Redox-Active Magnetic Composites for Anionic Contaminant Removal from Water

Kai Jher Tan; Satoshi Morikawa; Katherine R. Phillips; Nil Ozbek; T. Alan Hatton

doi:10.1021/acsami.1c21466

Redox-Active Magnetic Composites for Anionic Contaminant Removal from Water

Kai Jher Tan, Satoshi Morikawa, Katherine R. Phillips, Nil Ozbek, T. Alan Hatton^*

^*Corresponding author for this work

Massachusetts Institute of Technology

Research output: Contribution to journal › Article › peer-review

19 Citations (Scopus)

Abstract

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.

Original language	English
Pages (from-to)	8974-8983
Number of pages	10
Journal	ACS applied materials & interfaces
Volume	14
Issue number	7
DOIs	https://doi.org/10.1021/acsami.1c21466
Publication status	Published - 23 Feb 2022
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.

Funding

This work made use of the Materials Research Science and Engineering Centers (MRSEC) Shared Experimental Facilities at the Massachusetts Institute of Technology (supported by the National Science Foundation under Award No. DMR 1419807), the Center for Environmental Health Sciences at the Massachusetts Institute of Technology (supported by the National Institute of Environmental Health Sciences, National Institutes of Health under core center Grant No. P30-ES002109), the Institute for Solider Nanotechnologies (ISN) at the Massachusetts Institute of Technology, the Department of Chemistry Instrumentation Facility (DCIF) at the Massachusetts Institute of Technology, and the Center for Nanoscale Systems (CNS) at Harvard University (supported by the National Science Foundation under Award No. 1541959). The authors gratefully thank Prof. Takuya Harada for insightful discussions and help with initial material preparation. K.-J.T. was supported by a Natural Sciences and Engineering Research Council (NSERC) postgraduate doctoral scholarship (PGS D). N.O. greatly appreciates the support by The Scientific and Technological Research Council of Turkey (TUBITAK), 2219 International Postdoctoral Research Scholarship Program. K.-J.T. was supported by a Natural Sciences and Engineering Research Council (NSERC) postgraduate doctoral scholarship (PGS D). N.O. greatly appreciates the support by The Scientific and Technological Research Council of Turkey (TÜBİTAK), 2219 International Postdoctoral Research Scholarship Program.

Funders	Funder number
Center for Environmental Health Sciences
Center for Nanoscale Systems
Department of Chemistry Instrumentation Facility
Institute for Solider Nanotechnologies
TUBITAK
National Science Foundation	DMR 1419807
National Institutes of Health	P30-ES002109
National Institute of Environmental Health Sciences
Massachusetts Institute of Technology
Harvard University	1541959
Materials Research Science and Engineering Center, Harvard University
Natural Sciences and Engineering Research Council of Canada
Türkiye Bilimsel ve Teknolojik Araştirma Kurumu

Keywords

aqueous
contaminant
ferrocene
ion
magnetic
pyrrole
separation

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsami.1c21466

Cite this

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abstract = "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.",

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AU - Hatton, T. Alan

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ER -

Redox-Active Magnetic Composites for Anionic Contaminant Removal from Water

Abstract

Bibliographical note

Funding

Keywords

UN SDGs

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