Materials for Selective and Sustainable HydroCarbon Removal from Water
Synthesis and Properties of Functional Materials
Final Report Abstract
Water is essential for all life on earth – yet the supply of clean water in sufficient quantities is at risk. A crucial class of contaminants relate to the excessive use of hydrocarbons (HCs) including fossil fuels and all oil-based chemical refined products, which differ in their chemical structure, their molecular weight, and their properties. The concept of magnetic water cleaning is to collect HC contaminants magnetically. Naturally, HCs and their derivatives are not magnetic, but they can adsorb on surfaces of magnetic carriers. Once added, the loaded carriers (super paramagnetic iron oxide nanoparticles - SPIONs) can be removed from the water phase using common magnetic separation approaches. (SPIONs) exhibit large surface-to-volume ratios of > 100 m2ꞏ g–1 and attract efficiently to external magnetic fields. Chemically, SPIONs are particles smaller than 30 nm diameter of magnetite (Fe3O4) or maghemite (Fe2O3) – basically, they are harmless inexpensive rust. Within the project we have developed tailored surface functionalization of SPIONs, that allow to efficiently adsorb and to remove HCs from water - or more specifically to implement chemical recognition motifs towards dedicated HC contaminants to upgrade the simple rust to “smart rust”. We have realized SPION systems that are able to remediate HCs from small molecular hexane (liquid molecule with six carbon units) to cross-linked polyethylene (PE) microplastics (solid with infinite number of carbon units). Besides targeting simple alkylbased HCs [-CH2)n-], we have developed smart SPIONs that are able to remediate microand nanoplastics of different size (100 nm – 100 µm) and chemical composition (PS, PMMA, melamine resin, PE) as well as charge derivatives of aromatic compounds or soaps. We have created a huge library of novel smart SPIONs that allow further tailoring towards other classes of contaminants (e.g. hormones). In collaboration with groups from our university and external partners we could gain a fundamental understanding in the active principle of the interaction of contaminants with functional SPION surfaces and we have shown that these chemical recognitions can be used in highly responsive and highly selective sensors. Additional to efficient remediation of HCs with SPIONs we have addressed the aspect of sustainability of our concept/materials. We have demonstrated full loop recycling of SPIONs and even an upcycling concept as well as their non-toxicity. As output of the project we have published (so far) 9 peer-reviewed original research articles and we have widely contributed to scientific communication to the public audience by articles, TV reports or public events (e.g. panel discussions or pupil seminars).
Publications
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Chemical-recognition-driven selectivity of SnO2-nanowire-based gas sensors. Nano Today, 40, 101265.
Park, Hyoungwon; Kim, Jae-Hun; Vivod, Dustin; Kim, Sungil; Mirzaei, Ali; Zahn, Dirk; Park, Changkyoo; Kim, Sang Sub & Halik, Marcus
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Magnetic water cleaning. Nachrichten aus der Chemie, 69(9), 43-46.
Halik, Marcus; Sarcletti, Marco & Zahn, Dirk
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The remediation of nano-/microplastics from water. Materials Today, 48, 38-46.
Sarcletti, Marco; Park, Hyoungwon; Wirth, Janis; Englisch, Silvan; Eigen, Andreas; Drobek, Dominik; Vivod, Dustin; Friedrich, Bernhard; Tietze, Rainer; Alexiou, Christoph; Zahn, Dirk; Apeleo, Zubiri Benjamin; Spiecker, Erdmann & Halik, Marcus
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A universal concept for area‐selective assembly of metal oxide core‐shell nanoparticles, nanorods, and organic molecules via amide coupling reactions. Nano Select, 3(8), 1223-1231.
Zubets, Uladzislau; Zhao, Baolin; Park, Hyoungwon & Halik, Marcus
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Facile strategy for advanced selectivity and sensitivity of SnO2 nanowire-based gas sensor using chemical affinity and femtosecond laser irradiation. Sensors and Actuators B: Chemical, 372, 132657.
Park, Hyoungwon; Kim, Jae-Hun; Shin, Won-Sang; Mirzaei, Ali; Kim, Yoon-Jun; Kim, Sang Sub; Halik, Marcus & Park, Changkyoo
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Real-time monitoring of magnetic nanoparticle-assisted nanoplastic agglomeration and separation from water. Environmental Science: Nano, 9(7), 2427-2439.
Groppe, Philipp; Wintzheimer, Susanne; Eigen, Andreas; Gaß, Henrik; Halik, Marcus & Mandel, Karl
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Tunable Composition of Mixed Self‐Assembled Shell‐by‐Shell Structures on Nanoparticle Surfaces. Advanced Materials Interfaces, 9(32).
Eigen, Andreas; Stiegler, Lisa M. S.; Gradl, Susanne; Schneider, Vanessa; Wedler, Vincent; Gaß, Henrik; Müller, Lukas; Sarcletti, Marco; Heinrich, Markus R.; Hirsch, Andreas & Halik, Marcus
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A Sustainable Method for Removal of the Full Range of Liquid and Solid Hydrocarbons from Water Including Up‐ and Recycling. Advanced Science, 10(32).
Gaß, Henrik; Sarcletti, Marco; Müller, Lukas; Hübner, Sabine; Yokosawa, Tadahiro; Park, Hyoungwon; Przybilla, Thomas; Spiecker, Erdmann & Halik, Marcus
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Magnetic Removal of Micro‐ and Nanoplastics from Water—from 100 nm to 100 µm Debris Size. Small, 20(10).
Gaß, Henrik; Kloos, Tonya M.; Höfling, Anna; Müller, Lukas; Rockmann, Linda; Schubert, Dirk W. & Halik, Marcus
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Remediation of charged organic pollutants—binding motifs for highly efficient water cleaning with nanoparticles. Nano Select, 5(1).
Eigen, Andreas; Schmidt, Victoria; Sarcletti, Marco; Freygang, Selina; Hartmann‐Bausewein, Andreas; Schneider, Vanessa; Zehetmeier, Anna; Mauritz, Vincent; Müller, Lukas; Gaß, Henrik; Rockmann, Linda; Crisp, Ryan W. & Halik, Marcus
