晶界添加Ho纳米粉对烧结NdFeB性能的影响
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摘要
为了改善NdFeB磁性材料的磁性能和防腐性能,采用双合金法在晶界处添加Ho纳米粉制备高性能永磁材料。对烧结永磁体(PrNd)_(29.9)Dy_(0.1)B_1Co_1Cu_(0.15)Fe_(bal)+xHo(添加Ho纳米粉的质量分数分别为0、0.2%、0.4%、0.6%和0.8%)的形貌、微观结构及成分、磁性能和腐蚀性进行了分析。结果表明,随着Ho元素含量的增加,磁体矫顽力增幅变大;剩磁和最大磁能积降幅渐快,从0.6%到0.8%下降幅度最大。当Ho添加量为0.6%时,综合性能达到最佳。磁体矫顽力达到1108 kA·m~(-1),提升了5.8%,剩磁和最大磁能积略微下降,分别为0.3%和0.2%;并且在3.5%NaCl溶液中,添加0.6%Ho纳米粉的钕铁硼磁体,腐蚀电流最小,达到0.327μA·cm~(-2),提升了近一个数量级;I_((006))/I_((105))比值算出,添加量为0.6%Ho时取向度为1.45,磁体密度增加1.6%,达到7.61 g·cm~(-3)。
The NdFeB magnetic materials were prepared by double alloy method with adding Ho nanopowder to grain boundaries to improve the magnetic property and corrosion-resistant performance. The morphology, phase, magnetic property and corrosion-resistant performance of(PrNd)_(29.9)Dy_(0.1)B_1Co_1Cu_(0.15)Fe_(bal)+xHo(x=0,0.2%,0.4%,0.6% and 0.8%, Mass fraction) were analyzed, respectively. The results indicate that the coercive force was enhanced with increase of Ho content, and the remanence and maximum magnetic energy product declined. When content of Ho was from 0.6% to 0.8%, the decline of the remanence and maximum magnetic energy product was the fastest. When adding 0.6% Ho powders, the combination property of samples was the best, the coercive force reached 1108 kA·m~(-1), with a increase of 5.8%,and the remanence and maximum magnetic energy product were fell down by 0.3% and 0.2%, respectively. In the 3.5%NaCl solution, the sample with 0.6% Ho powders reached the smallest corrosion current of 0.327 μA·cm~(-2). And the orientation degree of samples was 1.45 calculated by I_((006))/I_((105)), the magnet density reached to 7.61 g·cm~(-3), with a increase of 1.6%.
The NdFeB magnetic materials were prepared by double alloy method with adding Ho nanopowder to grain boundaries to improve the magnetic property and corrosion-resistant performance. The morphology, phase, magnetic property and corrosion-resistant performance of(PrNd)_(29.9)Dy_(0.1)B_1Co_1Cu_(0.15)Fe_(bal)+xHo(x=0,0.2%,0.4%,0.6% and 0.8%, Mass fraction) were analyzed, respectively. The results indicate that the coercive force was enhanced with increase of Ho content, and the remanence and maximum magnetic energy product declined. When content of Ho was from 0.6% to 0.8%, the decline of the remanence and maximum magnetic energy product was the fastest. When adding 0.6% Ho powders, the combination property of samples was the best, the coercive force reached 1108 kA·m~(-1), with a increase of 5.8%,and the remanence and maximum magnetic energy product were fell down by 0.3% and 0.2%, respectively. In the 3.5%NaCl solution, the sample with 0.6% Ho powders reached the smallest corrosion current of 0.327 μA·cm~(-2). And the orientation degree of samples was 1.45 calculated by I_((006))/I_((105)), the magnet density reached to 7.61 g·cm~(-3), with a increase of 1.6%.
引文
[1] 张雪峰,史孟飞,李培忠,戴永峰,马强,李永峰.Ce对NdFeB永磁体磁性能和微观结构的影响[J].稀土,2013,34(4):12-16.Zhang X F,Shi M F,Li P Z,Dai Y F,Ma Q,Li Y F.Effect of Ce addition on magnetic properties and microstructure of NdFeB based rare earth permanent magnets[J].Chinese Rare Earths,2013,34(4):12-16.
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[4] Hu Z H,Qu H J,Ma D W,Luo C,Wang H J.Influence of dysprosium substitution on magnetic and mechanical properties of high intrinsic coercivity Nd-Fe-B magnets prepared by double-alloy powder mixed method[J].Journal of Rare Earths,2016,34(7):689-694.
[5] Cui X G,Cui C Y,Cheng X N,Xu X J.Effect of Dy2O3,intergranular addition on thermal stability and corrosion resistance of Nd-Fe-B magnets[J].Intermetallics,2014,55(31):118-122.
[6] Liu P,Ma T Y,Wang X H,Zhang Y J,Yan M.Role of hydrogen in Nd-Fe-B sintered magnets with DyHx addition[J].Journal of Alloys & Compounds,2015,628(628):282-286.
[7] 饶晓雷,钮萼,胡伯平.Ce对烧结钕铁硼磁体永磁性的影响[J].中国材料进展,2017,36(1):63-74.Rao X L,Niu E,Hu B P.Effects of cerium on permanent magnetic properties of sintered Nd-Fe-B magnets [J].China Material Progress,2017,36(1):63-74.
[8] Isotahdon E,Huttunen-Saarivirta E,Kuokkala V T.Characterisation of the microstructure and corrosion performance of Ce-alloyed Nd-Fe-B magnets[J].Journal of Alloys & Compounds,2017,692:190-197.
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[11] Lukin A A,Il′Yashenko E I,Skjeltorp A T,Helgesen G.Improvement of thermal stability of Nd-Tb-Fe-Co-B sintered magnets by additions of Pr,Ho,Al and Cu[J].Physics Research International,2012,416717:1-4.
[12] Tereshina I S,Pelevin I A,Tereshina E A,Burkhanov G S,Rogacki K,Miller M,Kudrevatykh N V,Markin P E,Volegov A S,Grechishkin R M,Dobatkin S V,Schultz L.Magnetic hysteresis properties of nanocrystalline (Nd,Ho)-(Fe,Co)-B alloy after melt spinning,severe plastic deformation and subsequent heat treatment[J].Journal of Alloys & Compounds,2016,681:555-560.
[13] Andreeva N V,Filimonov A V,Rudskoi A I,Burkhanov G S,Tereshina I S,Politova G A,Pelevin I A.A study of nanostructure magnetosolid Nd-Ho-Fe-Co-B materials via atomic force microscopy and magnetic force microscopy[J].Physics of the Solid State,2016,58(9):1862-1869.
[14] Tereshina I S,Kudrevatykh N V,Ivanov L A,Politova G A,Tereshina E A,Gorbunov D,Doerr M,Rogacki K.Magnetic properties of the nanocrystalline Nd-Ho-Fe-Co-B alloy at low temperatures:The influence of time and annealing[J].Journal of Materials Engineering & Performance,2017,(3):1-5.
[15] Nakamura H,Hirota K,Ohashi T,Minowa T.Coercivity distributions in Nd-Fe-B sintered magnets produced by the grain boundary diffusion process[J].Journal of Physics D:Applied Physics,2011,44(6):1-5.
[16] 周寿增,董清飞.超强永磁体-稀土铁系永磁材料 [M].北京:冶金工业出版社,2010.Zhou S Z,Dong Q F.Super Permanent Magnet Rare-earth Iron Permanent Magnet Material[M].Beijing:Metallurgical Industry Press,2010.
[17] 赵明静,刘国征,刘小鱼,武斌,鲁富强,赵瑞金.辅合金的粉末尺寸对烧结钕铁硼磁性能和微结构的影响[J].中国稀土学报,2013,31(2):175-180.Zhao M J,Liu G Z,Liu X Y,Wu B,Lu F Q,Zhao R J.Influence of granule size of auxiliary alloy on microstructure and magnetic properties of sintered NdFeB magnets[J].Journal of Rare Earths,2013,31 (2):175-180.
[18] Li Z J,Wang X E,Li J Y,Li J,Wang H Z.Effects of Mg nanopowders intergranular addition on the magnetic properties and corrosion resistance of sintered Nd-Fe-B[J].Journal of Magnetism & Magnetic Materials,2017,442:62-66.
[19] 聂帅,刘鹏宇,李宝城,田佳,鲍叶琳,刘兵.钕铁硼合金中13种元素辉光放电质谱法定量分析研究[J].稀有金属,2016,40(8):756-762.Nie S,Liu P Y,Li B C,Tian J,Bao Y L,Liu B.Quantitative analysis of 13 elements in NdFeB alloy by glow discharge mass spectrometry [J].Rare Metals,2016,40 (8):756-762.
[20] 史秋月,马冬威,瞿海锦,赵佳奇,罗成,胡志华.双合金混粉法添加镝对烧结Nd-Fe-B磁体的磁性能及微观结构的影响[J].中国稀土学报,2016,34(1):38-43.Shi Q Y,Ma D W,Qu H J,Zhao J Q,Luo C,Hu Z H.Effect of dysprosium addition on the magnetic properties and microstructure of sintered Nd-Fe-B magnets prepared by dual-alloy powder mixing method[J].Journal of Chinese Society of Rare Earths,2016,34(1):38-43.
[21] 李岩峰,赖彬,朱明刚,冯海波,李卫,杜安.烧结钕铁硼磁体边界相的调控技术机制[J].稀有金属,2015,39(11):988-992.Li Y F,Lai B,Zhu M G,Feng H B,Li W,Du A.Mechanism on control technology of grain boundary phase in sintered Nd-Fe-B magnet [J].Rare Metals,2015,39 (11):988-992.
[22] 孙丽达,竺培显,陈敬超,周生刚.自由电弧法与等离子电弧法制备超细粉末对比研究[J].稀有金属材料与工程,2010,39(6):1085-1088.Sun L D,Zhu P X,Chen J C,Zhou S G.Contrast study on free arc method and arc plasma method for ultrafine powder preparation [J].Rare Metal Materials and Engineering,2010,39(6):1085-1088.
[23] 刘同冈,鲍久圣,杨志伊.直流钨电弧法制备碳包覆铁纳米微粒的研究[J].中国矿业大学学报,2007,36(2):201-204.Liu T G,Bao J S,Yang Z Y.Preparation of carbon coated iron nanoparticles by DC tungsten arc diacharge[J].Journal of China University of Mining and Technology,2007,36(2):201-204.
[24] Ni J J,Ma T Y,Yan M.Changes of microstructure and magnetic properties of Nd-Fe-B sintered magnets by doping Al-Cu[J].Journal of Magnetism & Magnetic Materials,2011,323(21):2549-2553.
[25] 张秀芝,支晨琛,薛康.钕铁硼永磁体电镀镍工艺优化及镀层性能[J].电镀与涂饰,2016,35(9):454-459.Zhang X Z,Zhi C C,Xue K.Process optimization of nickel plating on neodymium-iron-boron permanent magnet and the properties of nickel coating obtained thereby [J].Platening and Coating,2016,35(9):454-459.
[26] Zhou B B,Li X B,Liang X L,Yan G L,Chen K,Yan A R.Improvement of the magnetic property,thermal stability and corrosion resistance of the sintered Nd-Fe-B magnets with Dy80Al20 addition[J].Journal of Magnetism & Magnetic Materials,2017,429:257-262.
[2] Coey J M D.Permanent magnets:Plugging the gap[J].Scripta Materialia,2012,67(6):524-529.
[3] Zhou Q Y,Chen R J,Liu Z,Guo S,Yan A R,Li D.Effect of refractory metal substitution on magnetic property and corrosion behavior of sintered NdFeB magnets[J].Rare Metal Materials & Engineering,2015,44(10):2376-2380.
[4] Hu Z H,Qu H J,Ma D W,Luo C,Wang H J.Influence of dysprosium substitution on magnetic and mechanical properties of high intrinsic coercivity Nd-Fe-B magnets prepared by double-alloy powder mixed method[J].Journal of Rare Earths,2016,34(7):689-694.
[5] Cui X G,Cui C Y,Cheng X N,Xu X J.Effect of Dy2O3,intergranular addition on thermal stability and corrosion resistance of Nd-Fe-B magnets[J].Intermetallics,2014,55(31):118-122.
[6] Liu P,Ma T Y,Wang X H,Zhang Y J,Yan M.Role of hydrogen in Nd-Fe-B sintered magnets with DyHx addition[J].Journal of Alloys & Compounds,2015,628(628):282-286.
[7] 饶晓雷,钮萼,胡伯平.Ce对烧结钕铁硼磁体永磁性的影响[J].中国材料进展,2017,36(1):63-74.Rao X L,Niu E,Hu B P.Effects of cerium on permanent magnetic properties of sintered Nd-Fe-B magnets [J].China Material Progress,2017,36(1):63-74.
[8] Isotahdon E,Huttunen-Saarivirta E,Kuokkala V T.Characterisation of the microstructure and corrosion performance of Ce-alloyed Nd-Fe-B magnets[J].Journal of Alloys & Compounds,2017,692:190-197.
[9] 刘湘涟.添加Ho对烧结钕铁硼磁体结构与性能的影响[C].全国高新磁性材料及器件产学研讨论会,2012.Liu X L.Effect of addition of Ho on structure and performance of sintered NdFeB magnets [C].National High-tech Magnetic Materials and Devices Manufacturing Symposium,2012.
[10] 姚茂海,王川,刘宇晖,陈云志,苏正夫.Ho对烧结钕铁硼永磁体性能的影响[J].稀有金属与硬质合金,2016,44(3):51-55.Yao M H,Wang C,Liu Y H,Chen Y Z,Su Z F.Effect of Ho on properties of sintered NdFeB permanent magnets [J].Rare Metal and Cemented Carbides,2016,44(3):51-55.
[11] Lukin A A,Il′Yashenko E I,Skjeltorp A T,Helgesen G.Improvement of thermal stability of Nd-Tb-Fe-Co-B sintered magnets by additions of Pr,Ho,Al and Cu[J].Physics Research International,2012,416717:1-4.
[12] Tereshina I S,Pelevin I A,Tereshina E A,Burkhanov G S,Rogacki K,Miller M,Kudrevatykh N V,Markin P E,Volegov A S,Grechishkin R M,Dobatkin S V,Schultz L.Magnetic hysteresis properties of nanocrystalline (Nd,Ho)-(Fe,Co)-B alloy after melt spinning,severe plastic deformation and subsequent heat treatment[J].Journal of Alloys & Compounds,2016,681:555-560.
[13] Andreeva N V,Filimonov A V,Rudskoi A I,Burkhanov G S,Tereshina I S,Politova G A,Pelevin I A.A study of nanostructure magnetosolid Nd-Ho-Fe-Co-B materials via atomic force microscopy and magnetic force microscopy[J].Physics of the Solid State,2016,58(9):1862-1869.
[14] Tereshina I S,Kudrevatykh N V,Ivanov L A,Politova G A,Tereshina E A,Gorbunov D,Doerr M,Rogacki K.Magnetic properties of the nanocrystalline Nd-Ho-Fe-Co-B alloy at low temperatures:The influence of time and annealing[J].Journal of Materials Engineering & Performance,2017,(3):1-5.
[15] Nakamura H,Hirota K,Ohashi T,Minowa T.Coercivity distributions in Nd-Fe-B sintered magnets produced by the grain boundary diffusion process[J].Journal of Physics D:Applied Physics,2011,44(6):1-5.
[16] 周寿增,董清飞.超强永磁体-稀土铁系永磁材料 [M].北京:冶金工业出版社,2010.Zhou S Z,Dong Q F.Super Permanent Magnet Rare-earth Iron Permanent Magnet Material[M].Beijing:Metallurgical Industry Press,2010.
[17] 赵明静,刘国征,刘小鱼,武斌,鲁富强,赵瑞金.辅合金的粉末尺寸对烧结钕铁硼磁性能和微结构的影响[J].中国稀土学报,2013,31(2):175-180.Zhao M J,Liu G Z,Liu X Y,Wu B,Lu F Q,Zhao R J.Influence of granule size of auxiliary alloy on microstructure and magnetic properties of sintered NdFeB magnets[J].Journal of Rare Earths,2013,31 (2):175-180.
[18] Li Z J,Wang X E,Li J Y,Li J,Wang H Z.Effects of Mg nanopowders intergranular addition on the magnetic properties and corrosion resistance of sintered Nd-Fe-B[J].Journal of Magnetism & Magnetic Materials,2017,442:62-66.
[19] 聂帅,刘鹏宇,李宝城,田佳,鲍叶琳,刘兵.钕铁硼合金中13种元素辉光放电质谱法定量分析研究[J].稀有金属,2016,40(8):756-762.Nie S,Liu P Y,Li B C,Tian J,Bao Y L,Liu B.Quantitative analysis of 13 elements in NdFeB alloy by glow discharge mass spectrometry [J].Rare Metals,2016,40 (8):756-762.
[20] 史秋月,马冬威,瞿海锦,赵佳奇,罗成,胡志华.双合金混粉法添加镝对烧结Nd-Fe-B磁体的磁性能及微观结构的影响[J].中国稀土学报,2016,34(1):38-43.Shi Q Y,Ma D W,Qu H J,Zhao J Q,Luo C,Hu Z H.Effect of dysprosium addition on the magnetic properties and microstructure of sintered Nd-Fe-B magnets prepared by dual-alloy powder mixing method[J].Journal of Chinese Society of Rare Earths,2016,34(1):38-43.
[21] 李岩峰,赖彬,朱明刚,冯海波,李卫,杜安.烧结钕铁硼磁体边界相的调控技术机制[J].稀有金属,2015,39(11):988-992.Li Y F,Lai B,Zhu M G,Feng H B,Li W,Du A.Mechanism on control technology of grain boundary phase in sintered Nd-Fe-B magnet [J].Rare Metals,2015,39 (11):988-992.
[22] 孙丽达,竺培显,陈敬超,周生刚.自由电弧法与等离子电弧法制备超细粉末对比研究[J].稀有金属材料与工程,2010,39(6):1085-1088.Sun L D,Zhu P X,Chen J C,Zhou S G.Contrast study on free arc method and arc plasma method for ultrafine powder preparation [J].Rare Metal Materials and Engineering,2010,39(6):1085-1088.
[23] 刘同冈,鲍久圣,杨志伊.直流钨电弧法制备碳包覆铁纳米微粒的研究[J].中国矿业大学学报,2007,36(2):201-204.Liu T G,Bao J S,Yang Z Y.Preparation of carbon coated iron nanoparticles by DC tungsten arc diacharge[J].Journal of China University of Mining and Technology,2007,36(2):201-204.
[24] Ni J J,Ma T Y,Yan M.Changes of microstructure and magnetic properties of Nd-Fe-B sintered magnets by doping Al-Cu[J].Journal of Magnetism & Magnetic Materials,2011,323(21):2549-2553.
[25] 张秀芝,支晨琛,薛康.钕铁硼永磁体电镀镍工艺优化及镀层性能[J].电镀与涂饰,2016,35(9):454-459.Zhang X Z,Zhi C C,Xue K.Process optimization of nickel plating on neodymium-iron-boron permanent magnet and the properties of nickel coating obtained thereby [J].Platening and Coating,2016,35(9):454-459.
[26] Zhou B B,Li X B,Liang X L,Yan G L,Chen K,Yan A R.Improvement of the magnetic property,thermal stability and corrosion resistance of the sintered Nd-Fe-B magnets with Dy80Al20 addition[J].Journal of Magnetism & Magnetic Materials,2017,429:257-262.