Aine G. Black , Alex Scrimshire , Dinu Iuga , Yan Lavallée , Kate A. Morrison , Paul A. Bingham , Tracey Taylor , Laura Leay , Mike T. Harrison , Frédéric Blanc , Maulik K. Patel
{"title":"锂浓度对核废料玻璃网络连通性的影响","authors":"Aine G. Black , Alex Scrimshire , Dinu Iuga , Yan Lavallée , Kate A. Morrison , Paul A. Bingham , Tracey Taylor , Laura Leay , Mike T. Harrison , Frédéric Blanc , Maulik K. Patel","doi":"10.1016/j.jnoncrysol.2024.123234","DOIUrl":null,"url":null,"abstract":"<div><div>Structure of borosilicate glasses with varying Li<sub>2</sub>O contents were investigated using Magic Angle Spinning (MAS) Nuclear Magnetic Resonance (NMR), employing <sup>6</sup>Li, <sup>11</sup>B, <sup>23</sup>Na, <sup>27</sup>Al and <sup>29</sup>Si nuclei. <sup>11</sup>B MAS NMR revealed that increasing Li<sub>2</sub>O contents result in formation of [BO<sub>4</sub>]<sup>−</sup> sites at the expense of BO<sub>3</sub>. <sup>11</sup>B{<sup>6</sup>Li} and <sup>27</sup>Al{<sup>6</sup>Li} dipolar heteronuclear multiple quantum correlation (D-HMQC) NMR revealed Li as a charge compensator for anionic tetrahedral sites with increased Li. <sup>11</sup>B{<sup>6</sup>Li} J-coupling mediated HMQC NMR suggested the possible association of Li with non-bridging oxygens on Q<sup>2</sup> and Q<sup>3</sup> sites, indicating its dual role in the glass network. <sup>29</sup>Si and <sup>23</sup>Na 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.</div></div>","PeriodicalId":16461,"journal":{"name":"Journal of Non-crystalline Solids","volume":"646 ","pages":"Article 123234"},"PeriodicalIF":3.2000,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of lithium concentration on the network connectivity of nuclear waste glasses\",\"authors\":\"Aine G. Black , Alex Scrimshire , Dinu Iuga , Yan Lavallée , Kate A. Morrison , Paul A. Bingham , Tracey Taylor , Laura Leay , Mike T. Harrison , Frédéric Blanc , Maulik K. Patel\",\"doi\":\"10.1016/j.jnoncrysol.2024.123234\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Structure of borosilicate glasses with varying Li<sub>2</sub>O contents were investigated using Magic Angle Spinning (MAS) Nuclear Magnetic Resonance (NMR), employing <sup>6</sup>Li, <sup>11</sup>B, <sup>23</sup>Na, <sup>27</sup>Al and <sup>29</sup>Si nuclei. <sup>11</sup>B MAS NMR revealed that increasing Li<sub>2</sub>O contents result in formation of [BO<sub>4</sub>]<sup>−</sup> sites at the expense of BO<sub>3</sub>. <sup>11</sup>B{<sup>6</sup>Li} and <sup>27</sup>Al{<sup>6</sup>Li} dipolar heteronuclear multiple quantum correlation (D-HMQC) NMR revealed Li as a charge compensator for anionic tetrahedral sites with increased Li. <sup>11</sup>B{<sup>6</sup>Li} J-coupling mediated HMQC NMR suggested the possible association of Li with non-bridging oxygens on Q<sup>2</sup> and Q<sup>3</sup> sites, indicating its dual role in the glass network. <sup>29</sup>Si and <sup>23</sup>Na 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.</div></div>\",\"PeriodicalId\":16461,\"journal\":{\"name\":\"Journal of Non-crystalline Solids\",\"volume\":\"646 \",\"pages\":\"Article 123234\"},\"PeriodicalIF\":3.2000,\"publicationDate\":\"2024-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Non-crystalline Solids\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0022309324004113\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, CERAMICS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Non-crystalline Solids","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0022309324004113","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, CERAMICS","Score":null,"Total":0}
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.
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.