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EP4202067A1 - Procédé de fabrication d'une bande électrique à grains orientés et bande électrique à grains orientés - Google Patents

Procédé de fabrication d'une bande électrique à grains orientés et bande électrique à grains orientés Download PDF

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Publication number
EP4202067A1
EP4202067A1 EP21216455.2A EP21216455A EP4202067A1 EP 4202067 A1 EP4202067 A1 EP 4202067A1 EP 21216455 A EP21216455 A EP 21216455A EP 4202067 A1 EP4202067 A1 EP 4202067A1
Authority
EP
European Patent Office
Prior art keywords
bound
ions
steel
layer
mgo
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.)
Withdrawn
Application number
EP21216455.2A
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German (de)
English (en)
Inventor
Carsten Schepers
Christian Hecht
Alice Sandmann
Andreas Allwardt
Ludger Lahn
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.)
ThyssenKrupp Electrical Steel GmbH
Original Assignee
ThyssenKrupp Electrical Steel GmbH
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 ThyssenKrupp Electrical Steel GmbH filed Critical ThyssenKrupp Electrical Steel GmbH
Priority to EP21216455.2A priority Critical patent/EP4202067A1/fr
Publication of EP4202067A1 publication Critical patent/EP4202067A1/fr
Withdrawn legal-status Critical Current

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    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D8/00Modifying the physical properties by deformation combined with, or followed by, heat treatment
    • C21D8/12Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of articles with special electromagnetic properties
    • C21D8/1277Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of articles with special electromagnetic properties involving a particular surface treatment
    • C21D8/1283Application of a separating or insulating coating
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D3/00Diffusion processes for extraction of non-metals; Furnaces therefor
    • C21D3/02Extraction of non-metals
    • C21D3/04Decarburising
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D8/00Modifying the physical properties by deformation combined with, or followed by, heat treatment
    • C21D8/12Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of articles with special electromagnetic properties
    • C21D8/1216Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of articles with special electromagnetic properties the working step(s) being of interest
    • C21D8/1233Cold rolling
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D8/00Modifying the physical properties by deformation combined with, or followed by, heat treatment
    • C21D8/12Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of articles with special electromagnetic properties
    • C21D8/1277Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of articles with special electromagnetic properties involving a particular surface treatment
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D8/00Modifying the physical properties by deformation combined with, or followed by, heat treatment
    • C21D8/12Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of articles with special electromagnetic properties
    • C21D8/1277Modifying the physical properties by deformation combined with, or followed by, heat treatment during manufacturing of articles with special electromagnetic properties involving a particular surface treatment
    • C21D8/1288Application of a tension-inducing coating
    • CCHEMISTRY; METALLURGY
    • C21METALLURGY OF IRON
    • C21DMODIFYING 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
    • C21D9/00Heat treatment, e.g. annealing, hardening, quenching or tempering, adapted for particular articles; Furnaces therefor
    • C21D9/46Heat treatment, e.g. annealing, hardening, quenching or tempering, adapted for particular articles; Furnaces therefor for sheet metals
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/001Ferrous alloys, e.g. steel alloys containing N
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/008Ferrous alloys, e.g. steel alloys containing tin
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/02Ferrous alloys, e.g. steel alloys containing silicon
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/04Ferrous alloys, e.g. steel alloys containing manganese
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/06Ferrous alloys, e.g. steel alloys containing aluminium
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C38/00Ferrous alloys, e.g. steel alloys
    • C22C38/18Ferrous alloys, e.g. steel alloys containing chromium
    • C22C38/20Ferrous alloys, e.g. steel alloys containing chromium with copper
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01FMAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
    • H01F1/00Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
    • H01F1/01Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
    • H01F1/03Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity
    • H01F1/12Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials
    • H01F1/14Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials characterised by their coercivity of soft-magnetic materials metals or alloys
    • H01F1/147Alloys characterised by their composition
    • H01F1/14766Fe-Si based alloys
    • H01F1/14775Fe-Si based alloys in the form of sheets
    • H01F1/14783Fe-Si based alloys in the form of sheets with insulating coating

Definitions

  • the invention relates to a method for producing a grain-oriented electrical strip that is coated with a forsterite layer, and to a grain-oriented electrical strip with very good adhesion of a forsterite film formed on it.
  • Grain-oriented "electrical strip” is understood to mean steel strips produced by cold rolling, which are provided in a special way with a forsterite layer and optionally with at least one layer additionally applied to the forsterite layer.
  • the cold-rolled steel strip of a grain-oriented electrical strip is also referred to below as “steel substrate” or “steel material”.
  • grain-oriented electrical steels of the type in question are 0.10-0.35 mm thick.
  • the cold-rolled, decarburization-annealed and primary recrystallized steel substrate of grain-oriented electrical strips of the type according to the invention typically consists of, in % by mass, 2.5-4.0% silicon (“Si”), ⁇ 0.30% manganese (“Mn”), ⁇ 0.50% copper (“Cu”), ⁇ 0.065% aluminum (“Al”), ⁇ 0.1% nitrogen (“N”) and optionally one or more elements from the group “chromium (“Cr”) , Nickel (“Ni”), Molybdenum (“Mo”), Phosphorus (“P”), Arsenic (“As”), Sulfur (“S”), Tin (“Sn”), Selenium (“Se”), antimony (“Sb”), tellurium (“Te”), boron (“B”) or bismuth (“Bi”)” with the proviso that the contents of the elements of this group are ⁇ 0.2% in each case, the remainder being iron and unavoidable impurities.
  • Si silicon
  • Mn manganese
  • Cu copper
  • a forsterite layer is built up on the respective electrical steel sheet in conventional production methods by subjecting a steel strip cold-rolled to its final thickness, which is composed within the framework of the general alloy specification given above, to a first annealing in order to bring about primary recrystallization and decarburization of the steel substrate and the Surface of the substrate to oxidize targeted.
  • the surface of the electrical strip treated in this way is then typically coated with a solution containing magnesium oxide (“MgO”) and suitable additives as a protection against adhesion.
  • MgO magnesium oxide
  • the electrical steel strip is wound into a coil and annealed again in the coil in order to effect secondary recrystallization and subsequent purification of the steel from precipitate-forming elements.
  • the anti-adhesive layer which essentially consists of MgO, reacts with the surface of the steel substrate existing oxides, consisting mainly of silicon oxide, and thus forms the desired forsterite layer ("Mg2SiO4"), which is also referred to as a "glass film".
  • This layer of forsterite merges into the steel substrate with roots, which ensures its adhesion to the steel substrate.
  • the forsterite layer can in a further step, such as from the DE 22 47 269 C3 is known, a solution based on magnesium phosphate or aluminum phosphate or mixtures of both with various additives such as chromium compounds and Si oxide are applied and baked at temperatures above 350 °C.
  • the layer system formed in this way on the electrical strip forms an insulating layer which transfers tensile stresses to the steel material, which have a favorable effect on the electromagnetic properties of the electrical strip or sheet.
  • the high-temperature annealing step that forms the forsterite layer typically takes 6-7 days and requires significant energy input. With conventional production methods, it is only after this long annealing period that it can be determined whether the forsterite layer has formed properly or whether it is not sufficiently adhering to the steel substrate. Interventions in the production process to eliminate a faulty formation of the forsterite layer can therefore only be made with a considerable delay. Because during this period the production continues to run, larger quantities of defective electrical steel may be produced until the cause of the defect has been rectified.
  • the task was to develop a process that reliably enables the production of grain-oriented electrical steel strips with an optimally developed forsterite layer that adheres to the steel substrate of the respective electrical steel strip.
  • a grain-oriented electrical strip should be specified in which the forsterite layer adheres optimally firmly to the steel substrate of the electrical strip.
  • the invention has achieved this object in that at least the work steps specified in claim 1 are completed in the production of grain-oriented electrical strips with an optimally adhering forsterite layer. It goes without saying that a person skilled in the art, when carrying out the method according to the invention and its variants and expansion options explained here, adds those work steps not explicitly mentioned here, which he knows from his practical experience that they are regularly used when carrying out such methods .
  • a grain-oriented electrical steel sheet that achieves the above-specified object according to the invention has at least the features specified in claim 5 .
  • the invention during the production of grain-oriented electrical steel, it is possible to use fixed criteria to decide at one point in time whether an intermediate product obtained before high-temperature annealing is suitable for forming a forsterite layer that optimally adheres to the steel substrate of the electrical steel.
  • the invention makes it possible to measure the subsequent adhesive strength of the forsterite layer in the process and thus provides a safe range of process parameters, which leads to perfect adhesive strength of the forsterite layer after annealing.
  • the invention is based on the knowledge that by time-of-flight secondary ion mass spectroscopy (English “Time of Flight Secondary Ions Mass Spectrometry", short “ToF-SIMS"), in which the surface to be examined of the intermediate product present after the decarburizing annealing with Cs Ions are bombarded with an acceleration voltage of 2keV and for analysis with Bi+ ions with an acceleration voltage of 25keV, the adhesive strength of the forsterite layer produced in the following work steps can be predicted.
  • This prediction is based on an evaluation of the proportion of the element Si on the examined surface of the steel substrate which is bound with the element Cs in relation to the proportion of the element Si which is not bound with Cs. The larger this relation is for the examined surface before the annealing step, the better the adhesion of the forsterite layer after the annealing step (step e)).
  • ToF-SIMS is an analytical method for the chemical characterization of surfaces. It is based on the time-resolved detection of secondary ions, which are generated from the examined surface by bombardment with high-energy primary ions (e.g. Bi). These primary ions, directed at the surface to be examined in a short ion pulse, penetrate the upper atomic layers of the surface and release so-called "secondary ions" from it. The kinetic energy of the primary ions is transferred to the released secondary ions, so that the secondary ions are accelerated and run through a drift path until they hit a detector system that records the intensity of the secondary ions as a function of the flight time with high time resolution.
  • primary ions e.g. Bi
  • the material to be examined is bombarded with sputter ions (e.g. Cs) in addition to the primary ions, so that material is continuously removed.
  • sputter ions e.g. Cs
  • the depth-resolved degree of affinity for this binding is the basis of the invention.
  • the intermediate product provided in step a) of the method according to the invention as a cold-rolled and decarburization-annealed steel strip can be produced in accordance with the manner established in the prior art for the production of grain-oriented electrical steel sheets. It is crucial that the steel strip is produced and decarburized with a composition that is typical for grain-oriented electrical steel sheets.
  • step b) of the method according to the invention it is then decided on the basis of the criteria specified according to the invention whether or not the steel strips provided have the potential for the formation of an optimally adhering forsterite layer. If the steel strip in question does not meet the requirements, it is no longer processed, but recycled as scrap and fed back into the steel strip production cycle for the manufacture of grain-oriented electrical steel strips. With the procedure according to the invention, only those cold-rolled steel strips reach the high-temperature annealing (step e)) in which it can be expected that the forsterite layer produced on them will meet the highest requirements with regard to their adhesion to the steel substrate of the electrical strip.
  • the steel substrate of a grain-oriented electrical steel sheet according to the invention consists of a steel which has the alloy specified above for step a) of the method according to the invention.
  • This MgO powder consists of at least 90% by mass of MgO, it being possible for the optionally remaining remainder of the powder to be filled with at least one additive. The sum of the contents of the additives is at most 10% by mass.
  • Additives that can be added to the MgO powder include, for example, titanium oxide, ammonium chloride or antimony chloride, the addition of which controls the density of the later forsterite layer and the gas exchange between the annealing atmosphere during high-temperature annealing and the metal.
  • Each of the measures i) - iii) can, seen alone, contribute to a grain-oriented electrical sheet according to the invention with optimal adhesion To generate forsterite layer, this succeeds particularly safely if all three measures i) - iii) are carried out.
  • the particle size distribution of the MgO powder can be determined in measure i) using methods known per se. For example, there are measuring instruments available on the market, such as the Mastersizer 2000 (see https://www.malvernpanalytical.com/de/support/productsupport/mastersizer-range/mastersizer-2000, accessed on December 7, 2019). Disposal.
  • the pH value can be recorded with any pH measuring device available on the market for this purpose, which enables a continuously updated measurement over a period beginning with the addition of the MgO powder to the citric acid solution.
  • the annealing of the steel strip, which is finally completed in step d), during which the forsterite layer (Mg2SiO4) forms, can also be carried out in a manner known per se.
  • the cold-rolled steel strip obtained after step d) and coated with the anti-tack layer formed from the MgO powder can be wound into a coil and kept in a hood furnace for 10-200 hours at a temperature of 1000-1600 K under an atmosphere that consists of at least 50% H 2 consists.
  • samples P1 - P7 were divided from eight cold-rolled steel strips originating from the normal production process, the respective composition of which is given in Table 1.
  • samples P1 - P8 examined in this way were then coated with an aqueous MgO suspension, the mass of which was adjusted by means of squeezing rollers.
  • the MgO powder used consisted of 94% by mass MgO and 6% by mass TiO 2 .
  • Table 3 shows an example of the result of the investigation of the citric acid activity CAA for samples 1, 2 and 7, with the MgO powder used in samples 1 and 2 complying with requirement iii) of the invention, whereas this is the case with the MgO powder used in sample 7 has been used is not the case.
  • the samples coated in this way were subjected to high-temperature annealing, during which they were kept in a top hat furnace for a period of 24 h at a temperature of 1450 K under a dry atmosphere of pure hydrogen.
  • the strength of the adhesion of the forsterite layer on the initially provided, cold-rolled steel substrate was determined on the samples P1 - P8 produced and tested in the manner explained above.
  • a sample was clamped in a cone mandrel bending device. The sample was bent 180° around a cone mandrel ranging continuously from a bending radius of 5 mm (cone apex) to 30 mm (cone base). After removal, the bending radius from which the coating flaked off was checked. The smaller this bending radius, the better the adhesion.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Electromagnetism (AREA)
  • Manufacturing & Machinery (AREA)
  • Dispersion Chemistry (AREA)
  • Power Engineering (AREA)
  • Chemical Treatment Of Metals (AREA)
EP21216455.2A 2021-12-21 2021-12-21 Procédé de fabrication d'une bande électrique à grains orientés et bande électrique à grains orientés Withdrawn EP4202067A1 (fr)

Priority Applications (1)

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EP21216455.2A EP4202067A1 (fr) 2021-12-21 2021-12-21 Procédé de fabrication d'une bande électrique à grains orientés et bande électrique à grains orientés

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Application Number Priority Date Filing Date Title
EP21216455.2A EP4202067A1 (fr) 2021-12-21 2021-12-21 Procédé de fabrication d'une bande électrique à grains orientés et bande électrique à grains orientés

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EP4202067A1 true EP4202067A1 (fr) 2023-06-28

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2247269C3 (de) 1971-09-27 1981-05-14 Nippon Steel Corp., Tokyo Verfahren zur Herstellung einer isolierenden sowie die Magnetostriktions-Charakteristika und den Eisenverlust verbessernden Schicht auf einem Silicimstahlblech
EP0239688A1 (fr) * 1986-04-03 1987-10-07 Nippon Steel Corporation Séparateur pour le recuit final d'une tôle en acier électrique à grain orienté
WO2003000951A1 (fr) 2001-06-22 2003-01-03 Thyssenkrupp Electrical Steel Ebg Gmbh Tole electrique a cristaux orientes dotee d'un revetement electriquement isolant
EP1411139A1 (fr) * 2001-07-16 2004-04-21 Nippon Steel Corporation Tole magnetique unidirectionnelle a densite de flux magnetique tres elevee, a caracteristiques de pertes dans le fer et de revetement dans un champ magnetique puissant excellentes, et procede de production associe
JP2007138199A (ja) * 2005-11-15 2007-06-07 Jfe Steel Kk 一方向性電磁鋼板の製造方法
DE102015114358A1 (de) * 2015-08-28 2017-03-02 Thyssenkrupp Electrical Steel Gmbh Verfahren zum Herstellen eines kornorientierten Elektrobands und kornorientiertes Elektroband

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2247269C3 (de) 1971-09-27 1981-05-14 Nippon Steel Corp., Tokyo Verfahren zur Herstellung einer isolierenden sowie die Magnetostriktions-Charakteristika und den Eisenverlust verbessernden Schicht auf einem Silicimstahlblech
EP0239688A1 (fr) * 1986-04-03 1987-10-07 Nippon Steel Corporation Séparateur pour le recuit final d'une tôle en acier électrique à grain orienté
WO2003000951A1 (fr) 2001-06-22 2003-01-03 Thyssenkrupp Electrical Steel Ebg Gmbh Tole electrique a cristaux orientes dotee d'un revetement electriquement isolant
EP1411139A1 (fr) * 2001-07-16 2004-04-21 Nippon Steel Corporation Tole magnetique unidirectionnelle a densite de flux magnetique tres elevee, a caracteristiques de pertes dans le fer et de revetement dans un champ magnetique puissant excellentes, et procede de production associe
JP2007138199A (ja) * 2005-11-15 2007-06-07 Jfe Steel Kk 一方向性電磁鋼板の製造方法
DE102015114358A1 (de) * 2015-08-28 2017-03-02 Thyssenkrupp Electrical Steel Gmbh Verfahren zum Herstellen eines kornorientierten Elektrobands und kornorientiertes Elektroband

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