US20050129567A1 - Thermostable and corrosion-resistant cast nickel-chromium alloy - Google Patents

Thermostable and corrosion-resistant cast nickel-chromium alloy Download PDF

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Publication number
US20050129567A1
US20050129567A1 US10/945,859 US94585904A US2005129567A1 US 20050129567 A1 US20050129567 A1 US 20050129567A1 US 94585904 A US94585904 A US 94585904A US 2005129567 A1 US2005129567 A1 US 2005129567A1
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Prior art keywords
chromium
nickel
aluminum
alloy
alloys
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Abandoned
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US10/945,859
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English (en)
Inventor
Rolf Kirchheiner
Dietlinde Jakobi
Petra Becker
Ricky Durham
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Schmidt and Clemens GmbH and Co KG
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Schmidt and Clemens GmbH and Co KG
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Priority to US10/945,859 priority Critical patent/US20050129567A1/en
Assigned to SCHMIDT + CLEMENS GMBH + CO. KG reassignment SCHMIDT + CLEMENS GMBH + CO. KG ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: BECKER, PETRA, DURHAM, RICKY, JAKOBI, DIETLINDE, KIRCHHEINER, ROLF
Publication of US20050129567A1 publication Critical patent/US20050129567A1/en
Priority to US12/169,229 priority patent/US10041152B2/en
Priority to US16/055,645 priority patent/US10724121B2/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
    • C22C19/05—Alloys based on nickel or cobalt based on nickel with chromium
    • C22C19/051—Alloys based on nickel or cobalt based on nickel with chromium and Mo or W
    • C22C19/053—Alloys based on nickel or cobalt based on nickel with chromium and Mo or W with the maximum Cr content being at least 30% but less than 40%
    • 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
    • C22C19/05—Alloys based on nickel or cobalt based on nickel with chromium
    • 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
    • C22C19/05—Alloys based on nickel or cobalt based on nickel with chromium
    • C22C19/051—Alloys based on nickel or cobalt based on nickel with chromium and Mo or W
    • C22C19/055—Alloys based on nickel or cobalt based on nickel with chromium and Mo or W with the maximum Cr content being at least 20% but less than 30%
    • 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
    • C22C19/05—Alloys based on nickel or cobalt based on nickel with chromium
    • C22C19/051—Alloys based on nickel or cobalt based on nickel with chromium and Mo or W
    • C22C19/056—Alloys based on nickel or cobalt based on nickel with chromium and Mo or W with the maximum Cr content being at least 10% but less than 20%
    • 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
    • C22C19/05—Alloys based on nickel or cobalt based on nickel with chromium
    • C22C19/058—Alloys based on nickel or cobalt based on nickel with chromium without Mo and W

Definitions

  • the present invention relates to a thermostable and corrosion-resistant cast nickel-chromium alloy.
  • High-temperature processes for example those used in the petrochemical industry, require materials which are not only heat-resistant but also sufficiently corrosion-resistant and in particular are able to withstand the loads imposed by hot product and combustion gases.
  • the tube coils used in cracking and reformer furnaces are externally exposed to strongly oxidizing combustion gases with a temperature of up to 1100° C. and above, whereas a strongly carburizing atmosphere at temperatures of up to 1100° C. prevails in the interior of cracking tubes, and a weakly carburizing, differently oxidizing atmosphere prevails in the interior of reformer tubes at temperatures of up to 900° C. and a high pressure.
  • contact with the hot combustion gases leads to nitriding of the tube material and to the formation of a layer of scale, which is associated with an increase in the external diameter of the tube by a few percent and a reduction in the wall thickness by up to 10%.
  • the carburizing atmosphere inside the tube causes carbon to diffuse into the tube material, where, at temperatures of over 900° C., it leads to the formation of carbides, such as M 23 C 6 , and, with increasing carburization, to the formation of the carbon-rich carbide M 7 C 3 .
  • carbides such as M 23 C 6
  • carburization to the formation of the carbon-rich carbide M 7 C 3 .
  • the consequence of this is internal stresses resulting from the increase in volume associated with the carbide formation or transformation and a decrease in the strength and ductility of the tube material.
  • graphite or dissociation carbon may form in the interior of the tube material, which can, in combination with internal stresses, lead to the formation of cracks, which in turn cause more carbon to diffuse into the tube material.
  • high-temperature processes require materials with a high creep strength or limiting rupture stress, microstructural stability and resistance to carburization and oxidation.
  • This requirement is—within limits—satisfied by alloys which, in addition to iron, contain 20 to 35% of nickel, 20 to 25% of chromium and, to improve the resistance to carburization, up to 1.5% of silicon, such as for example the nickel-chromium steel alloy 35Ni25Cr-1.5Si, which is suitable for centrifugally cast tubes and is still resistant to oxidation and carburization even at temperatures of 1100° C.
  • the high nickel content reduces the diffusion rate and the solubility of the carbon and therefore increases the resistance to carburization.
  • the alloys form a covering layer of Cr 2 O 3 , which acts as a barrier layer preventing the penetration of oxygen and carbon into the tube material beneath it.
  • the Cr 2 O 3 becomes volatile, and consequently the protective action of the covering layer is rapidly lost.
  • the resistance to carburization and oxidation is further put at risk by the limited creep rupture strength and ductility of the conventional nickel-chromium alloys, which lead to the formation of creep cracks in the chromium oxide covering layer and to the penetration of carbon and oxygen into the tube material via the cracks.
  • covering layer cracks may form and also the covering layer may become partially detached.
  • microstructural phase reactions in particular at higher silicon contents, for example of over 2.5%, evidently lead to a loss of ductility and to a reduction in the short-time strength.
  • a nickel-chromium casting alloy having defined aluminum and yttrium contents and comprising up to 0.8% of carbon up to 1% of silicon up to 0.2% of manganese 15 to 40% of chromium 0.5 to 13% of iron 1.5 to 7% of aluminum up to 2.5% of niobium up to 1.5% of titanium 0.01 to 0.4% of zirconium up to 0.06% of nitrogen up to 12% of cobalt up to 5% of molybdenum up to 6% of tungsten 0.01 to 0.1% of yttrium remainder nickel.
  • the total content of nickel, chromium and aluminum combined in the alloy should be from 80 to 90%.
  • the alloy individually or in combination with one another, to contain at most 0.7% of carbon, up to 30% of chromium, up to 12% of iron, 2.2 to 6% of aluminum, 0.1 to 2.0% of niobium, 0.01 to 1.0% of titanium, up to 0.15% of zirconium and—to achieve a high creep rupture strength—up to 10% of cobalt, at least 3% of molybdenum and up to 5% of tungsten, for example 4 to 8% of cobalt, up to 4% of molybdenum and 2 to 4% of tungsten, if the high resistance to oxidation is not the primary factor. Therefore, depending on the loads encountered in the specific circumstances, the cobalt, molybdenum and tungsten contents have to be selected within the content limits specified by the invention.
  • An alloy comprising at most 0.7% of carbon, at most 0.2, more preferably at most 0.1% of silicon, up to 0.2% of manganese, 18 to 30% of chromium, 0.5 to 12% of iron, 2.2 to 5% of aluminum, 0.4 to 1.6% of niobium, 0.01 to 0.6% of titanium, 0.01 to 0.15% of zirconium, at most 0.6% of nitrogen, at most 10% of cobalt, and at most 5% of tungsten, is particularly suitable.
  • the chromium content is at most 26.5%
  • the iron content is at most 11%
  • the aluminum content is from 3 to 6%
  • the titanium content is over 0.15%
  • the zirconium content is over 0.05%
  • the cobalt content is at least 0.2%
  • the tungsten content is over 0.05%
  • the yttrium content is 0.019 to 0.089%.
  • the high creep rupture strength of the alloy according to the invention for example a service life of 2000 hours under a load of from 4 to 6 MPa and a temperature of 1200° C., guarantees that a continuous, securely bonded oxidic barrier layer is retained in the form of an Al 2 O 3 layer which has the effect of preventing carburization and oxidation, results from the high aluminum content of the alloy and continues to top itself up or grow.
  • this layer comprises ⁇ -Al 2 O 3 and contains at most isolated spots of mixed oxides, which do not alter the essential nature of the ⁇ -Al 2 O 3 layer; at higher temperatures, in particular over 1050° C., in view of the rapidly decreasing stability of the Cr 2 O 3 layer of conventional materials at these temperatures, is increasingly responsible for protecting the alloy according to the invention from carburization and oxidation.
  • On the Al 2 O 3 barrier layer there may also—at least in part—be a covering layer of nickel oxide (NiO) and mixed oxides (Ni(Cr,Al) 2 O 4 ), the condition and extent of which, however, is not of great significance, since the Al 2 O 3 barrier layer below is responsible for protecting the alloy from oxidation and carburization. Cracks in the covering layer and the (partial) flaking of the covering layer which occurs at higher temperatures are therefore harmless.
  • the microstructure of the alloy according to the invention On account of its high aluminum content, the microstructure of the alloy according to the invention, at over 4% of aluminum, inevitably contains ⁇ ′ phase, which has a strengthening action at low and medium temperatures but also reduces the ductility or elongation at break. In individual cases, therefore, it may be necessary to reach a compromise between ductility and resistance to oxidation/carburization which is oriented according to the intended use.
  • the barrier layer according to the invention comprising ⁇ -Al 2 O 3 , which is the most stable Al 2 O 3 modification, is able to withstand all oxygen concentrations.
  • FIG. 1 shows a graphical illustration of various alloys, illustrating the elongation limit as a function of the temperature
  • FIG. 2 shows a graphical illustration of the alloys, illustrating the tensile strength as a function of the temperature
  • FIG. 3 shows a graphical illustration of the alloys, illustrating the elongation at break as a function of the temperature
  • FIG. 4 shows a graphical illustration of alloys, illustrating the load as a function of the Larson-Miller parameter/100
  • FIG. 5 shows a graphical illustration of other alloys, illustrating the load as a function of the Larson-Miller parameter/100;
  • FIG. 6 shows a graphical illustration of still other alloys, illustrating the load as a function of the Larson-Miller parameter/100
  • FIG. 7 shows a graphical illustration of comparative tests between alloys according to the invention and standard alloys at a temperature of 1100° C.
  • FIG. 8 shows a graphical illustration of alloys, illustrating the increase in weight as a function of time
  • FIGS. 9 and 10 show graphical illustrations of alloys, illustrating the increase in weight as a function of cycles
  • FIG. 11 shows a graphical illustration of test results of alloys with regard to influence of preliminary oxidation on the carburization behavior
  • FIG. 12 shows a graphical illustration of alloys, illustrating the increase in weight as a function of time between an alloy according to the invention and standard alloys;
  • FIG. 13 shows a graphical illustration of contents of the alloy according to the invention
  • FIG. 14 show a graphical illustration of a comparison between steel alloys according to the invention and alloys.
  • FIGS. 15 and 16 show graphical illustrations of an alloy according to the invention with respect to influence of the aluminum.
  • the table includes, as an example for two wrought alloys which are not covered by the invention and have a comparatively low carbon content and a very fine-grained microstructure with a grain size of ⁇ 10 ⁇ m, comparative alloys 5 and 7, whereas all the other test alloys are casting alloys.
  • Yttrium has a strong oxide-forming action which, in the alloy according to the invention, considerably improves the formation conditions and bonding of the ⁇ -Al 2 O 3 layer.
  • the aluminum content of the alloy according to the invention has an important role in that aluminum leads to the formation of a ⁇ ′ precipitation phase, which significantly increases the tensile strength.
  • the yield strength and the tensile strength of the three alloys according to the invention 13, 19, 20 to 900° C. are well above the corresponding strengths of the four comparative alloys.
  • the elongation at break of the alloys according to the invention substantially correspond to that of the comparative alloys; it increases considerably above approximately 900° C., as can be seen from the diagram presented in FIG. 3 , while the strength reaches the level of the comparative alloys ( FIGS. 1, 2 ). This can be explained by the fact that above approximately 900° C. the ⁇ ′ phase starts to form a solution, and is completely dissolved at above approximately 1000° C.
  • the deterioration in the resistance to carburization at lower aluminum contents can be explained by the fact that the inheritantly protective oxide layer cracks open or (partially) flakes off during cooling after the annealing treatment, so that carburization occurs in the region of the cracks and flaked-off areas.
  • the abovementioned Al 2 O 3 barrier layer is formed beneath the oxide layer (covering layer).
  • the straight line in the diagram shown in FIG. 13 divides the range of alloys with a sufficiently protective ⁇ -aluminum oxide layer above the straight line from the range of alloys with a resistance to carburization or catalytic coking which is adversely affected by mixed oxides.
  • the diagram illustrated in FIG. 14 reveals the superiority of the steel alloy according to the invention using six exemplary embodiments 21 to 26 by comparison with the conventional comparative alloys 1, 3, 4, 6 and 7.
  • the compositions of the comparative alloys 21 to 26 are given in the table.
  • FIGS. 15 and 16 compare the service life of the alloy according to the invention 13, comprising 2.4% of aluminum, as reference variable, with service life 1, in each case at 1100° C. ( FIG. 15 ) and 1200° C. ( FIG. 16 ) for three loading situations (15.9 MPa; 13.5 MPa; 10.5 MPa) with the service lives of the alloys according to the invention 19 (3.3% of aluminum) and 20 (4.8% of aluminum) referenced on the basis of the above reference variable.
  • the diagram shown in FIG. 15 reveals that in the case of alloy 19, with a medium aluminum content of 3.3%, the decrease in the service life becomes more intensive with increasing load, whereas in the case of alloy 20, with its high aluminum content of 4.8%, there is a strong but approximately equal decrease in the relative service life for all the loading situations.
  • the diagram for 1200° C. reveals a reduction in the service life when the aluminum content is increased from 2.4% (alloy 13) to 3.3% (alloy 19) for all three loading situations, with the relative service life dropping by approximately one third.
  • a further increase in the aluminum content to 4.8% (alloy 20) in turn reveals a load-dependent reduction in the relative service life.
  • the two diagrams reveal that as the aluminum content increases, the service life until fracture in the limiting rupture stress test is reduced. Furthermore, as the temperature increases and the duration of loading increases and/or the loading level decreases, the negative influence of the aluminum on the limiting rupture stress life decreases.
  • the alloys with a high aluminum content are particularly suitable for long-term use at temperatures for which it has hitherto been impossible to use cast or centrifugally cast materials.
  • the casting alloy according to the invention is particularly suitable for use as a material for furnace parts, radiant tubes for heating furnaces, rollers for annealing furnaces, parts of continuous-casting and strip-casting installations, hoods and muffles for annealing furnaces, parts of large diesel engines, containers for catalysts and for cracking and reformer tubes.
US10/945,859 2003-01-25 2004-09-21 Thermostable and corrosion-resistant cast nickel-chromium alloy Abandoned US20050129567A1 (en)

Priority Applications (3)

Application Number Priority Date Filing Date Title
US10/945,859 US20050129567A1 (en) 2003-01-25 2004-09-21 Thermostable and corrosion-resistant cast nickel-chromium alloy
US12/169,229 US10041152B2 (en) 2003-01-25 2008-07-08 Thermostable and corrosion-resistant cast nickel-chromium alloy
US16/055,645 US10724121B2 (en) 2003-01-25 2018-08-06 Thermostable and corrosion-resistant cast nickel-chromium alloy

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
DE10302989A DE10302989B4 (de) 2003-01-25 2003-01-25 Verwendung einer Hitze- und korrosionsbeständigen Nickel-Chrom-Stahllegierung
DE10302989.3 2003-01-25
PCT/EP2004/000504 WO2004067788A1 (de) 2003-01-25 2004-01-22 Hitze- und korrosionsbeständige nickel-chrom-grusslegierung
US10/945,859 US20050129567A1 (en) 2003-01-25 2004-09-21 Thermostable and corrosion-resistant cast nickel-chromium alloy

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US12/169,229 Expired - Lifetime US10041152B2 (en) 2003-01-25 2008-07-08 Thermostable and corrosion-resistant cast nickel-chromium alloy
US16/055,645 Expired - Lifetime US10724121B2 (en) 2003-01-25 2018-08-06 Thermostable and corrosion-resistant cast nickel-chromium alloy

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EP (1) EP1501953B8 (ja)
JP (1) JP4607092B2 (ja)
KR (1) KR20050092452A (ja)
CN (1) CN100351412C (ja)
AT (1) ATE362997T1 (ja)
AU (1) AU2004207921A1 (ja)
BR (1) BRPI0406570B1 (ja)
CA (1) CA2513830C (ja)
DE (2) DE10302989B4 (ja)
EA (1) EA008522B1 (ja)
EG (1) EG23864A (ja)
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HK (1) HK1075679A1 (ja)
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MA (1) MA27650A1 (ja)
MX (1) MXPA05007806A (ja)
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PT (1) PT1501953E (ja)
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US20100136368A1 (en) * 2006-08-08 2010-06-03 Huntington Alloys Corporation Welding alloy and articles for use in welding, weldments and method for producing weldments
US20100266865A1 (en) * 2005-06-01 2010-10-21 U Chicago Argonne Llc Nickel based alloys to prevent metal dusting degradation
US20100272597A1 (en) * 2009-04-24 2010-10-28 L. E. Jones Company Nickel based alloy useful for valve seat inserts
CN105463288A (zh) * 2016-01-27 2016-04-06 大连理工大学 高强高塑耐氯离子腐蚀的铸造合金及其制备方法
US9650698B2 (en) 2012-06-05 2017-05-16 Vdm Metals International Gmbh Nickel-chromium alloy having good processability, creep resistance and corrosion resistance
US9657373B2 (en) 2012-06-05 2017-05-23 Vdm Metals International Gmbh Nickel-chromium-aluminum alloy having good processability, creep resistance and corrosion resistance
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US10870908B2 (en) 2014-02-04 2020-12-22 Vdm Metals International Gmbh Hardening nickel-chromium-iron-titanium-aluminium alloy with good wear resistance, creep strength, corrosion resistance and processability
US11098389B2 (en) 2014-02-04 2021-08-24 Vdm Metals International Gmbh Hardened nickel-chromium-titanium-aluminum alloy with good wear resistance, creep resistance, corrosion resistance and workability
US11479836B2 (en) 2021-01-29 2022-10-25 Ut-Battelle, Llc Low-cost, high-strength, cast creep-resistant alumina-forming alloys for heat-exchangers, supercritical CO2 systems and industrial applications
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US10041152B2 (en) 2018-08-07

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