Co-Transport of Multi-Walled Carbon Nanotubes and Sodium Dodecylbenzenesulfonate in Chemically Heterogeneous Porous Media

Miaoyue Zhang a, S.A. Bradfordc, J. Šimůnekd, H. Vereeckenb, and E. Klumppb

aSchool of Environmental Science and Engineering, Sun Yat-sen University, 510006 Guangzhou, P.R. China

bAgrosphere Institute (IBG-3), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

cUnited States Department of Agriculture, Agricultural Research Service, U. S. Salinity Laboratory, Riverside, CA 92507, USA

dDepartment of Environmental Sciences, University of California Riverside,Riverside, CA 92521, USA

Email: zhangmy53@mail.sysu.edu.cn

Multi-walled carbon nanotubes (MWCNTs) are increasing used in commercial applications and may be released into the environment with anionic surfactants, such as sodium dodecylbenzenesulfonate (SDBS), in sewer discharge. Little research has examined the transport, retention, and remobilization of MWCNTs in the presence or absence of SDBS in porous media with controlled chemical heterogeneity, and batch and column scale studies were therefore undertaken to address this gap in knowledge. The adsorption isotherms of SDBS on quartz sand (QS), goethite coated quartz sand (GQS), and MWCNTs were determined. Adsorption of SDBS (MWCNTs >> GQS > QS) decreased zeta potentials for these materials, and produced a charge reversal for goethite. Transport of MWCNTs (5 mg/L) dramatically decreased with an increase in the fraction of GQS from 0 to 0.1 in the absence of SDBS. Conversely, co-injection of SDBS (10 and 50 mg/L) and MWCNTs radically increased the transport of MWCNTs when the GQS fraction was 0, 0.1, and 0.3, especially at a higher SDBS concentration, and altered the shape of retention profile. Mathematical modeling revealed that competitive blocking was not the dominant mechanism for the SDBS enhancement of MWCNT transport. Rather, SDBS sorption increased MWCNT transport by increasing electrostatic and/or steric interactions, or creating reversible interactions on rough surfaces. Sequential injection of pulses of MWCNTs and SDBS in sand (0.1 GQS fraction) indicated that SDBS could mobilize some of retained MWCNTs from the top to deeper sand layers, but only a small amount of released MWCNTs were recovered in the effluent. SDBS therefore had a much smaller influence on MWCNT transport in sequential injection than in co-injection, presumably because of a greater energy barrier to MWCNT release than retention. This research sheds novel insight on the roles of competitive blocking, chemical heterogeneity and nanoscale roughness, and injection sequence on MWCNT retention and release.

Keywords: Multi-walled carbon nanotubes, sodium dodecylbenzenesulfonate, competitive blocking, breakthrough curves, retention profiles, modeling

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