Research Status and Future Development of (Ce, La, Y)-Fe-B Permanent Magnets Based on Full High-Abundance Rare Earth Elements

doi:10.11900/0412.1961.2023.00117

Acta Metall Sin

2024, Vol. 60

Issue (5): 585-604 DOI: 10.11900/0412.1961.2023.00117

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Research Status and Future Development of (Ce, La, Y)-Fe-B Permanent Magnets Based on Full High-Abundance Rare Earth Elements

LIU Zhongwu¹(

), ZHOU Bang¹, LIAO Xuefeng¹^,², HE Jiayi¹^,³

1 School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China
2 Guangdong Provincial Key Laboratory of Rare Earth Development and Application, Institute of Resources Utilization and Rare Earth Development, Guangdong Academy of Sciences, Guangzhou 510650, China
3 School of Materials Science and Energy Engineering, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China

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LIU Zhongwu, ZHOU Bang, LIAO Xuefeng, HE Jiayi. Research Status and Future Development of (Ce, La, Y)-Fe-B Permanent Magnets Based on Full High-Abundance Rare Earth Elements. Acta Metall Sin, 2024, 60(5): 585-604.

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Abstract

The surging demand for Nd-Fe-B-based rare earth (RE) permanent magnets has led to a sharp increase in the consumption of critical RE elements, such as Nd, Pr, Dy, and Tb. As a result, the high cost of these elements has become a major issue. Judging from the perspective of economy and resource availablity, the overstock of abundant and inexpensive RE resources, including La, Ce, and Y, offers a new opportunity to develop cost-effective permanent magnets containing no critical RE elements. RE-Fe-B magnets based on full high-abundance REs, i.e., (Ce, La, Y)-Fe-B type magnets, are expected to serve as an alternative to fill the performance gap between hard ferrites and bonded Nd-Fe-B magnets. This approach can not only meet the diversified demand for permanent magnet materials in the middle- and low-end markets, but also contribute to a balanced use of RE resources. At present, however, the recognition and understanding of Ce-, La-, and Y-based RE-Fe-B permanent magnets still require further research, and the performance of these magnets in the laboratory is quite low, which makes practical applications difficult. Based on the latest domestic and overseas developments and the research results obtaned by the authors' research group, this review summarizes the research progress on Ce-, La-, and Y-based RE-Fe-B permanent magnetic alloys and associated densified magnets. The analysis highlights the magnetic properties and metallurgical behavior of rapidly quenched RE-Fe-B alloys, alloying composition design, and element interactions in multicomponent, rapidly quenched (Ce, La, Y)-Fe-B alloys. Moreover, the relationship between the preparation process, microstructure, and magnetic properties of bulk RE-Fe-B densified magnets is discussed. Finally, the improvement and future development trends of full high-abundance RE permanent magnets are also explored.

Key words: rare earth permanent magnet high abundance rare earth element interaction microstructure magnetic property

Received: 23 March 2023

ZTFLH:

TM273

Fund: National Natural Science Foundation of China(U21A2052);National Natural Science Foundation of China(52071143);China Postdoctoral Science Foundation(2022M720845)

Corresponding Authors: LIU Zhongwu, professor, Tel: (020)22236906, E-mail: zwliu@scut.edu.cn

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https://www.ams.org.cn/EN/10.11900/0412.1961.2023.00117 OR https://www.ams.org.cn/EN/Y2024/V60/I5/585

Fig.1 Relative abundance and utilization rate of rare earth (RE) element^[4-6] (a), RE metals and the corresponding RE oxides price^[7] (b), comparison of RE₂Fe₁₄B (RE = Ce, La, and Y) compounds in intrinsic magnetic properties, magnetic hardness parameter and formation energy, the data are extracted from an online database^[3,9] (c), and comparison of the properties of different types of permanent magnets^[11] (d) (E_for—formation energy, к— magnetic hardness parameter, J_s—saturation magnetic polarization, T_C—Curie temperature, H_A—anisotropy field, J_r—remanence, H_cj—intrinsic coercivity)

Fig.2 Schematic drawing of the Nd-Fe-B and Ce-Fe-B phase components (a), ⁵⁷Fe Mössbauer spectra of the melt-spun Ce₁₆Fe₇₈B₆ alloy measured at 300 and 77 K^[17] (b), TEM image and corresponding selected area diffraction (SAED) pattern (inset) for the melt-spun Ce₁₆Fe₇₈B₆ alloy (c), and the HRTEM image for selected area 1 in Fig.2c^[17] (d) (GB—grain boundary phase; d—interplanar distance, nm)

Fig.3 XRD spectra for the as-spun (La_{1 -}_x Y _x )₂Fe₁₄B alloys^[28] (a), bright field TEM image (b) and corresponding SAED (c) for the as-spun La₂Fe₁₄B alloy^[28], and bright field TEM image (d) and HRTEM image and corresponding fast Fourier transformation (inset) (e) for the as-spun Y₂Fe₁₄B alloy^[35]

Table 1 Phase precipitation behaviors of Ce₂Fe₁₄B, La₂Fe₁₄B, and Y₂Fe₁₄B amorphous alloys during heating stage^[19,29,35]

Type of alloy	Composition	H_cj kA·m^-1	J_r T	J_s T	(BH)_max kJ·m^-3	T_C K	300-400 K		Ref.
Type of alloy	Composition	H_cj kA·m^-1	J_r T	J_s T	(BH)_max kJ·m^-3	T_C K	α / (%·K^-1)	β / (%·K^-1)	Ref.
Ternary	Ce₂Fe₁₄B	211	0.42	1.08	17.0	424	-	-	[19]
	Ce₂Fe₁₄B	207	0.57	1.07	28.6	420	-0.623	-0.536	[40]
	Ce₁₀Fe₈₄B₆	135	0.60	1.19	11.3	-	-	-	[21]
	Ce₁₂Fe₈₂B₆	167	0.59	-	21.0	-	-	-	[43]
	Ce₁₆Fe₇₇B₆	367	0.47	0.90	33.3	-	-	-	[17]
	Ce₁₇Fe₇₇B₆	344	0.43	0.77	28.5	420	-	-	[44]
	Ce₁₆Fe₇₈B₆	350	0.49	0.93	33.8	420	-0.54	-0.74	[44]
	Ce₁₇Fe₇₈B₆	494	0.49	-	33.0	-	-	-	[22]
	Ce₁₇Fe₇₈B₆	438	0.46	-	34.2	424	-0.500	-0.663	[23]
	Ce₁₇Fe₇₈B₆	352	0.43	-	29.0	425	-0.56	-0.75	[45]
	La₂Fe₁₄B	14	0.11	-	-	-	-	-	[29]
	Y₂Fe₁₄B	149	0.88	1.43	54.1	553	-0.154	-0.03	[35]
	Y_2.5Fe₁₄B	230	0.75	1.27	51.7	542	-	-	[35]
	Y₃Fe₁₄B	281	0.72	1.18	42.2	546	-	-	[35]
	Y₁₆Fe₇₈B₆	240	0.61	-	21.0	-	-	-	[36]
Quaternary	(Ce_0.9La_0.1)₂Fe₁₄B	251	0.65	1.12	46.2	434	-0.402	-0.442	[40]
	(Ce_0.8La_0.2)₂Fe₁₄B	235	0.68	1.15	47.9	443	-0.356	-0.328
	(Ce_0.7La_0.3)₂Fe₁₄B	214	0.69	1.16	49.1	456	-0.292	-0.299
	(Ce_0.7La_0.3)₂Fe₁₄B	183	0.67	-	37.0	-	-	-
	(Ce_0.6La_0.4)₂Fe₁₄B	203	0.72	1.19	47.0	468	-0.259	-0.286
	(Ce_0.5La_0.5)₂Fe₁₄B	197	0.68	1.14	40.8	476	-0.220	-0.261
	(Ce_0.4La_0.6)₂Fe₁₄B	163	0.66	1.12	34.4	487	-0.207	-0.225
	(Ce_0.3La_0.7)₂Fe₁₄B	134	0.59	1.04	21.3	493	-0.179	-0.208
	(Ce_0.2La_0.8)₂Fe₁₄B	32	0.37	0.87	2.5	508	-	-
	(Ce_0.1La_0.9)₂Fe₁₄B	9	0.30	1.17	1.5	-	-	-
	(Ce_0.7La_0.3)_2.5Fe₁₄B	345	0.60	1.04	50.1	-	-	-	[38]
	(Ce_0.7La_0.3)₃Fe₁₄B	439	0.69	1.12	61.1	-	-	-
	(Ce_0.7La_0.3)₃Fe₁₄B	362	0.56	1.00	46.2	-	-	-
	(Ce_0.7La_0.3)_3.5Fe₁₄B	406	0.53	0.97	41.5	-	-	-
	(Ce_0.7La_0.3)₄Fe₁₄B	436	0.50	0.89	38.5	-	-	-
	(Ce_0.9La_0.1)₁₇Fe₇₈B₆	520	0.52	0.94	41.8	427	-0.463	-0.631
	(Ce_0.8La_0.2)₁₇Fe₇₈B₆	453	0.55	0.96	43.2	432	-0.437	-0.582
	(Ce_0.7La_0.3)₁₇Fe₇₈B₆	332	0.58	1.05	46.9	442	-	-
	(Y_0.9La_0.1)₂Fe₁₄B	140	0.86	1.41	52.1	552	-0.146	0.05	[28]
	(Y_0.8La_0.2)₂Fe₁₄B	138	0.83	1.40	46.2	550	-0.140	0.04
	(Y_0.7La_0.3)₂Fe₁₄B	133	0.81	1.39	43.5	547	-0.145	0.03
	(Y_0.6La_0.4)₂Fe₁₄B	122	0.79	1.38	39.4	543	-0.152	-0.02
	(Y_0.5La_0.5)₂Fe₁₄B	108	0.74	1.37	30.4	540	-0.160	-0.07
	(Y_0.4La_0.6)₂Fe₁₄B	92	0.71	1.36	26.2	536	-	-
	(Y_0.3La_0.7)₂Fe₁₄B	86	0.65	1.31	20.8	532	-	-
	(Y_0.2La_0.8)₂Fe₁₄B	60	0.56	1.12	5.1	528	-	-
	(Y_0.1La_0.9)₂Fe₁₄B	27	0.51	1.26	3.4	-	-	-
Quaternary	(Y_0.9Ce_0.1)₂Fe₁₄B	156	0.85	1.40	56.1	543	-0.153	0.009	[46]
	(Y_0.8Ce_0.2)₂Fe₁₄B	163	0.82	1.37	52.0	529	-0.164	-0.012
	(Y_0.7Ce_0.3)₂Fe₁₄B	170	0.78	1.33	51.1	519	-0.189	-0.079
	(Y_0.6Ce_0.4)₂Fe₁₄B	187	0.76	1.29	48.4	507	-0.209	-0.153
	(Y_0.5Ce_0.5)₂Fe₁₄B	211	0.75	1.25	49.8	493	-0.218	-0.182
	(Y_0.4Ce_0.6)₂Fe₁₄B	202	0.71	1.21	40.2	481	-0.276	-0.305
	(Y_0.3Ce_0.7)₂Fe₁₄B	207	0.68	1.16	40.3	465	-0.285	-0.342
	(Y_0.2Ce_0.8)₂Fe₁₄B	217	0.64	1.13	39.5	449	-0.319	-0.391
	(Y_0.1Ce_0.9)₂Fe₁₄B	209	0.62	1.10	25.5	435	-0.410	-0.488
	(Y_0.5Ce_0.5)₁₇Fe₇₈B₆	323	-	-	40.0	519	-	-	[47]
Quinary	[(Ce_0.7La_0.3)_0.9Y_0.1]₂Fe₁₄B	212	0.71	1.19	51.7	464	-0.277	-0.288
	[(Ce_0.7La_0.3)_0.8Y_0.2]₂Fe₁₄B	207	0.74	1.23	57.3	475	-0.246	-0.256	[48]
	[(Ce_0.7La_0.3)_0.7Y_0.3]₂Fe₁₄B	204	0.75	1.25	54.9	487	-0.236	-0.182
	[(Ce_0.7La_0.3)_0.6Y_0.4]₂Fe₁₄B	186	0.76	1.28	51.4	494	-0.213	-0.163
	[(Ce_0.7La_0.3)_0.5Y_0.5]₂Fe₁₄B	167	0.77	1.34	48.0	506	-0.199	-0.051
	[(Ce_0.7La_0.3)_0.8Y_0.2]₁₇Fe₇₈B₆	354	0.70	1.07	56.5	481	-	-0.246	[42]
	[(Ce_0.8La_0.2)_0.7Y_0.3]₁₇Fe₇₈B₆	400	0.63	-	58.9	488	-0.255	-0.241
	[(Ce_0.8La_0.2)_0.5Y_0.5]₁₇Fe₇₈B₆	332	0.66	-	60.0	515	-0.197	-0.102

Table 2 Magnetic properties of reported Ce-, La-, and Y-based RE-Fe-B melt-spun alloys^{[17,19,21-23,28,29,35,36,38,40,42-48]}

Fig.4 Demagnetization curves of as-spun (Ce, La, Y)₁₇Fe₇₈B₆ alloys (a), bright-field TEM image and EDS line scanning (inset) for the [(Ce_0.8La_0.2)_0.7Y_0.3]₁₇Fe₇₈B₆ alloy (b)^[42] (J—magnetic polarization, H—magnetic field)

Fig.5 Comparisons of H_cj and (BH)_max (a), and values of α and β (b) of the as-spun (Ce, La, Y)₁₇Fe₇₈B₆ alloys with reported Ce or Nd-based RE-Fe-B alloys^{[17,21-23,37,38,40,42-46,55-64]}; comparison of the cost performance for as-spun (Ce, La, Y)₁₇Fe₇₈B₆ alloys with commercial isotropic magnetic powders (c) and comparison of corrosion resistance (d) of RE-based permanent magnets^[28,65-70] (E_corr—self corrosion potential, i_corr—self corrosion current density)

Fig.6 Calculated formation energiesfor (Ce_{1 -}_x La _x )Fe₂ phase (Inset shows the schematic illustration of the cubic CeFe₂ crystal) (a), XRD refinement spectra for (Ce_{1 -}_x La _x )₁₇Fe₇₈B₆ alloys^[42] (b), demagnetization curves for the as-spun Ce₁₇Fe_{78 -}_x B₆Si _x (Insets in Fig.6c show the microstructure evolutions of Ce₁₇Fe_{78 -}_x B₆Si _x alloys)^[55] (c) and Ce₁₆Fe_{78 -}_x B₆Ge _x alloys (Inset shows the HRTEM image of Ce₁₆Fe_77.8B₆Ge_0.2 alloy)^[74] (d)

Fig.7 Demagnetization curves for the as-spun Ce₁₇Fe_{78 -}_x B₆Ta _x (x = 0, 0.75) alloys (Inset shows the bright-field TEM image of Ce₁₇Fe_77.25B₆Ta_0.75 alloy) (a), simulation demagnetization curves of the model magnets (Inset shows Ce-Fe-B magnet model with non-magnetic particles) (b), demagnetizing field distributions for both models in the saturation state (c), and magnetization reversal behaviors both models at different reversed magnetic fields (d, e)^[56] (w/o and w/ represent the magnet model without non-magnetic particles and the magnet model with non-magnetic particles, respectively; μ₀H_ext—external applied field, M_z —magnetization in z direction, M_s—saturation magnetization)

Fig.8 XRD spectra (a), SEM images (b1, b2), and J-H curves (c) of Ce₁₇Fe₇₈B₆ magnets spark plasma sintered (SPSed) at 650 and 700^oC^[83]

Fig.9 Hysteresis loops measured parallel (//) to the pressing direction of hot-deformed Ce₁₇Fe₇₈B₆, (Ce_0.9La_0.1)Fe₇₈B₆, and [(Ce_0.9La_0.1)_0.8Y_0.2)]₁₇Fe₇₈B₆ magnets (Inset shows the demagnetization curves of the hot-deformed magnets) (a), bright field TEM images of hot-deformed Ce₁₇Fe₇₈B₆ (b) and [(Ce_0.9La_0.1)_0.8Y_0.2)]₁₇Fe₇₈B₆ magnets (Insets show the HRTEM images of the hot-deformed magnets) (c), EDS line-scan profiles for hot-deformed Ce₁₇Fe₇₈B₆ magnet (d)^[89], and comparison of H_cj and J_r for hot-deformed (Ce, La)-Fe-B and (Ce, La, Y)-Fe-B magnets with available reported hot-deformed Ce-Fe-B magnets^[16,87-93] (e)

Fig.10 Demagnetizations curves (a) and stress-strain (σ-ε) curves (b) of Nd_26.4Fe_67.6Co₅B, Nd₆Pr₂La_6.7Ce_13.4Fe_69.3Zr_1.5B_1.1 and [(Ce_0.7La_0.3)_0.8Y_0.2]₁₇Fe₇₈B₆ bonded magnets (Inset shows the macroscopic image of bonded [(Ce_0.7La_0.3)_0.8Y_0.2]₁₇Fe₇₈B₆ magnet), and metallographic microstructures of Nd_26.4Fe_67.6Co₅B (c) and [(Ce_0.7La_0.3)_0.8Y_0.2]₁₇Fe₇₈B₆ bonded (d) magnets^[103]

Fig.11 Demagnetizations curves (Inset shows the optical image of [(Ce_0.7La_0.3)_0.8Y_0.2]₁₇Fe₇₈B₆ rubber magnet) (a) and tensile curves (Inset shows the metallographic microstructure of [(Ce_0.7La_0.3)_0.8Y_0.2]₁₇Fe₇₈B₆ rubber magnet) (b) of Nd_26.4Fe_67.6Co₅B, Nd₆Pr₂La_6.7Ce_13.4Fe_69.3Zr_1.5B_1.1, and [(Ce_0.7La_0.3)_0.8Y_0.2]₁₇Fe₇₈B₆ rubber magnets, comparison of magnetic properties of (Ce, La, Y)-Fe-B rubber magnets with commercial rubber ferrite and Nd-Fe-B rubber magnet (c), and potential applications of the (Ce, La, Y)-Fe-B rubber magnets (d)^[105]

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