Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics
The speciation of calcium carbonate in water is important to the geochemistry of the world's oceans and has ignited significant debate regarding the mechanism by which nucleation occurs. Here, it is vital to be able to quantify the thermodynamics of ion pairing versus higher order association p...
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| Format: | Journal Article |
| Language: | English |
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AMER CHEMICAL SOC
2020
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| Subjects: | |
| Online Access: | http://purl.org/au-research/grants/arc/FT130100463 http://hdl.handle.net/20.500.11937/84792 |
| _version_ | 1848764688923361280 |
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| author | Raiteri, Paolo Schuitemaker, Alicia Gale, Julian |
| author_facet | Raiteri, Paolo Schuitemaker, Alicia Gale, Julian |
| author_sort | Raiteri, Paolo |
| building | Curtin Institutional Repository |
| collection | Online Access |
| description | The speciation of calcium carbonate in water is important to the geochemistry of the world's oceans and has ignited significant debate regarding the mechanism by which nucleation occurs. Here, it is vital to be able to quantify the thermodynamics of ion pairing versus higher order association processes in order to distinguish between possible pathways. Given that it is experimentally challenging to quantify such species, here we determine the thermodynamics for ion pairing and multiple binding of calcium carbonate species using bias-enhanced molecular dynamics. In order to examine the uncertainties underlying these results, we derived a new polarizable force field for both calcium carbonate and bicarbonate in water based on the AMOEBA model to compare against our earlier rigid ion model, both of which are further benchmarked against ab initio molecular dynamics for the ion pair. Both force fields consistently indicate that the association of calcium carbonate ion pairs to form larger species is stable, though with an equilibrium constant that is lower than for ion pairing itself. |
| first_indexed | 2025-11-14T11:23:20Z |
| format | Journal Article |
| id | curtin-20.500.11937-84792 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| language | English |
| last_indexed | 2025-11-14T11:23:20Z |
| publishDate | 2020 |
| publisher | AMER CHEMICAL SOC |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-847922021-08-12T01:07:44Z Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics Raiteri, Paolo Schuitemaker, Alicia Gale, Julian Science & Technology Physical Sciences Chemistry, Physical Chemistry DIFFUSION-COEFFICIENTS DISSOCIATION-CONSTANTS SELF-DIFFUSION WATER MODEL SIMULATIONS DENSITY THERMODYNAMICS MECHANICS HYDRATION The speciation of calcium carbonate in water is important to the geochemistry of the world's oceans and has ignited significant debate regarding the mechanism by which nucleation occurs. Here, it is vital to be able to quantify the thermodynamics of ion pairing versus higher order association processes in order to distinguish between possible pathways. Given that it is experimentally challenging to quantify such species, here we determine the thermodynamics for ion pairing and multiple binding of calcium carbonate species using bias-enhanced molecular dynamics. In order to examine the uncertainties underlying these results, we derived a new polarizable force field for both calcium carbonate and bicarbonate in water based on the AMOEBA model to compare against our earlier rigid ion model, both of which are further benchmarked against ab initio molecular dynamics for the ion pair. Both force fields consistently indicate that the association of calcium carbonate ion pairs to form larger species is stable, though with an equilibrium constant that is lower than for ion pairing itself. 2020 Journal Article http://hdl.handle.net/20.500.11937/84792 10.1021/acs.jpcb.0c01582 English http://purl.org/au-research/grants/arc/FT130100463 http://purl.org/au-research/grants/arc/FL180100087 AMER CHEMICAL SOC fulltext |
| spellingShingle | Science & Technology Physical Sciences Chemistry, Physical Chemistry DIFFUSION-COEFFICIENTS DISSOCIATION-CONSTANTS SELF-DIFFUSION WATER MODEL SIMULATIONS DENSITY THERMODYNAMICS MECHANICS HYDRATION Raiteri, Paolo Schuitemaker, Alicia Gale, Julian Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics |
| title | Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics |
| title_full | Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics |
| title_fullStr | Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics |
| title_full_unstemmed | Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics |
| title_short | Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics |
| title_sort | ion pairing and multiple ion binding in calcium carbonate solutions based on a polarizable amoeba force field and ab initio molecular dynamics |
| topic | Science & Technology Physical Sciences Chemistry, Physical Chemistry DIFFUSION-COEFFICIENTS DISSOCIATION-CONSTANTS SELF-DIFFUSION WATER MODEL SIMULATIONS DENSITY THERMODYNAMICS MECHANICS HYDRATION |
| url | http://purl.org/au-research/grants/arc/FT130100463 http://purl.org/au-research/grants/arc/FT130100463 http://hdl.handle.net/20.500.11937/84792 |