Abstract
This work investigated the effects of solution pH and surface metal oxyhydroxides on the transport behaviors of carboxyl-functionalized graphene (GR) in saturated porous media. Column experiments were conducted to elucidate the transport behavior of functionalized GR in acid-cleaned and natural sand under different solution pH conditions (i.e., 5.6 and 8.3). The results showed that the functionalized GR was highly mobile in the acid-cleaned sand columns at both pH 5.6 and 8.3 with recovery rates close to 100 %. The deposition of the functionalized GR was higher in the natural sand columns, and the recovery rates were 88.4 and 96.5 % for pH 5.6 and 8.3, respectively. The reductions of the mobility of the functionalized GR in the natural sand columns could be caused by the interaction between carboxyl functional groups of the GR and the surface metal hydroxides on the sand grains, which is pH dependent. An advection–dispersion-reaction model was applied to the data and successfully simulated the transport of the functionalized GR through the acid-cleaned and natural sand columns.
References
Akhavan O, Ghaderi E (2010) Toxicity of graphene and graphene oxide nanowalls against bacteria. ACS Nano 4:5731–5736
Bin G, Cao X, Dong Y, Luo Y, Ma LQ (2011) Colloid deposition and release in soils and their association with heavy metals. Crit Rev Environ Sci Technol 41:336–372
Chiang SC, Radcliffe DE, Miller WP, Newman KD (1987) Hydraulic conductivity of three southeastern soils as affected by sodium, electrolyte concentration, and pH1. Soil Sci Soc Am J 51:1293–1299
Dreyer DR, Park S, Bielawski CW, Ruoff RS (2010) The chemistry of graphene oxide. Chem Soc Rev 39:228–240
Duch MC, Budinger GRS, Liang YT, Soberanes S, Urich D, Chiarella SE, Campochiaro LA, Gonzalez A, Chandel NS, Hersam MC, Mutlu GM (2011) Minimizing oxidation and stable nanoscale dispersion improves the biocompatibility of graphene in the lung. Nano Lett 11:5201–5207
Feriancikova L, Xu SP (2012) Deposition and remobilization of graphene oxide within saturated sand packs. J Hazard Mater 235:194–200
Gao B, Saiers JE, Ryan JN (2004) Deposition and mobilization of clay colloids in unsaturated porous media. Water Resour Res 40:W08602
Johnson PR, Sun N, Elimelech M (1996) Colloid transport in geochemically heterogeneous porous media: modeling and measurements. Environ Sci Technol 30:3284–3293
Johnson WP, Ma HL, Pazmino E (2011) Straining credibility: a general comment regarding common arguments used to infer straining as the mechanism of colloid retention in porous media. Environ Sci Technol 45:3831–3832
Kulkarni A, Amin R, Kim H, Hong BH, Park SH, Kim T (2012) Photoresistivity and optical switching of graphene with DNA lattices. Curr Appl Phys 12:623–627
Liao K-H, Lin Y-S, Macosko CW, Haynes CL (2011) Cytotoxicity of graphene oxide and graphene in human erythrocytes and skin fibroblasts. ACS Appl Mater Interfaces 3:2607–2615
Liu Y, Xie B, Zhang Z, Zheng Q, Xu Z (2012) Mechanical properties of graphene papers. J Mech Phys Solids 60:591–605
Liu L, Gao B, Wu L, Morales V, Yang L, Zhou Z, Wang H (2013) Deposition and transport of graphene oxide in saturated and unsaturated porous media. Chem Eng J 229:444–449
Miller WP, Newman KD, Frenkel H (1990) Flocculation concentration and sodium/calcium exchange of kaolinitic soil clays. Soil Sci Soc Am J 54:346–351
Pantelic RS, Meyer JC, Kaiser U, Stahlberg H (2012) The application of graphene as a sample support in transmission electron microscopy. Solid State Commun 152:1375–1382
Sanchez VC, Jachak A, Hurt RH, Kane AB (2011) Biological interactions of graphene-family nanomaterials: an interdisciplinary review. Chem Res Toxicol 25:15–34
Shahil KMF, Balandin AA (2012) Thermal properties of graphene and multilayer graphene: applications in thermal interface materials. Solid State Commun 152:1331–1340
Shan C, Yang H, Han D, Zhang Q, Ivaska A, Niu L (2009) Water-soluble graphene covalently functionalized by biocompatible poly-l-lysine. Langmuir 25:12030–12033
Smith J, Gao B, Funabashi H, Tran TN, Luo D, Ahner BA, Steenhuis TS, Hay AG, Walter MT (2007) Pore-scale quantification of colloid transport in saturated porous media. Environ Sci Technol 42:517–523
Swartz CH, Gschwend PM (1998) Mechanisms controlling release of colloids to groundwater in a southeastern coastal plain aquifer sand. Environ Sci Technol 32:1779–1785
Tian YA, Gao B, Silvera-Batista C, Ziegler KJ (2010) Transport of engineered nanoparticles in saturated porous media. J Nanopart Res 12:2371–2380
Tian Y, Gao B, Ziegler KJ (2011) High mobility of SDBS-dispersed single-walled carbon nanotubes in saturated and unsaturated porous media. J Hazard Mater 186:1766–1772
Tian Y, Gao B, Wang Y, Morales VL, Carpena RM, Huang QG, Yang LY (2012) Deposition and transport of functionalized carbon nanotubes in water-saturated sand columns. J Hazard Mater 213:265–272
Tufenkji N, Elimelech M (2005) Breakdown of colloid filtration theory: role of the secondary energy minimum and surface charge heterogeneities. Langmuir 21:841–852
Wang S, Yu D, Dai L, Chang DW, Baek J-B (2011) Polyelectrolyte-functionalized graphene as metal-free electrocatalysts for oxygen reduction. ACS Nano 5:6202–6209
Yan L, Zhao F, Li S, Hu Z, Zhao Y (2011) Low-toxic and safe nanomaterials by surface-chemical design, carbon nanotubes, fullerenes, metallofullerenes, and graphenes. Nanoscale 3:362–382
Yang K, Li Y, Tan X, Peng R, Liu Z (2012) Behavior and toxicity of graphene and its functionalized derivatives in biological systems. Small 9(9–10):1492–1503
Yang K, Gong H, Shi X, Wan J, Zhang Y, Liu Z (2013) In vivo biodistribution and toxicology of functionalized nano-graphene oxide in mice after oral and intraperitoneal administration. Biomaterials 34:2787–2795
Acknowledgments
This work was partially supported by the NSF through Grant CBET-1054405 and the NSFC through Grant 51179203.
Author information
Authors and Affiliations
Corresponding author
Electronic supplementary material
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Liu, L., Gao, B., Wu, L. et al. Effects of pH and surface metal oxyhydroxides on deposition and transport of carboxyl-functionalized graphene in saturated porous media. J Nanopart Res 15, 2079 (2013). https://doi.org/10.1007/s11051-013-2079-2
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11051-013-2079-2