Functional-Unit-Based Material Design: Ultralow Thermal Conductivity in Thermoelectrics with Linear Triatomic Resonant Bonds

Ji, Jialin1; Tang, Qinghang1,2,3; Yao, Mingjia1; Yang, Hongliang4,5; Jin, Yeqing1; Zhang, Yubo4,5,6,7; Xi, Jinyang1,8; Singh, David J.9; Yang, Jiong1; Zhang, Wenqing4,5,6,7

2022-09-01

10.1021/jacs.2c08062

Journal of the American Chemical Society   Impact Factor & Quartile

0002-7863

1520-5126

We demonstrate the use of functional-unit-based material design for thermoelectrics. This is an efficient approach for identifying high-performance thermoelectric materials, based on the use of combinations of functional fragments relevant to desired properties. Here, we reveal that linear triatomic resonant bonds (LTRBs) found in some Zintl compounds provide strong anisotropy both structurally and electronically, along with strong anharmonic phonon scattering. An LTRB is thus introduced as a functional unit, and compounds are then screened as potential thermoelectric materials. We identify 17 semiconducting candi-dates from the MatHub-3d database that contain LTRBs. Detailed transport calculations demonstrate that the LTRB-containing compounds not only have considerably lower lattice thermal conductivities than other compounds with similar average atomic masses, but also exhibit remarkable band anisotropy near the valence band maximums due to the LTRB. K5CuSb2 is adopted as an example to elucidate the fundamental correlation between the LTRB and thermoelectric properties. The [Sb-Cu-Sb]5- resonant structures demonstrate the delocalized Sb-Sb interaction within each LTRB, resulting in the softening of TA phonons and leading to large anharmonicity. The low lattice thermal conductivity (0.39 W/m center dot K at 300 K) combined with the band anisotropy results in a high thermoelectric figure of merit (ZT) for K5CuSb2 of 1.3 at 800 K. This work is a case study of the functional-unit-based material design for the development of novel thermoelectric materials.

SCI

English

NI Journal Papers

Corresponding

Key Research Project of Zhejiang Laboratory[2021PE0AC02] ; National Key Research and Development Program of China[2021YFB3502200] ; National Natural Science Foundation of China["52172216","92163212"] ; 111 Project[D16002]

Chemistry

Chemistry, Multidisciplinary

WOS:000862662400001

AMER CHEMICAL SOC

Web of Science

1.Shanghai Univ, Mat Genome Inst, Shanghai 200444, Peoples R China
2.Wuhan Univ, Key Lab Artificial Micro & Nanostruct, Minist Educ, Wuhan 430072, Peoples R China
3.Wuhan Univ, Sch Phys & Technol, Wuhan 430072, Peoples R China
4.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China
5.Southern Univ Sci & Technol, Shenzhen Inst Quantum Sci & Technol, Shenzhen 518055, Guangdong, Peoples R China
6.Southern Univ Sci & Technol, Shenzhen Municipal Key Lab Adv Quantum Mat & Devic, Shenzhen 518055, Guangdong, Peoples R China
7.Southern Univ Sci & Technol, Guangdong Prov Key Lab Computat Sci & Mat Design, Shenzhen 518055, Guangdong, Peoples R China
8.Zhejiang Lab, Hangzhou 311100, Zhejiang, Peoples R China
9.Univ Missouri, Dept Phys & Astron, Columbia, MO 65211 USA

Ji, Jialin,Tang, Qinghang,Yao, Mingjia,et al. Functional-Unit-Based Material Design: Ultralow Thermal Conductivity in Thermoelectrics with Linear Triatomic Resonant Bonds[J]. Journal of the American Chemical Society,2022.

Ji, Jialin.,Tang, Qinghang.,Yao, Mingjia.,Yang, Hongliang.,Jin, Yeqing.,...&Zhang, Wenqing.(2022).Functional-Unit-Based Material Design: Ultralow Thermal Conductivity in Thermoelectrics with Linear Triatomic Resonant Bonds.Journal of the American Chemical Society.

Ji, Jialin,et al."Functional-Unit-Based Material Design: Ultralow Thermal Conductivity in Thermoelectrics with Linear Triatomic Resonant Bonds".Journal of the American Chemical Society (2022).