二氧化鈦基高介電陶瓷的制備及物性研究
發(fā)布時(shí)間：2018-12-18 12:57
【摘要】：高介電材料是電容器、存儲(chǔ)器、諧振器、濾波器等重要電子器件向高性能化和尺寸微型化進(jìn)一步發(fā)展的重要基礎(chǔ)。由于器件小型化和高能量密度存儲(chǔ)的應(yīng)用需要,對(duì)高介電材料的探索是近年國(guó)內(nèi)外新材料研究領(lǐng)域的一個(gè)熱點(diǎn)。然而,在單一材料中同時(shí)實(shí)現(xiàn)高介電性、低損耗、工作頻帶寬、溫度穩(wěn)定和可耐強(qiáng)電場(chǎng)的優(yōu)異綜合介電性能仍然是一項(xiàng)極其具有挑戰(zhàn)性的任務(wù)。在此背景下,本論文主要開展了(In, Nb)摻雜Ti02高介電陶瓷材料的制備、物性及相關(guān)機(jī)理的研究。Ti02陶瓷作為研究最早的介電材料,具有較高的相對(duì)介電常數(shù)、低的介電損耗、低的電導(dǎo)率以及非常高的抗擊穿電場(chǎng)強(qiáng)度。因此,Ti02基陶瓷材料對(duì)于高儲(chǔ)能密度電容器的應(yīng)用是一類具有非常重要的研究?jī)r(jià)值和意義的介質(zhì)材料。近期,澳大利亞國(guó)立大學(xué)的研究組報(bào)道了(In, Nb)共摻雜TiO2等組分陶瓷具有良好的高介電性質(zhì),該研究組在低于實(shí)驗(yàn)測(cè)量頻率1 MHz的范圍內(nèi)同時(shí)實(shí)現(xiàn)了介電常數(shù)δ≥104、介電損耗tanδ≤0.05的性能,并且在80K至450K很寬的溫度范圍內(nèi)呈現(xiàn)出不怎么依存溫度和頻率的高介電常數(shù)和低的介電損耗。我們知道純TiO2的介電常數(shù)只有120左右,而進(jìn)行了(In, Nb)摻雜改性后介電常數(shù)提高到104,并且損耗保持在0.05以下,這極大的提高了TiO2的介電性能。雖然(In, Nb)摻雜后陶瓷呈現(xiàn)出如此高介電常數(shù)的物理機(jī)制尚存在一定爭(zhēng)議,但這一成果的發(fā)現(xiàn)對(duì)研究具有優(yōu)異介電性能的材料提供了一條新的途徑。本論文研究了利用傳統(tǒng)固相反應(yīng)法制備的(In, Nb)摻雜Ti02陶瓷樣品。考察了不同組分摻雜的陶瓷介電性質(zhì)以及燒結(jié)工藝、球磨時(shí)間對(duì)其介電性質(zhì)的影響,并初步探索了陶瓷的高介電性質(zhì)的物理機(jī)制。一、利用固相反應(yīng)法制備了一系列不同燒結(jié)溫度條件的(In, Nb)摻雜Ti02陶瓷樣品,系統(tǒng)地考察了它們的晶體結(jié)構(gòu)、微觀組織結(jié)構(gòu)、介電頻譜和復(fù)阻抗頻譜的電學(xué)性質(zhì)及其隨測(cè)試溫度的變化。首先利用普通燒結(jié)制備的陶瓷樣品的介電常數(shù)隨摻雜組分、燒結(jié)溫度、保溫時(shí)間都有一定規(guī)律性的變化,并且都具有極高的介電常數(shù)。但這種方法制備的樣品重復(fù)性較差,大部分陶瓷樣品的介電損耗低頻和高頻都在10%以上,只有中頻段損耗較低。為了能保證高介電常數(shù)的同時(shí)降低樣品的損耗,我們利用等靜壓成型燒結(jié)制備樣品,在通過熱處理后其介電性能得到了很大改善,尤其在800℃C退火樣品的介電性能最好。其介電常數(shù)在10 mHz～10 MHz都穩(wěn)定保持在104以上,并且介電損耗在很寬的頻率范圍內(nèi)都小于5%,另外隨測(cè)試溫度的變化其介電常數(shù)也基本不變,顯示了良好的溫度穩(wěn)定性。綜合來說,通過等靜壓成型燒結(jié)后退火處理的樣品各方面的介電性能都非常優(yōu)異。二、研究了一些(In, Nb)摻雜TiO2陶瓷呈現(xiàn)高介電常數(shù)的影響因素,對(duì)其高介電性起源的物理機(jī)制進(jìn)行初步探究。通過不等比例摻雜實(shí)驗(yàn),發(fā)現(xiàn)過量的In和Nb都會(huì)對(duì)陶瓷的介電性能產(chǎn)生影響,過量摻雜In會(huì)使陶瓷的介電常數(shù)和介電損耗降低,而過量的Nb會(huì)使陶瓷介電常數(shù)和損耗增大。作者推測(cè)只有In和Nb等比例摻雜才會(huì)出現(xiàn)高介電常數(shù)低損耗的陶瓷樣品。通過表面處理實(shí)驗(yàn),發(fā)現(xiàn)進(jìn)行表面處理后的樣品,介電常數(shù)急劇增大了一個(gè)數(shù)量級(jí),再經(jīng)過退火后陶瓷的介電常數(shù)又恢復(fù)到較低的數(shù)值,可以推測(cè)陶瓷的介電常數(shù)與表面氧化層的氧化程度有關(guān)。三、探討了不同球磨時(shí)間對(duì)陶瓷介電性能的影響。通過分析球磨前后粉料的SEM圖片看出球磨時(shí)間延長(zhǎng)粉料分散的更均勻,XRD圖譜也顯示沒有混入大量Zr02雜質(zhì)。對(duì)于球磨30 h的粉料,在不同燒結(jié)溫度樣品的介電頻譜測(cè)試發(fā)現(xiàn),其最佳燒結(jié)溫度為1400℃,另外測(cè)試了樣品變溫的介電頻譜和阻抗譜顯示了其介電性能在測(cè)試溫度范圍內(nèi)介電性能比較穩(wěn)定,這也是(In, Nb)摻雜Ti02這類陶瓷共有的一個(gè)規(guī)律。
[Abstract]:High dielectric material is an important base for the further development of high-performance and small-scale miniaturization of important electronic devices such as capacitors, memory, resonators, filters and the like. Due to the need of device miniaturization and high energy density storage, the exploration of high dielectric materials is a hot spot in the field of new material research in recent years. However, the excellent comprehensive dielectric properties of high dielectric, low loss, wide working band, temperature stability and strong electric field are still an extremely challenging task in a single material. In this paper, the preparation, physical properties and related mechanism of (In, Nb) doped Ti02 high dielectric ceramic materials are studied. As the earliest dielectric material, Ti02 ceramics have high relative dielectric constant, low dielectric loss, low electrical conductivity and very high resistance to electric field strength. Therefore, the application of Ti02-based ceramic materials to high-energy-storage-density capacitors is a kind of medium material with very important research value and significance. Recently, the study group of the Australian National University has reported that (In, Nb) co-doped TiO2 and other component ceramics have good dielectric properties, and the study group has realized the performance of the dielectric constant, the dielectric constant, the dielectric constant, the dielectric loss tan and the dielectric constant of 0.05 in the range below the experimental measurement frequency of 1 MHz. and exhibit a high dielectric constant and a low dielectric loss that are less dependent on temperature and frequency over a wide temperature range of 80k to 450k. We know that the dielectric constant of the pure TiO2 is about 120, and the dielectric constant is increased to 104 after (In, Nb) doping modification, and the loss is kept below 0.05, which greatly improves the dielectric property of the TiO2. Although (In, Nb) doped ceramic exhibits such a high dielectric constant, the physical mechanism is still controversial, but the discovery of this result provides a new way for the study of materials with excellent dielectric properties. In this paper, the (In, Nb) doped Ti02 ceramic samples prepared by the conventional solid-phase reaction method are studied. The influence of different component-doped ceramic dielectric properties as well as the sintering process and ball-milling time on the dielectric properties of the ceramics was investigated, and the physical mechanism of the high dielectric properties of the ceramics was preliminarily explored. In this paper, a series of (In, Nb) doped Ti02 ceramic samples with different sintering temperature conditions were prepared by solid-phase reaction, and their crystal structure, microstructure, dielectric and complex impedance spectra were systematically investigated. firstly, the dielectric constant of the ceramic sample prepared by ordinary sintering has a certain regular change with the doping component, the sintering temperature and the heat preservation time, and the ceramic sample has a very high dielectric constant. but the repeatability of the samples prepared by the method is poor, and the dielectric loss and the high frequency of a large part of the ceramic samples are more than 10%, and only the middle frequency band is low in loss. In order to ensure the high dielectric constant, the loss of the sample can be reduced, and the sample is prepared by isostatic pressing and sintering, and the dielectric property of the sample is greatly improved after the heat treatment, and the dielectric property of the sample is best in particular at the temperature of 800 DEG C. the dielectric constant is stable at 10mHz-10MHz, and the dielectric loss is less than 5% in a wide frequency range, and the dielectric constant of the dielectric constant is basically unchanged with the change of the test temperature, and good temperature stability is displayed. In general, the dielectric properties of each aspect of the sample treated by isostatic pressing are excellent. In this paper, the influence factors of high dielectric constant of (In, Nb) doped TiO2 ceramics are studied, and the physical mechanism of high dielectric constant of the (In, Nb) doped TiO2 ceramics is studied. In addition, the dielectric constant and dielectric loss of the ceramic can be reduced by the overdoping of In, and the dielectric constant and the loss of the ceramic can be increased. The authors speculate that only in-and-Nb-ratio doping results in high dielectric constant low-loss ceramic samples. The surface treatment experiment shows that the dielectric constant of the sample after surface treatment is increased by an order of magnitude, and the dielectric constant of the ceramic is restored to a lower value after the annealing, and the dielectric constant of the ceramic can be presumed to be related to the degree of oxidation of the surface oxide layer. The effect of different ball milling time on the dielectric properties of the ceramic was discussed. Through the analysis of the SEM pictures of the powder before and after the ball milling, it can be seen that the grinding time of the ball is more uniform than that of the powder, and the XRD pattern also shows that no large amount of the Zr02 impurity is mixed. For the powder of the ball mill for 30 h, the optimum sintering temperature is 1400 鈩，
本文編號(hào)：2385883
[Abstract]:High dielectric material is an important base for the further development of high-performance and small-scale miniaturization of important electronic devices such as capacitors, memory, resonators, filters and the like. Due to the need of device miniaturization and high energy density storage, the exploration of high dielectric materials is a hot spot in the field of new material research in recent years. However, the excellent comprehensive dielectric properties of high dielectric, low loss, wide working band, temperature stability and strong electric field are still an extremely challenging task in a single material. In this paper, the preparation, physical properties and related mechanism of (In, Nb) doped Ti02 high dielectric ceramic materials are studied. As the earliest dielectric material, Ti02 ceramics have high relative dielectric constant, low dielectric loss, low electrical conductivity and very high resistance to electric field strength. Therefore, the application of Ti02-based ceramic materials to high-energy-storage-density capacitors is a kind of medium material with very important research value and significance. Recently, the study group of the Australian National University has reported that (In, Nb) co-doped TiO2 and other component ceramics have good dielectric properties, and the study group has realized the performance of the dielectric constant, the dielectric constant, the dielectric constant, the dielectric loss tan and the dielectric constant of 0.05 in the range below the experimental measurement frequency of 1 MHz. and exhibit a high dielectric constant and a low dielectric loss that are less dependent on temperature and frequency over a wide temperature range of 80k to 450k. We know that the dielectric constant of the pure TiO2 is about 120, and the dielectric constant is increased to 104 after (In, Nb) doping modification, and the loss is kept below 0.05, which greatly improves the dielectric property of the TiO2. Although (In, Nb) doped ceramic exhibits such a high dielectric constant, the physical mechanism is still controversial, but the discovery of this result provides a new way for the study of materials with excellent dielectric properties. In this paper, the (In, Nb) doped Ti02 ceramic samples prepared by the conventional solid-phase reaction method are studied. The influence of different component-doped ceramic dielectric properties as well as the sintering process and ball-milling time on the dielectric properties of the ceramics was investigated, and the physical mechanism of the high dielectric properties of the ceramics was preliminarily explored. In this paper, a series of (In, Nb) doped Ti02 ceramic samples with different sintering temperature conditions were prepared by solid-phase reaction, and their crystal structure, microstructure, dielectric and complex impedance spectra were systematically investigated. firstly, the dielectric constant of the ceramic sample prepared by ordinary sintering has a certain regular change with the doping component, the sintering temperature and the heat preservation time, and the ceramic sample has a very high dielectric constant. but the repeatability of the samples prepared by the method is poor, and the dielectric loss and the high frequency of a large part of the ceramic samples are more than 10%, and only the middle frequency band is low in loss. In order to ensure the high dielectric constant, the loss of the sample can be reduced, and the sample is prepared by isostatic pressing and sintering, and the dielectric property of the sample is greatly improved after the heat treatment, and the dielectric property of the sample is best in particular at the temperature of 800 DEG C. the dielectric constant is stable at 10mHz-10MHz, and the dielectric loss is less than 5% in a wide frequency range, and the dielectric constant of the dielectric constant is basically unchanged with the change of the test temperature, and good temperature stability is displayed. In general, the dielectric properties of each aspect of the sample treated by isostatic pressing are excellent. In this paper, the influence factors of high dielectric constant of (In, Nb) doped TiO2 ceramics are studied, and the physical mechanism of high dielectric constant of the (In, Nb) doped TiO2 ceramics is studied. In addition, the dielectric constant and dielectric loss of the ceramic can be reduced by the overdoping of In, and the dielectric constant and the loss of the ceramic can be increased. The authors speculate that only in-and-Nb-ratio doping results in high dielectric constant low-loss ceramic samples. The surface treatment experiment shows that the dielectric constant of the sample after surface treatment is increased by an order of magnitude, and the dielectric constant of the ceramic is restored to a lower value after the annealing, and the dielectric constant of the ceramic can be presumed to be related to the degree of oxidation of the surface oxide layer. The effect of different ball milling time on the dielectric properties of the ceramic was discussed. Through the analysis of the SEM pictures of the powder before and after the ball milling, it can be seen that the grinding time of the ball is more uniform than that of the powder, and the XRD pattern also shows that no large amount of the Zr02 impurity is mixed. For the powder of the ball mill for 30 h, the optimum sintering temperature is 1400 鈩，
本文編號(hào)：2385883
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