Competitive effects of modifier charge and size on mechanical and chemical resistance of aluminoborate glasses

Mascaraque, Nerea; Frederiksen, Kristine F.; Januchta, Kacper; Youngman, Randall E.; Bauchy, Mathieu; Smedskjær, Morten Mattrup

doi:10.1016/j.jnoncrysol.2018.07.034

Cited by 7 publications

(8 citation statements)

References 36 publications

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“…Moreover, we have found that the abundance of B III non‐ring units is relatively higher in the Mg‐aluminoborate glasses compared to the Na‐ and Li‐aluminoborate glasses (see Figure ). This suggests that the magnesium could cause breakage of B III ring to B III non‐ring units by associating with the B III network through formation of B III –O–Mg bonds, which is possible due to its partial network‐former character with coordination number of four . Thus, the pronounced difference in the structure of the Mg‐series, compared to the Li‐ and Na‐series for the same Al/B ratio, is due to the significantly higher field strength of Mg 2+ (0.45 Å −2 ) compared to Li + (0.23 Å −2 ) and Na + (0.17 Å −2 ) and the dual nature of Mg 2+ in oxide glasses.…”

Section: Resultsmentioning

confidence: 99%

“…The dissolution mechanism of borate‐based glasses can be understood through the reactions of ion‐exchange (Equations and ) and hydrolysis (Equations and ) . In neutral solution, there is a mix of H + /H 3 O + and OH − ions, i.e., protonation and hydrolysis are strongly coupled with the possible reactions:

{[{(B,Al)O}_{4}]}^{-} - {normalM}^{+} + 4 {normalH}_{2} O \to false[{(B,Al)(OH)}_{4} false] + {normalM}^{+} + 4 {OH}^{-}

{[false(normalB, Al false) {normalO}_{4}]}_{2}^{-} - {normalM}^{2 +} + 8 {normalH}_{2} O \to {[false(normalB, Al false) {(OH)}_{4}]}_{2} + {normalM}^{2 +} + 8 {OH}^{-}

(B,Al) - O - B + {normalH}_{2} O \to 2 false((B,Al) - OH false)

…”

Section: Resultsmentioning

confidence: 99%

“…Indeed, substitution of Na 2 O with Li 2 O led to the discovery of a 24Li 2 O–21Al 2 O 3 –55B 2 O 3 glass that exhibits the highest crack resistance ever reported for any annealed, melt‐quenched oxide glass . In our recent study, the effect of modifier substitution in glasses with fixed Al/B ratio on the structural and mechanical properties was investigated. Magnesium aluminoborate glasses were found to exhibit the highest hardness and intermediate crack resistance.…”

Section: Introductionmentioning

confidence: 98%

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Structural dependence of chemical durability in modified aluminoborate glasses

et al. 2018

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Alkali and alkaline earth aluminoborate glasses feature high resistance to cracking under sharp contact loading compared to other oxide glasses. However, due to the high content of hygroscopic B2O3, it is expected that applications of these glasses could be hindered by poor chemical durability in aqueous solutions. Indeed, the compositional and structural dependence of their dissolution kinetics remains unexplored. In this work, we correlate the dissolution rates of aluminoborate glasses in acidic, neutral, and basic solutions with the structural changes induced by varying the aluminum‐to‐boron ratio. In detail, we investigate a total of seventeen magnesium, lithium, and sodium aluminoborate glasses with fixed modifier content of 25 mol%. We show that the structural changes induced by alumina depend on the network modifier. We also demonstrate a correlation between the chemical durability at various pH values and the structural changes in Mg‐, Li‐ and Na‐aluminoborate glasses. The substitution of alumina by boron oxide leads to a general decrease in chemical corrosion in neutral and acidic solutions. The lowest dissolution rate value is observed in Mg‐aluminoborate glasses, as a consequence of the intermediate character of magnesium which can increase the network cross‐linking. For basic solutions, the chemical durability is almost constant for the different amount of alumina in the three series, likely because B2O3 is susceptible to nucleophilic attack, which is favored in high‐OH− solutions.

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Section: Resultsmentioning

confidence: 99%

{[{(B,Al)O}_{4}]}^{-} - {normalM}^{+} + 4 {normalH}_{2} O \to false[{(B,Al)(OH)}_{4} false] + {normalM}^{+} + 4 {OH}^{-}

{[false(normalB, Al false) {normalO}_{4}]}_{2}^{-} - {normalM}^{2 +} + 8 {normalH}_{2} O \to {[false(normalB, Al false) {(OH)}_{4}]}_{2} + {normalM}^{2 +} + 8 {OH}^{-}

(B,Al) - O - B + {normalH}_{2} O \to 2 false((B,Al) - OH false)

…”

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 98%

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Structural dependence of chemical durability in modified aluminoborate glasses

et al. 2018

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“…We determine the values of m , C g , and ν for both the newly-synthesized glasses and those missing from previous studies [18,46,47,48,49], as shown in Table 1. First, the densities ( ρ ) of the glasses were determined using the Archimedes principle with ethanol as the immersion medium.…”

Section: Methodsmentioning

confidence: 99%

“…Since experimental data on oxide glasses with ν > 0.30 are scarce, we also synthesize a total of 20 new oxide glasses, particularly aluminoborate and zinc borate glasses as these have been found to have relatively high Poisson’s ratio [45,46]. To further expand the dataset, we also determine the missing property (e.g., m if only C g and ν are known) from previously synthesized glasses in our laboratory [18,46,47,48,49]. Moreover, we subject selected oxide glasses to high-temperature densification to induce a higher C g value in bulk samples and then probe whether it correlates with an expected increase in ν.…”

Section: Introductionmentioning

confidence: 99%

Revisiting the Dependence of Poisson’s Ratio on Liquid Fragility and Atomic Packing Density in Oxide Glasses

et al. 2019

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Poisson’s ratio (ν) defines a material’s propensity to laterally expand upon compression, or laterally shrink upon tension for non-auxetic materials. This fundamental metric has traditionally, in some fields, been assumed to be a material-independent constant, but it is clear that it varies with composition across glasses, ceramics, metals, and polymers. The intrinsically elastic metric has also been suggested to control a range of properties, even beyond the linear-elastic regime. Notably, metallic glasses show a striking brittle-to-ductile (BTD) transition for ν-values above ~0.32. The BTD transition has also been suggested to be valid for oxide glasses, but, unfortunately, direct prediction of Poisson’s ratio from chemical composition remains challenging. With the long-term goal to discover such high-ν oxide glasses, we here revisit whether previously proposed relationships between Poisson’s ratio and liquid fragility (m) and atomic packing density (Cg) hold for oxide glasses, since this would enable m and Cg to be used as surrogates for ν. To do so, we have performed an extensive literature review and synthesized new oxide glasses within the zinc borate and aluminoborate families that are found to exhibit high Poisson’s ratio values up to ~0.34. We are not able to unequivocally confirm the universality of the Novikov-Sokolov correlation between ν and m and that between ν and Cg for oxide glass-formers, nor for the organic, ionic, chalcogenide, halogenide, or metallic glasses. Despite significant scatter, we do, however, observe an overall increase in ν with increasing m and Cg, but it is clear that additional structural details besides m or Cg are needed to predict and understand the composition dependence of Poisson’s ratio. Finally, we also infer from literature data that, in addition to high ν, high Young’s modulus is also needed to obtain glasses with high fracture toughness.

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