Colloidal gels exhibit time-dependent bulk properties. However, the processes and mechanisms by which aging occurs are poorly understood, which complicates the prediction of macroscopic behavior in these systems. Using a model, thermoreversible, adhesive hard sphere system consisting of octadecyl-coated silica nanoparticles dispersed in tetradecane, rheological aging is quantitatively related to structural aging. By simultaneously measuring the bulk properties and gel microstructure using rheometry and small angle neutron scattering, respectively, we show a one-to-one correspondence between the time-dependent storage modulus and the microstructure, and further, that this correspondence is independent of the gel's thermal and shear history. At the working volume fraction, the gel is homogeneous and, unlike phase-separated gels, aging behavior is not due to heterogeneous coarsening. Instead, the results presented here are consistent with homogeneous, local particle rearrangements as the mechanism of rheological aging. By establishing a quantitative and predictive relationship between the underlying microstructure and bulk mechanical properties, the results of this study may be (1) industrially relevant to products that age on commercially relevant timescales, (2) applicable to other dynamically arrested systems, such as metallic glasses, and (3) valuable in the design of new materials.
References
1.
Cipelletti
, L.
, and L.
Ramos
, “Slow dynamics in glasses, gels and foams
,” Curr. Opin. Colloid Interface Sci.
7
, 228
–234
(2002
).2.
Guo
, H. Y.
, S.
Ramakrishnan
, J. L.
Harden
, and R. L.
Leheny
, “Gel formation and aging in weakly attractive nanocolloid suspensions at intermediate concentrations
,” J. Chem. Phys.
135
, 154903
(2011
).3.
Petekidis
, G.
, “Rheology of colloidal gels
,” J. Rheol.
58
, 1085
–1087
(2014
).4.
Royall
, C. P.
, S. R.
Williams
, T.
Ohtsuka
, and H.
Tanaka
, “Direct observation of a local structural mechanism for dynamic arrest
,” Nat. Mater.
7
, 556
–561
(2008
).5.
Jabbari-Farouji
, S.
, G. H.
Wegdam
, and D.
Bonn
, “Gels and glasses in a single system: Evidence for an intricate free-energy landscape of glassy materials
,” Phys. Rev. Lett.
99
, 065701
(2007
).6.
Lacks
, D. J.
, and M. J.
Osborne
, “Energy landscape picture of overaging and rejuvenation in a sheared glass
,” Phys. Rev. Lett.
93
, 255501
(2004
).7.
Eberle
, A. P. R.
, and L.
Porcar
, “Flow-SANS and Rheo-SANS applied to soft matter
,” Curr. Opin. Colloid Interface Science
17
, 33
–43
(2012
).8.
Eberle
, A. P. R.
, N. J.
Wagner
, and R.
Castaneda-Priego
, “Dynamical Arrest Transition in Nanoparticle Dispersions with Short-Range Interactions
,” Physical Review Letters
106
, 105704
(2011
).9.
Zaccarelli
, E.
, “Colloidal gels: equilibrium and non-equilibrium routes
,” J. Phys.-Condens. Matter
19
, 323101
(2007
).10.
Vanhelden
, A. K.
, J. W.
Jansen
, and A.
Vrij
, “Preparation and characterization of spherical monodisperse silica dispersions in non-aqueous solvents
,” J. Colloid Interface Sci.
81
, 354
–368
(1981
).11.
Chen
, M.
, and W. B.
Russel
, “Characteristics of flocculated silica dispersions
,” J. Colloid Interface Sci.
141
, 564
–577
(1991
).12.
Woutersen
, A. T. J. M.
, and C. G.
Dekruif
, “The rheology of adhesive hard-sphere dispersions
,” J. Chem. Phys.
94
, 5739
–5750
(1991
).13.
Grant
, M. C.
, and W. B.
Russel
, “Volume-fraction dependence of elastic-moduli and transition-temperatures for colloidal silica-gels
,” Phys. Rev. E
47
, 2606
–2614
(1993
).14.
Rueb
, C. J.
, and C. F.
Zukoski
, “Viscoelastic properties of colloidal gels
,” J. Rheol.
41
, 197
–218
(1997
).15.
Rueb
, C. J.
, and C. F.
Zukoski
, “Rheology of suspensions of weakly attractive particles: Approach to gelation
,” J. Rheol.
42
, 1451
–1476
(1998
).16.
Rouw
, P. W.
, and C. G.
Dekruif
, “Adhesive hard-sphere colloidal dispersions. 1. Diffusion-coefficient as a function of well depth
,” J. Chem. Phys.
88
, 7799
–7806
(1988
).17.
Eberle
, A. P. R.
, R.
Castaneda-Priego
, J. M.
Kim
, and N. J.
Wagner
, “Dynamical arrest, percolation, gelation, and glass formation in model nanoparticle dispersions with thermoreversible adhesive interactions
,” Langmuir
28
, 1866
–1878
(2012
).18.
Kim
, J. M.
, A. P. R.
Eberle
, A. K.
Gurnon
, L.
Porcar
, and N. J.
Wagner
, “The microstructure and rheology of a model, thixotropic nanoparticle gel under steady shear and large amplitude oscillatory shear (LAOS)
,” J. Rheol.
58
, 1301
–1328
(2014
).19.
Ramakrishnan
, S.
, and C. F.
Zukoski
, “Microstructure and rheology of thermoreversible nanoparticle gels
,” Langmuir
22
, 7833
–7842
(2006
).20.
Solomon
, M. J.
, and P.
Varadan
, “Dynamic structure of thermoreversible colloidal gels of adhesive spheres
,” Phys. Rev. E
63
, 051402
(2001
).21.
Eberle
, A. P. R.
, N. J.
Wagner
, B.
Akgun
, and S. K.
Satija
, “Temperature-dependent nanostructure of an end-tethered octadecane brush in tetradecane and nanoparticle phase behavior
,” Langmuir
26
, 3003
–3007
(2010
).22.
Negi
, A. S.
, C. G.
Redmon
, S.
Ramakrishnan
, and C. O.
Osuji
, “Viscoelasticity of a colloidal gel during dynamical arrest: Evolution through the critical gel and comparison with a soft colloidal glass
,” J. Rheol.
58
, 1557
–1579
(2014
).23.
Asakura
, S.
, and F.
Oosawa
, “Interaction between particles suspended in solutions of macromolecules
,” J. Polym. Sci.
33
, 183
–192
(1958
).24.
Poon
, W. C. K.
, L.
Starrs
, S. P.
Meeker
, A.
Moussaid
, Evans
, R. M. L.
, P. N.
Pusey
, and M. M.
Robins
, “Delayed sedimentation of transient gels in colloid-polymer mixtures: dark-field observation, rheology and dynamic light scattering studies
,” Faraday Discuss.
112
, 143
–154
(1999
).25.
Buscall
, R.
, T. H.
Choudhury
, M. A.
Faers
, J. W.
Goodwin
, P. A.
Luckham
, and S. J.
Partridge
, “Towards rationalising collapse times for the delayed sedimentation of weakly-aggregated colloidal gels
,” Soft Matter
5
, 1345
–1349
(2009
).26.
Lu
, P. J.
, E.
Zaccarelli
, F.
Ciulla
, A. B.
Schofield
, F.
Sciortino
, and D. A.
Weitz
, “Gelation of particles with short-range attraction
,” Nature
453
, 499
-U4
(2008
).27.
Zia
, R. N.
, B. J.
Landrum
, and W. B.
Russel
, “A micro-mechanical study of coarsening and rheology of colloidal gels: Cage building, cage hopping, and Smoluchowski's ratchet
,” J. Rheol.
58
, 1121
–1157
(2014
).28.
Verhaegh
, N. A. M.
, D.
Asnaghi
, H. N. W.
Lekkerkerker
, M.
Giglio
, and L.
Cipelletti
, “Transient gelation by spinodal decomposition in colloid-polymer mixtures
,” Physica A
242
, 104
–118
(1997
).29.
Zhang
, I.
, C. P.
Royall
, M. A.
Faers
, and P.
Bartlett
, “Phase separation dynamics in colloid-polymer mixtures: the effect of interaction range
,” Soft Matter
9
, 2076
–2084
(2013
).30.
Koumakis
, N.
, E.
Moghimi
, R.
Besseling
, W. C. K.
Poon
, J. F.
Brady
, and G.
Petekidis
, “Tuning colloidal gels by shear
,” Soft Matter
11
, 4640
–4648
(2015
).31.
Kim
, J. M.
, J.
Fang
, A. P. R.
Eberle
, R.
Castaneda-Priego
, and N. J.
Wagner
, “Gel transition in adhesive hard-sphere colloidal dispersions: The role of gravitational effects
,” Phys. Rev. Lett.
110
, 208302
(2013
).32.
Teece
, L. J.
, M. A.
Faers
, and P.
Bartlett
, “Ageing and collapse in gels with long-range attractions
,” Soft Matter
7
, 1341
–1351
(2011
).33.
Dymond
, J. H.
, and H. A.
Oye
, “Viscosity of selected liquid N-alkanes
,” J. Phys. Chem. Ref. Data
23
, 41
–53
(1994
).34.
Porcar
, L.
, D.
Pozzo
, G.
Langenbucher
, J.
Moyer
, and P. D.
Butler
, “Rheo-small-angle neutron scattering at the National Institute of Standards and Technology Center for Neutron Research
,” Rev. Sci. Instrum.
82
, 083902
(2011
).35.
Kline
, S. R.
, “Reduction and analysis of SANS and USANS data using IGOR Pro
,” J. Appl. Crystallogr.
39
, 895
–900
(2006
).36.
Winter
, H. H.
, and F.
Chambon
, “Analysis of linear viscoelasticity of a cross-linking polymer at the gel point
,” J. Rheol.
30
, 367
–382
(1986
).37.
Valadez-Perez
, N. E.
, Y.
Liu
, A. P. R.
Eberle
, N. J.
Wagner
, and R.
Castaneda-Priego
, “Dynamical arrest in adhesive hard-sphere dispersions driven by rigidity percolation
,” Phys. Rev. E
88
, 060302
(2013
).38.
Pusey
, P. N.
, and W.
Vanmegen
, “Observation of a glass-transition in suspensions of spherical colloidal particles
,” Phys. Rev. Lett.
59
, 2083
–2086
(1987
).39.
Mason
, T. G.
, and D. A.
Weitz
, “Linear viscoelasticity of colloidal hard-sphere suspensions near the glass-transition
,” Phys. Rev. Lett.
75
, 2770
–2773
(1995
).40.
Helgeson
, M. E.
, N. J.
Wagner
, and D.
Vlassopoulos
, “Viscoelasticity and shear melting of colloidal star polymer glasses
,” J. Rheol.
51
, 297
–316
(2007
).41.
Gotze
, W.
, and L.
Sjogren
, “Beta-relaxation at the glass-transition of hard-spherical colloids
,” Phys. Rev. A
43
, 5442
–5448
(1991
).42.
Baravian
, C.
, and D.
Quemada
, “Using instrumental inertia in controlled stress rheometry
,” Rheol. Acta
37
, 223
–233
(1998
).43.
McKenna
, G. B.
, T.
Narita
, and F.
Lequeux
, “Soft colloidal matter: A phenomenological comparison of the aging and mechanical responses with those of molecular glasses
,” J. Rheol.
53
, 489
–516
(2009
).44.
Kovacs
, A. J.
, R. A.
Stratton
, and J. D.
Ferry
, “Dynamic mechanical properties of polyvinyl acetate in shear in glass transition temperature range
,” J. Phys. Chem.
67
, 152
–161
(1963
).45.
Chen
, Y. L.
, and K. S.
Schweizer
, “Microscopic theory of gelation and elasticity in polymer-particle suspensions
,” J. Chem. Phys.
120
, 7212
–7222
(2004
).46.
Ramakrishnan
, S.
, Y. L.
Chen
, K. S.
Schweizer
, and C. F.
Zukoski
, “Elasticity and clustering in concentrated depletion gels
,” Phys. Rev. E
70
, 040401(R)
(2004
).47.
Eberle
, A. P. R.
, N.
Martys
, L.
Porcar
, S. R.
Kline
, W. L.
George
, J. M.
Kim
, P. D.
Butler
, and N. J.
Wagner
, “Shear viscosity and structural scalings in model adhesive hard-sphere gels
,” Phys. Rev. E
89
, 050302
(2014
).48.
Peng
, X. G.
, and G. B.
McKenna
, “Comparison of the physical aging behavior of a colloidal glass after shear melting and concentration jumps
,” Phys. Rev. E
90
, 050301
(2014
).49.
Siebenburger
, M.
, M.
Ballauff
, and T.
Voigtmann
, “Creep in colloidal glasses
,” Phys. Rev. Lett.
108
, 255701
(2012
).50.
Giordano
, V. M.
, and B.
Ruta
, “Unveiling the structural arrangements responsible for the atomic dynamics in metallic glasses during physical aging
,” Nat. Commun.
7
, 10344
(2016
).51.
Leunissen
, M. E.
, C. G.
Christova
, A. P.
Hynninen
, C. P.
Royall
, A. I.
Campbell
, A.
Imhof
, M.
Dijkstra
, R.
van Roij
, and A.
van Blaaderen
, “Ionic colloidal crystals of oppositely charged particles
,” Nature
437
, 235
–240
(2005
).52.
Yethiraj
, A.
, and A.
van Blaaderen
, “A colloidal model system with an interaction tunable from hard sphere to soft and dipolar
,” Nature
421
, 513
–517
(2003
).© 2016 The Society of Rheology.
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