The effect of water on the binding of glycosaminoglycan saccharides to hydroxyapatite surfaces: a molecular dynamics study

Ruiz‐Hernandez, Sergio E.; Streeter, Ian; Leeuw, Nora H. de

doi:10.1039/c5cp02630j

Cited by 29 publications

(38 citation statements)

References 63 publications

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“…In particular, the effect on the O-O structure is more pronounced in CaF 2 (aq), where for the 1.0 mol·kg −1 solution the second shell has collapsed into the first one (Figure 2c). A similar behavior in the interatomic distances of water was observed from MD Crystals 2017, 7, 57 6 of 17 simulations of NaCl and NaF aqueous solutions [45]. The stronger electrostatic field of F − compared with Cl − can be used to explain the more pronounced effect of fluorine ions on the structure of water.…”

Section: Analysis Of the Simulation Datasupporting

confidence: 54%

“…The water molecules were described using the simple point charge (SPC/E) model [42] because it gives a density, radial distribution functions, self-diffusion coefficient for water, and hydrogen-bond dynamics in good agreement with the experiment [42,43]. HAP-water interactions were described using non-bonded potentials derived in previous MD studies [44,45], which are compatible with the current HAP shell model. The interactions between Ca 2+ -X − and X − -X − pairs in solution (where X − designates Cl − or F − ), and between the ions in solution and the phosphate and hydroxyl groups of HAP were described using the Buckingham potentials developed by Rabone and de Leeuw for modeling natural apatite crystals [46].…”

Section: Interatomic Potential Modelmentioning

confidence: 96%

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Molecular Dynamics Simulations of Hydroxyapatite Nanopores in Contact with Electrolyte Solutions: The Effect of Nanoconfinement and Solvated Ions on the Surface Reactivity and the Structural, Dynamical, and Vibrational Properties of Water

et al. 2017

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Hydroxyapatite, the main mineral phase of mammalian tooth enamel and bone, grows within nanoconfined environments and in contact with aqueous solutions that are rich in ions. Hydroxyapatite nanopores of different pore sizes (20 Å ≤ H ≤ 110 Å, where H is the size of the nanopore) in contact with liquid water and aqueous electrolyte solutions (CaCl 2 (aq) and CaF 2 (aq)) were investigated using molecular dynamics simulations to quantify the effect of nanoconfinement and solvated ions on the surface reactivity and the structural and dynamical properties of water. The combined effect of solution composition and nanoconfinement significantly slows the self-diffusion coefficient of water molecules compared with bulk liquid. Analysis of the pair and angular distribution functions, distribution of hydrogen bonds, velocity autocorrelation functions, and power spectra of water shows that solution composition and nanoconfinement in particular enhance the rigidity of the water hydrogen bonding network. Calculation of the water exchange events in the coordination of calcium ions reveals that the dynamics of water molecules at the HAP-solution interface decreases substantially with the degree of confinement. Ions in solution also reduce the water dynamics at the surface calcium sites. Together, these changes in the properties of water impart an overall rigidifying effect on the solvent network and reduce the reactivity at the hydroxyapatite-solution interface. Since the process of surface-cation-dehydration governs the kinetics of the reactions occurring at mineral surfaces, such as adsorption and crystal growth, this work shows how nanoconfinement and solvation environment influence the molecular-level events surrounding the crystallization of hydroxyapatite.

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Section: Analysis Of the Simulation Datasupporting

confidence: 54%

Section: Interatomic Potential Modelmentioning

confidence: 96%

Molecular Dynamics Simulations of Hydroxyapatite Nanopores in Contact with Electrolyte Solutions: The Effect of Nanoconfinement and Solvated Ions on the Surface Reactivity and the Structural, Dynamical, and Vibrational Properties of Water

et al. 2017

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“…These substitutions HAP-based materials allowed the investigation of the interactions between HAP surfaces with biomolecules (Almora- Barrios et al 2009;Katti et al 2010;Kandori et al 2000a;Hernandez et al 2015;Lukasheva and Tolmachev 2015), water (Zhao et al 2014), ions (de Leeuw 2004a , b;Sakhno et al 2010 ), and gases (Chi-atti et al 2013). Water plays a crucial role during bone mineralization and in the protein interaction (Corno et al 2010;Qin et al 2012;Nair et al 2014;Lemaire et al 2015a) as they can act as a prominent charge carrier, transporting ions (Prakash et al 2009;Prakash and Subramanian 2011) and maintaining the pH of the medium.…”

Section: Introductionmentioning

confidence: 99%

Anisotropic diffusion of water molecules in hydroxyapatite nanopores

et al. 2017

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New insights into the dynamical properties of water in hydroxyapatite (HAP) nanopores, a model system for the fluid flow within nanosize spaces inside the collagen-apatite structure of bone, were obtained from molecular dynamics simulations of liquid water confined between two parallel HAP surfaces of different sizes (20 Å ≤ H ≤ 240 Å). Calculations were conducted using a coreshell interatomic potential for HAP together with the extended simple point charge model for water. This force field gives an activation energy for water diffusion within HAP nanopores that is in excellent agreement with available experimental data. The dynamical properties of water within the HAP nanopores were quantified in terms of the second-order water diffusion tensor. Results indicate that water diffuses anisotropically within the HAP nanopores, with the solvent molecules moving parallel to the surface twice as fast as the perpendicular direction. This unusual dynamic behaviour is linked to the strong polarizing effect of calcium ions, and the synergic interactions between the water molecules in the first hydration layer of HAP with the calcium, hydroxyl, and phosphate ions, which facilitates the flow of water molecules in the directions parallel to the HAP surface.

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“…, articular cartilage) (60–62) . GAGs are also found in the extrafibrillar matrix of bone (21,22) with strong affinity to extrafibrillar minerals (41,63–65) . Collagen-bound water is usually considered as a major source of organic-bound water in bone matrix since type I collagen comprises 90% of the organic matrix of the tissue and is highly hydrophilic (20) .…”

Section: Discussionmentioning

confidence: 99%

“…(60)(61)(62) GAGs are also found in the extrafibrillar matrix of bone (21,22) with strong affinity to extrafibrillar minerals. (41,(63)(64)(65) Collagen-bound water is usually considered as a major source of organic-bound water in bone matrix because type I collagen comprises 90% of the organic matrix of the tissue and is highly hydrophilic. (20) However, bound water retained in the extrafibrillar matrix by NCPs (10% of the organic phase), which are highly hydrophilic too, may also significantly affect the mechanical behavior of bone.…”

Section: Discussionmentioning

confidence: 99%

Age‐Related Deterioration of Bone Toughness Is Related to Diminishing Amount of Matrix Glycosaminoglycans (GAGs)

et al. 2018

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Hydration status significantly affects the toughness of bone. In addition to the collagen phase, recent evidence shows that glycosaminoglycans (GAGs) of proteoglycans (PGs) in the extracellular matrix also play a pivotal role in regulating the tissue-level hydration status of bone, thereby affecting the tissue-level toughness of bone. In this study, we hypothesized that the amount of GAGs in bone matrix decreased with age and such changes would lead to reduction in bound water and subsequently result in a decrease in the tissue-level toughness of bone. To test the hypothesis, nanoscratch tests were conducted to measure the tissue-level toughness of human cadaveric bone specimens, which were procured only from male donors in three different age groups: young (26 ± 6 years old), mid-aged (52 ± 5 years old) and elderly (73 ± 5 years old), with six donors in each group. Biochemical and histochemical assays were performed to determine the amount and major subtypes of GAGs and proteoglycans in bone matrix. In addition, low-field NMR measurements were implemented to determine bound water content in bone matrix. The results demonstrated that aging resulted in a statistically significant reduction (17%) of GAGs in bone matrix. Concurrently, a significant deterioration (20%) of tissue-level toughness of bone with age was observed. Most importantly, the deteriorated tissue-level toughness of bone was associated significantly with the age-related reduction (40%) of bound water, which was partially induced by the decrease of GAGs in bone matrix. Furthermore, we identified that chondroitin sulfate (CS) was a major subtype of GAGs and the amount of CS decreased with aging in accompany with a decrease of biglycan that is a major subtype of PGs in bone. The findings of this study suggests that reduction of GAGs in bone matrix is likely one of the molecular origins for age-related deterioration of bone quality.

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The effect of water on the binding of glycosaminoglycan saccharides to hydroxyapatite surfaces: a molecular dynamics study

Cited by 29 publications

References 63 publications

Molecular Dynamics Simulations of Hydroxyapatite Nanopores in Contact with Electrolyte Solutions: The Effect of Nanoconfinement and Solvated Ions on the Surface Reactivity and the Structural, Dynamical, and Vibrational Properties of Water

Molecular Dynamics Simulations of Hydroxyapatite Nanopores in Contact with Electrolyte Solutions: The Effect of Nanoconfinement and Solvated Ions on the Surface Reactivity and the Structural, Dynamical, and Vibrational Properties of Water

Anisotropic diffusion of water molecules in hydroxyapatite nanopores

Age‐Related Deterioration of Bone Toughness Is Related to Diminishing Amount of Matrix Glycosaminoglycans (GAGs)

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