基于磷化处理和双马来酰亚胺包覆铁粉的高性能磁粉芯的工艺优化

余红雅; 关少聪; 李竞舟; 刘仲武; 郭宝春; 陈榕寅

doi:10.13801/j.cnki.fhclxb.20220520.001

基于磷化处理和双马来酰亚胺包覆铁粉的高性能磁粉芯的工艺优化

doi: 10.13801/j.cnki.fhclxb.20220520.001

余红雅^{1, 2, 3, ,},
关少聪^{2, 3},
李竞舟¹,
刘仲武^{2, 3},
郭宝春^{1, 2, 3},
陈榕寅¹

1.
东莞铭普光磁股份有限公司，东莞 523330
2.
华南理工大学　材料科学与工程学院，广州 510640
3.
华南协同创新研究院，东莞 523808

基金项目: 东莞市引进创新科研团队项目(2020607231010)；广东省自然科学基金面上项目(2021A1515012464)

详细信息

通讯作者:
余红雅，博士，副教授，硕士生导师，研究方向为磁性功能材料、材料表面技术　E-mail: yuhongya@scut.edu.cn

中图分类号: TB331
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出版历程
- 收稿日期: 2022-03-28
- 修回日期: 2022-04-28
- 录用日期: 2022-05-08
- 网络出版日期: 2022-05-20
- 刊出日期: 2023-04-15

Process optimization of high-performance soft magnetic composite based on phosphate and bismaleimide coated iron powders

YU Hongya^{1, 2, 3
, ,},
GUAN Shaocong^{2, 3},
LI Jingzhou¹,
LIU Zhongwu^{2, 3},
GUO Baochun^{1, 2, 3},
CHEN Rongyin¹

1.
Dongguan Mentech Optical & Magnetic CO., LTD., Dongguan 523330, China
2.
School of Materials Science and Engineering, South China University of Technology, Guangzhou 510640, China
3.
South China Institute of Collaborative Innovation, Dongguan 523808, China

Funds: Dongguan Innovative Research Team Program (2020607231010); Guangdong Provincial Natural Science Fund of China (2021A1515012464)

摘要

摘要: 随着电子行业的迅速发展，电子器件正朝着小型化、集成化和高频化方向发展。磁粉芯材料会因应用频率提高引起磁损耗剧烈增加和严重发热而出现磁性能下降，磁粉芯材料的高频应用对其损耗特性和可靠性提出更高的要求。本文通过磷化处理和双马来酰亚胺树脂(BMI)包覆制备出了具有磷化-双马来酰亚胺@Fe结构的高性能磁粉芯，并研究了包覆方式对磁粉芯可靠性的影响。当BMI树脂添加量为2wt%，压制压力为800 MPa时，磁粉芯的综合磁性能最佳，有效磁导率为32.2，50 mT@200 kHz条件下的总损耗为1181 kW/m³，1 MHz条件下的品质因数Q可达到46.2。BMI树脂包覆形成的绝缘层可以起到应力缓冲的作用，减少压制过程中的内应力形成，降低磁粉芯的总损耗。傅里叶红外光谱分析证明磁粉芯的老化是由磁粉的氧化引起的，通过磷化处理和BMI树脂包覆能有效减缓磁粉氧化并提高磁粉芯的高温可靠性，经过180℃长期加速老化试验后，磁性能保持稳定。
- 磁性材料 /
- 双马来酰亚胺 /
- 磷化处理 /
- 耐热性 /
- 磁损耗 /
- 磁粉芯
Abstract: Electronic devices are developing towards miniaturization, integration, and high frequency with the development of electronic industry. The soft magnetic cores require better loss characteristics and higher reliability becaues their magnetic properties would decline due to the sharply increased magnetic loss and serious heating with the high-frequency application. In this work, high-performance soft magnetic composites with phosphate-bismaleimide@Fe structure were prepared by phosphating treatment and bismaleimide (BMI) coating, and the effects of insulation coating methods on the reliability of soft magnetic composites were investigated. The results indicate that the excellent comprehensive magnetic properties of soft magnetic composites have been obtained as the content of BMI resin is 2wt% and the compaction pressure is 800 MPa, the effective permeability is 32.2, the total loss is 1181 kW/m³ under the condition of 50 mT@200 kHz and the quality factor Q can reach 46.2 at 1 MHz. Moreover, it is found that the resin layer between iron powder particles can play a role of stress buffer to reduce the formation of internal stress and the total loss of soft magnetic composites. The aging of soft magnetic composites due to the oxidation of the magnetic powders which was proved by flourier infrared spectrum analysis. The phosphating treatment and BMI coating can effectively slow down the aging to improve the high-temperature reliability of soft magnetic composites and perform stable magnetic properties after long-term accelerated aging test at 180℃.
- magnetic material /
- bismaleimide /
- phosphate /
- heat resistance /
- magnetic loss /
- soft magnetic core

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图 1 磷化处理前后羰基铁粉的XRD图谱

Figure 1. XRD spectra of CIP before and after phosphating

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图 2 双马来酰亚胺树脂(BMI)树脂的DSC/TG曲线

Figure 2. DSC/TG curves of bismaleimide (BMI) resin

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图 3 磁粉的微观形貌：羰基铁粉(CIP)粉末((a)、(b))和磷化羰基铁粉(PCIP)粉末((c)、(d))；((e)~(h)) PCIP粉末的元素分布图

Figure 3. Micromorphologies of magnetic powders: Carbonyl iron powder (CIP) ((a), (b)) and phosphatized carbonyl iron powder (PCIP) ((c), (d)); ((e)-(h)) Element distribution diagram of PCIP

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图 4 不同BMI树脂添加量的PCIP微观形貌：(a) 1.0wt%；(b) 2.0wt%；(c) 3.0wt%

Figure 4. Micromorphologies of PCIP with different addition of BMI resin: (a) 1.0wt%; (b) 2.0wt%; (c) 3.0wt%

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图 5 不同磁粉的磁化曲线

Figure 5. Magnetization curves of different magnetic powders

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图 6 树脂添加量及压制压力对磁粉芯磁性能的影响：(a)密度ρ；(b) 磁导率μ_e；(c) 1 MHz条件下的品质因数Q

Figure 6. Effects of resin addition and press pressure on the magnetic properties of the composites: (a) Density ρ; (b) Permeability μ_e; (c) Quality factor Q under 1 MHz

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图 7 800 MPa压制压力下不同树脂添加量制备的磁粉芯磁性能：(a) 磁导率μ_e；(b) 品质因数Q

Figure 7. Magnetic properties of soft magnetic composites with different resin addition prepared under 800 MPa: (a) Permeability μ_e; (b) Quality factor Q

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图 8 800 MPa压制压力下BMI树脂添加量对总磁损耗P_s(50 mT@20~300 kHz)的影响

Figure 8. Effect of BMI resin addition on the sum of magnetic loss P_s (50 mT@20-300 kHz) of soft magnetic composites prepared under 800 MPa

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图 9 磁粉芯老化前后的表面形貌

Figure 9. Surface morphologies of soft magnetic composites before and after aging

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图 10 老化前后PCIP样品的傅里叶红外图谱

Figure 10. FTIR spectra of PCIP samples before and after aging

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表 1 磁粉样品的工艺参数

Table 1. Process parameters of magnetic powder samples

Sample number	Phosphoric acid solution concentration/wt%	BMI addition/wt%
CIP	0	0
PCIP	0.7	0
PCIP@1wt%BMI	0.7	1.0
PCIP@2wt%BMI	0.7	2.0
PCIP@3wt%BMI	0.7	3.0
CIP@2wt%BMI	0	2.0
Notes: BMI—Bismaleimide; CIP—Carbonyl iron powder; PCIP—Phosphatized carbonyl iron powder.

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表 2 800 MPa压制压力下磁粉芯的性能数据

Table 2. Properties data of soft magnetic composites prepared under 800 MPa

Sample number	ρ/(g·cm⁻³)	μ_e	Q_{(1 MHz)}	P_s/(kW·m⁻³)@50 mT
Sample number	ρ/(g·cm⁻³)	μ_e	Q_{(1 MHz)}	100 kHz	200 kHz	300 kHz
CIP	6.92	69.9	18.2	3358	18410	—
CIP@2wt%BMI	6.69	45.5	53.3	569	1171	1829
PCIP	6.80	52.7	62.2	630	1313	2013
PCIP@1wt%BMI	6.72	40.7	44.5	594	1123	1766
PCIP@2wt%BMI	6.43	32.2	46.2	612	1181	1858
PCIP@3wt%BMI	6.20	21.9	41.4	656	1290	2065

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表 3 高温加速老化实验前后磁粉芯磁性能

Table 3. Magnetic performance of soft magnetic composites before and after high-temperature accelerated aging test

Sample	Parameter	Aging time 0 h	Aging time 100 h	Change rate
PCIP	μ_e	44.6	43.8	1.7%
PCIP	Q_{(1 MHz)}	62.2	24.2	61.1%
CIP@2wt% BMI	μ_e	37.2	36.3	2.4%
CIP@2wt% BMI	Q_{(1 MHz)}	53.3	33.5	37.1%
PCIP@2wt% BMI	μ_e	29.3	28.7	2.0%
PCIP@2wt% BMI	Q_{(1 MHz)}	46.2	45.6	1.3%

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