Nanoscale, zero-valent iron is a promising reagent for in situ reduction of a variety of subsurface contaminants, but its utility in full-scale remediation projects is limited by material costs. Iron nanoparticles (20-100 nm diameter) supported on carbon (C-Fe0) were synthesized by reacting iron salts, adsorbed or impregnated from aqueous solutions onto 80 m2/g carbon black, at 600-800 degrees C under Ar. Similar products were obtained by heating the reactants under air in a covered alumina crucible. X-ray powder diffraction patterns show that Fe3O4 particles are formed at 300-500 degrees C in the initial stage of the reaction and that these particles are reduced to a mixture of alpha- and gamma-Fe nanoparticles above 600 degrees C. When C-Fe0 was combined with carboxymethylcellulose in a 5:1 weight ratio in water, the resulting material had similar transport properties to previously optimized nanoiron/polyanion suspensions in water-saturated sand columns. At a 10:3 Fe/Cr mole ratio, C-Fe0 reduced a 10 ppm Cr(VI) solution to approximately 1 ppm within three days. The surface area normalized first-order Cr removal rate was 1.2 h(-1) m(-2) under these conditions. These results demonstrate that reactive nanoiron with good transport properties in water-saturated porous media can be made in a scalable process from inexpensive starting materials by carbothermal reduction.
Sand-packed columns were used to study the transport of micro- and nanoiron particle suspensions modified with anionic polyelectrolytes. With microscale carbonyl iron powder (CIP), the profiles of initial and eluted particle diameters were compared with simulations based on classical filtration theory (CFT), using both the Tufenkji-Elimelech (TE) and Rajagopalan-Tien (RT) models. With particle size distributions that peaked in the submicron range, there was reasonable agreement between both models and the eluted distributions. With distributions that peaked in the 1.5 mirom range, however, the eluted distributions were narrower and shifted to a smaller particle size than predicted by CFT. Apparent sticking coefficients depended on column length and flow rate, and the profile of retained iron in the columns did not follow the log-linearform expected from CFT. These observations could be rationalized in terms of the secondary energy minimum model recently proposed by Tufenkji and Elimelech (Langmuir 2005, 21, 841). For microiron, sticking coefficients correlated well with particle zeta potentials and polyacrylate (PAA) concentration. With nanoscale iron particles, there was no apparent correlation between filtration length and total electrolyte concentration. However, mixtures of PAA with poly (4-styrenesulfonate) and bentonite clay significantly enhanced nanoiron transport, possibly by affecting the aggregation of the particles.
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