机械合金化过程对硫化铋块体热电性能的影响机理

葛振华; 张波萍; 于昭新; 刘勇; 李敬锋

doi:10.7498/aps.61.048401

摘要

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.

关键词:

Abstract

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.

Keywords:

作者及机构信息

1.
北京科技大学材料科学与工程学院, 北京市新能源材料与技术重点实验室, 北京 100083;

2.
清华大学材料科学与工程系, 新型陶瓷与精细制备工艺国家重点实验室, 北京 100084

基金项目: 国家自然科学基金(批准号: 50972012), 国家高技术研究发展计划(863计划)(批准号: 2009AA03Z216 ), 国家重点基础研究发展计划(973计划)(批准号: 2007CB607500)和北京市自然科学基金(批准号: 2112028)资助的课题.

Authors and contacts

1.
Beijing Key Lab of New Energy Materials and Technology, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China;

2.
State Key Laboratory of New Ceramics and Fine Processing, Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 50972012), the National High Technology Research and Development Program of China (Grant No. 2009AA03Z216), the National Basic Research Program of China (Grant No. 2007CB607500), and the Natural Science Foundation of Beijing, China (Grant No.2112028).

参考文献

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[3]	Tritt T M 1999 Science 283 804
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[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]
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[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
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施引文献

[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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