采用改进的柠檬酸法合成了Sc掺杂的锰酸锶镧(LSM)材料(LSMS), 即La0.8Sr0.2Mn1-xScxO3±δ (简写为LSMSx, x=0, 0.02, 0.05和0.1)复合氧化物. 采用X射线衍射(XRD)、程序升温还原(H2-TPR)及电化学方法分别对合成材料的结构、还原行为及以LSMSx-YSZ(即LSMSx与8%Y2O3掺杂的ZrO2复合物)为阴极的中温固体氧化物燃料电池的性能进行了表征. XRD结果表明,在焙烧温度900 ℃、 Sc掺杂量较低(x<0.1)时LSMS材料能形成纯钙钛矿结构,随着掺杂量和焙烧温度提高, LSMS发生了不同程度的Sc2O3偏析现象. H2-TPR结果表明,焙烧温度对材料还原峰的形状和温度影响较大. 由于Sc的掺杂以及Sc2O3的析出在样品结构中引入了结构缺陷,提高了LSMS中Mn4+和氧空位的浓度,加快了体相氧的迁移,改善了材料的还原性. 但是随着Sc含量和焙烧温度提高, Sc掺杂对样品的还原活性改善不明显,这是由于Sc2O3偏析量增加引起的. 电化学方法表征结果表明, LSMSx-YSZ复合阴极电池性能受Sc掺杂量、操作温度及阴极焙烧温度的影响. 在本研究的掺杂范围内, Sc的掺杂显著提高了LSM基阴极低温操作的性能. 这主要是由于Sc掺杂LSMS-YSZ复合阴极中氧空位的数目增加,导致阴极对氧还原反应的电化学活性提高,改善了LSM基阴极由于氧空位不足引起低温下极化损失严重的问题.
参考文献
[1] | Tsai T.;Barnett SA. .INCREASED SOLID-OXIDE FUEL CELL POWER DENSITY USING INTERFACIAL CERIA LAYERS[J].Solid state ionics,1997(3/4):191-196. |
[2] | Chen K F;Lü Z;Ai N;Chen X J Hu J Y Huang X Q Su W H .[J].Journal of Power Sources,2007,167(01):84. |
[3] | 张敏 .[D].大连:中国科学院大连化学物理研究所,2008. |
[4] | Dusastre V.;Kilner J.A. .Optimisation of composite cathodes for intermediate temperature SOFC applications[J].Solid state ionics,1999(1/2):163-174. |
[5] | Duan Z S;Yang M;Yan A;Hou Z F Dong Y L Cong Y Cheng M J Yang W S .[J].Journal of Power Sources,2006,160(01):57. |
[6] | 段枣树,闫爱宇,董永来,丛铀,程谟杰,杨维慎.Ba0.5Sr0.5Co0.8Fe0.2O3-δ为阴极的中温固体氧化物燃料电池[J].催化学报,2005(10):829-831. |
[7] | Xia CR.;Rauch W.;Chen FL.;Liu ML. .Sm0.5Sr0.5CoO3 cathodes for low-temperature SOFCs[J].Solid state ionics,2002(1/2):11-19. |
[8] | Carter S;Selcuk A;Chater R J;Kajda J Kilner J A Steele B C H .[J].Solid State Ionics,1992,53-56:597. |
[9] | Huang Y Y;Vohs J M;Gorte R J .[J].Journal of the Electrochemical Society,2006,153(06):A951. |
[10] | M. Petitjean;G. Caboche;E. Siebert .(La_(0.8)Sr_(0.2))(Mn_(1-y)Fe_y)O_(3+ - theta) oxides for ITSOFC cathode materials? Electrical and Ionic transport properties[J].Journal of the European Ceramic Society,2005(12):2651-2654. |
[11] | Porta P;De Rossi S;Faticanti M;Minelli G Pettiti I Lisi L Turco M .[J].Journal of Solid State Chemistry,1999,146(02):291. |
[12] | Lisi L;Bagnasco G;Ciambelli P;De Rossi S Porta P Russo G Turco M .[J].Journal of Solid State Chemistry,1999,146(01):176. |
[13] | Pena M A;Fierro J L G .[J].Chemical Reviews,2001,101(07):1981. |
[14] | Bell RJ.;Drennan J.;Millar GJ. .Influence of synthesis route on the catalytic properties of La1-xSrxMnO3[J].Solid state ionics,2000(3/4):211-220. |
[15] | Irusta S.;Menendez M.;Santamaria J.;Pina MP. .Catalytic combustion of volatile organic compounds over La-based perovskites[J].Journal of Catalysis,1998(2):400-412. |
[16] | Cimino S;Colonna S;De Rossi S;Faticanti M Lisi L Pettiti I Porta P .[J].Journal of Catalysis,2002,205(02):309. |
[17] | Mizusaki J.;Takai H.;Yonemura Y.;Minamiue H.;Tagawa H. Dokiya M.;Inaba H.;Naraya K.;Sasamoto T.;Hashimoto T.;Mori N. .Oxygen nonstoichiometry and defect equilibrium in the perovskite-type oxides La1-xSrxMnO3+d[J].Solid state ionics,2000(1/4):163-177. |
[18] | Pai M R;Wani B N;Sreedhar B;Singh S Gupta N M .[J].Journal of Molecular Catalysis A:Chemical,2006,246(1-2):128. |
[19] | Wang W;Zhang H B;Lin G D;Xiong Z T .[J].Applied Catalysis B:Environmental,2000,24(3-4):219. |
[20] | Yasuda I.;Hishinuma M.;Kawada T.;Dokiya M.;Ogasawara K. .OXYGEN TRACER DIFFUSION COEFFICIENT OF (LA,SR)MNO3+/-DELTA[J].Solid state ionics,1996(2):1197-1201. |
[21] | Nowotny J.;Rekas M. .Defect chemistry of (La,Sr)MnO3[J].Journal of the American Ceramic Society,1998(1):67-80. |
[22] | Desouza S.;Dejonghe LC.;Visco SJ. .THIN-FILM SOLID OXIDE FUEL CELL WITH HIGH PERFORMANCE AT LOW-TEMPERATURE[J].Solid state ionics,1997(1/2):57-61. |
[23] | Barbucci A;Viviani M;Carpanese P;Vladikova D Stoynov Z .[J].Electrochimica Acta,2006,51(8-9):1641. |
[24] | Zhang M;Yang M;Liu B;Hou Z F Dong Y L Cheng M J .[J].Journal of Power Sources,2008,175(02):739. |
[25] | Wang ZW;Cheng MJ;Dong YL;Zhang M;Zhang HM .Investigation of LSM1.1-ScSZ composite cathodes for anode-supported solid oxide fuel cells[J].Solid state ionics,2005(35/36):2555-2561. |
[26] | Murray EP.;Barnett SA. .(La,Sr) MnO3-(Ce,Gd)O2-x composite cathodes for solid oxide fuel cells[J].Solid state ionics,2001(3/4):265-273. |
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