Linear Polyethyleneimine-Based and Metal Organic Frameworks (DUT-67) Composite Hydrogels as Efficient Sorbents for the Removal of Methyl Orange, Copper Ions, and Penicillin V

Author:

Araque Luis M.12ORCID,Fernández de Luis Roberto3,Fidalgo-Marijuan Arkaitz34,Infantes-Molina Antonia5ORCID,Rodríguez-Castellón Enrique5ORCID,Pérez Claudio J.6ORCID,Copello Guillermo J.12ORCID,Lázaro-Martínez Juan M.12ORCID

Affiliation:

1. Departamento de Ciencias Químicas, Facultad de Farmacia y Bioquímica, Universidad de Buenos Aires, Buenos Aires 1113, Argentina

2. Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET), Instituto de Química y Metabolismo del Fármaco (IQUIMEFA-UBA-CONICET), Buenos Aires 1113, Argentina

3. BCMaterials, Basque Center for Materials, Applications and Nanostructures, UPV/EHU Science Park, 48940 Leioa, Spain

4. Departamento de Química Orgánica e Inorgánica, Facultad de Ciencia y Tecnología, University of the Basque Country (UPV/EHU), 48940 Leioa, Spain

5. Departamento de Química Inorgánica, Cristalografía y Mineralogía, Facultad de Ciencias, Universidad de Málaga, 29010 Malaga, Spain

6. Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET), Instituto de Investigaciones en Ciencia y Tecnología de Materiales (INTEMA), Facultad de Ingeniería, Universidad de Mar del Plata, Mar del Plata 7600, Argentina

Abstract

This research explores the integration of DUT-67 metal organic frameworks into polyethyleneimine-based hydrogels to assemble a composite system with enough mechanical strength, pore structure and chemical affinity to work as a sorbent for water remediation. By varying the solvent-to-modulator ratio in a water-based synthesis path, the particle size of DUT-67 was successfully modulated from 1 μm to 200 nm. Once DUT-67 particles were integrated into the polymeric hydrogel, the composite hydrogel exhibited enhanced mechanical properties after the incorporation of the MOF filler. XPS, NMR, TGA, FTIR, and FT Raman studies confirmed the presence and interaction of the DUT-67 particles with the polymeric chains within the hydrogel network. Adsorption studies of methyl orange, copper(II) ions, and penicillin V on the composite hydrogel revealed a rapid adsorption kinetics and monolayer adsorption according to the Langmuir’s model. The composite hydrogel demonstrated higher adsorption capacities, as compared to the pristine hydrogel, showcasing a synergistic effect, with maximum adsorption capacities of 473 ± 21 mg L−1, 86 ± 6 mg L−1, and 127 ± 4 mg L−1, for methyl orange, copper(II) ions, and penicillin V, respectively. This study highlights the potential of MOF-based composite hydrogels as efficient adsorbents for environmental pollutants and pharmaceuticals.

Funder

Agencia Nacional de Promoción de la Investigación, el Desarrollo Tecnológico y la Innovación

Universidad de Buenos Aires

Ministry of Science and Innovation

“ERDF A way of making Europe” by the European Union NextGenerationEU/PRTR

Publisher

MDPI AG

Subject

Polymers and Plastics,Organic Chemistry,Biomaterials,Bioengineering

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