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Revisiting the hydroxylation phenomenon of SiO2: a study through “hard-hard” and “soft–soft” interactions

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Abstract

Surface hydroxylation has been extensively studied over the years for a variety of applications, and studies involving hydroxylation of different silica surfaces are still carried out due to the interesting properties obtained from those modified surfaces. Although a number of theoretical studies have been employed to evaluate details on the hydroxylation phenomenon on silica (SiO2) surfaces, most of these studies are based on computationally expensive models commonly based on extended systems. In order to circumvent such an aspect, here we present a low-cost theoretical study on the SiO2 hydroxylation process aiming to evaluate aspects associated with water-SiO2 interaction. Details about local reactivity, chemical softness, and electrostatic potential were evaluated for SiO2 model substrates in the framework of the density functional theory (DFT) using a molecular approach. The obtained results from this new and promising approach were validated and complemented by fully atomistic reactive molecular dynamics (FARMD) simulations. Furthermore, the implemented approach proves to be a powerful tool that is not restricted to the study of hydroxylation, opening a promising route for low computational cost to analyze passivation and anchoring processes on a variety of oxide surfaces.

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Data availability

The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request.

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Funding

This work as supported by the Brazilian National Council for Scientific and Technological Development (CNPq) (grant numbers 448310/2014–7 and 420449/2018–3), the São Paulo Research Foundation (FAPESP) (grant number 2019/09431–0), and the CEPID (grant number 2013/07296–2). This research was also supported by resources supplied by the Center for Scientific Computing (NCC/Grid-UNESP) of São Paulo State University (UNESP).

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Authors and Affiliations

  1. School of Sciences, São Paulo State University (UNESP), POSMAT, Bauru, SP, 17033-360, Brazil

    Orisson P. Gomes, Leonardo F. G. Dias, Augusto Batagin-Neto & Paulo N. Lisboa-Filho

  2. São Paulo State University (UNESP), Campus of Itapeva, Itapeva, SP, 18409-010, Brazil

    Augusto Batagin-Neto

  3. Department of Physics, School of Sciences, São Paulo State University (UNESP), Bauru, SP, 17033-360, Brazil

    João P. C. Rheinheimer & Paulo N. Lisboa-Filho

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  1. Orisson P. Gomes
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  2. João P. C. Rheinheimer
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  3. Leonardo F. G. Dias
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  4. Augusto Batagin-Neto
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  5. Paulo N. Lisboa-Filho
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Contributions

The conception and design of the study were made by Orisson P. Gomes, Augusto Batagin-Neto, and Paulo N. Lisboa-Filho. Material preparation, data collection and analysis were performed by Orisson P. Gomes, João P. C. Rheinheimer, and Leonardo F. G. Dias. The first draft of the manuscript was written by Orisson P. Gomes and all authors commented and revised it critically for important intellectual content on previous versions of the manuscript. All authors read and approved the final manuscript.

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Correspondence to Orisson P. Gomes.

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Gomes, O.P., Rheinheimer, J.P.C., Dias, L.F.G. et al. Revisiting the hydroxylation phenomenon of SiO2: a study through “hard-hard” and “soft–soft” interactions. J Mol Model 28, 115 (2022). https://doi.org/10.1007/s00894-022-05107-w

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