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Chemically Stable Low-Dimensional Electrides in Transition Metal-Rich Monochalcogenides: Theoretical and Experimental Explorations

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Title
Chemically Stable Low-Dimensional Electrides in Transition Metal-Rich Monochalcogenides: Theoretical and Experimental Explorations
Author(s)
Kang, Se Hwang; Thapa, Dinesh; Regmi, Binod; Ren, Siyuan; Young-Min Kim; Kim, Seong-Gon; Kim, Sung Wng
Publication Date
2022-03
Journal
Journal of the American Chemical Society, v.144, no.10, pp.4496 - 4506
Publisher
American Chemical Society
Abstract
© 2022 American Chemical Society.Electrides, which are ionic crystals composed of excess anionic electrons, are of great interest as an exotic material for fundamental research and practical applications in broad fields of science and technology. However, an inherent chemical instability under ambient conditions at room temperature has been a fatal drawback to be addressed. Here, we report that transition metal-rich monochalcogenides are an emerging class of low-dimensional electrides with excellent chemical and thermal stability in air and water at room temperature through a comprehensive exploration of theoretical prediction and experimental verification. We predict new two-dimensional (2D) electrides crystallized in hexagonal P3¯ m1 and P63/mmc structures with strong localization of anionic electrons in a dumbbell shape at the tetrahedral cavity of the interlayer space, which are distinct from the anionic electrons localized at the octahedral cavity in the hexagonal R3¯ m structure of the previous 2D [Ca2N]+·e- and [Y2C]2+·2e- electrides. We successfully synthesized the room-temperature stable [Ti2O]2+·2e-, [Ti2S]2+·2e-, [Zr2S]2+·2e-, and primary solid solution [Hf2SxSe1-x]2+·2e- electrides, showing no structural degradation in air and water. Among them, we found that the synthesized [Ti2S]2+·2e- and [Zr2S]2+·2e- electrides are crystallized in orthorhombic symmetry (Pnnm), showing the feature of a one-dimensional (1D) electride with an anionic electron chain, which has never been reported yet. In addition to the successful finding of new 1D and 2D electrides, we discuss the self-passivation effect-driven chemical stability and the role of anionic electrons in determining the physical properties of the newly discovered electrides.
URI
https://pr.ibs.re.kr/handle/8788114/11581
DOI
10.1021/jacs.1c12367
ISSN
0002-7863
Appears in Collections:
Center for Integrated Nanostructure Physics(나노구조물리 연구단) > 1. Journal Papers (저널논문)
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