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[1]姜　媛,黄志良*,陈常连*,等.铝掺杂磷灰石型硅酸镧电解质的电导机理[J].武汉工程大学学报,2022,44(01):48-54.[doi:10.19843/j.cnki.CN42-1779/TQ.202010006]
　JIANG Yuan,HUANG Zhiliang*,CHEN Changlian*,et al.Conductance Mechanism of Al-Doped Apatite-Type Lanthanum Silicate Electrolyte[J].Journal of Wuhan Institute of Technology,2022,44(01):48-54.[doi:10.19843/j.cnki.CN42-1779/TQ.202010006]
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《武汉工程大学学报》[ISSN:1674-2869/CN:42-1779/TQ]

卷:
44
期数:
2022年01期
页码:
48-54
栏目:
材料科学与工程
出版日期:
2022-02-28

文章信息/Info

Title:
Conductance Mechanism of Al-Doped Apatite-Type Lanthanum Silicate Electrolyte
文章编号:
1674 - 2869（2022）01 - 0048 - 07
作者:
姜　媛; 黄志良*; 陈常连*; 鲁　冕; 吴昌胜; 陈　石
武汉工程大学材料科学与工程学院，湖北 武汉 430205
Author(s):
JIANG Yuan; HUANG Zhiliang*; CHEN Changlian*; LU Mian; WU Changsheng; CHEN Shi
School of Materials Science and Engineering，Wuhan Institute of Technology，Wuhan 430205，China
关键词:
燃烧法; 硅酸镧; 固体电解质; 铝掺杂; 电导增强机理
Keywords:
combustion method; lanthanum silicate; solid electrolyte; Al-doped; enhancing mechanism of conductance
分类号:
O646
DOI:
10.19843/j.cnki.CN42-1779/TQ.202010006
文献标志码:
A
摘要:
采用燃烧法在600 ℃下5~7 min内成功制备了铝掺杂的La9.33Si6-xAlxO26-0.5x（x=0.5，1.0，1.5，2.0）（LSAO）固体电解质粉体，在800 ℃预烧12 h后，经压制成型、烧结制得LSAO陶瓷体。X射线衍射、X射线光电子能谱、傅里叶变换红外光谱和扫描电子显微镜证实燃烧法制备的LSAO纯度高，具有典型的P63/m磷灰石型结构；掺杂的Al3+替换了Si4+进入了［SiO4］四面体结构中形成［Si（Al）O4］，并产生了氧空位；在1 500 ℃烧结3 h得到烧结性能最佳的LSAO陶瓷体。电化学阻抗谱显示当掺量x<0.5时，La9.33Si6O26（LSO）的电导率随掺量的增加而增强；当掺量x>0.5时，La9.33Si6O26（LSO）的电导率随掺量的增加而降低，这归因于Al3+掺杂形成氧空位，减小了氧离子传输过程中的空间阻力，电导率增大；然而，当Al3+掺量过多，LSAO结构中间隙氧浓度大量减少，电导率降低。当掺量x=0.5时，电导率在800 ℃达到最大值为1.26×10-2 S/cm。该电导增强机理为氧空位缺陷增强电导机理。
Abstract:
The Al-doped La9.33Si6-xAlxO26-0.5x （LSAO，x=0.0，0.5，1.0，1.5，2.0） solid electrolyte powders were successfully prepared at 600 ℃ within 5-7 minutes by combustion method. The LSAO ceramics were prepared from the powder calcined at 800 ℃ for 12 h via pressing， molding and sintering in sequence. The analyses of X-ray diffraction，X-ray photoelectron spectroscopy，Fourier transform infrared spectroscopy and scanning electron microscopy confirm that the LSAOs prepared by combustion method possess high purity and typical P63/m apatite structure. The doped Al3+ ions replace Si4+ ions and form ［Si（Al）O4］ in tetrahedral ［SiO4］，generating the oxygen vacancy. The LSAO ceramics with the best sintering properties were obtained by sintering at 1 500 ℃ for 3 h. The electrochemical impedance spectrum shows that when x＜0.5，the conductivity of LSAO increases with the increase of x，and when x>0.5，the conductivity of LSAO decreases with the increase of x，which is attributed to the formation of oxygen vacancy by Al3+ doping，thus reducing the spatial resistance of oxygen ions transport and increasing the conductivity. However，excessive incorporation of Al3+ leads to the large reduction in interstitial oxygen concentration and the decrease in conductivity. When x=0.5，the maximum conductivity reaches 1.26×10-2 S/cm（t=800 ℃）. The mechanism of enhanced conductance is oxygen vacancy defects enhancement mechanism.

参考文献/References:

［1］　DING X F，HUA G X，DING D，et al. Enhanced ionic conductivity of apatite-type lanthanum silicate electrolyte for IT-SOFCs through copper doping ［J］. Journal of Power Sources，2016，306：630-635.［2］　YOSHIOKA H. Enhancement of ionic conductivity of apatite-type lanthanum silicates doped with cations ［J］. Journal of the American Ceramic Society，2007，90（10）：3099-3105.［3］　XIANG J，CHEN H Q，OUYANG J H，et al. Stability and compatibility of lanthanum silicates electrolyte with standard cathode materials ［J］. Ceramics International，2019，45（5）：6183-6189.［4］　LóPEZ D M，MARTíN-SEDE?O M C，MARTíNEZ J P，et al. Evaluation of apatite silicates as solid oxide fuel cell electrolytes ［J］. Journal of Power Sources，2010，195（9）：2496-2506.［5］　WU R F，PAN W，REN X R，et al. An extremely low thermal conduction ceramic：RE9.33(SiO4)6O2 silicate oxyapatite ［J］. Acta Materialia，2012，60（15）：5536-5544.［6］　MINESHIGE A，OHNISHI Y，SAKAMOTO R，et al. Effect of cation doping on ionic and electronic properties for lanthanum silicate-based solid electrolytes ［J］. Solid State Ionics，2011，192（1）：195-199.［7］　KOBAYASHI K， HIRAI K， SUZUKI T S， et al. Sinterable powder fabrication of lanthanum silicate oxyapatite based on solid-state reaction method ［J］. Journal of the Ceramic Society of Japan，2015，123（4）：274-279.［8］　DAI L， HAN W， LI Y H， et al. Synthesis and characterization of Al3+ and M（M=W6+，In3+，Nb5+，Mg2+） co-doped lanthanum silicate oxy-apatite electrolytes ［J］. International Journal of Hydrogen Energy，2016，41（26）：11340-11350.［9］　ZHAO Y Q， DAI L， HE Z X， et al. Synthesis and characterization of Ba2+ and W6+ co-doped apatite-type lanthanum silicate electrolytes ［J］. Ceramics International，2020，46（4）：5420-5429.［10］　ZHANG L，HE H Q，WU H W，et al. Synthesis 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.［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］. International Journal of Hydrogen Energy，2014，39（33）：19093-19101.［12］　吴昌胜，雷红，黄江胜，等. 锶锌双掺杂磷灰石型硅酸镧电解质的制备与表征［J］. 武汉工程大学学报，2019，41（5）：453-456.［13］　TAO S W， IRVINE J T S. Preparation and characterisation of apatite-type lanthanum silicates by a sol-gel process ［J］. Materials Research Bulletin，2001，36（7/8）：1245-1258.［14］　YAMAGATA C， ELIAS D R，PAIVA M R S，et al. Facile preparation of apatite-type lanthanum silicate by a new water-based sol-gel process ［J］. Materials Research Bulletin，2013，48（6）：2227-2231.［15］　YANG T R，ZHAO H L，HAN J，et al. Synthesis and densification of lanthanum silicate apatite electrolyte for intermediate temperature solid oxide fuel cell via co-precipitation method ［J］. Journal of the European Ceramic Society，2014，34（6）：1563-1569.［16］　MA Y Z， MOLIERE M， YU Z X， et al. Novel chemical reaction co-precipitation method for the synthesis of apatite-type lanthanum silicate as an electrolyte in SOFC ［J］. Journal of Alloys and Compounds，2017，723：418-424.［17］　SKJARV? S H，WEFRING E T，NESDAL S K，et al. Interstitial oxygen as a source of p-type conductivity in hexagonal manganites ［J］. Nature Communica-tions，2016，7：13745：1-8.［18］　VORONKOV V V. Generation of thermal donors in silicon：oxygen aggregation controlled by self-interstitials［J］. Semiconductor Science and Technology，1993，8（12）：2037-2047.

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备注/Memo

备注/Memo:
收稿日期：2020-10-09基金项目：国家自然科学基金（51374155，51242010）；湖北省科技支撑计划（2014BCB034）；武汉工程大学研究生教育创新基金（CX2020167）作者简介：姜　媛，硕士研究生。E-mail:[email protected]*通讯作者：黄志良，博士，教授。E-mail:[email protected]； 陈常连，博士，副教授。E-mail:[email protected]引文格式：姜媛，黄志良，陈常连，等. 铝掺杂磷灰石型硅酸镧电解质的电导机理［J］. 武汉工程大学学报，2022，44（1）：48-54.
更新日期/Last Update: 2022-03-01