在5G信息技术迅速发展的当代，电子元件随着表面贴装技术（SMT）的普及，不断向片式化、小型化、多功能化等方向发展。本文以满足多层片式LC滤波器实际应用的角度出发，将(Zr0.8Sn0.2)TiO4（ZST）微波介质陶瓷和NiZn（NZ）铁氧体叠层共烧，研究两种材料的共烧兼容特性。从介电材料(Zr0.8Sn0.2)TiO4的低温烧结入手，通过湿化学法合成高纯粉体来作为叠层复合体的初始原料；利用衍射数据对ZST材料进行了结构精修，并采用第一性原理计算得到ZST陶瓷的能级结构、电子态密度及弹性常数等结构特征参数；采用叠压工艺制备了ZST-NZ叠层复合体，通过改变成型方式，烧结温度以及加入中间层等工艺技术，来研究叠层复合体的界面结合，界面扩散以及介电性能。主要内容和结论如下：
（1）采用水热-熔盐法在1000℃制备了纯相的ZST纳米粉体。与水热-固相法相比，水热-熔盐法可以在更低温度下制备出晶体生长更完整的粉体，其形貌呈规则的纳米棒状形貌，棒状晶体直径约为50-60 nm。而且合成的ZST纳米粉体具有一定的光催化特性和紫外屏蔽特性，为拓宽ZST粉体的应用领域提供了实验基础。
（2）对ZST晶体进行精修以及第一性原理计算，结果表明：(Zr0.8Sn0.2)TiO4是以ZrTiO4为基本结构的正交晶系化合物，通过计算所得晶格常数值与结构精修所得相应数据符合良好，三种离子占同一位置的概率大小顺序为Sn4+ >Zr4+ >Ti4+。通过第一性原理计算得到ZST带隙为2.61 eV，态密度主要的峰由O原子的p轨道、s轨道和Ti、Zr、Sn原子的p轨道、s轨道贡献，Ti-O、Zr-O、Sn-O的价键类型主要为离子键。
（3）以水热-熔盐法合成的ZST粉体作为初始原料，采用热压成型工艺，在1250 ℃制备的ZST陶瓷相对密度为ρR=99.3%，介电性能：ɛr=40.5，tanδ=1.32×10-3，采用干压成型工艺，在1250℃烧结的ZST陶瓷性能为：ɛr=37.2，tanδ=9.63×10-4，ρR=98.8%。
（4）采用叠压工艺制备出了界面结合较为紧密的ZST-NZ叠层复合体，但其内部，特别是NZ一侧存在很多裂纹，导致介电损耗增加。由于两种材料之间收缩率不匹配，导致ZST-NZ叠层复合体翘曲；ZST-NZ叠层复合体界面处形成扩散层，1200℃下扩散层厚度为13-15 μm左右，随温度的升高，扩散层的厚度不断增加，在1275℃时扩散层厚度达到25 μm左右。而且在扩散层中由于ZST以及NZ铁氧体的分解产生新相TiO2和Fe3O4。
（5）采用半无限扩散偶模型，建立了ZST/NZ互扩散偶中离子浓度分布函数并对离子扩散系数进行了计算。在ZST/NZ扩散偶中扩散系数大小顺序为：D(Fe3+) > D(Zn2+) > D(Sn4+) > D(Zr4+)；在1275 ℃时扩散激活能大小顺序为：Qd(Zr4+) > Qd(Sn4+) > Qd(Zn2+) > Qd(Fe3+)。
（6）将ZST和NZ按重量比1:1混合作为作为中间层材料，简称为Z1N1，采用叠压工艺制备出了界面结合紧密，无开裂的ZST-Z1N1-NZ叠层复合体。相比于ZST-NZ叠层复合体，缺陷明显减少，最佳性能试样的烧结温度从1275℃-1250℃，介电常数为34.3，介电损耗降低一个数量级；中间层的加入，在ZST和NZ材料之间起到了梯度层的作用，减小了离子层间浓度差，减缓了界面处离子的扩散行为；然而在ZST一侧加入掺杂剂，在一定程度上可以降低陶瓷的烧结温度，但也不可避免的导致内部缺陷增多，导致介电性能下降。
 

~In the contemporary era of rapid development of 5G information technology, electronic components continue to develop in the direction of chip, miniaturization and multi-functionalization with the popularity of surface mount technology (SMT). In this paper, (Zr0.8Sn0.2)TiO4 (ZST) microwave dielectric ceramics and NiZn (NZ) ferrite were co-fired in a stack to meet the practical application of multilayer chip LC filters, and the co-fired compatibility characteristics of the two materials were studied. Starting from the low-temperature sintering of the dielectric material (Zr0.8Sn0.2)TiO4, the high-purity powder was synthesized by wet chemical method as the initial raw material for the stacked composite. Structural refinement of the ZST material was carried out using diffraction data, and structural characteristic parameters such as energy level structure, electronic density of states and elastic constants of the ZST ceramics were calculated using the first-nature principle. The ZST-NZ stacked composite was prepared by the lamination process. and the interfacial bonding, interfacial diffusion and dielectric properties of the laminated composite were investigated by changing the molding method, sintering temperature and adding intermediate layers. The main contents and conclusions are as follows:
(1) Pure-phase ZST nanocrystals were prepared by the hydrothermal-molten salt method at 1000 °C. Compared with the hydrothermal-solid phase method, the hydrothermal-molten salt method produced more complete crystal growth, lower synthesis temperature, regular nanorod-like morphology, and rod-like crystal diameter of about 50-60 nm. Moreover, the synthesized ZST nanopowders have certain photocatalytic and UV-shielding properties, which provide an experimental basis for broadening the application of ZST nanopowders.
(2) Refinement of ZST crystals and first-principles calculations showed that (Zr0.8Sn0.2)TiO4 is an orthogonal crystal compound with ZrTiO4 as the basic structure, and the calculated lattice constant values are in good agreement with the corresponding data obtained from structural refinement, and the probability of the three ions occupying the same position is in the order of Sn4+ > Zr4+ > Ti4+. The results of the first-nature principle calculations showed that the ZST band gap is 2.61 eV, the peaks of the density of states are mainly contributed by the p-orbitals and s-orbitals of O atoms and the p-orbitals and s-orbitals of Ti, Zr, and Sn atoms, and the valence bond types of Ti-O, Zr-O, and Sn-O are mainly ionic bonds.
(3) Using ZST powder synthesized by hydrothermal-molten salt method as the initial raw material, the relative density of ZST ceramics prepared by hot press molding process at 1250 oC is ρR=99.3%, dielectric properties: ɛr=40.5, tanδ=1.32×10-3, and the properties of ZST ceramics sintered by dry press molding process at 1250 oC are: ɛr=37.2, tanδ= 9.63×10-4, and ρR=98.8%.
(4) The ZST-NZ laminated composite with tighter interfacial bonding was prepared by the lamination process, but there were many cracks inside, especially on the NZ side, leading to increased dielectric losses. Due to the mismatch of shrinkage between the two materials, the ZST-NZ laminated composite warps. A diffusion layer is formed at the interface of the ZST-NZ laminated composite, and the thickness of the diffusion layer is about 13-15 μm at 1200 oC, which increases continuously with the increase of temperature. The thickness of diffusion layer is about 25 μm at 1275 oC. Moreover, the new phases TiO2 and Fe3O4 are generated in the diffusion layer due to the decomposition of ZST and NZ ferrite.
(5) Using a semi-infinite diffusion couple model, the ion concentration distribution function in the ZST/NZ mutual diffusion couple was established and the ion diffusion coefficients were calculated. The order of diffusion coefficients in the ZST/NZ diffusion couple is: D(Fe3+) > D(Zn2+) > D(Sn4+) > D(Zr4+). The order of diffusion activation energy at 1275 oC is: Qd(Zr4+) > Qd(Sn4+) > Qd(Zn2+) > Qd(Fe3+).
(6) The ZST-Z1N1-NZ laminated composite with tightly bound interfaces and no cracking was prepared by the lamination process by mixing ZST and NZ in the weight ratio of 1:1 as the intermediate layer material, referred to as Z1N1. Compared with the ZST-NZ stacked composite, the defects were significantly reduced, and the best performance specimens were sintered from 1275 °C to 1250 °C with a dielectric constant of 34.3 and dielectric loss reduced by one order of magnitude; the addition of the intermediate layer played the role of a gradient layer between the ZST and NZ materials, reducing the ion interlayer concentration difference and slowing down the diffusion behavior of ions at the interface. The addition of the ZST side dopant, to a certain extent, reduces the sintering temperature of the ceramic, but also inevitably leads to an increase in internal defects, resulting in a decrease in dielectric properties.
 

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