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Mn을 첨가한 ZnO-TeO<sub>2</sub> 세라믹스의 소결과 전기적 특성
홍연우,신효순,여동훈,김종희,김진호,Hong, Youn-Woo,Shin, Hyo-Soon,Yeo, Dong-Hun,Kim, Jong-Hee,Kim, Jin-Ho 한국전기전자재료학회 2009 전기전자재료학회논문지 Vol.22 No.1
We investigated the sintering and electric properties of ZnO-1.0 at% $TeO_2$ (ZT1) and 1.0 at% Mn-doped ZT1(ZT1M1) system. $TeO_2$ itself melts at $732^{\circ}C$ in air but forms the $ZnTeO_3$ or $Zn_2Te_3O_8$ phase with ZnO as increasing temperature and therefore retards the densification of ZnO to $1000^{\circ}C$. In ZT1M1 system, also, the densification of ZnO was retarded up to $1000^{\circ}C$ and then reached > 90% of theoretical density above $1100^{\circ}C$. It was found that a good varistor characteristics(nonlinear coefficient $a{\sim}60$) were developed in ZT1M1 system sintered at $1100^{\circ}C$ due to Mn which known as improving the nonlinearity of ZnO varistors. The results of C-V characteristics such as barrier height (${\Phi}_b$), donor density ($N_D$), depletion layer (W), and interface state density ($N_t$) in ZT1M1 ceramics were $1.8{\times}10^{17}cm^{-3}$, 1.6 V, 93 nm, and $1.7{\times}10^{12}cm^{-2}$, respectively. Also we measured the resistance and capacitance of grain boundaries with temperature using impedance and electric modulus spectroscopy. It will be discussed about the stability and homogeneity of grain boundaries using distribution parameter ($\alpha$) simulated with the Z(T)"-logf plots.
홍연우,이영진,김세기,김진호,Hong, Youn-Woo,Lee, Young-Jin,Kim, Sei-Ki,Kim, Jin-Ho 한국재료학회 2012 한국재료학회지 Vol.22 No.12
We aimed to examine the co-doping effects of 1/6 mol% $Mn_3O_4$ and 1/4 mol% $Cr_2O_3$ (Mn:Cr = 1:1) on the reaction, microstructure, and electrical properties, such as the bulk defects and grain boundary properties, of ZnO-$Bi_2O_3-Sb_2O_3$ (ZBS; Sb/Bi = 0.5, 1.0, and 2.0) varistors. The sintering and electrical properties of Mn,Cr-doped ZBS, ZBS(MnCr) varistors were controlled using the Sb/Bi ratio. Pyrochlore ($Zn_2Bi_3Sb_3O_{14}$), ${\alpha}$-spinel ($Zn_7Sb_2O_{12}$), and ${\delta}-Bi_2O_3$ (also ${\beta}-Bi_2O_3$ at Sb/Bi ${\leq}$ 1.0) were detected for all of the systems. Mn and Cr are involved in the development of each phase. Pyrochlore was decomposed and promoted densification at lower temperature on heating in Sb/Bi = 1.0 system by Mn rather than Cr doping. A more homogeneous microstructure was obtained in all systems affected by ${\alpha}$-spinel. In ZBS(MnCr), the varistor characteristics were improved dramatically (non-linear coefficient, ${\alpha}$ = 40~78), and seemed to form ${V_o}^{\cdot}$(0.33 eV) as a dominant defect. From impedance and modulus spectroscopy, the grain boundaries can be seen to have divided into two types, i.e. one is tentatively assigned to ZnO/$Bi_2O_3$ (Mn,Cr)/ZnO (0.64~1.1 eV) and the other is assigned to the ZnO/ZnO (1.0~1.3 eV) homojunction.
ZnO-Zn<sub>2</sub>BiVO<sub>6</sub>-Co<sub>3</sub>O<sub>4</sub> 세라믹스의 액상소결과 전기적 특성
홍연우,김유비,백종후,조정호,정영훈,윤지선,박운익,Hong, Youn-Woo,Kim, You-Bi,Paik, Jong-Hoo,Cho, Jeong-Ho,Jeong, Young-Hun,Yun, Ji-Sun,Park, Woon-Ik 한국전기전자재료학회 2017 전기전자재료학회논문지 Vol.30 No.2
This study focuses on the effects of doping $Zn_2BiVO_6$ and $Co_3O_4$ on the sintering and electrical properties of ZnO; where, ZZ consists of 0.5 mol% $Zn_2BiVO_6$ in ZnO, and ZZCo consists of 1/3 mol% $Co_3O_4$ in ZZ. As ZnO was sintered at about $800^{\circ}C$, the liquid phases, which are composed of $Zn_2BiVO_6$ and $Zn_2BiVO_6$-rich phases, were found to be segregated at the grain boundaries of sintered ZZ and ZZCo, respectively, which demonstrates that $V_o^{\cdot}$(0.33~0.36 eV) are formed as dominant defects according to the analysis of admittance spectroscopy. As $Co_3O_4$ is doped to ZZ, the resistivity of ZnO decreases to ~38%, while donor density ($N_d$), interface state density ($N_t$), and barrier height (${\Phi}_b$) increase twice higher than those of ZZ, according to C-V characteristics. This result harbingers that ZZCo and its derivative compositions will open the gate for ZnO to be applied as more progressive varistors in the future, as well as the advantageous opportunity of manufacturing ZnO chip varistors at lower sintering temperatures below $900^{\circ}C$.
홍연우,이영진,김세기,김진호,Hong, Youn-Woo,Lee, Young-Jin,Kim, Sei-Ki,Kim, Jin-Ho 한국재료학회 2012 한국재료학회지 Vol.22 No.12
We have examined the co-doping effects of 1/2 mol% NiO and 1/4 mol% $Cr_2O_3$ (Ni:Cr = 1:1) on the reaction, microstructure, and electrical properties, such as the bulk defects and the grain boundary properties, of ZnO-$Bi_2O_3-Sb_2O_3$ (ZBS; Sb/Bi = 0.5, 1.0, and 2.0) varistors. The sintering and electrical properties of Ni,Cr-doped ZBS, ZBS(NiCr) varistors were controlled using the Sb/Bi ratio. Pyrochlore ($Zn_2Bi_3Sb_3O_{14}$), ${\alpha}$-spinel ($Zn_7Sb_2O_{12}$), and ${\delta}-Bi_2O_3$ were detected for all of compositions. For the sample with Sb/Bi = 1.0, the Pyrochlore was decomposed and promoted densification at lower temperature by Ni rather than by Cr. A homogeneous microstructure was obtained for all of the samples affected by ${\alpha}$-spinel. The varistor characteristics were not dramatically improved (non-linear coefficient, ${\alpha}$ = 5~24), and seemed to form ${Zn_i}^{{\cdot}{\cdot}}$(0.17 eV) and ${V_o}^{\cdot}$(0.33 eV) as dominant defects. From impedance and modulus spectroscopy, the grain boundaries were found to have been divided into two types, i.e., one is tentatively assigned to ZnO/$Bi_2O_3$ (Ni,Cr)/ZnO (0.98 eV) and the other is assigned to a ZnO/ZnO (~1.5 eV) homojunction.
홍연우,신효순,여동훈,김진호,Hong, Youn-Woo,Shin, Hyo-Soon,Yeo, Dong-Hun,Kim, Jin-Ho 한국전기전자재료학회 2011 전기전자재료학회논문지 Vol.24 No.12
In this study we aims to evaluate the effects of 1/3 mol% $Co_3O_4$ addition on the reaction, microstructure development, resultant electrical properties, and especially the bulk trap and grain boundary properties of $ZnO-Bi_2O_3-Sb_2O_3$ (Sb/Bi=2.0, 1.0, and 0.5) system (ZBS). The samples were prepared by conventional ceramic process, and characterized by XRD, density, SEM, I-V, impedance and modulus spectroscopy (IS & MS) measurement. In addition of $Co_3O_4$ in $ZnO-Bi_2O_3-Sb_2O_3$ (ZBSCo), the phase development, density, and microstructure were controlled by Sb/Bi ratio. Pyrochlore on cooling was reproduced in all systems. The more homogeneous microstructure was obtained in ZBSCo (Sb/Bi=1.0) system. In ZBSCo, the varistor characteristics were improved drastically (non-linear coefficient ${\alpha}$=23~50) compared to ZBS. Doping of $Co_3O_4$ to ZBS seemed to form $V^{\cdot}_o$(0.33 eV) as dominant defect. From IS & MS, especially the grain boundary of Sb/Bi=0.5 system is composed of electrically single barrier (0.93 eV) and somewhat sensitive to ambient oxygen with temperature.
ZnO-Bi<sub>2</sub>O<sub>3</sub>-Co<sub>3</sub>O<sub>4</sub> 바리스터의 전기적 특성
홍연우,신효순,여동훈,김진호,Hong, Youn-Woo,Shin, Hyo-Soon,Yeo, Dong-Hun,Kim, Jin-Ho 한국전기전자재료학회 2011 전기전자재료학회논문지 Vol.24 No.11
In this study, we have investigated the effects of Co doping on I-V curves, bulk trap levels and grain boundary characteristics of ZnO-$Bi_2O_3$ (ZB) varistor. From I-V characteristics the nonlinear coefficient (a) and the grain boundary resistivity (${\rho}_{gb}$) decreased as 32${\rightarrow}$22 and 18.4${\rightarrow}0.6{\times}10^9{\Omega}cm$ with sintering temperature (900~1,300$^{\circ}C$), respectively. Admittance spectra and dielectric functions show two bulk traps of zinc interstitial, $Zn_i^{{\cdot}{\cdot}}$(0.16~0.18 eV) and oxygen vacancy, $V_o^{{\cdot}}$ (0.28~0.33 eV). The barrier of grain boundaries in ZBCo (ZnO-$Bi_2O_3-Co_3O_4$) could be electrochemically single type. However, its thermal stability was slightly disturbed by ambient oxygen because the apparent activation energy of grain boundaries was changed from 0.93 eV at the 460~580 K to 1.13 eV at the 620~700 K. It is revealed that Co dopant in ZB reduced the heterogeneity of the barrier in grain boundaries and stabilized the barrier against the ambient temperature.
홍연우,이영진,김세기,김진호,Hong, Youn-Woo,Lee, Young-Jin,Kim, Sei-Ki,Kim, Jin-Ho 한국전기전자재료학회 2012 전기전자재료학회논문지 Vol.25 No.12
In this study, we have investigated the effects of Mn and Co co-doping on defects, J-E curves and grain boundary characteristics of ZnO-$Bi_2O_3$ (ZB) varistor. Admittance spectra and dielectric functions show two bulk defects of $Zn_i^{{\cdot}{\cdot}}$ (0.17~0.18 eV) and $V_o^{\cdot}$ (0.30~0.33 eV). From J-E characteristics the nonlinear coefficient (${\alpha}$) and resistivity (${\rho}_{gb}$) of pre-breakdown region decreased as 30 to 24 and 5.1 to 0.08 $G{\Omega}cm$ with sintering temperature, respectively. The double Schottky barrier of grain boundaries in ZB(MCo) ($ZnO-Bi_2O_3-Mn_3O_4-Co_3O_4$) could be electrochemically single type. However, its thermal stability was slightly disturbed by ambient oxygen because the apparent activation energy of grain boundaries was changed from 0.64 eV at lower temperature to 1.06 eV at higher temperature. It was revealed that a co-doping of Mn and Co in ZB reduced the heterogeneity of the barrier in grain boundaries and stabilized the barrier against an ambient temperature (${\alpha}$-factor= 0.136).
Mn<sub>3</sub>O<sub>4</sub> 함량에 따른 ZnO의 결함과 입계 특성
홍연우,신효순,여동훈,김진호,Hong, Youn-Woo,Shin, Hyo-Soon,Yeo, Dong-Hun,Kim, Jin-Ho 한국전기전자재료학회 2011 전기전자재료학회논문지 Vol.24 No.12
In this study, we investigated the effects of Mn dopant (0.1~3.0 at% $Mn_3O_4$ sintered at 1000$^{\circ}C$ for 1 h in air) on the bulk trap (i.e. defect) and grain boundary properties of ZnO, ZM(0.1~3.0) using admittance spectroscopy (AS), and impedance-modulus spectroscopy (IS & MS). As a result, three kinds of defect were found below the conduction band edge of ZnO as 0.09~0.14 eV (attractive coulombic center), 0.22~25 eV ($Zn^{{\cdot}{\cdot}}_i$), and 0.32~0.33 eV ($V^{\cdot}_o$). The oxygen vacancy increased with Mn doping. In ZM, an electrically single grain boundary as double Schottky barrier was formed with 0.82~1.0 eV of activation energies by IS & MS. We also find out that the barriers of grain boundary of Mn-doped ZnO (${\alpha}$-factor=0.13) were more stabilized and homogenized with temperature compared to pure ZnO.