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

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.5111521· OSTI ID:1574926

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.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1574926
Alternate ID(s):
OSTI ID: 1560761
Journal Information:
Journal of Chemical Physics, Vol. 151, Issue 10; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

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Cited By (2)

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

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