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@PHDTHESIS{Liang:153727,
author = {Liang, Yan},
title = {{T}ransport and {R}etention of {S}tabilized {S}ilver
{N}anoparticles in {P}orous {M}edia},
volume = {212},
school = {RWTH Aachen},
type = {Dissertation},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2014-03223},
isbn = {978-3-89336-957-7},
series = {Schriften des Forschungszentrums Jülich Reihe Energie $\&$
Umwelt / Energy $\&$ Environment},
pages = {IV, 109 S.},
year = {2014},
note = {Dissertation, RWTH Aachen, 2014},
abstract = {Due to the widespread application of silver nanoparticles
(AgNPs) and the resulting potential exposure in the
environment, information about their environmental transport
and fate is essential for risk assessment. AgNPs are
commonly modified with functional groups, surfactants, or
polymers to increase their stability in liquids and the
surface modification greatly influences the environmental
behavior of AgNPs. The aim of this study is therefore to
investigate the transport and retention of
surfactant-stabilized AgNPs under environmentally relevant
conditions. Experiments were conducted with water-saturated
columns packed with quartz sand, around $90\%$
water-saturated columns filled with undisturbed loamy sand
soil, and a lysimeter. Inductively coupled plasma-mass
spectrometry/optical emission spectrometry (ICP-MS/OES) was
used to analyze the concentrations of AgNPs, Ca$^{2+}$ , K+,
Fe, and Al. The experimental breakthrough curves (BTCs) and
retention profiles (RPs) from column experiments were
described using a numerical model that considers time- and
depth-dependent retention. Column experiments with quartz
sand packing were also conducted in the presence of
surfactant to deduce the influence of surfactant on AgNP
transport, especially on the spatial distribution of
retained AgNPs that determines the long-term transport
potential. In addition, to better understand the
interactions of AgNPs and the matrix in the environment,
remobilization of retained AgNPs from undisturbed soil was
studied by changing the solution chemistry such as change of
cation types and ionic strength reduction. Experimental
results showed that the normalized concentration in BTCs for
AgNPs obtained from water-saturated columns increased with a
decrease in solution ionic strength (IS), and an increase in
flow velocity ($\textit{q}$), sand grain size, and input
concentration (C$_{o}$). In contrast to the conventional
filtration theory, RPs in sand exhibited uniform,
nonmonotonic, or hyperexponential shapes that were sensitive
to physicochemical conditions. The simulated retention rate
coefficient (k$_{1}$) and maximum retained concentration on
the solid phase (S$_{max}$) increased with IS and as the
grain size and/or C$_{o}$ decreased. The RPs were more
hyperexponential in finer textured sand and at lower C$_{o}$
because of their higher values of S$_{max}$, which indicated
a larger retention capacity of the porous media. Conversely,
RPs were nonmonotonic or uniform at higher C$_{o}$ and in
coarser sand that had lower values of S$_{max}$, and tended
to exhibit higher peak concentrations in the RPs at lower
flow velocities and at higher solution IS. These
observations indicate that uniform and nonmonotonic RPs
occurred under conditions when S$_{max}$ was filled. The
sensitivity of the nonmonotonic RPs to IS and flow velocity
in coarser textured sand indicates that AgNPs were partially
interacting in a secondary energy minimum according to the
Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. However,
elimination of the secondary minimum only produced recovery
of a small portion (<10\%) of the retained AgNPs. These
results imply that AgNPs were largely irreversibly
interacting in a primary minimum associated with microscopic
heterogeneity of the porous [...]},
keywords = {Dissertation (GND)},
cin = {IBG-3},
cid = {I:(DE-Juel1)IBG-3-20101118},
pnm = {246 - Modelling and Monitoring Terrestrial Systems: Methods
and Technologies (POF2-246) / 255 - Terrestrial Systems:
From Observation to Prediction (POF3-255)},
pid = {G:(DE-HGF)POF2-246 / G:(DE-HGF)POF3-255},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
url = {https://juser.fz-juelich.de/record/153727},
}