锂浓度对核废料玻璃网络连通性的影响

IF 3.2 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Journal of Non-crystalline Solids Pub Date : 2024-10-01 DOI:10.1016/j.jnoncrysol.2024.123234
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引用次数: 0

摘要

利用魔角旋转(MAS)核磁共振(NMR)技术,采用 6Li、11B、23Na、27Al 和 29Si 核对不同 Li2O 含量的硼硅玻璃的结构进行了研究。11B MAS 核磁共振显示,Li2O 含量的增加会导致[BO4]- 位点的形成,从而牺牲了 BO3。11B{6Li} 和 27Al{6Li} 双极异核多重量子相关 (D-HMQC) NMR 显示,随着锂含量的增加,锂成为阴离子四面体位点的电荷补偿器。11B{6Li}11B{6Li} J 耦合介导的 HMQC NMR 显示,锂可能与 Q2 和 Q3 位点上的非桥氧结合,这表明锂在玻璃网络中具有双重作用。29Si 和 23Na MAS NMR 光谱显示,随着锂的增加,硅酸盐网络解聚,Na-O 键长度缩短。拉曼光谱和热分析表明,锂含量越高,硅酸盐网络越解聚,玻璃化转变温度越低,这为核磁共振结果提供了支持。
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Effect of lithium concentration on the network connectivity of nuclear waste glasses
Structure of borosilicate glasses with varying Li2O contents were investigated using Magic Angle Spinning (MAS) Nuclear Magnetic Resonance (NMR), employing 6Li, 11B, 23Na, 27Al and 29Si nuclei. 11B MAS NMR revealed that increasing Li2O contents result in formation of [BO4] sites at the expense of BO3. 11B{6Li} and 27Al{6Li} dipolar heteronuclear multiple quantum correlation (D-HMQC) NMR revealed Li as a charge compensator for anionic tetrahedral sites with increased Li. 11B{6Li} J-coupling mediated HMQC NMR suggested the possible association of Li with non-bridging oxygens on Q2 and Q3 sites, indicating its dual role in the glass network. 29Si and 23Na MAS NMR spectra showed depolymerisation of the silicate network and shortening of Na-O bond lengths with increased Li. NMR results are supported by Raman spectroscopy and thermal analysis that indicate depolymerisation of the silicate network and a reduction in glass transition temperature at higher Li content.
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来源期刊
Journal of Non-crystalline Solids
Journal of Non-crystalline Solids 工程技术-材料科学:硅酸盐
CiteScore
6.50
自引率
11.40%
发文量
576
审稿时长
35 days
期刊介绍: The Journal of Non-Crystalline Solids publishes review articles, research papers, and Letters to the Editor on amorphous and glassy materials, including inorganic, organic, polymeric, hybrid and metallic systems. Papers on partially glassy materials, such as glass-ceramics and glass-matrix composites, and papers involving the liquid state are also included in so far as the properties of the liquid are relevant for the formation of the solid. In all cases the papers must demonstrate both novelty and importance to the field, by way of significant advances in understanding or application of non-crystalline solids; in the case of Letters, a compelling case must also be made for expedited handling.
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