Reductive Dehalogenation of Herbicides Catalyzed by Pd0NPs in a H2-Based Membrane Catalyst-Film Reactor.
Environ Sci Technol
; 56(24): 18030-18040, 2022 12 20.
Article
em En
| MEDLINE
| ID: mdl-36383359
ABSTRACT
More food production required to feed humans will require intensive use of herbicides to protect against weeds. The widespread application and persistence of herbicides pose environmental risks for nontarget species. Elemental-palladium nanoparticles (Pd0NPs) are known to catalyze reductive dehalogenation of halogenated organic pollutants. In this study, the reductive conversion of 2,4-dichlorophenoxyacetic acid (2,4-D) was evaluated in a H2-based membrane catalyst-film reactor (H2-MCfR), in which Pd0NPs were in situ-synthesized as the catalyst film and used to activate H2 on the surface of H2-delivery membranes. Batch kinetic experiments showed that 99% of 2,4-D was removed and converted to phenoxyacetic acid (POA) within 90 min with a Pd0 surface loading of 20 mg Pd/m2, achieving a catalyst specific activity of 6.6 ± 0.5 L/g-Pd-min. Continuous operation of the H2-MCfR loaded with 20 mg Pd/m2 sustained >99% removal of 50 µM 2,4-D for 20 days. A higher Pd0 surface loading, 1030 mg Pd/m2, also enabled hydrosaturation and hydrolysis of POA to cyclohexanone and glycolic acid. Density functional theory identified the reaction mechanisms and pathways, which involved reductive hydrodechlorination, hydrosaturation, and hydrolysis. Molecular electrostatic potential calculations and Fukui indices suggested that reductive dehalogenation could increase the bioavailability of herbicides. Furthermore, three other halogenated herbicidesâatrazine, dicamba, and bromoxynilâwere reductively dehalogenated in the H2-MCfR. This study documents a promising method for the removal and detoxification of halogenated herbicides in aqueous environments.
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Bases de dados:
MEDLINE
Assunto principal:
Nanopartículas Metálicas
/
Herbicidas
Limite:
Humans
Idioma:
En
Revista:
Environ Sci Technol
Ano de publicação:
2022
Tipo de documento:
Article
País de afiliação:
China