Hydrodefluorination of Perfluorooctanoic Acid in the H 2 -Based Membrane Catalyst-Film Reactor with Platinum Group Metal Nanoparticles: Pathways and Optimal Conditions.

Autor: Long M; Biodesign Swette Center for Environmental Biotechnology, Arizona State University, Tempe, Arizona 85287-5701, United States.; Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment, Houston, Texas 77005, United States., Elias WC; Department of Chemical and Biomolecular Engineering, Rice University, Houston, Texas 77005-1892, United States., Heck KN; Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment, Houston, Texas 77005, United States.; Department of Chemical and Biomolecular Engineering, Rice University, Houston, Texas 77005-1892, United States., Luo YH; Biodesign Swette Center for Environmental Biotechnology, Arizona State University, Tempe, Arizona 85287-5701, United States., Lai YS; Biodesign Swette Center for Environmental Biotechnology, Arizona State University, Tempe, Arizona 85287-5701, United States., Jin Y; Arizona Metabolomics Laboratory, College of Health Solutions, Arizona State University, Phoenix, Arizona 85004, United States., Gu H; Arizona Metabolomics Laboratory, College of Health Solutions, Arizona State University, Phoenix, Arizona 85004, United States., Donoso J; Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment, Houston, Texas 77005, United States.; Department of Chemical and Biomolecular Engineering, Rice University, Houston, Texas 77005-1892, United States., Senftle TP; Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment, Houston, Texas 77005, United States.; Department of Chemical and Biomolecular Engineering, Rice University, Houston, Texas 77005-1892, United States., Zhou C; Biodesign Swette Center for Environmental Biotechnology, Arizona State University, Tempe, Arizona 85287-5701, United States.; Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment, Houston, Texas 77005, United States., Wong MS; Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment, Houston, Texas 77005, United States.; Department of Chemical and Biomolecular Engineering, Rice University, Houston, Texas 77005-1892, United States., Rittmann BE; Biodesign Swette Center for Environmental Biotechnology, Arizona State University, Tempe, Arizona 85287-5701, United States.; Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment, Houston, Texas 77005, United States.
Jazyk: angličtina
Zdroj: Environmental science & technology [Environ Sci Technol] 2021 Dec 21; Vol. 55 (24), pp. 16699-16707. Date of Electronic Publication: 2021 Dec 07.
DOI: 10.1021/acs.est.1c06528
Abstrakt: PFAAs (perfluorinated alkyl acids) have become a concern because of their widespread pollution and persistence. A previous study introduced a novel approach for removing and hydrodefluorinating perfluorooctanoic acid (PFOA) using palladium nanoparticles (Pd 0 NPs) in situ synthesized on H 2 -gas-transfer membranes. This work focuses on the products, pathways, and optimal catalyst conditions. Kinetic tests tracking PFOA removal, F - release, and hydrodefluorination intermediates documented that PFOA was hydrodefluorinated by a mixture of parallel and stepwise reactions on the Pd 0 NP surfaces. Slow desorption of defluorination products lowered the catalyst's activity for hydrodefluorination. Of the platinum group metals studied, Pd was overall superior to Pt, Rh, and Ru for hydrodefluorinating PFOA. pH had a strong influence on performance: PFOA was more strongly adsorbed at higher pH, but lower pH promoted defluorination. A membrane catalyst-film reactor (MCfR), containing an optimum loading of 1.2 g/m 2 Pd 0 for a total Pd amount of 22 mg, removed 3 mg/L PFOA during continuous flow for 90 days, and the removal flux was as high as 4 mg PFOA/m 2 /d at a steady state. The EPA health advisory level (70 ng/L) also was achieved over the 90 days with the influent PFOA at an environmentally relevant concentration of 500 ng/L. The results document a sustainable catalytic method for the detoxification of PFOA-contaminated water.
Databáze: MEDLINE
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