ruthenium (III) chloride solutions.
- the thin layers obtained in this way with dose rates of 0.1 to 0.5 Gy / min. are sufficient for the use of the radiation source as an eye applicator in the tumor treatment of the eye.
- these radiation sources are not suitable because they do not have the necessary dose rate due to the achievable only thin layers.
- the object of the invention was therefore to provide radioactive ruthenium radiation sources for medical applications which should have a high dose rate and which, despite the necessary thickness of the active ruthenium layer, should have the necessary flexibility and geometry, for example in the intravascular treatment of vascular anomalies to be able to be used.
- the object of the invention was also to demonstrate a method for producing such sources.
- radioactive ruthenium-106 radiation sources which comprise an activity carrier and an enclosure of the carrier made of a body-compatible material, a multi-layer system made of metals and / or alloys having at least two layers of radioactive ruthenium being applied to the carrier exist and between the radioactive ruthenium layers there are inactive intermediate layers of other metals or alloys.
- These radiation sources according to the invention have well-adhering ruthenium layers of the necessary thickness (and thus the necessary dose rate), which despite the typical bending stress, for example in the case of intravascular treatment of vascular anomalies, optically crack-free.
- the radiation sources according to the invention are produced by electrolytic deposition of this multilayer system on a conductive carrier.
- a galvanic radioactive ruthenium bath For the galvanic radioactive ruthenium bath,
- RuNC anionic ruthenium complex [Ru 2 NCl8 (H 2 0) 2 ]
- PPS sulfopropylpyridine
- the RuNC electrolyte is produced in one step by hydrolysis of ruthenium (III) chloride solution, which for the purposes of the invention contains at least 8 Ci / g ruthenium, in an excess of amidosulfonic acid. This production is essentially known from the literature. Under the present active conditions, refluxing is replaced by tempering to about 90 ° C.
- the electrolyte thus obtained can be used without further steps, so that, according to the invention, the preparation of the electrolyte is carried out directly in the electrolysis cell developed for the method according to the invention (cf. FIG. 1).
- Gold, nickel, titanium or their alloys can be deposited as metals between the individual ruthenium layers. It is also possible according to the invention not to produce all intermediate layers from the same metal, but to use different metals for the intermediate layers. If the activity carrier produced according to the invention is to be enclosed by means of an electrodeposable cover layer, gold is preferably used here. In a preferred embodiment, the intermediate layers are also made of gold, it being possible to use commercially available galvanic gold baths from Degussa.
- the “Auruna® 311” electrolyte for the first gold layer on the carrier which serves as an adhesion promoter between the carrier and the first ruthenium layer, and the “Auruna®” electrolyte for the intermediate layers 533 ". If the radiation source is to be enclosed by means of an electrodeposited cover layer, the Auruna® "533" electrolyte is also suitable for producing a hard gold layer.
- supports made of brass, copper, alloyed steels, nickel, titanium or their alloys, silver, gold or platinum metals are suitable as metallic supports which also serve as cathode.
- Nitinol or gold are preferably used as the carrier material.
- surface-modified, ie, electrically conductive, polymers as supports.
- the carrier can have any shape or form. It can also consist of several support elements, each of which has the multilayer system. A tube or several tubular elements, a single wire or an arrangement of several wires, a structured or unstructured film, a net, a rotationally symmetrical shaped body or a sphere can be used as the carrier. A wire or tube is preferably used.
- tubular elements with a circular cross section which can particularly preferably consist of gold, are used as supports, the outer diameter of which is larger at each end than in intermediate section (see FIG. 2a).
- the outer diameter of the tubular elements is up to 0.6 mm at the ends and up to 0.3 mm in the intermediate section.
- the length of the elements is 0.5-70 mm, depending on the desired application and the necessary flexibility.
- these tubular elements “threaded onto the wire” form the 106 Ru radiation source (cf. FIG. 3). Because the individual elements can be freely rotated, this radiation source is particularly flexible.
- the pretreatment of the carrier used is of essential importance for the adhesive strength of the multilayer coating according to the invention. This must be degreased and any oxide layers and any adhering particles must be removed. If nitinol is used as a carrier, a final pickling with a mixture of hydrofluoric acid and hydrochloric acid has proven to be advantageous. In a preferred embodiment, a gold layer is applied as an adhesion promoter to the carrier made of nitinol as the first layer.
- pre-gilding can of course be omitted. If tubular elements - as described above - are to be coated, the sections to be left free must be coated at the ends with a masking varnish.
- the electrolytic deposition of the ruthenium layers according to the invention takes place in compliance with the following operating parameters:
- the ruthenium concentration at the beginning of the electrolysis is typically 5 g / 1 and can drop to 0.2 g / 1 due to depletion of ruthenium.
- the temperature should be between 60-75 ° C, preferably 70 ° C, the pH must be kept between 1.3-1.8.
- the ruthenium concentration and the pH value are checked and adjusted at regular intervals.
- ruthenium-106 radiation sources are thus provided which have sufficiently thick, well-adhering, crack-free, homogeneous and flexible radioactive ruthenium layers.
- radioactive ruthenium layers with a thickness of up to 5 ⁇ m are achieved.
- ruthenium-106 total layer thicknesses of up to 30 ⁇ m are achieved, whereby as Total layer thickness is understood as the sum of all radioactive ruthenium layers.
- the ruthenium radiation sources produced from these multi-coated ruthenium activity carriers have a dose rate of at least 1.5 to 15 Gy per min at a distance of 2 mm (in water).
- the electrolysis cell preferably used according to the invention consists of a vessel 1 with a double jacket 7 for temperature control.
- the dimensions of the electrolysis vessel 1 must meet the requirement for a minimum working volume.
- the working volume should preferably not exceed 5 ml.
- the electrolysis vessel 1 must be suitable for the preparation and adjustment of the electrolyte in such a way that the addition of liquids via an opening 10 and stirring of the electrolyte by means of a stirrer 5 is possible.
- the cathode 2 must also be able to be positioned in the electrolyte in accordance with the desired active length.
- the electrolytic cell 1 was designed in such a way that the cathode 2 is connected to a device for opening the working space 3.
- the anode 4 coaxially surrounds the cathode 2.
- the electrolysis vessel 1 contains an element for the extraction of gases and vapors 6, so that a slight negative pressure can be permanently applied.
- FIG. 2 shows the tubular support elements used in a preferred embodiment, a) without and b) with a coating.
- Fig. 3 shows the coated on a wire "tubular" coated tubular elements in their
- Example 1 Electrolytic generation of radioactive ruthenium layers by using nitinol wire with a diameter of 0.3-0.5 mm and the intermediate layers and the cover layer being made of gold.
- Pre-gilding serves to promote adhesion between the substrate and the Ru layer.
- the commercial electrolyte Auruna® 311 was chosen as gold. A previous acid activation is already given by the pickling. Gold is also suitable as an intermediate layer between the Ru deposits, with the electrolyte Auruna® 533 being selected.
- the preactivation is carried out by pickling with sulfuric acid (5%, RT, 0.5 min). Both electrolytes are cyano-gold complexes from Degussa. 12
- Auruna® 533 (Degussa, 8 g / 1, 35 ° C, 7 mm, 1 A / dm 2 )
- the Ru complex RuNC is used as an electrolyte.
- the preparation takes place in advance directly in the specially developed electrolysis cell.
- the electrolyte was modified by adding PPS (sulfopropyl pyrid, 3 g / 1, from Raschig).
- the operating parameters of Ru electrolysis are: -Ru concentration range 4.8-0.2 g / 1 Ru
- this can also be made of hard gold (analogous to the intermediate layers using Auruna® 533).
- Radioactive ruthenium radiation source by electrolytic production of radioactive ruthenium layers on a conductive support, by coating a nitinol tube or wire with an outer diameter of 0.2-0.6 mm over a length of 0.5-7 cm and intermediate layers as well the gold top layer can be used. 13
- the quality parameters of the top layer must guarantee freedom from pores against the washing out of radioactive soot and freedom from cracks under typical mechanical stress and wear resistance against abrasion on HD-PE.
- Such a cover layer can be produced from hard gold (see example 1).
- the elements are made of gold and can only be coated with ruthenium on the thin, intermediate sections. This object is achieved in that sections to be left free are covered with a non-conductive masking lacquer.
- the carriers are pretreated as described in Example 1, with the omission of step 4.
- Example. 1 The cover layer is applied as described in Example 1. Since the cover layer is to be applied to the masked Rohrab ⁇ cuts, of these, the masking lacquer by dissolving in acetone is removed.
- the tubular members thus produced unit length ⁇ Licher be pushed onto a wire and secured at the ends against falling out (for example by welding an end piece).
- Pipe-like parts with different outer diameters in sections are used as carriers
- the elements are made of gold or titanium and can only be coated with ruthenium on the thin, intermediate sections. This object is achieved in that sections to be left free with a non-conductive
- the carriers are pretreated as described in Example 1.
- the ruthenium deposition is carried out as in Example 1.
- the Maskie ⁇ approximately lacquer by dissolving in acetone is removed.
- the gold top layer is not applied. Instead, the tubular parts are inserted into a larger tube of the same material.
- the uncoated edge of the carrier activity ⁇ (outer diameter 0.28 mm) is welded tubes with the closure at the ends.
- the now encapsulated tubular elements of uniform length are pushed onto a wire and fixed at both ends.
- different numbers of bodies can be threaded.
- the individual free rotatability of the individual bodies provides flexibility in the overall arrangement.
- the encapsulation of the individual bodies provides increased stability and, in particular, greater abrasion resistance.
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Electroplating Methods And Accessories (AREA)
- Electroplating And Plating Baths Therefor (AREA)
Abstract
Description
Claims
Priority Applications (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US09/424,895 US6319190B1 (en) | 1998-03-31 | 1999-03-30 | Medicinal radioactive ruthenium radiation sources with high dosage rate and method for producing the same |
EP99916898A EP0986818A1 (de) | 1998-03-31 | 1999-03-30 | Medizinische radioaktive ruthenium-strahlenquellen hoher dosisleistung und verfahren zur herstellung dieser |
JP54888099A JP2002500772A (ja) | 1998-03-31 | 1999-03-30 | 高線量率の医療用放射性ルテニウム放射線源とその製造方法 |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19815568A DE19815568C2 (de) | 1998-03-31 | 1998-03-31 | Verfahren zur Herstellung von medizinischen radioaktiven Ruthenium-Strahlenquellen durch elektrolytische Abscheidung von radioaktivem Ruthenium auf einem Träger, mit diesem Verfahren hergestellte Strahlenquellen und Elektrolysezelle zur Erzeugung von radioaktiven Ruthenium-Schichten |
DE19815568.9 | 1998-03-31 |
Publications (1)
Publication Number | Publication Date |
---|---|
WO1999050855A1 true WO1999050855A1 (de) | 1999-10-07 |
Family
ID=7863879
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/EP1999/002159 WO1999050855A1 (de) | 1998-03-31 | 1999-03-30 | Medizinische radioaktive ruthenium-strahlenquellen hoher dosisleistung und verfahren zur herstellung dieser |
Country Status (5)
Country | Link |
---|---|
US (1) | US6319190B1 (de) |
EP (1) | EP0986818A1 (de) |
JP (1) | JP2002500772A (de) |
DE (1) | DE19815568C2 (de) |
WO (1) | WO1999050855A1 (de) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US10818412B2 (en) | 2016-03-31 | 2020-10-27 | Autonetworks Technologies, Ltd. | Communication cable |
Families Citing this family (13)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US6471671B1 (en) | 2000-08-23 | 2002-10-29 | Scimed Life Systems, Inc. | Preloaded gas inflation device for balloon catheter |
US6416492B1 (en) | 2000-09-28 | 2002-07-09 | Scimed Life Systems, Inc. | Radiation delivery system utilizing intravascular ultrasound |
AU2003267309A1 (en) | 2000-11-16 | 2004-04-08 | Microspherix Llc | Flexible and/or elastic brachytherapy seed or strand |
US7074291B2 (en) | 2001-11-02 | 2006-07-11 | Worldwide Medical Technologies, L.L.C. | Delivery system and method for interstitial radiation therapy using strands constructed with extruded strand housings |
US7060020B2 (en) | 2001-11-02 | 2006-06-13 | Ideamatrix, Inc. | Delivery system and method for interstitial radiation therapy |
US7070554B2 (en) | 2003-01-15 | 2006-07-04 | Theragenics Corporation | Brachytherapy devices and methods of using them |
US6997862B2 (en) | 2003-05-13 | 2006-02-14 | Ideamatrix, Inc. | Delivery system and method for interstitial radiation therapy using seed strands with custom end spacing |
US7736293B2 (en) * | 2005-07-22 | 2010-06-15 | Biocompatibles Uk Limited | Implants for use in brachytherapy and other radiation therapy that resist migration and rotation |
US8187159B2 (en) | 2005-07-22 | 2012-05-29 | Biocompatibles, UK | Therapeutic member including a rail used in brachytherapy and other radiation therapy |
US7988611B2 (en) * | 2006-05-09 | 2011-08-02 | Biocompatibles Uk Limited | After-loader for positioning implants for needle delivery in brachytherapy and other radiation therapy |
US7878964B1 (en) | 2006-09-07 | 2011-02-01 | Biocompatibles Uk Limited | Echogenic spacers and strands |
US7874976B1 (en) | 2006-09-07 | 2011-01-25 | Biocompatibles Uk Limited | Echogenic strands and spacers therein |
KR101409458B1 (ko) * | 2007-11-28 | 2014-06-19 | 삼성전자주식회사 | 방향 기능을 갖는 휴대용 단말기 및 이를 구비한 단말기충전 장치 |
Citations (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
BE424536A (de) * | ||||
DE901685C (de) * | 1947-09-27 | 1954-01-14 | United States Radium Corp | Radioaktive Matallfolie |
FR1206612A (fr) * | 1956-01-23 | 1960-02-10 | Centre Nat Rech Scient | Procédé de préparation de dépôts et de revêtements de ruthénium métallique par électrolyse |
US3793162A (en) * | 1971-12-17 | 1974-02-19 | Int Nickel Co | Electrodeposition of ruthenium |
EP0018165A1 (de) * | 1979-04-10 | 1980-10-29 | Inco Europe Limited | Bad und Verfahren zum galvanischen Abscheiden von Ruthenium, konzentrierte Lösung zur Badherstellung und mit Ruthenium beschichteter Gegenstand |
Family Cites Families (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB1520140A (en) * | 1976-06-08 | 1978-08-02 | Inco Europ Ltd | Electrodeposition of ruthenium |
-
1998
- 1998-03-31 DE DE19815568A patent/DE19815568C2/de not_active Expired - Fee Related
-
1999
- 1999-03-30 EP EP99916898A patent/EP0986818A1/de not_active Withdrawn
- 1999-03-30 JP JP54888099A patent/JP2002500772A/ja active Pending
- 1999-03-30 WO PCT/EP1999/002159 patent/WO1999050855A1/de not_active Application Discontinuation
- 1999-03-30 US US09/424,895 patent/US6319190B1/en not_active Expired - Lifetime
Patent Citations (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
BE424536A (de) * | ||||
DE901685C (de) * | 1947-09-27 | 1954-01-14 | United States Radium Corp | Radioaktive Matallfolie |
FR1206612A (fr) * | 1956-01-23 | 1960-02-10 | Centre Nat Rech Scient | Procédé de préparation de dépôts et de revêtements de ruthénium métallique par électrolyse |
US3793162A (en) * | 1971-12-17 | 1974-02-19 | Int Nickel Co | Electrodeposition of ruthenium |
EP0018165A1 (de) * | 1979-04-10 | 1980-10-29 | Inco Europe Limited | Bad und Verfahren zum galvanischen Abscheiden von Ruthenium, konzentrierte Lösung zur Badherstellung und mit Ruthenium beschichteter Gegenstand |
Non-Patent Citations (1)
Title |
---|
HOLMES P A ET AL: "Preparation of thin-film tritium sources for determination of the neutrino mass", NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH, SECTION A (ACCELERATORS, SPECTROMETERS, DETECTORS AND ASSOCIATED EQUIPMENT), 1 JUNE 1988, NETHERLANDS, vol. A269, no. 1, ISSN 0168-9002, pages 29 - 32, XP002107598 * |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US10818412B2 (en) | 2016-03-31 | 2020-10-27 | Autonetworks Technologies, Ltd. | Communication cable |
Also Published As
Publication number | Publication date |
---|---|
JP2002500772A (ja) | 2002-01-08 |
DE19815568C2 (de) | 2000-06-08 |
US6319190B1 (en) | 2001-11-20 |
DE19815568A1 (de) | 1999-10-07 |
EP0986818A1 (de) | 2000-03-22 |
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