晶界添加PrCu合金对(Pr, Nd, Dy)32.2Co13Cu0.4FebalB0.98M1.05磁体磁性能与微观组织的影响

张家滕; 徐吉元; 金佳莹; 孟睿阳; 董生智

doi:10.7498/aps.71.20220406

摘要

通过在(Pr, Nd, Dy)_32.2Co₁₃Cu_0.4Fe_balB_0.98M_1.05(M = Al, Ga, Zr)磁体中添加低熔点合金Pr₈₀Cu₂₀, 提高磁体中的Cu含量, 从而调控Co在富稀土相中的分布. 相较于原磁体, 掺PrCu磁体的剩磁保持不变, 矫顽力提升约1.3 kOe, 居里温度、剩磁温度系数和不可逆磁损均有所改善. 通过微观组织观察发现, 原磁体二级回火态晶界处同时存在贫Co相与富Co相, 但掺PrCu磁体二级回火态中, Cu和Co在晶界相中的分布均匀性明显改善, 从而有效地消除了富Co相. 由于软磁性相R₂(Fe, Co)₁₇ (R = Pr, Nd, Dy) 容易与富Co相共生, 有害于永磁性能, 富Co相的消除可能是掺PrCu磁体二级回火态矫顽力提升的重要原因.

关键词:

Abstract

With the aim of increasing Cu concentration to regulate the distribution of Co elements in RE-rich phase, the low-melting-point Pr₈₀Cu₂₀ intergranular alloy is introduced into the (Pr, Nd, Dy)_32.2Co₁₃Cu_0.4Fe_balB_0.98M_1.05 (M = Al, Ga, Zr) magnet. Comparing with the original magnet, the remanence of PrCu-doped magnet is basically unchanged, and the coercivity is increased by approximately 1.3 kOe. Simultaneously, the Curie temperature, remanence temperature coefficient and irreversible flux loss are slightly improved. Microstructural study reveals that the Co-lean phase and the Co-rich phase coexist in the grain boundary in the 2^nd-annealed original magnet. However, for the PrCu-doped magnet, the uniform distribution of Cu and Co elements in the intergranular phase are evidently improved, resulting in the elimination of the Co-rich phase. Since the R₂(Fe, Co)₁₇ (R = Pr, Nd, Dy) soft magnetic phase easily coexist with the Co-rich phase and are detrimental to the coercivity, the elimination of Co-rich intergranular phase may be an important reason for the higher coercivity of the 2^nd-annealed PrCu-doped magnet than that of the original magnet.

Keywords:

sintered NdFeB magnet /
intergranular addition /
annealing /
opposite distribution between Cu and Co /
coercivity

作者及机构信息

1.
钢铁研究总院, 功能材料研究院, 北京　100081

2.
浙江大学材料科学与工程学院, 杭州　310027

通信作者: 董生智, dong_shengzhi@163.com

基金项目: 国家重点研发计划(批准号: 2021YFB3502900)资助的课题.

Authors and contacts

1.
Division of Functional Materials, Central Iron & Steel Research Institute, Beijing 100081, China

2.
School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China

Corresponding author: Dong Sheng-Zhi, dong_shengzhi@163.com

Funds: Project supported by the National Key R&D Program of China (Grant No. 2021YFB3502900).

文章全文

参考文献

[1]	Sagawa M, Fujimura S, Togawa N, Yamamoto H, Matsuura Y 1984 J. Appl. Phys. 55 2083 Google Scholar
[2]	Yan G L, McGuiness P J, Farr J P G, Harris I R 2010 J. Alloys Compd. J. Alloys Compd. 491 L20 Google Scholar
[3]	Mottram R S, Williams A J, Harris I R 2000 J. Magn. Magn. Mater. 217 27 Google Scholar
[4]	Hu Z H, Lian F Z, Zhu M G, Li W 2008 J. Magn. Magn. Mater. 320 2364 Google Scholar
[5]	Kostyuchenko N V, Tereshina I S, Gorbunoy D I, Tereshina-Chitrova E A, Rogacki K, Andreev A V, Doerr M, Politova G A, Zvezdin A K 2020 Intermetallics 124 106840 Google Scholar
[6]	Cui X G, Yan M, Ma T Y, Luo W, Tu S J 2009 Sci. Sinter. 41 91 Google Scholar
[7]	Brown D, Ma B M, Chen Z M 2002 J. Magn. Magn. Mater. 248 432 Google Scholar
[8]	Yan M, Yu L Q, Luo W, Wang W, Zhang W Y, Wen Y H 2006 J. Magn. Magn. Mater. 301 1 Google Scholar
[9]	Li W F, Ohkubo T, Hono K 2009 Acta Mater. 57 1337 Google Scholar
[10]	李栋, 董生智, 李磊, 徐吉元, 陈红升, 李卫 2020 物理学报 69 147501 Google Scholar Li D, Dong S Z, Li L, Xu J Y, Chen H S, Li W 2020 Acta Phys. Sin. 69 147501 Google Scholar
[11]	Kim A S, Camp F E 1996 J. Appl. Phys. 79 5035 Google Scholar
[12]	Pandian S, Chandrasekaran V, Markandeyulu G, Lyer K J L, Rao R 2002 J. Appl. Phys. 92 6082 Google Scholar
[13]	Ni J J, Ma T Y, Yan M 2011 J. Magn. Magn. Mater. 323 2549 Google Scholar
[14]	Li M, Tamura T 2021 J. Alloys Compd. 883 160915 Google Scholar
[15]	Luo S E, Lu Y J, Zou Y R, Zhong S W, Wu Y, Yang M N 2021 J. Magn. Magn. Mater. 523 167620 Google Scholar
[16]	张家滕, 徐吉元, 胡成林, 孟睿阳, 董生智 2022 中国稀土学报 40 235 Zhang J T, Xu J Y, Hu C L, Meng R Y, Dong S Z. 2022 J. Chin. Rare Earth Soc. 40 235
[17]	胡伯平, 饶晓雷, 王亦忠 2017 稀土永磁材料(上册) (北京: 冶金工业出版社) 第197页 Hu B P, Rao X L, Wang Y Z 2017 Rare-earth Permanent Magnet Materials (Vol. 1) (Beijing: Metallurgical Industry Press) p197 (in Chinese)
[18]	Kou X C, Zhao T S, R. Grössinger, de Boer F R 1992 Phys. Rev. B 46 6225 Google Scholar

施引文献

图 1 原磁体和掺PrCu磁体二级回火态样品不同温度下的退磁曲线

Fig. 1. Demagnetization curves of the 2^nd-annealed original-magnet and PrCu-doped magnet upon elevated temperatures.

下载: 全尺寸图片幻灯片

图 2 原磁体和掺PrCu磁体的温度稳定性对比　(a), (d) TG/DTG曲线; (b), (e) 不可逆磁损曲线; (c), (f) 剩磁温度系数

Fig. 2. Comparison of temperature stability of magnetic properties between original-magnet and PrCu-doped magnet: (a), (d) TG/DTG curves; (b), (e) irreversible flux loss curves; (c), (f) remanence temperature coefficient.

下载: 全尺寸图片幻灯片

图 3 (a) 原磁体烧结态、(b) 一级回火态和(c)二级回火态样品的扫描电镜背散射照片(BSE)及对应区域的能谱照片(EDS)

Fig. 3. SEM figure (BSE) and EDS figure of the corresponding region of original-magnet (a) as-sintered, (b) 1^st-annealing and (c) 2^nd-annealing.

下载: 全尺寸图片幻灯片

图 4 (a) 掺PrCu磁体烧结态、(b) 一级回火态和(c)二级回火态样品的扫描电镜背散射照片(BSE)及对应区域的能谱照片(EDS)

Fig. 4. SEM figure (BSE) and EDS figure of the corresponding region of PrCu-doped magnet (a) as-sintered, (b) 1^st-annealing and (c) 2^nd-annealing.

下载: 全尺寸图片幻灯片

图 5 原磁体透射电镜明场像照片(BF)及对应区域的元素面分布　(a) 烧结态; (b) 一级回火态; (c) 二级回火态

Fig. 5. Bright field image (BF) and corresponding EDX mapping of original-magnet: (a) As-sintered; (b) 1^st-annealing; (c) 2^nd-annealing.

下载: 全尺寸图片幻灯片

图 6 掺PrCu磁体透射电镜明场像照片(BF)及对应区域的选区电子衍射照片、元素面分布照片　(a) 烧结态; (b) 一级回火态; (c) 二级回火态

Fig. 6. Bright field image (BF) and corresponding Selected Area Electron Diffraction figure and EDX mapping of PrCu-doped magnet: (a) As-sintered; (b) 1^st-annealing; (c) 2^nd-annealing.

下载: 全尺寸图片幻灯片

表 1 原磁体和掺PrCu磁体的室温磁性能对比

Table 1. Comparison of magnetic properties between original-magnet and PrCu-doped magnet.

		剩磁B_r/kGs	矫顽力H_cj/kOe	最大磁能积 (BH)_max/ MGOe	方形度 H_k/H_cj/%
原磁体	烧结态	11.32	15.64	31.04	94.4
	一级回火态	11.30	17.22	30.88	95.0
	二级回火态	11.30	22.24	31.39	95.9
掺PrCu 磁体	烧结态	11.31	16.34	30.89	88.9
	一级回火态	11.30	17.60	30.51	89.3
	二级回火态	11.30	23.53	31.36	95.1

下载: 导出CSV

表 2 掺PrCu磁体三种状态样品中不同相的元素含量

Table 2. Element content of different phases in three kinds of PrCu-doped magnets.

	wt.%	O	Fe	Co	Cu	Pr	Nd	Dy
烧结态	主相	0.89	56.185	13.14	0.31	4.87	15.32	9.28
	贫Co相	4.02	4.63	1.98	1.13	24.68	56.75	6.83
	富Co相	0.96	20.54	23.62	0.47	13.66	34.62	6.14
一级回火态	主相	0.93	56.74	13.24	0.38	4.6	14.87	9.24
	贫Co相	4.79	2.67	1.79	1.61	25.37	56.98	6.79
	富Co相	1.15	11.72	16.01	0.58	20.15	44.2	6.19
二级回火态	主相	0.81	56.23	13.89	0.3	4.86	14.78	9.14
	贫Co相1	2.21	5.61	9.02	1.47	23.86	51.67	6.16
	贫Co相2	2.03	6.16	4.05	1.52	25.39	54.54	6.31

下载: 导出CSV

[1]	Sagawa M, Fujimura S, Togawa N, Yamamoto H, Matsuura Y 1984 J. Appl. Phys. 55 2083 Google Scholar
[2]	Yan G L, McGuiness P J, Farr J P G, Harris I R 2010 J. Alloys Compd. J. Alloys Compd. 491 L20 Google Scholar
[3]	Mottram R S, Williams A J, Harris I R 2000 J. Magn. Magn. Mater. 217 27 Google Scholar
[4]	Hu Z H, Lian F Z, Zhu M G, Li W 2008 J. Magn. Magn. Mater. 320 2364 Google Scholar
[5]	Kostyuchenko N V, Tereshina I S, Gorbunoy D I, Tereshina-Chitrova E A, Rogacki K, Andreev A V, Doerr M, Politova G A, Zvezdin A K 2020 Intermetallics 124 106840 Google Scholar
[6]	Cui X G, Yan M, Ma T Y, Luo W, Tu S J 2009 Sci. Sinter. 41 91 Google Scholar
[7]	Brown D, Ma B M, Chen Z M 2002 J. Magn. Magn. Mater. 248 432 Google Scholar
[8]	Yan M, Yu L Q, Luo W, Wang W, Zhang W Y, Wen Y H 2006 J. Magn. Magn. Mater. 301 1 Google Scholar
[9]	Li W F, Ohkubo T, Hono K 2009 Acta Mater. 57 1337 Google Scholar
[10]	李栋, 董生智, 李磊, 徐吉元, 陈红升, 李卫 2020 物理学报 69 147501 Google Scholar Li D, Dong S Z, Li L, Xu J Y, Chen H S, Li W 2020 Acta Phys. Sin. 69 147501 Google Scholar
[11]	Kim A S, Camp F E 1996 J. Appl. Phys. 79 5035 Google Scholar
[12]	Pandian S, Chandrasekaran V, Markandeyulu G, Lyer K J L, Rao R 2002 J. Appl. Phys. 92 6082 Google Scholar
[13]	Ni J J, Ma T Y, Yan M 2011 J. Magn. Magn. Mater. 323 2549 Google Scholar
[14]	Li M, Tamura T 2021 J. Alloys Compd. 883 160915 Google Scholar
[15]	Luo S E, Lu Y J, Zou Y R, Zhong S W, Wu Y, Yang M N 2021 J. Magn. Magn. Mater. 523 167620 Google Scholar
[16]	张家滕, 徐吉元, 胡成林, 孟睿阳, 董生智 2022 中国稀土学报 40 235 Zhang J T, Xu J Y, Hu C L, Meng R Y, Dong S Z. 2022 J. Chin. Rare Earth Soc. 40 235
[17]	胡伯平, 饶晓雷, 王亦忠 2017 稀土永磁材料(上册) (北京: 冶金工业出版社) 第197页 Hu B P, Rao X L, Wang Y Z 2017 Rare-earth Permanent Magnet Materials (Vol. 1) (Beijing: Metallurgical Industry Press) p197 (in Chinese)
[18]	Kou X C, Zhao T S, R. Grössinger, de Boer F R 1992 Phys. Rev. B 46 6225 Google Scholar

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晶界添加PrCu合金对(Pr, Nd, Dy)_32.2Co₁₃Cu_0.4Fe_balB_0.98M_1.05磁体磁性能与微观组织的影响

Effect of Pr₈₀Cu₂₀ grain boundary addition on microstructure and magnetic properties of (Pr, Nd, Dy)_32.2Co₁₃Cu_0.4Fe_balB_0.98M_1.05 magnet

摘要

Abstract

作者及机构信息

1.
钢铁研究总院, 功能材料研究院, 北京　100081

2.
浙江大学材料科学与工程学院, 杭州　310027

通信作者: 董生智, dong_shengzhi@163.com

Authors and contacts

1.
Division of Functional Materials, Central Iron & Steel Research Institute, Beijing 100081, China

2.
School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, China

Corresponding author: Dong Sheng-Zhi, dong_shengzhi@163.com

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