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Deposition and Release of Graphene Oxide Nanomaterials Using a Quartz Crystal Microbalance

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† National Research Council Research Associate, Athens, Georgia United States
‡ Departments of Material Science and Engineering, Chemistry, and Medicine, Northwestern University, Evanston, Illinois United States
§ National Exposure Research Laboratory, Ecosystem Research Division, United States Environmental Protection Agency, Athens, Georgia, United States
*Tel: 706-355-8333. E-mail: [email protected]
Cite this: Environ. Sci. Technol. 2014, 48, 2, 961–969
Publication Date (Web):December 17, 2013
https://doi.org/10.1021/es403247k
Copyright © 2013 American Chemical Society
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    Abstract

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    Interactions of graphene oxide (GO) with silica surfaces were investigated using a quartz crystal microbalance with dissipation monitoring (QCM-D). Both GO deposition and release were monitored on silica- and poly-l-lysine (PLL) coated surfaces as a function of GO concentration and in NaCl, CaCl2, and MgCl2 as a function of ionic strength (IS). Under favorable conditions (PLL-coated positive surface), GO deposition rates increased with GO concentration, as expected from colloidal theory. Increased NaCl concentration resulted in a greater deposition attachment efficiency of GO on the silica surface, indicating that deposition of GO follows Derjaguin–Landau–Verwey–Overbeek (DLVO) theory; GO deposition rates decreased at high IS, however, due to large aggregate formation. GO critical deposition concentration (CDC) on the silica surface is determined to be 40 mM NaCl which is higher than the reported CDC values of fullerenes and lower than carbon nanotubes. A similar trend is observed for MgCl2 which has a CDC value of 1.2 mM MgCl2. Only a minimal amount of GO (frequency shift <2 Hz) was deposited on the silica surface in CaCl2 due to the bridging ability of Ca2+ ions with GO functional groups. Significant GO release from silica surface was observed after adding deionized water, indicating that GO deposition is reversible. The release rates of GO were at least 10-fold higher than the deposition rates under similar conditions indicating potential high release and mobility of GO in the environment. Under favorable conditions, a significant amount of GO was released which indicates potential multilayer GO deposition. However, a negligible amount of deposited GO was released in CaCl2 under favorable conditions due to the binding of GO layers with Ca2+ ions. Release of GO was significantly dependent on salt type with an overall trend of NaCl > MgCl2 > CaCl2.

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    Additional table and figures regarding Δf3, ΔD3, deposition, and release rates as a function of NaCl, CaCl2, and MgCl2 This material is available free of charge via the Internet at http://pubs.acs.org.

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