Beyond rattling: tetrahedrites as incipient ionic conductorsMukherjee, 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
It is advisable to refer to the publisher's version if you intend to cite from this work. See Guidance on citing. To link to this item DOI: 10.1002/adma.202306088 Abstract/SummaryMaterials 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.
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