Simulation of Calcium Phosphate Prenucleation Clusters in Aqueous Solution: Association beyond Ion Pairing

Garcia, Natalya A.; Malini, Riccardo Innocenti; Freeman, Colin L.; Demichelis, Raffaella; Raiteri, Paolo; Sommerdijk, Nico A. J. M.; Harding, John H.; Gale, Julian D.

doi:10.1021/acs.cgd.9b00889

Cited by 52 publications

(39 citation statements)

References 50 publications

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“…We have equilibrated for an additional 150 ns using metadynamics and used the time interval 150–450 ns as a production run for collecting data. A similar approach has been successfully used to simulate ion adsorption on phospholipid membranes [ 66 ] and the formation of calcium phosphate prenucleation clusters [ 67 ].…”

Section: Models and Methodsmentioning

confidence: 99%

Effects of Amino Acid Side-Chain Length and Chemical Structure on Anionic Polyglutamic and Polyaspartic Acid Cellulose-Based Polyelectrolyte Brushes

et al. 2021

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We used atomistic molecular dynamics (MD) simulations to study polyelectrolyte brushes based on anionic α,L-glutamic acid and α,L-aspartic acid grafted on cellulose in the presence of divalent CaCl2 salt at different concentrations. The motivation is to search for ways to control properties such as sorption capacity and the structural response of the brush to multivalent salts. For this detailed understanding of the role of side-chain length, the chemical structure and their interplay are required. It was found that in the case of glutamic acid oligomers, the longer side chains facilitate attractive interactions with the cellulose surface, which forces the grafted chains to lie down on the surface. The additional methylene group in the side chain enables side-chain rotation, enhancing this effect. On the other hand, the shorter and more restricted side chains of aspartic acid oligomers prevent attractive interactions to a large degree and push the grafted chains away from the surface. The difference in side-chain length also leads to differences in other properties of the brush in divalent salt solutions. At a low grafting density, the longer side chains of glutamic acid allow the adsorbed cations to be spatially distributed inside the brush resulting in a charge inversion. With an increase in grafting density, the difference in the total charge of the aspartic and glutamine brushes disappears, but new structural features appear. The longer sides allow for ion bridging between the grafted chains and the cellulose surface without a significant change in main-chain conformation. This leads to the brush structure being less sensitive to changes in salt concentration.

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Section: Models and Methodsmentioning

confidence: 99%

Effects of Amino Acid Side-Chain Length and Chemical Structure on Anionic Polyglutamic and Polyaspartic Acid Cellulose-Based Polyelectrolyte Brushes

et al. 2021

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“…They proposed that during the PILP process, the charged polymer acted as a processing-directing agent, with the aid of which the conventional solution crystallization process was converted into an amorphous liquid precursor-like process [ 44 ]. Using the formation of calcium carbonate and CaP based on PILP as examples, the dynamic compositional evolution and interactions between the polymer and the amorphous precursor have been revealed recently with the aid of advanced analytical techniques, such as cryogenic transmission electron microscopy (cryo-TEM), in situ atomic force microscopy (AFM), nuclear magnetic resonance (NMR), and modeling simulations [ 45 , 46 , 47 , 48 ]. A comprehensive understanding of PILP theory along with its applications for bone regeneration has been reported recently [ 49 ].…”

Section: Intrafibrillar Mineralization Mechanismsmentioning

confidence: 99%

Biomineralization of Collagen-Based Materials for Hard Tissue Repair

Wei

2021

IJMS

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Hydroxyapatite (HA) reinforced collagen fibrils serve as the basic building blocks of natural bone and dentin. Mineralization of collagen fibrils play an essential role in ensuring the structural and mechanical functionalities of hard tissues such as bone and dentin. Biomineralization of collagen can be divided into intrafibrillar and extrafibrillar mineralization in terms of HA distribution relative to collagen fibrils. Intrafibrillar mineralization is termed when HA minerals are incorporated within the gap zone of collagen fibrils, while extrafibrillar mineralization refers to the minerals that are formed on the surface of collagen fibrils. However, the mechanisms resulting in these two types of mineralization still remain debatable. In this review, the evolution of both classical and non-classical biomineralization theories is summarized. Different intrafibrillar mineralization mechanisms, including polymer induced liquid precursor (PILP), capillary action, electrostatic attraction, size exclusion, Gibbs-Donnan equilibrium, and interfacial energy guided theories, are discussed. Exemplary strategies to induce biomimetic intrafibrillar mineralization using non-collagenous proteins (NCPs), polymer analogs, small molecules, and fluidic shear stress are discussed, and recent applications of mineralized collagen fibers for bone regeneration and dentin repair are included. Finally, conclusions are drawn on these proposed mechanisms, and the future trend of collagen-based materials for bone regeneration and tooth repair is speculated.

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“…We have equilibrated for an additional 150 ns using metadynamics and used the time interval 150-450 ns as a production run for collecting data. Similar approach has been successfully used to simulate ion adsorption on phospholipid membranes [66] and the formation of calcium phosphate prenucleation clusters [67].…”

Section: Metadynamics Simulation Parametersmentioning

confidence: 99%

Effects of Amino Acid Side Chain Length and Chemical Structure on Anionic Polyglutamic and Polyaspartic Acid Cellulose-Based Polyelectrolyte Brushes

Tolmachev¹,

Mamistvalov²,

Lukasheva³

et al. 2021

Preprint

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We used atomistic molecular dynamics (MD) simulations to study polyelectrolyte brushes based on anionic α-L-glutamic acid and α-L-aspartic acid grafted on cellulose in the presence of divalent CaCl2 salt at different concentrations. The motivation is the search of the ways to control properties such as sorption capacity and the structural response of the brush to multivalent salts. For this detailed understanding of the role of side chain length, chemical structure and their interplay is required. It was found that in the case of glutamic acid oligomers, the longer side chains facilitate attractive interactions with the cellulose surface, which forces the grafted chains to lie down on the surface. The additional methylene group in the side chain enables side chain rotation enhancing this effect. On the other hand, the shorter and more restricted side chains of aspartic acid oligomers prevent attractive interactions to a large degree and push the grafted chains away from the surface. The difference in side chain length also leads to differences in other properties of the brush in divalent salt solutions. At a low grafting density, the longer side chains of glutamic acid allow the adsorbed cations to be spatially distributed inside the brush resulting in a charge inversion. With an increase in grafting density, the difference in the total charge of the aspartic and glutamine brushes disappears, but new structural features appear. The longer sides allow for ion bridging between the grafted chains and the cellulose surface without a significant change in main chain conformation. This leads to the brush structure being less sensitive to changes in salt concentration.

show abstract

Simulation of Calcium Phosphate Prenucleation Clusters in Aqueous Solution: Association beyond Ion Pairing

Cited by 52 publications

References 50 publications

Effects of Amino Acid Side-Chain Length and Chemical Structure on Anionic Polyglutamic and Polyaspartic Acid Cellulose-Based Polyelectrolyte Brushes

Effects of Amino Acid Side-Chain Length and Chemical Structure on Anionic Polyglutamic and Polyaspartic Acid Cellulose-Based Polyelectrolyte Brushes

Biomineralization of Collagen-Based Materials for Hard Tissue Repair

Effects of Amino Acid Side Chain Length and Chemical Structure on Anionic Polyglutamic and Polyaspartic Acid Cellulose-Based Polyelectrolyte Brushes

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