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以机械合金化法(MA)结合放电等离子烧结技术(SPS)制备了Bi2S3多晶块体热电材料. 研究了MA过程中干磨转速、湿磨时间和湿磨介质对Bi2S3多晶热电材料电传输性能的影响. 分析了样品的物相, 观察了显微组织, 测试了电传输性能和热传输性能. 研究表明, 以无水乙醇为湿磨介质时, 随着湿磨时间的延长, 出现了微量Bi2O3第二相, 样品的晶粒尺寸减小, 电阻率大幅增加, 功率因子下降. 以丙酮为湿磨介质时, 虽然不存在微氧化反应, 但是由于样品中存在大量孔洞, 导致功率因子降低. 425 r/min 干磨15 h后未湿磨的样品在573 K取得最大的ZT值0.25, 是目前文献报道的最高值.Bismuth sulfide (Bi2S3) polycrystalline bulks are fabricated by spark plasma sintering (SPS) combined with a mechanical alloying (MA) process. The electrical transport properties are investigated with a special emphasis on dry-milling speed, wet-milling time and mediums in MA process. The phase structure, the microstructure, and the electrical/thermal transport properties for the bulk samples are measured. The results suggest that the second Bi2O3 phase is formed because of the micro-oxidation when the wet medium is fixed to absolute ethyl alcohol, which refines the grain sizes and affects electrical transport properties of the bulk samples. Prolonging the wet-milling time in absolute ethyl alcohol causes the increase of resistivity and the decrease of the power factor. The electrical transport properties degrade due to the porous microstructure in bulk samples even without oxidization as the acetone is used as a milling medium. The largest ZT value 0.25 is obtained at 573 K for the samples dry-milled under 425 r/min for 15 h without wet-milling, which is the highest value in the reported values so far.
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Keywords:
- mechanical alloying process /
- Bi2S3 /
- thermoelectric /
- micro oxidation
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[1] Stella M H 2002 Science 295 767
[2] Snyder G J, Toberer E S 2008 Nature Mater 7 105
[3] Tritt T M 1999 Science 283 804
[4] Jiang M B, Wu Z X, Zhou M, Huang J R, Li L F 2010 Acta Phys. Sin. 59 7314 (in Chinese) [蒋明波, 吴智雄, 周敏, 黄荣进, 李来风 2010 59 7314]
[5] Stordeur M, Rowe D M (Ed.) 1995 CRC Handbook of Thermoelectrics (Boca Raton: CRC Press)
[6] Chen G, Dresselhaus M S, Dresselhaus G, Fleurial J P, Caillat T 2003 Int. Mater. Rev. 48 1
[7] Li J F, Liu W S, Zhao L D, Zhou M 2010 NPG Asia Mater. 2 152
[8] Chen L D, Xiong Z, Bo S Q 2010 J. Inorg. Mater. 25 561 (in Chinese) [陈立东, 熊 震, 柏胜强 2010 无机材料学报 25 561]
[9] Zhang F, Zhu H T, Luo J, Liang J K, Rao G H, Liu Q L 2010 Acta Phys. Sin. 59 7232 (in Chinese) [张帆, 朱航天, 骆军, 粱敬魁, 饶光辉, 刘泉林 2010 59 7232]
[10] Luo X G, He J Z 2011 Chin. Phys. B 20 030509
[11] Poudel B, Hao Q, Ma Y, Lan Y C, Minnich A, Yu B, Yan X,Wang D Z, Muto A, Vashaee D, Chen X Y, Liu J M, Dresselhaus M S, Chen G, Ren Z F, 2008 Science 320 634.
[12] Chen B, Uher C, Iordanidis L, Kanatzidis M G, 1997 Chem. Mater. 9 1655
[13] Ge Z H, Zhang B P, Shang P P, Li J F 2011 J. Mater. Chem. 21 9194
[14] Zhao L D, Zhang B P, Liu W S, Zhang H L, Li J F 2008 J. Solid State Chem. 181 3278
[15] Ge Z H, Zhang B P, Shang P P, Yu Y Q, Chen C, Li J F 2011 J. Electron. Mater. 40 1087
[16] Suryanarayana C 2001 Prog. in Mater. Sci. 46 1
[17] Sikandar H, Tamboli S, Kamat V 2010 Arch. Phys. Res. 4 73
[18] Ioffe A M 1957 Semiconductor Thermoelements and Thermoelectric Cooling (London Infisearch Ltd., Press)
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