Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.

1, 2006

Current Status of Rare-Earth Permanent Magnet Research in USA

HADJIPANAYIS George C.1, LIU Jinfang2, GABAY Alexander1 and MARINESCU Melania1
(1. Department of Physics & Astronomy, University of Delaware, 223 Sharp Lab., Newark, DE 19716, USA
2. Electron Energy Corporation, 924 Links Ave, Landisville, PA 17528, USA)

Abstract. In the paper, we summarize the USA research activities in the past two years on high performance rare earth (R) based (nano)composite, nanostructured and hybrid permanent magnets. The work discussed is organized in three major sections (i) isotropic magnets based on the R2Fe14B hard phase, (ii) anisotropic magnets based on the R2Fe14B hard phase and (iii) magnets with a R-Co hard phase (1:5 and/or 2:17), including ultrahigh temperature Sm-Co magnets, Sm-Co permanent magnets with almost zero reversible temperature coefficient of residual induction for critical applications and ultrahigh temperature Sm-Co magnets with small reversible temperature coefficient of residual induction. Keywords: rare earth permanent magnets; nanocomposite magnets; hybrid magnets; high-temperature magnets; R2Fe14B; SmCo5; Sm2Fe17; exchange coupling; magnetostatic coupling; die-upsetting

1 Introduction
For the past few years, research for the development of advanced permanent magnets has been focused on the optimization of the magnetic performance of rare earth based (nano)composite and nanostructured magnets based on Nd-Fe-B and Sm-Co with or without a cellular structure, and the design of new hybrid magnets. According to the theoretical models, the nanocomposite magnets composed of a high magnetocrystalline anisotropy (or "hard") phase and a high-magnetization (or "soft") phase, have the potential to become about two times stronger than the currently existing magnets [1,2]. The typical hard phases used are the R2Fe14B, SmCo5 and Sm2Fe17 compounds, while the soft phase is usually -Fe(Co). The condition is that at least the hard magnetic phase is fully oriented (anisotropic) and the structure is refined to the nanoscale to allow an intergrain exchange coupling. However, our latest studies showed that an enhanced remanence effect and increased maximum energy product (BH)max can also be obtained in bulk composite magnets with grain size exceeding the nanoscale range suggesting that a positive magnetic coupling can also originate from magnetostatic interactions [3]. The macroscopic magnetic anisotropy derived from the crystallographic texture can be achieved by hot plastic deformation, usually via die-upsetting. The experimental results showed that this technique is very successful for R-rich R2Fe14B (R=rare earth) [4], somewhat effective for SmCo5 and PrCo5 [5] but ineffective for Sm2Co17 [6]. The R2Fe14B-based systems are important as high maximum energy product permanent magnets

used at lower temperatures, while the Sm2Co17 and SmCo5 magnets are mainly used for high temperature applications due to their high Curie temperatures. In this paper, we review the latest results on the current efforts in USA, to develop high performance rare earth permanent magnets, and to optimize their magnetic performance.

2 Isotropic magnets based on the R2Fe14B hard phase

Following our past experience, the efforts in producing isotropic nanocomposite R2Fe14B/-Fe ribbons at the University of Delaware were continued with a successful increase of the maximum energy products (BH)max to above 20 MGOe in ribbons with the following alloy compositions: Pr9Fe85B6, Pr5Nd5Fe79Co5B6 and Pr9Co5Fe80B6. Enhanced values of (BH)max were obtained by optimizing the temperature of the melt at ejection onto the quenching wheel, which then allowed the formation of a uniform nanophase structure. By keeping the wheel speed constant at its optimum value of 18 m/s, the alloy was spun at different ejection temperatures in the range of 13001500 oC. The maximum squareness of the demagnetization curve, associated with the highest value of the reduced remanence Mr/Ms = 0.8 and (BH)max = 21 MGOe, was obtained at an ejection temperature of 1360 oC [7]. Isotropic, nearly fully-dense Pr2Fe14B/-Fe nanocomposite magnets have also been prepared by underwater explosive shock consolidation at University of Texas at Arlington [8]. The plastic

Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.1, 2006

deformation of the powders with solid-state interfacial bonding of the ribbon flakes occurred during shock compaction ensuring a density close to the bulk value. The compacting procedure allowed the retention of the nano-scale structure, and an even further refinement of the grain size necessary for the exchange coupling between the hard and soft phases. The following values of the magnetic hysteresis parameters were reported: coercivity Hc of 6.56 kOe, remanence Mr of 95 emu/g, and maximum energy product (BH)max of 14 MGOe. The magnetic properties were proven to be better than those of resin-bonded magnets, since the magnetic dilution was avoided. The low values of energy products reported so far are attributed to the isotropic nature of the magnets. However, much higher values can be obtained in textured anisotropic magnets.

3 Anisotropic magnets based on the R2Fe14B hard phase

3.1 Single alloy technique Development of anisotropic two-phase R2Fe14B / -Fe composite magnets has been a challenge in the past few years mainly because of their theoretically predicted giant energy product (100 MGOe in ref. [2]). Hot plastic deformation is known to be an effective technique for inducing texture in nanocrystalline R-rich (overstoichiometric) RFeB magnets, but this still remains a challenge for the R-lean (understoichiometric) RFeB alloys. Typically, texture develops successfully in the presence of a Rrich phase, which is liquid at the temperature of deformation and provides a diffusion path that is necessary for the growth of favorably oriented grains [4]. Even though our earlier experiments led to the development of anisotropic understoichiometric R-Fe-B magnets, by die-upsetting blends of under- with over-stoichiometric alloys, the texture was induced only in the over-stoichiometric component [10]. On the other hand, the RF rapid inductive compaction technique proved to be highly effective in obtaining fully dense Nd-Fe-B magnets with 4 - 12 at.% Nd [9]. In order to enhance the deformability and texture development in the R2Fe14B / -Fe composite alloys processed by hot pressing followed by hot deformation via die-upsetting, the influence of the addition of Cu and Ga has been studied at the University of Delaware. The amorphous or partially amorphous precursors were obtained by (i) mechanical milling of nominally stoichiometric (12

at% R) alloys and (ii) melt spinning of understoichiometric (5-11.25 at% R) alloys. The milling was done for 4 hours in argon. Melt spinning was performed at a surface wheel speed of 26 m/s. The alloys were consolidated at 780810 C and subsequently die-upset by 7080% of their original height at 810825 C. It should be noted that, though the homogenized ternary Pr12Fe82B6 alloy contains practically no -Fe (0.3 wt%), in the dieupset magnet, the amount of the -Fe phase increases to 10.8 wt%. The die-upset magnet prepared from Pr12Fe80Cu1Ga1B6 contained as much as 17.2 wt% -Fe. The effect of Cu content on the properties of three different series of die-upset magnets is shown in Fig. 1. The intrinsic coercivity decreases monotonically with increasing the Cu content, while the remanence and maximum energy product increase with the addition of up to 1 at% Cu. For the alloys with Pr, the increase is larger than for those with Nd. The largest increases of 4Mr and (BH)max are observed for the Pr-based alloys doped with Ga. The remanence and energy product of the die-upset alloys with a nominal composition of Pr12Fe81xCuxGa1B6 increase from 10 kG and 16.1 MGOe for x=0 to 13 kG and 23.4 MGOe for x=1, respectively. Similar effects were observed in the case of under-stoichiometric melt-spun alloys (Fig. 2). While the PrFeB and PrFeCoB magnets are isotropic, the Cu-added magnets display a distinctly anisotropic demagnetization behavior. Due to the induced anisotropy, the remanence measured parallel to the pressure direction increases from 8.8 kG for Pr11.25Fe77.75Co5B6 to 10.9 kG for Pr11.25Fe76.75Co5Cu1B6. However, this 24% gain of 4Mr is accompanied by a significant loss of Hc, which drops from 4.7 to 2.7 kOe, and the increase in (BH)max is relatively modest, from 12.1 to 14.9 MGOe. Simultaneous addition of Cu and Ga increases (BH)max of the die-upset magnet from 12.2 MG Oe for Pr11.25Fe82.75B6 to 18.4 MG Oe for Pr11.25Fe80.75Cu1Ga1B6. The effect of Cu and (Cu,Ga) additions on the anisotropy of die-upset magnets is the same as in the case of mechanically milled alloys. TEM investigations on magnets fabricated from the melt-spun and annealed Pr11.25Fe80.75Cu1Ga1B6 alloys showed that the hotpressed magnet consists of equiaxed grains about 30 nm in size, whereas die upsetting forms a microstructure of oriented platelet grains with a long axis of 100200 nm and a short axis of 4070 nm, with the later one oriented along the pressure direction (Fig. 3).

Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.1, 2006

(a)

(b)

Fig.3 TEM microstructures of (a) hot-pressed and (b) dieupset Pr11.25Fe80.75Cu1Ga1B6 magnets made from the meltspun and annealed (for 30 min at 500 C) alloy. The labels indicate grains of the -Fe phase in the die-upset sample. Fig.1 Effect of Cu content on (a) maximum energy product, (b) remanence and (c) intrinsic coercivity of Nd12Fe82xCuxB6 (1), Pr12Fe82xCuxB6 (2) and Pr12Fe81xCuxGa1B6 (3) die-upset magnets made from mechanically milled alloys.

Fig.2 Demagnetization curves of (a) Pr11.25Fe82.75B6, (b) Pr11.25Fe77.75Co5B6, (c) Pr11.25Fe76.75Co5Cu1B6 and (d) Pr11.25Fe80.75Cu1Ga1B6 die-upset magnets made from meltspun alloys. Curves were measured parallel (solid lines) and perpendicular (broken lines) to the pressure direction.

In an attempt to obtain anisotropic 2:14:1 / -Fe magnets with a larger amount of the -Fe phase, a series of melt-spun R-lean alloys, (Pr0.8Tb0.2)zFe93zCu1B6 with z = 5, 6, 7 and 8 (-Fe phase is up to 63 wt% in the case of z = 5) have been prepared [11]. The alloys were doped with Tb in order to compensate for the detrimental effect of Cu on Hc. All four melt-spun alloys were successfully hot-pressed into fully dense magnets and subsequently die upset. The increase in the -Fe content with decreasing z was consistently accompanied by an increase in remanence. However, because of the dramatic decrease of Hc (0.7 kOe for z = 5), the enhanced remanence measured parallel to the applied field, 4Mr||, did not lead to an enhanced (BH)max. Moreover, the Mr||/Mr values of 1.1 - 1.2 indicates that no significant texture was developed by die-upsetting in the magnets with 5 - 8 at. % R. The TEM microstructure of these die-upset magnets revealed only equiaxed grains. 3.2 Blending technique Anisotropic (nano)composite magnets were prepared at University of Delaware by hot-pressing followed by hot deformation via die-upsetting of blends composed of higher-coercivity R-rich and higher-magnetization R-lean ribbon powders. The two components had the nominal compositions: (Nd0.96Dy0.04)14Fe75Co4.5Ga0.5B6 or (Nd0.75Dy0.25)14Fe75Co4.5Ga0.5B6 (as R-rich ribbons) and (Nd0.94Dy0.06)4Fe90Nb2B4 (as R-lean ribbons). The hot pressing has been performed in the temperature range of 780- 825oC and the dieupsetting, in the temperature range of 825- 900oC with a specimen height reduction of 65-80% at a

Despite the fact that all the die-upset composites contain a relatively coarse microstructure, the profile of the demagnetization curve in the 2nd quadrant is smooth indicating a magnetic coupling between the component phases, which promotes a magnetized state. Given that the grain size exceeds the nanoscale range necessary for exchange coupling, the only type of interactions is the longrange magnotostatic one.

Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.1, 2006

Hc (kOe) 4Mr (kG) (BH)max

(a)

strain rate of 0.008 s-1. In the hot-pressed compact, the grains are spherical with the diameter in the range of 50- 150 nm; die-upsetting produces platelet-like grains, as can be seen in Fig. 4. Given the refined microstructure, local exchange coupling may occur in some regions giving rise to enhanced values of the remanence. For the die-upset specimens, the addition of the R-lean alloy with higher magnetization, always decreases Hc and (BH)max (Fig. 5a). However, if the coercivity of the R-rich component is large enough, (e.g. Hc(R-rich) = 22.5 kOe) the remanence increases by adding the Rlean alloy (Fig. 5b).
(a) (b)

have observed that the hot deformed magnets actually contained 3 - 4 wt. % less -Fe than the corresponding starting blends due to the formation of new minority phases containing Fe.

% -Fe (MGOe)

30 20 10 0 14 12 10 20 10 0 40 30 20 10 0 10 20 30 40 50

Fig.4 SEM for [(Nd0.96Dy0.04)14Fe75Co4.5Ga0.5B6]1x[(Nd0.94Dy0.06)4Fe90Nb2B4]x composite magnets: (a) hotpressed and (b) die-upset.

To further investigate the effect of the structure morphology on the magnetic properties of the R2Fe14B / -Fe composite magnets, blends of R-rich R2Fe14B nanocrystalline powders and Fe micronsized powders have been processed at the University of Delaware [3]. The nominal compositions of Rrich R2Fe14B nanocrystalline powders were Nd14Fe79.5Ga0.5B6 and (Nd0.75Dy0.25)14Fe79.5Ga0.5B6 and they were obtained from melt-spun ribbons produced at a wheel speed of 26 m/s. The Fe powder had a particle size 44 m. For hot plastic deformation, the previously hot-pressed samples were heated again to 900oC and then they were upset at this temperature by 65% - 70% of their original height at the strain rate of 0.008 s-1. Figure 3 presents the SEM micrographs of the initial Fe powder and of the hot-pressed and hot-deformed 85% (Nd0.75Dy0.25)14Fe79.5Ga0.5B6 / 15% Fe composites. The initial Fe powder particles have an irregular shape with an average size of about 30 m. After hot pressing (Fig. 6b) many Fe particles preserve the size and shape of the starting particles (Fig. 6a), though some of them become thin platelets oriented perpendicular to the pressure direction. After deformation, (Fig. 6c) all the Fe particles become thin platelets oriented perpendicular to the pressure direction. The smallest thickness of the -Fe platelet was about 1 m. We

x (wt. %)
15

4M (kG)

10

x=0

x = 0.5 26.5% -Fe

-20 -15 -10 -5 0 5

0 -25

(b)

H (kOe)

Fig.5 (a) Variation of the -Fe amount and magnetic properties of die-upset [(Nd0.96Dy0.04)14Fe75Co4.5Ga0.5B6]1x[(Nd0.94Dy0.06)4Fe90Nb2B4]x (dash) and [(Nd0.75Dy0.25)14Fe79.5Ga0.5B6]1-x[(Nd0.94Dy0.06)4Fe90Nb2B4]x (solid) blends with the amount of the R-lean addition. (b) Demagnetization curves for hot-pressed (dash) and dieupset (solid) [(Nd0.96Dy0.04)14Fe75Co4.5Ga0.5B6]1x[(Nd0.94Dy0.06)4Fe90Nb2B4]x blends.

An increase of remanence with x was observed in (100-x)[Nd14Fe79.5Ga0.5B6] / xFe and (100x)[(Nd0.75Dy0.25)14Fe79.5Ga0.5B6] / xFe series of blends upon hot-deformation at 900oC. In the (100x)[(Nd0.75Dy0.25)14Fe79.5Ga0.5B6] / xFe magnets, addition of 15 wt. % -Fe to the starting blend increases 4Mr from 10.6 to 12.04 kG, i.e. by

Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.1, 2006
13.6%. The (BH)max is also increased from 27.3 to 29.5 MGOe for x = 10%. One 90% (Nd0.75Dy0.25)14Fe79.5Ga0.5B6 / 10% Fe exceptional specimen showed even a 23 % increase in maximum energy product, to 33.5 MGOe. Typical demagnetization curves for the (100x)[(Nd0.75Dy0.25)14Fe79.5Ga0.5B6] / xFe composite magnets are shown in Fig. 7. The non-constricted profile of the demagnetization curves for x = 5 15% demonstrates that the components of the composite magnets behave in a co-operative way. of magnetization should favor their magnetostatic coupling with the hard magnetic matrix. The magnetic coupling of the grains within the 90% (Nd0.75Dy0.25)14Fe79.5Ga0.5B6 / 10% Fe hotdeformed magnets that leads to a co-operative demagnetization process along the direction of the applied pressure during hot-deformation, was also supported by the irreversible susceptibility irrev measurements as a function of the reduced field H/Hc, where Hc is the intrinsic coercivity (Fig. 8). As revealed in Fig. 5, the irrev for the specimen containing Fe powder presents a well-defined peak as a function of the magnetic field implying a good magnetic coupling of the grains. The reversible component of the susceptibility, rev, of this specimen exhibits a peak at the low demagnetizing field, similar to the exchange-coupled magnets containing a soft magnetic phase.

Fig.6 (a) SEM image of Fe powder and SEM backscattered electron images of (b) hot-pressed and (c) hot-deformed 0.85[(Nd0.75Dy0.25)14Fe79.5Ga0.5B6] / 0.15Fe magnets. Arrows indicate the pressure direction.

Fig.8 Magnetic susceptibility measurements in (Nd0.75Dy0.25)14Fe79.5Ga0.5B6 (1 - open circles) and 0.90[(Nd0.75Dy0.25)14Fe79.5Ga0.5B6] / 0.10 Fe (2 - solid circles) hot-deformed magnets.

Fig.7 Room-temperature demagnetization curves for (Nd0.75Dy0.25)14Fe79.5Ga0.5B6 / Fe hot-deformed magnets.

At the University of Dayton, composite magnets with inclusions of the -Fe(Co) phase ranging from 20 to as much as 500 nm and (BH)max of around 50 MGOe have been obtained [10]. The magnets containing small -Fe grains (20 50 nm) showed very good squareness of the demagnetization curves and high coercivity over 14 kOe. Fig. 9 presents the magnetic properties as a function of the -Fe fraction.

Since the Fe particles have size in the micrometer size, exceeding by far the scale of exchange coupling and magnetic hardening by the 2:14:1 phase, we strongly believe that it is the magnetostatic interaction that is responsible for the magnetic coupling of the blending components. The microstructure with the magnetically soft layers (Fe platelets) arranged perpendicularly to the direction

Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.1, 2006

obtained by hot pressing at 700 to 780C for 1 to 2 min. Microstructure observations for Sm(Co0.85Fe0.15)8.9 sample shown in Fig. 11, reveal nanograins 5 to 40 nm in size. The magnetic properties vs. the (Co+Fe)/Sm ratio z are shown in Fig. 12. When z is 8.6 with ~ 1% soft phase, the isotropic nanocomposite magnets have (BH)max = 11.5 MGOe and Hc = 11 12 kOe. When z is increased to 10.8, the (BH)max increases to 14.1 MGOe, and Hc is decreased to ~ 7 kOe.

Fig.9 Effect of -Fe fraction on magnetic properties of Nd2Fe14B / -Fe magnets [9].

4 Magnets with a R-Co hard phase

4.1 Single alloy technique Though the R-Co permanent magnets cannot compete with the Nd-Fe-B magnets in the maximum energy product and cost, they are far more superior in the temperature stability and corrosion resistance. At the University of Delaware, we extended the work of Fuerst and Brewer [5] on PrCo5-based anisotropic magnets and developed high-coercivity Pr1xSmx(Co1yMy)z powders (nominal compositions) with x=0 - 0.3, z=5 - 6, M = Cu or Fe and y = 0.01 - 0.1 by high-energy ball milling, which then, we consolidated by hot-pressing and die-upsetting [11]. During the hot-pressing, the amorphous alloys crystallized into a nanocrystalline structure consisting of a mixture of the main 1:5 phase, the disordered hexagonal 2:17 phase and very small (5 nm) precipitates of the hexagonal 2:7 phase. The hot-pressed PrCo5 magnet had a relatively high coercivity Hc of 10.3 kOe. Dieupsetting was successful in inducing an anisotropy, but with decreased Hc to 8.2 kOe. Replacing up to 3 at% Co by Cu, does not significantly change 4Mr and Hc, but improves the loop squareness. The dieupset Pr0.9Sm0.1(Co0.98Cu0.02)5 magnet showed 4Mr of 9.2 kG, Hc of 10.5 kOe and (BH)max of 16.7 MGOe (Fig. 10). It is possible that Cu increases the amount of the 1:5 phase at the expense of 2:17 resulting in a better overall texture. Isotropic, hot pressed Sm(Co1-xFex)z magnets with x = 0 to 0.5 and z = 8.3 to 10.8 were made from mechanically alloyed powders at the University of Dayton [12]. Fully dense magnets with density ranging from 8.17 to 8.65 g/cm3 were
Fig.10 Demagnetization curves of (a) PrCo5 and (b) Pr0.9Sm0.1(Co0.98Cu0.02)5 magnets: hot-pressed (1) and dieupset (2).

Fig.11 TEM microstructure for the hot pressed Sm(Co0.85Fe0.15)8.9 magnet made from mechanically alloyed powder [12].

Fig.12 Isotropic magnetic properties vs. transition metal content, z, for isotropic nanocomposite of Sm(Co0.73Fe0.27)z [12].

Cast isotropic composite permanent magnets with a microstructure consisting of a cellular 2:17 / 1:5 matrix and Co(Fe) inclusions

Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.1, 2006
(Fig. 13) were obtained at the University of Delaware via a heat treatment of cast RCo(Fe) CuTi alloys containing less than 10 at. % R (R=Sm, Pr). Inclusions of the magnetically soft Co(Fe) phase were too large to be coupled with the hard matrix by magnetic exchange interactions. Nevertheless, a complete magnetostatic coupling between the soft and hard components was evident from the smooth demagnetization curves. The resulting cast composite magnets show moderate values of the coercivity and energy product up to 3.3 kOe and 5.1 MG Oe, respectively [13].

Wohlfarth rotation and ordinary domain-wall pinning [14].

4.2 Latest developments in ultrahigh temperature (UHT) SmCo magnets Lately, the US Air Force office of scientific research funded development work to improve the performance of high-temperature magnets under MURI and STTR programs. This was in response to the More Electric Aircraft (MEA) Initiative, which led to significant progress in improving the properties of sintered R-Co based magnets. As a result of this research, Electron Energy Corporation patented a series of ultra high temperature magnets with maximum operating temperatures up to 550 oC. Table 1 shows the typical magnetic properties of ultra high temperature sintered magnets based on the Sm2Co17 phase. The microstructure of these magnets consists basically of 100 nm cells of rhombohedral Sm2Co17 phase with the hexagonal SmCo5 phase cell boundaries. The complex heat treatment processes and strategic elemental additions (e.g. Cu, Fe, Zr, etc), which have specific impact on the microstructure and microchemistry, together with the high Curie temperatures and magnetocrystalline anisotropies of the component phases, determine the high values of coercivity at high temperatures.
Table 1 Typical magnetic properties of high temperature magnets.

Fig.13 TEM image of fully heat-treated (Sm0.7Pr0.3)7(Co0.85Fe0.15)82Cu9Ti2 alloy showing 2:17 / 1:5 cellular structure in the matrix and Co(Fe) inclusions [13].

Highly coercive 1:5 based SmCoCuTi particulate thin film magnets prepared by magnetron sputtering have been studied at the University of Nebraska. Juxtaposed with the high magnetocrystalline anisotropy as an intrinsic property, the development of coercivity is facilitated by the thin-film specific nanostructuring and, to some degree, by exploiting the surface and interface anisotropies. A microstructure consisting of SmCo5 grains with an average diameter of 8 nm embedded in a Cu-rich matrix (Fig. 14), has been precipitated by optimal annealing of SmCo/CuTi multilayered films. The room temperature coercivity of the granular film was 50.4 kOe.

Material Grade SmCo T550 SmCo T500 SmCo T450 SmCo T400

Br (kG) 8.5 9.2 9.6 10.1

Hc (kOe) 7.9 8.9 9.1 9.5

Hci (kOe) >25 >25 >25 >25

(BH)max (MGOe) 16 20 22 24

Maximum Operating Temp. (oC) 550 500 450 400

Fig.14 HRTEM images of a particulate SmCoCuTi thin film [14].

Figure 15 shows a comparison between the maximum energy products versus the maximum operating temperature for Nd-Fe-B and Sm-Co magnets. The trade-off between the magnetic performance at room temperature and the maximum operating temperature is very obvious.

The mechanism of coercivity in such a particulate media was explained as a discrete pinning mode intermediate between Stoner

Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.1, 2006

50 45
(BH)max (MGOe)

40 35 30 25 20 15 100 200 300 400 500

o

temperature-compensated, high-temperature magnet series with a small RTC of Br. The effects of Gd and Co were studied on magnetic properties and (RTC of Br) of Sm2M17 based magnet (M = transition metal), which led to the development of a TC400 series of SmCo magnets with small RTC and an operating temperature of 400oC.
600

Maximum Operating Temp. ( C)

Table 2 Magnetic properties and reversible temperature coefficients of Br () of temperaturecompensated TC400 high temperature magnets.
Br (kG) T400-22 TC400-20 TC400-18 9.6 9.1 8.7 8.3 7.9 7.4 6.9 Hci (kOe) >25 >25 >25 >25 >25 >25 >25 BHmax (MGOe) 21.9 19.9 18.0 16.5 14.7 13.0 11.5 RTC of Br* %/C -0.037 -0.034 -0.030 -0.020 -0.015 -0.007 +0.002 TM** C 400 400 400 400 400 400 400

Fig.15 Maximum energy product versus maximum operating temperature of Nd-Fe-B and Sm-Co magnets.
Magnet

4.3 Sm-Co permanent magnets with almost zero reversible temperature coefficient (RTC) of Br for critical applications The reversible temperature coefficient (RTC) of Br of SmCo 1:5 and 2:17 type magnets can be controlled by substituting a heavy R from the group of Gd, Tb, Dy, Ho and Er, for a portion of the Sm, which led to the development of zero RTC magnets. Figure 16 shows the demagnetization curves of zero RTC magnets at various temperatures. The residual induction of these magnets does not have noticeable changes between 50oC to +150oC. The maximum operating temperature of these magnets is 300oC.

TC400-16 TC400-14 TC400-13 TC400-11

*The RTC of Br () is calculated in the temperature range between 50oC and 150oC. **TM is the maximum operating temperature at which the straight-line demagnetization curve still exists. The TC400 magnet series are perfect high temperature magnets with a TM of 400oC because of their square intrinsic demagnetization curves and the straight-line extrinsic demagnetization curves over the entire temperature range up to 400oC. The addition of Gd does not have an adverse effect on the demagnetization curve shape, while it has the benefit of temperature compensation. The RTC of Br is almost zero for TC400-11 and TC400-13 magnets. 4.5 Blending technique At the Carnegie Mellon University, anisotropic Sm(Co0.67Fe0.234Cu0.07Zr0.024)7.5 / -Fe composites have been obtained via consolidation of the precursor powders by a combustion driven compaction [15]. During the consolidation the peak pressure reached 2 GPa while the temperature was estimated to be lower than 200 oC. The magnets of ~95% theoretical density exhibited (BH)max of 31.3 MGOe (Fig. 17).

Fig.16 Typical demagnetization curves of a temperature compensated (Sm,Gd)2Co17 based magnet.

4.4 UHT SmCo magnets with small reversible temperature coefficient Some applications, such as inertial devices and traveling wave tubes, require small reversible temperature coefficient (RTC) of Br, , as well as high temperature stability. The need for temperature compensated magnets with TM > 300oC prompted efforts to develop a

Manuscript published in Journal of Iron and Steel Research International 13: 12-22 Suppl.1, 2006
structure in 2:17 magnets), the magnetic hysteresis parameters showed a slight degrade. When lowering the stoichiometry to z = 7.5, an enhanced coercivity of 5 kOe is achieved at the expense of the remanence (Fig. 18). 5 Conclusions High values of the energy product can be obtained in anisotropic composite magnets. Recent studies have shown that small additions of other elements to Nd-Fe-B nanocomposite magnets can successfully assist the development of texture. The latest studies show that enhanced remanence and energy product can also be obtained in composites magnets due to the long-range magnetostatic coupling. Recent work pointed out that hybrid magnets made by blending different component powders (e.g. based on 2:14:1, 2:17, 1:5 as the hard magnetic phases and Fe as the soft magnetic phase) can show enhanced magnetic performance. The magnetic properties of the blends are determined by the specific characteristics of each component. Based on recent studies it was shown that the hot compaction /deformation techniques are very convenient and suitable in developing isotropic / anisotropic magnets with high density and tailored magnet properties. Other consolidation techniques of precursor magnet powder, including combustion driven compaction and explosive shock consolidation, can also lead to very high densities close to the bulk values, while preserving the original crystallographic structure. Significant improvements have been made in Sm-Co based high temperature magnets and with almost zero reversible temperature coefficient of Br.
Acknowledgment:

Fig.17 Demagnetization curves of anisotropic Sm(Co,Fe,Cu,Zr)7.5 / Fe composite magnets consolidated by combustion driven compaction [15].

Fig.18 Demagnetization curves of (1) blends of 50wt% SCu7 + 50wt% SCu11 (z=9) hot pressed at 820oC , (2) specimen (1) annealed at 820oC for 2h followed by slow cooling and (3) blends of 87.5wt% SCu7 + 12.5wt% SCu11 (z=7.5) hot pressed at 960oC.

In an attempt to develop composite magnets based on the 2:17 phase without the cellular structure, the joint team of the University of Delaware and Electron Energy Corporation, blended Sm(Co0.65Fe0.25Cu0.1)7 (code SCu7) with Sm(Co0.65Fe0.25Cu0.1)11 (code SCu11) alloy powders (intensively milled for 30 min.), and consolidated the blend by hot pressing at 820oC. The ingots have been previously homogenized at 1175oC for 6h. Two types of blends of SCu7 and SCu11 with 50:50 and 87.5:12.5 weight ratios have been consolidated at 820 and 960oC, respectively. The two ratios correspond to z=8.65 and z=7.37 in the Sm(Co0.65Fe0.2Cu0.1)z formula. The compact had a multi-phase structure (2:17 + 1:5 + 2:7 and -Fe) with submicron grain size. The hot-pressed compacts with z = 9 prepared by blending the SCu7 and SCu11 powder were isotropic and showed modest values of coercivity of 3.3 kOe (Fig. 15). The remanence value did not exceed 8 kG (in a maximum effective applied field of 16 kOe). After annealing the compact at 800oC for 2 h followed by slow cooling (which is the typical annealing sequence for inducing the cellular

The work was supported by US Department of Energy (DOE) and Air Force Office for Scientific Research (AFOSR).
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