运用传统固相法合成了Re掺杂的Mo3-xRexSb7(x=0,0.05,0.10)系列化合物,并通过热压烧结得到了致密样品.采用X射线粉末衍射(XRD)和X射线能量色散谱(EDS)表征了样品的相成分,同时经过第一性原理计算分析了Re掺杂对Mo3Sb7能带结构的影响,进而研究了Re掺杂对Mo3Sb7热电性能影响的规律.结果表明:当掺杂量x≤0.1时,Re均匀地掺杂于晶格中形成固溶体且所有样品均无第二相杂质生成,同时晶胞参数随着Re掺杂量的增长而减小.Mo3Sb7作为一种P型三维导电材料,当每化学单位的Mo3Sb7额外获得两个化学单位的价电子将由金属转变为半导体.在Re掺杂后Mo3 Sb7费米面上移,这是因为Re比Mo多一个价电子,但由于固溶度的限制,Re掺杂并不能使其转化为半导体,且Re掺杂对于费米面处能带形状以及禁带宽度的影响也非常有限.由于Re较多的价电子,因此Re的引入降低了化合物Mo3Sb7的电导率,并提高了其热电势值,而电导率的降低也必然会减小载流子贡献的热导率,同时Re掺杂增加了晶格无序也降低了其晶格热导率,因此Mo3Sb7总的热导率得到了降低,最后其热电性能得到了提高.其中,经过Re掺杂后的化合物Mo2.90Re0.10Sb7在860 K下ZT值达到0.127,比化合物Mo3Sb7提高了23.3％.
参考文献
| [1] | Enhancement of Thermoelectric Figure-of-Merit by a Bulk Nanostructuring Approach[J].Advanced functional materials,2010(3):357. |
| [2] | G.JEFFREY SNYDER;ERIC S.TOBERER .Complex thermoelectric materials[J].Nature materials,2008(2):105-114. |
| [3] | M. S. Dresselhaus;G. Chen;M. Y. Tang;R. G. Yang;H. Lee;D. Z. Wang;Z. F. Ren;J.-P. Fleurial;P. Gogna .New Directions for Low-Dimensional Thermoelectric Materials[J].Advanced Materials,2007(8):1043-1053. |
| [4] | Zhang H;Zhao JT;Grin Y;Wang XJ;Tang MB;Man ZY;Chen HH;Yang XX .A new type of thermoelectric material, EuZn2Sb2[J].The Journal of Chemical Physics,2008(16):164713-1-164713-5-0. |
| [5] | Joseph R. Sootsman;Duck Young Chung;Mercouri G. Kanatzidis .New and Old Concepts in Thermoelectric Materials[J].Angewandte Chemie,2009(46):8616-8639. |
| [6] | 段兴凯,江跃珍.真空电弧等离子体合成（BixSb1-x）2Te3纳米粉末材料[J].稀有金属,2011(03):394-397. |
| [7] | Franck Gascoin;Sandra Ottensmann;Daniel Stark;Sossina M. Haiele;G. Jeffrey Snyder .Zintl Phases as Thermoelectric Materials: Tuned Transport Properties of the Compounds Ca_xYb_(1-x)Zn_2Sb_2[J].Advanced functional materials,2005(11):1860-1864. |
| [8] | Holger Kleinke .New bulk Materials for Thermoelectric Power Generation: Clathrates and Complex Antimonides[J].Chemistry of Materials: A Publication of the American Chemistry Society,2010(3):604-611. |
| [9] | ZHU Yunguang,SHEN Honglie,CHEN Haili.Effects of nano-TiO2 dispersion on thermoelectric properties of Co4Sb11.7Te0.3 composites[J].稀有金属（英文版）,2012(01):43-47. |
| [10] | Hong Xu;Katja M. Kleinke;Tim Holgate;David Rossouw;Gianluigi Botton;Terry M. Tritt;H. Kleinke .Thermoelectric properties of A_(0.05)Mo_3Sb_(5.4)Te_(1.6) (A = Mn, Fe, Co, Ni)[J].Journal of Alloys and Compounds: An Interdisciplinary Journal of Materials Science and Solid-state Chemistry and Physics,2010(2):314-319. |
| [11] | HUQIN ZHANG;JIAN HE;BO ZHANG;ZHE SU;TERRY M. TRITT;NAVID SOHEILNIA;HOLGER KLEINKE .Thermoelectric Properties of Mo_(3)Sb_(5.4)Te_(1.6) and Ni_(0.06)Mo_(3)Sb_(5.4)Te_(1.6)[J].Journal of Electronic Materials,2007(7):727-731. |
| [12] | H. Xu;K. M. Kleinke;T. Holgate;H. Zhang;Z. Su;T. M. Tritt;H. Kleinke .Thermoelectric performance of Ni_(y)Mo_(3)Sb_(7-x)Te_(x) (y<=0.1, 1.5 <= x <= 1.7)[J].Journal of Applied Physics,2009(5):053703-1-053703-5-0. |
| [13] | C. CANDOLFI;J. LESZCZYNSKI;P. MASSCHELEIN;C. CHUBILLEAU;B. LENOIR;A. DAUSCHER;E. GUILMEAU;J. HEJTMANEK;S.J. CLARKE;R.I. SMITH .Crystal Structure and High-Temperature Thermoelectric Properties of the Mo_(3-x)Ru_(x)Sb_(7) Compounds[J].Journal of Electronic Materials,2010(9):2132-2135. |
| [14] | C. Candolfi;B. Lenoir;A. Dauscher;B. Malaman;E. Guilmeau;J. Hejtmanek;J. Tobola .High thermoelectric power factor in Fe-substituted Mo_(3)Sb_(7)[J].Applied physics letters,2010(26):262103-1-262103-3. |
| [15] | Xiaoya Shi;Yanzhong Pei;G. Jeffrey Snyder;Lidong Chen .Optimized thermoelectric properties of Mo_3Sb_(7-x)Te_x with significant phonon scattering by electrons[J].Energy & environmental science: EES,2011(10):4086-4095. |
| [16] | Candolfi, C;Lenoir, B;Chubilleau, C;Dauscher, A;Guilmeau, E .High temperature thermoelectric properties of Mo3Sb7-xTex (0.0 <= x <= 1.8)[J].Journal of Physics. Condensed Matter,2010(2):025801:1-025801:6. |
| [17] | Enkhtsetseg Dashjav;Aleksandra Szczepenowska;Holger Kleinke .Optimization of the thermopower of the antimonide Mo_3Sb_7 by a partial Sb/Te substitution[J].Journal of Materials Chemistry: An Interdisciplinary Journal dealing with Synthesis, Structures, Properties and Applications of Materials, Particulary Those Associated with Advanced Technology,2002(2):345-349. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%