Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Evolution of structure and dynamics of thermo-reversible nanoparticle gels—A combined XPCS and rheology study

Abstract

A combined X-ray photon correlation spectroscopy and rheology report is carried out to capture the evolution of structure, fast particle-scale dynamics, and moduli (elastic and loss) at early times of gel formation near the fluid-gel boundary of a suspension of nanoparticles. The system is made up of moderately concentrated suspensions of octadecyl silica in decalin (φ = 0.2) undergoing thermoreversible gelation. Near the gel boundary, the rate of gel formation is very sensitive to changes in attraction strength. Yet, we find that at different attraction strengths, the system goes through identical intermediate states of microscopic and macroscopic behavior, even though the absolute time needed to form a gel varies by orders of magnitude. We identify a single dimensionless time parameter, tw/tg, where tw is the wait time following the quench and tg is the rheologically determined gel time, that captures the similarity in gel formation at a range of attraction strengths. Following a temperature quench below the gel boundary, the system is initially fluidlike and forms diffusive clusters (similar to 8.5 times the particle diameter). After a lag-time, tL, clusters aggregate to form a network like structure which is characterized by the onset of mechanical rigidity and a rapid growthmore » in microscopic relaxation times. At tg, the Baxter parameter obtained from adhesive hard sphere fits of the structure factor attains a constant value corresponding to the theoretical percolation boundary, thus demonstrating that gelation is percolation driven.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2];  [3];  [3];  [4];  [3];  [2];  [3];  [5];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Florida A & M Univ.-Florida State Univ. (FAMU-FSU), Tallahassee, FL (United States). College of Engineering
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. AGH Univ. of Science and Technology, Krakow (Poland)
  4. Johns Hopkins Univ., Baltimore, MD (United States)
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1574926
Alternate Identifier(s):
OSTI ID: 1560761
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 10; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Bahadur, Divya, Zhang, Qingteng, Dufresne, Eric M., Grybos, Pawel, Kmon, Piotr, Leheny, Robert L., Maj, Piotr, Narayanan, Suresh, Szczygiel, Robert, Swan, James W., Sandy, Alec, and Ramakrishnan, Subramanian. Evolution of structure and dynamics of thermo-reversible nanoparticle gels—A combined XPCS and rheology study. United States: N. p., 2019. Web. doi:10.1063/1.5111521.
Copy to clipboard
Bahadur, Divya, Zhang, Qingteng, Dufresne, Eric M., Grybos, Pawel, Kmon, Piotr, Leheny, Robert L., Maj, Piotr, Narayanan, Suresh, Szczygiel, Robert, Swan, James W., Sandy, Alec, & Ramakrishnan, Subramanian. Evolution of structure and dynamics of thermo-reversible nanoparticle gels—A combined XPCS and rheology study. United States. https://doi.org/10.1063/1.5111521
Copy to clipboard
Bahadur, Divya, Zhang, Qingteng, Dufresne, Eric M., Grybos, Pawel, Kmon, Piotr, Leheny, Robert L., Maj, Piotr, Narayanan, Suresh, Szczygiel, Robert, Swan, James W., Sandy, Alec, and Ramakrishnan, Subramanian. Mon . "Evolution of structure and dynamics of thermo-reversible nanoparticle gels—A combined XPCS and rheology study". United States. https://doi.org/10.1063/1.5111521. https://www.osti.gov/servlets/purl/1574926.
Copy to clipboard
@article{osti_1574926,
title = {Evolution of structure and dynamics of thermo-reversible nanoparticle gels—A combined XPCS and rheology study},
author = {Bahadur, Divya and Zhang, Qingteng and Dufresne, Eric M. and Grybos, Pawel and Kmon, Piotr and Leheny, Robert L. and Maj, Piotr and Narayanan, Suresh and Szczygiel, Robert and Swan, James W. and Sandy, Alec and Ramakrishnan, Subramanian},
abstractNote = {A combined X-ray photon correlation spectroscopy and rheology report is carried out to capture the evolution of structure, fast particle-scale dynamics, and moduli (elastic and loss) at early times of gel formation near the fluid-gel boundary of a suspension of nanoparticles. The system is made up of moderately concentrated suspensions of octadecyl silica in decalin (φ = 0.2) undergoing thermoreversible gelation. Near the gel boundary, the rate of gel formation is very sensitive to changes in attraction strength. Yet, we find that at different attraction strengths, the system goes through identical intermediate states of microscopic and macroscopic behavior, even though the absolute time needed to form a gel varies by orders of magnitude. We identify a single dimensionless time parameter, tw/tg, where tw is the wait time following the quench and tg is the rheologically determined gel time, that captures the similarity in gel formation at a range of attraction strengths. Following a temperature quench below the gel boundary, the system is initially fluidlike and forms diffusive clusters (similar to 8.5 times the particle diameter). After a lag-time, tL, clusters aggregate to form a network like structure which is characterized by the onset of mechanical rigidity and a rapid growth in microscopic relaxation times. At tg, the Baxter parameter obtained from adhesive hard sphere fits of the structure factor attains a constant value corresponding to the theoretical percolation boundary, thus demonstrating that gelation is percolation driven.},
doi = {10.1063/1.5111521},
journal = {Journal of Chemical Physics},
number = 10,
volume = 151,
place = {United States},
year = {Mon Sep 09 00:00:00 EDT 2019},
month = {Mon Sep 09 00:00:00 EDT 2019}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.5111521
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Dynamical arrest in dense short-ranged attractive colloids
journal, September 2004

Controlled growth of monodisperse silica spheres in the micron size range
journal, January 1968

  • Stöber, Werner; Fink, Arthur; Bohn, Ernst
  • Journal of Colloid and Interface Science, Vol. 26, Issue 1, p. 62-69
  • DOI: 10.1016/0021-9797(68)90272-5

A micro-mechanical study of coarsening and rheology of colloidal gels: Cage building, cage hopping, and Smoluchowski's ratchet
journal, September 2014

  • Zia, Roseanna N.; Landrum, Benjamin J.; Russel, William B.
  • Journal of Rheology, Vol. 58, Issue 5
  • DOI: 10.1122/1.4892115

Role of shear-induced dynamical heterogeneity in the nonlinear rheology of colloidal gels
journal, January 2014

  • Hsiao, Lilian C.; Kang, Heekyoung; Ahn, Kyung Hyun
  • Soft Matter, Vol. 10, Issue 46
  • DOI: 10.1039/c4sm01375a

Microstructural regimes of colloidal rod suspensions, gels, and glasses
journal, January 2010

  • Solomon, Michael J.; Spicer, Patrick T.
  • Soft Matter, Vol. 6, Issue 7
  • DOI: 10.1039/b918281k

Structure and dynamics of colloidal depletion gels: Coincidence of transitions and heterogeneity
journal, October 2006

Extended corresponding-states behavior for particles with variable range attractions
journal, August 2000

  • Noro, Massimo G.; Frenkel, Daan
  • The Journal of Chemical Physics, Vol. 113, Issue 8
  • DOI: 10.1063/1.1288684

Viscoelasticity of a colloidal gel during dynamical arrest: Evolution through the critical gel and comparison with a soft colloidal glass
journal, September 2014

  • Negi, Ajay Singh; Redmon, Carissa G.; Ramakrishnan, Subramanian
  • Journal of Rheology, Vol. 58, Issue 5
  • DOI: 10.1122/1.4883675

Preparation and characterization of spherical monodisperse silica dispersions in nonaqueous solvents
journal, June 1981

Multiple Glassy States in a Simple Model System
journal, April 2002

Characterizing nanoparticle interactions: Linking models to experiments
journal, July 2000

  • Ramakrishnan, S.; Zukoski, C. F.
  • The Journal of Chemical Physics, Vol. 113, Issue 3
  • DOI: 10.1063/1.481901

Aging in short-ranged attractive colloids: A numerical study
journal, May 2004

  • Foffi, G.; Zaccarelli, E.; Buldyrev, S.
  • The Journal of Chemical Physics, Vol. 120, Issue 18
  • DOI: 10.1063/1.1695326

Gelation as arrested phase separation in short-ranged attractive colloid–polymer mixtures
journal, November 2008

Structural origins of dynamical heterogeneity in colloidal gels
journal, May 2008

Simulation Method of Colloidal Suspensions with Hydrodynamic Interactions: Fluid Particle Dynamics
journal, August 2000

Clustering and Mechanics in Dense Depletion and Thermal Gels †
journal, October 2005

  • Ramakrishnan, S.; Gopalakrishnan, V.; Zukoski, C. F.
  • Langmuir, Vol. 21, Issue 22
  • DOI: 10.1021/la050830w

The effect of attractions on the local structure of liquids and colloidal fluids
journal, December 2010

  • Taffs, Jade; Malins, Alex; Williams, Stephen R.
  • The Journal of Chemical Physics, Vol. 133, Issue 24
  • DOI: 10.1063/1.3516210

Quantifying the Reversible Association of Thermosensitive Nanoparticles
journal, October 2011

Gel Transition in Adhesive Hard-Sphere Colloidal Dispersions: The Role of Gravitational Effects
journal, May 2013

Elasticity and clustering in concentrated depletion gels
journal, October 2004

32k Channel Readout IC for Single Photon Counting Pixel Detectors with Pitch, Dead Time of 85 ns, Offset Spread and 2% rms Gain Spread
journal, April 2016

Preparation of monodisperse silica particles: Control of size and mass fraction
journal, August 1988

  • Bogush, G. H.; Tracy, M. A.; Zukoski, C. F.
  • Journal of Non-Crystalline Solids, Vol. 104, Issue 1, p. 95-106
  • DOI: 10.1016/0022-3093(88)90187-1

On the solid–fluid interface of adhesive spheres
journal, August 1993

  • Marr, D. W.; Gast, A. P.
  • The Journal of Chemical Physics, Vol. 99, Issue 3
  • DOI: 10.1063/1.465265

Phase separation dynamics in colloid–polymer mixtures: the effect of interaction range
journal, January 2013

  • Zhang, Isla; Royall, C. Patrick; Faers, Malcolm A.
  • Soft Matter, Vol. 9, Issue 6
  • DOI: 10.1039/c2sm27119b

Length scale dependence of dynamical heterogeneity in a colloidal fractal gel
journal, December 2006

Dynamic structure of thermoreversible colloidal gels of adhesive spheres
journal, April 2001

Dynamical heterogeneities close to a colloidal gel
journal, January 2004

  • Puertas, Antonio M.; Fuchs, Matthias; Cates, Michael E.
  • The Journal of Chemical Physics, Vol. 121, Issue 6
  • DOI: 10.1063/1.1768936

Decay of density fluctuations in gels
journal, January 1991

Structural and rheological evolution of silica nanoparticle gels
journal, January 2010

  • Cao, X. J.; Cummins, H. Z.; Morris, J. F.
  • Soft Matter, Vol. 6, Issue 21
  • DOI: 10.1039/c0sm00433b

Structural and microscopic relaxations in a colloidal glass
journal, January 2015

  • Augusto de Melo Marques, Flavio; Angelini, Roberta; Zaccarelli, Emanuela
  • Soft Matter, Vol. 11, Issue 3
  • DOI: 10.1039/c4sm02010c

Structure of colloidal gels at intermediate concentrations: the role of competing interactions
journal, January 2016

  • Capellmann, Ronja F.; Valadez-Pérez, Néstor E.; Simon, Benedikt
  • Soft Matter, Vol. 12, Issue 46
  • DOI: 10.1039/c6sm01822j

Gelation of particles with short-range attraction
journal, May 2008

  • Lu, Peter J.; Zaccarelli, Emanuela; Ciulla, Fabio
  • Nature, Vol. 453, Issue 7194
  • DOI: 10.1038/nature06931

Ultralow-angle dynamic light scattering with a charge coupled device camera based multispeckle, multitau correlator
journal, August 1999

  • Cipelletti, Luca; Weitz, D. A.
  • Review of Scientific Instruments, Vol. 70, Issue 8
  • DOI: 10.1063/1.1149894

Phase diagram of the adhesive hard sphere fluid
journal, January 2004

  • Miller, Mark A.; Frenkel, Daan
  • The Journal of Chemical Physics, Vol. 121, Issue 1
  • DOI: 10.1063/1.1758693

Critical exponents for the sol-gel transition
journal, August 1987

Role of isostaticity and load-bearing microstructure in the elasticity of yielded colloidal gels
journal, September 2012

  • Hsiao, L. C.; Newman, R. S.; Glotzer, S. C.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 40
  • DOI: 10.1073/pnas.1206742109

Hydrodynamic and interparticle potential effects on aggregation of colloidal particles
journal, February 2012

  • Cao, X. J.; Cummins, H. Z.; Morris, J. F.
  • Journal of Colloid and Interface Science, Vol. 368, Issue 1
  • DOI: 10.1016/j.jcis.2011.11.050

Interplay between Spinodal Decomposition and Glass Formation in Proteins Exhibiting Short-Range Attractions
journal, September 2007

Design and characterization of an undulator beamline optimized for small-angle coherent X-ray scattering at the Advanced Photon Source
journal, November 1999

  • Sandy, A. R.; Lurio, L. B.; Mochrie, S. G. J.
  • Journal of Synchrotron Radiation, Vol. 6, Issue 6
  • DOI: 10.1107/s0909049599009590

On the viscosity of adhesive hard sphere dispersions: Critical scaling and the role of rigid contacts
journal, March 2019

  • Wang, Gang; Fiore, Andrew M.; Swan, James W.
  • Journal of Rheology, Vol. 63, Issue 2
  • DOI: 10.1122/1.5063362

Gel formation and aging in weakly attractive nanocolloid suspensions at intermediate concentrations
journal, October 2011

  • Guo, Hongyu; Ramakrishnan, S.; Harden, James L.
  • The Journal of Chemical Physics, Vol. 135, Issue 15
  • DOI: 10.1063/1.3653380

Percolation behaviour of permeable and of adhesive spheres
journal, August 1983

Connecting nanoscale motion and rheology of gel-forming colloidal suspensions
journal, May 2010

Colloidal gelation with variable attraction energy
journal, March 2013

  • Zaccone, Alessio; Crassous, Jérôme J.; Ballauff, Matthias
  • The Journal of Chemical Physics, Vol. 138, Issue 10
  • DOI: 10.1063/1.4794695

Entropic barriers, activated hopping, and the glass transition in colloidal suspensions
journal, July 2003

  • Schweizer, Kenneth S.; Saltzman, Erica J.
  • The Journal of Chemical Physics, Vol. 119, Issue 2
  • DOI: 10.1063/1.1578632

Colloidal glasses and gels: The interplay of bonding and caging
journal, August 2009

  • Zaccarelli, E.; Poon, W. C. K.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 36
  • DOI: 10.1073/pnas.0902294106

Noise on photon correlation data: I. Auto-correlation
journal, December 1990

  • Schätzel, Klaus
  • Quantum Optics: Journal of the European Optical Society Part B, Vol. 2, Issue 6
  • DOI: 10.1088/0954-8998/2/6/505

Linking self-assembly, rheology, and gel transition in attractive colloids
journal, September 2014

  • Zaccone, A.; Winter, H. H.; Siebenbürger, M.
  • Journal of Rheology, Vol. 58, Issue 5
  • DOI: 10.1122/1.4878838

Microstructure and Rheology of Thermoreversible Nanoparticle Gels
journal, August 2006

  • Ramakrishnan, S.; Zukoski, C. F.
  • Langmuir, Vol. 22, Issue 18
  • DOI: 10.1021/la060168j

Dynamical Arrest Transition in Nanoparticle Dispersions with Short-Range Interactions
journal, March 2011

Higher-order glass-transition singularities in colloidal systems with attractive interactions
journal, December 2000

Viscoelastic properties of colloidal gels
journal, March 1997

  • Rueb, C. J.; Zukoski, C. F.
  • Journal of Rheology, Vol. 41, Issue 2
  • DOI: 10.1122/1.550812

Nonergodicity transitions in colloidal suspensions with attractive interactions
journal, May 1999

Fast multi-tau real-time software correlator for dynamic light scattering
journal, January 2001

Microscopic theory of gelation and elasticity in polymer–particle suspensions
journal, April 2004

  • Chen, Yeng-Long; Schweizer, Kenneth S.
  • The Journal of Chemical Physics, Vol. 120, Issue 15
  • DOI: 10.1063/1.1683077

Arrested demixing opens route to bigels
journal, November 2012

  • Varrato, F.; Di Michele, L.; Belushkin, M.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 47
  • DOI: 10.1073/pnas.1214971109

Dynamical arrest in adhesive hard-sphere dispersions driven by rigidity percolation
journal, December 2013

Direct observation of a local structural mechanism for dynamic arrest
journal, June 2008

  • Patrick Royall, C.; Williams, Stephen R.; Ohtsuka, Takehiro
  • Nature Materials, Vol. 7, Issue 7
  • DOI: 10.1038/nmat2219

Attractions in sterically stabilized silica dispersions
journal, December 1986

Dynamical Arrest, Percolation, Gelation, and Glass Formation in Model Nanoparticle Dispersions with Thermoreversible Adhesive Interactions
journal, January 2012

  • Eberle, Aaron P. R.; Castañeda-Priego, Ramón; Kim, Jung M.
  • Langmuir, Vol. 28, Issue 3
  • DOI: 10.1021/la2035054

Submillisecond X-ray photon correlation spectroscopy from a pixel array detector with fast dual gating and no readout dead-time
journal, April 2016

  • Zhang, Qingteng; Dufresne, Eric M.; Grybos, Pawel
  • Journal of Synchrotron Radiation, Vol. 23, Issue 3
  • DOI: 10.1107/s1600577516005166

The rheology and microstructure of an aging thermoreversible colloidal gel
journal, January 2017

  • Gordon, Melissa B.; Kloxin, Christopher J.; Wagner, Norman J.
  • Journal of Rheology, Vol. 61, Issue 1
  • DOI: 10.1122/1.4966039

Phase Diagram of a Model Adhesive Hard-Sphere Dispersion
journal, June 1995

  • Verduin, Henk; Dhont, Jan K. G.
  • Journal of Colloid and Interface Science, Vol. 172, Issue 2
  • DOI: 10.1006/jcis.1995.1273

Dynamics of concentrated colloidal suspensions: diffusion, aggregation and gelation
journal, May 2001

  • Romer, S.; Urban, C.; Bissig, H.
  • Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 359, Issue 1782
  • DOI: 10.1098/rsta.2000.0812

Linear viscoelasticity of attractive colloidal dispersions
journal, September 2015

  • Varga, Zsigmond; Swan, James W.
  • Journal of Rheology, Vol. 59, Issue 5
  • DOI: 10.1122/1.4928951

The vibrational motions of particle gels
journal, July 2001

  • Dawson, K.; Foffi, G.; Zaccarelli, E.
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 183-185
  • DOI: 10.1016/s0927-7757(01)00528-3

Gel transitions in colloidal suspensions
journal, December 1999

Attractions in sterically stabilized silica dispersions
journal, December 1986

Attractions in sterically stabilized silica dispersions
journal, December 1986

Attractions in sterically stabilized silica dispersions
journal, December 1986

How a liquid becomes a glass both on cooling and on heating
text, January 2007

Gelation as arrested phase separation in short-ranged attractive colloid-polymer mixtures
text, January 2008

The effect of attractions on the local structure of liquids and colloidal fluids
text, January 2011

Colloidal gelation with variable attraction energy
text, January 2013

Aging in short-ranged attractive colloids: A numerical study
text, January 2003

Dynamical heterogeneities close to a colloidal gel
text, January 2004

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Anisotropic and heterogeneous dynamics in an aging colloidal gel
    journal, January 2020

    • Jain, Avni; Schulz, Florian; Lokteva, Irina
    • Soft Matter, Vol. 16, Issue 11
    • DOI: 10.1039/c9sm02230a

    Anisotropic and heterogeneous dynamics in an aging colloidal gel
    text, January 2020

    • Jain, Avni; Schulz, Florian; Lokteva, Irina
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2020-01104
      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: