Maldistribution of Chemical Bond Strength Inducing Exceptional Anisotropy of Thermal Conductivity in Non‐Layered Materials

Hua, Yang; Bai, Wei; Dai, Shengnan; He, Rongjie; Nan, Pengfei; Liang, Sun; Yang, Jiong; Sun, Bo; Ge, Binghui; Xiao, Chong; Xie, Yi

doi:10.1002/anie.202303081

Cited by 6 publications

(3 citation statements)

References 53 publications

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“…The low dimensionality of both structures (1D for PbSnS 3 and 2D for PbSnS 2 ), characterized by weak Pb···S interchain interactions in PbSnS 3 and weak interlayer (Pb,Sn)–L···(Pb,Sn) interactions via the L lone pair of electrons of divalent cations in PbSnS 2 , supports this statement. Similar conclusions have been also reported recently by Hua et al in their study of the anisotropic transport properties of PbSnS 3 single crystals. However, the authors considered PbSnS 3 to have a “ nonlayered structure ”, i.e., a 3D structure, with the high contrast of chemical bond strength (“ maldistribution” ) between the intra Sn–S bonds and inter Pb···S interactions.…”

Section: Resultssupporting

confidence: 91%

Structure Low Dimensionality and Lone-Pair Stereochemical Activity: the Key to Low Thermal Conductivity in the Pb–Sn–S System

Acharyya,

Pal,

Zhang

et al. 2024

J. Am. Chem. Soc.

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Recently, metal sulfides have begun to receive attention as potential cost-effective materials for thermoelectric applications beyond optoelectronic and photovoltaic devices. Herein, based on a comparative analysis of the structural and transport properties of 2D PbSnS 2 and 1D PbSnS 3 , we demonstrate that the intrinsic effects that govern the low lattice thermal conductivity (κ L ) of these sulfides originate from the combination of the low dimensionality of their crystal structures with the stereochemical activity of the lone-pair electrons of cations. The presence of weak bonds in these materials, responsible for phonon scattering, results in inherently low κ L of 1.0 W/m K in 1D PbSnS 3 and 0.6 W/m K in 2D PbSnS 2 at room temperature. However, the nature of the thermal transport is quite distinct. 1D PbSnS 3 exhibits a higher thermal conductivity with a crystallinelike peak at low temperatures, while 2D PbSnS 2 demonstrates glassy thermal conductivity in the entire temperature range investigated. First-principles density functional theory calculations reveal that the presence of antibonding states below the Fermi level, especially in PbSnS 2 , contributes to the very low κ L . In addition, the calculated phonon dispersions exhibit very soft acoustic phonon branches that give rise to soft lattices and very low speeds of sounds.

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Section: Resultssupporting

confidence: 91%

Structure Low Dimensionality and Lone-Pair Stereochemical Activity: the Key to Low Thermal Conductivity in the Pb–Sn–S System

Acharyya,

Pal,

Zhang

et al. 2024

J. Am. Chem. Soc.

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“…We note that the attempt to obtain the superlattice without Fe and Sb is unsuccessful, leading to the product of PbSnS 3 , which is an orthorhombic ternary sulfide. 35 Measurement of the Thermal Conductivity of Hot-Pressed Samples. The obtained material was ground and then hot-pressed into a pallet at 773 K and 80 MPa.…”

Section: ■ Conclusionmentioning

confidence: 99%

Interlayer Phonon Coupling from Heavy and Light Sublayers in a Natural Van der Waals Superlattice

Bai,

Hua,

Nan

et al. 2023

J. Am. Chem. Soc.

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Layered compounds characterized by van der Waals gaps are often associated with relatively weak interlayer particle interactions. However, in specific scenarios, these seemingly feeble forces can exert an impact on interlayer interactions through subtle energy fluctuations, which can give rise to a diverse range of physical and chemical properties, particularly intriguing in the context of thermal transport. In this study, taking a natural superlattice composed of alternately stacked PbS and SnS 2 sublayers as a model, we proposed that in a superlattice, there is strong hybridization between acoustic phonons of heavy sublayers and optical phonons of light sublayers. We identified newly generated vibration modes in the superlattice, such as interlayer shear and breathing, which exhibit lower sound velocity and contribute less to heat transport compared to their parent materials, which significantly alters the thermal behaviors of the superlattice compared to its bulk counterparts. Our findings on the behavior of interlayer phonons in superlattices not only can shed light on developing functional materials with enhanced thermal dissipation capabilities but also contribute to the broader field of condensed matter physics, offering insights into various fields, including thermoelectrics and phononic devices, and may pave the way for technological advancements in these areas.

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“…Electronic copy available at: https://ssrn.com/abstract=4546830 P r e p r i n t n o t p e e r r e v i e w e d For instance, ZTE requests negligible lattice anharmonicity, whereas low thermal conductivity oppositely desires high lattice anharmonicity. [23] In terms of prototypical NTE materials with low thermal conductivity, they demonstrate so inferior electrical conductivities (as low as 10 -6 S/cm) that they are incapable of effective electrical conduction. [24,25] As regard NTE alloys, their high electrical conductivities are prone to result in unexpectedly overhigh thermal conductivity, disabling to resist thermal shock.…”

Section: Introductionmentioning

confidence: 99%

Integrating Abnormal Thermal Expansion and Ultralow Thermal Conductivity into (Cd,Ni)2re2o7 Via Synergy of Local Structure Distortion and Soft Acoustic Phonons

Qin,

Hu,

Zhu

et al. 2023

Preprint

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Maldistribution of Chemical Bond Strength Inducing Exceptional Anisotropy of Thermal Conductivity in Non‐Layered Materials

Cited by 6 publications

References 53 publications

Structure Low Dimensionality and Lone-Pair Stereochemical Activity: the Key to Low Thermal Conductivity in the Pb–Sn–S System

Structure Low Dimensionality and Lone-Pair Stereochemical Activity: the Key to Low Thermal Conductivity in the Pb–Sn–S System

Interlayer Phonon Coupling from Heavy and Light Sublayers in a Natural Van der Waals Superlattice

Integrating Abnormal Thermal Expansion and Ultralow Thermal Conductivity into (Cd,Ni)2re2o7 Via Synergy of Local Structure Distortion and Soft Acoustic Phonons

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