title: Palladium-indium catalyzed reduction of N-nitrosodimethylamine: indium as a promoter metal.
abstract: An emerging technology for the removal of N-nitrosodimethylamine (NDMA) from drinking and groundwater is reductive destruction using noble metal catalysts and hydrogen gas as a reducing agent. Bimetallic palladium-indium (Pd-In) supported on alumina combines the ability of Into activate NDMA with the hydrogen activating properties of Pd. This study examined the effect of In addition to a commercial 5% Pd by weight on gamma-Al2O3 catalyst on the efficacy of NDMA reduction. The pseudo-first-order rate constant increased proportionately to In loading from 0.057 h(-1) for 0% In to a maximum of 0.25 h(-1) for 1% In and then decreased with additional in loading. Data suggest that hydrogen activation occurred only on Pd surfaces and In activated NDMA 20 times more effectively than Pd on a mass basis. The rate-limiting factor was NDMA activation for In loadings below 1%. The decrease at higher loadings is interpreted as In blocking pore spaces and limiting access to Pd sites, suggesting monatomic hydrogen limitation. The only products detected were dimethylamine and ammonium with carbon and nitrogen balances in excess of 92%, consistent with a mechanism involving reductive N-N bond cleavage. Results from this study serve as a basis for optimizing bimetallic catalysts for treating NDMA contaminated waters.
authors.affiliation: Department of Civil & Environmental Engineering, Stanford University, Stanford, California 94305-4020, USA.
authors.forename: Matthew G
authors.initials: MG
authors.lastname: Davie
authors.forename: Kaimin
authors.initials: K
authors.lastname: Shih
authors.forename: Federico A
authors.initials: FA
authors.lastname: Pacheco
authors.forename: James O
authors.initials: JO
authors.lastname: Leckie
authors.forename: Martin
authors.initials: M
authors.lastname: Reinhard
mesh_terms: D000537:Aluminum Oxide / Q000737:chemistry*; D002384:Catalysis; D004128:Dimethylnitrosamine / Q000737:chemistry*; D007204:Indium / Q000737:chemistry*; D010084:Oxidation-Reduction; D010165:Palladium / Q000737:chemistry*; D014874:Water Pollutants, Chemical / Q000737:chemistry*; D018508:Water Purification / Q000379:methods*
chemical_list: D014874:Water Pollutants, Chemical; D007204:Indium; D010165:Palladium; D000537:Aluminum Oxide; D004128:Dimethylnitrosamine