Correlating Sulfur Solubility with Short-to-Intermediate Range Ordering in the Structure of Borosilicate Glasses

Autor(es)

Saini, Rajan ^{[1, 2]} ; Kapoor, Saurabh ^[3] ; Neuville, Daniel R. ^[4] ; Youngman, Randall E. ^[5] ; Cerrutti, Bianca M. ^[6] ; McCloy, John S. ^[7] ; Eckert, Hellmut ^{[8, 6]} ; Goel, Ashutosh ^[1]

Afiliação do(s) autor(es)

^[1] Rutgers State Univ, Dept Mat Sci & Engn, Piscataway, NJ 08854 - USA

^[2] Akal Univ, Dept Phys, Talwandi Sabo 151302, Punjab - India

^[3] Ctr Excellence Sterlite Technol Ltd, Aurangabad 431136, Maharashtra - India

^[4] Univ Paris, CNRS Geomat, Inst Phys Globe Paris, F-75005 Paris - France

^[5] Corning Inc, Sci & Technol Div, Corning, NY 14831 - USA

^[6] Univ Sao Paulo, Sao Carlos Inst Phys, BR-13566590 Sao Carlos, SP - Brazil

^[7] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 - USA

^[8] WWU Munster, Inst Phys Chem, D-48149 Munster - Germany

• Tipo de documento: Artigo Científico
• Fonte: Journal of Physical Chemistry C; JAN 2022.
• Citações Web of Science: 0

Resumo

The present study focuses on understanding the structural dependence of sulfur (as SO3) solubility in Na2O-B2O3-SiO2 glasses over a broad composition space exhibiting a rich variety of structural associations. The focus is on probing the impact of the (1) structural role of Na+, (2) degree of polymerization, and (3) network former connectivity (formation of Si-O-B and B-O-B linkages) on sulfur solubility in borosilicate glasses. By employing a suite of state-of-the-art characterization techniques, including inductively coupled plasma-optical emission spectroscopy (ICP-OES), magic-angle spinning (MAS) NMR spectroscopy, and Raman spectroscopy, an inverse correlation has been established between the sulfur solubility and the degree of network polymerization in the glasses across the investigated composition space. While the modification of SO3 leading to the formation of SO42- can successfully compete with the network depolymerization mechanisms (i.e., creation of nonbridging oxygens) and induce repolymerization in the glass network, the BO3 -> BO4 conversion facilitated by the charge compensation by alkali cations takes precedence. The results from this study, when extended to more complex borosilicate-based glass compositions, will not only add to our understanding of the fundamental science controlling the sulfur solubility in borosilicate-based real-world nuclear waste glasses but will also form a basis for the development of nonempirical quantitative structure-property relationship (QSPR)-based predictive models. (AU)

• Processo FAPESP: 13/07793-6 - CEPIV - Centro de Ensino, Pesquisa e Inovação em Vidros
• Beneficiário: Edgar Dutra Zanotto
• Modalidade de apoio: Auxílio à Pesquisa - Centros de Pesquisa, Inovação e Difusão - CEPIDs