无机材料学报 ›› 2022, Vol. 37 ›› Issue (10): 1079-1086.DOI: 10.15541/jim20220039 CSTR: 32189.14.10.15541/jim20220039

• 研究论文 • 上一篇    下一篇

Te与In共掺杂对Cu2SnSe3热电性能的影响

任培安(), 汪聪, 訾鹏, 陶奇睿, 苏贤礼(), 唐新峰()   

  1. 武汉理工大学 材料复合新技术国家重点实验室, 武汉 430070
  • 收稿日期:2022-01-24 修回日期:2022-03-04 出版日期:2022-10-20 网络出版日期:2022-04-07
  • 通讯作者: 唐新峰, 教授. E-mail: tangxf@whut.edu.cn;
    苏贤礼, 研究员. E-mail: suxianli@whut.edu.cn
  • 作者简介:任培安(1996-), 男, 硕士研究生. E-mail: renpeian@whut.edu.cn
  • 基金资助:
    国家自然科学基金(51972256);国家自然科学基金(51872219);国家自然科学基金(51632006);国家重点研发计划(2018YFB0703600)

Effect of Te and In Co-doping on Thermoelectric Properties of Cu2SnSe3 Compounds

REN PeiAn(), WANG Cong, ZI Peng, TAO Qirui, SU Xianli(), TANG Xinfeng()   

  1. State Key Laboratory of Advanced Technology for Material Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
  • Received:2022-01-24 Revised:2022-03-04 Published:2022-10-20 Online:2022-04-07
  • Contact: TANG Xinfeng, professor. E-mail: tangxf@whut.edu.cn;
    SU Xianli, professor. E-mail: suxianli@whut.edu.cn
  • About author:REN Peian (1996-), male, Master candidate. E-mail: renpeian@whut.edu.cn
  • Supported by:
    National Natural Science Foundation of China(51972256);National Natural Science Foundation of China(51872219);National Natural Science Foundation of China(51632006);National Key Research and Development Program of China(2018YFB0703600)

摘要:

Cu2SnSe3基化合物作为一种绿色环保的新型热电材料, 近年受到了研究者的广泛关注。然而, 本征Cu2SnSe3基化合物载流子浓度低、电性能较差。为优化Cu2SnSe3化合物的电热输运性能, 本研究采用熔融、退火结合放电等离子烧结技术制备了一系列Cu2SnSe3-xTex (x=0~0.2)和Cu2Sn1-yInySe2.9Te0.1 (y=0.005~0.03)样品, 研究了Te固溶和In掺杂对材料电热输运性能的影响。Te在Cu2SnSe3-xTex (x=0~0.2)化合物中的固溶度为0.10, Te固溶显著增加了材料的载流子有效质量, 从本征Cu2SnSe3样品的0.2me增加到Cu2SnSe2.9Te0.1样品的0.45me, 显著提高了材料的功率因子, Cu2SnSe2.99Te0.01样品在300 K下获得最大功率因子为1.37 μW·cm-1·K-2。为了进一步提高材料的电传输性能, 本研究以Cu2SnSe2.9Te0.1为基体并选取In在Sn位掺杂。In掺杂将Cu2SnSe3基化合物的载流子浓度从5.96×1018 cm-3 (Cu2SnSe2.9Te0.1)显著提高到2.06×1020 cm-3 (Cu2Sn0.975In0.025Se2.9Te0.1)。调控载流子浓度促进了材料多价带参与电传输, 材料的电导率和载流子有效质量显著增加, 功率因子得到大幅度提升, 在473 K下Cu2Sn0.995In0.005Se2.9Te0.1化合物获得最大功率因子为5.69 μW·cm-1·K-2。由于电输运行性能显著提升和晶格热导率降低, Cu2Sn0.985In0.025Se2.9Te0.1样品在773 K下获得最大ZT为0.4, 较本征Cu2SnSe3样品提高了4倍。

关键词: Cu2SnSe3基化合物, Te掺杂, In掺杂, 热电性能

Abstract:

Recently, Cu2SnSe3-based compounds, as a new environment-friendly thermoelectric material, have attracted worldwide attentions. However, the pristine Cu2SnSe3 compound possesses relatively low carrier concentration and thus an inferior electronic transport properties. To optimize the thermoelectric properties of Cu2SnSe3- based compounds, herein, two series of Cu2SnSe3-xTex (x=0-0.2) and Cu2Sn1-yInySe2.9Te0.1 (y=0.005-0.03) samples were synthesized through traditional melting-annealing technique combined with plasma activated sintering (PAS). The role of Te and In co-doping on the thermoelectric properties of Cu2SnSe3-based compounds were systematically investigated. The solubility limit of Te in the Cu2SnSe3-xTex compounds is around 0.10. The substitution of Te on Se site significantly increases the effective mass of charge carrier from 0.2me for pristine Cu2SnSe3 compound to 0.45me for Cu2SnSe2.9Te0.1 compound, which improves the power factor of the material. Cu2SnSe2.99Te0.01 compound attains the maximum power factor of 1.37 μW·cm-1·K-2 at 300 K. To further improve the electronic transport properties of the material, Cu2SnSe2.9Te0.1 was chosen as the matrix and In was selected to dope on Sn site. We found that doping with In significantly improves the carrier concentration of Cu2SnSe3-based compounds from 5.96×1018 cm-3 for Cu2SnSe2.9Te0.1 to 2.06×1020 cm-3 for Cu2Sn0.975In0.025Se2.9Te0.1, which promotes the participation of multiple valence bands in the electronic transport. All these produce the great enhancements on the electrical conductivity, effective mass of charge carriers and power factor. As a result, Cu2Sn0.995In0.005Se2.9Te0.1 compound obtains the maximum power factor of 5.69 μW·cm-1·K-2 at 473 K. Due to the significant improvement of electrical transport performance and the decrease in lattice thermal conductivity, the maximum ZT of 0.4 is achieved for Cu2Sn0.985In0.025Se2.9Te0.1 compound at 773 K, which is 4 times higher than that of pristine Cu2SnSe3 compound.

Key words: Cu2SnSe3-based compound, Te doping, In doping, thermoelectric property

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