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Beyond rattling: tetrahedrites as incipient ionic conductors

Mukherjee, S., Voneshen, D. J., Duff, A., Goodard, P., Powell, A. V. and Vaqueiro, P. ORCID: https://orcid.org/0000-0001-7545-6262 (2023) Beyond rattling: tetrahedrites as incipient ionic conductors. Advanced Materials, 35 (44). 2306088. ISSN 1521-4095

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To link to this item DOI: 10.1002/adma.202306088

Abstract/Summary

Materials with ultralow thermal conductivity are crucial to many technological applications, including thermoelectric energy harvesting, thermal barrier coatings, and optoelectronics. Liquid-like mobile ions are effective at disrupting phonon propagation, hence suppressing thermal conduction. However, high ionic mobility leads to degradation of liquid-like thermoelectric materials under operating conditions due to ion migration and metal deposition at the cathode, hindering their practical application. Here, we identify a new type of behaviour, incipient ionic conduction, which leads to ultralow thermal conductivity, while overcoming the issues of degradation inherent in liquid-like materials. Using neutron spectroscopy and molecular-dynamics simulations, we demonstrate that in tetrahedrite, an established thermoelectric material with a remarkably low thermal conductivity, copper ions although mobile above 200 K, are predominantly confined to cages within the crystal structure. Hence the undesirable migration of cations to the cathode can be avoided. These findings unveil a new approach for the design of materials with ultralow thermal conductivity, by exploring systems in which incipient ionic conduction may be present.

Item Type:Article
Refereed:Yes
Divisions:Life Sciences > School of Chemistry, Food and Pharmacy > Department of Chemistry
Interdisciplinary centres and themes > Energy Research
Interdisciplinary centres and themes > Chemical Analysis Facility (CAF) > Xray (CAF)
ID Code:112937
Publisher:Wiley

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