Chemistry:Oxonitridosilicate

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The oxonitridosilicates, also called sions (Si + O + N) or silicon-oxynitrides are inorganic ceramic compounds in which oxygen and nitrogen atoms are bound to a silicon atom.[1] A common variant also has aluminium replacing some silicon. They can be considered as silicates in which nitrogen partially replaces oxygen, or as nitridosilicates with oxygen partly replacing nitrogen.

Formation

A possible way to make these compounds is to heat metal oxides or carbonates with silicon nitride and silica in a nitrogen atmosphere.[2]

Properties

Oxonitridosilicates have diverse structures. At the small scale silicon forms tetrahedral shapes surrounded by four oxygen or nitrogen atoms. With oxygen, one point of a tetrahedron can be bridged to another denoted O[2], or the oxygen can be a terminal atom denoted O[1]. With nitrogen, it can be shared in more ways: terminal N[1], bridged between two tetrahedra N[2], or even three or four: N[3], N[4]. With nitrogen, tetrahedra can be fused on an edge, or a point, whereas oxygen only connects tetrahedra at a vertex.[3]

The condensation ratio, denoted by K indicates how condensed the tetrahedra are. K is the number of silicon atoms divided by the sum of oxygen and nitrogen. For SiN48− or SIO24+ K is 1/4 and it increases to 1/2 for SiO2.[3]

Use

Oxonitridosilicates doped with europium have been used as phosphors in white LEDs, as they convert some blue light to other colours that can mix to white.[3]

Listing

name formula crystal
system 		space
group 		unit cell volume phosphor

colour Eu2+

comments ref
LiSiNO [4]
Li3SiNO2 [5]
Li6SiN2O2 [6]
Li7SiN3O Fm3m a=4.6994 [7]
Li5SiNO3 [4]
Na3SiNO2 [5]
CaSi2O2N2 [8]
Ca2.89Si2N1.76O4.24

Ca3Si2O4N2

cubic Pa3

a = 15.0626 Å V = 3417.45 Å3 Z=24

green colourless [9][10]
SrSi2O2N2 green [8][11]
Li4Sr4[Si4O4N6]O tetragonal P42/nmc a=7.4833, c = 9.8365 V=552.81 Z = 2 orange band gap 3.6 eV [12]
Sr3Si13Al3O2N21 orthorhombic a = 9.037, b = 14.734, c = 7.464 green [13]
Y4SiO7N2 [14]
BaSi2O2N2 bluish green [15]
Ba3Si6O9N4 bluish green [16]
Ba3Si6O12N2 trigonal P3 a = 7.5046 c = 6.4703 green
La5Si3O12N hexagonal P63/m a=9.7051 c=7.2546 Z=1 591.76 white UV>261 [14]
La4SiO7N2 monoclinic P121/C1 a=8.036 b=10.992 c=11.109 β=110.92 Z=4 916.75 white UV>283 [14]
LaSiO2N hexagonal P6c2 a=7.310 c=9.550 V=441.95 Z=6 white UV>263 [14]
La3Si8O4N11 orthorhombic C2/c a=15.850 b=4.9029 c=18.039 Z=4 1271.05 white UV>243 [14]
La3[SiON3]O tetragonal I4/mcm a = 6.822, c = 11.074 Å, Z = 4 [17]
La16[Si8N22][SiON3]2 triclinic P1 a = 5.718, b = 11.391, c = 13.435, α = 112.02, β = 90.19, γ = 90.58 Z=2 811.1 [18]
Ce4[Si4O4N6]O green-yellow [1]
Ce3[SiON3]O tetragonal I4/mcm a = 6.723, c = 11.069 Å, Z = 4 dark red [17]
Sr3Ce10Si18Al12O18N36 [1]
Pr3[SiON3]O tetragonal I4/mcm a = 6.6979, c = 11.005 Å, Z = 4 [17]
Pr4Si2O7N2 [17]
Gd3[SiON3]O tetragonal I4/mcm [17]
Sr3Pr10Si18Al12O18N36 [1]
Sr3Nd10Si18Al12O18N36 [1]
Sr10Sm6Si30Al6O7N54 [1]
EuSi2O2N2 triclinic P1 a=7.095 b=7.246 c=7.256 α=88.69 β=84.77 γ=75.84 Z=4 [8]
ytterbium silicon oxynitride Yb4Si2O7N2 [19]

References

  1. ↑ 1.0 1.1 1.2 1.3 1.4 1.5 Schnick, Wolfgang (December 2001). "Nitridosilicates, oxonitridosilicates (sions), and oxonitridoaluminosilicates (sialons)" (in en). International Journal of Inorganic Materials 3 (8): 1267–1272. doi:10.1016/S1466-6049(01)00120-9. https://linkinghub.elsevier.com/retrieve/pii/S1466604901001209. 
  2. ↑ Wang, Baochen; Liu, Yan-gai; Huang, Zhaohui; Fang, Minghao; Wu, Xiaowen (December 2017). "Discovery of novel solid solution Ca3Si3−x O3+x N4−2x : Eu2+ phosphors: structural evolution and photoluminescence tuning". Scientific Reports 7 (1): 18103. doi:10.1038/s41598-017-18319-5. PMID 29273765. Bibcode: 2017NatSR...718103W. open access
  3. ↑ 3.0 3.1 3.2 Zeuner, Martin; Pagano, Sandro; Schnick, Wolfgang (16 August 2011). "Nitridosilicates and Oxonitridosilicates: From Ceramic Materials to Structural and Functional Diversity". Angewandte Chemie International Edition 50 (34): 7754–7775. doi:10.1002/anie.201005755. PMID 21774043. 
  4. ↑ 4.0 4.1 Podsiadło, S. (March 1987). "Formation and thermal decomposition of silicon oxynitride compounds II" (in en). Journal of Thermal Analysis 32 (2): 445–449. doi:10.1007/BF01912696. ISSN 0368-4466. http://link.springer.com/10.1007/BF01912696. 
  5. ↑ 5.0 5.1 Podsiadlo, S. (January 1987). "Formation and thermal decomposition of silicon oxynitride compounds I" (in en). Journal of Thermal Analysis 32 (1): 43–47. doi:10.1007/BF01914545. ISSN 0368-4466. http://link.springer.com/10.1007/BF01914545. 
  6. ↑ Podsiadło, S. (May 1987). "Formation and thermal decomposition of silicon oxynitride compounds. Part III" (in en). Journal of Thermal Analysis 32 (3): 771–775. doi:10.1007/BF01913762. ISSN 0368-4466. http://link.springer.com/10.1007/BF01913762. 
  7. ↑ Casas-Cabanas, M.; Santner, H.; Palacín, M.R. (May 2014). "The Li–Si–(O)–N system revisited: Structural characterization of Li21Si3N11 and Li7SiN3O". Journal of Solid State Chemistry 213: 152–157. doi:10.1016/j.jssc.2014.02.022. Bibcode: 2014JSSCh.213..152C. 
  8. ↑ 8.0 8.1 8.2 Oeckler, O.; Stadler, F.; Schnick, W. (2006-12-01). "Real structure investigations on oxonitridosilicates MSi2O2N2 (M = Ca, Sr, Ba, Eu)" (in en). Acta Crystallographica Section A 62 (a1): 202. doi:10.1107/S0108767306095973. ISSN 0108-7673. http://scripts.iucr.org/cgi-bin/paper?S0108767306095973. 
  9. ↑ Sharafat, Ali; Berastegui, Pedro; Esmaeilzadeh, Saeid; Eriksson, Lars; Grins, Jekabs (2011-11-15). "A cubic calcium oxynitrido-silicate, Ca 2.89 Si 2 N 1.76 O 4.24". Acta Crystallographica Section E 67 (11): i66. doi:10.1107/S1600536811042607. ISSN 1600-5368. PMID 22219731. PMC 3246911. http://scripts.iucr.org/cgi-bin/paper?S1600536811042607. 
  10. ↑ Yi-Chen Chiu, Chien-Hao Huang, Te-Ju Lee, Wei-Ren Liu, Yao-Tsung Yeh, ShyueMing Jang, and Ru-Shi Liu (9 May 2011). "Eu2+-activated silicon-oxynitride Ca3Si2O4N2: a green-emitting phosphor for white LEDs". Optics Express 19: A331-A339|issue=S3. doi:10.1364/OE.19.00A331. PMID 21643375. https://www.researchgate.net/publication/51193603. 
  11. ↑ Bachmann, Volker; Jüstel, Thomas; Meijerink, Andries; Ronda, Cees; Schmidt, Peter J. (December 2006). "Luminescence properties of SrSi2O2N2 doped with divalent rare earth ions" (in en). Journal of Luminescence 121 (2): 441–449. doi:10.1016/j.jlumin.2005.11.008. Bibcode: 2006JLum..121..441B. https://dspace.library.uu.nl/bitstream/handle/1874/20108/2006-001.pdf?sequence=1. 
  12. ↑ Niklaus, Robin; Neudert, Lukas; Stahl, Juliane; Schmidt, Peter J.; Schnick, Wolfgang (2018-11-19). "Orange-Emitting Li 4 Sr 4 [Si 4 O 4 N 6 O:Eu 2+ —a Layered Lithium Oxonitridosilicate Oxide"] (in en). Inorganic Chemistry 57 (22): 14304–14313. doi:10.1021/acs.inorgchem.8b02391. ISSN 0020-1669. PMID 30398336. https://pubs.acs.org/doi/10.1021/acs.inorgchem.8b02391. 
  13. ↑ Xie, Rong-Jun; Hirosaki, Naoto; Li, Yuanqiang; Takeda, Takashi (2010-06-21). "Rare-Earth Activated Nitride Phosphors: Synthesis, Luminescence and Applications" (in en). Materials 3 (6): 3777–3793. doi:10.3390/ma3063777. ISSN 1996-1944. Bibcode: 2010Mate....3.3777X. 
  14. ↑ 14.0 14.1 14.2 14.3 14.4 Dierre, Benjamin; Xie, Rong-Jun; Hirosaki, Naoto; Sekiguchi, T. (July 2007). "Blue emission of Ce 3+ in lanthanide silicon oxynitride phosphors" (in en). Journal of Materials Research 22 (7): 1933–1941. doi:10.1557/jmr.2007.0231. ISSN 0884-2914. Bibcode: 2007JMatR..22.1933D. https://www.cambridge.org/core/product/identifier/S0884291400025498/type/journal_article. 
  15. ↑ Pan, Huayan; Luo, Dong; Wang, Le; Li, Yanghui (2015). "Electronic structure and luminescence properties of BaSi2O2N2:Eu2+ phosphor for white LEDs" (in en). Proceedings of the 2015 6th International Conference on Manufacturing Science and Engineering. Qingdao, China: Atlantis Press. pp. 690–695. doi:10.2991/icmse-15.2015.123. ISBN 978-94-6252-137-7. http://www.atlantis-press.com/php/paper-details.php?id=25845650. 
  16. ↑ Luo, Dong; Wang, Le; Li, Yang-Hui; Xu, Guo-Tang; Pan, Hua-Yan; Liang, Pei; Chen, Ru-Biao; Zhang, Hong (October 2014). "Preparation of Ba3Si6O9N4:Eu2+ phosphor and characterization of their luminescence properties". 2014 International Conference on Manipulation, Manufacturing and Measurement on the Nanoscale (3M-NANO). Taipei, Taiwan: IEEE. pp. 44–47. doi:10.1109/3M-NANO.2014.7057295. ISBN 978-1-4799-7923-3. https://ieeexplore.ieee.org/document/7057295. 
  17. ↑ 17.0 17.1 17.2 17.3 17.4 Kechele, Juliane A.; Schmolke, Christian; Lupart, Saskia; Schnick, Wolfgang (January 2010). "Ln 3 [SiON 3 O ( Ln = La, Ce, Pr) - Three Oxonitridosilicate Oxides with Crystal Structures Derived from the Anti-Perovskite Structure Type"] (in en). Zeitschrift für anorganische und allgemeine Chemie 636 (1): 176–182. doi:10.1002/zaac.200900274. http://doi.wiley.com/10.1002/zaac.200900274. 
  18. ↑ Schmolke, Christian; Lupart, Saskia; Schnick, Wolfgang (February 2009). "La16[Si8N22[SiON3]2 – A nitridosilicate with isolated, corner-sharing and edge-sharing tetrahedra"] (in en). Solid State Sciences 11 (2): 305–309. doi:10.1016/j.solidstatesciences.2008.08.008. Bibcode: 2009SSSci..11..305S. https://linkinghub.elsevier.com/retrieve/pii/S129325580800280X. 
  19. ↑ Nishimura, Toshiyuki; Mitomo, Mamoru; Suematsu, Hisayuki (January 1997). "High temperature strength of silicon nitride ceramics with ytterbium silicon oxynitride" (in en). Journal of Materials Research 12 (1): 203–209. doi:10.1557/JMR.1997.0027. ISSN 0884-2914. Bibcode: 1997JMatR..12..203N. https://www.cambridge.org/core/product/identifier/S0884291400038218/type/journal_article. 



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