Sr_(0.955)Al_(2-x)B_xSi_2O_8∶0.025Eu~(2+)荧光粉的制备、晶体结构及发光性能（英文）
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摘要
通过高温固相反应在弱还原气氛下制备了Sr_(0.955)Al_(2-x)B_xSi_2O_8∶0.025Eu~(2+)(x=0～0.9)一系列荧光粉,研究了B(Ⅲ)取代基质晶格中的Al(Ⅲ)对荧光粉晶体结构和Eu~(2+)发光性能的影响。B(Ⅲ)以类质同相取代基质晶格中Al(Ⅲ),形成了连续固溶体。随着B(Ⅲ)取代量的增加,荧光粉的晶胞参数(a、b、c)和晶胞体积(V)呈线性递减,而晶胞参数(β)呈线性递增。荧光粉的激发光谱为位于225～400nm的宽峰,表观峰值位于350 nm,激发峰的半高宽(FWHM)随着B(Ⅲ)取代量的增加,从90 nm减小到102 nm。发射光谱位于370～600 nm的宽峰,可拟合为409和447 nm两个峰,表观峰值位于409 nm。随着B(Ⅲ)取代量的增加,2个拟合峰位均出现蓝移且2个峰强度比呈线性递减。根据试样荧光光谱,通过Van Uitert经验公式计算得出SrAl_2Si_2O_8∶Eu~(2+)中Sr~(2+)的配位数为9。随着B(Ⅲ)取代Al(Ⅲ)进入基质晶格,造成发光中心Eu与配体O距离增加,使得Eu~(2+)所处的晶体场强度减小,发光中心Eu~(2+)的5d能级分裂减小,造成Eu~(2+)最低发射能级重心上移,2个拟合谱峰峰位均呈线性蓝移。
A series of luminescence phosphors Sr_(0.955)Al_(2-x)B_xSi_2O_8∶0.025Eu~(2+)(x=0～0.9)were prepared via solid-state reaction in a weak reductive atmosphere.The lattice positions and the luminescent mechanism of Eu~(2+)in the host were discussed,the effects of B(Ⅲ)-substitution on the host lattices and spectral properties were also investigated.It was found that the complete solid solutions were formed in the whole range of x=0～0.9,as B(Ⅲ)substituted for Al(Ⅲ)entered to SrAl_2Si_2O_8.The lattice parameters(a,b,c)and unit cell volume(V)of phosphors Sr_(0.955)Al_(2-x)B_xSi_2O_8∶0.025Eu~(2+)(x=0～0.9)decreased linearly and lattice parameter(β)increased linearly as the increase of substitution amount of B(Ⅲ).A broad excitation spectrum consisted of four excitation bands,which was in a range of 225～400nm,and an apparent peak at 350 nm.Full width at half maximum(FWHM)increased from 90 to 102 nm as increase of the substitution amount of B(Ⅲ).The emission spectrum was a broad-band in a range of 370～600 nm,which could be fitted two peaks of 409 and 447 nm,and its apparent peak was at 409 nm.Two fitted peaks were blue shifted and the intensity ratio of the fitted peaks decreased linearly as the increase of the substitution amount of B(Ⅲ)).The coordination number of Sr~(2+)was 9 in SrAl_2Si_2O_8∶Eu~(2+),which has been confirmed by the experimental results and empirical formula of Van Uitert.The distance between the luminescent center Eu and the ligand O increased due to the Al(Ⅲ)replaced by B(Ⅲ),so that the crystal field strength of Eu~(2+)decreased,and the 5d energy level split of the luminescent center Eu~(2+)decreased,the center of gravity of the lowest emission level of Eu~(2+)was shifted upward,and the two fitted peaks were linearly blue-shifted.
A series of luminescence phosphors Sr_(0.955)Al_(2-x)B_xSi_2O_8∶0.025Eu~(2+)(x=0～0.9)were prepared via solid-state reaction in a weak reductive atmosphere.The lattice positions and the luminescent mechanism of Eu~(2+)in the host were discussed,the effects of B(Ⅲ)-substitution on the host lattices and spectral properties were also investigated.It was found that the complete solid solutions were formed in the whole range of x=0～0.9,as B(Ⅲ)substituted for Al(Ⅲ)entered to SrAl_2Si_2O_8.The lattice parameters(a,b,c)and unit cell volume(V)of phosphors Sr_(0.955)Al_(2-x)B_xSi_2O_8∶0.025Eu~(2+)(x=0～0.9)decreased linearly and lattice parameter(β)increased linearly as the increase of substitution amount of B(Ⅲ).A broad excitation spectrum consisted of four excitation bands,which was in a range of 225～400nm,and an apparent peak at 350 nm.Full width at half maximum(FWHM)increased from 90 to 102 nm as increase of the substitution amount of B(Ⅲ).The emission spectrum was a broad-band in a range of 370～600 nm,which could be fitted two peaks of 409 and 447 nm,and its apparent peak was at 409 nm.Two fitted peaks were blue shifted and the intensity ratio of the fitted peaks decreased linearly as the increase of the substitution amount of B(Ⅲ)).The coordination number of Sr~(2+)was 9 in SrAl_2Si_2O_8∶Eu~(2+),which has been confirmed by the experimental results and empirical formula of Van Uitert.The distance between the luminescent center Eu and the ligand O increased due to the Al(Ⅲ)replaced by B(Ⅲ),so that the crystal field strength of Eu~(2+)decreased,and the 5d energy level split of the luminescent center Eu~(2+)decreased,the center of gravity of the lowest emission level of Eu~(2+)was shifted upward,and the two fitted peaks were linearly blue-shifted.
引文
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[2] Ci Z P, Que M D, Shi Y R, et al. Inorg. Chem., 2014,53:2195-2199
[3] Xia Z G, Liu Q L. Prog. Mater. Sci., 2016,84:59-117
[4] Lin C C, MeijerinkA, Liu R S. J. Phys. Chem. Lett., 2016,7:495-503
[5] Zhong J S, Chen D Q, Yuan S, et al. Inorg. Chem., 2018,57:8978-8987
[6] Ye S, Xiao F, Pan Y X, et al. Mater. Sci. Eng. R, 2010,71:1-34
[7] Cai P Q, Qin L, Chen C L, et al. Inorg. Chem., 2018,57:3073-3081
[8] WANG Fei(王飞). Acta Photonica Sinica(光子学报), 2018,47(8):0816001
[9] Ray S, Tadge P, Nair G B, et al. Ceram. Int., 2018,44:5506-5512
[10]Homayoni H, Sahi S, Ma L. J. Lumin., 2018,198:132-137
[11]Tang Z B, Wang D Y, Khan W U, et al. J. Mater. Chem. C,2016,4:5307-5313
[12]Kalaycioglu N O, Circir E. J. Therm. Anal. Calorim., 2013,111:273-277
[13]Hai O, Jiang H Y, Xu D, et al. Mater. Res. Bull., 2016,76:358-364
[14]Yang W J, Luo L Y, Chen T M, et al. Chem. Mater., 2005,17:3883-3888
[15]Clabau F, Garcia A, Bonville P, et al. J. Solid State Chem.,2008,181:1456-1461
[16]WANG Fei(王飞), TIAN Yi-Guang(田一光), ZHANG Qiao(张乔). Chinese J. Inorg. Chem.(无机化学学报), 2014,30(11):2530-2536
[17]Shang M, Liang S, Qu N, et al. Chem. Mater., 2017,29:1813-1829
[18]Zhou J, Wang Y H, Liu B T, et al. J. Alloys Compd, 2009,484:439-443
[19]Chiari G, Calleri M, Bruno E, et al. Am. Mineral., 1975,60:111-115
[20]Van Uitert L G. J. Lumin., 1984,29:1-9
[21]Dorenbos P. J. Lumin., 2003,104:239-260
[22]Ye S, Liu Z S, Wang X T, et al. J. Lumin., 2009,129:50-54
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