Development and application of ReaxFF methodology for understanding the chemical dynamics of metal carbonates in aqueous solutions
Abstract
A new ReaxFF reactive force field has been developed for metal carbonate systems including Na+, Ca2+, and Mg2+ cations and the CO32– anion. This force field is fully transferable with previous ReaxFF water and water/electrolyte descriptions. The Me–O–C (Me = metal) three-body valence angle parameters and Me–C non-reactive parameters of the force field have been optimized against quantum mechanical calculations including equations of state, heats of formation, heats of reaction, angle distortions and vibrational frequencies. The new metal carbonate force field has been validated using molecular dynamics simulations to study the solvation and reactivity of metal and carbonate ions in water at 300 K and 700 K. The coordination radius and self-diffusion coefficient show good consistency with existing experimental and simulation results. The angular distribution analysis explains the structural preference of carbonate ions to form carbonates and bicarbonates, where Na+ predominantly forms carbonates due to weaker angular strain, while Ca2+ and Mg2+ prefer to form bicarbonate monodentate in nature. Residence time distribution analyses on different systems reveal the role of ions in accelerating and decelerating the dynamics of water and carbonate ions under different thermodynamic conditions. The formation and dissolution of bicarbonates and carbonates in solution were explored on themore »
- Authors:
-
- Pennsylvania State Univ., University Park, PA (United States)
- Publication Date:
- Research Org.:
- Univ. of Utah, Salt Lake City, UT (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1844392
- Alternate Identifier(s):
- OSTI ID: 1841449
- Grant/Contract Number:
- SC0019285
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 24; Journal Issue: 5; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Dasgupta, Nabankur, Chen, Chen, and van Duin, Adri C. T. Development and application of ReaxFF methodology for understanding the chemical dynamics of metal carbonates in aqueous solutions. United States: N. p., 2022.
Web. doi:10.1039/d1cp04790f.
Dasgupta, Nabankur, Chen, Chen, & van Duin, Adri C. T. Development and application of ReaxFF methodology for understanding the chemical dynamics of metal carbonates in aqueous solutions. United States. https://doi.org/10.1039/d1cp04790f
Dasgupta, Nabankur, Chen, Chen, and van Duin, Adri C. T. Fri .
"Development and application of ReaxFF methodology for understanding the chemical dynamics of metal carbonates in aqueous solutions". United States. https://doi.org/10.1039/d1cp04790f. https://www.osti.gov/servlets/purl/1844392.
@article{osti_1844392,
title = {Development and application of ReaxFF methodology for understanding the chemical dynamics of metal carbonates in aqueous solutions},
author = {Dasgupta, Nabankur and Chen, Chen and van Duin, Adri C. T.},
abstractNote = {A new ReaxFF reactive force field has been developed for metal carbonate systems including Na+, Ca2+, and Mg2+ cations and the CO32– anion. This force field is fully transferable with previous ReaxFF water and water/electrolyte descriptions. The Me–O–C (Me = metal) three-body valence angle parameters and Me–C non-reactive parameters of the force field have been optimized against quantum mechanical calculations including equations of state, heats of formation, heats of reaction, angle distortions and vibrational frequencies. The new metal carbonate force field has been validated using molecular dynamics simulations to study the solvation and reactivity of metal and carbonate ions in water at 300 K and 700 K. The coordination radius and self-diffusion coefficient show good consistency with existing experimental and simulation results. The angular distribution analysis explains the structural preference of carbonate ions to form carbonates and bicarbonates, where Na+ predominantly forms carbonates due to weaker angular strain, while Ca2+ and Mg2+ prefer to form bicarbonate monodentate in nature. Residence time distribution analyses on different systems reveal the role of ions in accelerating and decelerating the dynamics of water and carbonate ions under different thermodynamic conditions. The formation and dissolution of bicarbonates and carbonates in solution were explored on the basis of the protonation capability in different systems. Here, the nucleation phenomenon of metal carbonates at ambient and supercritical conditions is explained from the perspective of cluster formation over time: Ca2+ ions can form prenucleation clusters at ambient temperature but show saturation with increasing temperature, whereas Na+ and Mg2+ ions show a rapid increase in cluster size and amount upon increasing time and temperature.},
doi = {10.1039/d1cp04790f},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 5,
volume = 24,
place = {United States},
year = {Fri Jan 07 00:00:00 EST 2022},
month = {Fri Jan 07 00:00:00 EST 2022}
}
Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
A Molecular Dynamics Study of the Early Stages of Calcium Carbonate Growth
journal, August 2009
- Tribello, Gareth A.; Bruneval, Fabien; Liew, CheeChin
- The Journal of Physical Chemistry B, Vol. 113, Issue 34
ReaxFF molecular dynamics simulations of electrolyte–water systems at supercritical temperature
journal, May 2020
- Dasgupta, Nabankur; Shin, Yun Kyung; Fedkin, Mark V.
- The Journal of Chemical Physics, Vol. 152, Issue 20
Understanding the chemistry of cation leaching in illite/water interfacial system using reactive molecular dynamics simulations and hydrothermal experiments
journal, March 2020
- Muraleedharan, Murali Gopal; Herz-Thyhsen, Ryan; Dewey, Janet C.
- Acta Materialia, Vol. 186
The NIST Chemistry WebBook: A Chemical Data Resource on the Internet †
journal, September 2001
- Linstrom, Peter J.; Mallard, William G.
- Journal of Chemical & Engineering Data, Vol. 46, Issue 5
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Ion Pairing and Multiple Ion Binding in Calcium Carbonate Solutions Based on a Polarizable AMOEBA Force Field and Ab Initio Molecular Dynamics
journal, April 2020
- Raiteri, Paolo; Schuitemaker, Alicia; Gale, Julian D.
- The Journal of Physical Chemistry B, Vol. 124, Issue 17
A New Transferable Forcefield for Simulating the Mechanics of CaCO 3 Crystals
journal, September 2011
- Xiao, Shijun; Edwards, Scott A.; Gräter, Frauke
- The Journal of Physical Chemistry C, Vol. 115, Issue 41
The ReaxFF reactive force-field: development, applications and future directions
journal, March 2016
- Senftle, Thomas P.; Hong, Sungwook; Islam, Md Mahbubul
- npj Computational Materials, Vol. 2, Issue 1
Molecular Dynamics Study of the Solvation of Calcium Carbonate in Water
journal, October 2007
- Bruneval, Fabien; Donadio, Davide; Parrinello, Michele
- The Journal of Physical Chemistry B, Vol. 111, Issue 42
Derivation of an Accurate Force-Field for Simulating the Growth of Calcium Carbonate from Aqueous Solution: A New Model for the Calcite−Water Interface
journal, February 2010
- Raiteri, Paolo; Gale, Julian D.; Quigley, David
- The Journal of Physical Chemistry C, Vol. 114, Issue 13
Ab Initio Thermodynamics of Hydrated Calcium Carbonates and Calcium Analogues of Magnesium Carbonates: Implications for Carbonate Crystallization Pathways
journal, January 2018
- Chaka, Anne M.
- ACS Earth and Space Chemistry, Vol. 2, Issue 3
Molecular dynamics simulations of a lithium/sodium carbonate mixture
journal, February 2016
- Ottochian, Alistar; Ricca, Chiara; Labat, Frederic
- Journal of Molecular Modeling, Vol. 22, Issue 3
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
System-Size Dependence of Diffusion Coefficients and Viscosities from Molecular Dynamics Simulations with Periodic Boundary Conditions
journal, October 2004
- Yeh, In-Chul; Hummer, Gerhard
- The Journal of Physical Chemistry B, Vol. 108, Issue 40
The MgCO 3 –CaCO 3 –Li 2 CO 3 –Na 2 CO 3 –K 2 CO 3 melts: Thermodynamics and transport properties by atomistic simulations
journal, June 2019
- Desmaele, Elsa; Sator, Nicolas; Vuilleumier, Rodolphe
- The Journal of Chemical Physics, Vol. 150, Issue 21
Hydrogen-Bonding Structure and Dynamics of Aqueous Carbonate Species from Car−Parrinello Molecular Dynamics Simulations
journal, January 2009
- Kumar, P. Padma; Kalinichev, Andrey G.; Kirkpatrick, R. James
- The Journal of Physical Chemistry B, Vol. 113, Issue 3
ReaxFF Reactive Force Field for Molecular Dynamics Simulations of Hydrocarbon Oxidation
journal, February 2008
- Chenoweth, Kimberly; van Duin, Adri C. T.; Goddard, William A.
- The Journal of Physical Chemistry A, Vol. 112, Issue 5
Jaguar: A high-performance quantum chemistry software program with strengths in life and materials sciences
journal, July 2013
- Bochevarov, Art D.; Harder, Edward; Hughes, Thomas F.
- International Journal of Quantum Chemistry, Vol. 113, Issue 18
Role of molecular charge and hydrophilicity in regulating the kinetics of crystal growth
journal, December 2006
- Elhadj, S.; De Yoreo, J. J.; Hoyer, J. R.
- Proceedings of the National Academy of Sciences, Vol. 103, Issue 51, p. 19237-19242
Stable Prenucleation Calcium Carbonate Clusters
journal, December 2008
- Gebauer, Denis; Völkel, Antje; Cölfen, Helmut
- Science, Vol. 322, Issue 5909
ReaxFF: A Reactive Force Field for Hydrocarbons
journal, October 2001
- van Duin, Adri C. T.; Dasgupta, Siddharth; Lorant, Francois
- The Journal of Physical Chemistry A, Vol. 105, Issue 41
ReaxFF molecular dynamics simulations on the structure and dynamics of electrolyte water systems at ambient temperature
journal, February 2020
- Dasgupta, Nabankur; Kyung Shin, Yun; Fedkin, Mark V.
- Computational Materials Science, Vol. 172
Chemistry with ADF
journal, January 2001
- te Velde, G.; Bickelhaupt, F. M.; Baerends, E. J.
- Journal of Computational Chemistry, Vol. 22, Issue 9, p. 931-967
Prenucleation clusters and non-classical nucleation
journal, December 2011
- Gebauer, Denis; Cölfen, Helmut
- Nano Today, Vol. 6, Issue 6
Experimental investigation and mathematical modelling of the carbon dioxide sequestration of cement pastes during pressurized CO2 curing
journal, October 2021
- Tang, Wei; Zhan, Baojian; Wu, Cunran
- Construction and Building Materials, Vol. 302
Surface Reactivity and Leaching of a Sodium Silicate Glass under an Aqueous Environment: A ReaxFF Molecular Dynamics Study
journal, May 2019
- Hahn, Seung Ho; van Duin, Adri C. T.
- The Journal of Physical Chemistry C, Vol. 123, Issue 25
Surface Chemistry and Dissolution Kinetics of Divalent Metal Carbonates
journal, February 2002
- Pokrovsky, O. S.; Schott, J.
- Environmental Science & Technology, Vol. 36, Issue 3
Structure and dynamics of the hydrated magnesium ion and of the solvated magnesium carbonates: insights from first principles simulations
journal, January 2010
- Tommaso, Devis Di; de Leeuw, Nora H.
- Phys. Chem. Chem. Phys., Vol. 12, Issue 4
Development of the ReaxFF Methodology for Electrolyte–Water Systems
journal, February 2019
- Fedkin, Mark V.; Shin, Yun Kyung; Dasgupta, Nabankur
- The Journal of Physical Chemistry A, Vol. 123, Issue 10
Structural and Dynamical Nature of Hydration Shells of the Carbonate Ion in Water: An Ab Initio Molecular Dynamics Study
journal, January 2018
- Yadav, Sushma; Chandra, Amalendu
- The Journal of Physical Chemistry B, Vol. 122, Issue 4
Interfacial Reactivity and Speciation Emerging from Na-Montmorillonite Interactions with Water and Formic Acid at 200 °C: Insights from Reactive Molecular Dynamics Simulations, Infrared Spectroscopy, and X-ray Scattering Measurements
journal, April 2021
- Muraleedharan, Murali Gopal; Asgar, Hassnain; Hahn, Seung Ho
- ACS Earth and Space Chemistry, Vol. 5, Issue 5
Carbon dioxide storage potential of shales
journal, July 2008
- Busch, A.; Alles, S.; Gensterblum, Y.
- International Journal of Greenhouse Gas Control, Vol. 2, Issue 3
Thermodynamically Consistent Force Field for Molecular Dynamics Simulations of Alkaline-Earth Carbonates and Their Aqueous Speciation
journal, October 2015
- Raiteri, Paolo; Demichelis, Raffaella; Gale, Julian D.
- The Journal of Physical Chemistry C, Vol. 119, Issue 43
Interfacial Bonding Controls Friction in Diamond–Rock Contacts
journal, August 2021
- Bhamra, Jagjeevan S.; Ewen, James P.; Latorre, Carlos Ayestarán
- The Journal of Physical Chemistry C, Vol. 125, Issue 33
Surface Structure and Morphology of Calcium Carbonate Polymorphs Calcite, Aragonite, and Vaterite: An Atomistic Approach
journal, April 1998
- de Leeuw, Nora H.; Parker, Stephen C.
- The Journal of Physical Chemistry B, Vol. 102, Issue 16
The Role of Carbonate in Catalytic Oxidations
journal, September 2020
- Patra, Shanti Gopal; Mizrahi, Amir; Meyerstein, Dan
- Accounts of Chemical Research, Vol. 53, Issue 10
Development of a ReaxFF reactive force field for lithium ion conducting solid electrolyte Li 1+x Al x Ti 2−x (PO 4 ) 3 (LATP)
journal, January 2018
- Shin, Yun Kyung; Sengul, Mert Y.; Jonayat, A. S. M.
- Physical Chemistry Chemical Physics, Vol. 20, Issue 34
Water Is the Key to Nonclassical Nucleation of Amorphous Calcium Carbonate
journal, December 2010
- Raiteri, Paolo; Gale, Julian D.
- Journal of the American Chemical Society, Vol. 132, Issue 49
Flue gas purification from SO2 and NOx using molten mixture of alkali metal carbonates
journal, June 2021
- Dosmukhamedov, Nurlan; Kaplan, Valery
- International Journal of Coal Preparation and Utilization
The Onset of Calcium Carbonate Nucleation: A Density Functional Theory Molecular Dynamics and Hybrid Microsolvation/Continuum Study
journal, May 2008
- Tommaso, Devis Di; de Leeuw, Nora H.
- The Journal of Physical Chemistry B, Vol. 112, Issue 23
Dynamics of Confined Reactive Water in Smectite Clay–Zeolite Composites
journal, February 2012
- Pitman, Michael C.; van Duin, Adri C. T.
- Journal of the American Chemical Society, Vol. 134, Issue 6
Electronegativity Equalization Method: Parameterization and Validation for Large Sets of Organic, Organohalogene and Organometal Molecule
journal, July 2007
- Varekova, Radka; Jirouskova, Zuzanna; Vanek, Jakub
- International Journal of Molecular Sciences, Vol. 8, Issue 7