TY - JOUR
T1 - Redox-Active Magnetic Composites for Anionic Contaminant Removal from Water
AU - Tan, Kai Jher
AU - Morikawa, Satoshi
AU - Phillips, Katherine R.
AU - Ozbek, Nil
AU - Hatton, T. Alan
N1 - Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/2/23
Y1 - 2022/2/23
N2 - Global water security is jeopardized by the presence of anthropogenic contaminants, which can persist resiliently in the environment and adversely affect human health. Surface adsorption of polluting species is an effective technique for water purification. In this work, redox-active magnetic compounds were designed for the targeted removal of inorganic and organic anions in water via polymeric redox-active vinylferrocene (VFc) and pyrrole (Py) moieties. An Fe3O4@SiO2@PPy@P(VFc-co-HEMA) composite was prepared in a four-step process, with the outermost layer possessing heightened hydrophilicity as a result of the optimized incorporation of 2-hydroxyethylmethacrylate (HEMA) monomers into the backbone of the ferrocene macromolecule. The synthesized materials are able to separate carcinogenic hexavalent chromium oxyanions and other charged micropollutants, and exhibit a 2-fold or greater enhancement in adsorption uptake once the redox-active ferrocene groups are oxidized to ferrocenium cations, with capacities of 23, 49, 66, and 95 mg/g VFc for maleic acid, 2-(6-methoxy-2-naphthyl)propionic acid (Naproxen), (2,4-dichlorophenoxy)acetic acid (2,4-D), and (2-dodecylbenzene)sulfonic acid (DBS), respectively, and a > 99% extractability of chromium in the 1 ppm range. The application of redox-active components to a magnetic particulate scaffold improves maneuverability and phase contact, giving rise to new potential aqueous separation process frameworks for water or product purification.
AB - Global water security is jeopardized by the presence of anthropogenic contaminants, which can persist resiliently in the environment and adversely affect human health. Surface adsorption of polluting species is an effective technique for water purification. In this work, redox-active magnetic compounds were designed for the targeted removal of inorganic and organic anions in water via polymeric redox-active vinylferrocene (VFc) and pyrrole (Py) moieties. An Fe3O4@SiO2@PPy@P(VFc-co-HEMA) composite was prepared in a four-step process, with the outermost layer possessing heightened hydrophilicity as a result of the optimized incorporation of 2-hydroxyethylmethacrylate (HEMA) monomers into the backbone of the ferrocene macromolecule. The synthesized materials are able to separate carcinogenic hexavalent chromium oxyanions and other charged micropollutants, and exhibit a 2-fold or greater enhancement in adsorption uptake once the redox-active ferrocene groups are oxidized to ferrocenium cations, with capacities of 23, 49, 66, and 95 mg/g VFc for maleic acid, 2-(6-methoxy-2-naphthyl)propionic acid (Naproxen), (2,4-dichlorophenoxy)acetic acid (2,4-D), and (2-dodecylbenzene)sulfonic acid (DBS), respectively, and a > 99% extractability of chromium in the 1 ppm range. The application of redox-active components to a magnetic particulate scaffold improves maneuverability and phase contact, giving rise to new potential aqueous separation process frameworks for water or product purification.
KW - aqueous
KW - contaminant
KW - ferrocene
KW - ion
KW - magnetic
KW - pyrrole
KW - separation
UR - http://www.scopus.com/inward/record.url?scp=85125211912&partnerID=8YFLogxK
U2 - 10.1021/acsami.1c21466
DO - 10.1021/acsami.1c21466
M3 - Article
C2 - 35144378
AN - SCOPUS:85125211912
SN - 1944-8244
VL - 14
SP - 8974
EP - 8983
JO - ACS applied materials & interfaces
JF - ACS applied materials & interfaces
IS - 7
ER -