Transport and retention of multi-walled carbon nanotubes in saturated porous media: Effects of input concentration and grain size Daniela Kasel a, *, Scott A. Bradford b , Ji rı´ Sim unek c , Marc Heggen d,e , Harry Vereecken a , Erwin Klumpp a a Agrosphere Institute (IBG-3), Forschungszentrum Ju ¨ lich GmbH, 52425 Ju ¨ lich, Germany b US Salinity Laboratory, Agricultural Research Service, United States Department of Agriculture, Riverside, CA 92507, USA c Department of Environmental Sciences, University of California Riverside, Riverside, CA 92521, USA d Peter Gru ¨ nberg Institute (PGI-5), Forschungszentrum Ju ¨ lich GmbH, 52425 Ju ¨ lich, Germany e Ernst Ruska-Centre (ER-C), Forschungszentrum Ju ¨ lich GmbH, 52425 Ju ¨ lich, Germany article info Article history: Received 1 August 2012 Received in revised form 9 November 2012 Accepted 13 November 2012 Available online 23 November 2012 Keywords: Carbon nanotubes Column experiments Quartz sand Breakthrough curves Retention profiles Transport modeling abstract Water-saturated column experiments were conducted to investigate the effect of input concentration (C o ) and sand grain size on the transport and retention of low concentrations (1, 0.01, and 0.005 mg L 1 ) of functionalized 14 C-labeled multi-walled carbon nanotubes (MWCNT) under repulsive electrostatic conditions that were unfavorable for attachment. The breakthrough curves (BTCs) for MWCNT typically did not reach a plateau, but had an asymmetric shape that slowly increased during breakthrough. The retention profiles (RPs) were not exponential with distance, but rather exhibited a hyper-exponential shape with greater retention near the column inlet. The collected BTCs and RPs were simulated using a numerical model 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 MWCNT were both found to increase with decreasing grain size. These trends reflect greater MWCNT retention rates and a greater number of retention locations in the finer textured sand. The fraction of the injected MWCNT mass that was recovered in the effluent increased and the RPs became less hyper- exponential in shape with higher C o 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 MWCNT shape on MWCNT retention. In particular, MWCNT have a high aspect ratio and we hypothesize that solid phase MWCNT may create a porous network with enhanced ability to retain particles in smaller grain sized sand, especially at higher C o . Results demonstrate that model simulations of MWCNT transport and fate need to accurately account for observed behavior of both BTCs and RPs. ª 2012 Elsevier Ltd. All rights reserved. * Corresponding author. Tel.: þ49 2461 61 3521; fax: þ49 2461 61 2518. E-mail addresses: [email protected](D. Kasel), [email protected](S.A. Bradford), [email protected](J. Simunek), [email protected](M. Heggen), [email protected](H. Vereecken), [email protected](E. Klumpp). Available online at www.sciencedirect.com journal homepage: www.elsevier.com/locate/watres water research 47 (2013) 933 e944 0043-1354/$ e see front matter ª 2012 Elsevier Ltd. All rights reserved. http://dx.doi.org/10.1016/j.watres.2012.11.019
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Available online at w
journal homepage: www.elsevier .com/locate/watres
Transport and retention of multi-walled carbon nanotubes insaturated porous media: Effects of input concentration andgrain size
Daniela Kasel a,*, Scott A. Bradford b, Ji�rı �Sim�unek c, Marc Heggen d,e, Harry Vereecken a,Erwin Klumpp a
aAgrosphere Institute (IBG-3), Forschungszentrum Julich GmbH, 52425 Julich, GermanybUS Salinity Laboratory, Agricultural Research Service, United States Department of Agriculture, Riverside, CA 92507, USAcDepartment of Environmental Sciences, University of California Riverside, Riverside, CA 92521, USAdPeter Grunberg Institute (PGI-5), Forschungszentrum Julich GmbH, 52425 Julich, GermanyeErnst Ruska-Centre (ER-C), Forschungszentrum Julich GmbH, 52425 Julich, Germany
of this study suggest that functionalized MWCNT tend to be
mobile in sandy subsurface environments, and may be trans-
ported to depths greater than 500 cm. Thus, aquifer contami-
nation cannot be excluded. Further work is needed to assess
the mobility of MWCNT in natural porous media, such as
undisturbed soils.
Acknowledgements
This research was performed within the framework of the
‘NanoFlow’-project supported by the German Federal Ministry
of Education and Research. Analysis of bromide in the liquid
samples by Stephan Koppchen is highly appreciated. The
technical assistance of Herbert Philipp is gratefully acknowl-
edged. We also thank Wolfgang Schierenberg for the deter-
mination of the critical coagulation concentration.
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