Quantum chemical study on the influence of structural features of aminosilanes on the interfacial chemical interactions with zirconia

doi:10.19439/j.sjos.2026.05.003

Abstract

Abstract: PURPOSE: To study the influence of the structure characteristics of amino silanes (number, position and chain length of CH₂ groups) on the chemical interactions between silane and zirconia by quantum chemistry, further improving the binding efficiency between silane and zirconia. METHODS: Models of four amino silanes-such as 3-aminopropyl triethoxysilane (APTES), 3-aminopropyl dimethylethoxysilane (APDMES), (2-aminoethyl)-3-aminopropyl trimethoxysilane (AEAPTMS) and divinyltriaminopropyl trimethoxysilane (DETA)-along with their corresponding silanol derivatives, tetragonal and monoclinic Zr₄O₈ clusters (t/m-Zr₄O₈) and silanol-decorated tetragonal/monoclinic ZrO₂ complexes (silanol-t/m-ZrO₂), were constructed to analyze the chemical interaction between zirconia and amino silanes with different molecular structures using thermodynamic calculations. The reaction sites were further predicted by orbital-weighted dual descriptor (DD). RESULTS: Changes in Gibbs free energy (ΔG) values of total chemical reactions between AEAPTMS and t-ZrO₂ was -397.337 kJ/mol, which was lower than the other three silanes, indicating that AEAPTMS had the strongest spontaneous reaction tendencies with t-ZrO₂. Even if zirconia underwent low temperature degradation (LTD), AEAPTMS could still spontaneously react with m-Zr₄O₈ to form Zr-O-Si bonds. The blue isosurfaces around the primary and secondary amine groups of AEAPTMS suggested that DD here was negative with highly nucleophilic, which could easily be attacked by electrophilic reagents, resulting in electrophilic reactions and exhibiting characteristics of local Lewis bases, further covalently binding to biomolecules or coatings. CONCLUSIONS: AEAPTMS has strong chemical affinity with zirconia before and after aging, which is expected to construct a strong and stable active surface for zirconia which is not affected by LTD to further graft bioactive molecules.

Key words: Silane, Zirconia, Quantum chemistry, Low temperature degradation

CLC Number:

R783.1

Bai Zehua, Lu Xiaofeng, Yang Yusheng, Liang Yun. Quantum chemical study on the influence of structural features of aminosilanes on the interfacial chemical interactions with zirconia[J]. Shanghai Journal of Stomatology, 2026, 35(5): 464-469.

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