硅酸盐学报

新型固体氧化物燃料电池阳极材料LaxSr2–xMgMoO6–δ的结构与电化学性能

单位：1. 景德镇陶瓷学院材料学院江西景德镇 333001 2. 北京科技大学材料学院北京 100083

分类号：TM911.4

出版年,卷(期):页码：2016,44(6):817-823

DOI：10.14062/j.issn.0454-5648.2016.06.06

摘要：

通过柠檬酸络合法合成了LaxSr2–xMgMoO6–δ (LSMM)阳极材料。利用X射线衍射和扫描电子显微镜分析样品的物相结构、微观形貌及与电解质的化学相容性，采用四端引线法测试材料的电导率，利用电化学工作站测试其阳极阻抗特性，并以La0.8Sr0.2Ga0.8Mg0.2O3(LSGM)为电解质、PrBaCo2O5+δ为阴极制备了单电池，测试功率密度。结果表明：空气中La的掺杂量小于0.2(摩尔分数)时，还原后La的掺杂量可以达到0.6，La的掺杂导致晶胞体积增大。La掺杂的Sr2MgMoO6(SMMO)与电解质LSGM、Ce0.8Gd0.2O2–δ(GDC)在1 250 ℃煅烧10 h，均没有杂质相生成，具有良好的化学相容性。La掺杂显著提高了SMMO的电导率，800 ℃、5%H2/Ar气氛中，La0.6Sr1.4MgMoO6–δ的电导率为40 S/cm。La的掺杂降低了阳极材料的极化电阻，提高了电池功率密度。

LaxSr2–xMgMoO6–δ (LSMM) anode material was synthesized via a citrate acid complexing method. The phase composition was determined by X-ray diffraction, and the microstructure of the sintered samples was determined by scanning electron microscopy. The electrical conductivity of all samples was measured by a standard four-terminal dc method, and the AC electrochemical impedance spectra were detected in a symmetrical cell. Single fuel cells were prepared using an electrolyte-supported technique with La0.8Sr0.2Ga0.8Mg0.2O3(LSGM) as an electrolyte, LSMM as an anode and PrBaCo2O5+δ as a cathode. The results demonstrate that the doping limit of La is less than 0.2 in air, which is 0.6 after reducing in 5%H2/Ar. The doping leads to the increase of cell volume of LSMM. The LSMM anode material has a good chemical compatibility with GDC and LSGM electrolytes after calcining at 1 250 ℃ for 10 h. The La doping increases the electronic conductivity of La0.6Sr1.4MgMoO6–δ, which is 40 S/cm at 800 ℃ in 5%H2/Ar, and decreases the polarization resistance, resulting in the improvement of power density for single cells.

基金项目：

国家自然科学基金(51402136, 51402135)和江西省自然科学基金(20142BAB216007, 20142BAB216006)资助。

作者简介：

谢志翔(1982—)，男，博士，讲师。

参考文献：

[1] JIANG S P, YE Y, HE T, et al. Nanostructured palladium La0.75Sr0.25Cr0.5Mn0.5O3/Y2O3–ZrO2 composite anodes for direct methane and ethanol solid oxide fuel cells [J]. J Power Sources, 2008, 185(1): 179–182. [2] 韩敏芳, 彭苏萍. 固体氧化物燃料电池材料及制备[M]. 北京: 科学出版社, 2004. [3] KIM P, BRETT D J L, BRANDON N P. The effect of water content on the electrochemical impedance response and microstructure of Ni–CGO anodes for solid oxide fuel cells[J]. J Power Sources, 2009, 189(2): 1060–1065. [4] AI N, Lü Z, TANG J, et al. Improvement of output performance of solid oxide fuel cell by optimizing Ni/samaria-doped ceria anode functional layer[J]. J Power Sources, 2008, 185(1): 153–158. [5] CLEMMER R M C, CORBIN S F. The influence of pore and Ni morphology on the electrical conductivity of porous Ni/YSZ composite anodes for use in solid oxide fuel cell applications[J]. Solid State Ionics, 2009, 180(9/10): 721–730. [6] LOHSOONTORN P, BRETT D J L, BRANDON N P. The effect of fuel composition and temperature on the interaction of H2S with nickel–ceria anodes for Solid Oxide Fuel Cells[J]. J Power Sources, 2008, 183(1): 232–239. [7] DING D, LI L, FENG K, et al. High performance Ni–Sm2O3 cermet anodes for intermediate temperature solid oxide fuel cells[J]. J Power Sources, 2009, 187(2): 400–402. [8] HERNADI K, FONSECA A, NAGY J B, et al. Production of nanotubes by the catalytic decomposition of different carbon-containing compounds[J]. Appl Catal A, 2000, 199(2): 245–255. [9] KOH J H, YOO Y S, PARK J W, et al. Carbon deposition and cell performance of Ni–YSZ anode support SOFC with methane fuel[J]. Solid State Ionics, 2002, 149(3/4): 157–166. [10] HUANG Y H, DASS R I, XING Z L, et al. Double perovskites as anode materials for solid-oxide fuel cells[J]. Science, 2006, 312(5771): 254–257. [11] HUANG Y H, DASS R I, DENYSZYN J C, et al. Synthesis and characterization of Sr2MgMoO6–δ an anode material for the solid oxide fuel cell[J]. J Electrochem Soc, 2006, 153(7): A1266–A1272. [12] JI Y, HUANG Y H, YING J R, et al. Electrochemical performance of La-doped Sr2MgMoO6–δ in natural gas[J]. Electrochem Commun, 2007, 9(8): 1881–1885. [13] MARRERO–LOPEZ D, PENA–MARTINEZ J, RUIZ–MORALES J C, et al. High temperature phase transition in SOFC anodes based on Sr2MgMoO6–δ[J]. J Solid State Chem, 2009, 182(5): 1027–1034. [14] BERNUY–LOPEZ C, ALLIX M, BRIDGES C A, et al. Sr2MgMoO6–δ: Structure, phase stability, and cation site order control of reduction[J]. Chem Mater, 2007, 19(5): 1035–1043. [15] VASALA S, LETHIMAKI M, HUANG Y H, et al. Degree of order and redox balance in B-site ordered double-perovskite oxides, Sr2MMoO6–δ (M=Mg, Mn, Fe, Co, Ni, Zn)[J]. J Solid State Chem, 2010, 183(5): 1007–1021. [16] SHANNON, R D. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides[J]. Acta Cryst, 1976, 32(5): 751–767. [17] BALCELLS L I, NAVARRO J, BIBES M, et al. Cationic ordering control of magnetization in Sr2FeMoO6 double perovskite[J]. Appl Phys Lett, 2001(6), 78: 781–783. [18] GARCIA-HERNANDEZ M, MARTINEZ J L, MARTINEZ-LOPE M J, et al. Finding universal correlations between cationic disorder and low field magnetoresistance in Fe/Mo double perovskite series[J]. Phys Rev Lett, 2001, 86(11): 2443–2446. [19] ZHANG L L, HE T M. Performance of double-perovskite Sr2–xSmxMgMoO6–δ as solid-oxide fuel-cell anodes[J]. J Power Sources, 2011, 196(20): 8352–8359.

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