TY - JOUR

T1 - Composition-structure-property effects of antimony in soda-lime-silica glasses

AU - Chen, T.-Y.

AU - Rautiyal, P.

AU - Vaishnav, S.

AU - Gupta, G.

AU - Schlegl, H.

AU - Dawson, R.J.

AU - Evans, A.W.

AU - Kamali, S.

AU - Johnson, J.A.

AU - Johnson, C.E.

AU - Bingham, P.A.

N1 - This is the author’s version of a work that was accepted for publication in Journal of Non-Crystalline Solids. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Non-Crystalline Solids, 544, 2020 DOI: 10.1016/j.jnoncrysol.2020.120184

PY - 2020/9/15

Y1 - 2020/9/15

N2 - Float glass-type SiO 2-Na 2O-CaO glasses with 0 – 10 mol% Sb2O3 were melted and their compositional, structural, thermal and optical properties characterised. All glasses were X-ray amorphous and increasing Sb2O3 content progressively decreased glass transition temperature (Tg) and dilatometric softening point (T d), despite increases in Al2O3 content from greater crucible corrosion. 121Sb Mössbauer spectroscopy confirmed that Sb was predominantly incorporated as Sb 3+ (Sb 3+/ΣSb ~ 0.9) and Raman spectroscopy showed that Sb substantially decreased average (Si, Al)-O Qn speciation. Both techniques confirmed that Sb3+ ions were incorporated in trigonal pyramidal [:SbO 3] polyhedra. XRF and Raman spectroscopies confirmed that SO 3 content decreased with increasing Sb2O3 content. TGA analysis showed, as a linear function of Sb2O3 content, mass gain commencing at 700°C, reaching a maximum at 1175°C, then mass loss above 1175°C, consistent with oxidation (Sb3+ → Sb5+) then reduction (Sb5+ → Sb3+). The TGA samples were shown to have attained or approached Sb redox equilibrium during measurement. Optical absorption spectroscopy (UV-Vis-nIR) showed red-shifts of the UV absorption edge with increasing Sb 2O 3 content, consistent with increasing intensity of far-UV absorption bands from Sb3+ and Sb5+ s→p transitions. UV-Vis-nIR fluorescence spectroscopy evidenced a broad luminescence band centred at ~25,000 cm−1, attributed to the 3P 1→ 1S 0 transition of Sb 3+, which is Stokes shifted by ~15,000 cm −1 from the 1S0→ 3P1 absorption at ~40,000 cm−1. The most intense emission occurred at 0.5 mol% Sb 2O3, with concentration quenching reducing luminescence intensities at higher Sb 2O3 contents. Additions of Sb2O3 to float-type soda-lime-silica glasses could thus enable lower melting energies and/or new solar energy applications.

AB - Float glass-type SiO 2-Na 2O-CaO glasses with 0 – 10 mol% Sb2O3 were melted and their compositional, structural, thermal and optical properties characterised. All glasses were X-ray amorphous and increasing Sb2O3 content progressively decreased glass transition temperature (Tg) and dilatometric softening point (T d), despite increases in Al2O3 content from greater crucible corrosion. 121Sb Mössbauer spectroscopy confirmed that Sb was predominantly incorporated as Sb 3+ (Sb 3+/ΣSb ~ 0.9) and Raman spectroscopy showed that Sb substantially decreased average (Si, Al)-O Qn speciation. Both techniques confirmed that Sb3+ ions were incorporated in trigonal pyramidal [:SbO 3] polyhedra. XRF and Raman spectroscopies confirmed that SO 3 content decreased with increasing Sb2O3 content. TGA analysis showed, as a linear function of Sb2O3 content, mass gain commencing at 700°C, reaching a maximum at 1175°C, then mass loss above 1175°C, consistent with oxidation (Sb3+ → Sb5+) then reduction (Sb5+ → Sb3+). The TGA samples were shown to have attained or approached Sb redox equilibrium during measurement. Optical absorption spectroscopy (UV-Vis-nIR) showed red-shifts of the UV absorption edge with increasing Sb 2O 3 content, consistent with increasing intensity of far-UV absorption bands from Sb3+ and Sb5+ s→p transitions. UV-Vis-nIR fluorescence spectroscopy evidenced a broad luminescence band centred at ~25,000 cm−1, attributed to the 3P 1→ 1S 0 transition of Sb 3+, which is Stokes shifted by ~15,000 cm −1 from the 1S0→ 3P1 absorption at ~40,000 cm−1. The most intense emission occurred at 0.5 mol% Sb 2O3, with concentration quenching reducing luminescence intensities at higher Sb 2O3 contents. Additions of Sb2O3 to float-type soda-lime-silica glasses could thus enable lower melting energies and/or new solar energy applications.

KW - antimony

KW - glass

KW - Mossbauer

KW - Raman

KW - soda-lime-silica

KW - Absorption spectroscopy

KW - Alumina

KW - Aluminum corrosion

KW - Aluminum metallography

KW - Aluminum oxide

KW - Amorphous silicon

KW - Antimony compounds

KW - Calcium oxide

KW - Fluorescence spectroscopy

KW - Glass

KW - Glass transition

KW - Light absorption

KW - Lime

KW - Luminescence

KW - Raman spectroscopy

KW - Red Shift

KW - Silica

KW - Silicon

KW - Sodium compounds

KW - Solar energy

KW - Composition structure

KW - Concentration quenching

KW - Dilatometric softening

KW - Luminescence band

KW - Luminescence intensity

KW - Soda-lime silica glass

KW - Solar energy applications

KW - Ssbauer spectroscopies

KW - Antimony

U2 - 10.1016/j.jnoncrysol.2020.120184

DO - 10.1016/j.jnoncrysol.2020.120184

M3 - Journal article

VL - 544

JO - Journal of Non-Crystalline Solids

JF - Journal of Non-Crystalline Solids

SN - 0022-3093

M1 - 120184

ER -