B位Ce~(4+)掺杂对Sm_2Zr_2O_7组织结构及介电性能影响
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摘要
采用固相反应法制备了Sm_2(Zr_(1-x)Ce_x)_2O_7陶瓷材料,采用XRD和FT-IR技术分析了其晶体结构,用SEM技术分析了其显微组织,用阻抗仪测试其介电性能。结果表明,所制备Sm_2(Zr_(1-x)Ce_x)_2O_7陶瓷显微组织致密,晶粒大小比较均匀,晶界十分干净,并且Sm_2(Zr_(1-x)Ce_x)_2O_7陶瓷的相结构与掺杂量相关,Sm_2(Zr_(1-x)Ce_x)_2O_7(x=0,0.1)为焦绿石结构,Sm_2(Zr_(1-x)Ce_x)_2O_7(x=0.2,0.3,0.4)为萤石结构。Sm_2(Zr_(1-x)Ce_x)_2O_7陶瓷材料在B位大半径离子掺杂时,分子总极化率随掺杂量的增加而增大,介电常数和介电损耗随掺杂量的增加而增大。
The Sm_2(Zr_(1-x)Ce_x)_2O_7 ceramics were prepared by solid reaction method. The phase composition were analyzed by XRD and FT-IR technology, and the microstructure was observed by SEM technology. The dielectric constant was measured by an impedance meter. Results show that pure Sm_2(Zr_(1-x)Ce_x)_2O_7 ceramics were synthesized successfully. The grain size is relative even, the microstructure is dense and the grain boundaries are very clean. The phase structure of Sm_2(Zr_(1-x)Ce_x)_2O_7 ceramics is related to the doping amount. The phase structure of Sm_2Zr_2O_7 and Sm_2(Zr_(0.9)Ce_(0.1))_2O_7 ceramics are the pyrochlore structure, and other ceramics display the fluorite structure. The total polarizability of Sm_2(Zr_(1-x)Ce_x)_2O_7 ceramics increases with the increasing CeO_2 amount, and the dielectric constant and dielectric loss are also positive proportional to the doping amount.
The Sm_2(Zr_(1-x)Ce_x)_2O_7 ceramics were prepared by solid reaction method. The phase composition were analyzed by XRD and FT-IR technology, and the microstructure was observed by SEM technology. The dielectric constant was measured by an impedance meter. Results show that pure Sm_2(Zr_(1-x)Ce_x)_2O_7 ceramics were synthesized successfully. The grain size is relative even, the microstructure is dense and the grain boundaries are very clean. The phase structure of Sm_2(Zr_(1-x)Ce_x)_2O_7 ceramics is related to the doping amount. The phase structure of Sm_2Zr_2O_7 and Sm_2(Zr_(0.9)Ce_(0.1))_2O_7 ceramics are the pyrochlore structure, and other ceramics display the fluorite structure. The total polarizability of Sm_2(Zr_(1-x)Ce_x)_2O_7 ceramics increases with the increasing CeO_2 amount, and the dielectric constant and dielectric loss are also positive proportional to the doping amount.
引文
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[2]Wang Y F,Yang F,Xiao P.Glass-like thermal conductivities in(La1-x1Yx1)2(Zr1-x2Yx2)2O7-x2(x=x1+x2,0≤x≤1.0)solid solutions[J].Acta Mater,2012,60(20):7024-7033.
[3]Zhang Y H,Xie M,Zhou F,et al.Influence of Er substitution for La on the thermal conductivity of(La1-xErx)2Zr2O7 pyrochlores[J].Mater Res Bull,2015,64:175-181.
[4]M.Matsumoto,Development of plasma-sprayed thermal barrier coatings with low thermal conductivity and high oxidation resistance[J].J.Ceram.Soci.Japan,2007,115:11-123.
[5]Zhang H S,Liao S R,Yuan W,et al.Preparation and thermal conductivity of Y2Ce2O7 Ceramic material[J].Adv.Mater.Res.,2011,266:59-62.
[6]Song Z H,Ran L S,Kang G S.Preparation and thermal conductivity of Dy2Ce2O7 Ceramic material[J].J.Mater.Eng.Perf,2012,21:1046-1050.
[7]Song Z H,Gou L J,Gang L,et al.Investigation about thermo-physical properties of Ln2Ce2O7(Ln=Sm,Er and Yb)oxides for thermal barrier coatings[J].Mater Res.Bull,2012,47:4181-4186.
[8]Winter M R,Clarke D R.Oxide materials with low thermal conductivity[J].Acta Mater,2006,54:5051-5059.
[9]Cao X,Vassen R,Tietz F,et al.Lanthanum-ceriumoxide as a thermal barrier-coating material for hightemperature applications[J].Adv Mater,2003,15:1438-1442.
[10]Subramanian.M.A,Aravamudan.G and Subba Rao.G.V.Oxides pyrochlore-a review[J].Progress in Solid State Chem,1983,15:55-143.
[11]Elizabeth.J,Karl.R,Whittle,et al.Solid solubilities of(LaN d)2(ZrT i)2O7 phases deduced by neutron diffraction[J].J.Solid Chem,2005,178:800-810.
[12]JU-WOONG JANG,DAE-JOON KIM,DEUK YONGLEE.Size effect of trivalent oxides on low temperature phase stability of 2Y-TZP[J].J.Mater.Sci,2001,36:5391-5395.
[13]Lian.J,Wang.L.M,G.Haire.R,et al.Ion beam irradiation in La2Zr2O7-Ce2Zr2O7 pyrochlore[J].Nuclear Instru.Methods Phy.Res.B,2004,218:236-243.
[14]Withers.R.L,Thompson.J.G,Barlow.P.J.An electron and X-ray powder diffraction study of cubic fluoriterelated phase in various ZrO2-Ln2O3[J].J.Solid State Chem,1991,9(94):87-105.
[15]Withers.R.L,Thompson.J,G.Barlow.P.J,et al.A TEMstudy of superstructure ordering on either side of diphasic regions in some anion-deficent fluorite-ralated systems[J].J.Com-Assisted Microscopy,1992,12(4):315-317.
[16]Thomson.J.B,Armstrong.A.B,Bruce.P,et al.New class of pyrochlore solid solutions formed by chemical intercalation of oxygen[J].J.Amer.Chem.Soc,1996,11(118):111-129.
[17]Suda.A,Ukyo.Y,Sobukawa.H,et al.Improvement of oxygen storage capacity of CeO2-ZrO 2solid solution byheat treatment in reducing atmosphere[J].J.Ceram.Soc.Japan,2002,2(110):126-130.
[18]GongW.L,Lutze.W,Ewing.R.C.Zirconia ceramics for excess weapons plutonium waste[J].J.Nucear Mater.,2000,277:239-249.
[19]Omata.T,Kishimoto.H,Matsuo.S.O.Y,et al.Virbrational spectroscopic and X-ray diffraction studies of cerium zirconium oxides with Ce/Zr composition ratio=1 preparedby reduction and successive oxidation of t’-(Ce0.5Zr0.5)O2phase[J].J.Solid State Chem,1999,11(147):573-583
[20]Chaudhuri S P,Sarkar P.Dielectri behavior of porcelain in relation constitution[J].Ceram.Inter.,2000,26:865-875.
[21]Elkholy M M,Sharaf El-Deen L M.The dielectric properties of TeO2-P2O5 glasses[J].Mater.Chem.Phys.,2000,65:192-196.
[22]Du H L,Yao X.Dielectric relaxtion characteristics of bismuth zinc niobate pyrochlores containing titanium[J].Phys.B,2002,324:121-126.
[23]Ravinder D,Ranga M G,Sagar D R.High frequency dielectric behaviour of aluminium-substituted lithium ferrites[J].Mater.Lett.,2000,44:256-260.
[24]游效曾.离子的极化率[J].科学通报,1974,19(9):419-423.
[25]PAULING L.The theoretical prediction of the physical properties of mang-electron atoms and ion[J].Proc Roy Soc(A),1927,114:191.