EP0851037B1 - Nickellegierung mit hohem chromgehalt mit hohem schwefelwasserstoffkorrosionswiderstand - Google Patents

Nickellegierung mit hohem chromgehalt mit hohem schwefelwasserstoffkorrosionswiderstand Download PDF

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Publication number
EP0851037B1
EP0851037B1 EP96917716A EP96917716A EP0851037B1 EP 0851037 B1 EP0851037 B1 EP 0851037B1 EP 96917716 A EP96917716 A EP 96917716A EP 96917716 A EP96917716 A EP 96917716A EP 0851037 B1 EP0851037 B1 EP 0851037B1
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EP
European Patent Office
Prior art keywords
hydrogen sulfide
alloy
content
corrosion resistance
alloys
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP96917716A
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English (en)
French (fr)
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EP0851037A1 (de
EP0851037A4 (de
Inventor
Masakatsu Ueda
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Nippon Steel Corp
Original Assignee
Sumitomo Metal Industries Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Sumitomo Metal Industries Ltd filed Critical Sumitomo Metal Industries Ltd
Priority claimed from PCT/JP1996/001672 external-priority patent/WO1997048830A1/ja
Priority claimed from CA002212346A external-priority patent/CA2212346C/en
Publication of EP0851037A1 publication Critical patent/EP0851037A1/de
Publication of EP0851037A4 publication Critical patent/EP0851037A4/de
Application granted granted Critical
Publication of EP0851037B1 publication Critical patent/EP0851037B1/de
Anticipated expiration legal-status Critical
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Classifications

    • 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
    • C22C38/42—Ferrous alloys, e.g. steel alloys containing chromium with nickel with copper

Definitions

  • This invention relates to austenitic high-Cr and high-Ni alloys and more particularly, to high-Cr and high-Ni alloys which exhibit a good corrosion resistance when placed in an aqueous solution having a relatively low hydrogen sulfide concentration at a partial pressure of hydrogen sulfide gas of 1 atm., or below.
  • the examples of alloys which are employed in environments where they are in contact with hydrogen sulfide-containing liquids include drill pipes, pipes for flow lines from oil wells, oil country tubular goods for oil and natural gas wells, plate members for natural steam power stations, plate members for installation for desulfurization from exhaust gases, and the like. Especially, drilling of oil wells, exploitation and production of natural gas involve corrosive environments which are severe.
  • alloys which are to be employed in an environment containing hydrogen sulfide should have a good resistance to stress corrosion cracking.
  • Known alloys which are used in an environment such as of a hydrogen sulfide-containing oil well wherein a partial pressure of hydrogen sulfide is as high as approximately 10 atm. include Ni-Cr-Mo-Fe Ni-based alloys which contain Ni in amounts as great as 30 -50% (Japanese Laid-open Patent Application Nos. 57-131340, 57-134544 and 57-134545).
  • Japanese Laid-open Patent Application No. 57-131340 proposes an alloy which comprises, aside from Ni, Cr, Mo and W, Cu and Co, if necessary, in order to improve the resistance to stress corrosion cracking.
  • alloys for oil wells are so designed as to improve the corrosion resistance to hydrogen sulfide including a resistance to stress corrosion cracking. More particularly, the corrosion resistance to hydrogen sulfide is greatly influenced by the content of hydrogen sulfide present in raw oil and the temperature of the raw oil. Accordingly, when used in such an environment of hydrogen sulfide as having set out above, the alloy is so designed that a corrosion-resistant film is formed on the surfaces of the alloy.
  • the corrosion-resistant film should have a two-layer structure including an outer layer consisting of a Ni sulfide film and an inner layer consisting of a Cr oxide film. In order to facilitate the growth of the inner layer of the Cr oxide film, at least one of Mo and W is incorporated in the alloy.
  • the reason why the corrosion-resistant film is designed to have a double-layer structure is so that hydrogen sulfide is prevented from entering into the inner layer by means of the outer layer of the Ni sulfide film thereby preventing the breakage of the Cr oxide inner film with the hydrogen sulfide.
  • the Cr oxide inner film is able to suppress the dissolution of the alloy and thus, acts to improve the corrosion resistance, ensuring a good corrosion resistance to hydrogen sulfide.
  • the invention has for its object the provision of a high-Cr and high-Ni alloy which overcomes the problems involved in the prior art, which is imparted with good corrosion resistance to hydrogen sulfide under environmental conditions of a partial pressure of hydrogen sulfide of 1 atm., or below and a temperature of about 150°C, and which is low in cost.
  • the high-Cr and high-Ni alloy of the invention has a good corrosion resistance to hydrogen sulfide under environmental conditions of a partial pressure of hydrogen sulfide of 1 atm., or below and a temperature of about 150 °C.
  • the alloy is free of Mo and W which are expensive elements and is thus low in cost, and is mass-producible.
  • the alloy of the invention has the following chemical composition on the basis of percent by weight: Si: 0.05 - 1.0% Mn: 0.1 - 1.5% Cr: 20 - 30% Ni: 20 - 40% sol.
  • the contents of C, P and S in the incidental impurities should, respectively, be 0.05% or below, 0.03% or below and 0.01% or below.
  • REM, Y, Mg and Ca do not have to be added at all, however, if these elements are used, it is sufficient to add at least one of REM, Y, Mg and Ca.
  • Preferable contents of these elements are as follows: REM 0.001 - 0.10% Y 0.001 - 0.20% Mg 0.001 - 0.10% Ca 0.001 - 0.10%
  • Si is an element necessary for deoxidation of molten steel at the time of refining.
  • the content should be 0.05% or above.
  • the content of Si is in the range of 0.05 - 1.0%, preferably 0.2 - 0.5%.
  • Mn is an element necessary for deoxidation of molten steel.
  • the content of Mn should be 0.1% or above.
  • the content of Mn is in the range of 0.1 - 1.5%, preferably 0.5 - 0.75%.
  • Cr is an element which is effective for improving the corrosion resistance to hydrogen sulfide (especially, resistance to stress corrosion cracking) in co-existence with other major components of Ni and N. If the content is less than 20%, such an effect cannot be obtained satisfactorily. Cr tends to worsen hot workability. If the content is reduced to a range of less than 20%, no significant effect of improving the hot workability may be obtained. On the other hand, where the content of Cr exceeds 30%, any further improvement of the corrosion resistance to hydrogen sulfide cannot be attained using a higher content of Cr within the above range. Moreover, in the case where the content of Cr exceeds 30%, good hot workability cannot be expected even if the content of S is reduced. Accordingly, the content of Cr is in the range of 20 - 30%, preferably 22 - 27%.
  • Ni is effective in improving the corrosion resistance to hydrogen sulfide. This effect is shown when the content of Ni is 20% or above. However, when the content exceeds 40%, any further effect is not expected using a higher content within the above range. Where Ni (which is expensive) is contained in amounts higher than required, the resultant alloy becomes expensive, thus being economically poor. Accordingly, the content of Ni is in the range of 20 - 40%, preferably 22 - 30%.
  • Al like Si and Mn, is an element necessary for the deoxidation of molten steel.
  • the deoxidation effect is shown when the content of sol. Al (i.e.. Al contained in alloy and soluble in hydrochloric acid) is 001% or above.
  • the content of sol. Al exceeds 0.3%, hot workability is impeded. Accordingly, the content of sol. Al is in the range of 0.01 - 0.3%, preferably 0.1 - 0.15%.
  • Cu is the most important element for the invention which constitutes a characteristic feature of the high-Cr and high-Ni alloy of the invention.
  • Cu serves to remarkably improve the corrosion resistance to hydrogen sulfide in an environment of hydrogen sulfide gas whose partial pressure is as low as 1 atm., or below. In order to achieve this improvement, 0.5% or above of Cu should be present. However, if Cu is added in excess of 5.0%, no further improvement is expected. Additionally, when the content exceeds 5.0%, hot workability is degraded. Accordingly, the content of Cu is in the range of 0.5 - 5.0%, preferably 1.0 - 3.0%.
  • the alloy of the invention may contain one or more of REM (rare earth elements), Y, Mg and Ca in order to improve hot workability. These elements are effective in improving hot workability as in the case where the alloy is hot-worked under severe conditions.
  • each element is less than 0.001%, any significant effect of improving the hot workability is not obtained.
  • contents of the respective elements exceed the defined upper limits, coarse oxides are formed, thus impeding hot workability.
  • Major incidental impurities include C, P and S.
  • the content of C should preferably be not more than 0.05%.
  • the content of C exceeds 0.05% and Nb or V co-exist as an impurity, coarse carbide is formed along with the co-existing element, and Cr carbide is formed at grain boundaries in a contiguous state.
  • the formation of these carbides causes Cr depletion zones, so that stress corrosion cracking is liable to occur along the grain boundaries.
  • the upper limit of the content of C is determined at 0.05%, and the content of C is preferably 0.03% or below.
  • the content of P exceeds 0.03, the susceptibility to stress corrosion cracking in an environment of hydrogen sulfide increases. Accordingly, the upper limit is 0.03%.
  • the content is preferably 0.02% or below.
  • the content of S When the content of S exceeds 0.01%, hot workability is considerably impeded. Accordingly, the content of S is defined to be not more than 0.01. If the content of S is so great, hot workability is considerably impeded as set out above. In this connection, if the content of S is as low as about 0.0007% or below, hot workability is improved. Accordingly, if good hot workability under severe conditions is essential, it is preferred to reduce the content of S to a level of 0.0007% or below.
  • the incidental impurity elements may further comprise, aside from the above-stated C, P and S, 0.10% or below of B, Sn, As, Sb, Bi, Pb and Zn.
  • the impurities present in such amounts as set out above exerts little influence on the characteristics of the alloy of the invention.
  • the alloy of the invention and articles such as alloy pipes made of the alloy of the invention as a base metal can be made using manufacturing apparatus and methods which are employed for ordinary commercial manufacture. For instance, melting of the alloy may be conducted by utilizing electric furnaces, argon-oxygen decarburization furnaces (AOD furnaces), vacuum-oxygen decarburization furnaces (VOD furnaces) and the like.
  • the molten metal may be cast into ingots or may be cast into rod-shaped billets according to a continuous casting technique.
  • an extrusion pipe making processes such as the Ugine Sejournet process, or the Mannesman pipe making process.
  • the pipe making conditions such as a heating temperature of billets prior to pipe making may be those of the case using conventional high-Cr and high-Ni alloys.
  • each ingot was heated to 1250°C and subjected to hot forging at 1200°C to obtain a rod with a diameter of 150 mm.
  • the rod was cut into pieces having a length of 1000 mm to obtain billets for extrusion pipe making.
  • the billet was shaped into a pipe having a diameter of 60 mm, a thickness of 5 mm and a length of about 20 m according to the Ugine Sejournet hot extrusion pipe making process. Only one pipe was made for each alloy indicated in Table 1.
  • a sample piece was taken out from each pipe and subjected to a corrosion test in a hydrogen sulfide environment to check corrosion resistance to hydrogen sulfide.
  • the corrosion test in the hydrogen sulfide environment was conducted in the following manner. It should be noted that the hot workability was evaluated in terms of the presence (symbol "x” in Table 1) or the absence (symbol "o” in Table 1) of defects through visual observation of defects on the inner surfaces of a pipe obtained by extrusion pipe making. Two sample pieces for each alloy were used for the corrosion test in the hydrogen sulfide environment.
  • Table 1 the results of the corrosion test in the hydrogen sulfide environment and the results of evaluation of the hot workability are shown in Table 1. With respect to the corrosion resistance to hydrogen sulfide, where either pitting corrosion or cracking was not observed at all, this resistance is indicated as "o”. Where either of pitting corrosion or cracking was observed, this is indicated as "x”.
  • alloys of the inventive example (alloy Nos. 1 - 12), wherein the chemical compositions are within the range of the invention, were not recognized with respect to the pitting corrosion and the cracking in the corrosion test in the hydrogen sulfide environment. Moreover, no defect on the inner surface of the pipes obtained after pipe making was found.
  • the alloys of the invention are excellent in the corrosion resistance to hydrogen sulfide and hot workability.
  • the hot workability is better than that of the case where such an element is not added at all.
  • Comparative alloy Nos. 16 - 18 contain either or both of Mo and W and those alloys have been hitherto accepted as showing good corrosion resistance to hydrogen sulfide in an environment where a partial pressure of hydrogen sulfide gas is high. Nevertheless, as will be apparent from this example, these alloys were poor in corrosion resistance to hydrogen sulfide. These results revealed that where the partial pressure of hydrogen sulfide gas was low, like those conditions of this example, Mo and W did not serve to improve the corrosion resistance to hydrogen sulfide.
  • alloy No. 2 of the invention was further subjected to another corrosion test in the hydrogen sulfide environment where a partial pressure of hydrogen gas in the testing atmosphere was set at 0.8 atm., with the other conditions being the same as in Example 1.
  • a partial pressure of hydrogen gas in the testing atmosphere was set at 0.8 atm.
  • the inventive alloy was excellent in corrosion resistance to hydrogen sulfide.
  • the alloys of the invention exhibit an excellent corrosion resistance to hydrogen sulfide in an environment where a partial pressure of hydrogen sulfide gas is as low as about 1 atm., or below, along with good hot workability. Since it is not necessary to add Mo and W(which are expensive), the cost of raw materials for alloys making decreases. Moreover, the alloys of the invention can be made by use of manufacturing apparatus and method which have been conventionally used for the manufacture, thus making it possible to mass-produce the alloy inexpensively.
  • the alloy of the invention is employed, for example as a material for pipes which are in contact with a hydrogen sulfide-containing corrosive fluid produced from oil wells, good corrosion resistance is ensured.
  • the alloy of the invention thus has very high practical value for use as a material which is used in an environment where a partial pressure of hydrogen sulfide gas is relatively low.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Rigid Pipes And Flexible Pipes (AREA)

Claims (6)

  1. Hoch chrom- und hoch nickelhaltige Legierung, die eine gute Korrosionsbeständigkeit gegenüber Schwefelwasserstoff aufweist, mit den folgenden chemischen Komponenten auf der Basis von Gew.-%: SiM 0,05 - 1,0 %; Mn 0,1 - 1,5%; Cr 20,0 - 30,0 %; Ni 20,0 - 40,0 %; gel. Al 0,01 - 0,3%; Cu 0,5 - 5,0 %; Seltenerdmetalle 0,0 - 0,10%; Y 0,0 - 0,20%; Mg 0,0 - 0,10%; Ca 0,0 - 0,10%; Rest Fe und auftretende Verunreinigungen,
    vorausgesetzt, dass C, P und S in den auftretenden Verunreinigungen 0,05 % oder weniger bzw. 0,03 % oder weniger bzw. 0,01 % oder weniger umfassen.
  2. Hoch chrom- und hoch nickelhaltige Legierung nach Anspruch 1, dadurch gekennzeichnet, dass die Legierung auf der Basis von Gew.-% wenigstens eines umfasst: Seltenerdmetalle: 0,001 - 0,10 %, Y: 0,001 - 0, 20 %, Mg: 0,001 - 0,10 % und Ca: 0,001 - 0,10 %.
  3. Hoch chrom- und hoch nickelhaltige Legierung nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass auf der Basis von Gew.-% der Anteil an Kupfer zwischen 1,0 und 3,0 % liegt.
  4. Hoch chrom- und hoch nickelhaltige Legierung nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass auf der Basis von Gew.-% der Anteil an Cr zwischen 22 und 27 % liegt.
  5. Hoch chrom- und hoch nickelhaltige Legierung nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass auf der Basis von Gew.-% der Anteil an Ni zwischen 22 und 30 % liegt.
  6. Hoch chrom- und hoch nickelhaltige Legierung nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass auf der Basis von Gew.-% der Anteil an Kupfer zwischen 1,0 und 3,0 % liegt, der Anteil an Chrom zwischen 22 und 27 % liegt und der Anteil an Nickel zwischen 22 und 30 % liegt.
EP96917716A 1996-06-17 1996-06-17 Nickellegierung mit hohem chromgehalt mit hohem schwefelwasserstoffkorrosionswiderstand Expired - Lifetime EP0851037B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
PCT/JP1996/001672 WO1997048830A1 (fr) 1996-06-17 1996-06-17 Alliage possedant une forte teneur en chrome et en nickel et resistant a la corrosion par sulfure d'hydrogene
CA002212346A CA2212346C (en) 1996-06-17 1996-06-17 Hydrogen sulfide corrosion resistant high-cr and high ni alloys

Publications (3)

Publication Number Publication Date
EP0851037A1 EP0851037A1 (de) 1998-07-01
EP0851037A4 EP0851037A4 (de) 1999-12-01
EP0851037B1 true EP0851037B1 (de) 2002-09-04

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EP96917716A Expired - Lifetime EP0851037B1 (de) 1996-06-17 1996-06-17 Nickellegierung mit hohem chromgehalt mit hohem schwefelwasserstoffkorrosionswiderstand

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EP (1) EP0851037B1 (de)
AU (1) AU696908B2 (de)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2007124996A1 (de) * 2006-04-27 2007-11-08 Evonik Degussa Gmbh Reaktionsbehälter für die herstellung von schwefelwasserstoff

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
SE527319C2 (sv) 2003-10-02 2006-02-07 Sandvik Intellectual Property Legering för högtemperaturanvändning
US20080196797A1 (en) * 2007-02-16 2008-08-21 Holmes Kevin C Flow formed high strength material for safety systems and other high pressure applications

Family Cites Families (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3926620A (en) * 1970-07-14 1975-12-16 Sumitomo Metal Ind Low carbon ni-cr alloy steel having an improved resistance to stress corrosion cracking
US4816217A (en) * 1984-03-16 1989-03-28 Inco Alloys International, Inc. High-strength alloy for industrial vessels
US4816218A (en) * 1984-11-01 1989-03-28 Inco Alloys International, Inc. Process of using an iron-nickel-chromium alloy in an oxidation attacking environment
DE3716665A1 (de) * 1987-05-19 1988-12-08 Vdm Nickel Tech Korrosionsbestaendige legierung
JPH03103842A (ja) * 1989-09-19 1991-04-30 Seiko Epson Corp 投写型液晶表示装置
WO2004023462A1 (en) * 2002-09-05 2004-03-18 Koninklijke Philips Electronics N.V. Recordable optical record carrier comprising two sub-grooves

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2007124996A1 (de) * 2006-04-27 2007-11-08 Evonik Degussa Gmbh Reaktionsbehälter für die herstellung von schwefelwasserstoff

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Publication number Publication date
EP0851037A1 (de) 1998-07-01
EP0851037A4 (de) 1999-12-01
AU696908B2 (en) 1998-09-24
AU6017596A (en) 1998-01-07

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