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Title: Atomistic Structure of Mineral Nano-aggregates from Simulated Compaction and Dewatering

Abstract

The porosity of clay aggregates is an important property governing chemical reactions and fluid flow in low-permeability geologic formations and clay-based engineered barrier systems. Pore spaces in clays include interlayer and interparticle pores. Under compaction and dewatering, the size and geometry of such pore spaces may vary significantly (sub-nanometer to microns) depending on ambient physical and chemical conditions. Here we report a molecular dynamics simulation method to construct a complex and realistic clay-like nanoparticle aggregate with interparticle pores and grain boundaries. The model structure is then used to investigate the effect of dewatering and water content on micro-porosity of the aggregates. The results suggest that slow dewatering would create more compact aggregates compared to fast dewatering. Furthermore, the amount of water present in the aggregates strongly affects the particle-particle interactions and hence the aggregate structure. Detailed analyses of particle-particle and water-particle interactions provide a molecular-scale view of porosity and texture development of the aggregates. The simulation method developed here may also aid in modeling the synthesis of nanostructured materials through self-assembly of nanoparticles.

Authors:
 [1];  [1];  [2];  [1]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Geochemistry Dept.
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Nuclear Waste Disposal Research and Analysis Dept.
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1421627
Report Number(s):
SAND2017-12026J
Journal ID: ISSN 2045-2322; PII: 15639
Grant/Contract Number:  
NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; geochemistry; mineralogy

Citation Formats

Ho, Tuan Anh, Greathouse, Jeffery A., Wang, Yifeng, and Criscenti, Louise J. Atomistic Structure of Mineral Nano-aggregates from Simulated Compaction and Dewatering. United States: N. p., 2017. Web. doi:10.1038/s41598-017-15639-4.
Ho, Tuan Anh, Greathouse, Jeffery A., Wang, Yifeng, & Criscenti, Louise J. Atomistic Structure of Mineral Nano-aggregates from Simulated Compaction and Dewatering. United States. doi:10.1038/s41598-017-15639-4.
Ho, Tuan Anh, Greathouse, Jeffery A., Wang, Yifeng, and Criscenti, Louise J. Fri . "Atomistic Structure of Mineral Nano-aggregates from Simulated Compaction and Dewatering". United States. doi:10.1038/s41598-017-15639-4. https://www.osti.gov/servlets/purl/1421627.
@article{osti_1421627,
title = {Atomistic Structure of Mineral Nano-aggregates from Simulated Compaction and Dewatering},
author = {Ho, Tuan Anh and Greathouse, Jeffery A. and Wang, Yifeng and Criscenti, Louise J.},
abstractNote = {The porosity of clay aggregates is an important property governing chemical reactions and fluid flow in low-permeability geologic formations and clay-based engineered barrier systems. Pore spaces in clays include interlayer and interparticle pores. Under compaction and dewatering, the size and geometry of such pore spaces may vary significantly (sub-nanometer to microns) depending on ambient physical and chemical conditions. Here we report a molecular dynamics simulation method to construct a complex and realistic clay-like nanoparticle aggregate with interparticle pores and grain boundaries. The model structure is then used to investigate the effect of dewatering and water content on micro-porosity of the aggregates. The results suggest that slow dewatering would create more compact aggregates compared to fast dewatering. Furthermore, the amount of water present in the aggregates strongly affects the particle-particle interactions and hence the aggregate structure. Detailed analyses of particle-particle and water-particle interactions provide a molecular-scale view of porosity and texture development of the aggregates. The simulation method developed here may also aid in modeling the synthesis of nanostructured materials through self-assembly of nanoparticles.},
doi = {10.1038/s41598-017-15639-4},
journal = {Scientific Reports},
number = ,
volume = 7,
place = {United States},
year = {2017},
month = {11}
}

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Works referenced in this record:

Mesoscopic structure of dry-pressed clay samples from small-angle X-ray scattering measurements
journal, March 2007

  • Méheust, Yves; Dagois-Bohy, Simon; Knudsen, Kenneth D.
  • Journal of Applied Crystallography, Vol. 40, Issue s1
  • DOI: 10.1107/S0021889807008552

Hydrodynamics in Clay Nanopores
journal, July 2011

  • Boţan, Alexandru; Rotenberg, Benjamin; Marry, Virginie
  • The Journal of Physical Chemistry C, Vol. 115, Issue 32
  • DOI: 10.1021/jp204772c

Molecular Simulation of Carbon Dioxide Capture by Montmorillonite Using an Accurate and Flexible Force Field
journal, June 2012

  • Cygan, Randall T.; Romanov, Vyacheslav N.; Myshakin, Evgeniy M.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 24
  • DOI: 10.1021/jp3007574

Fast Synthesis and Size Control of Gibbsite Nanoplatelets, Their Pseudomorphic Dehydroxylation, and Efficient Dye Adsorption
journal, September 2013

  • Louaer, Seifeddine; Wang, Yao; Guo, Lin
  • ACS Applied Materials & Interfaces, Vol. 5, Issue 19
  • DOI: 10.1021/am402677v

Molecular simulation of aqueous solutions at clay surfaces
journal, June 2010


Clay mineralogical investigations related to nuclear waste disposal
journal, March 1998


Protonation and Charging of Nanosized Gibbsite (α-Al(OH) 3 ) Particles in Aqueous Suspension
journal, June 2002

  • Rosenqvist, Jörgen; Persson, Per; Sjöberg, Staffan
  • Langmuir, Vol. 18, Issue 12
  • DOI: 10.1021/la015753t

Numerical integration of the cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes
journal, March 1977

  • Ryckaert, Jean-Paul; Ciccotti, Giovanni; Berendsen, Herman J. C.
  • Journal of Computational Physics, Vol. 23, Issue 3
  • DOI: 10.1016/0021-9991(77)90098-5

Solvent-accessible surfaces of proteins and nucleic acids
journal, August 1983


Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


Effect of Polydispersity of Clay Platelets on the Aggregation And Mechanical Properties of Clay at the Mesoscale
journal, August 2016

  • Ebrahimi, Davoud; Whittle, AndrewJ.; Pellenq, RolandJ. -M.
  • Clays and Clay Minerals, Vol. 64, Issue 4
  • DOI: 10.1346/Ccmn.2016.0640407

Effect of water on methane and carbon dioxide sorption in clay minerals by Monte Carlo simulations
journal, November 2014


Caesium incorporation and retention in illite interlayers
journal, May 2015


Fast Method for Computing Pore Size Distributions of Model Materials
journal, August 2006

  • Bhattacharya, Supriyo; Gubbins, Keith E.
  • Langmuir, Vol. 22, Issue 18
  • DOI: 10.1021/la052651k

Derivation and evaluation of a flexible SPC model for liquid water
journal, August 2004


Coupled synthesis and self-assembly of nanoparticles to give structures with controlled organization
journal, November 1999

  • Li, Mei; Schnablegger, Heimo; Mann, Stephen
  • Nature, Vol. 402, Issue 6760
  • DOI: 10.1038/46509

Nanogibbsite: Synthesis and characterization
journal, December 2010

  • Kumara, C. K.; Ng, W. J.; Bandara, A.
  • Journal of Colloid and Interface Science, Vol. 352, Issue 2
  • DOI: 10.1016/j.jcis.2010.08.083

In Situ Molecular Spectroscopic Evidence for CO 2 Intercalation into Montmorillonite in Supercritical Carbon Dioxide
journal, April 2012

  • Loring, John S.; Schaef, Herbert T.; Turcu, Romulus V. F.
  • Langmuir, Vol. 28, Issue 18
  • DOI: 10.1021/la301136w

Fluid-driven metamorphism of the continental crust governed by nanoscale fluid flow
journal, August 2017

  • Plümper, Oliver; Botan, Alexandru; Los, Catharina
  • Nature Geoscience, Vol. 10, Issue 9
  • DOI: 10.1038/ngeo3009

Why Clays Swell
journal, December 2002

  • Hensen, Emiel J. M.; Smit, Berend
  • The Journal of Physical Chemistry B, Vol. 106, Issue 49
  • DOI: 10.1021/jp0264883

Clay swelling — A challenge in the oilfield
journal, February 2010


Modeling the Acid–Base Properties of Montmorillonite Edge Surfaces
journal, November 2016

  • Tournassat, Christophe; Davis, James A.; Chiaberge, Christophe
  • Environmental Science & Technology, Vol. 50, Issue 24
  • DOI: 10.1021/acs.est.6b04677

Molecular dynamics simulations of cesium adsorption on illite nanoparticles
journal, March 2017

  • Lammers, Laura N.; Bourg, Ian C.; Okumura, Masahiko
  • Journal of Colloid and Interface Science, Vol. 490
  • DOI: 10.1016/j.jcis.2016.11.084

Interfacial structures and acidity of edge surfaces of ferruginous smectites
journal, November 2015


Anion exclusion effects in compacted bentonites: Towards a better understanding of anion diffusion
journal, November 2007


Realistic molecular model of kerogen’s nanostructure
journal, February 2016

  • Bousige, Colin; Ghimbeu, Camélia Matei; Vix-Guterl, Cathie
  • Nature Materials, Vol. 15, Issue 5
  • DOI: 10.1038/Nmat4541

Molecular Models of Hydroxide, Oxyhydroxide, and Clay Phases and the Development of a General Force Field
journal, January 2004

  • Cygan, Randall T.; Liang, Jian-Jie; Kalinichev, Andrey G.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 4
  • DOI: 10.1021/jp0363287

Specific surface area and pore-size distribution in clays and shales
journal, January 2013


Structure of Hydrated Gibbsite and Brucite Edge Surfaces: DFT Results and Further Development of the ClayFF Classical Force Field with Metal–O–H Angle Bending Terms
journal, June 2017

  • Pouvreau, Maxime; Greathouse, Jeffery A.; Cygan, Randall T.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 27
  • DOI: 10.1021/acs.jpcc.7b05362

A molecular dynamics method for simulations in the canonical ensemble
journal, June 1984


Toward Modeling Clay Mineral Nanoparticles: The Edge Surfaces of Pyrophyllite and Their Interaction with Water
journal, November 2014

  • Martins, David M. S.; Molinari, Marco; Gonçalves, Mário A.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 47
  • DOI: 10.1021/jp5070853

Mobility of Na and Cs on Montmorillonite Surface under Partially Saturated Conditions
journal, August 2013

  • Churakov, Sergey V.
  • Environmental Science & Technology, Vol. 47, Issue 17
  • DOI: 10.1021/es401530n

Factors Influencing the Early Stages of the Compaction of Clays and Sands--Review
journal, January 1966


Molecular models and simulations of layered materials
journal, January 2009

  • Cygan, Randall T.; Greathouse, Jeffery A.; Heinz, Hendrik
  • Journal of Materials Chemistry, Vol. 19, Issue 17
  • DOI: 10.1039/b819076c

Molecular Simulation of Structure and Diffusion at Smectite–Water Interfaces: Using Expanded Clay Interlayers as Model Nanopores
journal, July 2015

  • Greathouse, Jeffery A.; Hart, David B.; Bowers, Geoffrey M.
  • The Journal of Physical Chemistry C, Vol. 119, Issue 30
  • DOI: 10.1021/acs.jpcc.5b03314

Molecular Dynamics of Supercritical Water Using a Flexible SPC Model
journal, December 1994

  • Mizan, Tahmid I.; Savage, Phillip E.; Ziff, Robert M.
  • The Journal of Physical Chemistry, Vol. 98, Issue 49
  • DOI: 10.1021/j100100a042

Clay, Water, and Salt: Controls on the Permeability of Fine-Grained Sedimentary Rocks
journal, August 2017


Small-angle neutron scattering from a nano-layered synthetic silicate
journal, October 2004


Nanostructural control of methane release in kerogen and its implications to wellbore production decline
journal, June 2016

  • Ho, Tuan Anh; Criscenti, Louise J.; Wang, Yifeng
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep28053

Up-Scaling of Molecular Diffusion Coefficients in Clays: A Two-Step Approach
journal, March 2011

  • Churakov, Sergey V.; Gimmi, Thomas
  • The Journal of Physical Chemistry C, Vol. 115, Issue 14
  • DOI: 10.1021/jp112325n

Mesoscale properties of clay aggregates from potential of mean force representation of interactions between nanoplatelets
journal, April 2014

  • Ebrahimi, Davoud; Whittle, Andrew J.; Pellenq, Roland J. -M.
  • The Journal of Chemical Physics, Vol. 140, Issue 15
  • DOI: 10.1063/1.4870932

Water and methane in shale rocks: Flow pattern effects on fluid transport and pore structure
journal, August 2015

  • Ho, Tuan A.; Striolo, Alberto
  • AIChE Journal, Vol. 61, Issue 9
  • DOI: 10.1002/aic.14869

Stability of dioctahedral 2:1 phyllosilicate edge structures based on pyrophyllite models
journal, August 2015

  • Lavikainen, Lasse P.; Hirvi, Janne T.; Kasa, Seppo
  • Theoretical Chemistry Accounts, Vol. 134, Issue 9
  • DOI: 10.1007/s00214-015-1715-6

Structure and stability of pyrophyllite edge surfaces: Effect of temperature and water chemical potential
journal, October 2016


Intercalation and Retention of Carbon Dioxide in a Smectite Clay promoted by Interlayer Cations
journal, March 2015

  • Michels, L.; Fossum, J. O.; Rozynek, Z.
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep08775

Temperature dependence of interfacial structures and acidity of clay edge surfaces
journal, July 2015


Absolute acidity of clay edge sites from ab-initio simulations
journal, October 2012


Vibrational Analysis of Brucite Surfaces and the Development of an Improved Force Field for Molecular Simulation of Interfaces
journal, April 2014

  • Zeitler, Todd R.; Greathouse, Jeffery A.; Gale, Julian D.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 15
  • DOI: 10.1021/jp411092b