硅酸盐熔体团粒结构类声子振动的高温拉曼光谱研究

doi:10.3964/j.issn.1000-0593(2010)05-1261-05

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摘要：硅酸盐熔体是典型的近程有序，远程无序的准稳定态分数维体系，文章采用X射线小角散射(SAXS)、低波数拉曼光谱(LWRS)及高温拉曼光谱(HTRS)实时、原位分析等技术，对高温熔融法和溶胶凝胶法合成的CaO-Al₂O₃-SiO₂和Na₂O-Al₂O₃-SiO₂系列低维非晶硅酸盐试样进行了团粒结构粒度及其类声子振动频率的定量测定，获得了低温硅酸盐凝胶、高温硅酸盐熔体及其淬火玻璃相均具有纳米级(几个纳米至几十纳米)自相似团粒结构和类声子振动模的重要结论，进而建立了测定高温熔体介观团粒结构粒度的HTRS测定法，结果表明硅酸盐熔体的团粒结构粒度在高温下均会比其室温玻璃相的团粒尺度小，且高温熔体的网络结构基元也向桥氧数减少之基元转变。这些结论为探索自然界岩浆的地球化学特征、岩浆的结晶和演化以及低维硅酸盐材料结构性能的改进提供重要理论依据及信息。

关键词：硅酸盐熔体;介观团粒结构;类声子振动;高温拉曼光谱

Abstract：Silicate melts are special fractal dimension system that is metastable state of near-way order and far-way disorder. In this paper，the size of nanometer aggregation structure and the frequences of phonon vibration like mode in the low dimension silicate series(CaO-Al₂O₃-SiO₂ and Na₂O-Al₂O₃-SiO₂ series) synthesized via high temperature melting and sol gel methods were measured by means of small-angle X-ray scattering (SAXS), low wavenumber Raman spectrum(LWRS) and high temperature Raman spectrum(HTRS in situ measuring). The nanometer self-similarity aggregation structure(it’s size is about a few nm to a few tens nm) and phonic phonon vibration like modes of low temperature silicate gel, high temperature silicate melts and it’s quenching glasses phases were obtained. So a quantitative method by HTRS for measuring the aggregation size in the high temperature melts was established. The results showed that the aggregation size of the silicate melts is smaller at high temperature than at room temperature and the number of bridge oxygen in one Si—O tetrahedron in network structure units is decreasing at high temperature. This study work provides important theory and information for deliberating geochemistry characteristic, crystallization & evolution of natural magma and enhancing performance of low dimension silicate matelials.

Key words：Silicate melts;Nanometer aggregation structure;Phonon vibration like modes;High temperature Raman spectrum

收稿日期: 2009-05-16 修订日期: 2009-08-20

中图分类号:

O741

通讯作者: 徐培苍 E-mail: xpc@jstu.edu.cn; xupeicang42@tom.com

引用本文:

徐培苍¹，李如璧¹，尚通明¹，周健¹，孙建华¹，尤静林² . 硅酸盐熔体团粒结构类声子振动的高温拉曼光谱研究[J]. 光谱学与光谱分析, 2010, 30(05): 1261-1265.
XU Pei-cang¹，LI Ru-bi¹，SHANG Tong-ming¹，ZHOU Jian¹，SUN Jian-hua¹，YOU Jing-lin² . A Study of Phonon Vibration Like Modes for Aggregation Structure in Silicate Melts by High Temperature Raman Spectrum . SPECTROSCOPY AND SPECTRAL ANALYSIS, 2010, 30(05): 1261-1265.

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