Effect of solution conditions on the product distribution of catalytic nitrate reduction using Pd-In catalysts in a continuous-flow packed-bed reactor

ENVR 175

Brian P. Chaplin, chaplin1@email.arizona.edu, Department of Chemical and Environmental Engineering, University of Arizona, 1133 E James E Rogers Way, Tucson, AZ 85721, John R. Shapley, shapley@uiuc.edu, Department of Chemistry and Center of Advanced Materials for the Purification of Water with Systems, University of Illinois at Urbana-Champaign, 505 S. Mathews, Urbana, IL 61801, and Charles J. Werth, werth@uiuc.edu, Department of Civil and Environmental Engineering and Center of Advanced Materials for Purification of Water with Systems, University of Illinois at Urbana-Champaign, 3215 Newmark Civil Engineering Laboratory, 205 N. Mathews Ave., Urbana, IL 61801.
This study tested alumina-supported Pd-In bimetallic catalysts for nitrate reduction with hydrogen in a continuous-flow packed-bed reactor. The goal was to assess the role that solution conditions have on the product distribution of catalytic nitrate reduction. Experimental results showed that nitrate at an influent concentration of 1 mM was reduced below the regulatory MCL of 0.71 mM by the addition of hydrogen, with no accumulation of nitrite or nitrous oxide. The final products were ammonia and nitrogen. Ammonia production increased with increases in pH, hydrogen and sulfide concentrations, and decreased by addition of dissolved oxygen. Sulfide was shown to completely foul the catalyst bed. Regeneration with NaOCl and NaHCO3 was able to restore nitrate reduction to near its pre-fouled level, but high ammonia production and low levels of nitrous oxide were observed. Ammonia production from the fresh and regenerated sulfide-fouled catalyst was 32.1±0.5 and 82.3±1.9% of nitrate reduced (on a molar basis), respectively. These results indicate that influent pH and hydrogen levels can be optimized to reduce ammonia production and that reduced sulfur species should be removed from nitrate-contaminated source waters before they come in contact with Pd-In catalysts.