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US20130263973A1 - Ni-Based Amorphous Alloy With High Ductility, High Corrosion Resistance and Excellent Delayed Fracture Resistance - Google Patents

Ni-Based Amorphous Alloy With High Ductility, High Corrosion Resistance and Excellent Delayed Fracture Resistance Download PDF

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Publication number
US20130263973A1
US20130263973A1 US13/880,280 US201113880280A US2013263973A1 US 20130263973 A1 US20130263973 A1 US 20130263973A1 US 201113880280 A US201113880280 A US 201113880280A US 2013263973 A1 US2013263973 A1 US 2013263973A1
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US
United States
Prior art keywords
amorphous alloy
based amorphous
corrosion resistance
ductility
acid
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Abandoned
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US13/880,280
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English (en)
Inventor
Ryurou Kurahashi
Tsunehiro Mimura
Kenji Amiya
Yasunori Saotome
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.)
Tohoku University NUC
Nakayama Steel Works Ltd
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Nakayama Steel Works Ltd
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Assigned to NAKAYAMA STEEL WORKS, LTD., TOHOKU UNIVERSITY reassignment NAKAYAMA STEEL WORKS, LTD. ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: AMIYA, KENJI, KURAHASHI, RYUROU, MIMURA, TSUNEHIRO, SAOTOME, YASUNORI
Publication of US20130263973A1 publication Critical patent/US20130263973A1/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
    • C22C45/00—Amorphous alloys
    • C22C45/04—Amorphous alloys with nickel or cobalt as the major constituent
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/01—Layered products comprising a layer of metal all layers being exclusively metallic
    • B32B15/013—Layered products comprising a layer of metal all layers being exclusively metallic one layer being formed of an iron alloy or steel, another layer being formed of a metal other than iron or aluminium
    • B32B15/015—Layered products comprising a layer of metal all layers being exclusively metallic one layer being formed of an iron alloy or steel, another layer being formed of a metal other than iron or aluminium the said other metal being copper or nickel or an alloy thereof
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/02—Making non-ferrous alloys by melting
    • C22C1/03—Making non-ferrous alloys by melting using master alloys
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/11—Making amorphous alloys
    • 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
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C45/00—Amorphous alloys
    • C22C45/02—Amorphous alloys with iron as the major constituent

Definitions

  • the invention according to Claims relates to Ni-based amorphous alloy which has high ductility, excellent resistance to delayed fracture caused by hydrogen, and high corrosion resistance, and can be used in large quantities as an industrial material.
  • Fe-based amorphous alloys such as the Fe—Cr series and the Fe—Cr—Mo series have excellent corrosion resistance. Thus, they have been studied for many years and numerous reports and patents are available.
  • a representative one is the Fe—Cr—Mo—P series disclosed in Japanese Patent No. 3805601.
  • P See the Report: Koji Hashimoto, Amorphous Stainless, Journal of the Japan Institute of Metals and Materials, Vol. 8, No. 5 (1979)] which is useful for the formation of a passive state with high corrosion resistant is primarily used.
  • the forms are primarily P-C and P-B.
  • the amorphous alloy in this partial component system has already been commercialized.
  • the product has been used as a coating on the surface of the pump shaft for carrying acids (hydrochloric acid, hydrofluoric acid, and phosphoric acid) at chemical plants for chemical agents.
  • the performance thereof is greater by 5 times or more than that of hastelloy alloys in terms of resistance both to corrosion and abrasion.
  • acids hydrochloric acid, hydrofluoric acid, and phosphoric acid
  • the Aforementioned Fe-Based Amorphous Alloys have a Low Ductility.
  • a adhesion bending (180 degrees) test of a ribbon was performed for evaluation of ductility and an amorphous ribbon for obtaining the ductility performance index was prepared as follows. For each amorphous alloy component, a mixture of pure metals and semimetals was dissolved by high frequency heating under an Ar atmosphere and cast in a Cu mold to obtain a mother alloy. This mother alloy was dissolved again by high frequency heating under an Ar atmosphere and blown over a single roller to obtain an amorphous ribbon. The formation of the amorphous alloy was confirmed by halo peaks by X-ray diffraction (See FIG. 1 ). The thickness of the amorphous ribbon was adjusted to 30 microns and 60 microns by changing the number of rotations of the single roller. An adhesion bending (180 degrees) test of the ribbon was performed and the performance index for ductility was measured based on the presence/absence of fracture of the ribbon. The performance index was expressed as follows:
  • Patent Literatures 3 and 4 were published.
  • the components as “Ni-based amorphous alloy having high strength and high corrosion resistance” are disclosed in a broad range. Namely, the component disclosed is Ni (80-w-x-y) Nb w Cr x Mo y P 20-z B z where 0.1 ⁇ W ⁇ 10, 4 ⁇ X ⁇ 18, 3 ⁇ Y ⁇ 12, and 4 ⁇ Z ⁇ 6.
  • Ni-based amorphous alloys disclosed in many references such as the above, most of semimetals include the combinations of P—B, P—C, and P—Si and also alloys are prepared by changing the aforementioned component ratios.
  • Ni 80-x —Cr x -16P-4B are often introduced.
  • Ni—Cr—B were also introduced.
  • Ni-based amorphous alloys use “P”, as a semimetal, which causes delayed fracture, for amorphization or the like. Due to a small amount of Ni, ductility is low, so that it is difficult to apply it and it is not spread widely as an industrial material.
  • the present invention provides amorphous alloys as authentic industrial materials in a broad application range which have the following features by solving the problems such as delayed fracture and ductility.
  • Ni-based amorphous alloy of the present invention is constituted as follows to have the aforementioned features. Namely, the following features are satisfied:
  • the amount (at %) of Ni which is the base element is set to be high.
  • the relationships between the amount (at %) of base substrate Ni and the ductility performance index for the multiple component system are shown in FIG. 2 .
  • the minimum amount of Ni is 63% (at %) or more although there are slight variations depending on the number of components of alloys and kinds thereof.
  • P As a semimetal used for amorphization, “P” which induces delayed fracture is not used.
  • B is used as the base semimetal. It should be noted that when P is not present, it is suitable as a material for a cleaning device of an IC substrate which should be extremely cautious about even slight contamination.
  • the present invention focuses on improvement of ductility.
  • the alloys used besides Ni and B are one or more of Cr, Mo, and Nb.
  • W, V, Ta, Co and the like can be added, but they cannot be added in a large amount (Amount roughly exceeding either Cr, Mo or Nb. For example, each 2 at % or more) in order to secure ductility.
  • the roles of respective components are as follows:
  • Nb Nb; It exhibits excellent corrosion resistance, and with combination of Mo, corrosion resistance is further improved.
  • Amorphous alloys in these component systems are as follows:
  • Ni—Cr—B This amorphous alloy is corrosion resistant not only to nitric acid, but also to sulfuric acid and sodium hypochlorite.
  • All of the aforementioned component systems have corrosion resistance also to phosphoric acid and caustic soda.
  • the amounts of Cr, Mo, and Nb are restricted from the aspect of corrosion resistance. Therefore, when abrasion resistance is requested, the amount of B is dropped to a minimum of 10% and the amounts of Cr and Mo are increased by the amount corresponding thereto to improve hardness.
  • the present invention relates to Ni-based amorphous alloys having the compositions described in Claims. If an appropriate amount of Cr, Mo, Nb, and B are added to Ni, the alloy exhibits excellent ductility (e.g., Ductility performance index 4 mentioned above), corrosion resistance, and delayed fracture resistance.
  • a Ni-based amorphous alloy of the present invention includes 63 at % or more of Ni and only element (B, C, Si, etc.) other than P as a semimetal for amorphization as mentioned above.
  • the semimetal may include, for example, 10 to 25 at % of B and one or more of Cr, Mo, and Nb as remaining main elements.
  • the following component systems are available as examples of the Ni-based amorphous alloys mentioned above. Note that all of the component systems exhibit excellent corrosion resistance to phosphoric acid and caustic soda.
  • the amorphous alloy expressed by the component system of Ni 100-x-y Mo x B y has ductility, excellent delayed fracture resistance, and excellent corrosion resistance performance to hydrochloric acid, sulfuric acid, and hydrofluoric acid under a reductive environment.
  • the amount of Ni is 66 at % ⁇ Ni and x and y of the alloy are in the range of 5 at % ⁇ x ⁇ 21 at % and 10 at % ⁇ y ⁇ 25 at %.
  • the performance exhibits excellent ductility and excellent corrosion resistance to the aforementioned chemicals.
  • the alloy has excellent delayed fracture resistance.
  • the amorphous alloy expressed by the component system of Ni 100-x-y-z Mo x Nb y B z has ductility, excellent delayed fracture resistance, and excellent corrosion resistance performance to hydrochloric acid, sulfuric acid, hydrofluoric acid, and sodium hypochlorite under a reductive environment.
  • the amount of Ni is 71.5 at % ⁇ Ni and x, y, and z in the formula are in the range of 0.1 at % ⁇ x ⁇ 15 at %, 0.1 at % ⁇ y ⁇ 10 at %, and 10 at % ⁇ z ⁇ 20 at %.
  • the performance exhibits excellent ductility and excellent corrosion resistance.
  • the alloy has excellent delayed fracture resistance.
  • the amorphous alloy expressed by the component system of Ni 100-x-y-z Cr x Mo y B z has ductility, excellent delayed fracture resistance, and excellent corrosion resistance performance to hydrochloric acid, sulfuric acid, hydrofluoric acid, and sodium hypochlorite under a reductive environment.
  • the amount of Ni is 64 at % ⁇ Ni and x, y and z in the formula are in the range of 10 at % ⁇ x ⁇ 25 at %, 0 at % ⁇ y ⁇ 10 at %, and 10 at % ⁇ z ⁇ 25 at %.
  • the performance exhibits excellent ductility and excellent corrosion resistance.
  • the alloy has excellent delayed fracture resistance.
  • the amorphous alloy expressed by the component system of Ni 100-w-x-y-z Cr w Mo x Nb y B z has ductility, excellent delayed fracture resistance, and excellent corrosion resistance performance to hydrochloric acid, sulfuric acid, hydrofluoric acid, and sodium hypochlorite under a reductive environment.
  • the amount of Ni is 64 at % ⁇ Ni and w, x, y, and z in the formula are in the range of 0.1 at % ⁇ w ⁇ 15 at %, 0.1 at % ⁇ x ⁇ 20 at %, 0.1 at % ⁇ y ⁇ 10 at %, and 10 at % ⁇ z ⁇ 25 at %.
  • the performance exhibits excellent ductility and excellent corrosion resistance.
  • the alloy has excellent delayed fracture resistance.
  • the amorphous alloy expressed by the component system of Ni 100-X-Y Cr X B y has ductility, excellent delayed fracture resistance, and excellent corrosion resistance to nitric acid, hydrofluoric acid, and sodium hypochlorite under an oxidative environment.
  • the amount of Ni is 63 at % ⁇ Ni and X and Y in the formula are in the range of 20 at % ⁇ x ⁇ 30 at % and 10 at % ⁇ y ⁇ 25 at %.
  • the performance exhibits excellent ductility and excellent corrosion resistance.
  • the alloy has excellent delayed fracture resistance.
  • Ni-based amorphous alloy of the present invention provides comprehensively excellent features such as excellent ductility, delayed fracture resistance, corrosion resistance, and abrasion resistance, and can be developed as an authentic industrial material in a broad application range.
  • FIG. 1 An X-ray diffraction profile for an amorphous ribbon prepared.
  • FIG. 2 A chart showing relationships between the amount (at %) of Ni in the amorphous alloy and the ductility performance index.
  • FIG. 3 Cross-sectional micrographs of the substrate and the amorphous alloy coating formed on the surface thereof by thermal spraying.
  • FIG. 3 ( a ) is a coating of Ni-15Mo-19B
  • FIG. 3 ( b ) is a coating of Fe—Cr—Mo series.
  • FIG. 4 ( a ), ( b ), and ( c ) are explanatory charts showing overview of the delayed fraction test.
  • the Ni-based amorphous alloy according to the present invention can be produced by so-called single roller method or double roller method using one or two cooled rollers. Furthermore, it can be produced by the thermal spraying method using a thermal spraying device with a quenching function.
  • the inventors prepared a ribbon (metallic film) made of a Ni-based amorphous alloy with a single roller method based on the following procedures. Namely, as for each amorphous alloy shown in Table 1, a mixture of pure metals and semimetals of corresponding components was dissolved by high frequency heating under an Ar atmosphere and cast in a Cu mold to obtain mother alloy. This mother alloy was dissolved again by high frequency heating under an Ar atmosphere and sprayed on the surface of a single roller rotating while cooling from the inside to obtain an amorphous ribbon. The thickness of the amorphous ribbon was adjusted to 30 ⁇ m and 60 ⁇ m by changing the number of rotations of the aforementioned single roller. The fact that the ribbon is amorphous was confirmed by observing halo peaks by X-ray diffraction (See FIG. 1 ).
  • An amorphous alloy coating of Ni-15Mo-19B with a good ductility (Ductility performance index: 4) and another amorphous alloy coating of Fe-35Cr-9Mo-8P-8C-8B with a poor ductility (Ductility performance index: 1) were formed on the surface of a substrate (iron material: SS41) with a thickness of 300 microns by thermal spraying.
  • the coating was formed using a thermal spraying device (for example, disclosed in Japanese Unexamined Patent Application Publication No. 2010-22895), wherein a flame containing material particle powder was sprayed using a thermal spraying gun towards the substrate to melt the powder in the flame and to cool the powder and flame with a cooling gas before reaching the substrate.
  • the powder for thermal spraying was produced by gas atomizing method and the alloy compositions were Ni-15Mo-19B and Ni-10Mo-5Nb-13.5B. This powder was used in the aforementioned device to form an amorphous coating on a transport roll for rolling, etc., having a range of thermal spraying of ⁇ 130 ⁇ 300 L. In this case, the substrate temperature was maintained at 100 to 150° C. during the thermal spraying and nitrogen pressure for cooling was 0.2 MPa. Further, an alloy powder of Fe-35Cr-9Mo-8P-8C-8B was thermally sprayed under the conditions of the same-shaped substrate and the same substrate retention temperature.
  • FIG. 3 A cross-sectional photo of the coating formed is shown in FIG. 3 .
  • the coating of the Ni-15Mo-19B ( FIG. 3 ( a )) demonstrates a clean surface without cracks and through-holes. It seems that a difference in the linear expansion between the substrate and the amorphous alloy is erased by ductility.
  • the coating formation of the Fe—Cr—Mo series in FIG. 3 ( b ) the coating becomes amorphous, but numerous cracks are identified, suggested that the quality of the coating is poor.
  • a cushion alloy coating is formed between the amorphous alloy and the substrate.
  • the hardness index HV showing abrasion resistance is 900, indicates sufficient abrasion resistance.
  • the amorphous alloy (aforementioned ribbon, for example) was cut to obtain a test specimen 1 in the shape shown in FIG. 4 ( a ), this was bent with a bending diameter of 4 mm as shown in FIG. 4 ( b ), and then fixed with a tool.
  • the test specimen 1 for example, in that state was immersed in a diluted hydrochloric acid electrolyte solution as shown in FIG. 4( c ) to make the test specimen 1 to be a negative electrode and then electric current at a current density of about 320 A/m2 was passed.
  • a time from the beginning of electrolysis to this time point was measured.
  • the test was conducted with amorphous alloys of 70Fe-10Cr-13P-7C and 66Ni-15Mo-19B. The results are shown in Table 3. The alloy of 70Fe-10Cr-13P-7C containing P was fractured in 7 minutes, whereas 66Ni-15Mo-19B was fractured in 29 minutes, indicated that the tolerance was 4 times greater. Although the relationships between the delayed fracture time in this test and the service life in an actual machine are not clear, it is certain that the service life before the delayed fracture is longer.
  • Ni-based amorphous alloy according to the present invention can be widely used as an industrial material requiring ductility, delayed fracture resistance, corrosion resistance and the like. For example, it can be also used as a surface coating of the pump shaft for carrying acids.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • ing And Chemical Polishing (AREA)
  • Powder Metallurgy (AREA)
  • Continuous Casting (AREA)
  • Coating By Spraying Or Casting (AREA)
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US13/880,280 2010-10-20 2011-10-19 Ni-Based Amorphous Alloy With High Ductility, High Corrosion Resistance and Excellent Delayed Fracture Resistance Abandoned US20130263973A1 (en)

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JP2010-235968 2010-10-20
JP2010235968 2010-10-20
PCT/JP2011/074079 WO2012053570A1 (fr) 2010-10-20 2011-10-19 ALLIAGE AMORPHE À BASE DE Ni AYANT UNE DUCTILITÉ ÉLEVÉE, UNE RÉSISTANCE ÉLEVÉE À LA CORROSION ET UNE EXCELLENTE RÉSISTANCE À LA FRACTURE RETARDÉE

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EP (1) EP2631316A4 (fr)
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KR (1) KR101830924B1 (fr)
CN (1) CN103189539B (fr)
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US9816166B2 (en) 2013-02-26 2017-11-14 Glassimetal Technology, Inc. Bulk nickel-phosphorus-boron glasses bearing manganese
US9863024B2 (en) 2012-10-30 2018-01-09 Glassimetal Technology, Inc. Bulk nickel-based chromium and phosphorus bearing metallic glasses with high toughness
US9863025B2 (en) 2013-08-16 2018-01-09 Glassimetal Technology, Inc. Bulk nickel-phosphorus-boron glasses bearing manganese, niobium and tantalum
US9920400B2 (en) 2013-12-09 2018-03-20 Glassimetal Technology, Inc. Bulk nickel-based glasses bearing chromium, niobium, phosphorus and silicon
US9920410B2 (en) * 2011-08-22 2018-03-20 California Institute Of Technology Bulk nickel-based chromium and phosphorous bearing metallic glasses
US9957596B2 (en) 2013-12-23 2018-05-01 Glassimetal Technology, Inc. Bulk nickel-iron-based, nickel-cobalt-based and nickel-copper based glasses bearing chromium, niobium, phosphorus and boron
US10000834B2 (en) 2014-02-25 2018-06-19 Glassimetal Technology, Inc. Bulk nickel-chromium-phosphorus glasses bearing niobium and boron exhibiting high strength and/or high thermal stability of the supercooled liquid
US10287663B2 (en) 2014-08-12 2019-05-14 Glassimetal Technology, Inc. Bulk nickel-phosphorus-silicon glasses bearing manganese
US10458008B2 (en) 2017-04-27 2019-10-29 Glassimetal Technology, Inc. Zirconium-cobalt-nickel-aluminum glasses with high glass forming ability and high reflectivity
WO2021091074A1 (fr) * 2019-11-06 2021-05-14 아토메탈테크 피티이 유한회사 Corps revêtu
US20210304936A1 (en) * 2020-03-24 2021-09-30 Tdk Corporation Alloy ribbon and magnetic core
US11371108B2 (en) 2019-02-14 2022-06-28 Glassimetal Technology, Inc. Tough iron-based glasses with high glass forming ability and high thermal stability
US11377720B2 (en) 2012-09-17 2022-07-05 Glassimetal Technology Inc. Bulk nickel-silicon-boron glasses bearing chromium
US11905582B2 (en) 2017-03-09 2024-02-20 Glassimetal Technology, Inc. Bulk nickel-niobium-phosphorus-boron glasses bearing low fractions of chromium and exhibiting high toughness

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US20140096873A1 (en) * 2012-10-08 2014-04-10 Glassimetal Technology, Inc. Bulk nickel-phosphorus-boron glasses bearing molybdenum
US9365916B2 (en) 2012-11-12 2016-06-14 Glassimetal Technology, Inc. Bulk iron-nickel glasses bearing phosphorus-boron and germanium
US9556504B2 (en) 2012-11-15 2017-01-31 Glassimetal Technology, Inc. Bulk nickel-phosphorus-boron glasses bearing chromium and tantalum
JP2014132116A (ja) 2013-01-07 2014-07-17 Glassimetal Technology Inc 鉄を含有するバルクニッケル−ケイ素−ホウ素ガラス
CN104278220B (zh) * 2014-09-29 2016-04-13 中南大学 一种高W含量Ni基非晶合金及其制备方法
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CN110387511B (zh) * 2019-08-21 2021-06-29 合肥工业大学 一种Co-Ni-Nb-B系非晶合金条带及其制备方法
CN111570810B (zh) * 2020-05-09 2022-10-11 中国航发北京航空材料研究院 一种深海采油树用耐蚀合金粉末及部件的制备方法

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RU2013122854A (ru) 2014-11-27
KR101830924B1 (ko) 2018-02-22
CN103189539A (zh) 2013-07-03
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