Dissertation / PhD Thesis FZJ-2014-00831

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Transport and deposition of functionalized multi-walled carbon nanotubes in porous media



2013
Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag Jülich
ISBN: 978-3-89336-929-4

Jülich : Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag, Schriften des Forschungszentrums Jülich Reihe Energie & Umwelt / Energy & Environment 201, VI, 103 S. () = RWTH Aachen, Diss., 2013

Abstract: The aim of this study was to gain more profound knowledge on the transport anddeposition of functionalized multi-walled carbon nanotubes (MWCNTs) in porous media. The use of $^{14}$C-labeled MWCNTs allowed investigations into very low concentrations and the determination of retention profiles. Transmission electron micrographs revealed that the MWCNTs exhibited average outer diameters of 10–50 nm and average lengths of up to several $\mu$m. The functionalization of the MWCNTs with nitric acid induced oxygen containing functional groups and reduced the amount of metal catalysts on the nanotubes. Since nanoparticles do not behave like solutes but rather like colloids, the applicability of the available experimental setups and procedures was evaluated for carbon nanotubes. The nanoparticles could not be injected using a sample loop or an irrigation head. Therefore,the MWCNTs were applied to the columns directly by a pump or a pipette, respectively. The effect of the input concentration (C$_{o}$) and sand grain size on the transport andretention of MWCNTs was investigated in water-saturated sand columns at conditions unfavorable for attachment (repulsive electrostatic forces). These experiments were performed at very low C$_{o}$ (0.005–1 mg L$^{-1}$), low ionic strength (1 mM KCl), and high flowrate (0.64 cm min$^{-1}$). The breakthrough curves (BTCs) for MWCNTs typically did notreach a plateau, but exhibited an asymmetric shape that slowly increased during breakthrough. The retention profiles (RPs) exhibited a hyper-exponential shape with greater retention near the column inlet. The collected BTCs and RPs were simulated using a numerical model within the HYDRUS-1D code that accounted for both time- and depth-dependent blocking functions on the retention coefficient. For a given C$_{o}$, the depth-dependent retention coefficient and the maximum solid phase concentration of MWCNTs were both found to increase with decreasing grain size. These trends reflect greater MWCNTs retention rates and a greater number of retention locations in the finer textured sand. The normalized concentration of MWCNTs in the effluent increased and the RPsbecame less hyper-exponential with higher Co due to enhanced blocking/filling of retention locations. This concentration dependency of MWCNT transport increased with smaller grain size because of the effect of pore structure and the shape of MWCNTs on their retention. In particular, MWCNTs have a high aspect ratio, and it was hypothesized that MWCNTs may create a porous network with an enhanced ability to retain further MWCNTs, especially in smaller grain-sized sand and at higher C$_{o}$. Results demonstrate that model simulations should accurately account for observed behavior of both BTCs andRPs to make reliable predictions on MWCNT transport.

Keyword(s): Dissertation


Note: RWTH Aachen, Diss., 2013

Contributing Institute(s):
  1. Agrosphäre (IBG-3)
Research Program(s):
  1. 245 - Chemicals in the Environment (POF2-245) (POF2-245)

Appears in the scientific report 2013
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 Record created 2014-01-27, last modified 2021-01-29


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