Realizing Intrinsically Ultralow and Glass‐Like Thermal Transport via Chemical Bonding Engineering
Abstract Crystals exhibiting glass‐like and low lattice thermal conductivity (κL) are not only scientifically intriguing but also practically valuable in various applications, including thermal barrier coatings, thermoelectric energy conversion, and thermal management. However, such unusual κL are t...
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Wiley
2025-05-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202417292 |
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| author | Zhonghao Xia Xingchen Shen Jun Zhou Yuling Huang Yali Yang Jiangang He Yi Xia |
| author_facet | Zhonghao Xia Xingchen Shen Jun Zhou Yuling Huang Yali Yang Jiangang He Yi Xia |
| author_sort | Zhonghao Xia |
| collection | DOAJ |
| description | Abstract Crystals exhibiting glass‐like and low lattice thermal conductivity (κL) are not only scientifically intriguing but also practically valuable in various applications, including thermal barrier coatings, thermoelectric energy conversion, and thermal management. However, such unusual κL are typically observed only in compounds containing heavy elements, with large unit cells, or at high temperatures. In this study, chemical bonding principles are utilized to weaken the Ag–Ag bonds and enhance lattice anharmonicity. The incorporation of a chalcogen anion as a bridge ligand is proposed to facilitate phonon rattling in Ag6‐octahedron‐based compounds. Guided by this design strategy, five Ag6 octahedron‐based compounds, AAg3X2 (A = Li, Na, and K; X = S and Se), which are characterized by low average atomic masses and exhibit exceptionally strong four‐phonon scattering, are theoretically identified. Consequently, these compounds demonstrate ultralow thermal conductivities (0.3–0.6 W m−1 K−1) with minimal temperature dependence (T−0.1) across a wide temperature range. Experimental validation confirms that the κL of NaAg3S2 is 0.45 W m−1 K−1 within the temperature range of 200–550 K. The results clearly demonstrate that weak chemical bonding plays a crucial role in designing compounds with glass‐like κL, highlighting the effectiveness of chemical bonding engineering in achieving desired thermal transport properties. |
| format | Article |
| id | doaj-art-74433ea84c874c639b6f3ccecfa3e19a |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-74433ea84c874c639b6f3ccecfa3e19a2025-08-20T03:48:47ZengWileyAdvanced Science2198-38442025-05-011217n/an/a10.1002/advs.202417292Realizing Intrinsically Ultralow and Glass‐Like Thermal Transport via Chemical Bonding EngineeringZhonghao Xia0Xingchen Shen1Jun Zhou2Yuling Huang3Yali Yang4Jiangang He5Yi Xia6Key Laboratory of Advanced Materials and Devices for Post‐Moore Chips Ministry of Education School of Mathematics and Physics University of Science and Technology Beijing Beijing 100083 ChinaCRISMAT, CNRS ENSICAEN Caen 14000 FranceBasic Experimental Center for Natural Science University of Science and Technology Beijing Beijing 100083 ChinaDepartment of Mechanical and Energy Engineering Southern University of Science and Technology (SUSTech) Shenzhen 518055 ChinaKey Laboratory of Advanced Materials and Devices for Post‐Moore Chips Ministry of Education School of Mathematics and Physics University of Science and Technology Beijing Beijing 100083 ChinaKey Laboratory of Advanced Materials and Devices for Post‐Moore Chips Ministry of Education School of Mathematics and Physics University of Science and Technology Beijing Beijing 100083 ChinaDepartment of Mechanical & Materials Engineering Portland State University Portland OR 97201 USAAbstract Crystals exhibiting glass‐like and low lattice thermal conductivity (κL) are not only scientifically intriguing but also practically valuable in various applications, including thermal barrier coatings, thermoelectric energy conversion, and thermal management. However, such unusual κL are typically observed only in compounds containing heavy elements, with large unit cells, or at high temperatures. In this study, chemical bonding principles are utilized to weaken the Ag–Ag bonds and enhance lattice anharmonicity. The incorporation of a chalcogen anion as a bridge ligand is proposed to facilitate phonon rattling in Ag6‐octahedron‐based compounds. Guided by this design strategy, five Ag6 octahedron‐based compounds, AAg3X2 (A = Li, Na, and K; X = S and Se), which are characterized by low average atomic masses and exhibit exceptionally strong four‐phonon scattering, are theoretically identified. Consequently, these compounds demonstrate ultralow thermal conductivities (0.3–0.6 W m−1 K−1) with minimal temperature dependence (T−0.1) across a wide temperature range. Experimental validation confirms that the κL of NaAg3S2 is 0.45 W m−1 K−1 within the temperature range of 200–550 K. The results clearly demonstrate that weak chemical bonding plays a crucial role in designing compounds with glass‐like κL, highlighting the effectiveness of chemical bonding engineering in achieving desired thermal transport properties.https://doi.org/10.1002/advs.202417292chemical bonding principleslattice thermal conductivitymaterial design and discoverysolid state chemistry |
| spellingShingle | Zhonghao Xia Xingchen Shen Jun Zhou Yuling Huang Yali Yang Jiangang He Yi Xia Realizing Intrinsically Ultralow and Glass‐Like Thermal Transport via Chemical Bonding Engineering Advanced Science chemical bonding principles lattice thermal conductivity material design and discovery solid state chemistry |
| title | Realizing Intrinsically Ultralow and Glass‐Like Thermal Transport via Chemical Bonding Engineering |
| title_full | Realizing Intrinsically Ultralow and Glass‐Like Thermal Transport via Chemical Bonding Engineering |
| title_fullStr | Realizing Intrinsically Ultralow and Glass‐Like Thermal Transport via Chemical Bonding Engineering |
| title_full_unstemmed | Realizing Intrinsically Ultralow and Glass‐Like Thermal Transport via Chemical Bonding Engineering |
| title_short | Realizing Intrinsically Ultralow and Glass‐Like Thermal Transport via Chemical Bonding Engineering |
| title_sort | realizing intrinsically ultralow and glass like thermal transport via chemical bonding engineering |
| topic | chemical bonding principles lattice thermal conductivity material design and discovery solid state chemistry |
| url | https://doi.org/10.1002/advs.202417292 |
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