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Research Article | Open Access

Cristobalite-suppressed Al–SiO2 ceramic coatings: DFT-guided nanoparticle design for durable oxidation resistance

Hao-Jie Yan1,†, Xian-Ze Meng1,†, Jun-Bao Chong2, Hao Li1, Ruo-Zhan Yin1, Xiao-Feng Zhang3( ), Lian-Kui Wu1( )
School of Materials, Sun Yat-sen University, Shenzhen 518107, China
School of Materials Science and Engineering, Inner Mongolia University of Science & Technology, Baotou 014017, China
Guangdong Provincial Key Laboratory of Modern Surface Engineering Technology, Guangzhou 510651, China

† Hao-Jie Yan and Xian-Ze Meng contributed equally to this work.

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Graphical Abstract

Abstract

To address the critical challenge of crack propagation in electrodeposited SiO2 coatings caused by cristobalite phase transitions, Al nanoparticles were incorporated into SiO2 coatings for enhanced phase stability and durable temperature oxidation resistance. The incorporation of Al inhibits and optimizes the generation of cristobalite, which suppresses the formation of cracks, thereby reducing the parabolic oxidation rate constant ( kp) of the SiO2 coating by 32.4% after oxidation at 900 °C for 100 h. Density functional theory (DFT) calculations demonstrate that the introduced Al preferentially exists in a substitutional form, effectively stabilizing the K@SiO2 lattice structure by inhibiting K migration-induced cristobalite precipitation. Thermodynamically, the negative solution energy (−4.367 eV) of K@Six−1AlO2x confirms the spontaneous incorporation of substitutional Al into the K@SiO2 lattice. Structurally, substitutional Al forms a shorter Al‒K bond (2.91 Å) than does the Si‒K bond (3.39 Å), which can mitigate K-induced channel distortion and hinder the migration of K. Charge distribution analysis reveals that the Mulliken charges of Al (1.040) partially neutralize the Mulliken charges of K (−2.187), reducing electrostatic repulsion and promoting localized bonding. Furthermore, the incorporation of Al can restrain the precipitation of the brittle Z-phase, further contributing to improved oxidation performance.

Keywords

SiO2 coatinghigh-temperature oxidationmodificationcrackcristobalite

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Journal of Advanced Ceramics
Volume 14 Issue 6,
June 2025
Article number: 9221090
DOI: 10.26599/JAC.2025.9221090
Cite this article:
Yan H-J, Meng X-Z, Chong J-B, et al. Cristobalite-suppressed Al–SiO2 ceramic coatings: DFT-guided nanoparticle design for durable oxidation resistance. Journal of Advanced Ceramics, 2025, 14(6): 9221090. https://doi.org/10.26599/JAC.2025.9221090

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Received: 17 March 2025
Revised: 03 May 2025
Accepted: 12 May 2025
Published: 27 June 2025
© The Author(s) 2025.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, http://creativecommons.org/licenses/by/4.0/).
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