Dissolution Mechanisms of Tetravalent Sulphur in Silicate Melts : Evidences from Sulphur K Edge XANES Studies on Glasses
Dissolution Mechanisms of Tetravalent Sulphur in Silicate Melts : Evidences from Sulphur K Edge XANES Studies on Glasses
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四价硫在硅酸盐熔体中的溶解机制：玻璃上硫 K Edge XANES 研究的证据
DOI：
10.1111/j.1551-2916.2007.02044.x
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发表时间：
2008
影响因子：
3.9
通讯作者：
Deubener
中科院分区：
文献类型：
--
作者：
Backnaes;L. Stelling;Behrens;Göttlicher;Mangold;Verheijen;Beerkens;R. G. C;Deubener
用X射线吸收近边结构（XANES）光谱研究了高温下熔体与含硫源反应产生的硅酸盐玻璃中硫的掺入。以三硅酸钠、钠钙硅酸盐和浮法玻璃为原料，进行了三种类型的合成：(i)在环境压力下用SO2或SO2/ o2气体混合物控制玻璃熔体的起泡；（ii）在超过熔体预期溶解度的情况下熔化含有各种盐（Na2SO4、Na2SO3、Na2S）的玻璃粉；（iii）在1000℃和100 MPa下，在低于预期硫溶解度的盐的添加量下，在金胶囊中熔化玻璃粉。在后面的一些实验中，引入水来改变系统中的氧逸度。通过燃烧和随后的红外光谱测定玻璃中的硫浓度；用红外光谱法测定了玻璃中的水浓度。用电子探针检测了玻璃的体组成和均匀性。在室温下获得的XANES光谱给出了在所有玻璃中存在硫酸盐（S6+）和/或硫化物（单硫化物[S2−]和/或多硫化物[Sx2−]）的证据，具体取决于起始材料和运行条件。在所有的光谱中都没有发现亚硫酸盐（S4+）的明显证据，这意味着在室温下玻璃制品中的这种硫化物等于或低于检测极限。我们认为，四价硫（如so2或Na2SO3）在溶解于简单硅酸盐熔体或冷却玻璃熔体时歧化成硫酸盐和硫化物。
Incorporation of sulphur in silicate glasses produced by reactions between melts and sulphur‐bearing sources at high temperatures was studied by X‐ray absorption near edge structure (XANES) spectroscopy at the sulphur K edge. Three types of syntheses were performed using sodium trisilicate, soda lime silicate, and float glass as starting materials: (i) controlled bubbling of glass melts with SO2or SO2/O2gas mixtures at ambient pressure, (ii) melting of glass powder containing various salts (Na2SO4, Na2SO3, Na2S) in excess to the expected solubility in the melt and (iii) fusion of glass powder in gold capsules at 1000°C and 100 MPa with an added amount of salts below the expected sulphur solubility. In some of the latter experiments water was introduced to vary the oxygen fugacity in the system. Sulphur concentrations in the glasses were determined by combustion and subsequent IR spectroscopy; water concentration in the glasses was measured by IR microspectroscopy. Bulk composition and homogeneity of glasses were checked by electron microprobe analyses. XANES spectra obtained at room temperature give evidence for incorporation of sulfate (S6+) and/or sulfide (monosulfide [S2−] and/or polysulfide [Sx2−]) in all glasses, depending on starting materials and run conditions. Clear evidence for sulfite (S4+) was not found in any of the spectra, implying that this sulphur species in glass products at room temperature is at or below the detection limit. We suggest that tetravalent sulphur (as SO2or Na2SO3) disproportionates into sulfate and sulfide when being dissolved in simple silicate melts or during cooling of the glass melt.
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影响因子：
1.4
作者：
S. Rossano;E. Balan;G. Morin;J.-P. Bauer;G. Calas;C. Brouder
通讯作者：
S. Rossano;E. Balan;G. Morin;J.-P. Bauer;G. Calas;C. Brouder
影响因子：
2.5
作者：
Ravel, B;Newville, M
通讯作者：
Newville, M
冷却时流纹石玻璃中 H2O + O →2 2OH 反应的动力学：地球速度测量法以及与玻璃化转变的比较
DOI：
--
发表时间：
1997
期刊：
影响因子：
--
作者：
Youxue Zhang;Juleen Jenkins;Zhengjiu Xu
通讯作者：
Zhengjiu Xu
钠钙硅玻璃熔体中的硫酸盐分解和氧化钠活性
影响因子：
3.9
作者：
R. Beerkens
通讯作者：
R. Beerkens
硫 K 边 XANES 光谱：硅酸盐玻璃中硫的化学状态和含量
DOI：
--
发表时间：
2005
期刊：
影响因子：
--
作者：
M. Fleet;Xiaoyang Liu;S. Harmer;P. King
通讯作者：
P. King