[go: up one dir, main page]

CN113860871B - 一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法 - Google Patents

一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法 Download PDF

Info

Publication number
CN113860871B
CN113860871B CN202111292700.9A CN202111292700A CN113860871B CN 113860871 B CN113860871 B CN 113860871B CN 202111292700 A CN202111292700 A CN 202111292700A CN 113860871 B CN113860871 B CN 113860871B
Authority
CN
China
Prior art keywords
nio
temperature
ceramic material
low
dielectric ceramic
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Active
Application number
CN202111292700.9A
Other languages
English (en)
Other versions
CN113860871A (zh
Inventor
邢孟江
曲明山
杨鸿宇
孙成礼
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Huzhou Porcelain Core Electronic Technology Co ltd
Original Assignee
University of Electronic Science and Technology of China
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by University of Electronic Science and Technology of China filed Critical University of Electronic Science and Technology of China
Priority to CN202111292700.9A priority Critical patent/CN113860871B/zh
Publication of CN113860871A publication Critical patent/CN113860871A/zh
Priority to US17/979,846 priority patent/US11873248B2/en
Application granted granted Critical
Publication of CN113860871B publication Critical patent/CN113860871B/zh
Active legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Images

Classifications

    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/495—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on vanadium, niobium, tantalum, molybdenum or tungsten oxides or solid solutions thereof with other oxides, e.g. vanadates, niobates, tantalates, molybdates or tungstates
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G53/00—Compounds of nickel
    • C01G53/40—Complex oxides containing nickel and at least one other metal element
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
    • C04B35/62605—Treating the starting powders individually or as mixtures
    • C04B35/6261—Milling
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
    • C04B35/62605—Treating the starting powders individually or as mixtures
    • C04B35/6261—Milling
    • C04B35/6262—Milling of calcined, sintered clinker or ceramics
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/64—Burning or sintering processes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B3/00—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties
    • H01B3/02—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of inorganic substances
    • H01B3/12—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of inorganic substances ceramics
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
    • C04B2235/3239—Vanadium oxides, vanadates or oxide forming salts thereof, e.g. magnesium vanadate
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
    • C04B2235/3251—Niobium oxides, niobates, tantalum oxides, tantalates, or oxide-forming salts thereof
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/327—Iron group oxides, their mixed metal oxides, or oxide-forming salts thereof
    • C04B2235/3279—Nickel oxides, nickalates, or oxide-forming salts thereof
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3281—Copper oxides, cuprates or oxide-forming salts thereof, e.g. CuO or Cu2O
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3284—Zinc oxides, zincates, cadmium oxides, cadmiates, mercury oxides, mercurates or oxide forming salts thereof
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3293—Tin oxides, stannates or oxide forming salts thereof, e.g. indium tin oxide [ITO]
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/34—Non-metal oxides, non-metal mixed oxides, or salts thereof that form the non-metal oxides upon heating, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3409—Boron oxide, borates, boric acids, or oxide forming salts thereof, e.g. borax
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/60—Aspects relating to the preparation, properties or mechanical treatment of green bodies or pre-forms
    • C04B2235/604—Pressing at temperatures other than sintering temperatures
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/65—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
    • C04B2235/656—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes characterised by specific heating conditions during heat treatment
    • C04B2235/6562—Heating rate
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/74—Physical characteristics
    • C04B2235/78—Grain sizes and shapes, product microstructures, e.g. acicular grains, equiaxed grains, platelet-structures
    • C04B2235/785—Submicron sized grains, i.e. from 0,1 to 1 micron
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/96—Properties of ceramic products, e.g. mechanical properties such as strength, toughness, wear resistance
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
    • C04B35/62605—Treating the starting powders individually or as mixtures
    • C04B35/62645—Thermal treatment of powders or mixtures thereof other than sintering
    • C04B35/62655—Drying, e.g. freeze-drying, spray-drying, microwave or supercritical drying
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
    • C04B35/62605—Treating the starting powders individually or as mixtures
    • C04B35/62645—Thermal treatment of powders or mixtures thereof other than sintering
    • C04B35/62675—Thermal treatment of powders or mixtures thereof other than sintering characterised by the treatment temperature
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
    • C04B35/63—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B using additives specially adapted for forming the products, e.g.. binder binders
    • C04B35/638—Removal thereof

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Organic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Inorganic Insulating Materials (AREA)
  • Compositions Of Oxide Ceramics (AREA)

Abstract

本发明属于电子陶瓷及其制造领域，具体为一种低温烧结改性NiO‑Ta2O5基微波介质陶瓷材料及其制备方法。是以离子掺杂改性为指导依据，不仅考虑到以相近半径的离子进行取代，如Zn2+取代Ni2+离子，V5+取代Ta5+离子；同时选择的掺杂氧化物仍具有低熔点的性质。因此可以实现改善NiO‑Ta2O5基陶瓷材料微波介电性能的同时仍能降低适宜的烧结温度。在本发明中，通过调节各原料的摩尔含量，直接一次合成了具有低温烧结、温度稳定且微波介电性能优异的NiO‑Ta2O5基陶瓷材料，可广泛应用于LTCC技术领域。

Description

一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备 方法
技术领域
本发明属于电子陶瓷及其制造领域，涉及一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法。
背景技术
随着移动通讯不断向高频化方向发展，电子元器件诸如介质滤波器、介质谐振器天线、介质波导等的重要性凸显，而微波介质陶瓷能够在300MHz～300GHz范围内发挥功能性，是目前被广泛用于制备上述电子元器件的关键基础性材料。
传统的微波设备重量大且昂贵，通讯行业发展至今，要求电路系统所占空间要尽可能小。作为一种新型的三维集成封装互联技术，低温共烧陶瓷(LTCC)技术因其满足高频应用，为制备内嵌电极的陶瓷模块或整体电路提供了可靠的解决方案，因此开发应用于LTCC技术的陶瓷体系成为该领域研究的重点。
具有四方Tri-rutile晶体结构的NiO-Ta2O5陶瓷材料在1400℃下的微波介电性能为：εr＝ 25，Q×f＝31200GHz，τf＝26ppm/℃，但由于过高的烧结温度导致无法与LTCC技术中的 Ag或Cu电极共烧(与Ag电极共烧需不超过950℃；与Cu电极共烧需不超过1000℃且在还原气氛下进行)，且谐振频率温度系数τf值也较大(τf值介于±10ppm/℃代表温度稳定性优异)。截至目前也并未发现有针对NiO-Ta2O5陶瓷的低温烧结探索。因此，降低NiO-Ta2O5基陶瓷的烧结温度并保持微波介电性能是亟需关注的重点。
发明内容
针对上述存在的问题或不足，为解决现有NiO-Ta2O5陶瓷因烧结温度过高导致无法与 LTCC技术中的Ag或Cu电极共烧的问题，本发明提供了一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法，在保持优异的微波介电性能的同时实现了低温烧结，其温度稳定，可广泛应用于LTCC技术领域。
本发明提供的一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料，其化学通式为：
(1.587y-0.198xy)ZnO-(2.597y-0.324xy)CuO-(1-x)NiO-(1.855y-0.231xy)B2O3-3xSnO2-(1-x)Ta2 O5-(0.284y-0.035xy)V2O5；其中0.1≤x≤0.2；0.03≤y≤0.09；经由固相法制备获得；晶体类型为 NiTa2O6结构；
该微波介质陶瓷材料的烧结温度为875～950℃，850～900℃大气气氛中预烧；介电常数为 17～21，品质因数Q×f值为14000～23000GHz，谐振频率温度系数为5～10ppm/℃。
作为优选，当x＝0.15且y＝0.06时，在925℃烧结温度下材料的介电常数为20.2，品质因数Q×f值为22417GHz，谐振频率温度系数为8.7ppm/℃，可广泛用于LTCC技术领域。
上述低温烧结改性NiO-Ta2O5基微波介质陶瓷材料的制备方法，包括以下步骤：
步骤1：将ZnO、CuO、NiO、B2O3、SnO2、Ta2O5与V2O5粉料按化学通式 (1.587y-0.198xy)ZnO-(2.597y-0.324xy)CuO-(1-x)NiO-(1.855y-0.231xy)B2O3-3xSnO2-(1-x)Ta2O5-(0 .284y-0.035xy)V2O5；(x＝0.1～0.2；y＝0.03～0.09)进行配料；
步骤2：将步骤1配好的粉体装入球磨罐，以氧化锆球和去离子水，按照粉料：氧化锆球：去离子水质的量比为1:5～7:3～5进行球磨，行星球磨6～8小时，取出后在80～120℃烘箱中烘干，以40～60目筛网过筛，后在850～900℃大气气氛中预烧3～5小时；
步骤3：将步骤2预烧后的粉体，再次按照粉体：锆球：去离子水质量比为1:4～6:1～3进行球磨，行星球磨混合3～6小时，取出烘干后，向得到的粉体中添加聚乙烯醇溶液进行剂造粒；
步骤4：将步骤3制得陶瓷生料压制成型，在600～650℃排胶后在875～950℃大气气氛中烧结4～6小时后，即可制得低温烧结的改性NiO-Ta2O5基微波介质陶瓷材料。
本发明不同于现有领域报道技术：也即通过向预烧后的NiO-Ta2O5材料中添加CuO、V2O5、B2O3等氧化物作为烧结助剂，在液相作用下实现低温烧结成瓷的目的，而是以离子掺杂改性为指导依据，不仅考虑到以相近半径的离子进行取代以实现固溶体陶瓷的制备，如Zn2+取代Ni2+离子，V5+取代Ta5+离子，(Ni1/3Ta2/3)4+复合离子被Sn4+取代，不同离子之间的协同作用反而使综合微波介电性能得到提升；同时选择的掺杂氧化物仍具有低熔点的性质，因此可以实现改善较低温度下合成NiO-Ta2O5材料主晶相的目的，并使该陶瓷材料保持优异微波介电性能的同时仍能降低烧结温度。
本发明提供一种可低温烧结的改性NiO-Ta2O5基陶瓷材料，其化学通式为(1.587y-0.198xy)ZnO-(2.597y-0.324xy)CuO-(1-x)NiO-(1.855y-0.231xy)B2O3-3xSnO2-(1-x)Ta2O5-(0 .284y-0.035xy)V2O5，通过调节各原料的摩尔含量，直接一次合成了具有低温烧结、温度稳定且微波介电性能优异的NiO-Ta2O5基陶瓷材料，可广泛应用于LTCC技术领域。
附图说明
图1对应实施例3的XRD衍射图谱；
图2对应实施例3的SEM形貌图。
具体实施方式
下面结合附图和实施例对本发明做进一步的详细说明。
步骤1、将ZnO、CuO、NiO、B2O3、SnO2、Ta2O5与V2O5粉料按化学通式(1.587y-0.198xy)ZnO-(2.597y-0.324xy)CuO-(1-x)NiO-(1.855y-0.231xy)B2O3-3xSnO2-(1-x)Ta2O5-(0.284y-0.035xy)V2O5(x＝0.15；y＝0.06)，采用摩尔比进行配料；
步骤2、将步骤1称量好的粉料混合并置于球磨罐中，在氧化锆球以及去离子水中按照粉料：氧化锆球：去离子水质量比1:6:3行星球磨6小时，然后在100℃的烘箱中烘干，以60 目筛网过筛，随后在900℃大气气氛中预烧3小时；
步骤3、将预烧后的粉料放入球磨罐中进行二次球磨，以粉体：氧化锆球：去离子水质量比1:6:2进行4小时的行星球磨，再取出烘干后向得到的粉料加入聚乙烯醇溶液进行造粒；
步骤4、将造粒好的粉体放入
Figure BDA0003335194340000033
的模具中在20MPa压力下干压成为圆柱体，随后将圆柱块体在650℃下保温2小时以除去粘结剂，然后升至875℃～950℃下保温4小时，最终制得低温烧结条件下的改性NiO-Ta2O5基微波介质陶瓷材料，其化学式的摩尔配比分别为：ZnO-CuO-NiO-B2O3-SnO2-Ta2O5-V2O5(3.7:6.1:33.7:4.3:17.8:33.7:0.7mol％)。
为更好的阐述本发明的效果，按照上述步骤制作了4份实施例样品。图1为实施例3的 XRD衍射图谱，经过检索陶瓷的物相组成与NiTa2O6的标准卡片JCPDS card No.32-0702对应，此时体系中并未发现第二相衍射峰的存在，则说明该类型陶瓷属于NiTa2O6结构的固溶体。
图2为实施例3的SEM形貌图，可以看出陶瓷试样的晶粒生长充分，晶界清晰可见，说明其低温烧结特性良好，但此时微观气孔仍存在。
各实施例样的成分和微波介电性能如下：
Figure BDA0003335194340000031
表1为各实施例样品组的成分
Figure BDA0003335194340000032
表2为各实施例样品的微波介电性能
从表1、表2展示的数据可以看出在x＝0.15且y＝0.06时，当烧结温度介于875～925℃范围内，改性NiO-Ta2O5基陶瓷材料的介电常数与Q×f值呈现出先增加后降低的趋势，并在925℃时取得最佳值：εr＝20.2，tanδ＝4.1×10-4，Q×f＝22417GHz，τf＝8.7ppm/℃，与现有文献报道相比烧结温度得到大幅度降低的同时保持了优异的温度稳定性以及微波介电特性，可广泛应用于LTCC技术领域。

Claims (3)

1.一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料，其特征在于，所述低温烧结改性NiO-Ta2O5基微波介质陶瓷材料化学通式为：
(1.587y-0.198xy)ZnO-(2.597y-0.324xy)CuO-(1-x)NiO-(1.855y-0.231xy)B2O3-3xSnO2-(1-x)Ta2O5-(0.284y-0.035xy)V2O5；其中0.1≤x≤0.2；0.03≤y≤0.09；经由固相法制备获得；晶体类型为NiTa2O6结构；
该微波介质陶瓷材料的烧结温度为875～950℃，850～900℃大气气氛中预烧；介电常数为17～21，品质因数Q×f值为14000～23000GHz，谐振频率温度系数为5～10ppm/℃。
2.根据权利要求1所述的一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料，其特征在于：当x＝0.15且y＝0.06时，在925℃烧结温度下材料的介电常数为20.2，品质因数Q×f值为22417GHz，谐振频率温度系数为8.7ppm/℃。
3.一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料的制备方法，其特征在于：包括以下步骤：
步骤1：将ZnO、CuO、NiO、B2O3、SnO2、Ta2O5与V2O5粉料按化学通式(1.587y-0.198xy)ZnO-(2.597y-0.324xy)CuO-(1-x)NiO-(1.855y-0.231xy)B2O3-3xSnO2-(1-x)Ta2O5-(0.284y-0.035xy)V2O5进行配料；其中0.1≤x≤0.2；0.03≤y≤0.09；
步骤2：将步骤1配好的粉体装入球磨罐，以氧化锆球和去离子水，按照粉料：氧化锆球：去离子水质的量比为1:5～7:3～5进行球磨，行星球磨6～8小时，取出后在80～120℃烘箱中烘干，以40～60目筛网过筛，后在850～900℃大气气氛中预烧3～5小时；
步骤3：将步骤2预烧后的粉体，再次按照粉体：锆球：去离子水质量比为1:4～6:1～3进行球磨，行星球磨混合3～6小时，取出烘干后，向得到的粉体中添加聚乙烯醇溶液进行剂造粒；
步骤4：将步骤3制得陶瓷生料压制成型，在600～650℃排胶后在875～950℃大气气氛中烧结4～6小时后，即可制得低温烧结的改性NiO-Ta2O5基微波介质陶瓷材料。
CN202111292700.9A 2021-11-03 2021-11-03 一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法 Active CN113860871B (zh)

Priority Applications (2)

Application Number Priority Date Filing Date Title
CN202111292700.9A CN113860871B (zh) 2021-11-03 2021-11-03 一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法
US17/979,846 US11873248B2 (en) 2021-11-03 2022-11-03 Modified NiO-Ta2O5-based microwave dielectric ceramic material sintered at low temperature and its preparation method

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202111292700.9A CN113860871B (zh) 2021-11-03 2021-11-03 一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法

Publications (2)

Publication Number Publication Date
CN113860871A CN113860871A (zh) 2021-12-31
CN113860871B true CN113860871B (zh) 2022-12-13

Family

ID=78986796

Family Applications (1)

Application Number Title Priority Date Filing Date
CN202111292700.9A Active CN113860871B (zh) 2021-11-03 2021-11-03 一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法

Country Status (2)

Country Link
US (1) US11873248B2 (zh)
CN (1) CN113860871B (zh)

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115925001B (zh) * 2022-12-22 2024-06-04 浙江大学山东工业技术研究院 Ta2O5/NiO复合空心纳米球材料及其制备方法和应用

Family Cites Families (16)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3920781A (en) * 1971-04-02 1975-11-18 Sprague Electric Co Method of forming a ceramic dielectric body
US4302610A (en) * 1980-05-27 1981-11-24 Allied Corporation Vanadium containing niobates and tantalates
KR100292915B1 (ko) * 1998-07-22 2001-09-22 김병규 유전체 세라믹 조성물
KR100365294B1 (ko) * 2000-04-21 2002-12-18 한국과학기술연구원 저온소결 저손실 고주파유전체 세라믹스 조성물 및 그 제조방법
KR100729998B1 (ko) * 2000-05-30 2007-06-20 쿄세라 코포레이션 유전체 자기, 유전체 자기조성물 및 제조방법과, 이것을사용한 유전체 공진기
KR100401943B1 (ko) * 2000-11-17 2003-10-17 홍국선 유전체 세라믹 조성물 및 이를 이용한 유전체 세라믹의 제조방법
KR100426219B1 (ko) * 2001-05-18 2004-04-06 홍국선 유전체 세라믹 조성물 및 이를 이용한 적층부품의 제조방법
JP5983265B2 (ja) * 2011-12-12 2016-08-31 Tdk株式会社 誘電体磁器組成物
KR102608243B1 (ko) * 2018-07-23 2023-11-29 삼성전자주식회사 세라믹 유전체, 세라믹 전자 부품 및 장치
CN109251029B (zh) * 2018-11-15 2019-07-02 西华大学 一种温度稳定型微波介质陶瓷材料及其制备方法
CN109574663B (zh) * 2018-12-14 2021-03-26 电子科技大学 一种Ni-Ti-Ta基微波介质陶瓷材料及其制备方法
CN109467433B (zh) * 2018-12-14 2021-03-30 电子科技大学 一种Co-Ti-Ta基介质陶瓷材料及其制备方法
KR102724895B1 (ko) * 2019-05-31 2024-11-01 삼성전기주식회사 유전체 자기 조성물 및 이를 포함하는 적층 세라믹 전자부품
CN110596217A (zh) * 2019-09-18 2019-12-20 吉林大学 NiTa2O6为敏感电极的糖尿病诊断用全固态丙酮传感器及其制备方法
US11935698B2 (en) * 2021-01-28 2024-03-19 Kemet Electronics Corporation Dielectric ceramic composition and multi-layered ceramic capacitor comprised thereof
CN113105237B (zh) * 2021-04-30 2023-02-17 昆明理工大学 一种ab2o6型钽酸盐陶瓷及其制备方法

Also Published As

Publication number Publication date
US11873248B2 (en) 2024-01-16
US20230145935A1 (en) 2023-05-11
CN113860871A (zh) 2021-12-31

Similar Documents

Publication Publication Date Title
CN106083033A (zh) 一种微波介质陶瓷材料及其制备方法
CN104003720B (zh) 可低温烧结微波介电陶瓷Li2Zn2W2O9及其制备方法
CN102584234B (zh) 一种环保型低温烧结高介微波介质陶瓷及其制备方法
CN104108929B (zh) 一种低温烧结复合微波介质陶瓷材料及其制备方法
CN107986774B (zh) 低温烧结高介电常数微波介质陶瓷材料及其制备方法
CN104003723B (zh) 可低温烧结的微波介电陶瓷Li3Zn4NbO8及其制备方法
CN107117967B (zh) 一种低温烧结复合微波介质陶瓷材料及其制备方法
JP2000044341A (ja) 誘電体セラミック組成物
CN103496973B (zh) 可低温烧结的微波介电陶瓷BiTiNbO6及其制备方法
CN108455986B (zh) 一种复合微波介质陶瓷材料及其制备方法
US11724966B2 (en) Microwave dielectric ceramic material and preparation method thereof
CN110229004B (zh) 一种低温烧结微波介质陶瓷材料及其制备方法
CN103496979B (zh) 可低温烧结的微波介电陶瓷La3Cu2VO9及其制备方法
CN103496981B (zh) 低温烧结温度稳定型微波介电陶瓷Bi14W2O27及其制备方法
CN113860871B (zh) 一种低温烧结改性NiO-Ta2O5基微波介质陶瓷材料及其制备方法
CN103467095B (zh) 可低温烧结的微波介电陶瓷SrCuV2O7及其制备方法
CN113354412B (zh) 温度稳定型低温烧结微波介质陶瓷材料及其制备方法
CN102603292A (zh) 一种用于可低温烧结微波介电陶瓷的复合氧化物
CN100378031C (zh) 一种低温烧结的微波介质陶瓷及其制备方法
CN106587991B (zh) 一种低温烧结复合微波介质陶瓷材料及其制备方法
CN113788676B (zh) 一种低温共烧改性NiTa2O6基微波介质陶瓷材料及其制备方法
CN112851347A (zh) 一种低温烧结低损耗氟氧化物微波介质陶瓷及其制备方法
CN103539449A (zh) 可低温烧结的微波介电陶瓷BiNbW2O10及其制备方法
CN103496969A (zh) 低温烧结温度稳定型微波介电陶瓷Bi14WO24及其制备方法
CN113292338B (zh) 一种Ba-Co-V基低介低烧微波陶瓷材料及其制备方法

Legal Events

Date Code Title Description
PB01 Publication
PB01 Publication
SE01 Entry into force of request for substantive examination
SE01 Entry into force of request for substantive examination
GR01 Patent grant
GR01 Patent grant
TR01 Transfer of patent right
TR01 Transfer of patent right

Effective date of registration: 20240119

Address after: Building 23, Zhigu Industrial Park, No. 1558 Dongpo Road, Kangshan Street, Huzhou City, Zhejiang Province, China, 313098

Patentee after: Huzhou Porcelain Core Electronic Technology Co.,Ltd.

Address before: 611731, No. 2006, West Avenue, Chengdu hi tech Zone (West District, Sichuan)

Patentee before: University of Electronic Science and Technology of China