US3852063A - Heat resistant, anti-corrosive alloys for high temperature service - Google Patents

Heat resistant, anti-corrosive alloys for high temperature service Download PDF

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US3852063A
US3852063A US00294981A US29498172A US3852063A US 3852063 A US3852063 A US 3852063A US 00294981 A US00294981 A US 00294981A US 29498172 A US29498172 A US 29498172A US 3852063 A US3852063 A US 3852063A
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percent
alloy
weight
alloys
high temperature
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I Niimi
Y Kaneko
Y Katori
M Noguchi
T Uchida
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Toyota Motor Corp
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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C38/00—Ferrous alloys, e.g. steel alloys
    • C22C38/18—Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/32—Ferrous alloys, e.g. steel alloys containing chromium with boron
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C38/00—Ferrous alloys, e.g. steel alloys
    • C22C38/18—Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/22—Ferrous alloys, e.g. steel alloys containing chromium with molybdenum or tungsten
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C38/00—Ferrous alloys, e.g. steel alloys
    • C22C38/18—Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/24—Ferrous alloys, e.g. steel alloys containing chromium with vanadium

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  • ABSTRACT The present invention relates to a heat resistant anticorrosive alloy characterized by good resistance to corrosion at high temperatures and high strength at high temperatures which is suitable as material for recombustion-type emission gas purifiers such as thermal reactors, after-burners, more specifically to a metal alloy substantially composed of ferrite phase, its major components being:
  • Fe-Cr-Al alloys conventionally employed in furnace heaters or various heat-resistant stainless alloys are conceivable.
  • the conventional Fe-Cr-Al alloys excel in high temperature corrosion resistance, but they have the drawbacks that they are liable to become brittle in high temperature service through coarsening of crystals and they lack high temperature strength.
  • austenitic stainless alloys and nickel base heat-resistant alloys characterized by excellence high temperature strength, lack in high temperature corrosion resistance and accordingly they need surface treatment; or they are so expensive that they are found unfit for mass production.
  • the present inventors setting an eye on the excellence of Fe-Cr-Al alloys in their high temperature corrosion resistance, investigated how to improve these alloys in the coarsening of their crystals and consequently from their investigation have successfully perfected the present invention of an alloy with remarkably better characteristics of high temperature corrosion resistance than that of the conventional austenitic stainless alloy or nickel base heat-resistant alloy, and better characteristics of high temperature strength, crystal coarsening and moldability than those of the conventional Fe-Cr-Al alloys.
  • the object of the present invention is to provide an alloy suitable as material for component members of a re-combustion-type emission gas purifier which is characterized by excellence in high temperature corrosion resistance, high temperature strength, crystal coarsening characteristics and moldability, the major alloying elements to constitute this alloy to attain this object bemg:
  • FIG. 1 is a diagram showing the results of comparison in anti-oxidization characteristics between the invented alloy and various conventional heat-resistant anticorrosive alloys
  • FIG. 2 is a diagram showing the results of comparison in corrosion resistance in a hot atmosphere of lead oxide between the invented alloy and various conventional heat-resistant anti-corrosive alloys,
  • FIG. 3 is a diagram showing the results of comparison in corrosion resistance in a hot atmosphere of sulphur between the invented alloy and various conventional heat-resistant anti-corrosive alloys,
  • FIG. 4 is a micrograph showing an intercrystalline corrosion recognized in an austenitic alloy (SUS 41) which has been etched by hot sulphur,
  • FIG. 5 schematically illustrates a specimen used in a Charpy test of the invented alloy.
  • the present invention relates to an alloy characterized by excellence in high temperature oxidation resistance, high temperature corrosion resistance in an at mosphere of lead oxide or sulphur and high temperature strength which can be applied as material for heatresistant members in various re-combustion-type emission gas purifiers and for vessels in a catalyst muffler, for engine parts exposed to hot emission gases, for components of gas turbinecombustion chambers and for furnace heaters.
  • the invention alloy is substantially constituted by a ferrite phase, its chemical composition being broadly as follows carbon below 0.15% silicon below 2.0% chrome l228% aluminum 03-60% molybdenum 0.23.0% vanadium 0.l-3.0%
  • niobium and tantalum ODS-3.0% boron 0.000l0.0050% titanium ODS-1.0% zirconium 0.01-1 .0%.
  • Addition of Y greatly improves the impact withstanding characteristics. Addition of Cr, A1, Y is effective for improving the anti-oxidation, anti-lead oxide, and anti-sulphur characteristics, but excessive addition of B is harmful.
  • N0'rE. 1 ⁇ Iark means that the relevant characteristic has been vastly improved.
  • O means that the ellt-et, though nnl ennspicuous, is positive. [1 means that the l-tluct is insignificant or practically Zero.
  • A means that. the elleet 15 rather negative.
  • X means that the effect is markedly negative.
  • Table 2 is a list of chemical compositions of speci- 1n FIGS. l-3 and Table 3, the characteristics of the.
  • FIG. 1 shows the etched depths of various alloys as measured after being submitted to 200 hours of oxida-' tion in an alumina boat in an atmospheric furnace pr'eliminarily heated to 1,200C; these .depths' represent the high temperature oxidation characteristic of these alloys. It is evident from FIG. 1 that some of the commercial heat-resistant stainless alloys, for instance, the specimens (g) (h) exhibit considerably good antioxidation characteristic, but even compared with them, the invented alloy as well as the known Fe-Cr-Al alloys is far superior in this characteristic.
  • FIG. 2 shows the etched depths of various alloys which represent their corrosion resistance in a hot atmosphere of P O, as measured after these alloys had been washed, degreased, coated with a slurry mixture of Pb 0 powder and waterglass solution(water: water glass 4:1 in volume ratio of 1:3; placed in an alumina boat; and then held for hours in a furnace preliminarily heated to 1200C.
  • FIG. 3 shows the etched depths of the specimens which represent their corrosion resistance in a hot atmosphere of sulphur, as measured after the specimens were coated with a slurry'mixture of powder sulphur and waterglass solution (water: waterglass 1:1) in volume ratio of 1:3; placed in an alumina boat; and held for 6 hours in a furnace preliminarily heated to 1,200C.
  • Table 3 summarizes the characteristics of the conventional Fe-Cr-Al alloys and the invented Fe-Cr-Al alloy, such as strength at room temperature and at high temperature; elongation at room temperature; impact strength; and crystal coarsening.
  • the invented alloys (A)(H) are remarkably better in high temperature strength characteristic than any Fe-Cr-Al alloy in the prior art; particularly the alloy (H) is about two times superior to any one of the conventional (j), (q), (t), (w) and (i).
  • the contents of Cr, Al and particularly that of A1 are supposed to made great contributions; in this characteristic, the invented alloys are generally superior to the known (i), (j), (q), (t) and (w). This is, as suggested by the performances of the tentative alloys (r), (n), (o), (s), presumably due to the addition of Ta being small and those of B, Si and V being well controlled.
  • the impact strength mentioned in the Table is ex pressed by the energy absorption needed to break a specimen of a special shape indicated in FIG. 5, using a kg-m small size Charpy impact tester, as divided by the original cross-sectional area of the specimen.
  • the crystal coarsening characteristic in Table 3 is expressed in terms of temperatures at which the ferrite crystal size becomes less than 1 when each alloy specimen has been held for 25 hours in the range of 800-l,200C at intervals of 50C and then observed for coarsening of crystals as the results of heating.
  • An increase in the contents of Cr and Al is apt to be accompanied by a slight rise in the coarsening tempera- TABLE 3
  • Comparison of various properties among different Fe-Cr-Al alloys (known, tentative and invented) Room temperature elongation High temperature tensile strength Kg/mm lmpact Strength Specimen Kglmlcol codes Crystal coarsening temperature (C) service as a thermal reactor, the invented alloy receives less thermal strain due to heating and cooling and accordingly suffers less thermal fatigue.
  • Carbon as a solid solution constitutes a part of the alloy and strengthens it.
  • it forms carbides, which contribute to the strengthening of the alloy, but its content should be limited to less than 0.15 percent, because too much carbon is likely to cause intercrystalline and intracrystalline precipitations of carbides (or nitrides) heated in the process, after permeating the carbon into the texture in the form of a solid solution; and thus, corrosion resistance is reduced through lack of Cr in the vicinity of the precipitates and with this, the moldability too becomes poor.
  • Si is effective for improving anti-oxidation, antisulphur and anti-PbO characteristics, but Si not as effective as Cr or Al. Meanwhile Si is likely to cause heavy deterioration in the moldability at room temperature and impact strength if used in large quantities. Thus, it is advisable to limit its content to less than 2 percent.
  • its content should be more than 12 percent, but should not exceed 28 percent, because its excess deteriorates the moldability or weldability and is likely to cause 475C brittleness and cr-phase precipitation.
  • Mo partly as a solid solution in the texture and partly as a carbide, is found useful for strengthening the alloy and preventing the coarsening of its crystals.
  • V similarly to M0, serves to strengthen the alloy partly through, its effect as a solid solution in the texture and partly through its effect as a carbide. Too much V,
  • the recommendable content of V should be 0.12.0 percent.
  • Ta when added to Fe-Cr-Al alloys, behaves uniquely; thereby a small amount of Ta can improve the high temperature strength, the crystal-coarsening characteristic and the room temperature elongation; but its excessive addition will heavily reduce the impact strength of the alloy.
  • the right addition of Ta should be 0.05-3.0 percent.
  • the effect of Nb is nearly the same as that of Ta. Besides, it would be so difficult to make separate use of Nb and Ta that a part of Ta addition might be substituted by Nb.
  • Y as a very small addition can improve the bonding of a protective film at high temperature heating and vastly enhance the high temperature anti-oxidation and anti-Pb characteristics.
  • Fe-Cr-Al alloys when they contain relatively low amounts of Cr and Al (Cr Al 3% they develop local and accelerated corrosion due to imperfectness of the protective film of d-Al O which should bring about a high corrosion resistance at high temperatures, in the case of the invented alloy with a Y-content, this film can be compact and can adhere well to the base metal, thereby compensating for the imperfectness of the film and exhibiting an excellent characteristic of high temperature corrosion resistance.
  • Y is an expensive metal; its addition exceeding 1.5 percent will not be so effective as might be expected and thus, 0.01-1.5 percent will be the limits of its addition.
  • rare earth elements other than Y i.e., Ce, La, Ca are practically as effective as Y and accordingly, a partial or whole addition of Y may be substituted by rare earth elements such as Ce, La, Ca.
  • Ti is an elementwhich is added to the conventional Fe-Cr-Al alloys, too;-it is foundeffective through formation of TiC for, fixation of solid-solution carbon or prevention of crystal coarsening. Since too much Ti is likely to deteriorate the anti-oxidation characteristic and impact strength of the alloy, it has been limited to 005-1 .0 percent.
  • Zr just like Ti, is an element added to the conventional Fe-Cr-Al alloys, too.
  • its addition should be more than 0.01 percent, but it is an expensive metal; moreover, its excessive addition is likely to result in poor elongation at room temperature and lower impact strength.
  • its appropriate addition should be from 0.011.0 percent.
  • Be is also known as an element which as a verysmall addition can vastly enhance the high temperature strength and can serve to prevent the coarsening of crystals. Accordingly, it constitutes one of the essential elements for the invented alloy, but it is extremely costly; besides, too much Be will deteriorate the room temperature elongation and the impact strength. Thus, the optimum addition of it should be 0.01-2.0 percent.
  • a heat-resistant, anti-corrosive alloy for high tem-' perature service said alloy consisting essentially of:
  • yttrium in an amount less than 1.5 percent by weight, beryllium in an amount less than 2.0 percent by weight, and boron in an amount less than 0.0050% by weight; and the balance of iron and inevitable impurities.
  • yttrium is present in an amount in the range of 0.03-0.4 percent by weight.

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US00294981A 1971-10-04 1972-10-04 Heat resistant, anti-corrosive alloys for high temperature service Expired - Lifetime US3852063A (en)

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Cited By (29)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3978193A (en) * 1974-01-29 1976-08-31 Gould Inc. Method and apparatus for treating exhaust gases
US4010049A (en) * 1975-10-06 1977-03-01 Jones & Laughlin Steel Corporation Columbium-stabilized high chromium ferritic stainless steels containing zirconium
US4055416A (en) * 1976-01-21 1977-10-25 The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration Tantalum modified ferritic iron base alloys
US4059440A (en) * 1975-02-01 1977-11-22 Nippon Steel Corporation Highly corrosion resistant ferritic stainless steel
US4065330A (en) * 1974-09-26 1977-12-27 The Foundation: The Research Institute Of Electric And Magnetic Alloys Wear-resistant high-permeability alloy
US4075010A (en) * 1976-02-05 1978-02-21 The International Nickel Company, Inc. Dispersion strengthened ferritic alloy for use in liquid-metal fast breeder reactors (LMFBRS)
US4140526A (en) * 1976-11-12 1979-02-20 Sumitomo Metal Industries, Ltd. Ferritic stainless steel having improved weldability and oxidation resistance
US4230489A (en) * 1978-04-28 1980-10-28 United Kingdom Atomic Energy Authority Alloys of Fe, Cr, Si, Y and Al
US4252561A (en) * 1976-09-21 1981-02-24 Showa Denko Kabushiki Kaisha Chromium-alloyed steel which is corrosion resistant to caustic alkaline solution
US4286986A (en) * 1979-08-01 1981-09-01 Allegheny Ludlum Steel Corporation Ferritic stainless steel and processing therefor
US4316743A (en) * 1973-10-29 1982-02-23 Tokyo Shibaura Electric Co., Ltd. High damping Fe-Cr-Al alloy
US4340424A (en) * 1974-04-23 1982-07-20 Daido Tokushuko Kabushiki Kaisha Ferritic stainless steel having excellent machinability and local corrosion resistance
US4398951A (en) * 1981-04-22 1983-08-16 Unisearch Limited Fermalloy(Fe-Mn-Al stainless steel)
US4459043A (en) * 1980-11-14 1984-07-10 Smiths Industries Public Limited Company Reflective elements and sensors including reflective elements
US4556423A (en) * 1982-01-08 1985-12-03 Nippon Kokan Kabushiki Kaisha Austenite stainless steels having excellent high temperature strength
US4668585A (en) * 1984-06-08 1987-05-26 Osaka Prefecture, Horonobu Oonishi and Kyocera Corporation Fe-Cr-Al type implant alloy composite for medical treatment
US4735771A (en) * 1986-12-03 1988-04-05 Chrysler Motors Corporation Method of preparing oxidation resistant iron base alloy compositions
US4891183A (en) * 1986-12-03 1990-01-02 Chrysler Motors Corporation Method of preparing alloy compositions
US4904540A (en) * 1986-04-21 1990-02-27 Kawasaki Steel Corp. Fe-Cr-Al stainless steel having high oxidation resistance and spalling resistance and Fe-Cr-Al steel for catalyst substrate of catalytic converter
US4999158A (en) * 1986-12-03 1991-03-12 Chrysler Corporation Oxidation resistant iron base alloy compositions
EP0492674A1 (en) * 1990-12-28 1992-07-01 Toyota Jidosha Kabushiki Kaisha Ferritic heat-resisting cast steel and a process for making the same
US5190722A (en) * 1990-12-28 1993-03-02 Tohoku Special Steel Works Limited High cold-forging electromagnetic stainless steel
EP0646657A4 (en) * 1993-03-19 1995-07-05 Nippon Yakin Kogyo Co Ltd STAINLESS, FERRITIC STEEL WITH RROUGHING OXIDATION RESISTANCE.
EP0735153A1 (fr) * 1995-03-29 1996-10-02 USINOR SACILOR Société Anonyme Acier inoxydable ferritique, utilisable notamment pour des supports de catalyseurs
CN1038051C (zh) * 1993-11-08 1998-04-15 亚瑞亚·勃朗勃威力有限公司 铁铝合金及其用途
US20030175174A1 (en) * 2002-03-13 2003-09-18 Siegfried Schneider Device for the continuous burning of carbon particles
WO2005100628A1 (en) * 2004-04-16 2005-10-27 Sandvik Intellectual Property Ab Ferritic stainless steel
US20150360198A1 (en) * 2005-11-01 2015-12-17 Asahi Kasei Chemicals Corporation Processes for production of isobutene and tertiary butanol
CN115896645A (zh) * 2022-11-22 2023-04-04 上海核工程研究设计院股份有限公司 一种核能用含铍铁素体不锈钢及其制备方法

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS607699B2 (ja) * 1981-03-31 1985-02-26 住友金属工業株式会社 高温での耐変色性にすぐれたフエライトステンレス鋼

Citations (4)

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US2750283A (en) * 1953-05-27 1956-06-12 Armco Steel Corp Stainless steels containing boron
US2985529A (en) * 1958-08-27 1961-05-23 Birmingham Small Arms Co Ltd Creep resistant non-austenitic steels
US3027252A (en) * 1959-09-29 1962-03-27 Gen Electric Oxidation resistant iron-chromium alloy
US3759705A (en) * 1971-06-10 1973-09-18 Armco Steel Corp Chromium containing alloy steel and articles

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2750283A (en) * 1953-05-27 1956-06-12 Armco Steel Corp Stainless steels containing boron
US2985529A (en) * 1958-08-27 1961-05-23 Birmingham Small Arms Co Ltd Creep resistant non-austenitic steels
US3027252A (en) * 1959-09-29 1962-03-27 Gen Electric Oxidation resistant iron-chromium alloy
US3759705A (en) * 1971-06-10 1973-09-18 Armco Steel Corp Chromium containing alloy steel and articles

Cited By (38)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4316743A (en) * 1973-10-29 1982-02-23 Tokyo Shibaura Electric Co., Ltd. High damping Fe-Cr-Al alloy
US3978193A (en) * 1974-01-29 1976-08-31 Gould Inc. Method and apparatus for treating exhaust gases
US4340424A (en) * 1974-04-23 1982-07-20 Daido Tokushuko Kabushiki Kaisha Ferritic stainless steel having excellent machinability and local corrosion resistance
US4065330A (en) * 1974-09-26 1977-12-27 The Foundation: The Research Institute Of Electric And Magnetic Alloys Wear-resistant high-permeability alloy
US4059440A (en) * 1975-02-01 1977-11-22 Nippon Steel Corporation Highly corrosion resistant ferritic stainless steel
US4010049A (en) * 1975-10-06 1977-03-01 Jones & Laughlin Steel Corporation Columbium-stabilized high chromium ferritic stainless steels containing zirconium
US4055416A (en) * 1976-01-21 1977-10-25 The United States Of America As Represented By The Administrator Of The National Aeronautics And Space Administration Tantalum modified ferritic iron base alloys
US4075010A (en) * 1976-02-05 1978-02-21 The International Nickel Company, Inc. Dispersion strengthened ferritic alloy for use in liquid-metal fast breeder reactors (LMFBRS)
US4252561A (en) * 1976-09-21 1981-02-24 Showa Denko Kabushiki Kaisha Chromium-alloyed steel which is corrosion resistant to caustic alkaline solution
US4140526A (en) * 1976-11-12 1979-02-20 Sumitomo Metal Industries, Ltd. Ferritic stainless steel having improved weldability and oxidation resistance
US4230489A (en) * 1978-04-28 1980-10-28 United Kingdom Atomic Energy Authority Alloys of Fe, Cr, Si, Y and Al
US4286986A (en) * 1979-08-01 1981-09-01 Allegheny Ludlum Steel Corporation Ferritic stainless steel and processing therefor
US4459043A (en) * 1980-11-14 1984-07-10 Smiths Industries Public Limited Company Reflective elements and sensors including reflective elements
US4398951A (en) * 1981-04-22 1983-08-16 Unisearch Limited Fermalloy(Fe-Mn-Al stainless steel)
US4556423A (en) * 1982-01-08 1985-12-03 Nippon Kokan Kabushiki Kaisha Austenite stainless steels having excellent high temperature strength
US4668585A (en) * 1984-06-08 1987-05-26 Osaka Prefecture, Horonobu Oonishi and Kyocera Corporation Fe-Cr-Al type implant alloy composite for medical treatment
US4904540A (en) * 1986-04-21 1990-02-27 Kawasaki Steel Corp. Fe-Cr-Al stainless steel having high oxidation resistance and spalling resistance and Fe-Cr-Al steel for catalyst substrate of catalytic converter
US4891183A (en) * 1986-12-03 1990-01-02 Chrysler Motors Corporation Method of preparing alloy compositions
US4735771A (en) * 1986-12-03 1988-04-05 Chrysler Motors Corporation Method of preparing oxidation resistant iron base alloy compositions
US4999158A (en) * 1986-12-03 1991-03-12 Chrysler Corporation Oxidation resistant iron base alloy compositions
WO1989009841A1 (en) * 1986-12-03 1989-10-19 Chrysler Motors Corporation Method of preparing oxidation resistant iron base alloy compositions
EP0492674A1 (en) * 1990-12-28 1992-07-01 Toyota Jidosha Kabushiki Kaisha Ferritic heat-resisting cast steel and a process for making the same
US5190722A (en) * 1990-12-28 1993-03-02 Tohoku Special Steel Works Limited High cold-forging electromagnetic stainless steel
EP0646657A4 (en) * 1993-03-19 1995-07-05 Nippon Yakin Kogyo Co Ltd STAINLESS, FERRITIC STEEL WITH RROUGHING OXIDATION RESISTANCE.
US5480608A (en) * 1993-03-19 1996-01-02 Nippon Yakin Kogyo Co., Ltd. Ferritic stainless steel having an excellent oxidation resistance
CN1038051C (zh) * 1993-11-08 1998-04-15 亚瑞亚·勃朗勃威力有限公司 铁铝合金及其用途
US5866065A (en) * 1995-03-29 1999-02-02 Usinor Sacilor Ferritic stainless steel of use in particular for catalyst supports
FR2732360A1 (fr) * 1995-03-29 1996-10-04 Ugine Savoie Sa Acier inoxydable ferritique utilisable, notamment pour des supports de catalyseurs
EP0735153A1 (fr) * 1995-03-29 1996-10-02 USINOR SACILOR Société Anonyme Acier inoxydable ferritique, utilisable notamment pour des supports de catalyseurs
US20030175174A1 (en) * 2002-03-13 2003-09-18 Siegfried Schneider Device for the continuous burning of carbon particles
EP1346769A1 (en) * 2002-03-13 2003-09-24 Capital Technology S.A. Device for the continuous burning of carbon particles
US7214350B2 (en) 2002-03-13 2007-05-08 Capital Technology, S.A. Device for the continuous burning of carbon particles
WO2005100628A1 (en) * 2004-04-16 2005-10-27 Sandvik Intellectual Property Ab Ferritic stainless steel
US20070292300A1 (en) * 2004-04-16 2007-12-20 Andreas Rosberg Ferritic Stainless Steel
US20150360198A1 (en) * 2005-11-01 2015-12-17 Asahi Kasei Chemicals Corporation Processes for production of isobutene and tertiary butanol
US9919283B2 (en) * 2005-11-01 2018-03-20 Asahi Kasei Chemicals Corporation Processes for production of isobutene and tertiary butanol
CN115896645A (zh) * 2022-11-22 2023-04-04 上海核工程研究设计院股份有限公司 一种核能用含铍铁素体不锈钢及其制备方法
CN115896645B (zh) * 2022-11-22 2024-05-31 上海核工程研究设计院股份有限公司 一种核能用含铍铁素体不锈钢及其制备方法

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