(CaO-SiO_(2))-xAl_(2)O_(3)三元系玻璃微结构的拉曼光谱定量研究  

Quantitative Study on Microstructure of(CaO-SiO_(2))-xAl_(2)O_(3) Ternary Glass by Raman Spectroscopy

作　　者：唐晓辉 尤静林[1] 王建[1] 王敏[1] 龚晓晔 张福 Kai Tang TANG Xiaohui;YOU Jinglin;WANG Jian;WANG Min;GONG Xiaoye;ZHANG Fu;Kai TANG(State Key Laboratory of Advanced Special Steel & Shanghai Key Laboratory of Advanced Ferrometallurgy, School of Materials Science and Engineering, Shanghai University, Shanghai 200444, P. R. China;SINTEF Industry, Trondheim, 7094, Norway)

机构地区：[1]省部共建高品质特殊钢冶金与制备国家重点实验室,上海市钢铁冶金新技术开发应用重点实验室,上海大学材料科学与工程学院,上海200444 [2]SINTEF Industry, Trondheim, 7094, Norway

出　　处：《光散射学报》2022年第1期22-29,共8页The Journal of Light Scattering

基　　金：国家自然科学基金(21773152);上海市科学技术委员会项目(12520709200);省部共建高品质特殊钢冶金与制备国家重点实验室开放课题(SKLASS2015-01,SKLASS2017-02);省部共建高品质特殊钢冶金与制备国家重点实验室自主课题(SKLASS2016-Z01);111引智项目(D17002);科技部中央引导基金(YDZX20173100001316C)。

摘　　要：本文采用气动悬浮装置成功制备了(CaO-SiO_(2))-xAl_(2)O_(3)(x=0,6,12,18,24,30)的一系列玻璃,并通过拉曼光谱技术结合量子化学从头计算方法、^(27)Al魔角旋转核磁共振技术(^(27)Al MAS-NMR)对其结构进行了定性及定量研究。研究结果表明,当碱度R(CaO/SiO_(2))=1时,随着Al_(2)O_(3)的加入,硅酸盐结构转变为铝硅酸盐结构。当x≤18时,Al主要以[^(Ⅳ)AlO_(4)]形式参与网络形成,并在x=18时达到最大,同时也观察到了[^(Ⅴ)AlO_(5)]、[^(Ⅵ)AlO_(6)]的存在;当x>18时,[^(Ⅳ)AlO_(4)]相对含量减少,[^(Ⅴ)AlO_(5)]、[^(Ⅵ)AlO_(6)]增加。拉曼光谱精细解谱的结果表明,Al的加入大大增加了体系的复杂性和无序性,具体表现为精细结构Qijklm含量的无规律变化,但对初级结构Q_(i)含量的影响不大,并主要以Q_(2)形式存在。A series of(CaO-SiO_(2))-xAl_(2)O_(3)(x=0,6,12,18,24,30)glasses were successfully prepared in a pneumatic suspension device,and their structures were qualitatively and quantitatively studied by Raman spectroscopy,quantum chemistry ab initio calculation and ^(27)Al MAS-NMR.It shows that when the basicity R(CaO/SiO_(2))=1,Al mainly participates in the network formation in the form of[^(Ⅳ)AlO_(4)]by x≤18 and reaches the maximum when x=18.At the same time,the existence of[^(Ⅴ)AlO_(5)]and[^(Ⅵ)AlO_(6)]is also observed;When x>18,the relative content of[^(Ⅳ)AlO_(4)]decreased,while[^(Ⅴ)AlO_(5)]and[^(Ⅵ)AlO_(6)]increased.The results of Raman fine resolution spectra show that the addition of Al greatly increases the complexity and disorder of the structure,which is manifested by the irregular change of the content of fine structure Qijklm,but has little effect on the content of primary structure Q_(i) which mainly exists in the form of Q_(2).

关 键 词：CaO-SiO_(2)-Al_(2)O_(3) 拉曼光谱 量子化学从头算 微结构定量 

分 类 号：O657.37[理学—分析化学]