Title
Topochemical nitridation with anion vacancy -assisted <tex>$N^{3-}/O^{2-}$</tex> exchangeTopochemical nitridation with anion vacancy -assisted <tex>$N^{3-}/O^{2-}$</tex> exchange
Author
Faculty/Department
Faculty of Sciences. Physics
Research group
Electron microscopy for materials research (EMAT)
Publication type
article
Publication
Washington, D.C.,
Subject
Chemistry
Source (journal)
Journal of the American Chemical Society. - Washington, D.C.
Volume/pages
138(2016):9, p. 3211-3217
ISSN
0002-7863
ISI
000371945800055
Carrier
E
Target language
English (eng)
Full text (Publishers DOI)
Affiliation
University of Antwerp
Abstract
We present how the introduction of anion vacancies in oxyhydrides enables a route to access new oxynitrides, by conducting ammonolysis of perovskite oxyhydride EuTiO3-xHx (x similar to 0.18). At 400 degrees C, similar to our studies on BaTiO3-xHx, hydride lability enables a low temperature direct ammonolysis of EUTi3.82+O-2.82/H-0.18, leading to the N3-/H--exchanged product EuTi4+O2.82No0.12 square 0.06 center dot When the ammonolysis temperature was increased up to 800 degrees C, we observed a further nitridation involving N3-/O2- exchange, yielding a fully oxidized Eu3+Ti4+O2N with the GdFeO3-type distortion (Pnma) as a metastable phase, instead of pyrochlore structure. Interestingly, the same reactions using the oxide EuTiO3 proceeded through a 1:1 exchange of N3- with O-2 only above 600 degrees C and resulted in incomplete nitridation to EuTi02.25N0.75, indicating that anion vacancies created during the initial nitridation process of EuTiO2.82H0.18 play a crucial role in promoting anion (N3-/O2-) exchange at high temperatures. Hence, by using (hydride-induced) anion-deficient precursors, we should be able to expand the accessible anion composition of perovskite oxynitrides.
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