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

IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Npg Asia Materials Pub Date : 2024-04-19 DOI:10.1038/s41427-024-00542-y
Yohei Onodera, Yasuyuki Takimoto, Hiroyuki Hijiya, Qing Li, Hiroo Tajiri, Toshiaki Ina, Shinji Kohara
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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 ZrOx 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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通过 X 射线多尺度分析法研究铝硅酸盐玻璃初始成核阶段氧化锆晶核的形成
了解玻璃中的成核机制对于开发新型玻璃陶瓷材料至关重要。在此,我们报告了一种具有重要商业价值的玻璃陶瓷 ZrO2 掺杂铝硅酸锂体系在其初始成核阶段的结构。我们进行了 X 射线多尺度分析,并利用衍射、小角散射、吸收和反常散射技术观察了从原子到纳米尺度的结构。原始玻璃中富锆区和贫锆区之间的固有相分离通过热处理得到了加强,但并没有改变纳米尺度的空间几何结构。利用反常 X 射线散射数据进行的元素特异对分布函数分析表明,在初始成核阶段形成了类似 ZrO2 的液态局部结构图案,ZrOx 多面体和(Si/Al)O4 四面体之间实现了边缘共享。此外,Zr4+ 离子的局部结构类似于立方或四方 ZrO2 结晶相,并在原始玻璃退火 2 小时后形成。因此,成核初期形成的以 Zr 为中心的周期性结构可能是掺杂 Zr 的锂铝硅酸盐玻璃陶瓷的初始晶核。
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来源期刊
Npg Asia Materials
Npg Asia Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
15.40
自引率
1.00%
发文量
87
审稿时长
2 months
期刊介绍: NPG Asia Materials is an open access, international journal that publishes peer-reviewed review and primary research articles in the field of materials sciences. The journal has a global outlook and reach, with a base in the Asia-Pacific region to reflect the significant and growing output of materials research from this area. The target audience for NPG Asia Materials is scientists and researchers involved in materials research, covering a wide range of disciplines including physical and chemical sciences, biotechnology, and nanotechnology. The journal particularly welcomes high-quality articles from rapidly advancing areas that bridge the gap between materials science and engineering, as well as the classical disciplines of physics, chemistry, and biology. NPG Asia Materials is abstracted/indexed in Journal Citation Reports/Science Edition Web of Knowledge, Google Scholar, Chemical Abstract Services, Scopus, Ulrichsweb (ProQuest), and Scirus.
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