Enhancement on Properties of MgO-MgAlON Composite Refractories by Introducing Solid Waste Containing BN and AlN

Abstract

Driven by the goals of carbon peaking and carbon neutrality, the resource utilization of solid waste has attracted considerable attention due to its scientific importance and environmental benefits. For this purpose, MgO-MgAlON-BN refractories with enhanced thermal shock and slag resistance were designed and successfully fabricated by introducing BN solid waste as an additive. The results indicate that the sample containing BN additives exhibits superior overall performance compared with those without additives. At a BN content of 3.26 wt.%, the cold compressive strength increases by 21.20%, and the contact angle at 1723 K increases by 50.01%. Further analysis reveals that the improved wetting behavior is mainly attributed to the introduction of BN additives, which promote the formation of numerous micro-convex structures. These structural characteristics restrict slag infiltration and inhibit slag penetration into the refractory matrix, thereby enhancing slag resistance. Consequently, a cost-effective and feasible reinforcement strategy for MgO-MgAlON-BN refractories is proposed, providing a promising pathway for the high-value utilization of solid waste resources.

Keywords

MgO-MgAlON-BN composite refractories / Solid waste / Apparent porosity / Strength / Slag resistance

Author Contributions

Methodology, Z.Z. and L.W.; Formal Analysis, L.W., C.S., H.Y., C.H., Y.W., S.S., X.R., G.L., C.Z., Y.L., C.D. and C.Y.; Data Curation, Z.Z.; Writing-Original Draft Preparation, Z.Z.; Writing-Review & Editing, B.M.; Supervision, C.L.; Funding Acquisition, B.M. and C.Y.

Ethics Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

All data supporting this study are included in the article.

Funding

This research was funded by the Open Project Program of State Key Laboratory of Advanced Refractories (Grant No. SKLAR26007ZW) and the National Natural Science Foundation of China (Grant No. U20A20239).

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

References

[1] Yu C, Dong B, Chen YF, Ma BY, Ding J, Deng CJ, et al. Enhanced oxidation resistance of low-carbon MgO-C refractories with ternary carbides: A review. J. Iron Steel Res. Int. 2022, 29, 1052-1062. DOI: 10.1007/s42243-022-00804-5

[2] Fan ST, Deng CJ, Yu C, Liu ZL, Ding J. Nano-laminated BN modified graphite reinforced unfired MgO-C refractories: Preparation, properties and strengthening mechanism. J. Mater. Res. Technol. 2024, 29, 4833-4844. DOI: 10.1016/j.jmrt.2024.02.201

[3] Luo YX, Liu ZL, Yu C, Deng CJ, Ding J. Enhanced service performances of in-situ Mg-Sialon/MgAl₂O₄ folding structure in low carbon Al₂O₃-C refractories: Phase reconfiguration of nano-MgSiN₂. J. Eur. Ceram. Soc. 2024, 44, 7953-7968. DOI: 10.1016/j.jeurceramsoc.2024.05.066

[4] Chong XC, Li KD, Xiao GQ, Ding DH, Hou X. Effect of C/MgO nanocomposite powders on the properties of low-carbon MgO-C refractories. Ceram. Int. 2023, 49, 34316-34326. DOI: 10.1016/j.ceramint.2023.08.152

[5] Ren XM, Ma BY, Sun SL, Wang ZH, Ji W, Hou SY, et al. Self-reinforced and eco-friendly porous MgO-based ceramics from magnesite tailings: The effect of La₂O₃ and firing temperature. Ceram. Int. 2024, 50, 12992-13002. DOI: 10.1016/j.ceramint.2024.01.209

[6] Feng CZ, Xiao GQ, Ding DH, Lei CK, Lv LH, Chong XC, et al. Enhanced thermal shock resistance of low-carbon Al₂O₃- C refractories via CNTs/MgAl₂O₄ whiskers composite reinforcement. J. Am. Ceram. Soc. 2024, 107, 3881-3894. DOI: 10.1111/jace.19673

[7] Luo YX, Wang X, Liu ZL, Yu C, Deng CJ, Ding J. Enhanced oxidation resistance and thermal shock resistance of low- carbon Al₂O₃-C refractories with nano-BN: A synergistic of mullitization behavior. J. Alloys Compd. 2024, 975, 172937. DOI: 10.1016/j.jallcom.2023.172937

[8] Zhang RS, Wang H, Tian M, Wang YZ, Liu MY, Wang HM, et al. Pressureless reaction sintering and hot isostatic pressing of transparent MgAlON ceramic with high strength. Ceram. Int. 2018, 44, 17383-17390. DOI: 10.1016/j.ceramint.2018.06.203

[9] Cheng X, Liu L, Xiao LH, Huo XT, Guo M, Zhang M. Effect of MgO on corrosion mechanism under LF refining slag for MgAlON-MgO composites synthesized from spent MgO-C brick: Wetting behaviour, reaction process and infiltration mechanism. J. Alloys Compd. 2023, 963, 171278. DOI: 10.1016/j.jallcom.2023.171278

[10] Wang LL, Zhou ZY, Zan WY, Liu CM, Fu GF, Ma BY, Green synthesis of MgAlON refractories with high strength and excellent slag corrosion resistance. Ceram. Int. 2023, 49, 37594-37603. DOI: 10.1016/j.ceramint.2023.09.086

[11] Wang LL, Zhou ZY, Liu CM, Yu C, Deng CJ, Ying ZW, et al. Enhancing the comprehensive performance of MgO-MgAlON composite refractories synthesized from natural minerals. Ceram. Int. 2024, 50, 30068-30077. DOI: 10.1016/j.ceramint.2024.05.305

[12] Ma BY, Wang YZ, Zhang W, Chen QY, Pressureless sintering and fabrication of highly transparent MgAlON ceramic from the carbothermal powder. J. Alloys Compd. 2018, 745, 617-623. DOI: 10.1016/j.jallcom.2018.02.254

[13] Liu JH, Lv XJ, Li J, Liu YX, Synthesis of molten-electrolyte corrosion resistant MgAl₂O₄-MgAlON sidewall materials by pressureless sintering. J. Alloys Compd. 2016, 687, 623-629. DOI: 10.1016/j.jallcom.2016.06.178

[14] Chen WB, Wang B, Liu LL, Wang H, WangXD. Preparation and slag erosion resistance mechanism of MgAlON based composite refractories synthesized from solid waste. Ceram. Int. 2020, 46, 26035-26043. DOI: 10.1016/j.ceramint.2020.07.096

[15] Zhou J, Li YJ, Duan XH, Chen J, Jin ED, Ding DH, et al. Effects of h-BN on the thermal shock and oxidation resistance of SiO₂-bonded SiC refractories. Int. J. Appl. Ceram. Technol. 2024, 21, 3526-3537. DOI: 10.1111/ijac.14764

[16] Zhang ZT, Teng LD, Li WC. Mechanical properties and microstructures of hot-pressed MgAlON-BN composites. J. Eur. Ceram. Soc. 2007, 27, 319-326. DOI: 10.1016/j.jeurceramsoc.2006.04.184

[17] Lin H, Feng GQ, Wang HY, Peng HY, Cao LL, Lin HX, et al. Effect of BN addition on mechanical and electrical properties of oxidative sintered porous Si₃N₄-BN composites. Ceram. Int. 2023, 49, 36637-36645. DOI: 10.1016/j.ceramint.2023.08.347

[18] Li Q, Yang ZH, Zhong J, Sun YS, Jia DC, Duan XM, et al. Effect of the starting AlN content on the phase formation and property of the novel in-situ fabricated X-SiAlON/BN composites. J. Eur. Ceram. Soc. 2019, 39, 934-943. DOI: 10.1016/j.jeurceramsoc.2018.12.035

[19] Li M, Zhang LG, Zhang C, Xu EX, Liu XH, Zhao F, et al. Effect of Y₂O₃ on the physical properties and biocompatibility of β-SiAlON ceramics. Ceram. Int. 2020, 46, 23427-23432. DOI: 10.1016/j.ceramint.2020.06.112

[20] Abreal A, Goeuriot D, Thevenot F, Lagace M, Gueroult B, Rigaud M. Effect of Y₂O₃ addition on alumina-hex boron nitride composites. J. Eur. Ceram. Soc. 1995, 15, 841-849. DOI: 10.1016/0955-2219(95)00056-Z

[21] Podonak MK, Paydar MH, Forghani M, Guo J. B₂O₃ as an effective additive for cold sintering of MgTiO₃. J. Eur. Ceram. Soc. 2024, 44, 261-269. DOI: 10.1016/j.jeurceramsoc.2023.08.038

[22] Qian F, Li HL, Yang WG, Guo HR, Liu GQ, Li HX, et al. Corrosion resistance of BN-ZrO₂ ceramics with different additives by molten steel. J. Iron Steel Res. Int. 2022, 29, 1101-1109. DOI: 10.1007/s42243-021-00696-x

[23] Li YL, Qiao GJ, Jin ZH. Machinable Al₂O₃/BN composite ceramics with strong mechanical properties. Mater. Res. Bull. 2002, 37, 1401-1409. DOI: 10.1016/S0025-5408(02)00786-9

[24] Cao RQ, Sun SL, Wang WH, Zan WY, Yuan XZ, Zhou ZY, et al. Preparation and performance optimization of MgO- SiAlON-SiC ceramics using silicon kerf waste. Ceram. Int. 2025, 51, 39337-39344. DOI: 10.1016/j.ceramint.2025.06.171

[25] Ren XM, Ma BY, Tian JH, Jiang ZH. The effects of pre-sintering temperature and La₂O₃ addition on sinterability and corrosion resistance of stoichiometric magnesium aluminate spinel. Ceram. Int. 2022, 48, 32470-32478. DOI: 10.1016/j.ceramint.2022.07.193

[26] Wang LL, Ma BY, Ren XM, Yu C, Tian JH, Liu CM, et al. Phase-engineering strategy of ZrO₂ for enhancing the mechanical properties of porous cordierite ceramics. Mater. Today Commun. 2022, 30, 103032. DOI: 10.1016/j.mtcomm.2021.103032

[27] Xu YH, Ji ZX, Yang ZY, Yang JS, Li R, Fu ZD, et al. Densification and comprehensive properties of h-BN-based refractories with in-situ formation of Y₃Al₅O₁₂. J. Alloys Compd. 2021, 875, 160018. DOI: 10.1016/j.jallcom.2021.160018

[28] Sun Y, Chen YS, Tian L, Li GH, Formation mechanism of MgAlON phase in aluminum-magnesia composite materials. Mater. Chem. Phys. 2017, 197, 65-69. DOI: 10.1016/j.matchemphys.2017.05.008

[29] Zhai FR, Li S, Sun JL, Yi ZZ. Microstructure, mechanical properties and thermal shock behavior of h-BN-SiC ceramic composites prepared by spark plasma sintering. Ceram. Int. 2017, 43, 2413-2417. DOI: 10.1016/j.ceramint.2016.11.030

[30] Ma BY, Tang YD, Deng CJ. Effects of Al₂O₃-Y₂O₃/Yb₂O₃ additives on microstructures and mechanical properties of silicon nitride ceramics prepared by hot-pressing sintering. Int. J. Appl. Ceram. Technol. 2022, 19, 2523-2532. DOI: 10.1111/ijac.14081

[31] Ren XM, Ma BY, Tang JH, Li YW, Yu JK. Fabrication of energy-saving MgO with large grain size and low thermal conductivity: Towards a new type of magnesia for high-temperature furnaces. Constr. Build. Mater. 2022, 342, 128097. DOI: 10.1016/j.conbuildmat.2022.128097

[32] Shi JL, Deguchi Y, Sakabe Y. Relation between grain growth, densification and surface diffusion in solid state sintering- A direct observation. J. Mater. Sci. 2005, 40, 5711-5719. DOI: 10.1007/s10853-005-1474-7

[33] Ren XM, Ma BY, Liu H, Wang ZF, Deng CJ, Liu GQ, et al. Designing low-carbon MgO-Al₂O₃-La₂O₃-C refractories with balanced performance for ladle furnaces. J. Eur. Ceram. Soc. 2022, 42, 3986-3995. DOI: 10.1016/j.jeurceramsoc.2022.03.051

[34] Zhang ZT, Seetharaman S, Li WC. Thermal diffusivity/conductivity of MgAlON-BN composites. Metall. Mater. Trans. B 2006, 37, 615-621. DOI: 10.1007/s11663-006-0045-4

[35] Evans AG, Faber KT. Toughening of ceramics by circumferential microcracking. J. Am. Ceram. Soc. 1981, 64, 394-398. DOI: 10.1111/j.1151-2916.1981.tb09877.x

[36] Retajczyk TF, Sinha AK. Elastic stiffness and thermal expansion coefficient of BN films. Appl. Phys. Lett. 1980, 36, 161-163. DOI: 10.1063/1.91415

[37] Wang ZJ, Alaniz JE, Jang WY, Garay JE, Dames C. Thermal conductivity of nanocrystalline silicon: Importance of grain size and frequency-dependent mean free paths. Nano Lett. 2011, 11, 2206-2213. DOI: 10.1021/nl1045395

[38] Schramm A, Nowak R, Bruzda G, Polkowski W, Fabrichnaya O, Aneziris CG. High temperature wettability and corrosion of ZrO₂, Al₂O₃, Al₂O₃-C, MgO and MgAlON ceramic substrates by an AZ91 magnesium alloy melt. J. Eur. Ceram. Soc. 2022, 42, 3023-3035. DOI: 10.1016/j.jeurceramsoc.2022.01.040

[39] Liu JH, Sheng HY, Yang X, He ZJ, Hou XM. Research on the wetting and corrosion behavior between converter slag with different alkalinity and MgO-C refractories. Oxid. Met. 2022, 97, 157-166. DOI: 10.1007/s11085-021-10083-2