Formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysis

Abstract Understanding the nucleation mechanism in glass is crucial for the development of new glass-ceramic materials. Herein, we report the structure of a commercially important glass-ceramic ZrO2-doped lithium aluminosilicate system during its initial nucleation stage. We conducted an X-ray multi...

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Main Authors: Yohei Onodera, Yasuyuki Takimoto, Hiroyuki Hijiya, Qing Li, Hiroo Tajiri, Toshiaki Ina, Shinji Kohara
Format: Article
Language:English
Published: Nature Portfolio 2024-04-01
Series:NPG Asia Materials
Online Access:https://doi.org/10.1038/s41427-024-00542-y
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author Yohei Onodera
Yasuyuki Takimoto
Hiroyuki Hijiya
Qing Li
Hiroo Tajiri
Toshiaki Ina
Shinji Kohara
author_facet Yohei Onodera
Yasuyuki Takimoto
Hiroyuki Hijiya
Qing Li
Hiroo Tajiri
Toshiaki Ina
Shinji Kohara
author_sort Yohei Onodera
collection DOAJ
description Abstract Understanding the nucleation mechanism in glass is crucial for the development of new glass-ceramic materials. Herein, we report the structure of a commercially important glass-ceramic ZrO2-doped lithium aluminosilicate system during its initial nucleation stage. We conducted an X-ray multiscale analysis, and this analysis was used to observe the structure from the atomic to the nanometer scale by using diffraction, small-angle scattering, absorption, and anomalous scattering techniques. The inherent phase separation between the Zr-rich and Zr-poor regions in the pristine glass was enhanced by thermal treatment without changing the spatial geometry at the nanoscale. Element-specific pair distribution function analysis using anomalous X-ray scattering data showed the formation of a liquid ZrO2-like local structural motif and edge sharing between the ZrO x polyhedra and (Si/Al)O4 tetrahedra during the initial nucleation stage. Furthermore, the local structure of the Zr4+ ions resembled a cubic or tetragonal ZrO2 crystalline phase and formed after 2 h of annealing the pristine glass. Therefore, the Zr-centric periodic structure formed in the early stage of nucleation was potentially the initial crystal nucleus for the Zr-doped lithium aluminosilicate glass-ceramic.
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spelling doaj-art-c43d29a2ac88476296d0b46d9e09a52a2025-01-19T12:28:31ZengNature PortfolioNPG Asia Materials1884-40572024-04-0116111310.1038/s41427-024-00542-yFormation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysisYohei Onodera0Yasuyuki Takimoto1Hiroyuki Hijiya2Qing Li3Hiroo Tajiri4Toshiaki Ina5Shinji Kohara6Center for Basic Research on Materials, National Institute for Materials ScienceInnovative Technology Laboratories, AGC, Inc.Materials Integration Laboratories, AGC, Inc.Materials Integration Laboratories, AGC, Inc.Scattering and Imaging Division, Japan Synchrotron Radiation Research Institute (JASRI, SPring-8)Spectroscopy Division, Japan Synchrotron Radiation Research Institute (JASRI, SPring-8)Center for Basic Research on Materials, National Institute for Materials ScienceAbstract Understanding the nucleation mechanism in glass is crucial for the development of new glass-ceramic materials. Herein, we report the structure of a commercially important glass-ceramic ZrO2-doped lithium aluminosilicate system during its initial nucleation stage. We conducted an X-ray multiscale analysis, and this analysis was used to observe the structure from the atomic to the nanometer scale by using diffraction, small-angle scattering, absorption, and anomalous scattering techniques. The inherent phase separation between the Zr-rich and Zr-poor regions in the pristine glass was enhanced by thermal treatment without changing the spatial geometry at the nanoscale. Element-specific pair distribution function analysis using anomalous X-ray scattering data showed the formation of a liquid ZrO2-like local structural motif and edge sharing between the ZrO x polyhedra and (Si/Al)O4 tetrahedra during the initial nucleation stage. Furthermore, the local structure of the Zr4+ ions resembled a cubic or tetragonal ZrO2 crystalline phase and formed after 2 h of annealing the pristine glass. Therefore, the Zr-centric periodic structure formed in the early stage of nucleation was potentially the initial crystal nucleus for the Zr-doped lithium aluminosilicate glass-ceramic.https://doi.org/10.1038/s41427-024-00542-y
spellingShingle Yohei Onodera
Yasuyuki Takimoto
Hiroyuki Hijiya
Qing Li
Hiroo Tajiri
Toshiaki Ina
Shinji Kohara
Formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysis
NPG Asia Materials
title Formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysis
title_full Formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysis
title_fullStr Formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysis
title_full_unstemmed Formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysis
title_short Formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by X-ray multiscale analysis
title_sort formation of a zirconium oxide crystal nucleus in the initial nucleation stage in aluminosilicate glass investigated by x ray multiscale analysis
url https://doi.org/10.1038/s41427-024-00542-y
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