能带调控与点缺陷工程改善Cu_(12)Sb_(4)S_(13)的热电性能  

Improvement of thermoelectric performance of tetrahedrite Cu_(12)Sb_(4)S_(13) by energy band regulation and point defect engineering

作　　者：杨超 姜淑印 李世叶 王杰 张晋 成世兴 YANG Chao;LI Shiye;WANG Jie;ZHANG Jin;CHENG Shixing;JIANG Shuyin(School of Materials Science and Engineering,Shanxi Institute of Science and Technology,Jincheng 048011,China;School of Chemistry and Chemical Engineering,Henan Polytechnic University,Jiaozuo 454003,China;Shanxi Yamei Daning Energy Co.,Ltd.,Jincheng 048100,China)

机构地区：[1]山西科技学院材料科学与工程学院,山西晋城048011 [2]河南理工大学化学化工学院,河南焦作454000 [3]山西亚美大宁能源有限公司,山西晋城048100

出　　处：《功能材料》2024年第8期8201-8207,共7页Journal of Functional Materials

基　　金：国家自然科学基金项目(51671109);山西省基础研究计划青年项目(自由探索类)(202303021212304,202303021212303和202303021212302);晋城市重点研发计划项目(20230102)。

摘　　要：研究采用廉价高价元素Ga取代Cu,利用高温熔融、退火结合放电等离子烧结技术(SPS)制备了Cu_(12-x)Ga_(x)Sb_(4)S_(13)(x=0,0.05,0.1和0.15)热电材料,并对样品的物相组成、能带结构和热电性能进行了表征与分析。结果表明,Ga掺杂能够在导带附近引入杂质带,起到施主能级的作用,降低空穴载流子浓度,提高材料的Seebeck系数。同时,随着Ga掺杂量的增加,热导率显著下降,当温度为770 K时,Cu_(11.85)Ga_(0.15)Sb_(4)S_(13)样品热导率下降到1.20 W/mK,比本征材料降低了29%。最终,Cu_(11.9)Ga_(0.1)Sb _(4)S_(13)样品获得最佳的热电性能,在770 K时ZT值为0.7,相比本征材料提高了40%。A series of Cu_(12-x)Ga_(x)Sb_(4)S_(13)(x=0,0.05,0.1 and 0.15)samples were synthesized through high-temperature melting method and heat annealing technique combined with spark plasma sintering(SPS).The phase composition,band structure and thermoelectric properties of the samples were characterized and analyzed.The results show that Ga doping can introduce impurity band near the conduction band,acting as donor energy level,thus reducing the hole carrier concentration and increasing the Seebeck coefficient of the samples.At the same time,with the increase of Ga doping content,the thermal conductivity of Ga-doped samples decreases significantly.When the temperature is 770 K,the thermal conductivity of Cu_(11.85)Ga_(0.15)Sb_(4)S_(13) sample decreases to 1.20 W/mK,which is 29%lower than that of the intrinsic material.Finally,the maximum ZT value of 0.7 is achieved for Cu_(11.9)Ga_(0.1)Sb _(4)S_(13) sample at 770 K,a 40%improvement over the intrinsic Cu_(12)Sb_(4)S_(13).

关 键 词：热电性能 SEEBECK系数 热导率 能带结构 掺杂 

分 类 号：TB34[一般工业技术—材料科学与工程]