Intrinsically low thermal conductivity from a quasi-one-dimensional crystal structure and enhanced electrical conductivity network via Pb doping in SbCrSe3

Abstract

The development of new routes for the production of thermoelectric materials with low-cost and high-performance characteristics has been one of the long-term strategies for saving and harvesting thermal energy. Herein, we report a new approach for improving thermoelectric properties by employing the intrinsically low thermal conductivity of a quasi-one-dimensional (quasi-1D) crystal structure and optimizing the power factor with aliovalent ion doping. As an example, we demonstrated that SbCrSe 3 , in which two parallel chains of CrSe 6 octahedra are linked by antimony atoms, possesses a quasi-1D property that resulted in an ultra-low thermal conductivity of 0.56 W m − 1 K − 1 at 900 K. After maximizing the power factor by Pb doping, the peak ZT value of the optimized Pb-doped sample reached 0.46 at 900 K, which is an enhancement of 24 times that of the parent SbCrSe 3 structure. The mechanisms that lead to low thermal conductivity derive from anharmonic phonons with the presence of the lone-pair electrons of Sb atoms and weak bonds between the CrSe 6 double chains. These results shed new light on the design of new and high-performance thermoelectric materials.

Sodium‐Doped Tin Sulfide Single Crystal: A Nontoxic Earth‐Abundant Material with High Thermoelectric Performance

“…Lowering the lattice thermal conductivity (κ L ), which is relatively independent of other parameters, is a comparatively easy method. Other well‐documented methods for enhancing phonon scattering include nanostructuring, dislocations, point defects, and strong lattice anharmonicity . Additional strategies to boost the power factor ( S 2 ρ −1 ) include carrier concentration optimization, band convergence, and creating band resonance levels…”

“…Fortunately, in the past decade, several general strategies have been developed to achieve high zT in various materials. [18][19][20] Additional strategies to boost the power factor (S 2 ρ −1 ) include carrier concentration optimization, [21,22] band convergence, [23,24] and creating band resonance levels. Other well-documented methods for enhancing phonon scattering include nanostructuring, [9][10][11] dislocations, [12,13] point defects, [14][15][16][17] and strong lattice anharmonicity.…”

Identification of vibrational mode symmetry and phonon anharmonicity in SbCrSe3 single crystal using Raman spectroscopy

“…Low-dimensional bulk materials that have a quasi-onedimensional (1D) or 2D structure have received growing research attention owing to their extraordinary electronic and thermal properties; they have emerged as highly attractive candidates used for next-generation electronic, optoelectronic, and thermoelectric devices [1][2][3][4][5][6][7][8]. In particular, low-dimensional intrinsic magnetic semiconductors-CrMX 3 ternary chromium trichalcogenides (M as a non-transition metal and X = S, Se or Te) have attracted considerable research interest in the magnetism and thermoelectricity fields owing to their appropriate band gaps and intrinsically low lattice thermal conductivity (κ L ) [9][10][11][12][13][14][15]. Intriguingly, the crystal structures of these compounds, by virtue of the different arrangements of CrX 6 octahedra, can transform from a quasi-2D layered structure into a 1D needlelike structure.…”

Ab Initio Study of Optoelectronic and Magnetic Properties of Ternary Chromium Chalcogenides

“…Because of the presence of chromium, these materials tend to exhibit magnetic properties and have recently seen a resurgence of interest [17,18]. Several of these materials, such as SbCrS 3 [19], SbCrSe 3 [18][19][20], and SiCrTe 3 [21,22], have been the subjects of recent experimental studies as magnetic materials with metallic or semiconducting behavior. However, many of these materials, including many of the lanthanide chromium sulfides, have not been thoroughly studied even though their syntheses have been reported a long time ago [11].…”