TY - JOUR
T1 - Accelerated Discovery and Design of Ultralow Lattice Thermal Conductivity Materials Using Chemical Bonding Principles
AU - He, Jiangang
AU - Xia, Yi
AU - Lin, Wenwen
AU - Pal, Koushik
AU - Zhu, Yizhou
AU - Kanatzidis, Mercouri G.
AU - Wolverton, Chris
N1 - Funding Information:
J.H. and Y.X. contributed equally to this work. The authors acknowledge support by the U.S. Department of Energy, Office of Science and Office of Basic Energy Sciences, under Award No. DE‐SC0014520 for lattice thermal conductivity calculations and the Center for Hierarchical Materials Design (CHiMaD) and from the U.S. Department of Commerce, National Institute of Standards and Technology, under Award No. 70NANB14H012 for materials screening. M.G.K. acknowledges support from the National Science Foundation through Grant DMR‐2003476 for materials exploration work. This research used computer resources from the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE‐AC02‐05CH11231, the Extreme Science and Engineering Discovery Environment, which is supported by National Science Foundation grant number ACI‐1548562, and the Quest high performance computing facility at Northwestern University.
Publisher Copyright:
© 2021 Wiley-VCH GmbH.
PY - 2022/4/4
Y1 - 2022/4/4
N2 - Semiconductors with very low lattice thermal conductivities are highly desired for applications relevant to thermal energy conversion and management, such as thermoelectrics and thermal barrier coatings. Although the crystal structure and chemical bonding are known to play vital roles in shaping heat transfer behavior, material design approaches of lowering lattice thermal conductivity using chemical bonding principles are uncommon. In this work, an effective strategy of weakening interatomic interactions and therefore suppressing lattice thermal conductivity based on chemical bonding principles is presented and a high-efficiency approach of discovering low κL materials by screening the local coordination environments of crystalline compounds is developed. The resulting first-principles calculations uncover 30 hitherto unexplored compounds with (ultra)low lattice thermal conductivities from 13 prototype crystal structures contained in the Inorganic Crystal Structure Database. Furthermore, an approach of rationally designing high-performance thermoelectrics is demonstrated by additionally incorporating cations with stereochemically active lone-pair electrons. These results not only provide atomic-level insights into the physical origin of the low lattice thermal conductivity in a large family of copper/silver-based compounds but also offer an efficient approach to discover and design materials with targeted thermal transport properties.
AB - Semiconductors with very low lattice thermal conductivities are highly desired for applications relevant to thermal energy conversion and management, such as thermoelectrics and thermal barrier coatings. Although the crystal structure and chemical bonding are known to play vital roles in shaping heat transfer behavior, material design approaches of lowering lattice thermal conductivity using chemical bonding principles are uncommon. In this work, an effective strategy of weakening interatomic interactions and therefore suppressing lattice thermal conductivity based on chemical bonding principles is presented and a high-efficiency approach of discovering low κL materials by screening the local coordination environments of crystalline compounds is developed. The resulting first-principles calculations uncover 30 hitherto unexplored compounds with (ultra)low lattice thermal conductivities from 13 prototype crystal structures contained in the Inorganic Crystal Structure Database. Furthermore, an approach of rationally designing high-performance thermoelectrics is demonstrated by additionally incorporating cations with stereochemically active lone-pair electrons. These results not only provide atomic-level insights into the physical origin of the low lattice thermal conductivity in a large family of copper/silver-based compounds but also offer an efficient approach to discover and design materials with targeted thermal transport properties.
KW - lattice thermal conductivity
KW - material design
KW - thermoelectric materials
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U2 - 10.1002/adfm.202108532
DO - 10.1002/adfm.202108532
M3 - Article
AN - SCOPUS:85121337589
SN - 1616-301X
VL - 32
JO - Advanced Functional Materials
JF - Advanced Functional Materials
IS - 14
M1 - 2108532
ER -