DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Self-Assembly of Silica Nanoparticles at Water–Hydrocarbon Interfaces: Insights from In Operando Small-Angle X-ray Scattering Measurements and Molecular Dynamics Simulations

Abstract

To achieve tunable controls on the interactions of siliceous materials in subsurface environments bearing water and hydrocarbons, it is essential to determine the influence of hydrocarbon–water interfaces on the self-assembly of the silica particles. The hydrophilic silica particle have a tendency to aggregate on the water front of the interface. Self-assembly of silica nanoparticles proceeds via the migration of these nanoparticles to the water–hydrocarbon interface followed by aggregation at the interface. Fractal-like morphologies of assembled silica nanoparticles at water–hydrocarbon interfaces are observed. Rapid assembly of the hydrophilic silica nanoparticles at water–hydrocarbon interfaces corresponds to an overall reduction in the surface tension of water–toluene and water–heptane systems. These studies demonstrate the silica aggregation that is the precursor of silica polymerization, or nucleation and growth is influenced by the presence of hydrocarbons in subsurface geologic environments. These insights were derived from in operando ultrasmall and small-angle X-ray scattering (USAXS/SAXS) measurements, cryo-scanning electron microscopy (Cryo-SEM) imaging, and classical molecular dynamics simulations. As a result, these studies are intended to inform current and future efforts aimed at tuning silica reactivity in subsurface geologic environments to enhance permeability, the design and use of silica-based proppants to enhance fractures, and the development of effective strategies tomore » control silica-based scaling behavior in subsurface reservoirs.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]
  1. Cornell Univ., Ithaca, NY (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Univ. of Utah, Salt Lake City, UT (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1721723
Alternate Identifier(s):
OSTI ID: 1797955
Grant/Contract Number:  
SC0019285; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Energy and Fuels
Additional Journal Information:
Journal Volume: 34; Journal Issue: 10; Journal ID: ISSN 0887-0624
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; Self organization; Emulsions; Hydrocarbons; Interfaces; Nanoparticles; MD simulations; interfacial tension

Citation Formats

Mohammed, Sohaib, Asgar, Hassnain, Kuzmenko, Ivan, and Gadikota, Greeshma. Self-Assembly of Silica Nanoparticles at Water–Hydrocarbon Interfaces: Insights from In Operando Small-Angle X-ray Scattering Measurements and Molecular Dynamics Simulations. United States: N. p., 2020. Web. doi:10.1021/acs.energyfuels.0c02759.
Mohammed, Sohaib, Asgar, Hassnain, Kuzmenko, Ivan, & Gadikota, Greeshma. Self-Assembly of Silica Nanoparticles at Water–Hydrocarbon Interfaces: Insights from In Operando Small-Angle X-ray Scattering Measurements and Molecular Dynamics Simulations. United States. https://doi.org/10.1021/acs.energyfuels.0c02759
Mohammed, Sohaib, Asgar, Hassnain, Kuzmenko, Ivan, and Gadikota, Greeshma. Wed . "Self-Assembly of Silica Nanoparticles at Water–Hydrocarbon Interfaces: Insights from In Operando Small-Angle X-ray Scattering Measurements and Molecular Dynamics Simulations". United States. https://doi.org/10.1021/acs.energyfuels.0c02759. https://www.osti.gov/servlets/purl/1721723.
@article{osti_1721723,
title = {Self-Assembly of Silica Nanoparticles at Water–Hydrocarbon Interfaces: Insights from In Operando Small-Angle X-ray Scattering Measurements and Molecular Dynamics Simulations},
author = {Mohammed, Sohaib and Asgar, Hassnain and Kuzmenko, Ivan and Gadikota, Greeshma},
abstractNote = {To achieve tunable controls on the interactions of siliceous materials in subsurface environments bearing water and hydrocarbons, it is essential to determine the influence of hydrocarbon–water interfaces on the self-assembly of the silica particles. The hydrophilic silica particle have a tendency to aggregate on the water front of the interface. Self-assembly of silica nanoparticles proceeds via the migration of these nanoparticles to the water–hydrocarbon interface followed by aggregation at the interface. Fractal-like morphologies of assembled silica nanoparticles at water–hydrocarbon interfaces are observed. Rapid assembly of the hydrophilic silica nanoparticles at water–hydrocarbon interfaces corresponds to an overall reduction in the surface tension of water–toluene and water–heptane systems. These studies demonstrate the silica aggregation that is the precursor of silica polymerization, or nucleation and growth is influenced by the presence of hydrocarbons in subsurface geologic environments. These insights were derived from in operando ultrasmall and small-angle X-ray scattering (USAXS/SAXS) measurements, cryo-scanning electron microscopy (Cryo-SEM) imaging, and classical molecular dynamics simulations. As a result, these studies are intended to inform current and future efforts aimed at tuning silica reactivity in subsurface geologic environments to enhance permeability, the design and use of silica-based proppants to enhance fractures, and the development of effective strategies to control silica-based scaling behavior in subsurface reservoirs.},
doi = {10.1021/acs.energyfuels.0c02759},
journal = {Energy and Fuels},
number = 10,
volume = 34,
place = {United States},
year = {Wed Sep 23 00:00:00 EDT 2020},
month = {Wed Sep 23 00:00:00 EDT 2020}
}

Works referenced in this record:

Scale Prediction for Oil and Gas Production
journal, February 2012

  • Kan, Amy T.; Tomson, Mason B.
  • SPE Journal, Vol. 17, Issue 02
  • DOI: 10.2118/132237-PA

Scale formation and control in oil and gas fields: A review
journal, May 2016


Oilfield scale formation and chemical removal: A review
journal, December 2018

  • Kamal, Muhammad Shahzad; Hussein, Ibnelwaleed; Mahmoud, Mohamed
  • Journal of Petroleum Science and Engineering, Vol. 171
  • DOI: 10.1016/j.petrol.2018.07.037

Permeability Changes Resulting from Quartz Precipitation and Dissolution around Upper Crustal Intrusions
journal, July 2018


Evidence for SiO 2 -NaCl complexing in H 2 O-NaCl solutions at high pressure and temperature
journal, September 2015


Silica Precipitation in Fractures and the Evolution of Permeability in Hydrothermal Upflow Zones
journal, April 1993


Silica Precipitation in Acidic Solutions: Mechanism, pH Effect, and Salt Effect
journal, June 2010

  • Gorrepati, Elizabeth A.; Wongthahan, Pattanapong; Raha, Sasanka
  • Langmuir, Vol. 26, Issue 13
  • DOI: 10.1021/la904685x

Pickering Emulsions for Food Applications: Background, Trends, and Challenges
journal, April 2015


Mesoporous Silica Nanoparticles: Synthesis, Biocompatibility and Drug Delivery
journal, February 2012


Mesoporous silica nanoparticles as controlled release drug delivery and gene transfection carriers
journal, August 2008

  • Slowing, I.; Vivero-Escoto, J.; Wu, C.
  • Advanced Drug Delivery Reviews, Vol. 60, Issue 11, p. 1278-1288
  • DOI: 10.1016/j.addr.2008.03.012

Solid Nanoparticles that Catalyze Biofuel Upgrade Reactions at the Water/Oil Interface
journal, December 2009


Phase-Selective Catalysis in Emulsions Stabilized by Janus Silica-Nanoparticles
journal, October 2010

  • Faria, Jimmy; Ruiz, M. Pilar; Resasco, Daniel E.
  • Advanced Synthesis & Catalysis, Vol. 352, Issue 14-15
  • DOI: 10.1002/adsc.201000479

Silica nanoparticles as carriers of antifouling ligands for PVDF ultrafiltration membranes
journal, April 2013


Fabrication of a novel thin-film nanocomposite (TFN) membrane containing MCM-41 silica nanoparticles (NPs) for water purification
journal, December 2012


Reducing surfactant adsorption on rock by silica nanoparticles for enhanced oil recovery
journal, May 2017


Nanofluid Enhanced Oil Recovery Using Hydrophobically Associative Zwitterionic Polymer-Coated Silica Nanoparticles
journal, July 2017


Polymer-coated nanoparticles for enhanced oil recovery
journal, March 2014

  • ShamsiJazeyi, Hadi; Miller, Clarence A.; Wong, Michael S.
  • Journal of Applied Polymer Science, Vol. 131, Issue 15
  • DOI: 10.1002/app.40576

Molecular Dynamics Simulation of Nanoparticle Self-Assembly at a Liquid−Liquid Interface
journal, July 2006

  • Luo, Mingxiang; Mazyar, Oleg A.; Zhu, Qing
  • Langmuir, Vol. 22, Issue 14
  • DOI: 10.1021/la0607196

Molecular Dynamics Simulations of Surfactant Functionalized Nanoparticles in the Vicinity of an Oil/Water Interface
journal, June 2010

  • Udayana Ranatunga, R. J. K.; Kalescky, Robert J. B.; Chiu, Chi-cheng
  • The Journal of Physical Chemistry C, Vol. 114, Issue 28
  • DOI: 10.1021/jp105355y

Nanoparticle Assembly and Transport at Liquid-Liquid Interfaces
journal, January 2003


Packing, Flipping, and Buckling Transitions in Compressed Monolayers of Ellipsoidal Latex Particles
journal, June 2006

  • Basavaraj, M. G.; Fuller, G. G.; Fransaer, J.
  • Langmuir, Vol. 22, Issue 15
  • DOI: 10.1021/la060465o

Self-assembly of nanoparticles at interfaces
journal, January 2007

  • Böker, Alexander; He, Jinbo; Emrick, Todd
  • Soft Matter, Vol. 3, Issue 10
  • DOI: 10.1039/b706609k

Fabricating colloidal particles with photolithography and their interactions at an air-water interface
journal, July 2000


Adsorption of surface functionalized silica nanoparticles onto mineral surfaces and decane/water interface
journal, October 2012

  • Metin, Cigdem O.; Baran, Jimmie R.; Nguyen, Quoc P.
  • Journal of Nanoparticle Research, Vol. 14, Issue 11
  • DOI: 10.1007/s11051-012-1246-1

Emulsions stabilized by the interaction of silica nanoparticles and palmitic acid at the water–hexane interface
journal, October 2014

  • Santini, Eva; Guzmán, Eduardo; Ferrari, Michele
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 460
  • DOI: 10.1016/j.colsurfa.2014.02.054

Synergistic Interaction in Emulsions Stabilized by a Mixture of Silica Nanoparticles and Cationic Surfactant
journal, March 2007

  • Binks, Bernard P.; Rodrigues, Jhonny A.; Frith, William J.
  • Langmuir, Vol. 23, Issue 7
  • DOI: 10.1021/la0634600

Oil-in-Water Emulsions Stabilized by Highly Charged Polyelectrolyte-Grafted Silica Nanoparticles
journal, October 2005

  • Saleh, Navid; Sarbu, Traian; Sirk, Kevin
  • Langmuir, Vol. 21, Issue 22
  • DOI: 10.1021/la050654r

Hydrophilic Silica Nanoparticles at the PDMS Droplet−Water Interface
journal, April 2003

  • Simovic, Spomenka; Prestidge, Clive A.
  • Langmuir, Vol. 19, Issue 9
  • DOI: 10.1021/la026803c

Stabilization of Carbon Dioxide-in-Water Emulsions with Silica Nanoparticles
journal, September 2004

  • Dickson, Jasper L.; Binks, Bernard P.; Johnston, Keith P.
  • Langmuir, Vol. 20, Issue 19
  • DOI: 10.1021/la0488102

Size-dependent properties of silica nanoparticles for Pickering stabilization of emulsions and foams
journal, March 2016

  • Kim, Ijung; Worthen, Andrew J.; Johnston, Keith P.
  • Journal of Nanoparticle Research, Vol. 18, Issue 4
  • DOI: 10.1007/s11051-016-3395-0

Nanoparticle stabilized oil in water emulsions: A critical review
journal, April 2018

  • Arab, Danial; Kantzas, Apostolos; Bryant, Steven L.
  • Journal of Petroleum Science and Engineering, Vol. 163
  • DOI: 10.1016/j.petrol.2017.12.091

Nanoparticle silica-stabilised oil-in-water emulsions: improving emulsion stability
journal, February 2005

  • Binks, Bernard P.; Whitby, Catherine P.
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 253, Issue 1-3
  • DOI: 10.1016/j.colsurfa.2004.10.116

Enhanced Stabilization of Emulsions Due to Surfactant-Induced Nanoparticle Flocculation
journal, July 2007

  • Binks, Bernard P.; Rodrigues, Jhonny A.
  • Langmuir, Vol. 23, Issue 14
  • DOI: 10.1021/la700597k

Thermal stability of oil-in-water Pickering emulsion in the presence of nanoparticle, surfactant, and polymer
journal, February 2015

  • Sharma, Tushar; Kumar, G. Suresh; Chon, Bo Hyun
  • Journal of Industrial and Engineering Chemistry, Vol. 22
  • DOI: 10.1016/j.jiec.2014.07.026

Amphiphilic Silica Nanoparticles at the Decane−Water Interface: Insights from Atomistic Simulations
journal, May 2011

  • Fan, Heng; Resasco, Daniel E.; Striolo, Alberto
  • Langmuir, Vol. 27, Issue 9
  • DOI: 10.1021/la200428r

Functionalized Silica Nanoparticles within Multicomponent Oil/Brine Interfaces: A Study in Molecular Dynamics
journal, March 2016

  • de Lara, Lucas S.; Rigo, Vagner A.; Miranda, Caetano R.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 12
  • DOI: 10.1021/acs.jpcc.5b11225

Ultra-small-angle X-ray scattering at the Advanced Photon Source
journal, April 2009

  • Ilavsky, Jan; Jemian, Pete R.; Allen, Andrew J.
  • Journal of Applied Crystallography, Vol. 42, Issue 3
  • DOI: 10.1107/S0021889809008802

Ultra-Small-Angle X-ray Scattering Instrument at the Advanced Photon Source: History, Recent Development, and Current Status
journal, October 2012

  • Ilavsky, J.; Zhang, F.; Allen, A. J.
  • Metallurgical and Materials Transactions A, Vol. 44, Issue 1
  • DOI: 10.1007/s11661-012-1431-y

Irena : tool suite for modeling and analysis of small-angle scattering
journal, February 2009


Designing CO 2 -Responsive Multifunctional Nanoscale Fluids with Tunable Hydrogel Behavior for Subsurface Energy Recovery
journal, June 2019


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

The missing term in effective pair potentials
journal, November 1987

  • Berendsen, H. J. C.; Grigera, J. R.; Straatsma, T. P.
  • The Journal of Physical Chemistry, Vol. 91, Issue 24
  • DOI: 10.1021/j100308a038

Development and Testing of the OPLS All-Atom Force Field on Conformational Energetics and Properties of Organic Liquids
journal, January 1996

  • Jorgensen, William L.; Maxwell, David S.; Tirado-Rives, Julian
  • Journal of the American Chemical Society, Vol. 118, Issue 45
  • DOI: 10.1021/ja9621760

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


Canonical dynamics: Equilibrium phase-space distributions
journal, March 1985


Strain fluctuations and elastic constants
journal, March 1982

  • Parrinello, M.; Rahman, A.
  • The Journal of Chemical Physics, Vol. 76, Issue 5
  • DOI: 10.1063/1.443248

Particle mesh Ewald: An N ⋅log( N ) method for Ewald sums in large systems
journal, June 1993

  • Darden, Tom; York, Darrin; Pedersen, Lee
  • The Journal of Chemical Physics, Vol. 98, Issue 12
  • DOI: 10.1063/1.464397

GROMACS: High performance molecular simulations through multi-level parallelism from laptops to supercomputers
journal, September 2015


The influence of CO2 on the structure of confined asphaltenes in calcite nanopores
journal, January 2019


The role of calcite and silica interfaces on the aggregation and transport of asphaltenes in confinement
journal, January 2019


The Effect of Hydration on the Structure and Transport Properties of Confined Carbon Dioxide and Methane in Calcite Nanopores
journal, August 2018


CO2-Induced displacement and diffusive transport of shale geofluids in silica nanopores of varying sizes
journal, July 2019


Small Angle X-ray Scattering for Nanoparticle Research
journal, April 2016


Oil-Water Interface Templating of Mesoporous Macroscale Structures
journal, August 1996


Preparation of Hard Mesoporous Silica Spheres
journal, January 1997

  • Huo, Qisheng; Feng, Jianglin; Schüth, Ferdi
  • Chemistry of Materials, Vol. 9, Issue 1
  • DOI: 10.1021/cm960464p

Synthesis of Oriented Zeolite Membranes at the Interface between Two Fluid Phases
journal, August 1997

  • Tricoli, V.; Sefcik, J.; McCormick, A. V.
  • Langmuir, Vol. 13, Issue 16
  • DOI: 10.1021/la962095h

Simple Method to Produce Janus Colloidal Particles in Large Quantity
journal, November 2006

  • Hong, Liang; Jiang, Shan; Granick, Steve
  • Langmuir, Vol. 22, Issue 23
  • DOI: 10.1021/la062716z

Properties of Fatty Amine–Silica Nanoparticle Interfacial Layers at the Hexane–Water Interface
journal, January 2012

  • Whitby, Catherine P.; Fornasiero, Daniel; Ralston, John
  • The Journal of Physical Chemistry C, Vol. 116, Issue 4
  • DOI: 10.1021/jp210870v

Nanoparticle Assembly at Fluid Interfaces:  Structure and Dynamics
journal, January 2005

  • Lin, Yao; Böker, Alexander; Skaff, Habib
  • Langmuir, Vol. 21, Issue 1
  • DOI: 10.1021/la048000q

Nanoparticles Adsorbed at the Water/Oil Interface: Coverage and Composition Effects on Structure and Diffusion
journal, December 2012

  • Luu, Xuan-Cuong; Yu, Jing; Striolo, Alberto
  • Langmuir, Vol. 29, Issue 24
  • DOI: 10.1021/la304828u

Influence of Particle Wettability on the Type and Stability of Surfactant-Free Emulsions
journal, November 2000


Assembly of Nanoparticles at Liquid Interfaces: Crowding and Ordering
journal, March 2014

  • Schwenke, Konrad; Isa, Lucio; Del Gado, Emanuela
  • Langmuir, Vol. 30, Issue 11
  • DOI: 10.1021/la404254n

Nanoparticle effects on the water-oil interfacial tension
journal, November 2012


Molecular dynamics study of nanoparticles and non-ionic surfactant at an oil–water interface
journal, January 2011

  • Ranatunga, R. J. K. Udayana; Nguyen, Chuong T.; Wilson, Blake A.
  • Soft Matter, Vol. 7, Issue 15
  • DOI: 10.1039/c1sm05145h