EP1941070B1 - Austenitic stainless steel - Google Patents

Austenitic stainless steel Download PDF

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Publication number
EP1941070B1
EP1941070B1 EP06851605.3A EP06851605A EP1941070B1 EP 1941070 B1 EP1941070 B1 EP 1941070B1 EP 06851605 A EP06851605 A EP 06851605A EP 1941070 B1 EP1941070 B1 EP 1941070B1
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Prior art keywords
manganese
article
manufacture
high temperature
austenitic stainless
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EP06851605.3A
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German (de)
English (en)
French (fr)
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EP1941070A2 (en
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James M. Rakowski
Charles P. Stinner
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ATI Properties LLC
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ATI Properties LLC
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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
    • C22C38/40—Ferrous alloys, e.g. steel alloys containing chromium with nickel
    • 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
    • C22C38/001—Ferrous alloys, e.g. steel alloys containing N
    • C—CHEMISTRY; METALLURGY
    • C21—METALLURGY OF IRON
    • C21D—MODIFYING THE PHYSICAL STRUCTURE OF FERROUS METALS; GENERAL DEVICES FOR HEAT TREATMENT OF FERROUS OR NON-FERROUS METALS OR ALLOYS; MAKING METAL MALLEABLE, e.g. BY DECARBURISATION OR TEMPERING
    • C21D6/00—Heat treatment of ferrous alloys
    • C21D6/004—Heat treatment of ferrous alloys containing Cr and Ni
    • 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
    • C22C38/02—Ferrous alloys, e.g. steel alloys containing silicon
    • 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
    • C22C38/40—Ferrous alloys, e.g. steel alloys containing chromium with nickel
    • C22C38/44—Ferrous alloys, e.g. steel alloys containing chromium with nickel 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
    • C22C38/40—Ferrous alloys, e.g. steel alloys containing chromium with nickel
    • C22C38/48—Ferrous alloys, e.g. steel alloys containing chromium with nickel with niobium or tantalum
    • 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
    • C22C38/40—Ferrous alloys, e.g. steel alloys containing chromium with nickel
    • C22C38/58—Ferrous alloys, e.g. steel alloys containing chromium with nickel with more than 1.5% by weight of manganese

Definitions

  • the present disclosure relates to austenitic stainless steels. More specifically, the present disclosure relates to austenitic stainless steels having improved creep resistance and/or improved corrosion resistance when subjected to high temperature environments.
  • austenitic stainless steels include various combinations of chromium, nickel, manganese, and other alloying additions. Nevertheless, stainless steels and certain other chromium-bearing heat-resistant alloys are susceptible to attack in high temperature air and in high temperature air containing water vapor. This attack takes two distinct forms. Low-alloy content stainless steels such as, for example, AISI Type 304 (nominally 18 weight percent chromium and 8 weight percent nickel, balance iron), suffer from accelerated oxidation in the presence of water vapor. The slow-growing chromium oxide film is displaced by a thick scale comprised of rapidly growing mixed iron and chromium oxides. The result is rapid metal wastage by conversion to oxide.
  • AISI Type 304 nominally 18 weight percent chromium and 8 weight percent nickel, balance iron
  • High-alloy content materials such as, for example, superferritic iron-chromium stainless steels and nickel-chromium superalloys, appear to be immune to this form of attack, but have been observed to suffer from weight loss during exposure to water vapor.
  • the oxide that forms on certain of the high-alloy content materials is very pure chromium oxide and is susceptible to evaporation through the formation of volatile chromium oxyhydroxides.
  • the result of this evaporative loss of chromium to the atmosphere is an abnormally high level of chromium depletion in the metal substrate, and this can lead to a loss of high temperature oxidation resistance.
  • the transition between the foregoing corrosion states is relatively complex, with aspects of both states noted in some alloys.
  • creep is the undesirable plastic deformation of alloys held for long periods of time at stresses lower than the normal yield strength.
  • creep may affect certain structural parts and other parts subject to high stresses and high temperatures in, for example, energy generation devices and related devices, and in equipment and parts for high temperature processing, treating, or extracting chemicals or minerals, or for high temperature treating or processing alloys.
  • it is often desirable that parts are formed from a material that has substantial resistance to corrosion in high temperature environments, and that also has substantial creep resistance.
  • the alloying element manganese has been shown play a role in mitigating the effects of chromium oxide vaporization.
  • Many stainless steel specifications include manganese at levels limited to 2 weight percent or less, with no required minimum level. The manganese in these steels is not an intentional alloying addition but, instead, is included in the steel as an incidental ingredient derived from the scrap starting materials.
  • One austenitic stainless steel adapted for use in high temperature, high water vapor content environments that includes an appreciable allowance for incidental manganese is NF709 alloy.
  • NF709 alloy has been available from Nippon Steel Corporation in forms including of seamless tubing for boiler applications.
  • NF709 alloy which is provided in the Nippon Steel publication "Quality and Properties of NF709 Austenitic Stainless Steel for Boiler Tubing Applications ,” is shown in Table 1.
  • the published composition specifies a manganese limit of 1.5 weight percent, with no specified minimum. According to various published accounts of research on this alloy, the typical commercial manganese content is approximately 1 weight percent.
  • Certain other austenitic stainless steels are also shown in Table 1. Elemental concentrations throughout the present description are weight percentages based on total alloy weight unless otherwise indicated. "NS" in Table 1 indicates that the particular UNS specification does not specify a concentration for the element.
  • Type 201 stainless steel is similar to standard 18 chromium-8 nickel stainless steels, but with a fraction of nickel replaced with manganese to lower alloy cost.
  • Type 201 alloy does not possess sufficient creep and oxidation resistance for use at elevated temperatures.
  • Higher-alloyed materials such as the NITRONIC® family of alloys, Esshete 1250 alloy, and 21-6-9 alloy (UNS S21900), include low nickel levels (about 11 weight percent maximum) and significant manganese levels (5-10 weight percent), and are typically designed for high creep strength and moderate environmental resistance.
  • Commercially available heat-resistant stainless steels such as AISI Types 309S and 310S generally include manganese at levels up to about 2 weight percent. These alloys are somewhat deficient in terms of metallurgical stability, which may be tied to their basic compositions inasmuch as the nickel-to-chromium ratio for these two grades results in the formation of significant amounts of brittle phases at typical use temperatures.
  • austenitic stainless steels having improved high temperature creep resistance and/or resistance to corrosive attack in high temperature air and/or in high temperature air containing appreciable levels of water vapor.
  • stainless steels exhibiting substantial corrosion resistance in high temperature air including water vapor could be advantageously employed in, for example, parts of energy generation devices including, for example, gas turbines, steam turbines, and fuel cells, which are subjected to highly corrosive high temperature-high water vapor content environments.
  • Such parts include heat exchangers, recuperators, tubing, pipe, and certain structural parts.
  • Alloys exhibiting substantial corrosion resistance in high temperature air also may be advantageously applied in certain devices for high temperature processing, treatment, or extraction of chemicals or minerals, or for high temperature processing or treatment of alloys.
  • Stainless steels exhibiting both substantial high temperature creep resistance as well as significant corrosion resistance could be advantageously adapted for use in parts of the foregoing devices that are subjected to high stresses.
  • the invention provides an austenitic stainless steel in accordance with claim 1 of the appended claims.
  • austenitic stainless steels having improved high temperature creep resistance and/or improved resistance to corrosion when exposed to a high temperature air environment.
  • high temperature refers to temperatures in excess of about 100°F (about 37.8°C).
  • an austenitic stainless steel is provided including: 0.05 to 0.2 carbon; 0.08 to 0.2 nitrogen; 20 to 23 chromium; 25 to 27 nickel; 1 to 2 molybdenum; 1.6 to 4.0 manganese; 0.20 to 0.75 niobium; 0 up to 0.1 titanium; iron; and incidental impurities.
  • the austenitic stainless steel further includes one or more of the following elements: greater than 0 to 0.50 silicon; greater than 0 to 0.30 aluminum; greater than 0 to 0.02 sulfur; greater than 0 to 0.05 phosphorus; greater than 0 to 0.1 zirconium; and greater than 0 to 0.1 vanadium.
  • the titanium and/or aluminum content of the steel is no greater than 0.1 weight percent.
  • an austenitic stainless steel that consists essentially of the following: 0.05 to 0.2 carbon; 0.08 to 0.2 nitrogen; 20 to 23 chromium; 25 to 27 nickel; 1 to 2 molybdenum; 1.6 to 4.0 manganese; 0.20 to 0.75 niobium; up to 0.1 titanium; up to 0.50 silicon; up to 0.30 aluminum; up to 0.02 sulfur; up to 0.05 phosphorus; up to 0.1 zirconium; up to 0.1 vanadium; iron; and incidental impurities.
  • an austenitic stainless steel that consists of: 0.05 to 0.2 carbon; 0.08 to 0.2 nitrogen; 20 to 23 chromium; 25 to 27 nickel; 1 to 2 molybdenum; 1.6 to 4.0 manganese; 0.20 to 0.75 niobium; up to 0.1 titanium; up to 0.50 silicon; up to 0.30 aluminum; up to 0.02 sulfur; up to 0.05 phosphorus; up to 0.1 zirconium; up to 0.1 vanadium; iron; and incidental impurities.
  • an article of manufacture including an austenitic stainless steel having a composition according to the present disclosure.
  • the article of manufacture include, for example, energy generation devices and parts of such devices.
  • the article of manufacture may be selected from a gas turbine, a steam turbine, a fuel cell, a heat exchanger, a recuperator, a tube, a pipe, a structural part, and other parts for any of those devices.
  • Other examples of the article of manufacture include equipment or piping, tubing, and other parts for equipment for high temperature processing, treatment, or extraction of chemicals and minerals, or for high temperature processing or treatment of alloys.
  • any numerical range recited herein is intended to include the range boundaries and all sub-ranges subsumed therein.
  • a range of "1 to 10" is intended to include all sub-ranges between (and including) the recited minimum value of 1 and the recited maximum value of 10, that is, having a minimum value equal to or greater than I and a maximum value of equal to or less than 10.
  • certain austenitic stainless steels have been used in articles and parts exposed to high temperature air or to high temperature air containing significant water vapor.
  • Parts subjected to such conditions include, for example, affected parts of energy generation devices, such as gas turbines, steam turbines, and fuel cells, and heat exchangers and recuperators, and in equipment and parts for high temperature processing, treatment, or extraction of chemicals or minerals, or high temperature processing or treatment of alloys.
  • energy generation devices such as gas turbines, steam turbines, and fuel cells, and heat exchangers and recuperators
  • These steels still suffer from a level of corrosive attack when subjected over time to these conditions. Accordingly, the present inventors undertook to determine whether certain modified austenitic stainless steel chemistries further improved corrosion resistance in high temperature environments.
  • the inventors determined that alloys containing 1.5 weight percent or less manganese are subject to oxide scale evaporation and subsequent degradation in air containing water vapor.
  • the inventors' work focused on certain novel austenitic stainless steel chemistries including more than 1.5 weight percent manganese, along with appreciable levels of chromium and nickel.
  • the present inventors concluded that an austenitic stainless steel having the broad composition and, more preferably, the nominal composition listed in Table 2 would have substantial resistance to chromium oxide scale evaporation in high temperature air environments and in high temperature air environments including water vapor.
  • the proposed alloy's manganese content is controlled at a minimum level, which was found to significantly improve resistance to high temperature corrosive attack.
  • Table 3 provides information on several alloys evaluated during the testing. All heats were melted and subsequently rolled to foil gauge. Heats 1 and 3 were lab heats, heat 2 was prepared as a pilot coil, and heat 4 was a plant heat prepared as a production coil. Heats 1, 3, and 4 were prepared with an aim of 1.0 weight percent manganese, and heat 2 was prepared with an aim of 1.6 weight percent manganese. Heat 2 is within the scope of the invention. Heats 1, 3 and 4 are comparative.
  • Figure 2 shows weight change over time for samples of high manganese (heat 2) and the low manganese (heat 4) alloys when the samples were exposed at 1400°F (760°C) in air containing 7% water vapor.
  • the samples exhibited significantly different oxidation kinetics under these conditions.
  • the high manganese sample gained weight rapidly during the initial portion of the test, but then the weight gain slowed significantly. After completion of the 5,000 hour test, the two samples exhibited essentially identical weight gain.
  • Figure 3 shows weight change overtime for samples of high manganese (heat 2) and the low manganese (heat 4) alloys when the samples were exposed at 1500°F (815°C) in air containing 7% water vapor.
  • the curve shows that the lower manganese sample exhibited significant oxide scale evaporation during the test period.
  • the higher manganese alloy did not exhibit the same weight change over the limited test exposure.
  • the low manganese material did not exhibit manganese saturation (i.e., a MnO/Cr 2 O 3 ratio of 1.0) at the scale/gas interface at 1300°F (704°C) and was borderline saturated at 1400°F (760°C). Achieving manganese saturation in the spinel is believed to be important in providing resistance to evaporation.
  • Figure 6 plots the chromium concentration as a function of depth into the sample surface for high manganese and low manganese samples, from heats 2 and 4, respectively, exposed for 5,000 hours at 1300°F (704°C) in air containing 10% water vapor.
  • the depletion observed for the low manganese sample is significantly greater in terms of chromium concentration directly adjacent the scale/metal interface Depth of depletion between the samples does not appear to be noticeably different.
  • the chromium profiles derived from each sample appear extremely sharp, indicating that chromium cannot diffuse rapidly from the interior of the sample to the scale/alloy interface.
  • Figure 7 is a plot of chromium concentration as a function of depth into the sample surface for high manganese and low manganese samples, heats 2 and 4, respectively, exposed for 5,000 hours at 1400°F (760°C) in air containing 7% water vapor.
  • chromium depletion for the low manganese sample was significantly greater than for the high manganese sample at the scale/metal interface. It was observed that the effect of chromium depletion at 1400°F (760°C) is not substantially greater in terms of terminal chromium content at the scale/alloy interface relative to what is shown in Figure 6 , but the gradient shown in Figure 7 runs much deeper into the substrate. This may have resulted because the diffusion of chromium in the metal is rapid enough at 1400°F (760°C) to delocalize the effects of chromium depletion due to oxidation.
  • Figure 8 is a graph showing oxide composition, measured as a molar ratio of MnO to Cr 2 O 3 , using XEDS in the SEM (semi-quantitative) for high manganese and low manganese samples, derived from heats 2 and 4, respectively, subjected to high temperature air containing 7% water vapor. The measurements were taken at the scale/alloy interface and the scale/gas interface. The evaluations conducted after exposure to 1300°F (704°C) and to 1400°F (760°C) air were conducted after about 5,000 hours of exposure time. Those conducted after exposure at 1500°F (815°C) were performed after about 3,000 hours of exposure time.
  • the low manganese material did not exhibit manganese saturation (i.e., a MnO/Cr 2 O 3 ratio of 1.0) at the scale/gas interface at 1300°F (704°C) and at 1500°F (815°C), and was borderline saturated at 1400°F (760°C).
  • Figure 9 is a plot of sample weight change over time for samples of the alloys of heat 2 (1.61 weight percent manganese), heat 5 (2.04 weight percent manganese), and heat 6 (3.82 weight percent manganese) exposed at 1400°F (760°C) in air containing 7% water vapor.
  • the results indicate that higher manganese levels produce higher initial weight gain through oxide scale formation. While the weight gains shown in Figure 9 did not appear to be problematic, it is believed that higher manganese levels, above about 4 weight percent, would result in further scale formation and weight gains, and the consequent undesirable result of spallation of the material.
  • Heats 7 and 8 in Table 5 were prepared. The heats included less than 0.1 weight percent titanium. Heats 7 and 8 also included less than 0.1 weight percent aluminum. Table 5 Heat 7 Heat 8 Carbon 0.086 0.088 Molybdenum 1.54 1.52 Chromium 20.99 20.95 Nickel 25.92 26.02 Niobium 0.30 0.30 Manganese 1.61 1.79 Titanium 0.010 0.01 Nitrogen 0.0955 0.1130 Silicon 0.41 0.40 Sulfur ⁇ 0.01 ⁇ 0.01 Aluminum ⁇ 0.01 ⁇ 0.01 Boron 0.0033 0.0029
  • austenitic stainless steels subjected to stress at high temperature for prolonged periods can be subject to creep.
  • Most austenitic stainless steels include relatively minor levels of titanium and aluminum to facilitate deoxidation of the molten metal during melting and casting. These elements also are precipitated as nitrides and, possibly, intermetallic phases in the solid state. These precipitated phases are very difficult or impractical to dissolve during processing. Excessive nitride formation will have the effect of reducing the level of nitrogen in solid solution, which will reduce the creep strength of the alloy. Nitrides and intermetallic phases also can make processing more difficult, particularly when the steel is formed by being folded or stamped into part shapes.
  • a preferred chemistry for the austenitic stainless steels of the present disclosure includes at least one of no greater than 0.1 weight percent titanium and no greater than 0.1 weight percent aluminum. More preferably, to better enhance creep resistance and formability, the austenitic stainless steels of the present disclosure includes no greater than 0.1 weight percent titanium and no greater than 0.1 weight percent aluminum.
  • an austenitic stainless having the investigated chemistries and including manganese at levels of 1.6 weight percent up to about 4 weight percent should exhibit advantageous resistance to high temperature attack in air, which may include significant water vapor, and without suffering from excessive scale formation and spallation. More specifically, the broad and nominal alloy compositions shown in Table 2 are proposed as austenitic stainless steels with substantial resistance to corrosive attack in high temperature air and in high temperature air including water vapor.
  • a preferred manganese level is at least 1.6 up to about 4 weight percent, and a more preferred manganese level is at least 1.6 up to about 2.0 weight percent manganese.
  • An additional proposed alloy chemistry having improved creep resistance and improved formability has the general chemistry shown in Table 2, but includes no greater than 0.1 weight percent titanium and/or no greater than 0.1 weight percent aluminum.
  • the expected improvement in creep resistance resulting from the limits on titanium and/or aluminum content can be exhibited by an alloy having improved high temperature corrosion resistance provided by controlling the manganese content to the range of 1.6 weight percent up to about 4 weight percent. Accordingly, the alloy in the following Table 6 should exhibit advantageous creep resistance and formability properties, and a preferred chemistry includes no greater than 0.1 weight percent titanium and no greater than 0.1 weight percent aluminum.
  • An alloy exhibiting advantageous high temperature creep resistance, improved formability, and advantageous resistance to corrosive attack in high temperature air including water vapor would have the composition shown in Table 6 and wherein the composition is further controlled such that the manganese content is 1.6 up to about 4.0 weight percent, and preferably is at least 1.6 up to about 2.0 weight percent.
  • Such an alloy could be advantageously applied in making, for example, structural parts and other parts of the previously mentioned energy generation devices and processing, treatment, or extraction devices that are both subjected to stress and exposed to high temperature air including water vapor.
  • Heats of the novel corrosion resistant austenitic stainless steels disclosed herein may be made by conventional means, such as by the conventional technique of vacuum melting scrap and other feed materials.
  • the resulting heats may be processed by conventional techniques into billets, slabs, plates, coils, sheets, and other intermediate articles, and then further processed into final articles of manufacture.
  • the enhanced formability of embodiments of alloys within the present disclosure including no greater than 0.1 weight percent of titanium and/or no greater than 0.1 weight percent aluminum allows flat mill products (such as strip, sheet, plate, coil, and the like) formed from the alloys to be further processed into articles having relatively complicated shapes. This characteristic of the alloys is an advantage relative to NF709 alloy, which has more limited formability and has commonly only been processed by extrusion into seamless pipe.
  • novel austenitic stainless steels according to the present disclosure may be used in any suitable application and environment, but the alloys are particularly suited for use in equipment and parts subjected for extended periods to high temperature, or to both high temperature and significant water vapor.
  • the creep resistance and/or high temperature corrosion resistance of the alloys disclosed herein makes them particularly suitable for use in: tubing, piping, structural parts, and other parts of equipment adapted for high temperature processing, treatment, or extraction of chemicals or minerals, or high temperature processing or treatment of alloys; tubing, piping, structural parts, and other parts of energy generation devices such as, for example, gas turbines, steam turbines, and fuel cells; and parts of heat exchangers, recuperators, and other equipment handling gas streams used or generated by energy generation devices.
  • Other applications for the alloys disclosed herein will be apparent to those of ordinary skill upon considering the present description of the alloys.

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EP06851605.3A 2005-06-03 2006-04-07 Austenitic stainless steel Not-in-force EP1941070B1 (en)

Applications Claiming Priority (3)

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US68740005P 2005-06-03 2005-06-03
US11/270,279 US20060275168A1 (en) 2005-06-03 2005-11-09 Austenitic stainless steel
PCT/US2006/013175 WO2008041961A2 (en) 2005-06-03 2006-04-07 Austenitic stainless steel

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EP1941070A2 EP1941070A2 (en) 2008-07-09
EP1941070B1 true EP1941070B1 (en) 2015-09-30

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US (1) US20060275168A1 (pt)
EP (1) EP1941070B1 (pt)
JP (1) JP5068760B2 (pt)
KR (2) KR101412893B1 (pt)
AU (1) AU2006344097B2 (pt)
BR (1) BRPI0607922B1 (pt)
DK (1) DK1941070T3 (pt)
ES (1) ES2551868T3 (pt)
NO (1) NO20076693L (pt)
RU (1) RU2429308C2 (pt)
WO (1) WO2008041961A2 (pt)

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KR101412893B1 (ko) 2014-06-26
JP5068760B2 (ja) 2012-11-07
WO2008041961A2 (en) 2008-04-10
BRPI0607922A2 (pt) 2009-10-20
AU2006344097A1 (en) 2008-04-10
KR20130043247A (ko) 2013-04-29
ES2551868T3 (es) 2015-11-24
AU2006344097B2 (en) 2011-07-07
JP2008545889A (ja) 2008-12-18
RU2007149031A (ru) 2009-07-20
BRPI0607922B1 (pt) 2017-09-12
RU2429308C2 (ru) 2011-09-20
US20060275168A1 (en) 2006-12-07
DK1941070T3 (en) 2016-01-11
WO2008041961A3 (en) 2008-05-29
KR20080053437A (ko) 2008-06-13
EP1941070A2 (en) 2008-07-09
NO20076693L (no) 2008-02-29

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