Modulation doping of p-type Cu12Sb4S13 toward improving thermoelectric performance

Khak Ho Lim ¹Mingquan Li ²Yu Zhang ³Yue Wu ⁴Qimin Zhou ¹Qingyue Wang ¹Xuan Yang ⁵Pingwei Liu ⁵Wen-Jun Wang ⁵Ka Wai Wong ⁶Ka Ming Ng ⁷Yu Liu ²Andreu Cabot⁸

扫码查看

作者信息

1. Institute of Zhejiang University-Quzhou,Quzhou 324000,China;College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310007,China
2. School of Chemistry and Chemical Engineering,Hefei University of Technology,Hefei 230009,China
3. Materials Research Institute,The Pennsylvania State University,University Park,PA 16802,USA
4. Institute of Zhejiang University-Quzhou,Quzhou 324000,China
5. College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310007,China
6. Ostia Technologies Limited,United Kingdom
7. Department of Chemical and Biological Engineering,The Hong Kong University of Science and Technology,Clear Water Bay,Hong Kong,China
8. ICREA,Pg.Lluis Companys 23,Barcelona 08010,Spain;Catalonia Energy Research Institute-IREC,Sant Adria del Besos,Barcelona 08930,Spain
折叠

Abstract

The commercial viability of thermoelectric(TE)devices relies heavily on two factors:cost reduction and efficiency enhancement.In this study,we first produce p-type Cu12Sb4S16-x(x=0,3,4)using a low-temperature bottom-up approach and demonstrate Cu12Sb4S13 to show the best TE performance among the three tested compositions.Subsequently,the TE energy conversion efficiency of Cu12Sb4S13 is further enhanced by optimizing its electronic band structure through the incorporation of small amounts of tel-lurium.At an optimal Te content of 5 mol％,more than a twofold increase in the TE figure of merit(zT)is obtained.To gain insight into the mechanism of improvement on the transport properties of the mate-rial,we compare the interphase transport mechanism by incorporating nanodomains of different metals(Ag and Cu)into the Cu12Sb4S13 matrix.The improved electrical conductivity obtained with Cu12Sb4S13-Te nanocomposites is attributed to a charge flooding of the Cu12Sb4S13 surface.In contrast,excessive down-ward band-bending at the interphases of Ag/Cu metal-semiconductor drastically reduces the electrical conductivity.Besides,a weighted mobility(μw)analysis shows a dominant thermal activation of carri-ers in Cu12Sb4S13-Te nanocomposites.In this material,a strong decrease in lattice thermal conductivity is also found,which is associated with a phonon-carrier scattering mechanism.Our work shows the impor-tance of proper band-engineering in TE nanocomposites to decouple electrical and thermal transport to enhance TE performance,and the efficacy of μw for electrical and thermal transport analysis.

Key words

Modulation doping/Thermoelectric/Interphase transport/Charge flooding/Phonon-carrier scattering

引用本文复制引用

基金项目

National Natural Science Foundation of China(22208293)

Research Funds of the Institute of Zhejiang University-Quzhou(IZQ2021RCZX003)

Research Funds of the Institute of Zhejiang University-Quzhou(IZQ2021RCZX002)

Research Funds of the Institute of Zhejiang University-Quzhou(IZQ2021KJ2024)

Research Funds of the Institute of Zhejiang University-Quzhou(IZQ2022KYZX09)

State Key Laboratory of Fluorinated Greenhouse gases Replacement and Treatment(SKLFGGRT2022001)

State Key Laboratory of Electrical Insulation and Power Equipment(EIPE23201)

National Natural Science Foundation of China(NSFC)(22209034)

Innovation and Entrepreneurship Project of Overseas Returnees in Anhui Province(2022LCX002)

出版年

2024

材料科学技术(英文版)

中国金属学会中国材料研究学会中国科学院金属研究所

材料科学技术(英文版)

CSTPCD

影响因子：0.657

ISSN：1005-0302

参考文献量51

段落导航