Citation: Shi Feng, Hu Lili, Ren Jinjun, Yang Qiuhong. Structural Investigation of Alkaline-Earth Phosphosilicate Glasses Containing Six-Coordinated Silicon by Solid-State NMR[J]. Acta Physico-Chimica Sinica, ;2020, 36(4): 190201. doi: 10.3866/PKU.WHXB201902018 shu

Structural Investigation of Alkaline-Earth Phosphosilicate Glasses Containing Six-Coordinated Silicon by Solid-State NMR

Shi Feng ^1,2 ,
Hu Lili ² ,
Ren Jinjun ^2,, ,
Yang Qiuhong ¹

1.
School of Materials Science and Engineering, Shanghai University, Shanghai 200444, P. R. China
2.
Key Laboratory of Materials for High Power Laser, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, P. R. China

Corresponding author: Ren Jinjun, renjinjunsiom@163.com
Received Date: 22 February 2019
Revised Date: 15 April 2019
Accepted Date: 16 April 2019
Available Online: 19 April 2019
Fund Project: The project was supported by the National Natural Science Foundation of China (61675218) and the 100 Talents Program of Chinese Academy of Sciencesthe National Natural Science Foundation of China 61675218

Phosphate glass is widely used in optical applications; however, its generally low chemical stability and poor thermal mechanical properties hinder the application of phosphate glass to the rapidly evolving laser industry. The addition of a small amount of silicon can form a six-coordinate Si (Si⁽⁶⁾) network and improve the above-mentioned poor properties of phosphate glass. Therefore, it is important to characterize and understand the structural details of phosphosilicate glasses. It is difficult to investigate the glass structure because of its complicated and disordered characteristics. However, solid-state nuclear magnetic resonance (NMR) spectroscopy can provide detailed local structural information, regardless of the presence of its long-range order. To study the effect of alkaline earth metals on Si⁽⁶⁾ species formation, we prepared phosphosilicate glasses (2MO-3P₂O₅)_(1−x)·(SiO₂)_x (M = Ca, Sr, Ba) by conventional melt-quenching, and the glass structure was investigated by solid-state NMR and Raman spectroscopy. The ³¹P and ²⁹Si NMR spectra indicated that the glass networks consisted of P⁽²⁾ and P⁽³⁾ tetrahedrons linked via four- and six-fold coordinated silicon units (Si⁽⁴⁾ and Si⁽⁶⁾). The fraction of six-coordinated silicon Si⁽⁶⁾ decreased with increasing SiO₂ content. Similarly, the Raman spectra showed that the vibration band of the P＝O stretching mode in P⁽³⁾ linked with Si⁽⁶⁾ neighbors reduced as the silica content increased. The connectivities between various phosphorus species were probed by ³¹P one- and two-dimensional refocused INADEQUATE experiments. This experimental technique is based on homonuclear J-coupling and yields correlation peaks between nuclei engaged in P―O―P linkages (P⁽²⁾ and P⁽³⁾ units). The signals from isolated ³¹P nuclei are suppressed because of the absence of J-coupling, which precludes the formation of double quantum coherences. The results indicated the segregation of P⁽²⁾ and P⁽³⁾ units in the prepared glass, which were also compared with those in the previously reported Na₂O-P₂O₅-SiO₂ glasses. They differed from alkali phosphosilicate glasses, where each P⁽³⁾ unit exhibited a maximum average of one Si⁽⁶⁾―O―P⁽³⁾ linkage, and in the alkaline earth phosphosilicate glasses, the average was approximately 0.4–0.7. When the content of Si⁽⁶⁾ units reached its maximum, further increase in the SiO₂ content did not increase the Si⁽⁶⁾ content, and the surplus Si were present as Si⁽⁴⁾. Alkaline earth metal ions exhibit weaker stabilizing effects for Si⁽⁶⁾ species. Based on the results presented herein, we constructed sketches to illustrate the local structural organization of the glass. The relationships between the compositions and structures are important for glass composition and property design. It is important to improve the performance of phosphate glass by changing its composition, particularly for large laser device applications.
- Solid state NMR,
- Glass structure,
- Six-coordination silica,
- Akaline-earth,
- Phosphosilicate glasses
1. [1]
  Stebbins, J. F. J. Non-Cryst. Solids 1988, 106, 359. doi: 10.1016/0022-3093(88)90289-X doi: 10.1016/0022-3093(88)90289-X
2. [2]
  Richard, K. B. J. Non-Cryst. Solids 2000, 263, 1. doi: 10.1016/S0022-3093(99)00620-1 doi: 10.1016/S0022-3093(99)00620-1
3. [3]
  Onodera, Y.; Kohara, S.; Masai, H.; Koreeda, A.; Okamura, S.; Ohkubo, T. Nat. Commun. 2017, 8, 15449. doi: 10.1038/ncomms15449 doi: 10.1038/ncomms15449
4. [4]
  Edén, Mattias. Annu. Rep. Prog. Chem. Sect. C: Phys. Chem. 2012, 108, 177. doi: 10.1039/C2PC90006H doi: 10.1039/C2PC90006H
5. [5]
  Schmidt-Rohr, K.; Spiess, H. W. Phys. Rev. Lett. 1991, 66, 3020. doi: 10.1103/PhysRevLett.66.3020 doi: 10.1103/PhysRevLett.66.3020
6. [6]
  Dupree, R.; Holland, D.; Mortuza, M. G.; Collins, J. A.; Lockyer, M. W. G. J. Non-Cryst. Solids 1989, 112, 111. doi: 10.1016/0022-3093(89)90504-8 doi: 10.1016/0022-3093(89)90504-8
7. [7]
  Dirken, P.; Kohn, S.; Smith, M. E.; Eck, E. R. H. Chem. Phys. Lett. 1997, 266, 568. doi: 10.1016/S0009-2614(97)00041-9 doi: 10.1016/S0009-2614(97)00041-9
8. [8]
  Meade, C.; Hemley, R. J.; Mao, H. K. Phys. Rev. Lett. 1992, 69, 1387. doi: 10.1103/PhysRevLett.69.1387 doi: 10.1103/PhysRevLett.69.1387
9. [9]
  Ping, T.; Sung, P. S.; Greenblatt, M. J. Non-Cryst. Solids 1991, 135, 131. doi: 10.1016/0022-3093(91)90413-Z doi: 10.1016/0022-3093(91)90413-Z
10. [10]
  Ren, J. J.; Eckert, H. J. Phys. Chem. C 2014, 118, 15386. doi: 10.1021/jp504023k doi: 10.1021/jp504023k
11. [11]
  Massiot, D.; Messinger, R. J.; Cadars, S.; Deschamps, M.; Montouillout, V.; Pellerin, N.; Veron, E.; Allix, M.; Florian, P.; Fayon, F. Acc. Chem. Res. 2013, 46, 1975. doi: 10.1021/ar3003255 doi: 10.1021/ar3003255
12. [12]
  Li, C.; Shen, M.; Hu, B. W. Acta Phys. -Chim. Sin. 2020, 36, 1902019. doi: 10.3866/PKU.WHXB201902019
13. [13]
  Xu, W. B.; Ren, J. J.; Shao, C. Y.; Wang, X.; Wang, M.; Zhang, L. Y.; Chen, D. P.; Wang, S. K.; Yu, C. L.; Hu, L. L. J. Lumin. 2015, 167, 8. doi: 10.1016/j.jlumin.2015.05.061 doi: 10.1016/j.jlumin.2015.05.061
14. [14]
  Kim, E. J.; Fei, Y.; Lee, S. K. Geochim. Cosmochim. Acta 2018, 224, 327. doi: 10.1016/j.gca.2018.01.006 doi: 10.1016/j.gca.2018.01.006
15. [15]
  Ren, J. J; Eckert, H. J. Phys. Chem. C 2012, 116, 12747. doi: 10.1021/jp301383x doi: 10.1021/jp301383x
16. [16]
  Larink, D.; Eckert, H.; Reichert, M.; Martin, S. W. J. Phys. Chem. C 2012, 116, 26162. doi: 10.1021/jp307085t20152201012 doi: 10.1021/jp307085t20152201012
17. [17]
  Sava, B. A.; Elisa, M.; Vasiliu, I. C.; Nastase, F.; Simon, S. J. Non-Cryst. Solids 2012, 358, 2877. doi: 10.1016/j.jnoncrysol.2012.07.016 doi: 10.1016/j.jnoncrysol.2012.07.016
18. [18]
  Oliveira, M. D.; Aitken, B.; Eckert, H. J. Phys. Chem. C 2018, 122, 19807. doi: 10.1021/acs.jpcc.8b06055 doi: 10.1021/acs.jpcc.8b06055
19. [19]
  Campbel, J. H.; Suratwala, T. I. J. Non-Cryst. Solids 2000, 263, 318. doi: 10.1016/S0022-3093(99)00645-6 doi: 10.1016/S0022-3093(99)00645-6
20. [20]
  Campbell, J. H.; Hayden, J. S.; Marker, A. Int. J. Appl. Glass Sci. 2011, 2, 3. doi: 10.1111/j.2041-1294.2011.00044.x doi: 10.1111/j.2041-1294.2011.00044.x
21. [21]
  Ebendorff-Heidepriem, H.; Ehrt, D. J. Non-Cryst. Solids 1996, 208, 205. doi: 10.1016/S0022-3093(96)00524-8 doi: 10.1016/S0022-3093(96)00524-8
22. [22]
  Toratani, H. Properties of Laser Glasses. Ph.D. Dissertation, Kyoto University, Japan, 1989.
23. [23]
  Dupree, R.; Holland, D.; Mortuza, M. G. Nature 1987, 328, 416. doi: 10.1038/328416a0 doi: 10.1038/328416a0
24. [24]
  Weeding, T.; Jong, B. D.; Veeman, W.; Aitken, B. J. Nature 1985, 318, 352. doi: 10.1038/318352a0 doi: 10.1038/318352a0
25. [25]
  Radovanovic, E.; Gozzi, M.; Gonçalves, M.; Yoshida, I. J. Non-Cryst. Solids 1999, 248, 37. doi: 10.1016/S0022-3093(99)00101-5 doi: 10.1016/S0022-3093(99)00101-5
26. [26]
  Ide, J.; Ozutsumi, K.; Kageyama, H.; Handa, K.; Umesaki, N. J. Non-Cryst. Solids 2007, 353, 1966. doi: 10.1016/j.jnoncrysol.2007.02.022 doi: 10.1016/j.jnoncrysol.2007.02.022
27. [27]
  Ahsan, M. R.; Mortuza, M. G. J. Non-Cryst. Solids 2005, 351, 2333. doi: 10.1016/j.jnoncrysol.2005.05.030 doi: 10.1016/j.jnoncrysol.2005.05.030
28. [28]
  Miyabe, D.; Takahashi, M.; Tokuda, Y.; Yoko, T.; Uchino, T. Phys. Rev. B 2005, 71, 2202. doi: 10.1103/PhysRevB.71.172202 doi: 10.1103/PhysRevB.71.172202
29. [29]
  Yamashita, H.; Yoshino, H.; Nagata, K.; Yamaguchi, I.; Ookawa, M.; Maekawa, T. J. Ceram. Soc. Jpn. 1998, 106, 539. doi: 10.2109/jcersj.106.539 doi: 10.2109/jcersj.106.539
30. [30]
  Sakida, S.; Nanba, T.; Miura, Y. Chem. Lett. 2006, 35, 1268. doi: 10.1246/cl.2006.1268 doi: 10.1246/cl.2006.1268
31. [31]
  Fleet, M.; Muthupari, S.; Kasrai, M.; Prabakar, S. J. Non-Cryst. Solids 1997, 220, 85. doi: 10.1016/S0022-3093(97)00222-6 doi: 10.1016/S0022-3093(97)00222-6
32. [32]
  Li, D; Bancroft, G.; Fleet, M. E. Am. Mineral. 1996, 81, 111. doi: 10.2138/am-1996-1-214 doi: 10.2138/am-1996-1-214
33. [33]
  Ren, J.J.; Eckert, H. J. Phys. Chem. C 2018, 122, 27620. doi: 10.1021/acs.jpcc.8b09779 doi: 10.1021/acs.jpcc.8b09779
34. [34]
  Massiot, D.; Fayon, F.; Capron, M.; King, I.; Calvé, I.; Alonso, B.; Durand, J. O.; Bujoli, B.; Gan, Z.; Hoatson, G. Magn. Reson. Chem. 2002, 40, 70. doi: 10.1002/mrc.984 doi: 10.1002/mrc.984
35. [35]
  Lesage, A.; Bardet, M.; Emsley, L. J. Am. Chem. Soc. 1999, 121, 10987. doi: 10.1021/ja992272b doi: 10.1021/ja992272b
36. [36]
  Guerry, P.; Smith, M. E.; Brown, S. P. J. Am. Chem. Soc. 2009, 131, 11861. doi: 10.1021/ja902238s doi: 10.1021/ja902238s
37. [37]
  Hudgens, J. J.; Brow, R. K.; Tallant, R. D.; Martin, S. W. J. Non-Cryst. Solids 1998, 223, 21. doi: 10.1016/S0022-3093(97)00347-5 doi: 10.1016/S0022-3093(97)00347-5
38. [38]
  Hermansen, C.; Guo, X.; Youngman, R. E.; Mauro, J. C.; Smedskjaer, M. M.; Yue, Y. J. Chem. Phys. 2015, 143, 064510. doi: 10.1063/1.4928330 doi: 10.1063/1.4928330
39. [39]
  Plotnichenko, V.; Sokolov, V.; Koltashev, V.; Dianov, E. J. Non-Cryst. Solids 2002, 306, 209. doi: 10.1016/S0022-3093(02)01172-9 doi: 10.1016/S0022-3093(02)01172-9
40. [40]
  Nelson, B.; Exarho, G. J. Chem. Phys. 1979, 71, 2739. doi: 10.1063/1.438679 doi: 10.1063/1.438679
41. [41]
  Magi, M.; Lippmaa, E.; Samoson, A.; Engelhardt, G.; Grimmer, A. J. Chem. Phys. 1984, 88, 1518. doi: 10.1021/j150652a015 doi: 10.1021/j150652a015
42. [42]
  Stebbins, J. F.; McMillan, P. J. Non-Cryst. Solids 1993, 160, 116. doi: 10.1016/0022-3093(93)90292-6 doi: 10.1016/0022-3093(93)90292-6
43. [43]
  Jiang, Q.; Zeng, H. D; Li, X.; Ren, J. J.; Chen, G.; Liu, F. J. Chem. Phys. 2014, 141, 124506. doi: 10.1063/1.4896150 doi: 10.1063/1.4896150
44. [44]
  Youngman, R.; Hogue, C.; Aitken, B. MRS Online Proc. Libr. 2006, 984, 84. doi: 10.1557/PROC-984-0984-MM12-03 doi: 10.1557/PROC-984-0984-MM12-03
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