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Deformation and Failure Mechanisms of Thermoelectric Type-I Clathrate Ba₈Au₆Ge₄₀

Zhang, Xiaolian and Zhai, Pengcheng and Huang, Xiege and Morozov, Sergey I. and Duan, Bo and Li, Wenjuan and Chen, Gang and Li, Guodong and Goddard, William A., III (2022) Deformation and Failure Mechanisms of Thermoelectric Type-I Clathrate Ba₈Au₆Ge₄₀. ACS Applied Materials & Interfaces, 14 (3). pp. 4326-4334. ISSN 1944-8244. doi:10.1021/acsami.1c22730. https://resolver.caltech.edu/CaltechAUTHORS:20220113-233466947

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[img] PDF (Supercells employed to perform the ⟨100⟩, ⟨110⟩, ⟨111⟩ tension and {100}/⟨010⟩, {110}/⟨001⟩, {111}/⟨2–1–1⟩ shearing calculations; the entire bond lengths’ evolution of the tetrakaidecahedral cage framework; and the calculation details of the fracture...) - Supplemental Material
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Abstract

Type-I clathrate Ba₈Au₆Ge₄₀, possessing an interesting structure stacked by polyhedrons, is a potential “phonon-glass, electron-crystal” thermoelectric material. However, the mechanical properties of Ba₈Au₆Ge₄₀ vital for industrial applications have not been clarified. Here, we report the first density functional theory calculations of the intrinsic mechanical properties of thermoelectric clathrate Ba₈Au₆Ge₄₀. Among the different loading directions, the {110}/⟨001⟩ shearing and ⟨110⟩ tension are the weakest, with strengths of 4.51 and 6.64 GPa, respectively. Under {110}/⟨001⟩ shearing, the Ge–Ge bonds undergo significant stretching and twisting, leading to a severe distortion of the tetrakaidecahedral cage, giving rise to the fast softening of the flank Au–Ge bonds. At a strain of 0.2655, the Au–Ge bonds suddenly break, resulting in the collapse of the cage and the failure of the material. Under a ⟨110⟩ tension, the stretching of the Ge–Ge bonds keeps accelerating the softening of the Au–Ge bonds in the top/bottom hexagons, which releases the stress and disables the structure. The Au–Ge bonds are more rigid, contributing two-thirds of the structural deformation resistance. This work provides a new insight to understand the failure mechanisms of type-I clathrates with varied framework constitutions, which should help inform the design of robust thermoelectric clathrate materials.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsami.1c22730DOIArticle
ORCID:
AuthorORCID
Zhai, Pengcheng0000-0002-5737-5220
Morozov, Sergey I.0000-0001-6226-5811
Duan, Bo0000-0003-0536-843X
Li, Guodong0000-0002-4761-6991
Goddard, William A., III0000-0003-0097-5716
Alternate Title:Deformation and Failure Mechanisms of Thermoelectric Type-I Clathrate Ba8Au6Ge40
Additional Information:© 2022 American Chemical Society. Received: November 23, 2021; Accepted: January 4, 2022; Published: January 12, 2022. This work was supported by the National Natural Science Foundation of China (nos. 52022074; 92163119, and 92163215), the Hubei Provincial Natural Science Foundation of China (2020CFB202), and the Fundamental Research Funds for the Central Universities (WUT: 2021III058). S.M. is thankful for the support by the Supercomputer Simulation Laboratory of South Ural State University. WAG thanks the US Office of Naval Research (ONR N00014-19-1-2081) for support. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China52022074
National Natural Science Foundation of China92163119
National Natural Science Foundation of China92163215
Natural Science Foundation of Hubei Province2020CFB202
Central University Basic Research Fund of ChinaWUT: 2021III058
Office of Naval Research (ONR)N00014-19-1-2081
Subject Keywords:thermoelectric clathrate; DFT; stress−strain; deformation mode; elastic properties; fracture toughness
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1533
Issue or Number:3
DOI:10.1021/acsami.1c22730
Record Number:CaltechAUTHORS:20220113-233466947
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20220113-233466947
Official Citation:Deformation and Failure Mechanisms of Thermoelectric Type-I Clathrate Ba8Au6Ge40. Xiaolian Zhang, Pengcheng Zhai, Xiege Huang, Sergey I. Morozov, Bo Duan, Wenjuan Li, Gang Chen, Guodong Li, and William A. Goddard. ACS Applied Materials & Interfaces 2022 14 (3), 4326-4334; DOI: 10.1021/acsami.1c22730
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:112887
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:13 Jan 2022 14:40
Last Modified:12 Oct 2022 03:49

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  • Zhang, Xiaolian and Zhai, Pengcheng and Huang, Xiege and Morozov, Sergey I. and Duan, Bo and Li, Wenjuan and Chen, Gang and Li, Guodong and Goddard, William A., III Deformation and Failure Mechanisms of Thermoelectric Type-I Clathrate Ba₈Au₆Ge₄₀. (deposited 13 Jan 2022 14:40) [Currently Displayed]

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