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Experimental and Theoretical Studies on the Controlled Synthesis of Alkali‐Metal‐Doped Rare‐Earth Oxysulfide Nanocrystals
Author(s) -
Zhang Tao,
Gu Jun,
Ding Yi,
Zhang YaWen,
Yan ChunHua
Publication year - 2013
Publication title -
chempluschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.801
H-Index - 61
ISSN - 2192-6506
DOI - 10.1002/cplu.201300092
Subject(s) - alkali metal , lanthanide , doping , materials science , phase (matter) , inorganic chemistry , nanocrystal , ternary operation , alkaline earth metal , chemistry , nanotechnology , organic chemistry , ion , optoelectronics , computer science , programming language
Alkali‐metal (Li, Na, K)‐doped lanthanum oxysulfide nanoplates were obtained in the hexagonal phase by thermolysis of metal acetylacetonates in organic solvents with high boiling points and sulfurization using sulfur powders. The characterization results showed that the size, shape, crystallinity, composition, and phase stability of the La 2 O 2 S nanocrystals were affected by the doped alkali metals. Combined with first‐principles calculations of the formation energy of anionic defects in the lattices, the ternary phase diagrams for the formation of rare‐earth oxysulfides (RE 2 O 2 S) were calculated. Both the experimental results and the phase diagrams have demonstrated that the doped alkali metals are capable of promoting the formation of RE 2 O 2 S nanocrystals in the order of K≈Na>Li. With K acting as the doping alkali metal, the phase‐formation capability for different RE 2 O 2 S (e.g., Eu, Gd, Yb, Lu) along the lanthanide series was also explored under the guidance of the hard and soft acid and base (HSAB) theory. Moreover, the as‐developed synthetic route could be applied also to the production of K/Eu‐ and K/Tb‐codoped La 2 O 2 S nanoplates, which displayed intense red and green emissions, respectively, under ultraviolet‐light excitations.