ARTICLE IN PRESS

Journal of Magnetism and Magnetic Materials 269 (2004) 333340

Columnar grain growth in non-oriented electrical steels

!& ! F. Kovac, M. D& ubinsky*,1, Y. Sidor z
Institute of Materials Research of Slovak Academy of Sciences, Steel Metallurgy, Watsonova 47, Ko&ice 043 53, Slovak Republic s Received 21 March 2003; received in revised form 10 July 2003

Abstract Decarburising annealing in the two-phase region is a known method to provide columnar grain growth in silicon non-oriented electrical steel that can improve magnetic properties. This method includes long-term preliminary annealing in vacuum and subsequent decarburising annealing in a wet hydrogen atmosphere (J. Mater. Eng. Perform. 5 (1996) 316). In the present paper an alternative method to produce the columnar microstructure in low and medium silicon non-oriented electrical steel without preliminary vacuum annealing is described. The inuence of applied annealing temperature regimes and atmospheres on the development of the material microstructure are studied under the conditions of industrial continuous annealing. The dependence of the nal material texture on the aforementioned conditions is presented. r 2003 Elsevier B.V. All rights reserved.
PACS: 81.30; 81.40 Keywords: Non-oriented electrical steel; Decarburising annealing in intercritical region; Columnar microstructure; Texture

1. Introduction A lot of work has been carried out in steels to tailor the properties. A difculty in many cases is the inhomogeneity of the microstructure and the texture of steel as a result of the production process. This is of particular importance in electrical steels. For low-carbon steel it is possible to apply a special thermal treatment that leads to the columnar-grained microstructure with a spe*Corresponding author. Tel.: +42155633-81-15; fax: +42155633-71-08. E-mail addresses: kovacf@saske.sk (F. Kov! c), a& dzub@saske.sk (M. D& ubinsk! ). z y 1 At the moment Marie Curie Fellow at Swinden Technology Centre, Corus Research, Development & Technology, Moorgate, Rotherham S60 3AR, UK.

cic type of the texture, thus avoiding the inhomogeneity. Columnar-grained microstructures can be obtained in solid state either by directional annealing using a temperature gradient [2] or by decarburising annealing in the intercritical region [3]. The former method is applicable when a reasonably large volume of material is being treated. The latter method is suitable for columnar microstructure growth in thin sheets, when the microstructure is aligned with normal direction to the sheet plane. The aim of the present work was to investigate development of the columnar-type microstructure in thin strips of non-oriented electrical steel. The advantages of the cube texture in electrical steel sheets have been recognised during the last

0304-8853/$ - see front matter r 2003 Elsevier B.V. All rights reserved. doi:10.1016/S0304-8853(03)00628-0

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half of the 20th century. The (1 1 0) /0 0 1S and (1 0 0) /0 v wS textures are ideal ones for the grain-oriented and non-oriented electrical steels, respectively. But growth of the cube-oriented grains is not possible by applying ordinary rolling and annealing processes. Assumus rst pointed out that high-temperature annealing of very thin SiFe sheets leads to an abnormal growth of the cube grains [4]. In this case, the secondary recrystallisation process of the cube-oriented grains is controlled by the gasmetal interfacial energy, which is lowest at the (1 0 0) orientation in a high-purity inert atmosphere or in vacuum [57]. Another possible method to increase the proportion of the cube-oriented grains is cross-rolling and subsequent high-temperature annealing of the silicon steel sheets [8]. Recently developed process for cube-oriented grain growth in silicon steels consists of annealing in vacuum to remove the manganese and subsequent annealing in the g or a g two-phase region in a decarburising atmosphere [1,9], or high-temperature annealing in vacuum with application of an oxide separator between the sheets [10]. Nevertheless, all these processes cannot be applied under industrial conditions. The latter two processes themselves are diffusion-induced a g-a phase transformation in the surface layer and subsequent abnormal growth of the ferrite surface grains into the two-phase matrix towards the mid-thickness of the sheet as a result of the material decarburisation. Such abnormal grain growth, assisted by the decarburisation process, under optimum conditions results in the formation of a columnar microstructure [11]. The columnar microstructure can also be formed during the carburisation. In this case it is austenitic columnar grains that grow. If the decarburisation/carburisation process occurs in the binary FeC system, then the creation of the two-phase zone is not observed. In the case of the ternary FeCSi system, the austenite+ferrite transition zone is likely to be formed. Formation of the a g region is typically expected during carburisation, even if the content of Si is minimal. Contrary to carburisation, during decarburisation the two-phase region might not be formed even at

high contents of Si [12]. According to Kowalik and Marder [13], the columnar microstructure in the steels is formed only if the decarburisation annealing is performed in the a g region and a sharp interface exists between the decarburised ferrite and two-phase area. Generally, it is suggested that formation of the columnar microstructure would be expected when the velocity of the transformation front is higher than the nucleation speed of the phase transformation [14]. As was mentioned above, apart from decarburisation the temperature gradient in the material could be another way to provide conditions for columnar grain growth, ferritic one in Ref. [15]. Nevertheless, the decarburisation process in the two-phase region can be an efcient controlling mechanism for obtaining the columnar ferritic microstructure in the solid state. Decarburisation in steel proceeds according to the following chemical reactions [16]: CFe 2H2 CH4 ; CFe H2 O CO H2 ; CFe CO2 2CO; 1 2 3

where reaction (1) is typical for the temperature range of To530 C, reaction (2)FT  6702690 C, and reaction (3)FT > 700 C. Nonoriented electrical steel sheets, regardless of production type, i.e. semi- processed (SP) or fully processed (FP), are typically given a nal annealing in the temperature range where Eq. (1) is valid. Usually for an effective decarburisation process, the decarburising atmosphere has to be wet, because the rate of chemical reaction (1) is proportional to the so-called oxidation potential PH2 O =PH2 : The optimum value of the oxidation potential of the decarburising atmosphere (if PH2 =PN2 X0:5) is B0.5 [16]. The theory of decarburisation kinetics with phase transformation (i.e. g-a or a g-a) had been developed by Wagner [17], Swisher [18], and Pyyry and Kettunen [19]. For the case of an FeC alloy with an initial microstructure of a g at the decarburisation temperature Ar1 oToAr3 ; the

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following equation is valid [18,19]: s   1 6Df Cb t Cb % Ci C Ci ; a 3Ci bCb 2

% where C is the average carbon concentration after decarburisation (in wt%), Ci is the initial carbon concentration, a is the sheet half-thickness in cm, Df is the diffusion coefcient of carbon in ferrite in cm2/s, Cb is the carbon concentration in ferrite in equilibrium with the austenite, t is time in seconds and the constant b 2 [18] or b 3 [19]. Furthermore, according to Swisher and Smith [18,20]: Df 0:256 e2400=RT ; Cb 0:1395 1:099 10 T;
4

inhibits the diffusion of the carbon to the surface and its removal. Hence, the annealing temperature as well as the content and the dew point of the decarburising atmosphere are crucial factors that inuence development of the columnar microstructure during decarburisation in the two-phase region. The main goal of the present work was to nd the optimum conditions for obtaining the proper columnar microstructure with depressed deformation texture component and increased cube or near-cube one.

5 6

2. Experiment Both SP and FP types of the electrical nonoriented steel were used as experimental material (see Table 1). The thickness of both SP and FP sheets was 0.65 mm. SP steel samples were taken from the industrial process after temper rolling and samples of FPafter cold rolling. The samples were laboratory annealed in the decarburising atmosphere (cracked ammonia with dew point +35 C) according to the stepped-temperature schedule (see Fig. 1) in the intercritical region. Three different heating rates V1 > V2 > V3 to temperature T1 have been applied with xed initial and subsequent temperatures and times, T1 ; T2 ; t1 and t2 (see Table 2). T1 and t1 were designed to result in a ne primary recrystallised microstructure and a thin decarburised a-region on the sheet surface. T2 was chosen with the aim to provide the efcient decarburisation of the material and was the same for both steels. The total time of annealing was chosen to match that of typical industrial continuous annealing. The textures of all laboratory treated samples and corresponding samples from the industrial

where R is the universal gas constant and T is the temperature in K: If the initial microstructure is g; rather than a g; the decarburisation develops a concentration gradient in g, and then the following equation is applicable [18]: " p 1 % 2kCa Df t C Ci a # p 1:128Ci Ca Da t expk2 Df =Da p ; 7 1 erfk Df =Da where Ca is carbon concentration in austenite in equilibrium with ferrite, and Da ; the diffusion coefcient of carbon in austenite in cm2/s, is: Da 0:07 0:06Ci e32000=RT ; 8

k is a function of Ci and T; and can be established empirically. According to Marder et al. [21], the maximum decarburisation rate is around 815 C and is virtually independent of the initial C content. The decrease of the decarburisation rate at T > 816 C can be explained by a transition from the internal oxidation mode to the external one [22]. At lower temperatures (internal oxidation), the base metal matrix is available for the diffusion of carbon to the surface of the material. At TB8102820 C, the commencement of the external oxidation is observed, when a continuous layer of the oxide is present at the oxidation front, which

Table 1 Chemical composition of steel (in wt%) Steel SP FP C 0.05 0.03 Mn 0.36 0.38 Si 0.24 1.01 P 0.068 0.134 S 0.008 0.008 Al 0.109 0.157 N 0.005 0.007

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T1 T2 temperature

air cooling

utilising the Epstein strip of the dimensions of 305 30 mm2. SSTs have been conducted at frequency of 50 Hz.

3. Results and discussion After primary recrystallisation has nished, both steels under investigation had a strong texture gradient normal to the plane of the sheet. In Fig. 2, the IPF map (longitudinal cross-section) of the sample of the SP steel after primary recrystallisation is shown. From this map, the domination of the specic orientations within different bands through the sheet thickness is obvious. In Fig. 3, ODFs of the specic steel states at j2 45 are presented. It is obvious that after the primary recrystallisation, near the sheet surface the texture has developed a strong y0 -bre /0 0 1S||ND and a weak (1 1 0) [111] peak (Fig. 3a, SP steel), and contrary to this, the texture in the mid-thickness has a strong J-component (1 1 4) [110] (Fig. 3b, SP steel). Therefore, during the subsequent secondary recrystallisation process assisted by the decarburisation, when grains are growing from the surface region towards the centre, it is possible to expect strong cubic/near cubic texture components in the nal state. In Figs. 4a and b, development of the columnar microstructure in the SP steel during columnar annealing with the optimum heating rate V is shown. The sample in Fig. 4a was taken after the nish of the rst stage of the annealing (T1 ; t1 ), when thin layer of the columnar microstructure is formed in the surface regions. During the second stage of the annealing at T2 ; the decarburisation promotes the growth of the ferrite columnar grains from the surface region towards the two-phase middle region of the sheet. After the nish of the decarburisation process at T2 ; the microstructure is fully ferritic and grains have columnar shape (see Fig. 4b). Highly non-stable conditions of grain growth near the sheet surface leads to the formation of a thin layer of inhomogeneous relatively ne ferritic grains at the surface. The microstructure of the same SP steel annealed according to the standard EN 10 126/95 has a

time

Fig. 1. Schematic schedule of decarburising annealing in the intercritical region.

Table 2 Parameters of laboratory decarburising annealing Steel SP FP t1 (s) 120140 130150 T1 ( C) 870890 900920 t2 (s) 210240 240270 T2 ( C) 800820 810830

processing were measured in longitudinal section by means of the TSL EBSD system linked with the Phillips XL40 SEM microscope utilising the Orientation Imaging Microscopy (OIMt) software package. Results of the measurements are presented in the form of inverse pole gure (IPF) maps and spatial diagrams of specic sections of the orientation distribution function (ODF) utilising Bunge Euler angles. In the case of the relatively ne polygonal microstructure with a mean grain size of E40 mm, the ODF was calculated from the whole thickness of the sheet, i.e. from an area of 0.65 1.47 mm2. For a reasonable description of the texture of the coarse columnar microstructure samples, the data from six random cross-sections of 0.65 1.47 mm2 were collected, and the ODF was created from the merged batch of the data of all six areas. The magnetic properties of the steel were measured using modied Single Sheet Test

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Fig. 2. IPF map of the longitudinal cross-section of the primarily recrystallised SP steel strip, full thickness.

Fig. 3. ODFs, j2 45 : (a) SP steel after primary recrystallisation, subsurface at 1 of sheet thickness; (b) SP steel after primary 8 recrystallisation, mid-thickness; (c) FP steel after decarburising annealing, sample with columnar microstructure, laboratory experiment; (d) FP steel after decarburising annealing, sample with polygonal microstructure, industrial processing.

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300 m
(a) (b)

300 m

300 m
(c) (d)

300 m

300 m
(e) (f)

300 m

Fig. 4. Microstructure of samples under investigation, magn. 60: SP steel, at the commencement of the second part of columnar annealing (T2 ; t1 ); SP steel, after the columnar annealing; SP steel after the customer annealing according to EN 10 126/95; FP steel after the continuous industrial annealing; FP steel after the columnar annealing with heating rate of V2 to T1 ; FP steel after the columnar anneal with heating rate of V1 to T1 :

polygonal and highly inhomogeneous microstructure (see Fig. 4c). In Figs. 4e and f, the inuence of the heating rate V V1 > V2 during annealing in the intercri-

tical region according to the schedule in Fig. 1 on the microstructure of the FP steel is studied. If the material is heated with a low heating rate V2 ; intensive normal grain growth proceeds

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!c F. Kova& et al. / Journal of Magnetism and Magnetic Materials 269 (2004) 333340 Table 3 Electromagnetic properties of steels under investigation Steel Columnar microstructure, laboratory annealing B25 (T) SP FP 1.69 1.7 P1:0 (W/kg) 2.05 1.95 Polygonal microstructure, industrial annealing B25 (T) 1.65 1.66 P1:0 (W/kg) 2.53 2.95 339

simultaneously with the decarburisation, and the nal material has an inhomogeneous polygonal microstructure (Fig. 4e). If heating to T1 is realised with a high heating rate V1 ; and the holding time t1 at T1 is short, instead of the equiaxed grain growth, the abnormal columnar grain growth, assisted by the decarburisation process, is observed at T2 (see the nal microstructure after this process in Fig. 4f). The same material treated under the industrial conditions (continuous annealing) has the polygonal inhomogeneous microstructure (Fig. 4d) similar to the laboratory-annealed steel in the two-phase region with a low heating rate to T1 : In Figs. 3c and d, the ODF at j2 45 of the FP steel sample with the columnar microstructure is compared to the corresponding ODF of the same steel sample with the polygonal industrial microstructure. The texture of the former sample has a strong cubic H-component (0 0 1) [110] and weakly developed J component (1 1 4) [110]. The texture of the latter one is fairly random with a weak non-uniform y0 -bre, weak J component and weak (1 1 0) [111] peak. Hence, the intensity of the cubic orientation is higher in the sample with the columnar microstructure. Also in both these textures the absence of g-bre is registered. Increasing cubic component and depressing intensity of the g-bre are reected in an improvement of the magnetic properties of the material (see Table 3). Generally, after the primary recrystallisation, the material under investigation has the highest density of cube/near cube-oriented grains not right on the surface, but in a subsurface layer. To increase the probability of selective abnormal growth of the cube-oriented primary recrystallised

grains assisted by the decarburisation process, it is necessary to establish the optimum conditions of the cold/temper rolling. This can be achieved by the optimisation of the rolls radii, reduction value, roughness of rolls, etc. [2325]. These optimum conditions of cold deformation should provide a wide band of the cube-oriented primary recrystallised grains as close to the steel surface as possible. Another possible way to increase the probability of abnormal growth of the cube grains in the primary recrystallised matrix is adjustment of the annealing regime in the intercritical region. Under specic conditions of the decarburisation in the two-phase region, it is possible to expect the creation of continuously growing ferritic zones inside of the two-phase region (deeper than the a=a g front) due to the intensive redistribution of C and Si atoms near the surface of the sheet [11]. In such a situation, the nucleation of the abnormal grain growth at some sheet depth increases the probability that these grains have the cube orientation. Another process, that could increase the probability of the abnormal growth of cubic grains, is a special chemical treatment of the steel surface. Grains with different orientations react in a different way with the chemical reagent. The formation of the reaction product layers of the different thickness on the grains with different orientations can be expected. By nding proper chemical reagent and regime of the treatment, it is possible to provide a decrease of the rate of the decarburisation process of the non-cube-oriented primary recrystallised grains. A stronger cubic component of the nal texture is expected in this case as a result of growth advantage of cubeoriented grains of the primary recrystallised microstructure.

4. Summary 1. The proposed two-step decarburising continuous annealing process in the intercritical region of non-oriented electrical steels with either low or medium content of Si leads to the columnar microstructure of the nal sheet.

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340 !c F. Kova& et al. / Journal of Magnetism and Magnetic Materials 269 (2004) 333340 [4] F. Assumus, K. Detert, G. Ibe, Zur. Metallk. 48 (1957) 344. [5] K. Detert, Acta Metall. 7 (1959) 589. [6] J.L. Walter, Acta Metall. 7 (1959) 424. [7] J.L. Walter, C.G. Dunn, Trans. Metall. Soc. AIME 218 (1960) 914. [8] S. Taguchi, A. Sakakura, Kinzoku Butsuri (in Japanese) 7 (1968) 221. [9] T. Tomida, J. Appl. Phys. 79 (1996) 5443. [10] T. Tomida, N. Sano, K. Ueda, K. Fujiwara, N. Takahashi, J. Magn. Magn. Mater. 254255 (2003) 315. [11] V.I. Movchan, N.A. Grudeva, Russ. Metall. 1 (1983) 121. [12] B.I. Movchan, V.V. Vladimirova, Izv. Akad. Nauk. SSSR, Met. 4 (1982) 91 (in Russian). [13] J.A. Kowalik, A.R. Marder, In: G.W. Lorimer (Ed.), Proceedings of the Phase Transformation87, Cambridge, UK, July 1987, The Institute of Metals, 1988, p. 482. [14] T. Okita, T. Tomita, K. Nakaoka, Tetsu-to-nagane 70 (1984) 2120 (in Japanese). [15] K. Kim, J.H. Beynon, C.M. Sellars, Scr. Mater. 44 (2001) 141. [16] B.M. Mogutnov, L.P. Emeljanenko, A.A. Kononov, A.I. Rogov, L.A. Shvartsman, Physical Chemistry of Electrical Steel Treatment Processes (in Russian), Metallurgija, Moscow, 1990. [17] C. Wagner, J. Metals 4 (1952) 91. [18] J.H. Swisher, Trans. Metall. Soc. AIME 242 (1968) 763. [19] J. Pyyry, P. Kettunen, Scand. J. Met. 2 (1973) 265. [20] R.P. Smith, Trans. Metall. Soc. AIME 242 (1962) 105. [21] A.R. Marder, S.M. Perpetua, J.A. Kowalik, E.T. Stephenson, Metall. Trans. A 16A (1985) 1160. [22] W.F. Block, N. Jayaraman, Mater. Sci. Tech. 2 (1986) 23. [23] A.D. Rollett, M.L. Storch, E.J. Hilinski, S.R. Goodman, Metall. Mater. Trans. A 32A (2001) 2595. [24] L. Kestens, J.J. Jonas, P. van Houtte, E. Aernoudt, Metall. Mater. Trans. A 27A (1996) 2347. [25] R. Kawamata, T. Kubota, K. Yamada, JMEPEG 6 (1997) 701.

2. The texture of the columnar microstructured material has a stronger cube component in comparison to the same steel with the polygonal microstructure. 3. The efciency of the development of the columnar microstructure with preferable cube orientation could be increased by the optimisation of the cold/temper rolling parameters, application of a proper regime of decarburising annealing in the intercritical range or by the special chemical treatment of the steel surface before annealing.

Acknowledgements This work was supported by the Slovak Grant Agency VEGA, project No. 2/1063/21. Authors are grateful to the Corus group for the provided opportunity to conduct texture measurements at Swinden Technology Centre, Corus Research, Development and Technology under Marie Curie Host Industrial Fellowship scheme.

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