US20040013560A1 - Nickel-based alloy - Google Patents

Nickel-based alloy Download PDF

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Publication number
US20040013560A1
US20040013560A1 US10/448,651 US44865103A US2004013560A1 US 20040013560 A1 US20040013560 A1 US 20040013560A1 US 44865103 A US44865103 A US 44865103A US 2004013560 A1 US2004013560 A1 US 2004013560A1
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United States
Prior art keywords
nickel
alloy
based alloy
content
spark
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Abandoned
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US10/448,651
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English (en)
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Klaus Hrastnik
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Robert Bosch GmbH
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Individual
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Assigned to ROBERT BOSCH GMBH reassignment ROBERT BOSCH GMBH ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: HRASTNIK, KLAUS
Publication of US20040013560A1 publication Critical patent/US20040013560A1/en
Abandoned legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C19/00—Alloys based on nickel or cobalt
    • C22C19/03—Alloys based on nickel or cobalt based on nickel
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01T—SPARK GAPS; OVERVOLTAGE ARRESTERS USING SPARK GAPS; SPARKING PLUGS; CORONA DEVICES; GENERATING IONS TO BE INTRODUCED INTO NON-ENCLOSED GASES
    • H01T13/00—Sparking plugs
    • H01T13/20—Sparking plugs characterised by features of the electrodes or insulation
    • H01T13/39—Selection of materials for electrodes

Definitions

  • the present invention relates to a nickel-based alloy containing silicon, yttrium and aluminum as alloy ingredients.
  • Nickel-based alloys are particularly suitable for producing electrodes for spark plugs in internal combustion engines.
  • spark plugs essentially have a stopper which includes a ceramic, a middle electrode and a terminal pin.
  • a spark plug also has a steel casing having one or more ground electrodes mounted on it. These electrodes are usually made of corrosion-resistant and heat-resistant metals such as nickel, into which a heat-conducting core such as copper may be introduced.
  • the function of the spark plug is defined by the fact that an electric spark which sparks over between the electrodes at a voltage between 15 kV and 30 kV ignites an air-gasoline mixture present in a combustion chamber.
  • the materials i.e., the components
  • the functional parts of the spark plugs such as an electrode which protrudes into a combustion chamber of an internal combustion engine, are exposed to particularly extreme stresses because average operating temperatures between 400° C. and 950° C. occur simultaneously with an alternation between oxidizing and reducing atmospheres.
  • an electrode should have a good thermal conductivity, adequate electric conductivity and a high wear resistance with respect to sulfidation, carburization, reduction and nitration.
  • Other selection criteria for an electrode material include a sufficiently high melting point, good processability and a favorable price of the material.
  • nickel-based alloys, cobalt-based alloys, and iron-based alloys are preferred as electrode materials, and in addition, noble metal pins or noble metal plates are applied to the base electrodes to increase the replacement intervals for spark plugs from the original 30,000 km to 60,000 km to more than 100,000 km, because noble metals and their alloys, in particular platinum, iridium and rhodium, have a very good erosion resistance and corrosion resistance.
  • iron alloys at high temperatures are susceptible to carburization and nitriding.
  • Cobalt alloys have a very good high-temperature corrosion resistance, but because of their low spark erosion resistance they are also less suitable than nickel-based alloys.
  • iron alloys are more difficult to work in comparison with nickel and cobalt alloys, because iron has a body-centered cubic structure.
  • Nickel-based alloys have a good thermal stability and a high corrosion resistance in comparison with iron alloys and cobalt alloys.
  • nickel alloys are easily weldable and processable by cold drawing, which is why nickel-based alloys are particularly suitable as electrode materials in comparison with iron and cobalt alloys.
  • a nickel-based alloy is described in German Patent Application No. 29 36 312 and contains 0.2 wt % to 3 wt % silicon, up to 0.5 wt % manganese, 0.2 wt % to 3 wt % aluminum, 0.01 wt % to 1 wt % yttrium, 0.2 wt % to 3 wt % chromium, the remainder being nickel.
  • the silicon content should preferably be 0.5 wt % to 2.5 wt %
  • the aluminum content should preferably be 0.5 wt % to 2.5 wt %
  • the yttrium content should preferably be 0.1 wt % to 0.5 wt % in order to make the nickel-based alloy more resistant to oxidation and spark erosion when used as an electrode material for spark plugs.
  • the nickel-based alloy contains manganese as an alloy component, because manganese has a negative effect on oxidation stability.
  • the preferred yttrium range between 0.1 wt % and 0.5 wt % results in the formation of intermetallic compounds, i.e., secondary phases such as Ni 17 Y 2 . These phases also have a negative effect on oxidation stability because in particular the occurrence of these secondary phases on the surface of the workpiece results in corrosion or in breakthrough of a protective oxide layer on the surface of the material.
  • a material which has a high oxidation resistance in particular when used as a material for electrodes of spark plugs, is available with the nickel-based alloy containing 1.8 wt % to 2.2 wt % silicon, 0.05 wt % to 0.1 wt % yttrium and/or hafnium and/or zirconium, 2 wt % to 2.4 wt % aluminum and the remainder nickel.
  • the special combination of the proportion ranges of the alloy elements according to the present invention with regard to the change in mass and the depth of oxidation offers some crucial advantages over the combination of broader proportion ranges known from the related art.
  • the low yttrium content in a nickel-based alloy having the alloy amounts according to the present invention results in a good high-temperature oxidation protection which yields a particularly good oxidation resistance of the alloy according to the present invention, particularly in combination with the quantity ranges of aluminum and silicon according to the present invention.
  • Targeted selection of the composition of the nickel-based alloy according to the present invention yields a material which has been characterized in extensive experimental series by an excellent thermal shock behavior and a high oxidation stability, i.e., a low depth of oxidation and a small change in mass, at high stresses.
  • the nickel-based alloy according to the present invention has a good spark erosion resistance and a homogenous structure because the development of secondary phases such as intermetallic compounds such as Ni 17 Y 2 , is reduced or prevented entirely because of the low yttrium content, so the disadvantages of such secondary phases mentioned above advantageously do not occur at all.
  • FIG. 1 shows several curves of the change in weight of nickel-based alloys having different alloy elements and different alloy quantities as a function of time.
  • FIG. 2 shows several curves for the depth of corrosion of nickel-based alloys as a function of temperature from FIG. 1.
  • the nickel-based alloy according to the present invention contains various alloy elements; different alloy components will first be presented below and then their effects on the alloy will be described.
  • Carbon as an alloy constituent of a nickel-based alloy is allowed only as an impurity, i.e., the amount in the nickel-based alloy must be less than 0.05 wt %, because carbon drastically reduces the liquidus temperature of nickel. Carbon also results in formation of carbide, which in turn results in an increase in creep resistance, but greatly reduces the oxidation stability of a nickel-based alloy.
  • Manganese as an alloy component is likewise allowed to be present only as an impurity, i.e., the manganese content in the nickel-based alloy should be less than 0.01 wt %, because manganese has a very negative effect on the oxidation stability of the nickel-based alloy.
  • chromium is vaporized as chromium oxide at use temperatures above approx. 900° C., so that increased vaporization of chromium oxide occurs in particular when subjected to spark-erosion where temperatures up to 2000° C. occur on the electrode surface, and a nickel-based alloy containing chromium as an alloy element has a very poor spark erosion stability.
  • chromium reacts with combustion gases in the combustion chamber to form carbides and nitrides, which increase the creep resistance of a nickel-based alloy but also result in a reduction in its oxidation stability. Therefore, chromium as an alloy component is omitted on the whole in the alloy according to the present invention.
  • the use of aluminum as an alloy component of a nickel-based alloy results in an increase in the oxidation stability, and an increase in the spark erosion stability is also achieved by adding aluminum in particular.
  • An amount of at least 1 wt % is necessary to achieve the desired effects.
  • secondary phases which are formed and deposited as AlNi 3 have a very negative effect on formability and weldability.
  • the strength of nickel-based alloys is increased by adding aluminum.
  • yttrium or other rare earths are added to a nickel-based alloy.
  • the yttrium content should essentially not exceed its solubility in nickel, because if the yttrium content exceeds the solubility limit of yttrium in nickel, intermetallic compounds, i.e., secondary phases such as Ni 17 Y 2 will develop. These secondary phases have a negative effect on the oxidation stability, i.e., the corrosion resistance. When such secondary phases occur at the surface of an electrode, corrosion takes place preferentially or a protective oxide layer on the electrode is broken through.
  • these secondary phases of nickel and yttrium interfere with the production processes of spark plug electrodes such as wire drawing, flow pressing or welding.
  • the secondary phases have a notch effect in the material and thus increase the probability of failure of spark plug electrodes under mechanical loads.
  • hafnium and zirconium may also be added to a nickel-based alloy, and adding these elements to low-alloy nickel materials results in an increase in spark erosion resistance. Furthermore, hafnium and/or zirconium may also be added as alloy components to the nickel-based alloy as alternatives to yttrium.
  • Adding the element cobalt to nickel-based alloys results in improved thermal stability and greater creep strength. Moreover, an improvement in high-temperature corrosion resistance may be achieved by adding cobalt, the amount of cobalt optionally amounting to as much as 5 wt %.
  • a dense oxide layer must be formed on a spark plug electrode to achieve effective oxidation protection.
  • the term “dense oxide layer” is understood to refer to an oxide layer which is formed without pores. Numerous experiments have shown that this is achieved only when the alloy quantity of aluminum and silicon is greater than 7 at %.
  • FIG. 1 shows several curves of the change in weight in grams per square meter over time t in hours at a temperature of 900° C. for various nickel-based alloys; it is apparent that starting from an aluminum and silicon content of 1 wt % each, an increasing amount of aluminum and silicon with a simultaneous reduction in yttrium content, starting from 0.25 wt %, will result in a marked increase in the oxidation stability of a nickel-based alloy.
  • the term “change in weight” as used here is understood to refer to an increase in the mass of a material which results from a reaction between oxygen and the nickel-based alloy at the surface of the material. Because of this reaction, oxidation layers develop at the surface of the nickel-based alloy and remain at the surface when there is an increase in mass. A reduction in the mass of a nickel-based alloy results from the flaking of the developing oxidation layers at higher process temperatures.
  • the addition of aluminum, silicon and yttrium in the ranges proposed according to the present invention results in the oxide layers which develop at the surface of the nickel-based alloy becoming very dense and developing a passivation layer so that diffusion of oxygen into the oxide layer is greatly reduced and the depth of oxidation is kept low.
  • Curve 1 representing a change in mass of a material NiAl1Si1Y 0.25 overtime shows a sharp unwanted increase.
  • Curve 2 of an alloy NiAl1Si1Y 0.12 shows that reducing the yttrium content of a nickel-based alloy from 0.25 wt % to 0.12 wt % is associated with a further reduction in the change in mass.
  • Curve 3 shows a change in mass of an alloy NiAl1.8Si1Y 0.1 over time.
  • a comparison of curves 2 and 3 shows that an increase in aluminum content from 1 wt % to 1.8 wt % results in an improvement in the oxidation stability of a nickel alloy, which is reflected in a reduction in the change in mass.
  • Curve 4 represents the behavior of an alloy NiAl2Cr2Si2Mn 0.2 which also contains chromium and manganese as alloy components in addition to aluminum and silicon. At the beginning, this alloy has a behavior similar to that of alloy NiAl1Si1Y 0.25. With an increase in testing time, curve 4 of the change in mass is similar curve 3 for alloy NiAl1.8Si1Y 0.1.
  • a curve 5 which reflects the change in mass of an alloy NiAl2.4Si1Y 0.1, shows that in comparison with curves 1 , 2 , and 3 , increasing the aluminum content from 1 wt % to 2.4 wt % with a simultaneous reduction in yttrium content to 0.1 wt % results in a considerable improvement in oxidation stability.
  • Curve 6 which represents a change in mass of an alloy NiAl2.2Si2Y 0.1 over time, shows that an increase in silicon content from 1 wt % to 2.2 wt % in comparison with alloy NiAl2.4Si1Y 0.1 of curve 5 and a simultaneous reduction in aluminum content from 2.4 wt % to 2.2 wt % result in a considerable improvement in oxidation stability.
  • FIG. 2 shows curves for the depth of corrosion in micrometers as a function of the temperature in degrees Celsius for a test time of 200 hours for the alloys mentioned in the description of FIG. 1.
  • the curves for the depth of the corrosion of the alloys from FIG. 2 have been labeled with the same reference numbers as the curves in FIG. 1, but for better differentiation, each reference number in FIG. 2 has been supplemented by adding the letter A.
  • the depth of oxidation i.e., the depth of corrosion
  • the depth of corrosion is the distance in an electrode, i.e., in the material of which it is made, from an original metal surface of a component without any surface attack through an oxidized area into the depth of the material to a metal structure which is not oxidized.
  • Curves 1 A through 6 A for the depth of corrosion from FIG. 2 show that an increase in the alloy amounts of aluminum and silicon in a nickel-based alloy with a simultaneous reduction in the yttrium content results in a marked reduction in the depth of corrosion.
  • a comparison of curves 1 A through 6 A shows that alloy NiAl2.2Si2Y 0.1 has the best stability even at the depth of corrosion.
  • a silicon content between 1.8 wt % and 2.2 wt % should also be established at the same time to improve the oxidation stability of a nickel-based alloy. Furthermore, a particularly good oxidation stability of a nickel-based alloy is achieved if an yttrium content in the range of 0.05 wt % to 0.1 wt % is established.
  • a particularly good oxidation stability of a nickel alloy is obtained with an yttrium content of 0.06 wt %, an aluminum content of 2.2 wt % and a silicon content of 2 wt %, the spark erosion stability being equally good in comparison with nickel-based alloys having a higher yttrium content.
  • the sum of all alloy amounts of the alloy elements of a nickel-based alloy should preferably not exceed 5 wt %.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Spark Plugs (AREA)
US10/448,651 2002-06-04 2003-05-29 Nickel-based alloy Abandoned US20040013560A1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE10224891.5 2002-06-04
DE10224891A DE10224891A1 (de) 2002-06-04 2002-06-04 Legierung auf Nickelbasis

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Cited By (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20070159046A1 (en) * 2005-11-16 2007-07-12 Osamu Yoshimoto Spark plug for internal-combustion engines
US20080308057A1 (en) * 2007-06-18 2008-12-18 Lykowski James D Electrode for an Ignition Device
US20090009048A1 (en) * 2007-07-06 2009-01-08 Ngk Spark Plug Co., Ltd. Spark plug
US20100003163A1 (en) * 2006-07-29 2010-01-07 Jutta Kloewer Nickel-Based Alloy
US7825571B2 (en) 2005-01-31 2010-11-02 Ngk Spark Plug Co., Ltd. Spark plug for internal combustion engine
US8784730B2 (en) 2010-06-21 2014-07-22 Outokumpu Vdm Gmbh Nickel-based alloy
US20150017729A1 (en) * 2012-02-02 2015-01-15 Simitomo Electric Industries, Ltd. Method for evaluation testing of material for internal combustion engine
US9184570B2 (en) 2012-08-20 2015-11-10 Denso Corporation Spark plug for internal combustion engine of motor vehicles
US9360051B2 (en) 2013-04-03 2016-06-07 Nidec Gpm Gmbh Shaft bearing with a shaft seal
US9887519B1 (en) * 2016-07-15 2018-02-06 Ngk Spark Plug Co., Ltd. Spark plug
US9932656B2 (en) 2013-03-14 2018-04-03 Vdm Metals International Gmbh Nickel-based alloy with silicon, aluminum, and chromium
CN108220688A (zh) * 2017-11-29 2018-06-29 重庆材料研究院有限公司 高抗核辐射的核场测温用热电偶负极材料及制备方法

Families Citing this family (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP4706441B2 (ja) * 2004-11-04 2011-06-22 日立金属株式会社 点火プラグ用電極材料
JP4699867B2 (ja) * 2004-11-04 2011-06-15 日立金属株式会社 点火プラグ用電極材料
DE102006023374A1 (de) * 2006-05-16 2007-11-22 Beru Ag Legierung auf der Basis von Nickel und deren Verwendung für Zündkerzenelektroden
DE102007040722A1 (de) * 2007-08-29 2009-03-05 Robert Bosch Gmbh Zündkerzenelektrode hergestellt aus verbessertem Elektrodenmaterial
DE102008007605A1 (de) * 2008-02-04 2009-08-06 Uhde Gmbh Modifiziertes Nickel
DE102009046005A1 (de) * 2009-10-26 2011-04-28 Robert Bosch Gmbh Zündkerzenelektrode, hergestellt aus verbessertem Elektrodenmaterial
JP4921540B2 (ja) * 2009-11-26 2012-04-25 日本特殊陶業株式会社 スパークプラグ用の電極材料
EP2698439B1 (de) * 2012-08-17 2014-10-01 Alstom Technology Ltd Oxidationsbeständige Nickellegierung
DE102020211810A1 (de) 2020-09-22 2022-04-14 Robert Bosch Gesellschaft mit beschränkter Haftung Vorkammer-Zündkerze mit einer Kappe aus einem optimierten Material
DE102020211897A1 (de) 2020-09-23 2022-03-24 Robert Bosch Gesellschaft mit beschränkter Haftung Zündkerzenelektrode sowie Zündkerze mit der Zündkerzenelektrode und Herstellungsverfahren für die Zündkerzenelektrode
JP7429725B2 (ja) 2022-02-18 2024-02-08 日本特殊陶業株式会社 スパークプラグ用主体金具およびスパークプラグ

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US4329174A (en) * 1978-09-07 1982-05-11 Ngk Spark Plug Co., Ltd. Nickel alloy for spark plug electrodes
US4388125A (en) * 1981-01-13 1983-06-14 The International Nickel Company, Inc. Carburization resistant high temperature alloy
US4764225A (en) * 1979-05-29 1988-08-16 Howmet Corporation Alloys for high temperature applications
US5204059A (en) * 1988-07-25 1993-04-20 Mitsubishi Metal Corporation Ni base alloy for spark plug electrodes of internal combustion engines
US6387193B1 (en) * 1998-11-24 2002-05-14 General Electric Company Repair material, process of repairing using the repair material, and article repaired
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US3874938A (en) * 1971-04-06 1975-04-01 Int Nickel Co Hot working of dispersion-strengthened heat resistant alloys and the product thereof
US3794530A (en) * 1971-10-13 1974-02-26 Elect & Magn Alloys Res Inst High-permeability ni-fe-ta alloy for magnetic recording-reproducing heads
US4019900A (en) * 1976-04-01 1977-04-26 Olin Corporation High strength oxidation resistant nickel base alloys
US4329174A (en) * 1978-09-07 1982-05-11 Ngk Spark Plug Co., Ltd. Nickel alloy for spark plug electrodes
US4764225A (en) * 1979-05-29 1988-08-16 Howmet Corporation Alloys for high temperature applications
US4388125A (en) * 1981-01-13 1983-06-14 The International Nickel Company, Inc. Carburization resistant high temperature alloy
US5204059A (en) * 1988-07-25 1993-04-20 Mitsubishi Metal Corporation Ni base alloy for spark plug electrodes of internal combustion engines
US6387193B1 (en) * 1998-11-24 2002-05-14 General Electric Company Repair material, process of repairing using the repair material, and article repaired
US6458318B1 (en) * 1999-06-30 2002-10-01 Sumitomo Metal Industries, Ltd. Heat resistant nickel base alloy

Cited By (17)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8288928B2 (en) 2005-01-31 2012-10-16 Ngk Spark Plug Co., Ltd. Spark plug for internal combustion engine
US20110012500A1 (en) * 2005-01-31 2011-01-20 Ngk Spark Plug Co., Ltd. Spark plug for internal combustion engine
US7825571B2 (en) 2005-01-31 2010-11-02 Ngk Spark Plug Co., Ltd. Spark plug for internal combustion engine
US7859177B2 (en) * 2005-11-16 2010-12-28 Ngk Spark Plug Co., Ltd. Spark plug for internal-combustion engines
US20070159046A1 (en) * 2005-11-16 2007-07-12 Osamu Yoshimoto Spark plug for internal-combustion engines
US20100003163A1 (en) * 2006-07-29 2010-01-07 Jutta Kloewer Nickel-Based Alloy
US20080308057A1 (en) * 2007-06-18 2008-12-18 Lykowski James D Electrode for an Ignition Device
US8164242B2 (en) * 2007-07-06 2012-04-24 Ngk Spark Plug Co., Ltd. Spark plug
EP2012398A3 (de) * 2007-07-06 2012-12-05 NGK Spark Plug Co., Ltd. Zündkerze
US20090009048A1 (en) * 2007-07-06 2009-01-08 Ngk Spark Plug Co., Ltd. Spark plug
US8784730B2 (en) 2010-06-21 2014-07-22 Outokumpu Vdm Gmbh Nickel-based alloy
US20150017729A1 (en) * 2012-02-02 2015-01-15 Simitomo Electric Industries, Ltd. Method for evaluation testing of material for internal combustion engine
US9184570B2 (en) 2012-08-20 2015-11-10 Denso Corporation Spark plug for internal combustion engine of motor vehicles
US9932656B2 (en) 2013-03-14 2018-04-03 Vdm Metals International Gmbh Nickel-based alloy with silicon, aluminum, and chromium
US9360051B2 (en) 2013-04-03 2016-06-07 Nidec Gpm Gmbh Shaft bearing with a shaft seal
US9887519B1 (en) * 2016-07-15 2018-02-06 Ngk Spark Plug Co., Ltd. Spark plug
CN108220688A (zh) * 2017-11-29 2018-06-29 重庆材料研究院有限公司 高抗核辐射的核场测温用热电偶负极材料及制备方法

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JP2004011024A (ja) 2004-01-15

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