Abstract
A new silicate fluoride, NaBa3Si2O7F, has been successfully synthesized by a high-temperature solution method. It crystallizes in the orthorhombic space group Cmcm (No. 63). NaBa3Si2O7F is the first barium-containing alkali metal silicate fluoride with the [NaO6] polyhedra, the [BaO8F] polyhedra and isolated [Si2O7] units. The optical characterizations indicate that NaBa3Si2O7F possesses wide transparent window and available luminescence properties. To confirm the coordination surroundings of anionic groups and its thermostability, infrared spectroscopy and thermal behaviors were also analyzed, which proved the existence of tetrahedronly coordinated silicium atoms and the good stability of NaBa3Si2O7F at high temperature. First-principles calculation was also implemented for better understanding the relationship between the structure of NaBa3Si2O7F and its property. Additionally, to further explore the structural novelty of NaBa3Si2O7F, the comparison of the anionic structures was carried out in mixed alkali and alkaline-earth metal silicate fluorides. Interestingly, the result indicates the isolated [Si2O7] dimer is rare among the above systems, which enriches the structural chemistry of silicate fluorides.
摘要
本文采用高温熔液法成功合成了新型硅酸盐氟化物NaBa3 Si2O7F. 它结晶于正交晶系, 空间群为Cmcm (No. 63). NaBa3Si2O7F 是已知的第一例含钡碱金属硅酸盐氟化物, 它包含了[NaO6]多面 体、[BaO8F]多面体和孤立的[Si2O7]二聚体. 光学表征表明该化合物具有宽的透过窗口和良好的荧光性质. 为了确定该化合物的阴离子基团的配位环境及热稳定性, 还对其进行了红外光谱测试和热学行为分析, 结果证明其结构中存在硅氧四面体且该化合物具有良好的热稳定性. 为了更好地理解结构和性能之间的关系, 对该化合物进行了第一性原理计算. 与此同时, 为了进一步探索NaBa3Si2O7F的结构新颖性, 我们还对混合碱金属和/或碱土金属硅酸盐氟化物的阴离子结构进行了比较, 结果表明孤立的[Si2O7]二聚体在上述体系中较为少见, 这一研究结果丰富了硅酸盐氟化物的结构化学.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (U1703132, 51872325 and 61835014), Tianshan Innovation Team Program (2018D14001), Xinjiang International Science & Technology Cooperation Program (2017E01014), the National Key Research Project (2016YFB0402104), the Science and Technology Project of Urumqi (P161010002), Xinjiang Key Research and Development Program (2016B02021), Major Program of Xinjiang Uygur Autonomous Region of China during the 13th Five-Year Plan Period (2016A02003), and West Light Foundation of the Chinese Academy of Sciences (2016-YJRC-2).
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Author contributions Miao Z, Yang Y and Abudouwufu T performed the experiments, data analysis, and paper writing; Wei Z and Yang Z performed the theoretical data analysis; Pan S designed the concept and supervised the experiments. All authors contributed to the general discussion.
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Conflict of interest The authors declare that they have no conflict of interest.
Zhaohong Miao received her BSc degree in Shandong Normal University in 2016. She then joined Professor Shilie Pan’s research group as a master student at the University of Chinese Academy of Sciences (UCAS). Her research is currently focusing on the optical materials.
Yun Yang completed her PhD in material physics and chemistry under the supervision of Professor Shilie Pan at UCAS in 2011. She started her career as an assistant professor at Xinjiang Technical Institute of Physics & Chemistry of CAS (XTIPC, CAS) in 2007. In 2013, she was promoted to associate professor at XTIPC. In 2018, she was promoted to programs fellow and worked as a full professor at XTIPC. Her current research interest focuses on optical materials.
Shilie Pan received his BSc degree in chemistry from Zhengzhou University in 1996. He completed his PhD under the supervision of Professor Yicheng Wu (Academician) at the University of Science & Technology of China in 2002. From 2002 to 2004, he was a post-doctoral fellow at the Technical Institute of Physics & Chemistry of CAS in the laboratory of Professor Chuangtian Chen (Academician). From 2004 to 2007, he was a post-doctoral fellow at the Northwestern University in the laboratory of Professor Kenneth R. Poeppelmeier in USA. Since 2007, he has worked as a full professor at XTIPC, CAS. His current research interests include the design, synthesis, crystal growth and evaluation of new optical-electronic functional materials.
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Miao, Z., Yang, Y., Wei, Z. et al. A new barium-containing alkali metal silicate fluoride NaBa3Si2O7F with deep-UV optical property. Sci. China Mater. 62, 1454–1462 (2019). https://doi.org/10.1007/s40843-019-9448-y
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DOI: https://doi.org/10.1007/s40843-019-9448-y