EP1996739B1 - Use of a heat exchanger tube - Google Patents
Use of a heat exchanger tube Download PDFInfo
- Publication number
- EP1996739B1 EP1996739B1 EP07711975A EP07711975A EP1996739B1 EP 1996739 B1 EP1996739 B1 EP 1996739B1 EP 07711975 A EP07711975 A EP 07711975A EP 07711975 A EP07711975 A EP 07711975A EP 1996739 B1 EP1996739 B1 EP 1996739B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- heat exchanger
- tube
- exchanger tube
- tube according
- heat
- 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.)
- Active
Links
Classifications
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28F—DETAILS OF HEAT-EXCHANGE AND HEAT-TRANSFER APPARATUS, OF GENERAL APPLICATION
- F28F21/00—Constructions of heat-exchange apparatus characterised by the selection of particular materials
- F28F21/08—Constructions of heat-exchange apparatus characterised by the selection of particular materials of metal
- F28F21/081—Heat exchange elements made from metals or metal alloys
- F28F21/085—Heat exchange elements made from metals or metal alloys from copper or copper alloys
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C9/00—Alloys based on copper
Definitions
- the present invention relates to the use of a heat exchanger tube made of a copper alloy.
- CO2 as a natural refrigerant that does not contribute to the destruction of the ozone layer and is neutral in its direct contribution to the greenhouse effect, is an ecologically interesting and economically viable alternative to the HFC refrigerants currently in use in Europe.
- the working range of the refrigerant CO2 is at pressures up to 130 bar and thus far above the usual for CFC and HFC safety refrigerants pressures up to 35 bar. But Depending on the application, permissible pressures of up to 50 bar are also required for evaporators, in particular if hot gas defrosting is provided.
- a Cu-Zn-P-Ni-Fe-Sn-Co alloy which can be used for heat exchange tubes.
- properties such as yield strength or tensile strength are of central importance in connection with some refrigerants.
- the material properties ultimately determine the required tube wall thickness, which is required, for example, for the CO 2 refrigerant for higher pressures.
- the invention has for its object to seek alternative solutions that allow the use of copper alloys at low pipe thicknesses even at high pressure levels.
- the invention is based on the consideration that a heat exchanger tube with an inside substantially smooth or textured surface for use in the gas cooler, condenser or evaporator of a working with CO2 chiller or heat pump is used.
- the term includes on the inside substantially smooth also by welding seams resulting surfaces.
- the working medium CO2 flows on the inside of the heat exchanger tubes and, depending on the temperature conditions of the specific application, has a pressure position that clearly stands out from the pressures known for CFC and HFC safety refrigerants and places high demands on the pressure resistance of the tubes used.
- the particular advantage is that by the higher-strength Cu alloys according to the invention, which allow small wall thicknesses even at high pressure levels, thus significant material savings and thus weight and cost advantage can be achieved.
- these Cu alloys have excellent processing properties, especially expansion, bending and brazing.
- the pipe outside diameter may be in the range of 3-16 mm.
- the ratio of the wall thickness to the pipe outside diameter is advantageously selected in the range of 0.025 to 0.08. This results in pipe wall thicknesses which are in the similar size range as today for HFC safety refrigerants usually used copper tubes are made of Cu-DHP and thus can be expected very good properties with respect to the further processing,
- the pipe material may have a yield strength R p0.2 over 160 N / mm 2 . It is also essential that the tube material has a tensile strength R m above 300 N / mm 2 . This results, for example, for a pipe with an outer diameter of 9.52 mm and an operating pressure of 130 bar necessary pipe wall thicknesses of at most 0.55 mm and thus a material saving of more than 40% compared to pipes made of Cu-DHP.
- the heat exchanger tube may be formed of a strip material and have a weld.
- welds come into consideration, which extend in the axial direction or are spirally encircling.
- As a possible joining method for pipe production is particularly suitable for the high-frequency welding process. This results in particular advantages over other joining methods on the one hand, realizable high production speeds and, secondly, a microstructure state, which after a usually following annealing process has no loss of strength over the material not influenced by the joining process.
- the heat exchanger tube may be seamless.
- seamless tubes and welded tubes may be considered equivalent in the use of the invention.
Landscapes
- Engineering & Computer Science (AREA)
- Mechanical Engineering (AREA)
- Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- General Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Heat-Exchange Devices With Radiators And Conduit Assemblies (AREA)
- Devices That Are Associated With Refrigeration Equipment (AREA)
- Sorption Type Refrigeration Machines (AREA)
Abstract
Description
Die vorliegende Erfindung betrifft die Verwendung eines Wärmeaustauscherrohrs aus einer Kupferlegierung.The present invention relates to the use of a heat exchanger tube made of a copper alloy.
Nachdem die chlorhaltigen Sicherheitskältemittel (FCKW) aufgrund ihrer ozonschädigenden Wirkung durch chlorfreie Sicherheitskältemittel (HFKW) ersetzt wurden, kam schon bald die Diskussion um deren hohes Treibhauspotential auf. Vermehrt in den Blick rückten aus diesem Grund die natürlichen Kältemittel, vor allem CO2.After the chlorine-containing safety refrigerants (CFCs) were replaced by chlorine-free safety refrigerants (HFCs) due to their ozone-damaging effect, the discussion about their high global warming potential soon came up. For this reason, the natural refrigerants, especially CO2, increasingly came into view.
CO2 ist als natürliches Kältemittel, das nicht zur Zerstörung der Ozonschicht beiträgt und sich bezüglich des direkten Beitrags zum Treibhauseffekt neutral verhält, eine ökologisch interessante und je nach Anwendung und Rahmenbedingung wirtschaftliche Alternative zu den heute in Europa überwiegend eingesetzten HFKW-Kältemitteln.CO2, as a natural refrigerant that does not contribute to the destruction of the ozone layer and is neutral in its direct contribution to the greenhouse effect, is an ecologically interesting and economically viable alternative to the HFC refrigerants currently in use in Europe.
So sind in der Kältetechnik Anwendungen im Kaskadenbetrieb mit NH3 bekannt, in denen CO2 Verdampfer und Kondensatoren im unterkritischen Betrieb eingesetzt werden, aber auch transkritische CO2-Kälteprozesse und -Wärmepumpen, in denen der Verdampfer unterhalb und der dem Kondensator entsprechende Gaskühler oberhalb des kritischen Punktes von CO2 arbeiten.In the refrigeration industry, for example, applications in cascade operation with NH3 are known, in which CO2 evaporators and condensers are used in subcritical operation, but also transcritical CO2 refrigeration processes and heat pumps in which the evaporator below and the condenser corresponding gas cooler above the critical point of CO2 work.
Insbesondere im letzteren Fall des Gaskühlers liegt der Arbeitsbereich des Kältemittel CO2 bei Drücken bis zu 130 bar und somit weit oberhalb der bei FCKW- und HFKW-Sicherheitskältemitteln üblichen Drücke bis zu 35 bar. Aber auch für Verdampfer werden je nach Anwendung zulässige Drücke bis 50 bar gefordert, insbesondere wenn eine Heißgasabtauung vorgesehen ist.Especially in the latter case of the gas cooler, the working range of the refrigerant CO2 is at pressures up to 130 bar and thus far above the usual for CFC and HFC safety refrigerants pressures up to 35 bar. But Depending on the application, permissible pressures of up to 50 bar are also required for evaporators, in particular if hot gas defrosting is provided.
Diese Druckanforderungen sind mit Kupferrohren aus Cu-DHP, welche üblicherweise in mit FCKW- und HFKW-Sicherheitkältemitteln betriebenen Wärmeaustauschern eingesetzt werden, nur schwer zu realisieren, da sehr große Rohrwandstärken einzusetzen sind, mit entsprechend negativen Auswirkungen auf die Verarbeitbarkeit, insbesondere das Aufweiten und Biegen, das Gewicht des Wärmeaustauschers und die Apparatekosten. Stattdessen ist es heute Stand der Technik, Rohre aus feuerverzinktem Stahl oder Edelstahl einzusetzen, mit denen die genannten Drücke relativ einfach zu beherrschen sind.These pressure requirements are difficult to realize with copper pipes made of Cu-DHP, which are usually used in heat exchangers operated with CFC and HFC safety refrigerants, since very large pipe wall thicknesses are to be used, with correspondingly negative effects on the processability, in particular the expansion and bending , the weight of the heat exchanger and the apparatus costs. Instead, it is now state of the art to use pipes made of hot-dip galvanized steel or stainless steel, with which the said pressures are relatively easy to control.
Allerdings weisen auch die bisher eingesetzten Rohre aus Stahl bzw. Edelstahl deutliche Nachteile gegenüber Kupfer in Bezug auf die Verarbeitbarkeit, die Effizienz und die Kosten auf.However, the steel or stainless steel pipes used hitherto also show considerable disadvantages compared to copper in terms of processability, efficiency and costs.
Aus der Druckschrift
Der Erfindung liegt die Aufgabe zugrunde, Alternativlösungen zu suchen, die auch bei hohen Drucklagen den Einsatz von Kupferlegierungen bei kleinen Rohrvandstärken erlauben.The invention has for its object to seek alternative solutions that allow the use of copper alloys at low pipe thicknesses even at high pressure levels.
Die Erfindung wird durch die Merkmale des Anspruchs 1 wiedergegeben. Die weiteren rückbezogenen Ansprüche betreffen vorteilhafte Aus- und Weiterbildungen der Erfindung.The invention is represented by the features of claim 1. The other dependent claims relate to advantageous embodiments and further developments of the invention.
Die Erfindung geht dabei von der Überlegung aus, dass ein Wärmeaustauscherrohr mit einer innenseitig im Wesentlichen glatten oder strukturierten Oberfläche zum Einsatz im Gaskühler, Kondensator oder Verdampfer einer mit CO2 arbeitenden Kältemaschine oder Wärmepumpe verwendet wird. In diesem Zusammenhang schließt der Begriff innenseitig im Wesentlichen glatt auch durch Schweißnähte entstehende Oberflächen mit ein. Das Arbeitsmedium CO2 fließt dabei auf der Innenseite der Wärmeaustauscherrohre und weist abhängig von den Temperaturbedingungen der speziellen Anwendung eine Drucklage auf, die sich deutlich von den für FCKW- und HFKW-Sicherheitskältemitteln bekannten Drücken abhebt und hohe Anforderungen an die Druckbeständigkeit der eingesetzten Rohre stellt.The invention is based on the consideration that a heat exchanger tube with an inside substantially smooth or textured surface for use in the gas cooler, condenser or evaporator of a working with CO2 chiller or heat pump is used. In this context, the term includes on the inside substantially smooth also by welding seams resulting surfaces. The working medium CO2 flows on the inside of the heat exchanger tubes and, depending on the temperature conditions of the specific application, has a pressure position that clearly stands out from the pressures known for CFC and HFC safety refrigerants and places high demands on the pressure resistance of the tubes used.
Bisher wurden in entsprechenden Anwendungen zumeist Edelstähle und Stähle bevorzugt eingesetzt, da die in der Kälte-/Klimatechnik sonst üblichen Kupferrohre aus Cu-DHP aufgrund der Drucklage und der erforderlichen großen Wandstärken bisher hohe Kostennachteile aufwiesen.So far, stainless steels and steels have usually been used with preference in corresponding applications, since the copper pipes made of Cu-DHP which are otherwise customary in refrigeration / air conditioning technology have hitherto had high cost disadvantages owing to the pressure situation and the required large wall thicknesses.
Der besondere Vorteil besteht darin, dass durch die erfindungsgemäßen höherfesten Cu-Legierungen, die auch bei hohen Drucklagen kleine Wandstärken erlauben, somit deutliche Materialeinsparungen ermöglicht und dadurch Gewichts- und Kostenvorteil erzielt werden. Zudem weisen diese Cu-Legierungen exzellente Eigenschaften bei der Verarbeitung, insbesondere dem Aufweiten, Biegen und Löten auf.The particular advantage is that by the higher-strength Cu alloys according to the invention, which allow small wall thicknesses even at high pressure levels, thus significant material savings and thus weight and cost advantage can be achieved. In addition, these Cu alloys have excellent processing properties, especially expansion, bending and brazing.
In bevorzugter Ausgestaltung der Erfindung kann der Rohraußendurchmesser im Bereich von 3-16 mm liegen. In diesem Zusammenhang wird das Verhältnis der Wandstärke zum Rohraußendurchmesser vorteilhafterweise im Bereich von 0,025 bis 0,08 gewählt. Hierdurch ergeben sich Rohrwandstärken, welche im ähnlichen Größenbereich wie heute für HFKW-Sicherheitskältemittel üblicherweise verwendete Kupferrohre aus Cu-DHP liegen und somit sehr gute Eigenschaften bzgl. der Weiterverarbeitbarkeit erwarten lassen,In a preferred embodiment of the invention, the pipe outside diameter may be in the range of 3-16 mm. In this connection, the ratio of the wall thickness to the pipe outside diameter is advantageously selected in the range of 0.025 to 0.08. This results in pipe wall thicknesses which are in the similar size range as today for HFC safety refrigerants usually used copper tubes are made of Cu-DHP and thus can be expected very good properties with respect to the further processing,
In bevorzugter Weiterbildung kann das Rohrmaterial eine Dehngrenze Rp0,2 über 160 N/mm2 aufweisen. Es ist weiterhin wesentlich, dass das Rohrmaterial eine Zugfestigkeit Rm über 300 N/mm2 besitzt. Hierdurch ergeben sich zum Beispiel für ein Rohr mit Außendurchmesser 9,52mm und einem Betriebsdruck von 130 bar notwendige Rohrwandstärken von höchstens 0,55 mm und damit eine Materialeinsparung von mehr als 40 % gegenüber Rohren aus Cu-DHP.In a preferred development, the pipe material may have a yield strength R p0.2 over 160 N / mm 2 . It is also essential that the tube material has a tensile strength R m above 300 N / mm 2 . This results, for example, for a pipe with an outer diameter of 9.52 mm and an operating pressure of 130 bar necessary pipe wall thicknesses of at most 0.55 mm and thus a material saving of more than 40% compared to pipes made of Cu-DHP.
Vorzugsweise kann das Wärmeaustauscherrohr aus einem Bandmaterial geformt sein und eine Schweißnaht aufweisen. Dabei kommen auch Schweißnähte in Betracht, die sich in axialer Richtung erstrecken oder spiralig umlaufend sind. Als mögliches Fügeverfahren zur Rohrherstellung eignet sich insbesondere das Hochfrequenzschweißverfahren. Hierdurch ergeben sich als besondere Vorteile gegenüber anderen Fügeverfahren zum einen realisierbare hohe Fertigungsgeschwindigkeiten und zum anderen ein Gefügezustand, der nach einem üblicherweise folgenden Glühprozess keine Festigkeitseinbußen gegenüber dem vom Fügeprozess nicht beeinflussten Material aufweist.Preferably, the heat exchanger tube may be formed of a strip material and have a weld. In this case, welds come into consideration, which extend in the axial direction or are spirally encircling. As a possible joining method for pipe production is particularly suitable for the high-frequency welding process. This results in particular advantages over other joining methods on the one hand, realizable high production speeds and, secondly, a microstructure state, which after a usually following annealing process has no loss of strength over the material not influenced by the joining process.
Alternativ kann das Wärmeaustauscherrohr nahtlos sein. Nahtlose Rohre und geschweißte Rohre können jedoch in der erfindungsgemäßen Verwendung als gleichwertig angesehen werden.Alternatively, the heat exchanger tube may be seamless. However, seamless tubes and welded tubes may be considered equivalent in the use of the invention.
Weitere Vorteile ergeben sich, wenn die Oberfläche der Innenseite des Rohres strukturiert ist. Hierdurch lassen sich der Wärmeübergangskoeffizient und damit die Wärmeübertragungsleistung steigern.Further advantages arise when the surface of the inside of the tube is structured. This can increase the heat transfer coefficient and thus the heat transfer performance.
Claims (6)
- Use of a heat exchanger tube composed of a copper alloy which comprises the alloy elements [in % by weight]
0.05 - 3 % of Fe,
0.01 - 0.15 % of P,
and optionally
0.05 - 0.2 % of Zn
0.02 - 0.05 % of Sn
and remainder Cu and unavoidable impurities, as a condenser tube, evaporator tube or gas cooler tube for an operating pressure above the critical point of a refrigerator or heat pump operating with CO2, the ratio of the wall thickness to the external tube diameter being in the range of from 0.025 to 0.08 and the tube material having a tensile strength Rm above 300 N/mm2. - Use of a heat exchanger tube according to claim 1, characterised in that the external tube diameter is in the range of 3 - 16 mm.
- Use of a heat exchanger tube according to claim 1 or 2, characterised in that the tube material has a yield strength Rp0.2 above 160 N/mm2 .
- Use of a heat exchanger tube according to any one of claims 1 to 3, characterised in that the heat exchanger tube is formed from a strip material and has a weld seam.
- Use of a heat exchanger tube according to any one of claims 1 to 3, characterised in that the heat exchanger tube is seamless.
- Use of a heat exchanger tube according to any one of claims 1 to 5, characterised in that the surface of the inside of the tube is structured.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE102006013384A DE102006013384B4 (en) | 2006-03-23 | 2006-03-23 | Use of a heat exchanger tube |
| PCT/EP2007/002379 WO2007110165A1 (en) | 2006-03-23 | 2007-03-17 | Use of a heat exchanger tube |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| EP1996739A1 EP1996739A1 (en) | 2008-12-03 |
| EP1996739B1 true EP1996739B1 (en) | 2011-07-27 |
Family
ID=38072155
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| EP07711975A Active EP1996739B1 (en) | 2006-03-23 | 2007-03-17 | Use of a heat exchanger tube |
Country Status (9)
| Country | Link |
|---|---|
| US (1) | US20090301701A1 (en) |
| EP (1) | EP1996739B1 (en) |
| JP (1) | JP2009530581A (en) |
| CN (1) | CN101395289B (en) |
| AT (1) | ATE518013T1 (en) |
| DE (1) | DE102006013384B4 (en) |
| DK (1) | DK1996739T3 (en) |
| ES (1) | ES2370352T3 (en) |
| WO (1) | WO2007110165A1 (en) |
Families Citing this family (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP5446163B2 (en) * | 2008-08-04 | 2014-03-19 | ダイキン工業株式会社 | Grooved tube for heat exchanger |
| KR20150003311A (en) * | 2012-04-16 | 2015-01-08 | 가부시키가이샤 유에이씨제이 | Level wound coil, method for manufacturing level wound coil, cross fin tube type heat exchanger, and method for manufacturing cross fin tube type heat exchanger |
| FR2995383B1 (en) | 2012-09-12 | 2015-04-10 | Kme France Sas | COPPER ALLOYS FOR HEAT EXCHANGERS |
| AT518424B1 (en) * | 2016-09-13 | 2017-10-15 | Josef Höller Gmbh | Cooling and heating plate |
| CN114085978A (en) * | 2021-10-15 | 2022-02-25 | 福建捷思金属科技发展有限公司 | Ultrahigh-pressure-resistant copper-iron alloy pipe fitting for refrigeration system and preparation method |
| WO2025131864A1 (en) | 2023-12-22 | 2025-06-26 | Elvalhalcor Hellenic Copper & Aluminium Industry S.A. | Copper alloy tube for use in hvacr system |
Family Cites Families (20)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US2373116A (en) * | 1941-10-31 | 1945-04-10 | Bundy Tubing Co | Method of uniting metals |
| US4064914A (en) * | 1974-05-08 | 1977-12-27 | Union Carbide Corporation | Porous metallic layer and formation |
| JPS5853057B2 (en) * | 1974-05-20 | 1983-11-26 | 株式会社神戸製鋼所 | Highly conductive copper-based alloy |
| JPS53149121A (en) * | 1977-06-01 | 1978-12-26 | Tamagawa Kikai Kinzoku Kk | Flexible pipe made of copperrbased alloy |
| JPS5835249B2 (en) * | 1977-11-30 | 1983-08-01 | 三菱マテリアル株式会社 | Cu alloy for seamless pipe manufacturing |
| JPS5534616A (en) * | 1978-08-29 | 1980-03-11 | Furukawa Electric Co Ltd:The | High tensile copper alloy with high electric conductivity |
| JPS58153747A (en) * | 1982-03-05 | 1983-09-12 | Nippon Denso Co Ltd | Corrosion-resistant copper alloy for heat exchanger fins |
| US4674566A (en) * | 1985-02-14 | 1987-06-23 | Olin Corporation | Corrosion resistant modified Cu-Zn alloy for heat exchanger tubes |
| JPH0688177A (en) * | 1992-09-10 | 1994-03-29 | Kobe Steel Ltd | Production of copper alloy pipe |
| MY115423A (en) * | 1993-05-27 | 2003-06-30 | Kobe Steel Ltd | Corrosion resistant copper alloy tube and fin- tube heat exchanger |
| JP3813317B2 (en) * | 1997-08-12 | 2006-08-23 | 東芝キヤリア株式会社 | Refrigeration cycle equipment |
| JPH11211378A (en) * | 1998-01-23 | 1999-08-06 | Hitachi Cable Ltd | Heat exchanger tubes for heat exchangers |
| JP3303778B2 (en) * | 1998-06-16 | 2002-07-22 | 三菱マテリアル株式会社 | Seamless copper alloy tube for heat exchanger with excellent 0.2% proof stress and fatigue strength |
| US20030066632A1 (en) * | 2001-10-09 | 2003-04-10 | Charles J. Bishop | Corrosion-resistant heat exchanger |
| JP3794341B2 (en) * | 2002-03-28 | 2006-07-05 | 株式会社コベルコ マテリアル銅管 | Internal grooved tube and manufacturing method thereof |
| KR100576141B1 (en) * | 2003-03-03 | 2006-05-03 | 삼보신도고교 가부기키가이샤 | Heat-resistant copper alloy material and its manufacturing method |
| JP4550451B2 (en) * | 2004-03-11 | 2010-09-22 | 古河電気工業株式会社 | Heat exchanger using inner surface grooved heat transfer tube and inner surface grooved heat transfer tube |
| JP4441467B2 (en) * | 2004-12-24 | 2010-03-31 | 株式会社神戸製鋼所 | Copper alloy with bending workability and stress relaxation resistance |
| CN1687684A (en) * | 2005-04-05 | 2005-10-26 | 佛山市顺德区精艺万希铜业有限公司 | Rifled tube and making method thereof |
| CN105779810A (en) * | 2009-11-25 | 2016-07-20 | 诺而达埃斯波公司 | Copper alloys and heat exchanger tubes |
-
2006
- 2006-03-23 DE DE102006013384A patent/DE102006013384B4/en active Active
-
2007
- 2007-03-17 EP EP07711975A patent/EP1996739B1/en active Active
- 2007-03-17 ES ES07711975T patent/ES2370352T3/en active Active
- 2007-03-17 CN CN2007800079346A patent/CN101395289B/en active Active
- 2007-03-17 DK DK07711975.8T patent/DK1996739T3/en active
- 2007-03-17 AT AT07711975T patent/ATE518013T1/en active
- 2007-03-17 WO PCT/EP2007/002379 patent/WO2007110165A1/en not_active Ceased
- 2007-03-17 JP JP2009500752A patent/JP2009530581A/en not_active Withdrawn
- 2007-03-17 US US12/225,514 patent/US20090301701A1/en not_active Abandoned
Also Published As
| Publication number | Publication date |
|---|---|
| CN101395289B (en) | 2011-10-12 |
| ES2370352T3 (en) | 2011-12-14 |
| JP2009530581A (en) | 2009-08-27 |
| DK1996739T3 (en) | 2011-11-21 |
| CN101395289A (en) | 2009-03-25 |
| DE102006013384A1 (en) | 2007-09-27 |
| DE102006013384B4 (en) | 2009-10-22 |
| WO2007110165A1 (en) | 2007-10-04 |
| ATE518013T1 (en) | 2011-08-15 |
| EP1996739A1 (en) | 2008-12-03 |
| US20090301701A1 (en) | 2009-12-10 |
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