Ceramic powder and preparation method thereof, preparation method and application of ceramic material

Abstract

The application discloses a ceramic powder and a preparation method and application thereof, and a preparation method of a ceramic material, relates to the technical field of medical ultrasonic treatment equipment and piezoelectric ceramic material, and the ceramic powder comprises a powder with a chemical formula of (1-2)at.%Me2O3-(1-x-y-z)Pb(Co 1 / 3 Ta 2 / 3 )O3-(x)Pb(Mg 1 / 3 Ta 2 / 3 )O3-(y)Pb(Sc 2 / 3 W 1 / 3 )O3-(z)PbTiO3; wherein Me includes at least one of La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc and Y; x, y and z represent molar fractions, and 0.05<=x<=0.4, 0.05<=y<=0.4 and 0.05<=z<=0.9. The application generates an internal bias field by doping (1-2)at.% rare earth elements Me, pins the ferroelectric domain, reduces the domain activity, and improves the mechanical quality factor (Q m ) to 3000, so that the purpose of realizing non-invasive precise treatment of liver cancer, pancreatic cancer and other deep tumors in a high intensity focused ultrasound (HIFU) system is achieved.

Description

Technical Field

[0001] This invention relates to the technical field of cross-integration of medical ultrasound therapy equipment and piezoelectric ceramic materials, specifically to a ceramic powder and its preparation method, a method for preparing ceramic materials, and their applications. Background Technology

[0002] Tumor treatment technologies are gradually developing towards minimally invasive, precise, and multimodal approaches. Among numerous non-invasive treatment methods, High-Intensity Focused Ultrasound (HIFU) has shown broad application prospects in the clinical treatment of solid tumors such as liver cancer, uterine fibroids, and prostate cancer due to its non-invasive, radiation-free, and high-efficiency characteristics. In recent years, as the advantages of cavitation effect treatment mechanisms (such as Histotripsy) and its hybrid modes (HH) in tissue mechanical destruction, immune activation, and precise treatment boundary control have been gradually revealed, how to achieve stable excitation and precise control of high-energy-density sound fields has become one of the core technical bottlenecks in the design of such devices.

[0003] Currently, most HIFU systems on the market employ ultrasonic transducer structures such as lens-type, phased array, or multi-element array. Among these, lens-type structures have limitations such as low acoustic energy utilization and difficulty in achieving high-intensity focusing; phased array structures are costly, complex to control, and difficult to achieve high-power transient focused output. In contrast, the "self-focusing" transducer structure, with its inherent energy-focusing geometry and high acoustic-electric conversion efficiency, exhibits higher acoustic intensity output, better treatment efficiency, and stronger system adaptability in tissue-targeted therapy with deep depth and complex pathways.

[0004] Against this backdrop, Chengdu Haike Medical Equipment Co., Ltd. independently developed the "HKSFU-1D High-Intensity Self-Focusing Ultrasound Tumor Treatment System." This system innovatively integrates three treatment modes: conventional thermal effect (HIFU), pure cavitation effect (CH), and thermal-cavitation hybrid effect (HH). It can flexibly switch between treatment modes according to lesion type and treatment target, achieving broader coverage and higher treatment precision. The system employs a high-performance piezoelectric transducer with a self-focusing structure, achieving peak output of >10,000 W electrical power and >8,000 W acoustic power, a maximum treatment depth of 180 mm, and a peak positive pressure exceeding 100 MPa, far surpassing the technical level of mainstream international products (such as the HistoSonics Edison system).

[0005] However, the key to achieving such a high-power, wide-bandwidth, and controllable output self-focusing transducer lies in the performance of the piezoelectric ceramic material used. Conventional piezoelectric materials such as the PZT (Pb(Zr,Ti)O3) series are relatively mature in low-frequency, low-power applications, but face many challenges in high-power, high-intensity focusing applications, including: low Curie temperature, susceptibility to thermal failure; Q... m Insufficient mechanical quality factor leads to high energy loss; poor pressure resistance makes it difficult to withstand high-amplitude drives; and it is prone to generating nonlinear harmonics, affecting focusing performance.

[0006] To meet the extreme working requirements of high-intensity self-focusing therapy systems, the selected piezoelectric ceramics must simultaneously possess the following characteristics: (1) High Q m (1) Reduce heat dissipation; (2) High voltage electroactivity to improve energy conversion efficiency; (3) High mechanical strength and low thermal expansion coefficient to ensure structural stability; (4) Wideband response and high sound velocity matching to achieve efficient focusing; (5) High dielectric breakdown strength and fatigue resistance to cope with voltage pulse impact during long-term continuous operation. Domestic and foreign research on high-power acoustic transducer materials mainly focuses on hard-doped PZT system, Pb(Mn) 1 / 3 Nb 2 / 3 While some progress has been made in the development of O3-Pb(Zr,Ti)O3 systems and rare earth co-doped systems, they generally still suffer from problems such as insufficient stability and performance, poor process reproducibility, and incompatibility with the processing of complex structural parts.

[0007] Therefore, there is an urgent need to develop a technology that combines high Q... m This technology develops a high-intensity, high-thermal-stability, and highly machinable hard piezoelectric ceramic material, coupled with a high-density sintering and highly uniform polarization fabrication process to meet the stringent application requirements of self-focusing high-intensity energy-dissipating (HIFU) systems. This technological breakthrough will not only significantly improve the clinical efficacy of HKSFU systems in the treatment of deep-seated and refractory tumors such as liver cancer, pancreatic cancer, and kidney cancer, but also expand its applications to bone tumors, soft tissue sarcomas, and neuromodulation, demonstrating significant social and economic value, especially considering the relatively low mechanical quality factors of hard piezoelectric materials. Summary of the Invention

[0008] The purpose of this invention is to provide a ceramic powder and its preparation method, a method for preparing ceramic materials, and their applications. By doping with (1~2) at.% rare earth element Me to generate an internal bias field, pinning ferroelectric domains and reducing domain activity, the invention aims to solve the problem of insufficient stability and performance of ceramic materials under voltage pulse impact during long-term continuous operation in the prior art.

[0009] First, this invention provides a ceramic powder comprising the chemical formula (1~2)at.%Me2O3-(1-xyz)Pb(Co) 1 / 3 Ta2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3– (y)Pb(Sc) 2 / 3 W 1 / 3 Powder of O3-(z)PbTiO3;

[0010] The element Me includes at least one of the following: La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc, and Y.

[0011] x, y, and z represent mole fractions, and 0.05 ≤ x ≤ 0.4, 0.05 ≤ y ≤ 0.4, and 0.05 ≤ z ≤ 0.9.

[0012] Secondly, this invention also provides a method for preparing ceramic powder, including the following steps:

[0013] S1: Prepare Me2O3 powder and Pb(Co) powder respectively. 1 / 3 Ta 2 / 3 O3 powder, Pb(Mg) 1 / 3 Ta 2 / 3 O3 powder, Pb(Sc) 2 / 3 W 1 / 3 O3 powder and PbTiO3 powder;

[0014] S2: Preparation of (1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 )O3-(z)PbTiO3 powder;

[0015] S3: Me2O3 powder is doped into the powder prepared in S2 to prepare (1~2)at.%Me2O3-(1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3– (y)Pb(Sc) 2 / 3 W 1 / 3 )O3-(z)PbTiO3 powder.

[0016] As an optional implementation, the preparation process of the Me2O3 powder includes: mixing at least one of rare earth elements La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc, and Y, milling with anhydrous ethanol as the medium for 30 to 40 hours, and drying at 80 to 120°C to obtain Me2O3 powder.

[0017] As an optional implementation, the Pb(Co) 1 / 3 Ta 2 / 3 The preparation process of O3 powder includes: using CoCO3 and Ta2O5 as raw materials, sand milling with anhydrous ethanol as medium for 30-40 hours, drying and pre-calcining at 800-1200°C for 3-5 hours to synthesize CoTa2O6 powder.

[0018] Then, using CoTa2O6 powder and Pb3O4 as raw materials, the mixture was milled in anhydrous ethanol for 30-40 hours, dried, and pre-calcined at 700-1100°C for 1-3 hours to synthesize Pb(Co) 1 / 3 Ta 2 / 3 )O3 powder.

[0019] As an optional implementation, the Pb(Mg) 1 / 3 Ta 2 / 3 The preparation process of O3 powder includes: using MgCO3 and Ta2O5 as raw materials, grinding with anhydrous ethanol as medium for 30-40 hours, drying and pre-calcining at 800-1200°C for 3-5 hours to synthesize MgTa2O6 powder.

[0020] Then, using MgTa2O6 powder and Pb3O4 as raw materials, the mixture was milled in anhydrous ethanol for 30-40 hours, dried, and pre-calcined at 700-1100°C for 1-3 hours to synthesize Pb(Mg) 1 / 3 Ta 2 / 3 )O3 powder.

[0021] As an optional implementation, the Pb(Sc) 2 / 3 W 1 / 3 The preparation process of Sc2O3 powder includes: using Sc2O3 and WO3 as raw materials for mixing, sand milling with anhydrous ethanol as medium for 30-40 hours, drying and pre-calcining at 800-1200°C for 3-5 hours to synthesize Sc2WO6 powder;

[0022] Then, using Sc2WO6 powder and Pb3O4 as raw materials, the mixture was milled in anhydrous ethanol for 30-40 hours, dried, and pre-calcined at 700-1100°C for 1-3 hours to synthesize Pb(Sc 2 / 3 W 1 / 3 )O3 powder.

[0023] As an optional implementation, the preparation process of the PbTiO3 powder includes: using Pb3O4 and TiO2 as raw materials for batching, milling with anhydrous ethanol as the medium for 1 to 3 hours, drying, and then pre-calcining at 600 to 900°C for 1 to 3 hours to synthesize PbTiO3 powder.

[0024] As an optional implementation, the preparation of (1-xyz)Pb(Co) in S2 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 The O3-(z)PbTiO3 powder is synthesized by mixing ingredients according to its chemical formula, sand milling with anhydrous ethanol as the medium for 11-13 hours, drying, and pre-calcining at 800-1000°C for 1-3 hours.

[0025] The process of doping Me2O3 powder into the powder prepared in S2 as described in S3 includes: mixing Me2O3 powder with (1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 The O3-(z)PbTiO3 powder was sand-milled in anhydrous ethanol for 20-30 hours and then dried.

[0026] Furthermore, embodiments of the present invention provide a method for preparing a ceramic material, comprising the following steps: preparing the (1~2)at.%Me2O3-(1-xyz)Pb(Co) material as described above. 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 PbTiO3 powder was mixed with 1-3 wt% PVA solution, granulated, and pressed into discs;

[0027] The disc is kept at 600-700°C for 1-3 hours to remove PVA;

[0028] The PVA-free discs are subjected to a two-step sintering process. The first step involves heating to a sintering temperature of 1000~1350°C, and the second step involves cooling to 900~1050°C and holding at that temperature for 2~4 hours.

[0029] The sintered disc is processed into a smooth, thin sheet on both sides and coated with silver electrodes.

[0030] Finally, this embodiment of the invention provides an application of a ceramic material, which is used in a high-intensity self-focusing ultrasound tumor treatment system.

[0031] Compared with the prior art, the embodiments of the present invention have the following advantages and beneficial effects:

[0032] 1. The ceramic powder provided in this embodiment of the invention generates an internal bias field by doping with (1~2) at.% rare earth element Me, pinning ferroelectric domains, reducing domain activity, and improving the mechanical quality factor (Q). m The Q value was increased to 3000. After the ceramic powder was prepared into ceramic materials, it exhibited excellent stability in the range of -60°C to 120°C, and after 100 million cycles, the Q value was [missing information]. m The reduction is less than 1.5%. High-intensity focused ultrasound (HIFU) systems enable non-invasive, precise treatment of deep tumors such as liver and pancreatic cancer, supporting thermal effects, Histotripsy, and hybrid thermal-cavitation modes to improve treatment efficiency and the range of indications. They are also suitable for neuromodulation, acoustic imaging, and industrial high-power ultrasound equipment, demonstrating broad application potential.

[0033] 2. In this embodiment of the invention, the doping amount of rare earth element Me is set to (1~2) at.%, which is determined based on the solid solubility of rare earth ions at the B site of perovskite and the formation mechanism of the internal bias field. When the doping amount is less than 1 at.%, the solid solubility of rare earth ions is insufficient, and an effective internal bias field cannot be formed; when it exceeds 2 at.%, rare earth ions are prone to enrichment at grain boundaries to form a second phase, leading to increased dielectric loss and degraded piezoelectric performance. Experiments in this embodiment of the invention demonstrate that (1~2) at.% can simultaneously improve Q. m Up to 3000 and remain at a high level 33 .

[0034] 3. The ceramic powder Pb(Co) prepared in the embodiments of the present invention 1 / 3 Ta 2 / 3 O3, Pb(Mg) 1 / 3 Ta 2 / 3 O3, Pb(Sc) 2 / 3 W 1 / 3 The combination of O3 and PbTiO3 four phases embodies the synergistic design of hard and soft phases. The first two provide a high mechanical quality factor, the third phase enhances thermal stability, and the fourth phase improves the piezoelectric coefficient and Curie temperature. The values ​​of x, y, and z are taken in the ranges of 0.05~0.4, 0.05~0.4, and 0.05~0.9, respectively, to ensure a balance between lattice distortion and phase stability. Exceeding these ranges will lead to phase separation or increased dielectric loss.

[0035] 4. The hard piezoelectric ceramic material prepared in the embodiments of the present invention supports thermal effect (HIFU), cavitation effect (Histotripsy) and thermal-cavitation hybrid mode (HH) in the HKSFU-1D high-intensity self-focusing ultrasound tumor treatment system, achieving ultra-high performance output of >10000 W electrical power, >8000 W acoustic power, 180 mm maximum treatment depth and peak positive pressure >100 MPa, far exceeding traditional PZT materials.

[0036] 5. The embodiments of this invention employ a stepwise synthesis and stepwise sintering process (pre-firing temperature of each precursor is 600~1200℃, and composite powder is sintered into ceramic at 800~1000℃). Through rare earth element doping, an internal bias field is generated, strongly pinning ferroelectric domains, improving the mechanical quality factor, and maintaining excellent stability within the range of -60°C to 120°C. After 100 million cycles, Q... m The decrease is less than 1.5%, which is significantly better than the stability and fatigue resistance of existing hard-doped PZT systems.

[0037] 6. The preparation process of this invention optimizes the grain size and uniformity by sand milling for 30-40 hours and two-step sintering, resulting in high density. It is compatible with the processing of complex structural parts and meets the high consistency requirements of in vitro, in vivo and clinical trials (such as liver cancer treatment), overcoming the limitation of poor reproducibility of traditional processes. Attached Figure Description

[0038] To more clearly illustrate the technical solutions of the exemplary embodiments of the present invention, the accompanying drawings used in the embodiments will be briefly described below. It should be understood that the following drawings only show some embodiments of the present invention and should not be considered as a limitation of the scope. For those skilled in the art, other related drawings can be obtained based on these drawings without creative effort. In the drawings:

[0039] Figure 1 The X-ray diffraction pattern of the ceramic material prepared in Example 1;

[0040] Figure 2 The image shows the scanning electron microscope (SEM) pattern of the ceramic material prepared in Example 1.

[0041] Figure 3 The graphs show the changes in dielectric constant and dielectric loss of the ceramic material prepared in Example 1 as a function of temperature.

[0042] Figure 4 The hysteresis loop is the hysteresis loop of the ceramic material prepared in Example 1. Detailed Implementation

[0043] To make the objectives, technical solutions, and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below. Obviously, the described embodiments are some embodiments of the present invention, but not all embodiments.

[0044] Therefore, the detailed description of the embodiments of the present invention provided below is not intended to limit the scope of the claimed invention, but merely to illustrate selected embodiments of the invention. All other embodiments obtained by those skilled in the art based on the embodiments of the present invention without inventive effort are within the scope of protection of the present invention.

[0045] First, this invention provides a method for preparing ceramic powder, comprising the following: (1~2)at.%Me2O3-(1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x) Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y) Pb(Sc) 2 / 3 W 1 / 3 In the formula )O3-(z)PbTiO3, Me is at least one of the rare earth elements La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc, and Y, and x, y, and z represent the mole fractions, where 0.05 ≤ x ≤ 0.4, 0.05 ≤ y ≤ 0.4, and 0.05 ≤ z ≤ 0.9.

[0046] (1) First, prepare the ingredients according to the chemical formula Me2O3 (where Me is at least one of the rare earth elements La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc, Y), and then grind the rare earth elements in anhydrous ethanol for 30 to 40 hours to reduce the particle size. Then, dry the powder at 80 to 120°C to obtain a highly reactive Me2O3 powder.

[0047] (2) According to the chemical formula Pb(Co) 1 / 3 Ta 2 / 3 CoTa2O6 powder was synthesized by using CoCO3 and Ta2O5 as raw materials, milling with anhydrous ethanol for 30-40 hours, drying, and pre-calcining at 800-1200°C for 4 hours. Then, Pb(Co)3O4 powder and Pb3O4 were used as raw materials, milled with anhydrous ethanol for 30-40 hours, dried, and pre-calcined at 700-1100°C for 2 hours. 1 / 3 Ta 2 / 3 )O3 powder;

[0048] (3) According to the chemical formula Pb(Mg)1 / 3 Ta 2 / 3 MgTa₂O₆ powder was synthesized by using MgCO₃ and Ta₂O₅ as raw materials, milling with anhydrous ethanol for 30-40 hours, drying, and pre-calcining at 800-1200°C for 3-5 hours. Then, Pb(Mg)₂O₆ powder and Pb₃O₄ were used as raw materials for further synthesis, milling with anhydrous ethanol for 30-40 hours, drying, and pre-calcining at 700-1100°C for 1-3 hours. 1 / 3 Ta 2 / 3 )O3 powder;

[0049] (4) According to the chemical formula Pb(Sc) 2 / 3 W 1 / 3 Sc2WO6 powder was synthesized by using Sc2O3 and WO3 as raw materials, milling with anhydrous ethanol for 30-40 hours, drying, and pre-calcining at 800-1200°C for 3-5 hours. Then, Pb(Sc)O3 powder and Pb3O4 were used as raw materials for further synthesis, milling with anhydrous ethanol for 30-40 hours, drying, and pre-calcining at 700-1100°C for 1-3 hours. 2 / 3 W 1 / 3 )O3 powder;

[0050] (5) PbTiO3 powder is synthesized by using Pb3O4 and TiO2 as raw materials according to the chemical formula PbTiO3, sand milling for 1 to 3 hours with anhydrous ethanol as medium, drying and pre-calcining at 600 to 900°C for 1 to 3 hours.

[0051] (6) According to the chemical formula (1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–x Pb(Mg) 1 / 3 Ta 2 / 3 )O3–y Pb(Sc 2 / 3 W 1 / 3 (1-xyz)Pb(Co) was synthesized by mixing O3-zPbTiO3, where x, y, and z represent mole fractions, 0.05≤x≤0.4, 0.05≤y≤0.4, and 0.05≤z≤0.9. The mixture was milled in anhydrous ethanol for 11-13 hours, dried, and then pre-calcined at 800-1000°C for 1-3 hours. 1 / 3 Ta 2 / 3 O3–(x) Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 )O3-(z)PbTiO3 powder;

[0052] (7) The resulting powder is (1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x) Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3W 1 / 3 Me₂O₃-(1-xyz)Pb(Co)O₃ powder, and at least one of the rare earth elements La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc, and Y, are subjected to high-energy sand milling with anhydrous ethanol as the medium for 20-30 hours, and dried to obtain powder (1-2)at.%Me₂O₃-(1-xyz)Pb(Co)O₃. 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y) Pb(Sc) 2 / 3 W 1 / 3 )O3-(z)PbTiO3 powder.

[0053] Secondly, this invention also provides a method for preparing a ceramic material, comprising the following:

[0054] (1) Take the powder obtained above (1~2)at.%Me2O3-(1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3Ta 2 / 3 O3–(y) Pb(Sc) 2 / 3 W 1 / 3 PbTiO3 powder was mixed with 1-3 wt% PVA solution, granulated, and pressed into discs;

[0055] (2) Place the disc at 600~700°C for 1~3 hours to remove PVA;

[0056] (3) The PVA-free discs are subjected to a two-step sintering method. The first step is to raise the temperature to the sintering temperature of 1000~1350°C, and the second step is to lower the temperature to 900~1050°C and hold for 2~4 hours.

[0057] (4) The sintered disc is processed into a smooth sheet with a diameter of about 100 mm and a thickness of about 3 mm, and coated with silver electrodes.

[0058] Example 1: A method for preparing ceramic powder and a method for preparing ceramic materials are provided, including the following:

[0059] (1) 2.445 g of La2O3 with a purity of 99.99% was used as the raw material. The rare earth elements were milled for 36 hours with anhydrous ethanol as the medium to reduce the particle size. The La2O3 powder with strong reactivity was obtained by drying at 100°C.

[0060] (2) Using 99.99% pure CoCO3 and Ta2O5 as raw materials, 59.45 g and 110.475 g of each were weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 1000°C for 4 hours to synthesize CoTa2O6 powder. Then, using CoTa2O6 powder and Pb3O4 as raw materials, 114.25 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 900°C for 2 hours to synthesize Pb(Co)2O6. 1 / 3 Ta 2 / 3 )O3 powder;

[0061] (3) Using MgCO3 and Ta2O5 with a purity of 99.99% as raw materials, 42.15 g and 110.475 g of MgCO3 and Ta2O5 respectively were weighed and mixed. The mixture was then milled in anhydrous ethanol for 36 hours, dried, and pre-calcined at 1000°C for 4 hours to synthesize MgTa2O6 powder. Then, using MgTa2O6 powder and Pb3O4 as raw materials, 114.25 g of Pb3O4 was weighed and mixed. The mixture was then milled in anhydrous ethanol for 36 hours, dried, and pre-calcined at 900°C for 2 hours to synthesize Pb(Mg)2O6. 1 / 3 Ta 2 / 3 )O3 powder;

[0062] (4) Using Sc2O3 and WO3 with a purity of 99.99% as raw materials, 23 grams and 38.65 grams of Sc2O3 and WO3 respectively were weighed and mixed. The mixture was then milled in anhydrous ethanol for 36 hours, dried, and pre-calcined at 1000°C for 4 hours to synthesize Sc2WO6 powder. Then, using Sc2WO6 powder and Pb3O4 as raw materials, 114.25 grams of Pb3O4 were weighed and mixed. The mixture was then milled in anhydrous ethanol for 36 hours, dried, and pre-calcined at 900°C for 2 hours to synthesize Pb(Sc2WO6) powder. 2 / 3 W 1 / 3 )O3 powder;

[0063] (5) Using 99.99% pure Pb3O4 and TiO2 as raw materials, weigh 804.85g and 279.55g respectively for batching, and use anhydrous ethanol as medium for sand milling for 2 hours. After drying, PbTiO3 powder is synthesized by pre-calcination at 750°C for 2 hours.

[0064] (6) According to the chemical formula 0.1Pb(Co) 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3 Ta 2 / 3O3–0.1Pb(Sc) 2 / 3 W 1 / 3) O3–0.7PbTiO3 was used for batching, and Pb(Co) was weighed separately. 1 / 3 Ta 2 / 3 O3 197.75 g, Pb(Mg) 1 / 3 Ta 2 / 3 O3 191.95 g, Pb(Sc) 2 / 3 W 1 / 3 173.25 g of O3 and 1060.75 g of PbTiO3 were milled in anhydrous ethanol for 12 hours, dried, and then pre-calcined at 900°C for 2 hours to synthesize 0.1 Pb(Co) 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 )O3–0.7PbTiO3 powder;

[0065] (7) Take the 0.1Pb(Co) powder obtained in step (6) 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3W 1 / 3 )O3–0.7PbTiO3 powder, with 24.45 g of La2O3, was high-energy milled for 24 hours in anhydrous ethanol, and dried to obtain 1.5 at.%La2O3–0.1Pb(Co)O3 powder. 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 )O3–0.7PbTiO3 powder;

[0066] (8) The powder obtained in step (7) is mixed with 2 wt% PVA solution, granulated, and pressed into discs;

[0067] (9) Place the disc from step (8) at 650°C for 2 hours to remove PVA;

[0068] (10) The disc obtained in step (9) is sintered in two steps. The first step is to heat the disc to the sintering temperature of 1200°C without holding it at that temperature. The second step is to rapidly cool the disc to 1000°C and hold it at that temperature for 3 hours.

[0069] (11) The sintered disc from step (10) is processed into a smooth sheet with a diameter of 100 mm and a thickness of about 3 mm, and coated with silver electrodes. Its impedance resonance spectrum is tested and the mechanical quality factor is calculated, and its mechanical quality factor is found to be 3000.

[0070] Example 2: A method for preparing ceramic powder and a method for preparing ceramic materials are provided, including the following:

[0071] (1) 3.39 g of Y2O3 with a purity of 99.99% was used as the raw material. The rare earth elements were milled for 30 hours with anhydrous ethanol as the medium to reduce the particle size. The powder was dried at 80°C to obtain Y2O3 powder with strong reactivity.

[0072] (2) Using 99.99% pure CoCO3 and Ta2O5 as raw materials, 5.95 g and 11.05 g of each were weighed and mixed. The mixture was milled in anhydrous ethanol for 30 hours, dried, and then pre-calcined at 800°C for 5 hours to synthesize CoTa2O6 powder. Then, using CoTa2O6 powder and Pb3O4 as raw materials, 11.41 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 30 hours, dried, and then pre-calcined at 700°C for 3 hours to synthesize Pb(Co)2O6. 1 / 3 Ta 2 / 3 )O3 powder.

[0073] (3) Using MgCO3 and Ta2O5 with a purity of 99.99% as raw materials, 4.22 g and 11.05 g of each were weighed and mixed. The mixture was then milled in anhydrous ethanol for 30 hours, dried, and pre-calcined at 800°C for 4 hours to synthesize MgTa2O6 powder. Then, using MgTa2O6 powder and Pb3O4 as raw materials, 11.41 g of Pb3O4 was weighed and mixed. The mixture was then milled in anhydrous ethanol for 30 hours, dried, and pre-calcined at 700°C for 3 hours to synthesize Pb(Mg)2O6. 1 / 3 Ta 2 / 3 )O3 powder.

[0074] (4) Using Sc2O3 and WO3 with a purity of 99.99% as raw materials, 4.60 g and 7.73 g of Sc2O3 and WO3 respectively were weighed and mixed. The mixture was then milled in anhydrous ethanol for 30 hours, dried, and pre-calcined at 800°C for 5 hours to synthesize Sc2WO6 powder. Then, using Sc2WO6 powder and Pb3O4 as raw materials, 22.85 g of Pb3O4 was weighed and mixed. The mixture was then milled in anhydrous ethanol for 30 hours, dried, and pre-calcined at 700°C for 3 hours to synthesize Pb(Sc2WO6) powder. 2 / 3 W1 / 3)O3 powder.

[0075] (5) Using 99.99% pure Pb3O4 and TiO2 as raw materials, weigh 182.83 g and 63.89 g respectively for batching, and use anhydrous ethanol as medium for sand milling for 1 hour. After drying, PbTiO3 powder is synthesized by pre-calcining at 600°C for 3 hours.

[0076] (6) According to the chemical formula 0.05Pb(Co) 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 The ingredients were prepared by mixing O3–0.8PbTiO3, and the weights of Pb(Co) were weighed separately. 1 / 3 Ta 2 / 3 )O3 19.77 g, Pb(Mg 1 / 3 Ta 2 / 3 O3 19.20 g, Pb(Sc) 2 / 3W 1 / 3 34.65 g of O3 and 242.45 g of PbTiO3 were milled in anhydrous ethanol for 11 hours, dried, and then pre-calcined at 800°C for 3 hours to synthesize 0.05 Pb(Co)3. 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 )O3–0.8PbTiO3 powder;

[0077] (7) Take the 0.05Pb(Co) powder obtained in step (6) 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 Y₂O₃–0.8PbTiO₃ powder was mixed with 3.39 g of Y₂O₃ and high-energy milled for 24 hours in anhydrous ethanol. After drying, 1.5 at.% Y₂O₃–0.05Pb(Co)₂O₃ was obtained. 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 )O3–0.9PbTiO3 powder;

[0078] (8) Mix the powder obtained in step (7) with 1 wt% PVA solution, granulate, and press into discs;

[0079] (9) Place the disc from step (8) at 600°C for 3 hours to remove PVA;

[0080] (10) The disc obtained in step (9) is sintered in two steps. The first step is to heat the disc to the sintering temperature of 1000°C without holding it at that temperature. The second step is to rapidly cool the disc to 900°C and hold it at that temperature for 4 hours.

[0081] (11) The sintered disc from step (10) is processed into a smooth sheet with a diameter of 100 mm and a thickness of about 3 mm, and coated with silver electrodes. Its impedance resonance spectrum is tested and the mechanical quality factor is calculated, and its mechanical quality factor is found to be 3100.

[0082] Example 3: A method for preparing ceramic powder and a method for preparing ceramic materials are provided, including the following:

[0083] (1) 5.05 g of Nd2O3 with a purity of 99.99% was used as the raw material. The rare earth elements were milled for 40 hours with anhydrous ethanol as the medium to reduce the particle size. The powder was dried at 120°C to obtain Nd2O3 powder with strong reactivity.

[0084] (2) Using 99.99% pure CoCO3 and Ta2O5 as raw materials, 2.77 g and 10.31 g of each were weighed and mixed. The mixture was milled in anhydrous ethanol for 40 hours, dried, and then pre-calcined at 1200°C for 3 hours to synthesize CoTa2O6 powder. Then, using CoTa2O6 powder and Pb3O4 as raw materials, 15.99 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 40 hours, dried, and then pre-calcined at 1100°C for 1 hour to synthesize Pb(Co)2O6. 1 / 3 Ta 2 / 3 )O3 powder.

[0085] (3) Using MgCO3 and Ta2O5 with a purity of 99.99% as raw materials, 1.69 g and 8.84 g of each were weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 1200°C for 3 hours to synthesize MgTa2O6 powder. Then, using MgTa2O6 powder and Pb3O4 as raw materials, 13.71 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 40 hours, dried, and then pre-calcined at 1100°C for 1 hour to synthesize Pb(Mg) 1 / 3 Ta 2 / 3 )O3 powder.

[0086] (4) Using Sc2O3 and WO3 with a purity of 99.99% as raw materials, 3.22 g and 5.41 g of Sc2O3 and WO3 were weighed and mixed respectively. The mixture was milled in anhydrous ethanol for 40 hours, dried, and then pre-calcined at 1200°C for 5 hours to synthesize Sc2WO6 powder. Then, using Sc2WO6 powder and Pb3O4 as raw materials, 15.99 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 40 hours, dried, and then pre-calcined at 1100°C for 1 hour to synthesize Pb(Sc2WO6) powder. 2 / 3 W 1 / 3 )O3 powder.

[0087] (5) Using 99.99% pure Pb3O4 and TiO2 as raw materials, weigh 182.83 g and 63.89 g respectively for batching, and use anhydrous ethanol as medium for sand milling for 3 hours. After drying, PbTiO3 powder is synthesized by pre-calcining at 900°C for 1 hour.

[0088] (6) According to the chemical formula 0.07Pb(Co) 1 / 3 Ta 2 / 3 O3–0.06Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.07Pb(Sc) 2 / 3 W 1 / 3 The ingredients were prepared by mixing O3–0.9PbTiO3, and the weights of Pb(Co) were weighed separately. 1 / 3 Ta 2 / 3 )O3 27.68 g, Pb(Mg) 1 / 3 Ta 2 / 3 O3 23.04 g, Pb(Sc) 2 / 3W 1 / 3 24.25 g of O3 and 24.45 g of PbTiO3 were milled in anhydrous ethanol for 13 hours, dried, and then pre-calcined at 1000°C for 1 hour to synthesize 0.07Pb(Co) 1 / 3 Ta 2 / 3 O3–0.06Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.07Pb(Sc) 2 / 3 W 1 / 3 )O3–0.8PbTiO3 powder;

[0089] (7) The 0.07Pb(Co) powder obtained in step (6) 1 / 3 Ta 2 / 3 O3–0.06Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.07Pb(Sc) 2 / 3 W 1 / 3)O3–0.8PbTiO3 powder, with 5.05 g of Nd2O3, was high-energy milled for 30 hours in anhydrous ethanol, and dried to obtain 1.5 at.% Nd2O3–0.07Pb(Co)O3. 1 / 3 Ta 2 / 3 O3–0.06Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.07Pb(Sc) 2 / 3 W 1 / 3) O3–0.8PbTiO3 powder;

[0090] (8) Mix the powder obtained in step (7) with 3wt% PVA solution, granulate, and press into discs;

[0091] (9) Place the disc from step (8) at 700°C for 1 hour to remove PVA;

[0092] (10) The disc obtained in step (9) is sintered in two steps. The first step is to heat the disc to the sintering temperature of 1350°C without holding it at that temperature. The second step is to rapidly cool the disc to 1050°C and hold it at that temperature for 2 hours.

[0093] (11) The sintered disc from step (10) is processed into a smooth sheet with a diameter of 100 mm and a thickness of about 3 mm, and coated with silver electrodes. Its impedance resonance spectrum is tested and the mechanical quality factor is calculated, and its mechanical quality factor is found to be 3000.

[0094] Example 4: A method for preparing ceramic powder and a method for preparing ceramic materials are provided, including the following:

[0095] (1) 4.95 g of Pr2O3 with a purity of 99.99% was used as the raw material. The rare earth elements were milled for 36 hours with anhydrous ethanol as the medium to reduce the particle size. The powder was dried at 100°C to obtain Pr2O3 powder with strong reactivity.

[0096] (2) Using 99.99% pure CoCO3 and Ta2O5 as raw materials, 1.98 g and 7.36 g of each were weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 1000°C for 4 hours to synthesize CoTa2O6 powder. Then, using CoTa2O6 powder and Pb3O4 as raw materials, 11.43 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 850°C for 2 hours to synthesize Pb(Co)2O6. 1 / 3 Ta 2 / 3 )O3 powder.

[0097] (3) Using MgCO3 and Ta2O5 with a purity of 99.99% as raw materials, 1.41 g and 7.36 g of each were weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 1000°C for 4 hours to synthesize MgTa2O6 powder. Then, using MgTa2O6 powder and Pb3O4 as raw materials, 11.43 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 850°C for 2 hours to synthesize Pb(Mg) 1 / 3 Ta 2 / 3 )O3 powder.

[0098] (4) Using Sc2O3 and WO3 with a purity of 99.99% as raw materials, 4.60 g and 7.73 g of Sc2O3 and WO3 were weighed and mixed respectively. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 1000°C for 4 hours to synthesize Sc2WO6 powder. Then, using Sc2WO6 powder and Pb3O4 as raw materials, 22.85 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 850°C for 2 hours to synthesize Pb(Sc2WO6) powder. 2 / 3 W 1 / 3 )O3 powder.

[0099] (5) Using 99.99% pure Pb3O4 and TiO2 as raw materials, weigh 182.83 g and 63.89 g respectively for batching, and use anhydrous ethanol as medium for sand milling for 2 hours. After drying, PbTiO3 powder is synthesized by pre-calcination at 750°C for 2 hours.

[0100] (6) According to the chemical formula 0.05Pb(Co) 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 The ingredients were prepared by mixing O3–0.8PbTiO3, and the weights of Pb(Co) were weighed separately. 1 / 3 Ta 2 / 3 )O3 19.77 g, Pb(Mg 1 / 3 Ta 2 / 3 O3 19.20 g, Pb(Sc) 2 / 3W 1 / 3 34.65 g of O3 and 242.45 g of PbTiO3 were milled in anhydrous ethanol for 12 hours, dried, and then pre-calcined at 900°C for 2 hours to synthesize 0.05Pb(Co) 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W1 / 3 )O3–0.8PbTiO3 powder;

[0101] (7) Take the 0.05Pb(Co) powder obtained in step (6) 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 Pr₂O₃–0.8PbTiO₃ powder was mixed with 4.95 g of Pr₂O₃ and high-energy milled for 24 hours in anhydrous ethanol. After drying, 1.5 at.% Pr₂O₃–0.05Pb(Co)₂O₃ was obtained. 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 )O3–0.8PbTiO3 powder;

[0102] (8) The powder obtained in step (7) is mixed with 2 wt% PVA solution, granulated, and pressed into discs;

[0103] (9) Place the disc from step (8) at 650°C for 2 hours to remove PVA;

[0104] (10) The disc obtained in step (9) is sintered in two steps. The first step is to heat the disc to the sintering temperature of 1200°C without holding it at that temperature. The second step is to rapidly cool the disc to 950°C and hold it at that temperature for 3 hours.

[0105] (11) The sintered disc from step (10) is processed into a smooth sheet with a diameter of 100 mm and a thickness of about 3 mm, and coated with silver electrodes. Its impedance resonance spectrum is tested and the mechanical quality factor is calculated, and its mechanical quality factor is found to be 3050.

[0106] Example 5: A method for preparing ceramic powder and a method for preparing ceramic materials are provided, including the following:

[0107] (1) 5.23 g of Sm2O3 with a purity of 99.99% was used as the raw material. The rare earth element particles were reduced by sand milling for 36 hours with anhydrous ethanol as the medium. The powder was dried at 100°C to obtain Sm2O3 powder with strong reactivity.

[0108] (2) Using 99.99% pure CoCO3 and Ta2O5 as raw materials, 1.98 g and 7.36 g of each were weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 1000°C for 4 hours to synthesize CoTa2O6 powder. Then, using CoTa2O6 powder and Pb3O4 as raw materials, 11.43 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 900°C for 2 hours to synthesize Pb(Co)2O6. 1 / 3 Ta 2 / 3 )O3 powder.

[0109] (3) Using MgCO3 and Ta2O5 with a purity of 99.99% as raw materials, 1.41 g and 7.36 g of each were weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 1000°C for 4 hours to synthesize MgTa2O6 powder. Then, using MgTa2O6 powder and Pb3O4 as raw materials, 11.43 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 950°C for 2 hours to synthesize Pb(Mg) 1 / 3 Ta 2 / 3 )O3 powder.

[0110] (4) Using Sc2O3 and WO3 with a purity of 99.99% as raw materials, 4.60 g and 7.73 g of Sc2O3 and WO3 respectively were weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 1000°C for 4 hours to synthesize Sc2WO6 powder. Then, using Sc2WO6 powder and Pb3O4 as raw materials, 22.85 g of Pb3O4 was weighed and mixed. The mixture was milled in anhydrous ethanol for 36 hours, dried, and then pre-calcined at 950°C for 2 hours to synthesize Pb(Sc2WO6) powder. 2 / 3 W 1 / 3 )O3 powder.

[0111] (5) Using 99.99% pure Pb3O4 and TiO2 as raw materials, weigh 182.83 g and 63.89 g respectively for batching, and use anhydrous ethanol as medium for sand milling for 2 hours. After drying, PbTiO3 powder is synthesized by pre-calcination at 800°C for 2 hours.

[0112] (6) According to the chemical formula 0.05Pb(Co) 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 The ingredients were prepared by mixing O3–0.8PbTiO3, and the weights of Pb(Co) were weighed separately. 1 / 3 Ta 2 / 3 )O3 19.77 g, Pb(Mg1 / 3 Ta 2 / 3 O3 19.20 g, Pb(Sc) 2 / 3W 1 / 3 34.65 g of O3 and 242.45 g of PbTiO3 were milled in anhydrous ethanol for 12 hours, dried, and then pre-calcined at 900°C for 2 hours to synthesize 0.05Pb(Co) 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 )O3–0.8PbTiO3 powder;

[0113] (7) Take the 0.05Pb(Co) powder obtained in step (6) 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 0.8PbTiO3 powder was mixed with 5.23 g of Sm2O3 and high-energy milled for 24 hours in anhydrous ethanol. After drying, 1.5 at.% Sm2O3-0.05Pb(Co) was obtained. 1 / 3 Ta 2 / 3 O3–0.05Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 )O3–0.8PbTiO3 powder;

[0114] (8) The powder obtained in step (7) is mixed with 2 wt% PVA solution, granulated, and pressed into discs;

[0115] (9) Place the disc from step (8) at 650°C for 2 hours to remove PVA;

[0116] (10) The disc obtained in step (9) is sintered in two steps. The first step is to heat the disc to a sintering temperature of 1000-1350°C without holding it at that temperature. The second step is to rapidly cool the disc to 950°C and hold it at that temperature for 3 hours.

[0117] (11) The sintered disc from step (10) is processed into a smooth sheet with a diameter of 100 mm and a thickness of about 3 mm, and coated with silver electrodes. Its impedance resonance spectrum is tested and the mechanical quality factor is calculated, and its mechanical quality factor is found to be 3000.

[0118] Example 6: A method for preparing ceramic powder and ceramic materials is provided. The difference from Example 1 is that the rare earth doping amount is 1.0 at.% Y₂O₃, and the final product is a ceramic powder with the chemical formula 1.0 at.% Y₂O₃-0.1Pb(Co). 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 Using O3–0.7PbTiO3 powder, with the remaining process steps kept the same, the resulting ceramic sample had high density and uniform grain distribution, and its mechanical quality factor was 3100.

[0119] Example 7: A method for preparing ceramic powder and ceramic materials is provided. The difference from Example 1 is that the rare earth doping amount is 2.0 at.% Y₂O₃, and the final product is prepared with the chemical formula 2.0 at.% Y₂O₃-0.1Pb(Co). 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 O3–0.7PbTiO3 powder was used, and the remaining process steps were kept the same, resulting in a mechanical quality factor of 3200.

[0120] Example 8: A method for preparing ceramic powder and ceramic materials is provided. The difference from Example 1 is that the proportion of intermediate components is adjusted to finally prepare a ceramic powder with the chemical formula 1.5at.%Y₂O₃-0.5Pb(Co). 1 / 3 Ta 2 / 3 O3–0.4Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.05Pb(Sc) 2 / 3 W 1 / 3 Using 0.05PbTiO3 powder and keeping the other process steps the same, a mechanical quality factor of 3050 was obtained, which showed good dielectric and mechanical stability.

[0121] Example 9: A method for preparing ceramic powder and ceramic materials is provided. The difference from Example 1 is that the proportion of intermediate components is adjusted to finally prepare a ceramic powder with the chemical formula 1.5 at.% Y₂O₃-0.2Pb(Co). 1 / 3 Ta 2 / 3 O3–0.2Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.2Pb(Sc) 2 / 3 W 1 / 3Using PbTiO3 powder with a content of 0.4%, and keeping the other process steps the same, the mechanical quality factor was 2900. When the PbTiO3 content was less than 0.7%, the material grains were slightly coarsened and the dielectric loss increased slightly.

[0122] Example 10: A method for preparing ceramic powder and ceramic material is provided. The difference from Example 1 is that only one sintering step is used in step 10. The temperature is directly raised to 1000°C and held for 3 hours. The other steps remain unchanged. The mechanical quality factor is 2850. The sintering density of this sample is slightly lower, but it still maintains a high mechanical quality factor.

[0123] Comparative Example 1: A method for preparing ceramic powder and ceramic material is provided. The difference from Example 1 is that rare earth element doping is not performed, and the final product is 0.1Pb(Co) 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 Using O3–0.7PbTiO3 powder, with the remaining process steps and parameters kept the same, the mechanical quality factor was obtained as 2600.

[0124] Comparative Example 2: A method for preparing ceramic powder and ceramic material is provided. The difference from Example 1 is that the rare earth doping amount is less than 1.0 at.%, and the final product is Y₂O₃-0.1Pb(Co)₂. 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 Using O3–0.7PbTiO3 powder, with the remaining process steps and parameters kept the same, the mechanical quality factor was obtained as 2700.

[0125] Comparative Example 3: A method for preparing ceramic powder and ceramic materials is provided. The difference from Example 1 is that the rare earth doping amount is greater than 2.0 at.%, and the final product is Y₂O₃-0.1Pb(Co)₂. 1 / 3 Ta 2 / 3 O3–0.1Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 Using O3–0.7PbTiO3 powder, with the remaining process steps and parameters kept the same, the mechanical quality factor was obtained as 2800.

[0126] Comparative Example 4: A method for preparing ceramic powder and ceramic materials is provided, the difference from Example 1 being that Pb(Mg) is not added to the raw materials used. 1 / 3 Ta 2 / 3 The final product obtained was 1.5 at.% Y₂O₃-0.05Pb(Co)O₃. 1 / 3 Ta 2 / 3 O3–0.05Pb(Sc) 2 / 3 W 1 / 3 Using O3–0.9PbTiO3 powder, with the remaining process steps and parameters kept the same, the mechanical quality factor was obtained as 2750.

[0127] Comparative Example 5: A method for preparing ceramic powder and ceramic materials is provided, the difference from Example 1 being that Pb(Co) is not added to the raw materials used. 1 / 3 Ta 2 / 3 The final product obtained was 1.5 at.% Y₂O₃–0.1Pb(Mg)O₃. 1 / 3Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3 Using O3–0.8PbTiO3 powder, with the remaining process steps and parameters kept the same, the mechanical quality factor was obtained as 2600.

[0128] Comparative Example 6: A method for preparing ceramic powder and ceramic materials is provided. The difference from Example 1 is that PbTiO3 was not added to the raw materials used, and the final product obtained is 1.5 at.%La2O3-0.4Pb(Co) 1 / 3 Ta 2 / 3 O3–0.4Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.2Pb(Sc) 2 / 3 W 1 / 3 O3 powder, with the remaining process steps and parameters kept the same, yielded a mechanical quality factor of 2600.

[0129] Comparative Example 7: A method for preparing ceramic powder and ceramic materials is provided. The difference from Example 1 is that x is greater than 0.4 in the raw materials used, and the final product obtained has the chemical formula 1.5at.%La2O3-0.2Pb(Co) 1 / 3 Ta 2 / 3 O3–0.5Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.1Pb(Sc) 2 / 3 W 1 / 3Using O3–0.2PbTiO3 powder, with the remaining process steps and parameters kept the same, the mechanical quality factor was obtained as 2800.

[0130] Comparative Example 8: A method for preparing ceramic powder and ceramic materials is provided. The difference from Example 1 is that x is less than 0.05 in the raw materials used, and the final product obtained has the chemical formula 1.5at.%La2O3-0.5Pb(Co) 1 / 3 Ta 2 / 3 O3–0.04Pb(Mg) 1 / 3 Ta 2 / 3 O3–0.06Pb(Sc) 2 / 3 W 1 / 3 Using O3–0.4PbTiO3 powder, with the remaining process steps and parameters kept the same, the mechanical quality factor was obtained as 2900.

[0131] Experimental verification: The ceramic materials prepared in Examples 1-10 and Comparative Examples 1-8 were subjected to performance testing. The testing methods were all performed according to GB / T 12766.2-2021 "Test Methods for Performance of Piezoelectric Ceramic Materials" and IEC 60483 standard. The mechanical quality factor Q was also tested. m The resonant-anti-resonant method was used for measurement, 1×10 8 Q after the second loop m The density reduction rate was calculated using cyclic loading tests (20 kHz, room temperature to 120°C range). The density change rate during thermal aging was determined according to GB / T 5593-2019 "Methods for Determination of Density of Ceramic Materials". The test results are shown in Table 1 below:

[0132] Table 1

[0133]

[0134] The X-ray diffraction pattern of the ceramic material prepared in Example 1 is shown below. Figure 1 As shown, the ceramic material exhibits distinct diffraction peaks, indicating its good crystallinity; the scanning electron microscope (SEM) pattern is shown below. Figure 2 As shown, the surface of the ceramic material exhibits a polygonal granular structure, with the particles tightly packed together to form a dense microstructure, which improves the material's mechanical strength and thermal stability; the dielectric constant and dielectric loss change with temperature as shown in the graphs. Figure 3 As shown, the dielectric constant and dielectric loss exhibit excellent stability and reach their peak values ​​within a certain temperature range, indicating that the material possesses excellent dielectric properties within this temperature range; the hysteresis loop is as follows. Figure 4As shown, the hysteresis loop exhibits typical characteristics of ferroelectric materials, namely, the material becomes polarized under the influence of an electric field and retains a certain polarization state after the electric field is removed. This behavior is crucial for realizing an internal bias field and pinning ferroelectric domains, and helps to improve the material's mechanical quality factor Q. m .

[0135] Referring to Table 1, a comparison between Examples 1-10 and Comparative Example 1 shows that the embodiments of the present invention generate an internal bias field by doping with (1~2) at.% rare earth element Me, pinning ferroelectric domains, reducing domain activity, and improving the mechanical quality factor Q. m Increasing the dielectric constant to 3000, in Comparative Example 1, the absence of rare earth element doping leads to uneven grain size and the precipitation of a second phase at grain boundaries, resulting in an increase in dielectric constant but Q. m The decrease is manifested in enhanced domain reversibility and increased energy loss.

[0136] A comparison of Example 1 with Comparative Examples 2 and 3 shows that a Me₂O₃ doping amount of (1~2) at.% is more suitable. In Comparative Example 2, insufficient doping leads to inadequate lattice distortion and weak domain wall pinning, resulting in low Q. m The density decreased to approximately 2600; however, in Comparative Example 3, excessive doping caused second-phase precipitation and lattice stress concentration, reducing density and Q. m It dropped to approximately 2800.

[0137] As can be seen from the comparison between Example 1 and Comparative Example 4, Comparative Example 4 lacks Pb(Mg) 1 / 3 Ta 2 / 3 O3 weakens the relaxation characteristics inside the material, the dielectric peak becomes sharper, the temperature stability decreases, and the ferroelectric hysteresis loop is severely distorted, indicating that the synergistic effect of relaxation phase is destroyed.

[0138] As can be seen from the comparison between Example 1 and Comparative Example 5, Comparative Example 5 lacks Pb(Co) 1 / 3 Ta 2 / 3 At O3, the grains coarsen significantly, internal stress accumulates, polarization hysteresis intensifies, and the dielectric constant changes drastically with temperature. m It has dropped to around 2600.

[0139] A comparison between Example 1 and Comparative Example 6 shows that in Comparative Example 6, the lack of PbTiO3 significantly reduces the Curie temperature and leads to incomplete ferroelectric phase transformation, resulting in decreased polarizability and Q. m It dropped to 2600.

[0140] A comparison between Example 1 and Comparative Example 7 shows that in Comparative Example 7, x is greater than 0.4, the proportion of A-site components is too high, lattice distortion increases, some domain walls are excessively pinned, polarization reversal is hindered, dielectric loss increases, and Q... m It dropped to approximately 2800.

[0141] A comparison of Example 1 and Comparative Example 8 shows that in Comparative Example 8, when x is less than 0.05, the A-site composition is insufficient, the relaxation characteristics are not obvious, the grains are uneven, the dielectric response is reduced, and Q... m It dropped to approximately 2750.

[0142] Excessive values ​​of y and z can cause phase separation, while excessively small values ​​can suppress relaxation coupling. Therefore, the performance is better when the values ​​of x, y, and z are in the ranges of 0.05~0.4, 0.05~0.4, and 0.05~0.9, respectively. A comparison between Example 1 and Example 10 shows that, because Example 10 did not use a two-step sintering method, the sintering resulted in a decrease in density, insufficient grain boundary diffusion, and an increase in dielectric loss. m The temperature dropped to approximately 2850, indicating that the two-step sintering process can improve grain uniformity and mechanical quality.

[0143] The specific embodiments described above further illustrate the purpose, technical solution, and beneficial effects of the present invention. It should be understood that the above description is only a specific embodiment of the present invention and is not intended to limit the scope of protection of the present invention. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the scope of protection of the present invention.

Claims

1. A ceramic powder, characterized in that, The ceramic powder contains the chemical formula (1~2)at.%Me2O3-(1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3– (y)Pb(Sc) 2 / 3 W 1 / 3 Powder of O3-(z)PbTiO3; The element Me includes at least one of the following: La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc, and Y. x, y, z represent mole fractions, and 0.05≤x≤0.4, 0.05≤y≤0.4, 0.05≤z≤0.9, (1-xyz)>0.

2. A method for preparing ceramic powder as described in claim 1, characterized in that, Includes the following steps: S1: Prepare Me2O3 powder and Pb(Co) powder respectively. 1 / 3 Ta 2 / 3 O3 powder, Pb(Mg) 1 / 3 Ta 2 / 3 O3 powder, Pb(Sc) 2 / 3 W 1 / 3 O3 powder and PbTiO3 powder; S2: Preparation of (1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 )O3-(z)PbTiO3 powder; S3: Me2O3 powder is doped into the powder prepared in S2 to prepare (1~2)at.%Me2O3-(1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3– (y)Pb(Sc) 2 / 3 W 1 / 3 )O3-(z)PbTiO3 powder.

3. The method for preparing ceramic powder according to claim 2, characterized in that, The preparation process of the Me2O3 powder includes: mixing at least one of rare earth elements La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Sc, and Y, grinding with anhydrous ethanol as the medium for 30 to 40 hours, and drying at 80 to 120°C to obtain Me2O3 powder.

4. The method for preparing ceramic powder according to claim 2, characterized in that, The Pb(Co) 1 / 3 Ta 2 / 3 The preparation process of O3 powder includes: using CoCO3 and Ta2O5 as raw materials, sand milling with anhydrous ethanol as medium for 30-40 hours, drying and pre-calcining at 800-1200°C for 3-5 hours to synthesize CoTa2O6 powder. Then, using CoTa2O6 powder and Pb3O4 as raw materials, the mixture was milled in anhydrous ethanol for 30-40 hours, dried, and pre-calcined at 700-1100°C for 1-3 hours to synthesize Pb(Co) 1 / 3 Ta 2 / 3 )O3 powder.

5. The method for preparing ceramic powder according to claim 2, characterized in that, The Pb(Mg) 1 / 3 Ta 2 / 3 The preparation process of O3 powder includes: using MgCO3 and Ta2O5 as raw materials, grinding with anhydrous ethanol as medium for 30-40 hours, drying and pre-calcining at 800-1200°C for 3-5 hours to synthesize MgTa2O6 powder. Then, using MgTa2O6 powder and Pb3O4 as raw materials, the mixture was milled in anhydrous ethanol for 30-40 hours, dried, and pre-calcined at 700-1100°C for 1-3 hours to synthesize Pb(Mg) 1 / 3 Ta 2 / 3 )O3 powder.

6. The method for preparing ceramic powder according to claim 2, characterized in that, The Pb(Sc) 2 / 3 W 1 / 3 The preparation process of Sc2O3 powder includes: using Sc2O3 and WO3 as raw materials for mixing, sand milling with anhydrous ethanol as medium for 30-40 hours, drying and pre-calcining at 800-1200°C for 3-5 hours to synthesize Sc2WO6 powder; Then, using Sc2WO6 powder and Pb3O4 as raw materials, the mixture was milled in anhydrous ethanol for 30-40 hours, dried, and pre-calcined at 700-1100°C for 1-3 hours to synthesize Pb(Sc 2 / 3 W 1 / 3 )O3 powder.

7. The method for preparing ceramic powder according to claim 2, characterized in that, The preparation process of the PbTiO3 powder includes: using Pb3O4 and TiO2 as raw materials for batching, sand milling with anhydrous ethanol as medium for 1-3 hours, drying, and pre-calcining at 600-900°C for 1-3 hours to synthesize PbTiO3 powder.

8. The method for preparing ceramic powder according to claim 2, characterized in that, The preparation of (1-xyz)Pb(Co) as described in S2 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 The O3-(z)PbTiO3 powder is synthesized by mixing ingredients according to its chemical formula, sand milling with anhydrous ethanol as the medium for 11-13 hours, drying, and pre-calcining at 800-1000°C for 1-3 hours. The process of doping Me2O3 powder into the powder prepared in S2 as described in S3 includes: mixing Me2O3 powder with (1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 The O3-(z)PbTiO3 powder was sand-milled in anhydrous ethanol for 20-30 hours and then dried.

9. A method for preparing a ceramic material, characterized in that, The process includes the following steps: obtaining the ceramic powder as described in claim 1, and then... (1~2)at.%Me2O3-(1-xyz)Pb(Co) 1 / 3 Ta 2 / 3 O3–(x)Pb(Mg) 1 / 3 Ta 2 / 3 O3–(y)Pb(Sc) 2 / 3 W 1 / 3 PbTiO3 powder was mixed with 1-3 wt% PVA solution, granulated, and pressed into discs; The disc is kept at 600-700°C for 1-3 hours to remove PVA; The PVA-free discs are subjected to a two-step sintering method. The first step is to heat the discs to a sintering temperature of 1000~1350°C, and the second step is to cool them down to 900~1050°C and hold them for 2~4 hours. The sintered disc is processed into a smooth, thin sheet on both sides and coated with silver electrodes.

10. An application of a ceramic material, characterized in that, The ceramic material is prepared by the method described in claim 9 and is used in a high-intensity self-focusing ultrasound tumor treatment system.

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