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A simple chemical guide for finding novel n-type dopable Zintl pnictide thermoelectric materials
P. Gorai, , E.S. Toberer, V. Stevanović
Published in Royal Society of Chemistry
2019
Volume: 7
   
Issue: 33
Pages: 19385 - 19395
Abstract
Computations have predicted good thermoelectric performance for a number of Zintl phases when doped n-type. Combined with the successful experimental realization of n-type KGaSb4, KAlSb4, and Mg3Sb2 with zT ≳ 1, this has fueled efforts to discover novel n-type dopable Zintl phases. However, a majority of Zintl phases exhibit strong proclivity toward p-type doping and prior successes in finding n-type dopable Zintls were largely serendipitous. Herein we use modern first-principles defect calculations to study trends in the dopability of Zintl pnictides and find that the average oxidation state of the anion is a useful chemical guide to identify novel n-type dopable phases. Specifically, we observe that Zintl pnictides with average oxidation of the anion near -1 are n-type dopable. The trend is mainly a consequence of the high formation energy of native acceptor defects (e.g. cation vacancies) and the resulting absence of charge (electron) compensation. Using the oxidation state guide in conjunction with a descriptor of thermoelectric performance, we conduct a large-scale materials search and identify promising candidates that are n-type dopable. © 2019 The Royal Society of Chemistry.
About the journal
JournalJournal of Materials Chemistry A
PublisherRoyal Society of Chemistry
ISSN20507488