학술논문
Earth Abundant Oxidation Catalysts for Removal of Contaminants of Emerging Concern from Wastewater: Homogeneous Catalytic Screening of Monomeric Complexes.
Document Type
Article
Author
Garcia, Leslie; Koper, Makynna R.; Mondal, Somrita; Priddle, Joshua T.; Truong, William A.; Allbritton, Elisabeth M. A.; McAdoo, Ashtyn G.; Cannon-Smith, Desiray J.; Funwie, Neil L.; Hoang, Tuyet; Kim, Inseo; Hubin, David J.; Krause, Jeanette A.; Oliver, Allen G.; Prior, Timothy J.; Hubin, Timothy J.
Source
Subject
*EMERGING contaminants
*WATER purification
*CATALYTIC oxidation
*OXIDATION states
*BLEACHING (Chemistry)
*OXIDATION
*DYES & dyeing
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Language
ISSN
1420-3049
Abstract
Twenty novel Mn, Fe, and Cu complexes of ethylene cross-bridged tetraazamacrocycles with potentially copolymerizable allyl and benzyl pendant arms were synthesized and characterized. Multiple X-ray crystal structures demonstrate the cis-folded pseudo-octahedral geometry forced by the rigidifying ethylene cross-bridge and show that two cis coordination cites are available for interaction with substrate and oxidant. The Cu complexes were used to determine kinetic stability under harsh acidic and high-temperature conditions, which revealed that the cyclam-based ligands provide superior stabilization with half-lives of many minutes or even hours in 5 M HCl at 50–90 °C. Cyclic voltammetry studies of the Fe and Mn complexes reveal reversible redox processes indicating stabilization of Fe2+/Fe3+ and Mn2+/Mn3+/Mn4+ oxidation states, indicating the likelihood of catalytic oxidation for these complexes. Finally, dye-bleaching experiments with methylene blue, methyl orange, and rhodamine B demonstrate efficient catalytic decolorization and allow selection of the most successful monomeric catalysts for copolymerization to produce future heterogeneous water purification materials. [ABSTRACT FROM AUTHOR]