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Published on: November 28, 2017
Topochemical Reaction Involving Double-to-Single Layer Conversion: Mo3Ta2O10N with a Kagomé Lattice.
Ryoya Higuchi1, Kohdai Ishida1, Cédric Tassel1,2
1Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan.
This study reveals a novel topochemical reaction in Mo2Ta2O11, creating a unique Mo-based kagomé lattice (Mo3Ta2O10N) by collapsing tetrahedral layers. This unprecedented structural reorganization expands possibilities for metastable material synthesis.
Area of Science:
- Materials Science
- Solid-State Chemistry
- Inorganic Chemistry
Background:
- Topochemical reactions in transition metal oxides typically preserve the metal framework, modifying valence and coordination.
- Conventional reactions like SrFeO3 → SrFeO2 maintain a 1:1 structural correspondence.
- Metastable phases with diverse functionalities are accessible via topochemical transformations.
Purpose of the Study:
- To report an unprecedented topochemical transformation in Mo2Ta2O11.
- To investigate the structural and electronic consequences of collapsing MoO4 tetrahedral bilayers.
- To explore the synthesis of novel materials with unique structural motifs and electronic properties.
Main Methods:
- Ammonolysis of Mo2Ta2O11 at 500 °C in the presence of Mo(CO)6.
- Structural characterization using X-ray diffraction (implied by space group determination).
- Electronic and magnetic property measurements (magnetic susceptibility, NMR).
Main Results:
- Successful collapse of MoO4 tetrahedral bilayers into MoO6 octahedral layers, breaking the 1:1 structural correspondence.
- Formation of a new compound, Mo3Ta2O10N, with an 18% contraction along the c-axis.
- Discovery of an Mo-based kagomé lattice with finite d-electrons (Mo4.33+), unlike the d0 precursor.
Conclusions:
- Topochemical reactions can induce extensive structural reorganizations beyond conventional framework preservation.
- The synthesized Mo3Ta2O10N exhibits itinerant kagomé system characteristics.
- This work expands the scope of low-temperature synthesis routes for complex metastable materials.
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