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A nitrogen-contained solid solution Ca2Si(O4-xNx):Eu2+ green phosphors was successfully synthesized using the method of mixing Ca-Si-O xerogel precursor with Si3N4 powders in a non-reducing atmosphere (pure nitrogen). The structure, morphology, and luminescent properties of the phosphors are characterized by X-ray diffraction (XRD), \text {scanning} electron microscopy (SEM) and photoluminescence (PL) spectra. Results show that the Ca2Si(O4-xNx):Eu2+ is obtained and especially the reduction of Eu3+ to Eu2+ occurs when the mixture of Si3N4 and precursor is calcined at 1100℃ in pure nitrogen atmosphere. XRD results show that the crystalline structure of N-contained solid solution Ca2Si(O4-xNx):Eu2+ is consistent with that of βup -Ca2SiO4 phase. The phosphors can be efficiently excited at a wavelength of 270–400 nm and shows a single intense broadband emission (450–600 nm). Significantly, the red-shift (501 nm to 504 nm) of emission peak occurs and the luminescent intensity is improved significantly with increasing N concentration. With increasing Eu2+ concentration, luminescent intensity of the phosphors increases continuously and reaches a maximum value at the concentration of 0.25 mol% Eu2+. Then the luminescent intensity decreases significantly and the concentration quenching effect appears when Eu2+ concentration is above 0.25 mol%.
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Keywords:
- white LED /
- phosphors /
- sol-gel method /
- Si3N4
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[20] Zhang M, He X, Ding W J, Wang J 2010 Prog. Chem. 22 376(in Chinese) [张梅, 何鑫, 丁维嘉, 王静 2010 化学进展 22 376]
[21] Su Q, Zeng Q H, Pei Z W 2000 Chin. J. Inorg. Chem. 16 293(in Chinese) [苏锵, 曾庆华, 裴治武 2000 无机化学学报 16 293]
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[1] Zhang X H, Lu Z M, Meng F B, Lu F, Hu L, Xu X W, Tang C C 2012 Mater. Lett. 66 16
[2] Chen Y, Zhang J, Zhang L, Han P D, Wang L X, Zhang Q T 2012 Rare Matals. 31 479
[3] Yu Y, Liu Z J, Chen Q Q, Dai N L, Li J Y, Yang L Y 2013 Acta Phys. Sin. 62 017804(in Chinese) [余阳, 刘自军, 陈乔乔, 戴能利, 李进延, 杨旅云 2013 物理学报 62 017804]
[4] Li K, Shen C Y 2012 Appl. Opt. 123 621
[5] Kuo C H, Sheu J K, Chang S J, Su Y K, Wu L W, Tsai J M, Liu C H, Wu R K 2003 Jpn. J. App. Phys. 42 2284
[6] Li P L, Yang Z P, Wang Z L, Guo Q L 2008 Chin. Phys. B 17 1137
[7] Qi Z J, Huang W G 2013 Acta Phys. Sin. 62 197801(in Chinese) [齐智坚, 黄维刚 2013 物理学报 62 197801]
[8] Zhang X, Fei Q N, Mao Z Y, Liu Y H, Cai Y, Lu Q F, Tian H, Wang D J 2011 J. Rare Earths 29 522
[9] Wu Y, Wang Y S, He D W, Fu M, Chen W Y, Li Y, Mao F 2011 Spectrosc. Spec. Anal. 31 890(in Chinese) [邬洋, 王永生, 何大伟, 富鸣, 陈震旻, 李玥, 苗峰 2011 光谱学与光谱分析 31 890]
[10] Li P L, Wang Z J, Yang Z P, Guo Q L, Li X 2009 J. Chin. Ceram. Soc. 37 462
[11] Choi N S, Park K W, Park B W, Zhang X M, Kim J S, Kung P, Kim S M 2010 J. Lumin. 130 560
[12] Yang Z P, Liu Y F 2006 Acta Phys.Sin. 55 4946(in Chinese) [杨志平, 刘玉峰 2006 物理学报 55 4946]
[13] Yang Z P, Tian J, Li X, Yang G W, Wang S L, Li P L 2008 J. Synth. Cryst. 37 368(in Chinese) [杨志平, 田晶, 李旭, 杨广伟, 王少丽, 李盼来 2008 人工晶体学报 37 368]
[14] Liu Y H, Mao Z Y, Yu W H, Lu Q F, Wang D J 2010 J. Alloys Comp. 493 406
[15] Gu Y X, Zhang Q H, Li Y G, Wang H Z 2011 J. Alloys Comp. 509 L109
[16] Li P L, Yang Z P, Wang Z J, Xiong Z J, Guo Q L 2008 Acta Phys. Chim. Sin. 24 179(in Chinese) [李盼来, 杨志平, 王志军, 熊志军, 郭庆林 2008 物理化学学报 24 179]
[17] Luo Y Y, Jo D S, Senthil K, Tezuka S, Kakihana M, Toda K, Masaki T, Yoon D H 2012 J. Solid State Chem. 189 68
[18] Wang Z J, Li P L, Wang G, Yang Z P, Guo Q L 2008 Acta Phys. Sin. 57 4575(in Chinese) [王志军, 李盼来, 王刚, 杨志平, 郭庆林 2008 物理学报 57 4575]
[19] Zheng X, Fei Q N, Mao Z Y, Liu Y H, Cai Y, Lu Q F, Tian H, Wang D J 2011 J. Rare Earths 29 522
[20] Zhang M, He X, Ding W J, Wang J 2010 Prog. Chem. 22 376(in Chinese) [张梅, 何鑫, 丁维嘉, 王静 2010 化学进展 22 376]
[21] Su Q, Zeng Q H, Pei Z W 2000 Chin. J. Inorg. Chem. 16 293(in Chinese) [苏锵, 曾庆华, 裴治武 2000 无机化学学报 16 293]
[22] Li J Y 2003 Rare Earth Luminescent Material and Applications (Beijing: Chemical Industry Press) pp3-4 (in Chinese) [李建宇 2000 稀土发光材料及其应用(北京: 化学化工出版社)第3–4页]
[23] Choi S W, Hong S H, Kim Y J 2009 J. Am. Ceram. Soc. 92 2025
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