n型SnS热电材料的制备与性能研究  

Preparation and Thermoelectric Property of n-type SnS

作　　者：黄志成 姚瑶[1] 裴俊 董金峰 张波萍[1] 李敬锋 尚鹏鹏[3] HUANG Zhi-Cheng;YAO Yao;PEI Jun;DONG Jin-Feng;ZHANG Bo-Ping;LI Jing-Feng;SHANG Peng-Peng(The Beijing Municipal Key Laboratory of New Energy Materials and Technologies,School of Materials Science and Engineering,University of Science and Technology Beijing,Beijing 100083,China;State Key Laboratory of New Ceramics and Fine Pro-cessing,School of Materials Science and Engineering,Tsinghua University,Beijing 100084,China;College of Chemistry and Material Science,Shandong Agricultural University,Tai'an 271018,China)

机构地区：[1]北京科技大学材料科学与工程学院北京新能源材料与技术重点实验室,北京100083 [2]清华大学材料学院新型陶瓷与精细工艺国家重点实验室,北京100084 [3]山东农业大学化学与材料科学学院,泰安271018

出　　处：《无机材料学报》2019年第3期321-327,共7页Journal of Inorganic Materials

基　　金：国家重点研发计划(2018YFB0703600);国家自然科学基金(11474176)~~

摘　　要：SnS由低毒、廉价、高丰度的元素组成,在热电研究领域受到广泛关注。采用机械合金化(MA)结合放电等离子烧结(SPS)工艺制备了n型SnS_(1-x)Cl_x(x=0,0.02,0.03,0.04,0.05,0.06)多晶块体热电样品,并研究了Cl^-掺杂量对SnS物相、微观结构以及电热输运性能的影响。结果表明:Cl^-的引入会提高电子浓度,使SnS由本征p型转变为n型半导体。随着Cl^-掺杂量的增加,n型SnS半导体室温下的霍尔载流子浓度从6.31×10^(14) cm^(-3)(x=0.03)增加到7.27×10^(15 )cm^(-3)(x=0.06)。x=0.05样品在823 K取得最大的电导率为408 S·m^(-1),同时具有较高的泽贝克系数为-553μV?K^(-1),使其获得最大功率因子为1.2μW·cm^(-1)·K^(-2)。Cl^-的掺入会引入点缺陷,散射声子,使晶格热导率κ_(lat)由0.67 W·m^(-1)·K^(-1)(x=0)降至0.5 W·m^(-1)·K^(-1)(x=0.02)。x=0.04样品在823 K获得了最大ZT为0.17,相比于x=0样品(ZT～0.1)提高了70%。SnS composed of low toxicity, low-cost and earth-abundant elements, has extensive attention in the field of thermoelectric research. The n-type SnS1-xClx (x=0, 0.02, 0.03, 0.04, 0.05, 0.06) polycrystalline bulk thermoelectric samples were prepared by mechanical alloying (MA) combined with Spark Plasma Sintering (SPS). Effect of Cl^- amounts on the phase structure, microstructure and thermoelectric transport properties were systematically studied. Results show that introduction of Cl^- enhances electron concentration which makes in-trinsic p-type SnS change to n-type. With the amount of Cl^- increasing, the Hall carrier concentration of n-type SnS semiconductor increases from 6.31×1014 cm^-3 (x=0.03) to 7.27×1015 cm^-3 (x=0.06) at room temperature. The maximum electrical conductivity of 408 S^-m^-1 and the relatively high Seebeck coefficient of ^-553 μV^-K^-1 are obtained at 823 K for x=0.05 sample, which produces the maximum power factor of 1.2 μW·cm^-1·K^-2. Addition of Cl^- can introduce point defects to scatter phonons, which makes the lattice thermal conductivity reduce from 0.67 W·m^-1·K^-1 (x=0) to 0.5 W·m^-1·K^-1 (x=0.02). The highest ZT^0.17 is obtained at 823 K for x=0.04 sample, which is 70% higher than that (ZT^0.1) of the pristine SnS.

关 键 词：SNS Cl掺杂 N型半导体 热电性能 

分 类 号：TB34[一般工业技术—材料科学与工程]