Modeling the Water−Bioglass Interface by Ab Initio Molecular Dynamics Simulations

Tilocca, Antonio; Cormack, Alastair N.

doi:10.1021/am900198t

Cited by 98 publications

(120 citation statements)

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“…The resulting OH − is initially associated to the Na cation, but the trajectory also shows that the OH − charge can be transported elsewhere in the liquid by a sequence of rapid proton transfers along water molecules (Tilocca & Cormack 2009). On the bioglass surface, the close association with a Lewis acid such as Na + appears thus necessary to convert an exposed NBO into a silanol group through water dissociation.…”

Section: Resultsmentioning

confidence: 99%

“…This computationally demanding ab initio approach, employing periodic supercells and finite-temperature molecular dynamics (MD), represents a suitable way to investigate the highly heterogeneous energy landscape of a multicomponent glass surface (Tilocca 2010a). In particular, the strength of selected surface sites can be probed by examining their interaction with an isolated water molecule (Tilocca & Cormack 2008), as well as with an extended film mimicking a bulk solvent (Tilocca & Cormack 2009). These recent simulations have highlighted the role of exposed Na cations in coordinating water and promoting solvent penetration in the earliest stages of the dissolution mechanism.…”

Section: Introductionmentioning

confidence: 99%

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The initial stages of bioglass dissolution: a Car–Parrinello molecular-dynamics study of the glass–water interface

Tilocca

Cormack

2011

Proc. R. Soc. A.

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The initial dissolution stages following implantation of a biomaterial in a physiological environment are critical for its bioactive properties. Car-Parrinello molecular-dynamics (CPMD) simulations of the interface between the 45S5 bioglass surface and liquid water have been carried out to investigate these processes. The analysis of a 40 ps CPMD trajectory has highlighted the potential mechanism of Na + /H + exchange, leading to formation of surface silanols through water dissociation. Moreover, by comparing the properties of water layers arranged at different distances from the glass surface, we discuss the way in which the particular structure and composition of the bioglass surface affects the hydrogen-bond network and orientation of water in its close proximity.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

The initial stages of bioglass dissolution: a Car–Parrinello molecular-dynamics study of the glass–water interface

Tilocca

Cormack

2011

Proc. R. Soc. A.

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“…The majority of this work has been performed by Tilocca and colleagues 39 who investigated the stability of multicomponent bioactive glasses in aqueous environments. Many of the lessons learned and best practices from the investigation of bioactive glasses can be extended, and will provide insight into the role of surfaces on the dissolution behaviors of complex nuclear waste glass compositions.…”

Section: First-principles-based Simulations Of Glass-water Interactionsmentioning

confidence: 99%

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Rimsza

2017

npj Mater Degrad

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Computer simulations at the atomistic scale play an increasing important role in understanding the structure features, and the structure-property relationships of glass and amorphous materials. In this paper, we reviewed atomistic simulation methods ranging from first principles calculations and ab initio molecular dynamics (AIMD) simulations, to classical molecular dynamics (MD), and meso-scale kinetic Monte Carlo (KMC) simulations and their applications to study the reactions and interactions of inorganic glasses with water and the dissolution behaviors of inorganic glasses. Particularly, the use of these simulation methods in understanding the reaction mechanisms of water with oxide glasses, water-glass interfaces, hydrated porous silica gels formation, the structure and properties of multicomponent glasses, and microstructure evolution are reviewed. The advantages and disadvantageous of these simulation methods are discussed and the current challenges and future direction of atomistic simulations in glass dissolution presented.npj Materials Degradation (2017) 1:16 ; doi:10.1038/s41529-017-0017-yThe corrosion or degradation of glasses in aqueous solutions are critical in a number of engineering and technological processes ranging from microelectronic packaging, glass reaction chambers, and the immobilization of nuclear waste materials, as well as in healthcare and biomedical fields such as dissolution of inhaled glass fibers and bioactive glasses for biomedical applications. In particular, immobilizing radioactive waste in borosilicate glasses is widely accepted as a preferred method to treat nuclear waste materials generated from civilian and military sources. This process, also known as vitrification, is a critical component of the cycle of nuclear energy to combat global environmental and energy challenges. Researchers from around the world have extensively invested in understanding glass corrosion in an effort to predict the long-term stability and release rate radionuclides to the environment during nuclear waste storage. 1,2Various mechanisms for glass corrosion have been proposed and despite intensive experimental investigations with advanced characterization techniques results are unclear. It is generally accepted that the corrosion of glass consists of a set of complex processes including hydration, hydrolysis, and ion-exchange that are coupled during glass dissolution. The initial stage is interdiffusion of proton or hydronium ions from the solution with sodium or other alkali ions in the glass.3 This is followed by the hydrophilic attack of water on the Si-O-Si or Si-O-Al linkages that lead to hydroxylation of the silicate glass network. The remaining hydrolyzed glass skeleton then undergoes condensation and repolymerization to form the hydrated nanoporous silica rich gel layer which can be protective, decreasing dissolution to a residual rate. [4][5][6] The morphology of the gel layer, such as thickness, pore structure, and chemical composition, depends on the original glass composition and the pH...

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“…closer to the solvent, (see concentrations in Table 2), as in other compositions. Previous studies have shown that Na + −water interactions are potential initiators of surface degradation 50 , whereas it is also known that a quick release of Na + will favour Na + /H + (solvent) exchange, leading to high alkalinity where the increasing amount of OH-induces the breaking of P−O−P bonds [49][50][51] . The surfaces with higher concentrations of sodium at the interface will thus dissolve more quickly.…”

Section: Discussionmentioning

confidence: 99%

“…Another study combined x-ray and neutron diffraction along with modelling, via a reverse Monte Carlo simulation, to probe the short-range structure of (P 2 O 5 ) 0.50 (CaO) 0. 50 22 .…”

Section: Development Of An Interatomic Force-mentioning

confidence: 99%

Structures and properties of phosphate-based bioactive glasses from computer simulation: a review

et al. 2017

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This is an Accepted Manuscript, which has been through the Royal Society of Chemistry peer review process and has been accepted for publication.Accepted Manuscripts are published online shortly after acceptance, before technical editing, formatting and proof reading. Using this free service, authors can make their results available to the community, in citable form, before we publish the edited article. We will replace this Accepted Manuscript with the edited and formatted Advance Article as soon as it is available.You can find more information about Accepted Manuscripts in the author guidelines.Please note that technical editing may introduce minor changes to the text and/or graphics, which may alter content. The journal's standard Terms & Conditions and the ethical guidelines, outlined in our author and reviewer resource centre, still apply. In no event shall the Royal Society of Chemistry be held responsible for any errors or omissions in this Accepted Manuscript or any consequences arising from the use of any information it contains. ture at the surface, and how this changes from that of the bulk.In the past few years, our groups and others have extensively used state-of-the-art highperformance computing methods, usually molecular dynamics (MD) simulations, to characterise the structure and properties of PBGs. In molecular dynamics, the individual atoms move due to the interatomic forces they experience from other atoms. Because the full three-dimensional structure of the material is available at all times, an MD trajectory contains a great deal of information from which the material's properties may be deduced. Our work has involved new methodological developments in the form of a new model of the phosphate interatomic forces 9 , and MD simulations have given new insight into the structural motifs which affect the dissolution which are not accessible to experimental methods 10 . Recently, the different properties of PBG at the surface of the glass, from where the dissolution takes place have been shown, which will also be important in unravelling the full connections between structure and dissolution 11 . Molecular dynamics methods for preparation of glassesA full review of molecular dynamics methods is beyond the scope of this paper; the reader is invited to turn to relevant books 12,13 . Broadly, there are two types of molecular dynamics used to prepare realistic glass models: classical and first-principles. In classical MD, the interatomic forces are represented by an empirical expression with a small number of parameters which are chosen to reproduce existing data on the material. This method has the advantage of being relatively easy to implement and computationally inexpensive, allowing for large models (typically ∼ 10 3 − 10 4 atoms) to be simulated over long timescales (typically ns). The disadvantage is that the accuracy of the simulation is limited by the accuracy of the approximations of the interatomic potential model. First-principles MD, by contrast, uses a quantum-mechanical expression for th...

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Modeling the Water−Bioglass Interface by Ab Initio Molecular Dynamics Simulations

Cited by 98 publications

References 66 publications

The initial stages of bioglass dissolution: a Car–Parrinello molecular-dynamics study of the glass–water interface

The initial stages of bioglass dissolution: a Car–Parrinello molecular-dynamics study of the glass–water interface

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Structures and properties of phosphate-based bioactive glasses from computer simulation: a review

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