全高丰度稀土<strong>(Ce, La, Y)-Fe-B</strong>永磁的研究现状和未来发展

doi:10.11900/0412.1961.2023.00117

金属学报

2024, Vol. 60

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

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全高丰度稀土(Ce, La, Y)-Fe-B永磁的研究现状和未来发展

刘仲武¹(

), 周帮¹, 廖雪峰¹^,², 何家毅¹^,³

1 华南理工大学材料科学与工程学院广州 510640
2 广东省科学院资源利用与稀土开发研究所广东省稀土开发及应用研究重点实验室广州 510650
3 中国科学院深圳先进技术研究院材料科学与能源工程学院深圳 518055

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

引用本文:

刘仲武, 周帮, 廖雪峰, 何家毅. 全高丰度稀土(Ce, La, Y)-Fe-B永磁的研究现状和未来发展[J]. 金属学报, 2024, 60(5): 585-604.
Zhongwu LIU, Bang ZHOU, Xuefeng LIAO, Jiayi HE. Research Status and Future Development of (Ce, La, Y)-Fe-B Permanent Magnets Based on Full High-Abundance Rare Earth Elements[J]. Acta Metall Sin, 2024, 60(5): 585-604.

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摘要:

随着市场对Nd-Fe-B永磁材料需求的不断增加，昂贵的Nd、Pr、Dy和Tb等关键稀土元素的消耗也日益增加，而廉价的Ce、La和Y等高丰度稀土元素积压严重。开发不含关键稀土元素的全高丰度永磁材料有望填补永磁铁氧体和黏结Nd-Fe-B磁体之间的性能空白，不仅可以满足中低端市场领域对永磁材料的多样化需求，也利于实现稀土资源的平衡利用。然而，目前针对Ce、La、Y基稀土永磁的理解和认识还有待深入，所获得的高丰度稀土永磁的性能普遍较低，难以实际应用。本文基于国内外最新进展和作者团队的研究工作，总结了近期关于不含关键稀土Nd、Pr、Dy和Tb的(Ce, La, Y)-Fe-B永磁合金和磁体的研究现状。重点关注了纳米晶快淬三元合金的相结构和冶金行为以及多元合金的成分设计与元素交互作用，详细阐述了全高丰度稀土基致密化磁体的制备工艺、显微组织与磁性能之间的关系。最后对全高丰度稀土永磁的未来发展趋势进行了展望。

关键词 ：稀土永磁, 高丰度稀土, 元素交互作用, 微观结构, 磁性能

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

收稿日期: 2023-03-23

ZTFLH:

TM273

基金资助:国家自然科学基金项目(U21A2052);国家自然科学基金项目(52071143);中国博士后科学基金面上项目(2022M720845)

通讯作者: 刘仲武，zwliu@scut.edu.cn，主要从事稀土永磁材料、软磁材料、先进金属材料研究

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

作者简介: 刘仲武，男，1971年生，教授，博士

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图1 稀土元素的地壳丰度、价格和各自在Nd-Fe-B磁体中的使用率[4~7]，高丰度稀土RE2Fe14B化合物的相关性能参数[3,9]以及各类永磁材料的性能对比[11]

图2 Nd-Fe-B和Ce-Fe-B相组分示意图，快淬Ce16Fe78B6合金在300和77 K时57Fe的Mössbauer谱以及合金在室温下的微观结构[17]

图3 (La1 - x Y x )2Fe14B快淬合金的XRD谱与微观结构[28,35]

表1 Ce2Fe14B、La2Fe14B和Y2Fe14B非晶合金热处理过程中的相析出行为[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

表2 基于高丰度稀土Ce、La、Y的RE-Fe-B快淬合金的硬磁性能[17,19,21~23,28,29,35,36,38,40,42~48]

图4 (Ce, La, Y)17Fe78B6快淬合金的退磁曲线，及TEM像和晶界处的EDS线扫结果[42]

图5 (Ce, La, Y)17Fe78B6合金与其他RE-Fe-B合金在磁性能[17,21~23,37,38,40,42~46,55~64]、性价比以及腐蚀性能[28,65~70]方面的对比

图6 (Ce1 - x La x )Fe2相的形成能、(Ce1 - x La x )17Fe78B6快淬合金的XRD精修图谱[42]以及Ce17Fe78 - x B6Si x[55]和Ce16Fe78 - x B6Ge x 快淬合金的退磁曲线[74]

图7 Ce17Fe78 - x B6Ta x (x = 0、0.75) 快淬合金的退磁曲线及其对应的微磁学模拟结果[56] (w/o和w/分别表示不含非磁性析出相的磁体模型和含有非磁性析出相的磁体模型)

图8 不同温度下放电等离子烧结(SPS)制备Ce17Fe78B6磁体的微观结构和磁性能[83]

图9 Ce-Fe-B、(Ce, La)-Fe-B和(Ce, La, Y)-Fe-B热变形磁体的磁滞回线、微观结构[89]以及与其他铈基热变形磁体[16,87~93]的性能对比

图10 Nd26.4Fe67.6Co5B, Nd6Pr2La6.7Ce13.4Fe69.3Zr1.5B1.1和[(Ce0.7La0.3)0.8Y0.2]17Fe78B6黏结磁体的退磁曲线、压缩应力/应变曲线以及金相显微组织[103]

图11 [(Ce0.7La0.3)0.8Y0.2]17Fe78B6橡胶磁体的退磁曲线、拉伸曲线、性能对比及其潜在的应用领域[105]

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