Synergistic effect of bonding heterogeneity and phonon localization in introducing excellent thermoelectric properties in layered heteroanionic NdZnSbO material

IF 13.1 1区 化学 Q1 Energy
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Abstract

Layered rare-earth metal oxides, harnessing the dual properties of oxides and two-dimensional layered materials, exhibit remarkable thermal stability and quantum confinement effects. Therefore, this work adopts the first-principles calculation combined with the Boltzmann transport theory to predict the thermoelectric properties of NdZnSbO compound. The coexistence of weak interlayer van der Waals interactions, robust intralayer ionic bonding, and partial covalent bonding leads to remarkable bonding heterogeneity, which engenders pronounced phonon scattering and imposes constraints on thermal transport along the out-of-plane direction. The weakened chemical bonds induced by the antibonding states, together with the rattling-like behavior of the Zn atom, culminate in the profound anharmonicity in the layered NdZnSbO compound. The weakening bond and heavy element contribute to the softness of phonon modes, which significantly diminishes the phonon group velocity. The redistribution-dominated four-phonon scattering process spans a large optical gap, which effectively reduces the lattice thermal conductivity. The NdZnSbO compound exhibits direct semiconductor characteristic with a bandgap of 0.73 eV by adopting the Heyd-Scuseria-Ernzerhof (HSE06) functional in combination with spin–orbit coupling (SOC) effect. The multi-valley feature of NdZnSbO compound augur favorably for band degeneracy, thus amplifying the power factor. Consequently, an optimal figure-of-merit (ZT) of 3.40 at 900 K is achieved for the n-type NdZnSbO compound. The present study delves deeply insights into the origins for the low thermal conductivity of NdZnSbO compound and proposes an optimization scheme to enhance overall thermoelectric performance.

Abstract Image

在层状异阴离子 NdZnSbO 材料中引入优异热电性能的成键异质性和声子定位协同效应
层状稀土金属氧化物具有氧化物和二维层状材料的双重特性,具有显著的热稳定性和量子约束效应。因此,本研究采用第一性原理计算结合玻尔兹曼输运理论来预测 NdZnSbO 化合物的热电性能。弱层间范德华相互作用、强层内离子键和部分共价键的共存导致了显著的成键异质性,从而产生了明显的声子散射,并对沿平面外方向的热传输造成了限制。反键态引起的化学键弱化,加上锌原子的嘎嘎作响行为,最终导致层状 NdZnSbO 化合物产生了深刻的非谐波性。键和重元素的削弱导致声子模式的软化,从而大大降低了声子的群速度。以再分布为主的四声子散射过程跨越了很大的光隙,从而有效降低了晶格热导率。通过采用 Heyd-Scuseria-Ernzerhof (HSE06) 函数并结合自旋轨道耦合(SOC)效应,NdZnSbO 化合物显示出直接半导体特性,其带隙为 0.73 eV。NdZnSbO 化合物的多谷特征有利于实现带变性,从而放大功率因数。因此,n 型 NdZnSbO 化合物在 900 K 时的最佳功率因数(ZT)达到了 3.40。本研究深入探讨了 NdZnSbO 化合物热导率低的原因,并提出了一种优化方案,以提高整体热电性能。
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来源期刊
Journal of Energy Chemistry
Journal of Energy Chemistry CHEMISTRY, APPLIED-CHEMISTRY, PHYSICAL
CiteScore
19.10
自引率
8.40%
发文量
3631
审稿时长
15 days
期刊介绍: The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies. This journal focuses on original research papers covering various topics within energy chemistry worldwide, including: Optimized utilization of fossil energy Hydrogen energy Conversion and storage of electrochemical energy Capture, storage, and chemical conversion of carbon dioxide Materials and nanotechnologies for energy conversion and storage Chemistry in biomass conversion Chemistry in the utilization of solar energy
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