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采用固相反应法成功制备了(La1-x Ndx )5.5 WO12-δ(x=1/3,1/2)质子-电子混合导体.运用 X射线衍射仪(XRD)、扫描电子显微镜(SEM)分别对试样的物相结构、微观形貌进行了表征.测试了试样在湿润CO2气氛中的化学稳定性,应用交流阻抗法测定了其在空气和湿润5% H 2/Ar 气氛中的电导率,并研究了试样在不同温度、不同氢分压下的透氢量.结果表明,(La1-xNdx)5.5 WO12-δ(x=1/3,1/2)经1550℃烧结后均形成立方萤石结构的致密烧结体;试样在800℃湿润CO2气氛中均表现出良好的化学稳定性;试样在湿润5% H 2/Ar 气氛下的电导率明显高于空气气氛,在湿润5% H2/Ar 气氛中850℃时,(La1/2 Nd1/2)5.5 WO12-δ的电导率达到6.58×10-3 S/cm;在900℃、50% H2/N2时,厚度为1.56 mm 的(La1/2 Nd1/2)5.5 WO12-δ透氢膜获得最大透氢量为0.079 mL/(min?cm2).

Mixed proton-electron conductors of (La1-xNdx)5.5 WO12-δ(x=1/3,1/2)were successfully synthe-sized by the solid state reaction route.The phase composition and microstructures of the samples were investiga-ted by XRD and SEM,respectively.Chemical stability against humid CO2 was tested.The total conductivities of the samples in air and wet 5% H2/Ar atmospheres were measured by the AC impedance spectroscopy.Hydro-gen permeation performance of the membranes was tested at different temperatures and hydrogen partial pres-sures.The results indicate that the samples sintered at 1 550 ℃ were cubic fluorite structure and the samples were extremely dense.The samples are quite stable in humid CO2 atmosphere.The samples have higher conduc-tivities in wet 5% H2/Ar and (La1/2 Nd1/2 )5.5 WO12-δpresents a high conductivity in wet 5% H2/Ar,which was about 6.58×10-3 S/cm at 850 ℃.Using 50% H2/N2 as feed gas,the highest hydrogen flux for (La1/2 Nd1/2 )5.5 WO12-δmembrane with thickness of 1.56 mm was 0.079 mL/(min??cm2)at 900 ℃.

参考文献

[1] Shimura T.;Iwahara H.;Fujimoto S. .Proton conduction in non-perovskite-type oxides at elevated temperatures[J].Solid state ionics,2001(1):117-123.
[2] Haugsrud R .Defects and transport properties in Ln(6)WO(12) (Ln = La, Nd, Gd, Er)[J].Solid state ionics,2007(7/10):555-560.
[3] Sonia Escolastico;Vicente B. Vert;Jose M. Serra .Preparation and Characterization of Nanocrystalline Mixed Proton-Electronic Conducting Materials Based on the System Ln6WO_(12)[J].Chemistry of Materials: A Publication of the American Chemistry Society,2009(14):3079-3089.
[4] Ragnhild Hancke;Zuoan Li;Reidar Haugsrud .Thermogravimetric relaxation study of the proton conductor lanthanum tungstate, La_(28-x)W_(4+x)O_(54+δ)V_(2-δ), x = 0.85[J].International journal of hydrogen energy,2012(9):8043-8050.
[5] Manuel Weirich;Jonas Gurauskis;Vanesa Gil;Kjell Wiik;Man-Ann Einarsrud .Preparation of lanthanum tungstate membranes by tape casting technique[J].International journal of hydrogen energy,2012(9):8056-8061.
[6] Eric Q;Kostiantyn V K;Olivier J .Compatibility of pro-ton conducting La6 WO12 electrolyte with standard cathode materials[J].Solid State Ionics,2012,216:19-24.
[7] Sonia Escoldstico;Cecilia Soli's;Jose M. Sena .Hydrogen separation and stability study of ceramic membranes based on the system Nd5LnWO12[J].International journal of hydrogen energy,2011(18):11946-11954.
[8] Anna Magraso;Jonathan M. Polfus;Carlos Frontera .Complete structural model for lanthanum tungstate: a chemically stable high temperature proton conductor by means of intrinsic defects[J].Journal of Materials Chemistry: An Interdisciplinary Journal dealing with Synthesis, Structures, Properties and Applications of Materials, Particulary Those Associated with Advanced Technology,2012(5):1762-1764.
[9] Jordal K;Bredesen R;Kvamsdal H M et al.Integration of H2-separating membrane technology in gas turbine processes for CO2 sequestration[J].Energy,2004,29(9-10):1269-1278.
[10] Fontaine M L;Larring Y;Norby T et al.Dense ceram-ic membranes based on ion conducting ceramics[J].Ann Chim Sci Mat,2007,32(02):197-212.
[11] Magrasó, A.;Frontera, C.;Marrero-López, D.;Nú?ez, P. .New crystal structure and characterization of lanthanum tungstate "la_6WO_(12)" prepared by freeze-drying synthesis[J].Dalton transactions: An international journal of inorganic chemistry,2009(46):10273-10283.
[12] J.J. Roa;A. Magraso;M. Morales .Determination of hardness, Young's modulus and fracture toughness of lanthanum tungstates as novel proton conductors[J].CERAMICS INTERNATIONAL,2011(5):1593-1599.
[13] Vanesa Gil;Jonas Gurauskis;Christian Kj?lseth;Kjell Wiik;Man-Ann Einarsrud .Hydrogen permeation in asymmetric La_(28) -~ xW_(4 + x)O_(54 + 3x/2) membranes[J].International journal of hydrogen energy,2013(7):3087-3091.
[14] Sonia E;Cecilia S;Jose M S .Study of hydrogen perme-ation in(La5/6 Nd1/6)5.5 WO12-δ membranes[J].Solid State Ionics,2012,216:31-35.
[15] Michel, C.R.;Martínez-Preciado, A.H.;Contreras, N.L.L..Gas sensing properties of Nd_2O_3 nanostructured microspheres[J].Sensors and Actuators, B. Chemical,2013:8-14.
[16] Zhiwen Zhu;Litao Yan;Haowei Liu;Wenping Sun;Qingping Zhang;Wei liu .A mixed electronic and protonic conducting hydrogen separation membrane with asymmetric structure[J].International journal of hydrogen energy,2012(17):12708-12713.
[17] 李英,龚江宏,谢裕生,唐子龙,陈运法,张中太.Y2O3稳定ZrO2材料的电导活化能[J].无机材料学报,2002(04):811-816.
[18] Jean-Baptiste Jorcin;Mark E. Orazem;Nadine Pebere;Bernard Tribollet .CPE analysis by local electrochemical impedance spectroscopy[J].Electrochimica Acta,2006(8/9):1473-1479.
[19] 吕敬德,王岭,郭红霞,高会元.质子-电子混合导体透氢膜[J].化工新型材料,2008(03):1-4.
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