The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits

Erhan İbrahimoğlu

doi:10.16984/saufenbilder.1925009

The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits

Abstract

The environmental pollution created by waste glass frits generated in industrial production processes makes the conversion of these materials into secondary products important in terms of both sustainability and resource efficiency. In this context, the recycling of waste glasses not only reduces the need for disposal but also offers an alternative way to access high value-added engineering materials. Waste glass frits that generated in enamel applications can be used as the alternative materials. Therefore, in this study, the waste glass frit with SiO2-ZrO2-B2O3-Na2O-ZnO-CaO-Al2O3-K2O-Fe2O3 oxide components generated in enamel applications was transformed into an adaptable composite for advanced applications. For this purpose, Si3N4 was added to the waste frit matrix at rates of 5%, 10%, 15%, and 20% wt., and the samples were shaped and sintered using powder metallurgy processes to obtain the final products. Microstructural (SEM–EDS), mechanical (hardness), and physical (density) characterizations were performed on the produced samples to determine Si3N4 effect on the structural properties. Additionally, the changes in optical absorbance and band gap were evaluated using UV-Vis spectroscopy. It was observed that increasing the Si3N4 content significantly transformed the microstructure by altering the reinforcement-matrix interface within the structure. The hardness and density results revealed that Si3N4 addition directly affected the mechanical behavior, while the changes in optical response showed that the matrix-reinforcement interaction also reshaped the optical performance. In the 15 wt.% Si3N4 sample exhibited improvement on density (2.57 g/cm3) and Vickers hardness (14 GPa), indicating enhanced mechanical consolidation. The same composition also showed a narrowing optical band gap (4.61 eV) compared to the other samples, confirming a clear modification of the electronic structure due to Si3N4 addition.

Keywords

References

Choudhary, and R. Mandolia, "Evaluating resistance of ceramic waste tile self-compacting concrete to sulphuric acid attack," Constr. Build. Mater., vol. 393, Aug. 2023, Art. no. 132042, doi: 10.1016/j.conbuildmat.2023.132042.
Y.-W. Lin, W.-T. Lin, B.-X. Zhang, and K.-L. Lin, "Recycling waste tiles and waste catalysts for high-strength eco-porous ceramics in building applications," Sustain. Chem. Pharm., vol. 42, Dec. 2024, Art. no. 101846, doi: 10.1016/j.scp.2024.101846.
P. Güzelgün Hangün, N. Derin Coşkun, and E. Keskin, "Low-temperature glass formation from industrial enamel frit production waste," Coatings, vol. 16, no. 2, Feb. 2026, Art. no. 159, doi: 10.3390/coatings16020159.
G. C. S.-D. Bó, M. D. Bó, and A. M. Bernardin, "Reuse of laminated glass waste in the manufacture of ceramic frits and glazes," Mater. Chem. Phys., vol. 257, Jan. 2021, Art. no. 123847, doi: 10.1016/j.matchemphys.2020.123847.
T. Komatsu, "Design and control of crystallization in oxide glasses," J. Non-Cryst. Solids, vol. 428, pp. 156–175, Nov. 2015, doi: 10.1016/j.jnoncrysol.2015.08.017.
L. R. Pinckney, "Glass ceramics," in Encyclopedia of Materials: Science and Technology, 2nd ed., K. H. J. Buschow, R. W. Cahn, M. C. Flemings, B. Ilschner, E. J. Kramer, and S. Mahajan, Eds. Oxford, U.K.: Elsevier, 2001, pp. 3535–3540, doi: 10.1016/B0-08-043152-6/00629-X.
G. Singh, M. Sharma, and R. Vaish, "Emerging trends in glass-ceramic photocatalysts," Chem. Eng. J., vol. 407, Mar. 2021, Art. no. 126971, doi: 10.1016/j.cej.2020.126971.
J. Deubener and W. Höland, “Editorial: nucleation and crystallization of glasses and glass-ceramics,” Front. Mater., vol. 4, May 2017, Art. no. 14, doi: 10.3389/fmats.2017.00014.

M. Romero, R. D. Rawlings, and J. Ma Rincón, “Crystal nucleation and growth in glasses from inorganic wastes from urban incineration,” J. Non-Cryst. Solids, vol. 271, no. 1–2, pp. 106–118, Jun. 2000, doi: 10.1016/S0022-3093(00)00082-X.
X. Liu, B. Li, and Y. Wu, "The pretreatment of non-ferrous metallurgical waste slag and its research progress in the preparation of glass-ceramics," J. Clean. Prod., vol. 404, Jun. 2023, Art. no. 136930, doi: 10.1016/j.jclepro.2023.136930.
L. Fu, H. Engqvist, and W. Xia, "Glass-ceramics in dentistry: a review," Materials, vol. 13, no. 5, Mar. 2020, Art. no. 1049, doi: 10.3390/ma13051049.
M. Kırkbınar, E. İbrahimoğlu, S. H. Yetgin, and F. Çalışkan, "Investigation on tribological behaviour of poly(methyl methacrylate) biocomposite containing hydroxyapatite," Emerg. Mater. Res., vol. 13, no. 1, pp. 15–28, 2023, doi: 10.1680/jemmr.23.00039.
J. S. Alzahrani et al., "Influence of Fe2O3 on synthesis, structure, hardness, and radiation shielding properties of apatite–wollastonite glass ceramics for bone implantation and shielding applications," Ceram. Int., vol. 50, no. 18, pp. 32884–32892, Sep. 2024, doi: 10.1016/j.ceramint.2024.06.099.
W. Zou, W. Zhang, Y. Pi, Y. Zhang, Y. Chen, and L. Zhang, "Study on preparation of glass-ceramics from multiple solid waste and coupling mechanism of heavy metals," Ceram. Int., vol. 48, no. 24, pp. 36166–36177, Dec. 2022, doi: 10.1016/j.ceramint.2022.08.173.
Y. Zhang, T. Wu, C. Li, Y. Wang, Y. Geng, and G. Dong, "Numerical simulations of grinding force and surface morphology during precision grinding of leucite glass ceramics," Int. J. Mech. Sci., vol. 231, Oct. 2022, Art. no. 107562, doi: 10.1016/j.ijmecsci.2022.107562.
A. M. Abdel-Aziz, M. S. Shams, E. M. Ahmed, Y. S. Rammah, and R. A. Elsad, "Fabrication, physical, FTIR, ultrasonic waves, and mechanical properties of quaternary B2O3–Bi2O3–NaF–ZrO2 glasses: Experimental study," Appl. Phys. A, vol. 128, Jul. 2022, Art. no. 585, doi: 10.1007/s00339-022-05732-5.
R. A. Rahimi, A. Ahmadi, S. Kakooei, and S. K. Sadrnezhaad, "Corrosion behavior of ZrO2–SiO2–Al2O3 refractories in lead silicate glass melts," J. Eur. Ceram. Soc., vol. 31, no. 5, pp. 715–721, May 2011, doi: 10.1016/j.jeurceramsoc.2010.11.022.
E. Apel, C. van’t Hoen, V. Rheinberger, and W. Höland, "Influence of ZrO2 on the crystallization and properties of lithium disilicate glass-ceramics derived from a multi-component system," J. Eur. Ceram. Soc., vol. 27, no. 2–3, pp. 1571–1577, Jan. 2007, doi: 10.1016/j.jeurceramsoc.2006.04.103.
Y. Nobuta et al., "Formation and photoluminescence of zirconia dendrites in borosilicate glass-ceramics," J. Ceram. Soc. Jpn., vol. 125, no. 4, pp. 343–347, Apr. 2017, doi: 10.2109/JCERSJ2.17001.
Y. Guo et al., "Effect of ZrO2 crystallization on ion exchange properties in aluminosilicate glass," J. Eur. Ceram. Soc., vol. 40, no. 5, pp. 2179–2184, May 2020, doi: 10.1016/j.jeurceramsoc.2020.01.001.
K. J. Hong, J. M. Kim, and H. S. Kim, "Microstructure and properties of CaO–ZrO2–SiO2 glass–ceramics prepared by sintering," J. Eur. Ceram. Soc., vol. 23, no. 13, pp. 2193–2202, Dec. 2003, doi: 10.1016/S0955-2219(03)00089-X.
Q. Liu, M. Qian, and Y. Huang, "Studies on the preparation of rare-earth-doped alkaline borosilicate glass and its optical properties," Next Mater., vol. 9, Oct. 2025, Art. no. 100969, doi: 10.1016/j.nxmate.2025.100969.
E. M. Abou Hussein and A. Sobhy, "Experimental investigation of new rare earth borosilicate glasses from municipal waste ash as high-dose radiation dosimeters," Ceram. Int., vol. 50, no. 13, part A, pp. 23012–23022, Jul. 2024, doi: 10.1016/j.ceramint.2024.04.023.
S. O. Adeleye et al., "A review of the physical, optical and photoluminescence properties of rare earth ions doped glasses," Trends Sci., vol. 21, no. 12, Dec. 2024, Art. no. 8759, doi: 10.48048/tis.2024.8759.
S. Poolprasroed et al., "Low-cost samarium-doped mixed alkali borosilicate glasses: structural, thermal, and optical characterization for luminescent applications in art and decoration," J. Alloys Compd., vol. 1043, Oct. 2025, Art. no. 184167, doi: 10.1016/j.jallcom.2025.184167.
M. Eltohamy, I. Youssof, M. S. Abdel Aal, and R. Seoudi, "Optical and fluorescence behavior of Er3+-doped low-melting lead borosilicate glass for laser applications," Curr. Appl. Phys., vol. 81, pp. 29–37, Jan. 2026, doi: 10.1016/j.cap.2025.11.002.
B. Li, S. Wang, and Y. Fang, "Effect of Cr2O3 addition on crystallization, microstructure and properties of Li2O–Al2O3–SiO2 glass ceramics," J. Alloys Compd., vol. 693, pp. 9–15, Feb. 2017, doi: 10.1016/j.jallcom.2016.09.043.
B. Li, Q. Long, and D. Duan, "Effects of ZrO2 on properties of BaO–Al2O3–B2O3–SiO2 composites for LTCC applications," J. Mater. Sci., Mater. Electron., vol. 27, pp. 2824–2829, Mar. 2016, doi: 10.1007/s10854-015-4096-7.
A. Quintas, D. Caurant, O. Majérus, P. Loiseau, T. Charpentier, and J.-L. Dussossoy, “ZrO2 addition in soda-lime aluminoborosilicate glasses containing rare earths: impact on the network structure,” J. Alloys Compd., vol. 714, pp. 47–62, Aug. 2017, doi: 10.1016/j.jallcom.2017.04.182.
M. Salah, E. S. Moustafa, and A. A. Showahy, "Structural and optical investigations of multi-component lead-borosilicate glasses containing PbO, BaO, and TiO2," Opt. Mater., vol. 164, Jul. 2025, Art. no. 116915, doi: 10.1016/j.optmat.2025.116915.
H. Singh et al., "Evaluating the role of Er3+ ion on the structural, optical and thermal properties of CaO–ZrO2–Y2O3–B2O3–SiO2 glasses," Ceram. Int., vol. 50, no. 20, part B, pp. 39898–39906, Oct. 2024, doi: 10.1016/j.ceramint.2024.07.370.
T. Walia and K. Singh, "Mixed alkaline earth modifiers effect on thermal, optical and structural properties of SrO-BaO-SiO2-B2O3-ZrO2 glass sealants," J. Non-Cryst. Solids, vol. 564, Jul. 2021, Art. no. 120812, doi: 10.1016/j.jnoncrysol.2021.120812.
E. Kocaman and F. Çalışkan, “Ultra-fine beta SiC nanowires isothermally converted from high activated silica by carbothermic reduction and carburization at low temperature,” Mater. Chem. Phys., vol. 256, Dec. 2020, Art. no. 123716, doi: 10.1016/j.matchemphys.2020.123716.
F. Çalışkan, E. Kocaman, and S. Cömert, “Synthesis of the in-situ Si3N4-SiC composite nano powders by carbothermal reduction,” Acta Phys. Pol. A, vol. 131, no. 3, pp. 601–604, Mar. 2017, doi: 10.12693/APhysPolA.131.601.
M. U. Sarki et al., "Structural, electronic and optical properties of α-Si3N4, β-Si3N4 and γ-Si3N4 using density functional theory," Next Res., vol. 1, no. 2, Dec. 2024, Art. no. 100048, doi: 10.1016/j.nexres.2024.100048.
A. Sayyadi-Shahraki, S. M. Rafiaei, S. Ghadami, and K. A. Nekouee, “Densification and mechanical properties of spark plasma sintered Si3N4/ZrO2 nano-composites,” J. Alloys Compd., vol. 776, pp. 798–806, Mar. 2019, doi: 10.1016/j.jallcom.2018.10.243.
C. Luo, N. Li, and T. Deng, “Enhancement of Si3N4 ceramics via evolution of grain interface between ZrO2 and Si3N4 under pressureless sintering,” J. Amer. Ceram. Soc., vol. 106, no. 11, pp. 7043–7056, Nov. 2023, doi: 10.1111/jace.19263.
L. Y. Beliaev, E. Shkondin, A. V. Lavrinenko, and O. Takayama, “Optical, structural and composition properties of silicon nitride films deposited by reactive radio-frequency sputtering, low pressure and plasma-enhanced chemical vapor deposition,” Thin Solid Films, vol. 763, Dec. 2022, Art. no. 139568, doi: 10.1016/j.tsf.2022.139568.
M. Kırkbınar, "Physical, chemical, mechanical and radiation shielding properties of ZrO2–B2O3–SiO2 based waste glass ceramics containing different Bi2O3 concentrations," Radiat. Phys. Chem., vol. 238, Jan. 2026, Art. no. 113176, doi: 10.1016/j.radphyschem.2025.113176.
E. İbrahimoğlu, “The structural and radiation attenuation potential of the recycled multi oxide-based waste glass ceramics depending on different SiC reinforcement ratios,” Ann. Nucl. Energy, vol. 235, Sep. 2026, Art. no. 112360, doi: 10.1016/j.anucene.2026.112360.
S. Wu et al., "Preparation of high hardness and high fracture toughness Si3N4 ceramics by combining in-situ nitriding and hot-press sintering," Vacuum, vol. 239, Sep. 2025, Art. no. 114402, doi: 10.1016/j.vacuum.2025.114402.
B. P. Shanmugavel, S. H. Senthil Kumar, C. N. Aruna, and M. V. Ramesh, "Development of TiCN-Co-Cr3C2-Si3N4-based cermets with improved hardness and toughness for cutting tool applications," Powder Metall., vol. 66, no. 5, pp. 571–581, Dec. 2023, doi: 10.1080/00325899.2023.2243115.
Y. Al-Hadeethi, M. S. Al-Buriahi, and M. I. Sayyed, "Bioactive glasses and the impact of Si3N4 doping on photon attenuation up to radiotherapy energies," Ceram. Int., vol. 46, no. 4, pp. 5306–5314, Mar. 2020, doi: 10.1016/j.ceramint.2019.10.281.
N. D. Thien et al., "Optical properties of SiO2 opal crystals decorated with silver nanoparticles," Opt. Mater. X, vol. 24, Dec. 2024, Art. no. 100362, doi: 10.1016/j.omx.2024.100362.
D. Singh et al., "Optical and structural properties of ZnO-PbO-B2O3 and ZnO–PbO–B2O3–SiO2 glasses," J. Phys.: Condens. Matter, vol. 20, no. 7, Feb. 2008, Art. no. 075228, doi: 10.1088/0953-8984/20/7/075228.
Z. Huang et al., "Electronic and optical properties of Y-doped Si3N4 by density functional theory," J. Alloys Compd., vol. 637, pp. 376–381, Jul. 2015, doi: 10.1016/j.jallcom.2015.02.213.
R. El-Mallawany, W. M. Abou-Taleb, M. A. Naeem, S. M. Kotb, M. E. Krar, and S. Talaat, "Impact of B2O3 on physical, optical characteristics and radiation attenuation factors of borotellurite glasses," J. Mater. Res. Technol., vol. 18, pp. 2531–2545, May 2022, doi: 10.1016/j.jmrt.2022.03.107.
A. B. Semerci, E. Ibrahimoğlu, M. Kirkbinar, Y. Suyun, T. Ongun Sevindik, and F. Çalişkan, “From nature to high-tech: boron-doped biosourced silica as a multifunctional material for advanced radiation shielding and optical applications,” Ann. Nucl. Energy, vol. 239, Dec. 2026, Art. no. 112604, doi: 10.1016/j.anucene.2026.112604.
J. S. Alzahrani et al., "Optical properties and photon-shielding performance of B2O3-based glasses," Optik, vol. 264, Aug. 2022, Art. no. 169343, doi: 10.1016/j.ijleo.2022.169343.
J. Zhu, S. Hu, W. Wang, W. Xia, H. Chen, and X. Chen, "Luminescent amorphous silicon carbide ultrafine nanoparticles fabricated by pulsed-laser ablation," Appl. Phys. A, vol. 123, no. 4, Apr. 2017, Art. no. 244, doi: 10.1007/s00339-017-0888-3.
G. L. Plautz, I. L. Graff, W. H. Schreiner, and A. G. Bezerra, "Evolution of size distribution, optical properties, and structure of Si nanoparticles obtained by laser-assisted fragmentation," Appl. Phys. A, vol. 123, no. 5, May 2017, Art. no. 359, doi: 10.1007/s00339-017-0961-y.
N. M. Ravindra and J. Narayan, "Optical properties of amorphous silicon and silicon dioxide," J. Appl. Phys., vol. 60, no. 3, pp. 1139–1146, Aug. 1986, doi: 10.1063/1.337358.
D. B. Borgekov et al., "The effect of oxygen vacancies on the optical and thermophysical properties of (1-x)Si3N4 – xAl2O3 ceramics," Opt. Mater., vol. 157, part 1, Nov. 2024, Art. no. 116056, doi: 10.1016/j.optmat.2024.116056.
Y. Liu et al., “Effects of particle size and color on photocuring performance of Si3N4 ceramic slurry by stereolithography,” J. Eur. Ceram. Soc., vol. 41, no. 4, pp. 2386–2394, Apr. 2021, doi: 10.1016/j.jeurceramsoc.2020.11.032.
R. Ding, S. Liu, W. Yi, and L. Wei, “Influence of particle agglomeration on the spectral characteristics of hematite and the underlying mechanisms,” Minerals, vol. 16, no. 2, Feb. 2026, Art. no. 190, doi: 10.3390/min16020190.
F. Liu, "The effect of alpha particle irradiation on the performance of α-Si3N4 antireflection film for solar cells," Radiat. Phys. Chem., vol. 237, Dec. 2025, Art. no. 112993, doi: 10.1016/j.radphyschem.2025.112993.
V. R. Kumar, K. K. Kumar, L. Vijayalakshmi, J. Lim, V. R. Kumar, and N. Veeraiah, "Optimized reddish-orange emission in Pr3+ doped Pb3O4-ZrO2-B2O3-SiO2 glasses for advanced photonic applications," J. Non-Cryst. Solids, vol. 673, Jan. 2026, Art. no. 123878, doi: 10.1016/j.jnoncrysol.2025.123878.

Details

Primary Language

English

Subjects

Material Production Technologies, Materials Engineering (Other)

Journal Section

Research Article

Authors

Erhan İbrahimoğlu ^*
0000-0002-8073-5570
Türkiye

Early Pub Date

October 27, 2026

Publication Date

October 30, 2026

Submission Date

April 7, 2026

Acceptance Date

July 21, 2026

Published in Issue

Year 2026 Volume: 30 Number: 5

DOI

https://doi.org/10.16984/saufenbilder.1925009

IZ

https://izlik.org/JA44JL49LP

Cite

RIS / Bibtex

APA

İbrahimoğlu, E. (2026). The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits. Sakarya University Journal of Science, 30(5), 679-695. https://doi.org/10.16984/saufenbilder.1925009

AMA

1.İbrahimoğlu E. The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits. SAUJS. 2026;30(5):679-695. doi:10.16984/saufenbilder.1925009

Chicago

İbrahimoğlu, Erhan. 2026. “The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits”. Sakarya University Journal of Science 30 (5): 679-95. https://doi.org/10.16984/saufenbilder.1925009.

EndNote

İbrahimoğlu E (October 1, 2026) The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits. Sakarya University Journal of Science 30 5 679–695.

IEEE

[1]E. İbrahimoğlu, “The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits”, SAUJS, vol. 30, no. 5, pp. 679–695, Oct. 2026, doi: 10.16984/saufenbilder.1925009.

ISNAD

İbrahimoğlu, Erhan. “The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits”. Sakarya University Journal of Science 30/5 (October 1, 2026): 679-695. https://doi.org/10.16984/saufenbilder.1925009.

JAMA

1.İbrahimoğlu E. The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits. SAUJS. 2026;30:679–695.

MLA

İbrahimoğlu, Erhan. “The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits”. Sakarya University Journal of Science, vol. 30, no. 5, Oct. 2026, pp. 679-95, doi:10.16984/saufenbilder.1925009.

Vancouver

1.Erhan İbrahimoğlu. The Effect of Si3N4 Reinforcement on Optical Band Gap and Absorption Behavior in Recycled Glass Frits. SAUJS. 2026 Oct. 1;30(5):679-95. doi:10.16984/saufenbilder.1925009