Control of Biomineralization Dynamics by Interfacial Energies

Tang, Ruikang; Darragh, Molly R.; Orme, Christine A.; Guan, Xiangying; Hoyer, John R.; Nancollas, G.H.

doi:10.1002/anie.200500153

Cited by 81 publications

(128 citation statements)

References 22 publications

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“…Given this insight, the reduction in step density can be interpreted as an increase in step-edge free energy associated with citrate binding at the surface. Tang et al (2005) verified this result by using a thinlayer, wicking method to measure the surface energies of brushite powders in the absence and presence of citrate, finding that the interfacial energy increased from 4.5 mJ m −2 in pure solutions to 8.9 mJ m −2 at 10 mM citrate. A higher interfacial energy is also expected to increase the barrier to nucleation (equation (3.1)), leading to a longer induction time, which was also verified experimentally.…”

Section: Ii) the Impact Of Citrate On Brushite Growthmentioning

confidence: 72%

“…Both growth and dissolution data report that the [100] Cc step has the slowest kinetics (Scudiero et al 1999;Kanzaki et al 2002;Tang et al 2005). There are several features that make this step unique compared with the other two.…”

Section: (G) Step Anisotropymentioning

confidence: 99%

“…Constant composition experiments showed that citrate, C 3 H 5 O(COO) 3− 3 , inhibited the bulk growth rate of brushite seeds (Tang et al 2005). Concentrations of 2.1 and 10 mM citrate reduced the growth rate by 50 and 95 per cent, respectively.…”

Section: Ii) the Impact Of Citrate On Brushite Growthmentioning

confidence: 99%

“…In other words, the large surface area of this facet is due to low surface energy rather than to kinetic barriers associated with dehydration. And, in fact, brushite has a relatively low interfacial energy of 4.5 mJ m −2 (Tang et al 2005) compared with other biominerals such as 8 mJ m −2 for apatite on May 10, 2018 http://rsta.royalsocietypublishing.org/ Downloaded from for calcium oxalate monohydrate (COM; Wu & Nancollas 1999). Surface X-ray diffraction studies show that this water layer is crystalline, but not ice-like and does not impart order of water molecules into the solution as might be expected from ice (Arsic et al 2004).…”

Section: (A)mentioning

confidence: 99%

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Molecular mechanisms of crystallization impacting calcium phosphate cements

Giocondi

El-Dasher

Nancollas

et al. 2010

Phil. Trans. R. Soc. A.

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The biomineral calcium hydrogen phosphate dihydrate (CaHPO 4 ·2H 2 O), known as brushite, is a malleable material that both grows and dissolves faster than most other calcium minerals, including other calcium phosphate phases, calcium carbonates and calcium oxalates. Within the body, this ready formation and dissolution can play a role in certain diseases, such as kidney stone and plaque formation. However, these same properties, along with brushite's excellent biocompatibility, can be used to great benefit in making resorbable biomedical cements. To optimize cements, additives are commonly used to control crystallization kinetics and phase transformation. This paper describes the use of in situ scanning probe microscopy to investigate the role of several solution parameters and additives in brushite atomic step motion. Surprisingly, this work demonstrates that the activation barrier for phosphate (rather than calcium) incorporation limits growth kinetics and that additives such as magnesium, citrate and bisphosphonates each influence step motion in distinctly different ways. Our findings provide details of how, and where, molecules inhibit or accelerate kinetics. These insights have the potential to aid in designing molecules to target specific steps and to guide synergistic combinations of additives.

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Section: Ii) the Impact Of Citrate On Brushite Growthmentioning

confidence: 72%

Section: (G) Step Anisotropymentioning

confidence: 99%

Section: Ii) the Impact Of Citrate On Brushite Growthmentioning

confidence: 99%

Section: (A)mentioning

confidence: 99%

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Molecular mechanisms of crystallization impacting calcium phosphate cements

Giocondi

El-Dasher

Nancollas

et al. 2010

Phil. Trans. R. Soc. A.

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“…21 Nancollas et al demonstrated the general inhibitory effect of citrate on brushite growth as a function of the citric acid concentration. 22 Citric acid is commonly utilised to slow down the setting and hence increase the workability and handling of CPCs. It decreases the supersaturation of setting liquid due to its affinity to bind calcium ions.…”

Section: Introductionmentioning

confidence: 99%

Monetite promoting effect of citric acid on brushite cement setting kinetics

Şahin

Çiftçioğlu

2013

Materials Research Innovations

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Brushite forming calcium phosphate cements receive growing interest in hard tissue scaffold applications due to their high surface area and high bioresorbability. The finer microstructure of monetite, the dehydrated form of brushite, has attracted attention for bone tissue engineering applications. The reduction in brushite content of the b-tricalcium phosphate-monocalcium phosphate monohydrate cement system by selective inhibition of growth upon addition of citric acid to excess setting liquid was investigated. The relaxation period during cement setting was monitored by pH stat titration and free drift runs. Spectrometric analysis revealed that the change in solubility of calcium phosphates upon addition of citric acid caused the inhibition of brushite formation and promotion of monetite precipitation. Dissolution of monetite crystals was insensitive to citrate adsorption despite their lower surface area compared to brushite. Overall brushite/ monetite ratio decreased consistently with increasing citric acid concentration in the of 0?1-0?5M range.

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Dynamics of Biomineralization and Biodemineralization

Wang¹,

Nancollas²

2008

Biomineralization

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In order to understand the fundamental processes leading to biomineralization, this chapter focuses on the earliest events of homo/heterogeneous nucleation from an initial supersaturated solution phase and subsequent growth involving various possible precursor phases (amorphous or crystalline) to the final mineral phase by specific template and other influences. We also discuss how the combination of macroscopic constant composition and microscopic atomic force microscopy provides insights into the physical mechanisms of crystal growth and phase stability and the influences of proteins, peptides or other small molecules.Biodemineralization reactions of tooth enamel and bone may be inhibited or even suppressed when particle sizes fall into certain critical nanoscale levels. This phenomenon actually involves particle-size-dependent critical conditions of energetic control at the molecular level. Clearly, this dissolution termination is a kinetic phenomenon and cannot be attributed to reaction retardation as a result of surface modification by additives. Almost all biomineralized structures are highly hierarchical at many different length scales. At the lowest level they often consist of tiny crystals, typically tens to hundreds of nanometers. This size is not arbitrary; rather, it seems to give biominerals such as bone and tooth remarkable physical characteristics.

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Control of Biomineralization Dynamics by Interfacial Energies

Cited by 81 publications

References 22 publications

Molecular mechanisms of crystallization impacting calcium phosphate cements

Molecular mechanisms of crystallization impacting calcium phosphate cements

Monetite promoting effect of citric acid on brushite cement setting kinetics

Dynamics of Biomineralization and Biodemineralization

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