期刊
CHEMISTRY OF MATERIALS
卷 30, 期 16, 页码 5639-5647出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.8b01914
关键词
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资金
- Center for Hierarchical Materials Design
- U.S. Department of Commerce, National Institute of Standards and Technology [70NANB14H012]
- U.S. Department of Energy, Office of Science and Office of Basic Energy Sciences [DE-SC0014520]
- National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility [DE-AC02-05CH11231]
A high power factor and low lattice thermal conductivity are two essential ingredients of highly efficient thermoelectric materials. Although monolayers of transition-metal dichalcogenides possess high power factors, high lattice thermal conductivities significantly impede their practical applications. Our first-principles calculations show that these two ingredients are well fulfilled in the recently synthesized Pd2Se3 monolayer, whose crystal structure is composed of [Se-2](2-) dimers, Se2- anions, and Pd2+ cations coordinated in a square-planar manner. Our detailed analysis of third-order interatomic force constants reveals that the anharmonicity and soft phonon modes associated with covalently bonded [Se-2](2-) dimers lead to ultralow lattice thermal conductivities in Pd2Se3 monolayers (1.5 and 2.9 W m(-1) K-1 along the a- and b-axes at 300 K, respectively), which are comparable to those of high-performance bulk thermoelectric materials such as PbTe. Moreover, the pudding-mold type band structure, caused by Pd2+ (d(8)) cations coordinated in a square-planar crystal field, leads to high power factors in Pd2Se3 monolayers. Consequently, both electron- and hole-doped thermoelectric materials with a considerably high zT can be achieved at moderate carrier concentrations, suggesting that Pd2Se3 is a promising two-dimensional thermoelectric material. Our results suggest that hierarchical chemical bonds, that is, coexistence of different types of chemical bonds, combined with a square-planar crystal field is a promising route for designing high-efficiency thermoelectric materials.
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