Simulation of Calcium Phosphate Pre-Nucleation Clusters in Aqueous Solution: Association Beyond Ion Pairing

© 2019 American Chemical Society. Classical molecular dynamics simulations and free energy methods have been used to obtain a better understanding of the molecular processes occurring prior to the first nucleation event for calcium phosphate biominerals. The association constants for the formation o...

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Main Authors: Garcia, Natalya, Innocenti Malini, R., Freeman, C., Demichelis, Raffaella, Raiteri, Paolo, Sommerdijk, N., Harding, J., Gale, Julian
Format: Journal Article
Language:English
Published: American Chemical Society 2019
Subjects:
Online Access:http://purl.org/au-research/grants/arc/DP160100677
http://hdl.handle.net/20.500.11937/77068
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author Garcia, Natalya
Innocenti Malini, R.
Freeman, C.
Demichelis, Raffaella
Raiteri, Paolo
Sommerdijk, N.
Harding, J.
Gale, Julian
author_facet Garcia, Natalya
Innocenti Malini, R.
Freeman, C.
Demichelis, Raffaella
Raiteri, Paolo
Sommerdijk, N.
Harding, J.
Gale, Julian
author_sort Garcia, Natalya
building Curtin Institutional Repository
collection Online Access
description © 2019 American Chemical Society. Classical molecular dynamics simulations and free energy methods have been used to obtain a better understanding of the molecular processes occurring prior to the first nucleation event for calcium phosphate biominerals. The association constants for the formation of negatively charged complexes containing calcium and phosphate ions in aqueous solution have been computed, and these results suggest that the previously proposed calcium phosphate building unit, [Ca(HPO4)3]4-, should only be present in small amounts under normal experimental conditions. However, the presence of an activation barrier for the removal of an HPO42- ion from this complex indicates that this species could be kinetically trapped. Aggregation pathways involving CaHPO4, [Ca(HPO4)2]2-, and [Ca(HPO4)3]4- complexes have been explored with the finding that dimerization is favorable up to a Ca/HPO4 ratio of 1:2.
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language English
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publishDate 2019
publisher American Chemical Society
recordtype eprints
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spelling curtin-20.500.11937-770682021-01-08T07:54:28Z Simulation of Calcium Phosphate Pre-Nucleation Clusters in Aqueous Solution: Association Beyond Ion Pairing Garcia, Natalya Innocenti Malini, R. Freeman, C. Demichelis, Raffaella Raiteri, Paolo Sommerdijk, N. Harding, J. Gale, Julian Science & Technology Physical Sciences Technology Chemistry, Multidisciplinary Crystallography Materials Science, Multidisciplinary Chemistry Materials Science MOLECULAR-DYNAMICS SIMULATIONS POSNERS CLUSTER FORCE-FIELD HYDROXYAPATITE NUCLEATION THERMODYNAMICS GROWTH MODEL WATER ACID © 2019 American Chemical Society. Classical molecular dynamics simulations and free energy methods have been used to obtain a better understanding of the molecular processes occurring prior to the first nucleation event for calcium phosphate biominerals. The association constants for the formation of negatively charged complexes containing calcium and phosphate ions in aqueous solution have been computed, and these results suggest that the previously proposed calcium phosphate building unit, [Ca(HPO4)3]4-, should only be present in small amounts under normal experimental conditions. However, the presence of an activation barrier for the removal of an HPO42- ion from this complex indicates that this species could be kinetically trapped. Aggregation pathways involving CaHPO4, [Ca(HPO4)2]2-, and [Ca(HPO4)3]4- complexes have been explored with the finding that dimerization is favorable up to a Ca/HPO4 ratio of 1:2. 2019 Journal Article http://hdl.handle.net/20.500.11937/77068 10.1021/acs.cgd.9b00889 English http://purl.org/au-research/grants/arc/DP160100677 http://purl.org/au-research/grants/arc/FL180100087 http://purl.org/au-research/grants/arc/FT130100463 http://purl.org/au-research/grants/arc/FT180100385 http://creativecommons.org/licenses/by/4.0/ American Chemical Society fulltext
spellingShingle Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Crystallography
Materials Science, Multidisciplinary
Chemistry
Materials Science
MOLECULAR-DYNAMICS SIMULATIONS
POSNERS CLUSTER
FORCE-FIELD
HYDROXYAPATITE
NUCLEATION
THERMODYNAMICS
GROWTH
MODEL
WATER
ACID
Garcia, Natalya
Innocenti Malini, R.
Freeman, C.
Demichelis, Raffaella
Raiteri, Paolo
Sommerdijk, N.
Harding, J.
Gale, Julian
Simulation of Calcium Phosphate Pre-Nucleation Clusters in Aqueous Solution: Association Beyond Ion Pairing
title Simulation of Calcium Phosphate Pre-Nucleation Clusters in Aqueous Solution: Association Beyond Ion Pairing
title_full Simulation of Calcium Phosphate Pre-Nucleation Clusters in Aqueous Solution: Association Beyond Ion Pairing
title_fullStr Simulation of Calcium Phosphate Pre-Nucleation Clusters in Aqueous Solution: Association Beyond Ion Pairing
title_full_unstemmed Simulation of Calcium Phosphate Pre-Nucleation Clusters in Aqueous Solution: Association Beyond Ion Pairing
title_short Simulation of Calcium Phosphate Pre-Nucleation Clusters in Aqueous Solution: Association Beyond Ion Pairing
title_sort simulation of calcium phosphate pre-nucleation clusters in aqueous solution: association beyond ion pairing
topic Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Crystallography
Materials Science, Multidisciplinary
Chemistry
Materials Science
MOLECULAR-DYNAMICS SIMULATIONS
POSNERS CLUSTER
FORCE-FIELD
HYDROXYAPATITE
NUCLEATION
THERMODYNAMICS
GROWTH
MODEL
WATER
ACID
url http://purl.org/au-research/grants/arc/DP160100677
http://purl.org/au-research/grants/arc/DP160100677
http://purl.org/au-research/grants/arc/DP160100677
http://purl.org/au-research/grants/arc/DP160100677
http://hdl.handle.net/20.500.11937/77068