基于精细结构对二元钠硅酸盐玻璃核磁共振波谱的研究
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摘要
利用精细结构表征系列(Q_i~(jklm))对二元钠硅酸盐玻璃的核磁共振波谱进行解析,并结合量子化学模拟了多种精细结构.研究结果表明,精细结构的29Si化学位移与桥氧键角呈线性相关;实验所得Q_i~(jklm)结构的化学位移不随玻璃成分的改变而波动,且Q_i~(jklm)结构的高斯峰更窄,说明精细结构表征是二元钠硅酸盐玻璃基本特征结构的表达,导致初级微结构的29Si化学位移变化的本质是精细结构含量的变化.核磁共振波谱表征的是近邻结构的空间信息,采用Q_i~(jklm)结构表征能更精确地描述硅酸盐的微结构信息.
A series of fine structure denotations( Q_i~(jklm)) was applied to analysis NMR spectra of binary sodium silicate glasse,and a variety of clusters was simulated by quantum chemistry ab initio. The results shows that the(29)~Si chemical shift of the fine structure with the same Q_i is linearly related to the bridging oxygen bond angle. The chemical shifts of the experimental Q_i~(jklm)structure does not fluctuate with the glass' composition,and the Gaussian peak of the Q_i~(jklm)structure is narrower. It is indicated that the fine structure characterization is a representation of the basic characteristic structure of the binary sodium silicate glass. It is found that there is a certain gap between theoretical values and experimental values. The results shows that there are multiple configurations of Q_i~(jklm)structures coexisting in the glass,and the interaction between neighboring structures was characterized by NMR. However,the Q_i~(jklm)structural characterization can describe the configuration of various silicate-oxygen tetrahedron more precisely.
A series of fine structure denotations( Q_i~(jklm)) was applied to analysis NMR spectra of binary sodium silicate glasse,and a variety of clusters was simulated by quantum chemistry ab initio. The results shows that the(29)~Si chemical shift of the fine structure with the same Q_i is linearly related to the bridging oxygen bond angle. The chemical shifts of the experimental Q_i~(jklm)structure does not fluctuate with the glass' composition,and the Gaussian peak of the Q_i~(jklm)structure is narrower. It is indicated that the fine structure characterization is a representation of the basic characteristic structure of the binary sodium silicate glass. It is found that there is a certain gap between theoretical values and experimental values. The results shows that there are multiple configurations of Q_i~(jklm)structures coexisting in the glass,and the interaction between neighboring structures was characterized by NMR. However,the Q_i~(jklm)structural characterization can describe the configuration of various silicate-oxygen tetrahedron more precisely.
引文
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[4] Sen S.,Youngman R. E.,J. Non-Crys. Sol.,2003,331(1),100—107
[5] Mahler J.,Sebald A.,Sol. Sta. N. M. R.,1995,5(1),63—64
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[7] Zhang P.,Philip J.,Stebbins J. F.,J. Phys. Chem. B,1997,101(20),4004—4008
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[9] Olivier L.,Yuan X.,Cormack A. N.,J. Non-Crys. Sol.,2001,293(1),53—66
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[11] Azizi S. N.,Rostami A. A.,Godarzian A.,J. Phys. Soc. Jap.,2005,74(5),1609—1620
[12] You J. L.,Jiang G. C.,Hou H. Y.,J. Raman Spectro.,2005,36(3),237—249
[13] Masanori M.,Masaki A.,Mol. Sim.,1991,6(4—6),239—244
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[15] Wang P.,Pan Z. L.,Weng L. B.,System Mineralogy(Album),Geolog Publishing House,Beijing,1984,206—236(王濮,潘兆橹,翁玲宝.系统矿物学(中册),北京:地质出版社,1984,206—236)
[16] Engelhardt S.,Hein L.,Wiesmann F.,Lohse M. J.,Pro. Nat. Aca. Sci.,1999,96(12),7059—7064
[17] Farnan I.,Grandinetti P. J.,Baltisberger J. H.,Nature,1992,358(6381),31—35
[18] Charpentier T.,Ispas S.,Profeta M.,J. Phys. Chem. B,2004,108(13),4147—4161
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[20] Pant A.,Acta Crys. B,Stru. Crys. Crys. Chem.,1968,24(8),1077—1083
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[22] Takéuchi Y.,Ghose S.,Nowacki W.,Zeit. F. Kris.,1965,121(5),321—348
[23] Dupree R.,Holland D.,Mc Millan P. W.,Pettifer R.,J. Non-Crys. Sol.,1984,68(2),399—410
[24] Grimmer A. R.,Von Lampe F.,Tarmak M.,Chem. Phys. Lett.,1983,97(2),185—187
[25] Stebbins J. F.,Zhao P.,Lee S. K.,Cheng X.,Amer. Miner.,1999,84(10),1680—1684
[26] Tsvetkov E.,Davydov A.,Ancharov A.,Yudaev I.,J. Crys. Gro.,2006,294(1),22—28
[27] Tossell J. D.,Rev. Miner. Geochem.,2001,42(1),437—458
[28] You J. L.,Jiang G. C.,Hou H. Y.,Wu Y. Q.,Xu K. D.,Chinese Phys. Lett.,2004,21(4),640—641
[29] Wang W. F.,Tan J.,You J. L.,Zhao S. R.,Zhang D.,Jiang G. C.,J. Chinese Cer. Soc.,2003,1(31),41—46(王卫锋,谭劲,尤静林,赵珊茸,张德,蒋国昌.中国硅酸盐学会,2003,1(31),41—46)