CN114206804B - 钌掺杂的z型六方铁氧体 - Google Patents

钌掺杂的z型六方铁氧体 Download PDF

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CN114206804B
CN114206804B CN202080053600.8A CN202080053600A CN114206804B CN 114206804 B CN114206804 B CN 114206804B CN 202080053600 A CN202080053600 A CN 202080053600A CN 114206804 B CN114206804 B CN 114206804B
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ferrite
gigahertz
ferrite composition
article
frequency
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CN114206804A (zh
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李启凡
陈亚杰
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Rogers Corp
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Abstract

在一个方面中，铁氧体组合物包含具有式(Ba3‑xMx)Co2(M'Ru)yFe24‑2y‑zO41的Ru‑Co2Z铁氧体，其中M为Sr、Pb或Ca中的至少一者；M'为Co、Zn、Mg或Cu中的至少一者；x为1至3；y为大于0至为2；以及z为‑4至4。在另一个方面中，制品包含所述铁氧体组合物。在又一个方面中，制造所述铁氧体组合物的方法包括将包含Fe、Ba、Co和Ru的铁氧体前体化合物混合；以及在氧气气氛中对所述铁氧体前体化合物进行烧结以形成所述Ru‑Co2Z铁氧体。

Description

钌掺杂的Z型六方铁氧体
相关申请的交叉引用
本申请要求2019年8月5日提交的美国临时专利申请序列号62/882,681的权益。相关申请通过引用整体并入本文。
背景技术
需要改善的性能和小型化以满足在超高频(ultrahigh frequency，UHF)、L波段和S波段应用中使用的装置的不断增长的需求，其在各种商业和国防相关行业中特别受关注。作为雷达和现代无线通信***中的重要组件，正在不断开发具有紧凑尺寸的天线元件。然而，开发用于这样的高频应用中的铁氧体材料具有挑战性，因为大多数铁氧体材料在高频下表现出相对高的磁损耗。通常，六角铁氧体或六方铁氧体为具有六方晶体结构并且表现出磁特性的一类铁氧化物陶瓷化合物。已知数种类型的六方铁氧体族，包括Z型铁氧体Ba3Me2Fe24O41和Y型铁氧体Ba2Me2Fe12O22，其中Me可以为可以替代Ba的小的2+阳离子，例如Co、Ni、或Zn和Sr。另外的六方铁氧体类型包括M型铁氧体((Ba,Sr)Fe12O19)、W型铁氧体((Ba,Sr)Me2Fe16O27)、X型铁氧体((Ba,Sr)2Me2Fe28O46)和U型铁氧体((Ba,Sr)4Me2Fe36O60)。
与尖晶石铁氧体相比，一些六方铁氧体例如钴替代钡的Y型(Co2Y)和Z型(Co2Z)六方铁氧体可以具有高得多的铁磁共振频率和磁导率，使得它们在高频应用中具有吸引力。尽管具有这些改善，但它们在高频和微波装置中的使用受到限制，因为这些替代也导致磁损耗的增加。虽然Z型铁氧体为高阻抗磁介电复合材料的候选者，但是高的磁损耗限制了其使用。因此期望改善的Z型铁氧体。
发明内容
本文公开了钌掺杂的z型六方铁氧体。
在一个方面中，铁氧体组合物包含具有式(Ba3-xMx)Co2(M'Ru)yFe24-2y-zO41的Ru-Co2Z铁氧体，其中M为Sr、Pb或Ca中的至少一者；M'为Co、Zn、Mg或Cu中的至少一者；x为1至3；y为大于0至为2；以及z为-4至4。
在另一个方面中，制品包含所述铁氧体组合物或铁氧体复合材料中的至少一者。
在又一个方面中，制造所述铁氧体组合物的方法包括将包含Fe、Ba、Co和Ru的铁氧体前体化合物混合；以及在氧气气氛中对所述铁氧体前体化合物进行烧结以形成Ru-Co2Z铁氧体。
上述特征和其他特征通过以下附图、具体实施方式和权利要求书来例示。
附图说明
以下附图为示例性实施方案，提供这些附图是为了举例说明本公开内容。附图是说明实施例的，其不旨在将根据本公开内容制造的装置限于本文中阐述的材料、条件或工艺参数。
图1是实施例1、2、4和6的磁导率和磁损耗角正切随频率的图示说明；
图2是实施例3、5和7的磁导率和磁损耗角正切随频率的图示说明；
图3是实施例4、6和8的磁导率和磁损耗角正切随频率的图示说明；
图4是实施例4、6和8的介电常数和介电损耗角正切随频率的图示说明；
图5是实施例9和10的磁导率和磁损耗角正切随频率的图示说明；以及
图6是实施例9和10的介电常数和介电损耗角正切随频率的图示说明。
具体实施方式
发现用钌替代Z型六方铁氧体中的至少一部分铁离子可以产生具有改善的特性的Ru-Co2Z铁氧体。具体地，Ru-Co2Z铁氧体可以具有以下通式：
(Ba3-xMx)Co2(M′Ru)yFe24-2y-zO41
其中M为Sr、Pb或Ca中的至少一者；M'为Co、Zn、Mg或Cu中的至少一者；x为1至3；y大于0至为2、或0.001至2；以及z为-4至4。M'可以为Co。Ru与M'的比率可以为0.01至3或0.01至1。可变的z可以修改成不为零以包括非化学计量的式。
Ru-Co2Z铁氧体可以具有平面易磁化(c-平面)。Ru-Co2Z铁氧体可以具有高磁导率、高工作频率或低磁损耗中的至少一者，使得其适合于用作在S-L波段频率下的天线或感应器。Ru-Co2Z铁氧体在固体陶瓷的形式下在1吉赫至2吉赫或2吉赫至4吉赫的频率下可以具有大于或等于3.5、或者大于或等于5、或者5至10的磁导率。Ru-Co2Z铁氧体在固体陶瓷的形式下在1吉赫至2吉赫的频率下可以具有小于或等于0.4、小于或等于0.2、或者小于或等于0.1、或者小于或等于0.08、或者0.04至0.4的磁损耗角正切tanδμ。Ru-Co2Z铁氧体在固体陶瓷的形式下在1吉赫至2吉赫的频率下可以具有6至15、或6至12、或10至14的介电常数。Ru-Co2Z铁氧体在固体陶瓷的形式下在1吉赫至2吉赫的频率下可以具有小于或等于0.15、小于或等于0.009、或者小于或等于0.008、或者0.002、或者0.001至0.15的介电损耗角正切tanδε。Ru-Co2Z铁氧体在固体陶瓷的形式下可以具有0.1吉赫至4吉赫、或0.5吉赫至2吉赫、或1吉赫至2吉赫的工作频率。
Ru-Co2Z铁氧体在超高频范围内可以具有低的介电损耗角正切tanδε或磁损耗角正切tanδμ中的至少一者。例如，Ru-Co2Z铁氧体在固体陶瓷的形式下在1吉赫至2吉赫的频率下可以具有以下中的至少一者：小于或等于0.01、或者小于或等于0.008、或0.006至0.01的介电损耗角正切tanδε；或者小于或等于0.12、或者小于或等于0.08、或0.05至0.12的磁损耗角正切tanδμ。
如本文所用，磁特性和介电特性使用Nicholson-Ross-Weir(NRW)法通过矢量网络分析仪(vector network analyzer，VNA)在同轴空气线(coaxial airline)中测量，并且磁导率值和介电常数值分别为相对磁导率和相对介电常数。
Ru-Co2Z铁氧体可以使用任何合适的方法来制备。通常，Ru-Co2Z铁氧体可以通过首先形成包含前体化合物的混合物来形成，所述前体化合物包括至少Ba、M、Co、Ru和Fe的氧化物，其中M为Sr、Pb或Ca中的至少一者。例如，混合物可以包含至少BaCO3、MCO3、Co3O4、RuO2和Fe2O3。基于混合物的总重量，混合物可以包含5重量百分比至20重量百分比的BaCO3。基于混合物的总重量，混合物可以包含5重量百分比至50重量百分比的MCO3。基于混合物的总重量，混合物可以包含2重量百分比至15重量百分比的Co3O4。基于混合物的总重量，混合物可以包含0.1重量百分比至10重量百分比的RuO2。基于混合物的总重量，混合物可以包含50重量百分比至80重量百分比的Fe2O3。混合物还可以包含Zn、Mg或Cu中的至少一者的氧化物。应注意，混合物的重量百分比可以基于混合物中的氧化物的总重量。
可以将混合物在空气中煅烧以形成包含Z型铁氧体的铁氧体。煅烧可以在800摄氏度(℃)至1300℃的煅烧温度下进行。煅烧可以进行0.5小时至20小时、1小时至10小时、或2小时至5小时的煅烧时间。应注意，煅烧步骤是任选的，并且唯一的加热步骤可以是进行烧结以形成铁氧体。
可以将铁氧体破碎并任选地进行筛分以形成颗粒状物。筛分可以包括通过10目至100目筛网进行筛分。可以将粗颗粒进一步研磨以减小颗粒尺寸。颗粒状物按体积计的中值D50颗粒尺寸可以为0.5微米至50微米、或0.5微米至10微米。颗粒尺寸可以使用Horiba LA-910激光散射PSD分析仪或者如根据ASTM D4464-15所确定的来确定。可以将铁氧体与粘结剂混合。粘结剂可以包含聚(乙烯醇)、甲基纤维素、聚(乙烯醇缩丁醛)、聚(乙二醇)或聚(碳酸亚烷酯)中的至少一者。基于铁氧体加粘结剂的总量，粘结剂可以以8重量百分比至12重量百分比的量存在。粘结剂可以促进铁氧体的成形并且可以在烧结期间被完全烧掉。粘结的铁氧体按体积计的中值D50颗粒尺寸可以为10微米至300微米、或50微米至300微米。
可以任选地使铁氧体成形并烧结以形成Ru-Co2Z铁氧体。成形的方法没有限制并且可以包括单轴压缩、等静压、铸造、压制等中的至少一者。压制可以在0.5公吨/平方厘米至2公吨/平方厘米的压力下进行。烧结可以在1000℃至1300℃、或1200℃至1250℃的烧结温度下进行。从烧结温度向上和向下的渐变温度可以各自独立地以1℃/分钟至5℃/分钟的渐变速率进行。烧结可以进行1小时至20小时、或5小时至12小时的烧结时间。烧结可以在氧气环境中进行，以帮助降低介电损耗。可以以0.1升/分钟至10升/分钟的流量向烧结室中引入氧气。经烧结的Ru-Co2Z铁氧体可以根据应用以任何期望的方式例如通过切割或抛光进行精加工。
在烧结之前，可以向铁氧体中添加一定量的氧化铋。基于铁氧体的总重量，氧化铋可以以0.2重量百分比至5重量百分比的量添加。添加可以存在于Z型铁氧体相的晶界处的Bi2O3可以有助于实现具有相等或基本上相等的磁导率值和介电常数值同时保持低的磁损耗角正切和介电损耗角正切的组合物。
Ru-Co2Z铁氧体的平均晶粒尺寸可以为1微米至100微米、或5微米至50微米。晶粒尺寸可以使用透射电子显微术、场发射扫描电子显微术或X射线衍射中的至少一者来测量。
Ru-Co2Z铁氧体可以为块体陶瓷或者可以存在于复合材料例如包含Ru-Co2Z铁氧体和聚合物的复合材料中。所述聚合物可以包括热塑性的或热固性的。如本文所用，术语“热塑性的”是指这样的材料：其是塑性的或可变形的，当加热时熔化成液体，并且当充分冷却时冷冻结成脆性的玻璃态。可以使用的热塑性聚合物的实例包括环烯烃聚合物(包括聚降冰片烯和包含降冰片烯基单元的共聚物，例如诸如降冰片烯的环状聚合物与诸如乙烯或丙烯的无环烯烃的共聚物)、含氟聚合物(例如，聚氟乙烯(PVF)、聚偏二氟乙烯(PVDF)、氟化乙烯-丙烯(FEP)、聚四氟乙烯(PTFE)、聚(乙烯-四氟乙烯)(PETFE)或全氟烷氧基(PFA))、聚缩醛(例如，聚氧乙烯和聚甲醛)、聚(C1-6烷基)丙烯酸酯、聚丙烯酰胺(包括未经取代的和单-N-或二-N-(C1-8烷基)丙烯酰胺)、聚丙烯腈、聚酰胺(例如，脂族聚酰胺、聚邻苯二甲酰胺或聚芳酰胺)、聚酰胺酰亚胺、聚酸酐、聚亚芳基醚(例如，聚苯醚)、聚亚芳基醚酮(例如，聚醚醚酮(PEEK)和聚醚酮酮(PEKK))、聚亚芳基酮、聚亚芳基硫醚(例如，聚苯硫醚(PPS))、聚亚芳基砜(例如，聚醚砜(PES)、聚苯砜(PPS)等)、聚苯并噻唑、聚苯并
Figure BDA0003487202400000051
唑、聚苯并咪唑、聚碳酸酯(包括均聚碳酸酯或聚碳酸酯共聚物，例如聚碳酸酯-硅氧烷、聚碳酸酯-酯或聚碳酸酯-酯-硅氧烷)、聚酯(例如，聚对苯二甲酸乙二醇酯、聚对苯二甲酸丁二醇酯、聚芳酯或聚酯共聚物例如聚酯-醚)、聚醚酰亚胺(例如，诸如聚醚酰亚胺-硅氧烷共聚物的共聚物)、聚酰亚胺(例如，诸如聚酰亚胺-硅氧烷共聚物的共聚物)、聚(C1-6烷基)甲基丙烯酸酯、聚烷基丙烯酰胺(例如，未经取代的和单-N-或二-N-(C1-8烷基)丙烯酰胺)、聚烯烃(例如聚乙烯，如高密度聚乙烯(HDPE)、低密度聚乙烯(LDPE)和线性低密度聚乙烯(LLDPE)、聚丙烯、及其卤化衍生物(例如聚四氟乙烯)、及其共聚物(例如乙烯-α-烯烃共聚物))、聚/>
Figure BDA0003487202400000052
二唑、聚甲醛、聚苯酞(polyphthalide)、聚硅氮烷、聚硅氧烷(有机硅)、聚苯乙烯(例如，诸如丙烯腈-丁二烯-苯乙烯(ABS)或甲基丙烯酸甲酯-丁二烯-苯乙烯(MBS)的共聚物)、聚硫化物、聚磺酰胺、聚磺酸酯、聚砜、聚硫酯、聚三嗪、聚脲、聚氨酯、乙烯基聚合物(例如，聚乙烯醇、聚乙烯酯、聚乙烯醚、聚卤代乙烯(例如聚氯乙烯)、聚乙烯酮、聚乙烯腈、或聚乙烯硫醚)、石蜡等。可以使用包含前述热塑性聚合物中的至少一者的组合。
热固性聚合物源自经聚合或固化而可以不可逆地硬化并变得不可溶的热固性单体或预聚物(树脂)，所述聚合或固化可以通过热或暴露于辐射(例如紫外光、可见光、红外光或电子束(e-beam)辐射)来引发。热固性聚合物包括醇酸树脂、双马来酰亚胺聚合物、双马来酰亚胺三嗪聚合物、氰酸酯聚合物、苯并环丁烯聚合物、苯并
Figure BDA0003487202400000061
嗪聚合物、邻苯二甲酸二烯丙酯聚合物、环氧树脂、羟甲基呋喃聚合物、三聚氰胺-甲醛聚合物、酚醛树脂(包括酚-甲醛聚合物，例如酚醛清漆和甲阶酚醛树脂)、苯并/>
Figure BDA0003487202400000062
嗪、聚二烯例如聚丁二烯(包括其均聚物和共聚物，例如聚(丁二烯-异戊二烯))、聚异氰酸酯、聚脲、聚氨酯、氰脲酸三烯丙酯聚合物、异氰脲酸三烯丙酯聚合物、某些有机硅、以及可聚合预聚物(例如，具有烯属不饱和性的预聚物，如不饱和聚酯、聚酰亚胺)等。预聚物可以是例如用诸如以下的反应性单体下聚合的、共聚的或交联的：苯乙烯、α-甲基苯乙烯、乙烯基甲苯、氯苯乙烯、丙烯酸、(甲基)丙烯酸、丙烯酸(C1-6烷基)酯、甲基丙烯酸(C1-6烷基)酯、丙烯腈、乙酸乙烯酯、乙酸烯丙酯、氰脲酸三烯丙酯、异氰脲酸三烯丙酯、或丙烯酰胺。
形成复合材料的方法没有限制并且可以包括注射成型、反应注射成型、层合、挤出、压缩成型、压延、铸造等。复合材料可以不含空隙空间。
制品可以包含Ru-Co2Z铁氧体。制品可以为天线或感应器芯。制品可以用于0.1吉赫至4吉赫范围内或0.5吉赫至2吉赫范围内的频率。制品可以用于可在超高频范围内工作的各种装置例如高频或微波天线、滤波器、感应器、环行器或移相器。制品可以是可在大于或等于0.1GHz的频率下、或者在大于或等于0.3GHz的频率下工作的。这样的制品可以用于商业应用和军事应用、天气雷达、科学通信、无线通信、自控车辆、飞机通信、空间通信、卫星通信、或监测。
如本文所公开的，铁氧体组合物可以包含具有式(Ba3-xMx)Co2(M'Ru)yFe24-2y-zO41的Ru-Co2Z铁氧体，其中M为Sr、Pb或Ca中的至少一者；M'为Co、Zn、Mg或Cu中的至少一者；x为1至3；y大于0至为2、或0.001至2；以及z为-4至4。M'可以为至少Co。Ru与M'的比率可以为0.01至3。基于铁氧体组合物的总重量，铁氧体组合物还可以以0.2重量百分比至5.0重量百分比的量包含Bi2O3。铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下可以具有大于或等于3.5的磁导率。铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下可以具有6至15的介电常数。铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下可以具有小于或等于0.12、或者小于或等于0.08的磁损耗角正切tanδμ。铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下可以具有小于或等于0.01、或者小于或等于0.008的介电损耗角正切tanδε。复合材料可以包含铁氧体组合物和聚合物。制品可以包含铁氧体组合物或复合材料。制品可以为天线、滤波器、感应器、环行器、或移相器。制品可以为微波天线。天线可以是可在大于或等于0.1吉赫、或者大于或等于0.3吉赫、或者0.1吉赫至4吉赫的频率下工作的。
制造铁氧体组合物的方法可以包括：将包含Fe、Ba、Co和Ru的铁氧体前体化合物混合；以及在氧气气氛中对铁氧体前体化合物进行烧结以形成Ru-Co2Z铁氧体。铁氧体前体化合物可以包含BaCO3、MCO3、Co3O4、RuO2和Fe2O3，其中M为Sr、Pb或Ca中的至少一者。铁氧体前体化合物可以包含5重量百分比至20重量百分比的BaCO3、5重量百分比至20重量百分比的MCO3、2重量百分比至15重量百分比的Co3O4、0.1重量百分比至10重量百分比的RuO2、和50重量百分比至80重量百分比的Fe2O3；全部均基于混合物的总重量。烧结可以在1000℃至1300℃、或1200℃至1250℃的烧结温度下进行1小时至20小时、或5小时至12小时的烧结时间。所述方法还可以包括在烧结之前在空气中对铁氧体前体化合物进行煅烧。所述方法还可以包括在烧结之前将铁氧体前体化合物与粘结剂混合。所述方法还可以包括在烧结之前使铁氧体前体化合物成形。
提供以下实施例以举例说明本公开内容。实施例仅为说明性的，并不旨在将根据本公开内容制造的装置限于本文中阐述的材料、条件或工艺参数。
实施例
在实施例中，使用Nicholson-Ross-Weir(NRW)法通过矢量网络分析仪(VNA)在0.1GHz至10GHz的频率下在同轴空气线中测量所得铁氧体样品的磁导率。
实施例1至8：Ru-Co2Z铁氧体样品的制备
改变通式(Ba1.5Sr1.5)Co2(CoRu)yFe22.4-2yO41中钌的量y以形成如表1所示的铁氧体组合物来形成Ru-Co2Z铁氧体样品。通过在湿式行星式磨机中将指定的适当量的BaCO3、SrCO3、Co3O4、Fe2O3和RuO2混合以形成混合物来制备Ru-Co2Z铁氧体。在空气中将该混合物煅烧至1200℃的煅烧温度持续4小时的保温时间以形成铁氧体。将铁氧体破碎并通过40目筛网进行筛分。将粗颗粒在湿式行星式磨机中研磨以形成按体积计的中值D50颗粒尺寸为0.5微米至10微米的颗粒状物。通过将该颗粒状物与聚(乙烯醇)混合来形成粒状混合物，基于粒状混合物的总量，聚(乙烯醇)为0.5重量百分比至5重量百分比。然后将该粒状混合物在1公吨/平方厘米的压力下压缩以形成外径为7毫米、内径为3毫米且厚度为3毫米至3.5毫米的环状颗粒体。将该环状颗粒体在通过使氧气以0.5升/分钟的速率流动的氧气气氛中使用3℃/分钟的升温速率和-3℃/分钟的冷却速率在1200℃、1220℃或1240℃的烧结温度下烧结10小时。
Figure BDA0003487202400000081
制备了多种铁氧体组合物，其中烧结温度和y值示于表2和表3中。磁导率(实线)和磁损耗角正切(虚线)作为频率的函数示于图1、图2和图3中，以及不同组合物的具体值示于表2中。应注意，在图3中，带星号的样品为重复样品。数个样品的介电常数(实线)和介电损耗角正切(虚线)作为频率的函数示于图4中，以及不同组合物的具体值示于表3中。
Figure BDA0003487202400000082
结果显示，增加钌的量实现从1吉赫至2吉赫磁损耗角正切显著减小，同时仍然保持大于或等于3的磁导率μ'。结果还显示，仅通过升高烧结温度，可以提高磁导率，同时还减小磁损耗角正切。
Figure BDA0003487202400000091
表3和图4示出了升高烧结温度可以实现介电常数增大，同时保持低的介电正切值。
实施例9至10：使用1步烧结法制备Ru-Co2Z铁氧体样品
改变通式(Ba1.5Sr1.5)Co2(CoRu)yFe22.4-2yO41中钌的量y以形成如表1所示的铁氧体组合物来形成Ru-Co2Z铁氧体样品。通过将适当量的BaCO3、SrCO3、Co3O4、RuO2和Fe2O3在湿式行星式磨机中混合以形成混合物来制备Ru-Co2Z铁氧体。通过将颗粒状物与聚(乙烯醇)混合来形成混合物，基于混合物的总量，聚(乙烯醇)为0.5重量百分比至5重量百分比。然后将该混合物在1公吨/平方厘米的压力下压缩以形成外径为7毫米、内径为3毫米且厚度为3毫米至3.5毫米的环装颗粒体。将该环状颗粒体在通过使氧气以0.5升/分钟的速率流动的氧气气氛中使用3℃/分钟的升温速率和-3℃/分钟的冷却速率在1220℃或1240℃的烧结温度下烧结10小时。
制备了多种铁氧体组合物，其中烧结温度和y值示于表4和表5中。磁导率(实线)和磁损耗角正切(虚线)作为频率的函数示于图5中，以及不同组合物的具体值示于表4中。数个样品的介电常数(实线)和介电损耗角正切(虚线)作为频率的函数示于图6中，以及不同组合物的具体值示于表5中。
Figure BDA0003487202400000101
Figure BDA0003487202400000102
结果显示，使用1步烧结法保持了良好的磁导率和磁损耗角正切值。
实施例11至14：包含铁氧体组合物的复合材料的制备
改变通式(Ba1.5Sr1.5)Co2(CoRu)yFe22.4-2yO41中钌的量y以形成如表1所示的铁氧体组合物来形成Ru-Co2Z铁氧体样品。通过在湿式行星式磨机中将指定的适当量的BaCO3、SrCO3、Co3O4、Fe2O3和RuO2混合以形成混合物来制备Ru-Co2Z铁氧体。在空气中将该混合物煅烧至1200℃的煅烧温度持续4小时的保温时间以形成铁氧体。将该铁氧体破碎并通过100目筛网进行筛分。将粗颗粒在空气中在1240℃下烧结10小时，在湿式行星式磨机中研磨以形成颗粒状物，并在以0.4升/分钟的速率流动的氧气中在900℃下退火2小时以形成铁氧体粉末。该铁氧体粉末的中值D50颗粒尺寸为3微米至6微米。将该铁氧体粉末与石蜡混合以形成包含40体积百分比的铁氧体粉末和60体积百分比的石蜡的复合材料。将该复合材料成型为外径为7毫米、内径为3毫米且壁厚为2.5毫米的环状物，并测量磁特性和介电特性。
磁特性示于表6中，以及介电特性示于表7中。
Figure BDA0003487202400000111
Figure BDA0003487202400000112
结果显示了包含所述铁氧体颗粒的复合材料的良好的磁导率和磁损耗角正切值。
下面阐述的是本公开内容的非限制性方面。
方面1：一种铁氧体组合物，包含具有式(Ba3-xMx)Co2(M'Ru)yFe24-2y-zO41的Ru-Co2Z铁氧体，其中M为Sr、Pb或Ca中的至少一者；M'为Co、Zn、Mg或Cu中的至少一者；x为1至3；y为大于0至为2；以及z为-4至4。
方面2：根据方面1所述的铁氧体组合物，其中y为0.001至2。
方面3：根据前述方面中任一者或更多者所述的铁氧体组合物，其中M'为至少Co。
方面4：根据前述方面中任一者或更多者所述的铁氧体组合物，其中Ru与M'的比率为0.01至3。
方面5：根据前述方面中任一者或更多者所述的铁氧体组合物，还包含基于所述铁氧体组合物的总重量的量为0.2重量百分比至5.0重量百分比的Bi2O3。
方面6：根据前述方面中任一者或更多者所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有大于或等于3.5的磁导率。
方面7：根据前述方面中任一者或更多者所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有6至15的介电常数。
方面8：根据前述方面中任一者或更多者所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有小于或等于0.12或者小于或等于0.08的磁损耗角正切tanδμ。
方面9：根据前述方面中任一者或更多者所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有小于或等于0.01或者小于或等于0.008的介电损耗角正切tanδε。
方面10：一种制品，包含根据前述方面中任一者或更多者所述的铁氧体组合物。
方面11：根据方面10所述的制品，其中所述制品为天线、滤波器、感应器、环行器或移相器。
方面12：根据方面10至11中任一者或更多者所述的制品，其中所述制品为微波天线。
方面13：根据方面10至12中任一者或更多者所述的制品，其中所述制品为能够在大于或等于0.1吉赫、或者大于或等于0.3吉赫、或者0.1吉赫至4吉赫的频率下工作的天线。
方面14：一种制造铁氧体组合物，例如根据前述方面中任一者或更多者所述的铁氧体组合物的方法，包括：将包含Fe、Ba、Co和Ru的铁氧体前体化合物混合；以及在氧气气氛中对所述铁氧体前体化合物进行烧结以形成Ru-Co2Z铁氧体。
方面15：根据方面14所述的方法，其中所述铁氧体前体化合物包含BaCO3、MCO3、Co3O4、RuO2和Fe2O3，其中M为Sr、Pb或Ca中的至少一者。
方面16：根据方面15所述的方法，其中所述铁氧体前体化合物包含5重量百分比至20重量百分比的BaCO3、5重量百分比至20重量百分比的MCO3、2重量百分比至15重量百分比的Co3O4、0.1重量百分比至10重量百分比的RuO2、和50重量百分比至80重量百分比的Fe2O3；上述含量全部均基于混合物的总重量。
方面17：根据方面14至16中任一者或更多者所述的方法，其中所述烧结在1000℃至1300℃或1200℃至1250℃的烧结温度下进行1小时至20小时或5小时至12小时的烧结时间。
方面18：根据方面14至16中任一者或更多者所述的方法，还包括在所述烧结之前在空气中对所述铁氧体前体化合物进行煅烧。
方面19：根据方面14至18中任一者或更多者所述的方法，还包括在所述烧结之前将所述铁氧体前体化合物与粘结剂混合。
方面20：根据方面14至19中任一者或更多者所述的方法，还包括在所述烧结之前使所述铁氧体前体化合物成形。
方面21：一种复合材料，包含根据前述方面中任一者或更多者所述的铁氧体组合物，
组合物、方法和制品可以替代地包括本文所公开的任何合适的材料、步骤或组分，由本文所公开的任何合适的材料、步骤或组分组成，或者基本上由本文所公开的任何合适的材料、步骤或组分组成。组合物、方法和制品可以另外地或替代地被表达为不含或基本上不含对于实现所述组合物、方法和制品的功能或目的不是另外必需的任何材料(或物质)、步骤或组分。
如本文所用，除非上下文另外明确地指出，否则“一个”、“一种”、“所述”和“至少一者”不表示数量的限制，并且旨在涵盖单数和复数二者。例如，除非上下文另外明确地指出，否则“要素”具有与“至少一个要素”相同的含义。术语“组合”包括共混物、混合物、合金、反应产物等。此外，“中的至少一者”意指列表独立地包括各个要素，以及列表中的两个或更多个要素的组合，以及列表中的至少一个要素与未列举的类似要素的组合。
除非通过上下文另外明确地指出，否则术语“或”意指“和/或”。在整个说明书中提及“一个方面”、“另一个方面”、“一些方面”等意指结合所述方面描述的特定要素(例如，特征、结构、步骤或特性)包括在本文所述的至少一个方面中，并且可以存在或可以不存在于其他方面中。此外，应理解，所描述的要素可以在各个方面中以任何适当的方式组合。
除非本文相反地规定，否则所有测试标准均为截至本申请的申请日(或者，如果要求优先权的话，则为其中出现所述测试标准的最早优先权申请的申请日)生效的最新标准。
涉及相同组分或特性的所有范围的端点包括端点在内，可独立地组合，并且包括所有中间点和范围。例如，“高至25体积％或5体积％至20体积％”的范围包括端点和“5体积％至25体积％”范围的所有中间值，例如10体积％至23体积％等。
除非另外限定，否则本文所使用的技术和科学术语均具有与本公开内容所属领域的技术人员通常理解的相同的含义。
所有引用的专利、专利申请和其他参考文献均通过引用整体并入本文。然而，如果本申请中的术语与并入的参考文献中的术语矛盾或冲突，则来自本申请的术语优先于来自并入的参考文献的冲突术语。
虽然已经描述了特定实施方案，但是申请人或本领域其他技术人员可以想到目前没有预见或可能目前无法预见的替代方案、修改方案、变化方案、改进方案和实质等同方案。因此，所提交的和可以被修改的所附权利要求旨在涵盖所有这样的替代方案、修改变化方案、改进方案和实质等同方案。

Claims (26)

1.一种铁氧体组合物，包含具有下式的Ru-Co2Z铁氧体：
(Ba3-xMx)Co2(M′Ru)yFe24-2y-zO41
其中M为Sr、Pb或Ca中的至少一者；M'为Co、Zn、Mg或Cu中的至少一者；x为1至3；y为大于0至为2；以及z为-4至4。
2.根据权利要求1所述的铁氧体组合物，其中y为0.001至2。
3.根据权利要求1或2中任一项所述的铁氧体组合物，其中M'为至少Co。
4.根据权利要求1或2中任一项所述的铁氧体组合物，还包含基于所述铁氧体组合物的总重量的量为0.2重量百分比至5.0重量百分比的Bi2O3。
5.根据权利要求1或2中任一项所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有大于或等于3.5的磁导率。
6.根据权利要求1或2中任一项所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有6至15的介电常数。
7.根据权利要求1或2中任一项所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有小于或等于0.12的磁损耗角正切tanδμ。
8.根据权利要求1或2中任一项所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有小于或等于0.08的磁损耗角正切tanδμ。
9.根据权利要求1或2中任一项所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有小于或等于0.01的介电损耗角正切tanδε。
10.根据权利要求1或2中任一项所述的铁氧体组合物，其中所述铁氧体组合物在固体陶瓷的形式下在1吉赫至2吉赫的频率下具有小于或等于0.008的介电损耗角正切tanδε。
11.一种复合材料，包含聚合物和根据权利要求1至10中任一项所述的铁氧体组合物。
12.一种制品，包含根据权利要求1至10中任一项所述的铁氧体组合物或者根据权利要求11所述的复合材料。
13.根据权利要求12所述的制品，其中所述制品为天线、滤波器、感应器、环行器或移相器。
14.根据权利要求12至13中任一项所述的制品，其中所述制品为微波天线。
15.根据权利要求12至13中任一项所述的制品，其中所述制品为能够在大于或等于0.1吉赫的频率下工作的天线。
16.根据权利要求12至13中任一项所述的制品，其中所述制品为能够在大于或等于0.3吉赫的频率下工作的天线。
17.根据权利要求12至13中任一项所述的制品，其中所述制品为能够在0.1吉赫至4吉赫的频率下工作的天线。
18.一种制造根据权利要求1至10中任一项所述的铁氧体组合物的方法，包括：
将包含Fe、Ba、Co、Ru、M和M'的铁氧体前体化合物混合；以及
在氧气气氛中对所述铁氧体前体化合物进行烧结以形成Ru-Co2Z铁氧体。
19.根据权利要求18所述的方法，其中所述铁氧体前体化合物包含BaCO3、MCO3、Co3O4、RuO2和Fe2O3，其中M为Sr、Pb或Ca中的至少一者。
20.根据权利要求19所述的方法，其中所述铁氧体前体化合物包含5重量百分比至20重量百分比的BaCO3、5重量百分比至20重量百分比的MCO3、2重量百分比至15重量百分比的Co3O4、0.1重量百分比至10重量百分比的RuO2、和50重量百分比至80重量百分比的Fe2O3；上述含量全部均基于混合物的总重量。
21.根据权利要求18至20中任一项所述的方法，其中所述烧结在1000℃至1300℃的烧结温度下进行1小时至20小时的烧结时间。
22.根据权利要求21所述的方法，其中所述烧结时间为5小时至12小时。
23.根据权利要求21所述的方法，其中所述烧结温度为1200℃至1250℃。
24.根据权利要求18至20中任一项所述的方法，还包括在所述烧结之前在空气中对所述铁氧体前体化合物进行煅烧。
25.根据权利要求18至20中任一项所述的方法，还包括在所述烧结之前将所述铁氧体前体化合物与粘结剂混合。
26.根据权利要求18至20中任一项所述的方法，还包括在所述烧结之前使所述铁氧体前体化合物成形。
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