Supersaturated calcium carbonate solutions are classical

doi:10.1126/sciadv.aao6283

Title: Supersaturated calcium carbonate solutions are classical

Full Record
Other Related Research

Abstract

We will present a description of nucleation phenomena in the condensed phase that takes into account non-ideal solution effects associated with cluster-cluster interaction. To do this we employ aggregation-volume bias Monte Carlo simulation, making the estimation of free-energy of large pre-critical clusters of sizes 10-20 tractable. We will compare and contrast empirical potential and electronic structure (e.g. Density functional theory) based descriptions of molecular interaction associated with the nucleation of CaCO3, highlighting free-energy trends and qualitative differences in populations of pre-critical clusters as a function of supersaturation. The influence of how the precise local interaction influences the non-ideal solution behavior on the nucleation and growth processes will be highlighted. This research was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences.

Authors:

;

; Xto, Jacinta M.; Pin, Sonia;

;

Publication Date:: 2018-01-01

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1430413

Report Number(s):: PNNL-SA-128147
Journal ID: ISSN 2375-2548; KC0301050

DOE Contract Number:: AC05-76RL01830

Resource Type:: Journal Article

Journal Name:: Science Advances

Additional Journal Information:: Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2375-2548

Publisher:: AAAS

Country of Publication:: United States

Language:: English

Citation Formats


                    Henzler, Katja, Fetisov, Evgenii O., Galib, Mirza, Baer, Marcel D., Legg, Benjamin A., Borca, Camelia, Xto, Jacinta M., Pin, Sonia, Fulton, John L., Schenter, Gregory K., Govind, Niranjan, Siepmann, J. Ilja, Mundy, Christopher J., Huthwelker, Thomas, and De Yoreo, James J. Supersaturated calcium carbonate solutions are classical.  United States: N. p., 2018. 
        Web.  doi:10.1126/sciadv.aao6283.

Copy to clipboard


                    Henzler, Katja, Fetisov, Evgenii O., Galib, Mirza, Baer, Marcel D., Legg, Benjamin A., Borca, Camelia, Xto, Jacinta M., Pin, Sonia, Fulton, John L., Schenter, Gregory K., Govind, Niranjan, Siepmann, J. Ilja, Mundy, Christopher J., Huthwelker, Thomas, & De Yoreo, James J. Supersaturated calcium carbonate solutions are classical.  United States.  doi:10.1126/sciadv.aao6283.

Copy to clipboard


                    Henzler, Katja, Fetisov, Evgenii O., Galib, Mirza, Baer, Marcel D., Legg, Benjamin A., Borca, Camelia, Xto, Jacinta M., Pin, Sonia, Fulton, John L., Schenter, Gregory K., Govind, Niranjan, Siepmann, J. Ilja, Mundy, Christopher J., Huthwelker, Thomas, and De Yoreo, James J. Mon .  
        "Supersaturated calcium carbonate solutions are classical".  United States.  doi:10.1126/sciadv.aao6283.

Copy to clipboard


                    
@article{osti_1430413,

  title        = {Supersaturated calcium carbonate solutions are classical},

  author       = {Henzler, Katja and Fetisov, Evgenii O. and Galib, Mirza and Baer, Marcel D. and Legg, Benjamin A. and Borca, Camelia and Xto, Jacinta M. and Pin, Sonia and Fulton, John L. and Schenter, Gregory K. and Govind, Niranjan and Siepmann, J. Ilja and Mundy, Christopher J. and Huthwelker, Thomas and De Yoreo, James J.},

  abstractNote = {We will present a description of nucleation phenomena in the condensed phase that takes into account non-ideal solution effects associated with cluster-cluster interaction. To do this we employ aggregation-volume bias Monte Carlo simulation, making the estimation of free-energy of large pre-critical clusters of sizes 10-20 tractable. We will compare and contrast empirical potential and electronic structure (e.g. Density functional theory) based descriptions of molecular interaction associated with the nucleation of CaCO3, highlighting free-energy trends and qualitative differences in populations of pre-critical clusters as a function of supersaturation. The influence of how the precise local interaction influences the non-ideal solution behavior on the nucleation and growth processes will be highlighted. This research was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences.},

  doi          = {10.1126/sciadv.aao6283},

  journal      = {Science Advances},

  issn         = {2375-2548},

  number       = 1,

  volume       = 4,

  place        = {United States},

  year         = {2018},

  month        = {1}

}

Copy to clipboard

Journal Article:

DOI: 10.1126/sciadv.aao6283

Other availability

Find in Google Scholar

Search WorldCat to find libraries that may hold this journal

Save / Share:

Export Metadata

Save to My Library

Similar records in OSTI.GOV collections:

Supersaturated calcium carbonate solutions are classical

Journal Article Henzler, Katja ; Fetisov, Evgenii O. ; Galib, Mirza ; ... - Science Advances

We will present a description of nucleation phenomena in the condensed phase that takes into account non-ideal solution effects associated with cluster-cluster interaction. To do this we employ aggregation-volume bias Monte Carlo simulation, making the estimation of free-energy of large pre-critical clusters of sizes 10-20 tractable. We will compare and contrast empirical potential and electronic structure (e.g. Density functional theory) based descriptions of molecular interaction associated with the nucleation of CaCO ₃, highlighting free-energy trends and qualitative differences in populations of pre-critical clusters as a function of supersaturation. The influence of how the precise local interaction influences the non-ideal solutionmore »« less
DOI: 10.1126/sciadv.aao6283
Investigating the significance of zero-point motion in small molecular clusters of sulphuric acid and water

Journal Article Stinson, Jake L. ; Kathmann, Shawn M. ; Ford, Ian J. - Journal of Chemical Physics, 140(2):024306

The nucleation of particles from trace gases in the atmosphere is an important source of cloud condensation nuclei (CCN), and these are vital for the formation of clouds in view of the high supersaturations required for homogeneous water droplet nucleation. The methods of quantum chemistry have increasingly been employed to model nucleation due to their high accuracy and efficiency in calculating configurational energies; and nucleation rates can be obtained from the associated free energies of particle formation. However, even in such advanced approaches, it is typically assumed that the nuclei have a classical nature, which is questionable for some systems.more »« less
DOI: 10.1063/1.4860973
Charge and Electric Field Fluctuations in Aqueous NaCl Electrolytes

Journal Article Sellner, Bernhard ; Valiev, Marat ; Kathmann, Shawn M. - Journal of Physical Chemistry B, 117(37):10869-10882

Conventional wisdom concerning crystallization assumes that when NaCl crystallizes from a supersaturated solution, the solvated ions retain their ionic character and simply relocate from their hydration spheres to their most stable positions in the crystal lattice. However, this conventional picture is at odds with observations over 200 years ago reporting the emission of long-lived light resulting from the crystallization of certain salts – appropriately referred to as crystalloluminescence. This suggests that electronic structure plays an essential role in crystallization. Strong electric field fluctuations in the gas or condensed phases can drive changes in electronic structure. We have calculated the fluctuationmore »« less
DOI: 10.1021/jp405578w
Structure, dynamics and stability of water/scCO ₂/mineral interfaces from ab initio molecular dynamics simulations

Journal Article Lee, Mal -Soon ; Peter McGrail, B. ; Rousseau, Roger ; ... - Scientific Reports

Here, the interface between a solid and a complex multi-component liquid forms a unique reaction environment whose structure and composition can significantly deviate from either bulk or liquid phase and is poorly understood due the innate difficulty to obtain molecular level information. Feldspar minerals, as typified by the Ca-end member Anorthite, serve as prototypical model systems to assess the reactivity and ion mobility at solid/water-bearing supercritical fluid (WBSF) interfaces due to recent X-ray based measurements that provide information on water-film formation, and cation vacancies at these surfaces. Using density functional theory based molecular dynamics, which allows the evaluation of reactivitymore »« less
Cited by 5
DOI: 10.1038/srep14857

Full Text Available
Ground and excited states of the [Fe(H2O)6]2+ and [Fe(H2O)6]3+ clusters: Insight into the electronic structure of the [Fe(H2O)6]2+ – [Fe(H2O)6]3+ complex

Journal Article Miliordos, Evangelos ; Xantheas, Sotiris S. - Journal of Chemical Theory and Computation, 11(4):1549-1563

We report the ground and low lying electronically excited states of the [Fe(H2O)6]2+ and [Fe(H2O)6]3+ clusters using multi-configuration electronic structure theory. In particular, we have constructed the Potential Energy Curves (PECs) with respect to the iron-oxygen distance when removing all water ligands at the same time from the cluster minima and established their correlation to the long range dissociation channels. Due to the fact that both the second and third ionization potentials of iron are larger than the one for water, the ground state products asymptotically correlate with dissociation channels that are repulsive in nature at large separations as theymore »« less
DOI: 10.1021/ct501143c

Similar Records