Effect of adsorbed polyelectrolyte and humic acid on TCE dechlorination by Fe0/Fe-oxide nanoparticles

ENVR 172

Gregory V. Lowry, glowry@cmu.edu1, Tanapon Phenrat, tphenrat@andrew.cmu.edu1, Yueqiang Liu, Alan.Liu@WestonSolutions.com2, Hye-Jin Kim, hyejink@andrew.cmu.edu1, and Robert D. Tilton, tilton@andrew.cmu.edu3. (1) Department of Civil & Environmental Engineering, Carnegie Mellon University, Pittsburgh, PA 15213-3890, (2) Weston Solutions, Inc, 1 Wall St., Ste 201, Manchester, NH 03101, (3) Department of Biomedical Engineering and Department of Chemical Engineering, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, PA 15213
Reactive Fe0/Fe-oxide nanoparticles are surface modified with polyelectrolytes to enhance colloidal stability and mobility in the subsurface. In the environment, these nanoparticles further interact with natural organic matter (NOM). A mechanistic understanding of how adsorbed polyelectrolyte and NOM affect their reactivity is not available. The objectives of this study are to determine the reasons for the decreased surface reactivity for TCE dechlorination upon adsorption of polyelectrolyte and/or humic acid. The TCE dechlorination rate is systematically measured as a function of the adsorbed mass of polyelectrolyte and humic acid. The layer thickness of the sorbed polyelectrolytes is estimated by Ohshima's soft particle analysis and the partitioning coefficient of TCE onto each polyelectrolyte is measured. These data and Scheutjens-Fleer theory for polymer adsorption indicate that reactivity loss at low adsorbed mass is from reactive site blocking at points of polyelectrolyte attachment and that mass transfer resistance in the polyelectrolyte brush is significant at higher adsorbed mass of polyelectrolyte where an extended brush conformation develops. This conceptual model explains the decrease in the observed TCE dechlorination rate constant for both adsorbed polyelectrolytes and humic acid on Fe0/Fe-oxide nanoparticles.