Technical Papers
Aug 2, 2016

Transport of Single-Layered Graphene Oxide Nanosheets through Quartz and Iron Oxide–Coated Sand Columns

Publication: Journal of Environmental Engineering
Volume 143, Issue 2

Abstract

Single-layered graphene oxide (SLGO) nanosheets are distinguished from other colloids by their extreme anisotropy, which likely exerts a strong control on their transport behavior. Hence, this study investigates the influence of both environmentally relevant pH and ionic strength on the transport of SLGO nanosheets through saturated quartz or iron oxide–coated sands. Both the nanosheets and quartz sands are negatively charged throughout the experimental conditions, resulting in very little nanosheet deposition onto the quartz sands. However, increasing ionic strength and decreasing pH did cause measurable increases in nanosheet deposition, likely due to decreases in the magnitude of negative charges near the respective surfaces. Conversely, nanosheets and iron oxide–coated sands are oppositely charged throughout the experimental conditions, resulting in significant nanosheet deposition onto the iron oxide–coated sands. These trends suggest that nanosheet deposition is largely controlled by electrostatic forces, although the deposition rate of the high ionic strength iron oxide–coated sand treatment could not be explained by electrostatic interactions alone and instead may be influenced by nanosheet aggregation. Collectively, these measurements enable prediction of SLGO transport throughout a range of realistic environmental and geologic conditions.

Get full access to this article

View all available purchase options and get full access to this article.

Acknowledgments

This research was supported, in part, by fellowships to the first author from the Arthur J. Schmitt Foundation and the National Research Council. In addition, the authors performed most experiments and analyses using instrumentation at the Center for Environmental Science and Technology (University of Notre Dame). The authors also acknowledge a substantial technical contribution by Jennifer Szymanowski (ND) and additional research guidance by Dr. Lauren Greenlee (NIST). The second author’s contribution was supported by the USDOE Office of Nuclear Energy’s Nuclear Energy University Programs, the U.S. National Science Foundation’s Environmental Engineering Program, the donors of the ACS Petroleum Research Fund, and the University of Notre Dame Sustainable Energy Initiative. Contribution of the National Institute of Standards and Technology, an agency of the United States government; not subject to copyright in the United States. Certain commercial equipment, instruments, databases, or materials may be identified in this paper to foster understanding. Such identification does not imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that the materials or equipment identified are necessarily the best available for the purpose.

References

Ams, D. A., Fein, J. B., Dong, H. L., and Maurice, P. A. (2004). “Experimental measurements of the adsorption of Bacillus subtilis and Pseudomonas mendocina onto Fe-oxyhydroxide-coated and uncoated quartz grains.” Geomicrobiol. J., 21(8), 511–519.
Bradford, S. A., Simunek, J., Bettahar, M., Van Genuchten, M. T., and Yates, S. R. (2003). “Modeling colloid attachment, straining, and exclusion in saturated porous media.” Environ. Sci. Technol., 37(10), 2242–2250.
Bradford, S. A., Yates, S. R., Bettahar, M., and Simunek, J. (2002). “Physical factors affecting the transport and fate of colloids in saturated porous media.” Water Resour. Res., 38(12), 63/1–63/12.
Chen, C. M., et al. (2009). “Self-assembled free-standing graphite oxide membrane.” Adv. Mater., 21(35), NA–NA.
Chowdhury, I., Duch, M. C., Mansukhani, N. D., Hersam, M. C., and Bouchard, D. (2013). “Colloidal properties and stability of graphene oxide nanomaterials in the aquatic environment.” Environ. Sci. Technol., 47(12), 6288–6296.
Davis, J. A., and Leckie, J. O. (1978). “Surface ionization and complexation at oxide-water interface. 2: Surface properties of amorphous iron oxyhydroxide and adsorption of metal ions.” J. Colloid Interface Sci., 67(1), 90–107.
Dentz, M., and Bolster, D. (2010). “Distribution- versus correlation-induced anomalous transport in quenched random velocity fields.” Phys. Rev. Lett., 105(24), 244301/1–244301/4.
Dogan, A. U., Dogan, M., Onal, M., Sarikaya, Y., Aburub, A., and Wurster, D. E. (2006). “Baseline studies of the clay minerals society source clays: Specific surface area by the Brunauer Emmett Teller (BET) method.” Clays Clay Miner., 54(1), 62–66.
Dogan, M., Dogan, A. U., Yesilyurt, F. I., Alaygut, D., Buckner, I., and Wurster, D. E. (2007). “Baseline studies of The Clay Minerals Society special clays: Specific surface area by the Brunauer Emmett Teller (BET) method.” Clays Clay Miner., 55(5), 534–541.
Dreyer, D. R., Park, S., Bielawski, C. W., and Ruoff, R. S. (2010). “The chemistry of graphene oxide.” Chem. Soc. Rev., 39(1), 228–240.
Duster, T. A., Szymanowski, J. E. S., Na, C., Showalter, A. R., Bunker, B. A., and Fein, J. B. (2015). “Surface complexation modeling of proton and metal sorption onto graphene oxide.” Colloids Surf. A: Physicochem. Eng. Aspects, 466, 28–39.
Feriancikova, L., and Xu, S. P. (2012). “Deposition and remobilization of graphene oxide within saturated sand packs.” J. Hazard. Mater., 235, 194–200.
Gao, W., Alemany, L. B., Ci, L. J., and Ajayan, P. M. (2009). “New insights into the structure and reduction of graphite oxide.” Nat. Chem., 1(5), 403–408.
Gao, Y., et al. (2012). “Adsorption and removal of tetracycline antibiotics from aqueous solution by graphene oxide.” J. Colloid Interface Sci., 368(1), 540–546.
Hartono, T., Wang, S. B., Ma, Q., and Zhu, Z. H. (2009). “Layer structured graphite oxide as a novel adsorbent for humic acid removal from aqueous solution.” J. Colloid Interface Sci., 333(1), 114–119.
Hummers, W. S., and Offeman, R. E. (1958). “Preparation of graphitic oxide.” J. Am. Chem. Soc., 80(6), 1339.
Ion, A. C., Alpatova, A., Ion, I., and Culetu, A. (2011). “Study on phenol adsorption from aqueous solutions on exfoliated graphitic nanoplatelets.” Mater. Sci. Eng. B-Adv. Funct. Solid-State Mater., 176(7), 588–595.
Jaisi, D. P., and Elimelech, M. (2009). “Single-walled carbon nanotubes exhibit limited transport in soil columns.” Environ. Sci. Technol., 43(24), 9161–9166.
Jaisi, D. P., Saleh, N. B., Blake, R. E., and Elimelech, M. (2008). “Transport of single-walled carbon nanotubes in porous media: Filtration mechanisms and reversibility.” Environ. Sci. Technol., 42(22), 8317–8323.
Johnson, P. R., Sun, N., and Elimelech, M. (1996). “Colloid transport in geochemically heterogeneous porous media: Modeling and measurements.” Environ. Sci. Technol., 30(11), 3284–3293.
Johnson, W. P., and Logan, B. E. (1996). “Enhanced transport of bacteria in porous media by sediment-phase and aqueous-phase natural organic matter.” Water Res., 30(4), 923–931.
Konkena, B., and Vasudevan, S. (2012). “Understanding aqueous dispersibility of graphene oxide and reduced graphene oxide through pK(a) measurements.” J. Phys. Chem. Lett., 3(7), 867–872.
Kretzschmar, R., Barmettler, K., Grolimund, D., Yan, Y. D., Borkovec, M., and Sticher, H. (1997). “Experimental determination of colloid deposition rates and collision efficiencies in natural porous media.” Water Resour. Res., 33(5), 1129–1137.
Kretzschmar, R., Borkovec, M., Grolimund, D., and Elimelech, M. (1999). “Mobile subsurface colloids and their role in contaminant transport.” Adv. Agron., 66, 121–193.
Lagaly, G. (2006). “Colloid clay science.” Handbook of clay science, F. Bergaya, B. K. G. Theng, and G. Lagaly, eds., Elsevier, Amsterdam, Netherlands, 141–245.
Lanphere, J. D., Luth, C. J., and Walker, S. L. (2013). “Effects of solution chemistry on the transport of graphene oxide in saturated porous media.” Environ. Sci. Technol., 47(9), 4255–4261.
Lee, D. W., et al. (2010). “The structure of graphite oxide: Investigation of its surface chemical groups.” J. Phys. Chem. B, 114(17), 5723–5728.
Lerf, A., He, H. Y., Forster, M., and Klinowski, J. (1998). “Structure of graphite oxide revisited.” J. Phys. Chem. B, 102(23), 4477–4482.
Liu, L., et al. (2013a). “Deposition and transport of graphene oxide in saturated and unsaturated porous media.” Chem. Eng. J., 229, 444–449.
Liu, L., Gao, B., Wu, L., Yang, L. Y., Zhou, Z. H., and Wang, H. (2013b). “Effects of pH and surface metal oxyhydroxides on deposition and transport of carboxyl-functionalized graphene in saturated porous media.” J. Nanoparticle Res., 15(11), 2079.
Novoselov, K. S., et al. (2004). “Electric field effect in atomically thin carbon films.” Science, 306(5696), 666–669.
Pagnanelli, F., Bornoroni, L., Moscardini, E., and Toro, L. (2006). “Non-electrostatic surface complexation models for protons and lead(II) sorption onto single minerals and their mixture.” Chemosphere, 63(7), 1063–1073.
Park, S., and Ruoff, R. S. (2009). “Chemical methods for the production of graphenes.” Nat. Nano Technol., 4(4), 217–224.
Peigney, A., Laurent, C., Flahaut, E., Bacsa, R. R., and Rousset, A. (2001). “Specific surface area of carbon nanotubes and bundles of carbon nanotubes.” Carbon, 39(4), 507–514.
Qi, Z., Zhang, L., and Chen, W. (2014a). “Transport of graphene oxide nanoparticles in saturated sandy soil.” Environ. Sci.: Process. Impacts, 16(10), 2268–2277.
Qi, Z., Zhang, L., Wang, F., Hou, L., and Chen, W. (2014b). “Factors controlling transport of graphene oxide nanoparticles in saturated sand columns.” Environ. Toxicol. Chem., 33(5), 998–1004.
Redman, J. A., Walker, S. L., and Elimelech, M. (2004). “Bacterial adhesion and transport in porous media: Role of the secondary energy minimum.” Environ. Sci. Technol., 38(6), 1777–1785.
Romanchuk, A. Y., Slesarev, A. S., Kalmykov, S. N., Kosynkin, D. V., and Tour, J. M. (2013). “Graphene oxide for effective radionuclide removal.” Phys. Chem. Chem. Phys., 15(7), 2321–2327.
Ryan, J. N., and Elimelech, M. (1996). “Colloid mobilization and transport in groundwater.” Colloids Surf. A-Physicochem. Eng. Aspects, 107, 1–56.
Salerno, M. B., Flamm, M., Logan, B. E., and Velegol, D. (2006). “Transport of rodlike colloids through packed beds.” Environ. Sci. Technol., 40(20), 6336–6340.
Sen, T. K., and Khilar, K. C. (2006). “Review on subsurface colloids and colloid-associated contaminant transport in saturated porous media.” Adv. Colloid Interface Sci., 119(2–3), 71–96.
Seymour, M. B., Chen, G. X., Su, C. M., and Li, Y. S. (2013). “Transport and retention of colloids in porous media: Does shape really matter?” Environ. Sci. Technol., 47(15), 8391–8398.
Sitko, R., et al. (2013). “Adsorption of divalent metal ions from aqueous solutions using graphene oxide.” Dalton Trans., 42(16), 5682–5689.
Smith, J., et al. (2008). “Pore-scale quantification of colloid transport in saturated porous media.” Environ. Sci. Technol., 42(2), 517–523.
Song, L., and Elimelech, M. (1993). “Dynamics of colloid deposition in porous media—Modeling the role of retained particles.” Colloids Surf. A-Physicochem. Eng. Aspects, 73, 49–63.
Stankovich, S., et al. (2007). “Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide.” Carbon, 45(7), 1558–1565.
Szabo, T., Berkesi, O., Forgo, P., Josepovits, K., Sanakis, Y., Petridis, D., and Dekany, I. (2006a). “Evolution of surface functional groups in a series of progressively oxidized graphite oxides.” Chem. Mater., 18(11), 2740–2749.
Szabo, T., Tombacz, E., Illes, E., and Dekany, I. (2006b). “Enhanced acidity and pH-dependent surface charge characterization of successively oxidized graphite oxides.” Carbon, 44(3), 537–545.
Tong, M. P., Ding, J. L., Shen, Y., and Zhu, P. T. (2010). “Influence of biofilm on the transport of fullerene (C-60) nanoparticles in porous media.” Water Res., 44(4), 1094–1103.
Tournassat, C., Neaman, A., Villieras, F., Bosbach, D., and Charlet, L. (2003). “Nanomorphology of montmorillonite particles: Estimation of the clay edge sorption site density by low-pressure gas adsorption and AFM observations.” Am. Miner., 88(11–12), 1989–1995.
Tufenkji, N., and Elimelech, M. (2004). “Correlation equation for predicting single-collector efficiency in physicochemical filtration in saturated porous media.” Environ. Sci. Technol., 38(2), 529–536.
Wang, S. B., Sun, H. Q., Ang, H. M., and Tade, M. O. (2013). “Adsorptive remediation of environmental pollutants using novel graphene-based nanomaterials.” Chem. Eng. J., 226, 336–347.
Weiss, T. H., Mills, A. L., Hornberger, G. M., and Herman, J. S. (1995). “Effect of bacterial-cell shape on transport of bacteria in porous media.” Environ. Sci. Technol., 29(7), 1737–1740.
Xu, S. P., Gao, B., and Saiers, J. E. (2006). “Straining of colloidal particles in saturated porous media.” Water Resour. Res., 42(12), W12S16.
Yao, K. M., Habibian, M. M., and Omelia, C. R. (1971). “Water and waste water filtration—Concepts and applications.” Environ. Sci. Technol., 5(11), 1105–1112.
Zhang, J. L., Yang, H. J., Shen, G. X., Cheng, P., Zhang, J. Y., and Guo, S. W. (2010). “Reduction of graphene oxide via L-ascorbic acid.” Chem. Commun., 46(7), 1112–1114.
Zhang, W. J., et al. (2011). “Fast and considerable adsorption of methylene blue dye onto graphene oxide.” Bull. Environ. Contam. Toxicol., 87(1), 86–90.
Zhao, G. X., et al. (2011a). “Removal of Pb(II) ions from aqueous solutions on few-layered graphene oxide nanosheets.” Dalton Trans., 40(41), 10945–10952.
Zhao, G. X., et al. (2012). “Preconcentration of U(VI) ions on few-layered graphene oxide nanosheets from aqueous solutions.” Dalton Trans., 41(20), 6182–6188.
Zhao, G. X., Li, J. X., Ren, X. M., Chen, C. L., and Wang, X. K. (2011c). “Few-layered graphene oxide nanosheets as superior sorbents for heavy metal ion pollution management.” Environ. Sci. Technol., 45(24), 10454–10462.

Information & Authors

Information

Published In

Go to Journal of Environmental Engineering
Journal of Environmental Engineering
Volume 143Issue 2February 2017

History

Received: Nov 20, 2015
Accepted: May 24, 2016
Published online: Aug 2, 2016
Discussion open until: Jan 2, 2017
Published in print: Feb 1, 2017

Permissions

Request permissions for this article.

Authors

Affiliations

Thomas A. Duster [email protected]
Geochemist, Applied Chemicals and Materials Division, Material Measurement Laboratory, National Institute of Standards and Technology, 325 Broadway, Boulder, CO 80305; formerly, Ph.D. Student, Dept. of Civil and Environmental Engineering and Earth Sciences, Univ. of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, IN 46556 (corresponding author). E-mail: [email protected]
Chongzheng Na
Assistant Professor, Dept. of Civil and Environmental Engineering and Earth Sciences, Univ. of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, IN 46556.
Diogo Bolster
Assistant Professor, Dept. of Civil and Environmental Engineering and Earth Sciences, Univ. of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, IN 46556.
Jeremy B. Fein
Professor, Dept. of Civil and Environmental Engineering and Earth Sciences, Univ. of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, IN 46556.

Metrics & Citations

Metrics

Citations

Download citation

If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.

Cited by

View Options

Get Access

Access content

Please select your options to get access

Log in/Register Log in via your institution (Shibboleth)
ASCE Members: Please log in to see member pricing

Purchase

Save for later Information on ASCE Library Cards
ASCE Library Cards let you download journal articles, proceedings papers, and available book chapters across the entire ASCE Library platform. ASCE Library Cards remain active for 24 months or until all downloads are used. Note: This content will be debited as one download at time of checkout.

Terms of Use: ASCE Library Cards are for individual, personal use only. Reselling, republishing, or forwarding the materials to libraries or reading rooms is prohibited.
ASCE Library Card (5 downloads)
$105.00
Add to cart
ASCE Library Card (20 downloads)
$280.00
Add to cart
Buy Single Article
$35.00
Add to cart

Get Access

Access content

Please select your options to get access

Log in/Register Log in via your institution (Shibboleth)
ASCE Members: Please log in to see member pricing

Purchase

Save for later Information on ASCE Library Cards
ASCE Library Cards let you download journal articles, proceedings papers, and available book chapters across the entire ASCE Library platform. ASCE Library Cards remain active for 24 months or until all downloads are used. Note: This content will be debited as one download at time of checkout.

Terms of Use: ASCE Library Cards are for individual, personal use only. Reselling, republishing, or forwarding the materials to libraries or reading rooms is prohibited.
ASCE Library Card (5 downloads)
$105.00
Add to cart
ASCE Library Card (20 downloads)
$280.00
Add to cart
Buy Single Article
$35.00
Add to cart

Media

Figures

Other

Tables

Share

Share

Copy the content Link

Share with email

Email a colleague

Share