Regeneration of sulfur-fouled bimetallic Pd-based catalysts.
Pd-based catalysts provide efficient and selective reduction of several drinking water contaminants, but their long-term application requires effective treatments for catalyst regeneration following fouling by constituents in natural waters. This studytested alumina-supported Pd-Cu and Pd-In bimetallic catalysts for nitrate reduction with H2 after sulfide fouling and oxidative regeneration procedures. Both catalysts were severely deactivated after treatment with microM levels of sulfide. Regeneration was attempted with dissolved oxygen, hydrogen peroxide, sodium hypochlorite, and heated air. Only sodium hypochlorite and heated air were effective regenerants, specifically restoring nitrate reduction rates for a Pd-In/gamma-Al2O3 catalyst from 20% to between 39 and 60% of original levels. Results from ICP-MS revealed that sodium hypochlorite caused dissolution of Cu from the Pd-Cu catalyst but that the Pd-In catalyst was chemically stable over a range of sulfide fouling and oxidative regenerative conditions. Analysis byXPS indicated that PdS and In2S3 complexes form during sulfide fouling, where sulfur is present as S2-, and that regeneration with sodium hypochlorite converts a portion of the S2- to S6+, with a corresponding increase in reduction rates. These results indicate that Pd-In catalysts show exceptional promise for being robust under fouling and regeneration conditions that may occur when treating natural waters.
Chaplin
Brian P
BP
Center of Advanced Materials for the Purification of Water with Systems and Department of Civil and Environmental Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.
Shapley
John R
JR
Werth
Charles J
CJ
D000641:Ammonia / Q000737:chemistry; D002384:Catalysis; D003300:Copper / Q000737:chemistry; D004777:Environment; D007204:Indium / Q000737:chemistry; D013058:Mass Spectrometry; D009566:Nitrates / Q000737:chemistry; D009573:Nitrites / Q000737:chemistry; D010084:Oxidation-Reduction; D010165:Palladium / Q000737:chemistry*; D013057:Spectrum Analysis; D013455:Sulfur / Q000737:chemistry*; D013816:Thermodynamics