Rhombohedral polytypes of the layered honeycomb delafossites with optical brilliance in the visible

Inorganic Chemistry
J H RoudebushR J Cava

Abstract

We report the synthesis of the Delafossite honeycomb compounds Cu3Ni2SbO6 and Cu3Co2SbO6 via a copper topotactic reaction from the layered α-NaFeO2-like precursors Na3Ni2SbO6 and Na3Co2SbO6. The low-temperature exchange reaction exclusively produces the rhombahedral 3R polytype subcell, whereas only the hexagonal 2H polytype subcell has been made by conventional synthesis. The thus-synthesized 3R variants are visually striking; they are bright lime-green (Ni variant) and terracotta-orange (Co variant), while both of the conventionally synthesized 2H variants have a burnt-red color. The new structures are characterized by powder X-ray diffraction and Rietveld analysis as well as magnetic susceptibility, X-ray photoelectron spectroscopy (XPS), and diffuse-reflectance optical spectroscopy. Using thermogravimetric analysis, we identify a second order 3R → 2H phase transition as well as a first-order structural transition associated with rearrangement of the honeycomb stacking layers. The optical absorbance spectra of the samples show discrete edges that correlate well to their visual colors. Exposing Cu3Ni2SbO6 to O2 and heat causes the sample to change color. XPS confirms the presence of Cu(2+) in these samples, which implies that...Continue Reading

References

Jun 13, 2006·Nature Materials·Minhyea LeeN P Ong
Apr 20, 2011·Inorganic Chemistry·R BerthelotC Delmas
Jan 11, 2014·Journal of the American Chemical Society·Jing GuAndrew B Bocarsly
Jul 19, 2012·The Journal of Physical Chemistry Letters·Carrie G ReadKyoung-Shin Choi

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Citations

Jul 28, 2015·Inorganic Chemistry·Rebecca W SmahaRobert J Cava
Apr 1, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·E A ZverevaA N Vasiliev
May 31, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Dileep Kumar YadavS Uma
Feb 13, 2021·Chemical Society Reviews·Godwill Mbiti KanyoloHajime Matsumoto

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