title: Doping of biogenic Pd catalysts with Au enables dechlorination of diclofenac at environmental conditions.
abstract: By using the metal reducing capacities of bacteria, Pd nanoparticles can be produced in a sustainable way ('bio-Pd'). These bio-Pd nanoparticles can be used as a catalyst in, for example, dehalogenation reactions. However, some halogenated compounds are not efficiently degraded using a bio-Pd catalyst. This study shows that the activity of bio-Pd can be improved by doping with Au(0) ('bio-Pd/Au'). In contrast with bio-Pd, bio-Pd/Au could perform the removal of the model pharmaceutical compound diclofenac from an aqueous medium in batch experiments at neutral pH and with H(2) as the hydrogen donor (first order decay constant of 0.078 ± 0.009 h(-1)). Dehalogenation was for both catalysts the only observed reaction. For bio-Pd/Au, a disproportional increase of catalytic activity was observed with increasing Pd-content of the catalyst. In contrast, when varying the Au-content of the catalyst, a Pd/Au mass ratio of 50/1 showed the highest catalytic activity (first order decay value of 0.52 ± 0.02 h(-1)). The removal of 6.40 μg L(-1) diclofenac from a wastewater treatment plant effluent using bio-Pd was not possible even after prolonged reaction time. However, by using the most active bio-Pd/Au catalyst, 43.8 ± 0.5% of the initially present diclofenac could be removed after 24 h. This study shows that doping of bio-Pd nanoparticles with Au(0) can be a promising approach for the reductive treatment of wastewaters containing halogenated contaminants.
authors.affiliation: Laboratory of Microbial Ecology and Technology (LabMET), Ghent University, Coupure Links 653, B-9000 Gent, Belgium.
authors.forename: Simon
authors.initials: S
authors.lastname: De Corte
authors.forename: Tom
authors.initials: T
authors.lastname: Sabbe
authors.forename: Tom
authors.initials: T
authors.lastname: Hennebel
authors.forename: Lynn
authors.initials: L
authors.lastname: Vanhaecke
authors.forename: Bart
authors.initials: B
authors.lastname: De Gusseme
authors.forename: Willy
authors.initials: W
authors.lastname: Verstraete
authors.forename: Nico
authors.initials: N
authors.lastname: Boon
mesh_terms: D001673:Biodegradation, Environmental; D002220:Carbamazepine / Q000302:isolation & purification; D002384:Catalysis; D002853:Chromatography, Liquid; D003973:Diatrizoate / Q000302:isolation & purification; D004008:Diclofenac / Q000737:chemistry / Q000302:isolation & purification*; D006046:Gold / Q000378:metabolism*; D054879:Halogenation; D006761:Hospitals; D007700:Kinetics; D013058:Mass Spectrometry; D008506:Medical Waste / Q000032:analysis; D010165:Palladium / Q000378:metabolism*; D020592:Shewanella / Q000378:metabolism*; D013997:Time Factors; D014865:Waste Disposal, Fluid; D018508:Water Purification
chemical_list: D008506:Medical Waste; D003973:Diatrizoate; D004008:Diclofenac; D002220:Carbamazepine; D010165:Palladium; D006046:Gold