Ba 2+和In 3+共掺杂硅酸镧固体电解质的制备及性能
收稿日期: 2019-08-08
网络出版日期: 2020-02-26
基金资助
国家自然基金项目(51672080);国家自然基金项目(51472073)
Preparation and performance of Ba 2+ and In 3+ co-doped lanthanum oxyapatite solid electrolyte
Received date: 2019-08-08
Online published: 2020-02-26
采用高温固相法制备磷灰石型硅酸镧陶瓷La9.4Ba0.6Si6-xInxO27-δ（x=0,0.1,0.2,0.3,0.4）。采用XRD、SEM和拉曼光谱等测试分析手段表征了La9.4Ba0.6Si6-xInxO27-δ固体电解质掺杂体系的相组成和微观形貌特征;采用交流阻抗谱测试研究了La9.4Ba0.6Si6-xInxO27-δ掺杂体系在不同温度下的电导率变化规律。研究发现,所有La9.4Ba0.6Si6-xInxO27-δ陶瓷试样的结晶度良好且均具有氧基磷灰石结构;仅在La位掺杂Ba 2+时,La9.4Ba0.6Si6O27-δ试样晶粒形貌不规则,In 3+掺杂后晶粒呈等轴状均匀生长。各个试样的总电导率与测试温度之间符合Arrhenius关系。In 3+最佳掺杂量x为0.2,此时La9.4Ba0.6Si5.8In0.2O27-δ陶瓷具有最高的电导率,其电导率（1 073 K）、活化能和指前因子分别为5.08×10 -3 S/cm、0.86 eV和2.91×10 11 S·K/cm。
赵艳琴 , 闫书山 , 王岭 , 曹吉林 . Ba 2+和In 3+共掺杂硅酸镧固体电解质的制备及性能[J]. 无机盐工业, 2020 , 52(1) : 49 -53 . DOI: 10.11962/1006-4990.2019-0116
Apatite-type lanthanum silicate ceramic La9.4Ba0.6Si6-xInxO27-δ（x=0,0.1,0.2,0.3,0.4） were synthesized by the high-temperature solid-phase reaction method.The phase composition and microstructure characteristics of the La9.4Ba0.6Si6-xInxO27-δ solid electrolyte doped system were characterized by XRD,SEM and Raman spectrum.The change law of conductivity at different temperatures of La9.4Ba0.6Si6-xInxO27-δ were studied by AC impedance spectroscopy test.It was found that all the ceramic samples of La9.4Ba0.6Si6-xInxO27-δ had good crystallinity and oxygen radicals apatite structure.The grain shape of La9.4Ba0.6Si6O27-δ sample only doping Ba 2+ in La was irregular.The grain of the samples grew evenly in uniform axis after doped by In 3+.There was Arrhenius behavior between total conductivity of all samples and test temperatures.The optimal doping amount x of In 3+ was 0.2.La9.4Ba0.6Si5.8In0.2O27-δ ceramic had the highest conductivity.The conductivity（1 073 K）,activation energy and former factors were 5.08×10 -3 S/cm,0.86 eV and 2.91×10 11 S·K/cm,respectively.
| [1] | 韩炳旭, 王岭, 戴磊 , 等. 磷灰石型硅酸镧基氧离子导体研究进展[J]. 功能材料, 2013,44(S1):21-27. |
| [2] | 田立朋, 任志华 . 磷灰石结构硅酸镧氧离子导体的研究进展[J]. 材料导报, 2012,26(z1):216-219. |
| [3] | Zhang Lan, He Hongquan, Wu Hongwei , et al. Synjournal and characterization of doped La9ASi6O26.5(A=Ca、Sr、Ba) oxyapatite electrolyte by a water-based gel-casting route[J]. International Journal of Hydrogen Energy, 2011,36(11):6862-6874. |
| [4] | Xiang Jun, Liu Zhanguo, Ouyang Jiahu , et al. Synjournal,structure and electrical properties of rare-earth doped apatite-type lanthanum silicates[J]. Electrochemical Acta, 2012,65:251-256. |
| [5] | Yuan Wenhui, Shen Rongping, Li Li . Synjournal and conductivity of oxyapatite ionic conductor La10-xVx(SiO4)6O3+x[J]. Chinese Journal of Chemical Engineering, 2010,18(2):328-332. |
| [6] | Feng Yadi, Dai Lei, Meng Wei , et al. Microstructure and electrical conductivity of alkaline elements doped apatite-type La10Si6O27 electrolytes[J]. Ceramics International, 2017,43(1):289-295. |
| [7] | Xiang Jun, Liu Zhanguo, Ouyang Jiahu , et al. Synjournal and electrical conductivity of La10Si5.5B0.5O27+δ(B=In,Si,Sn,Nb) ceramics[J]. Solid State Ionics, 2012,220:7-11. |
| [8] | Yin G C, Yin H, Wang X , et al. Mg doping effect on high-pressure behaviors of apatite-type lanthanum silicate[J]. J.Alloys Comp., 2014,611:24-29. |
| [9] | Shi Q, Lu L, Jin H , et al. Electrical properties and thermal expansion of cobalt doped apatite-type lanthanum silicates based electrolytes for IT-SOFC[J]. Mater.Res.Bull., 2012,47:719-723. |
| [10] | Cao X G, Jiang S P . Sinterability and conductivity of barium doped aluminium lanthanum oxyapatite La9.5Ba0.5Si5.5Al0.5O26.5 electrolyte of solid oxide fuel cells[J]. J.Alloys Comp., 2012,523:127-133. |
| [11] | Cao X G, Jiang S P . Effect of Sr and Al or Fe co-doping on the sinterability and conductivity of lanthanum silicate oxyapatite electrolytes for solid oxide fuel cells[J]. Int.J.Hydrogen Energy, 2014,39:19093-19101. |
| [12] | Cao X G, Jiang S P, Li Y Y . Synjournal and characterization of calcium and iron co-doped lanthanum silicate oxyapatites by sol-gel process for solid oxide fuel cells[J]. J.Power Sources, 2015,293:806-814. |
| [13] | Dai Lei, Han Wen, Li Yuehua , et al. Synjournal and characterization of Al 3+ and M (M =W 6+,In 3+,Nb 5+,Mg 2+) co-doped lanthanum silicate oxy-apatite electrolytes [J]. International Journal of Hydrogen Energy, 2016,41(26):11340-11350. |
| [14] | Nojiri Y, Tanase S, Iwasa M , et al. Ionic conductivity of apatite-type solid electrolyte material,La10-xBaxSi6O27-x/2(x=0-1),and its fuel cell performance[J]. J.Power Sources, 2010,195:4059-4064. |
| [15] | 相珺 . 阳离子掺杂氧基磷灰石型硅酸镧的组织结构与电学性能[D]. 哈尔滨:哈尔滨工业大学, 2013. |
| [16] | 周勇华, 方莹, 李镇 , 等. 铁位掺杂对磷酸铁锂电化学性能的影响[J]. 无机盐工业, 2014,46(3):75-78. |
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