Fluorinated pharmaceuticals are of increasing interest among pharmaceutical industry because they have improved pharmacological properties compared to their non-fluorinated analogues without significantly altering their sizes and shapes. With their growing uses, fluorinated pharmaceuticals such as fluoxetine have been detected in natural and engineered water systems. While most pharmaceuticals can be transformed to recalcitrant products via advanced oxidation technology, C-F bonds in fluorinated pharmaceuticals do not readily break up and only limited study is available on toxicity and fate of fluorine-containing intermediates in the environment. There is a need for a novel treatment process that can defluorinate and transform these contaminants. In this study, we firstly report the feasibility of heterogeneous bimetallic catalysts (i.e., Pd-Rh/Al2O3, Rh-Pt/Al2O3, Pd-Pt/Al2O3, Pd-Ru/Al2O3, Ph-Ru/Al2O3, and Pt-Ru/Al2O3) for reductive defluorination and degradation of four fluorinated pharmaceuticals (i.e., Fluoxetine (FLX), Flunixin (FX), Levofloxacin (LFX), and Sitagliptin (SGT)). Kinetic experiments of reduction and defluorination of fluorinated pharmaceuticals were conducted using monometallic catalysts of Pd, Rh, Pt, and Ru and bimetallic catalysts of combinations of these metals in the presence of H2 as reductant. The degradation products and intermediates were determined using analytical instruments such as LC-MS and GC-MS. Different reduction pathways were observed for different metal combinations and Pd-Ru bimetallic catalysts exhibited fastest reduction kinetics compared to other catalysts. A series of characterization techniques such as field-emission TEM, H2-pulse chemisorption, and X-ray photoelectron spectroscopy were performed to investigate physicochemical properties of catalysts and their changes after the reaction. We have also investigated effect of various environmental parameters (e.g., metal loading, catalyst loading, and pH) on the catalytic activity as well as longevity of catalyst over repeated cycles of reduction experiments.

Reductive defluorination and removal of aqueous fluorinated pharmaceuticals using heterogeneous alumina supported bimetallic catalysts

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.