Development of Isotropic Bonded Magnets with (BH)max of 120 kj/m3 Shinya Sakurada, Akihiko Tsutai and Tomohisa Arai 1 Corporate Research & Development

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Development of Isotropic Bonded Magnets with (BH)max of 120 kj/m3 Shinya Sakurada, Akihiko Tsutai and Tomohisa Arai 1 Corporate Research & Development Center, Toshiba Corp., 1 Komukai Toshiba-cho Saiwai-ku, Kawasaki 212-8582. 2 Display Devices & Components Control Center, Toshiba Corp., 8 Shinsugita-cho Isogo-ku, Yokohama 235-8522. Received May 8, 2003 SYNOPSIS We have developed isotropic magnet powder with the composition of (Sm,Zr)(Fe,Co)zB0.1NX (z=9-10) prepared by rapid quenching, annealing, and nitrogenation. The presence of both zirconium and cobalt make it possible to realize a nearly single phase of the TbCu7 structure with a c/a ratio as high as 0.87. These powders show a high saturation magnetization of 1.6-1.7 T. A small addition of boron is effective for forming the amorphous phase in the rapidly quenched alloys and for obtaining uniform and fine grains of the ThCu7 phase after annealing. The combination of the high saturation magnetization and the fine grains leads to high Br and high (BH)max. The magnetic properties of these powders are as follows: Br=1.00-1.07T, HcJ=640-880kA/m, (BH)max=160-180kJ/m3. Isotropic bonded magnets fabricated using such powder show highest (BH)max of 120kJ/m3. These bonded magnets also show good thermal stability and good oxidation resistance. KEY WORDS TbCu7 structure, rapid quenching, nitrogenation, isotropic magnet powder, isotropic bonded magnet

Fig.1 X-ray diffraction patterns for NdFe10Si2 and Nd0.75Zr0.25Fe10Si2. Fig.2 Variation in lattice constants of ThMn12 phase in RFe10Si2 with mean atomic radius of rare earth site element.

Fig.3 X-ray diffraction patterns for rapidly quenched (Nd1-xZrx)Fe10 alloys. Fig.4 X-ray diffraction patterns for rapidly quenched (Nd0.5Zr0.5) (Fe1-xCox)10 alloys.

Fig.5 (a) Magnetization curves for rapidly quenched (Nd0.75Zr0.25) (Fe0.7Co0.3)z alloys having a TbCu7 structure with various c/a and (b) saturation magnetization as a function of c/a. Fig.6 Magnetization curves for rapidly quenched (R0.75Zr0.25) (Fe0.7Co0.3)10 alloy ribbons and their nitrogenated powders: (a) R = Nd and (b) R = Sm.

Fig.7 X-ray diffraction patterns for rapidly quenched (Smo.7Zr0.3) (FeossCo0.05)9Bx. Fig.8 Fig.9 Saturation magnetization and anisotropy field for (Sm0.7Zr0.3) DSC curves for rapidly quenched (Sm0.7Zr0.3)(Fe0.95Co0.05)9Bx. (Fe1-yCoy)9B0.1Nx.

120(kJ/ms)等 方 性 ボ ン ド磁 石 の 開 発 Fig.10 TEM micrograph for (Sm0.7Zr0.3)(Fe0.8Co0.2)9B0.1Nx. Fig.11 Process of fabricating magnet powder newly developed and bonded 631 Fig.12 Demagnetizationcurvesfor (Sm0.7Zr0.3)(Fe0.8Co0.2)9B0.1Nx at varioustemperatures. Fig.13 Results of atmospheric exposure tests for Sm-Zr-Fe-Co-BN and Nd-Fe-B magnet powders at various temperatures. Sm-Zr-Fe-Co-B-N magnet. 度 特 性 を期 待 で き る.Fig.12に 磁 石 粉 末 の 減 磁 曲線 を示 す が, 用 コ ンパ ウ ン ドの リサ イ クル 性 改 善 や防 錆 コー テ ィング の簡 略 Brの 温 度係 数 は-0.034%/ 化 を もた らす と と も に,ボ ン ド磁 石 化 す る樹 脂 の選 択 肢 が増 で あ り,本 合 金 系 で は総 じてNd- Fe-B系 超 急冷 粉 末 の1/2以 下 の 値 が 得 られ る.Hdの は-0.40%rcで あ り,室 温 で 同 じHdを 温 度係 数 持 つNd-Fe-B系 超急 え,特 徴 あ るボ ン ド磁 石 を提 供 で き る もの と思 わ れ る.た だ し,磁 化 の 熱 ゆ ら ぎ に起 因 す る不 可 逆 減 磁 率 は 同 じHdを 冷 粉 末 と同等 の値 で あ る.な お,着 磁 性 も同 等 のHcJを 持 つ 持 つNd-Fe-B系 Nd-Fe-B系 るた め に は 改 善 が 必 要 で あ る. 超 急 冷粉 末 と同 レベ ル にあ る.ま た,開 発 した磁 石 粉 末 は耐 酸 化性 に も優 れ て い る.Fig.13は 開 発 したSm-Zr-FeCo-B-N粉 末 とNd-Fe-B系 超 急 冷 粉 末 につ い て それ ぞ れ 大 気 中 で 各温 度1時 間 放 置 し,室 温 に戻 した 後 にVSM(試 型磁 力計)で(BH)maxを 料振 動 評 価 した結 果 で あ る.両 者 と も室 温 か ら200 ま で そ の値 は ほ ぼ 変 化 しな い が,そ れ 以 上 の 温 度 で は 開 発 粉 末 の(BH)max値 開発 した磁 石 粉 末 を用 い て ラ ボ レベ ル で 試作 した圧 縮成 形 ボ ン ド磁 石 の 減 磁 曲線 をFig.14に 示 す.最 大 エ ネ ル ギ ー積 は 120kJ/m3に 達 し,Nd-Fe-B系 超 急 冷 粉 末 を 用 い て製 造 され る ボ ン ド磁 石 の 最 大 エ ネ ル ギ ー 積40 95kJ/m3を 大 き く上 回 る 値 が 実 現 され た. が 安定 で あ るの に対 して,Nd-Fe-B 系 超 急 冷 粉 末 は 急 激 に劣 化 す る.こ れ は 酸 化 に よ る劣 化 と考 えて い る.開 発 粉 末 は 熱 に よ る劣 化 が 小 さい た め,射 出 成 形 2003年8月 ボ ン ド磁 石 と 同 等 で あ り,磁 石 を 高温 で用 い 7ま と め 以 上 述 べ て きた よ うに,筆 者 らは 強 力 な磁 石 の 開発 を 目指

Fig.14 Demagnetization curve for isotropic bonded magnet prepared by (Sm0.7Zr0.3)(Fe0.8Co0.2)9B0.1Nx powder. phases R3(Fe,M)29Xn: (R=Ce, Pr, Nd, Sm, Gd; M=Ti, V, Cr, Mn; and X=H, N, C", J. Appl. Phys., 76(1994)6138-6143. 9) R.Verhoef, F.R.de Boer, Z.Zhi-dong and K.H.J.Buschow: "Moment reduction in RFe 12-xTx compounds (R=Gd, Y and T= Ti, Cr, V, Mo, W)", J. Magn. Magn. Mater., 75(1988)319-322. 10) S.Sakurada, A.Tsutai and M.Sahashi: "A study on the formation of ThMn12 and NaZn13 structures in RFe10Si2", J. Alloys Compounds, 187(1992)67-71. 1) M.Sagawa, S.Fujimura, N.Togawa, H.Yamamoto and Y.Matsuura: "New material for permanent magnets on a base of Nd and Fe", J. Appl. Phys., 55(1984)2083-2087. 2) J.J.Croat, J.F.Herbst, R.W.Lee and F.E.Pinkerton: "Pr-Fe and Nd-Fe-based materials: A new class of high-performance permanent magnets", J. Appl. Phys., 55(1984)2078-2082. 3) J.M.D.Coey and H.Sun: "Improved magnetic properties by treatment of iron-based rare-earth intermetallic compounds in ammonia", J. Magn. Magn. Mater., 87(1990)L251-L254. 4) T.Iriyama, K.Kobayashi, N.Imaoka, T.Fukuda, H.Kato and Y.Nakagawa: "Effect of Nitrogen Content on Magnetic Properties of Sm2Fe17Nx (0<x<6)", IEEE Trans. Magn., 28 (1992)2326-2331. 5) M.Katter, J.Wecker and L.Schultz: "Structural and hard magnetic properties of rapidly solidified Sm-Fe-N", J. Appl. Phys., 70 (1991)3188-3196. 6) K.Ohashi, T.Yokoyama, R.Osugi and Y.Tawara: "The magnetic and structural properties of R-Ti-Fe ternary compounds", IEEE Trans. Magn., MAG-23(1987)3101-3103. 7) D.B.Mooij and K.H.J.Buschow: "A new class of ferromagnetic materials: RFe10V2", Philips J. Res., 42(1987)246-251. 8) J.M.Cadgan, H.-S.Li, A.Margarian, J.B.Dunlop, D.H.Ryan, S.J.Collocott and R.L.Davis: "New rare-earth intermetallic 11) S.Sakurada, A.Tsutai, T.Hirai, Y.Yanagida, M.Sahashi, S.Abe and T.Kaneko: "Structural and magnetic properties of rapidly quenched (R,Zr)(Fe,Co)10Nx (R=Nd,Sm)", J. Appl. Phys., 79 (1996)4611-4613. 13) F.Kawashima, S.Sakurada, T.Sawa, T.Arai, A.Tsutai and M.Sahashi: "Magnetic Properties and Microstructure of Rapidly Quenched SmZrFeCoN Magnets", IEEE Trans. Magn., 35 (1999)3289-3291. 14) S.Sakurada, K.Nakagawa, F.Kawashima, T.Sawa, T.Arai, A.Tsutai and M.Sahashi: "Isotropic Sm-Zr-Fe-Co-B-N Bonded Magnets with High (BH)max", Proc. 17th International Workshop on Rare-Earth Magnets and Their Applications, H.Kaneko, M.Homma and M.Okada, Sendai, The Japan Institute of Metals, (2000)719-726.

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