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Self-Assembled TEMPO Cellulose Nanofibers: Graphene Oxide-Based Biohybrids for Water Purification
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Number of Authors: 32017 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 24, p. 21048-21058Article in journal (Refereed) Published
Abstract [en]

Nanocellulose, graphene oxide (GO), and their combinations there off have attracted great attention for the application of water purification recently because of their unique adsorption capacity, mechanical characteristics, coordination with transition metal ions, surface charge density, and so on. In the current study, (2,2,6,6-tetramethylpiperidine-1-oxylradical) (TEMPO)-mediated oxidized cellulose nanofibers (TOCNF) and GO sheets or graphene oxide nanocolloid (nanoGO) biohybrids were prepared by vacuum filtration method to obtain self-assembled adsorbents and membranes for water purification. The porous biohybrid structure, studied using advanced microscopy techniques, revealed a unique networking and self-assembling of TOCNF, GO, and nanoGO, driven by the morphology of the GO phase and stabilized by the intermolecular H-bonding between carboxyl groups and hydroxyl groups. The biohybrids exhibited a promising adsorption capacity toward Cu(II) due to TOCNF and formed a unique arrested state in water because of ionic cross-linking between adsorbed Cu(II) and the negatively charged TOCNF and GO phase. The mechanical performance of the freestanding biohybrid membranes investigated using PeakForce Quantative NanoMechanics characterization confirmed the enhanced modulus of the hybrid membrane compared to that of the TOCNF membrane. Besides, the TOCNF+nanoGO membrane shows unique hydrolytic stability and recyclability even under several cycles of adsorption and desorption and strong sonication. This study shows that TOCNF and nanoGO hybrids can generate new water-cleaning membranes with synergistic properties because of their high adsorption capacity, flexibility, hydrolytic stability, and mechanical robustness.

Place, publisher, year, edition, pages
2017. Vol. 9, no 24, p. 21048-21058
Keywords [en]
TEMPO cellulose nanofibers, graphene oxide nanocolloids, biohybrid, water purification, PF-QNM
National Category
Chemical Sciences
Research subject
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-145202DOI: 10.1021/acsami.7b06358ISI: 000404090000087PubMedID: 28557432OAI: oai:DiVA.org:su-145202DiVA, id: diva2:1128923
Available from: 2017-07-31 Created: 2017-07-31 Last updated: 2018-04-23Bibliographically approved
In thesis
1. Nanocellulose and Its Biohybrids for Water Purification: Atomic Force Microscopy as a Tool to Probe Surface Properties and Interactions
Open this publication in new window or tab >>Nanocellulose and Its Biohybrids for Water Purification: Atomic Force Microscopy as a Tool to Probe Surface Properties and Interactions
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Nanocellulose has been explored extensively in recent years as an adsorbent due to its promising performance in the removal of charged contaminants from water. In this thesis, various atomic force microscopy (AFM) techniques are used to understand the surface characteristics and specific interactions of nanocellulose with water contaminants (heavy metal ions and dyes) and nanoscale entities (Graphene Oxide (GO) and Graphene Oxide nanocolloids (nanoGO)), and explain the mechanisms related to adsorption, metal ion clustering, self-assembly and mechanical reinforcement.

AFM probes functionalised with microscale and nanoscale celluloses were used as colloidal probes to study specific surface interactions with heavy metal ions and dyes in the aqueous medium. This approach enabled quantitative measurements of the adhesion force between nanocellulose and the water pollutants under in situ conditions by direct or in-direct methods. Adhesion forces, including the piconewton range, were measured, and the forces depended on the surface groups present on the nanocellulose.

AFM imaging in dry and/or wet conditions was successfully used to investigate the adsorption, self-assembly, morphology and mechanical properties of nanocellulose and its bio-hybrids. The self-assembly, the metal nanolayer and the nanoclusters on the surface of nanocellulose and its biohybrids after adsorption were confirmed and explained by advanced microscopy, spectroscopy and computational modelling.

The adhesion and stiffness measurement of single nanocellulose fibers using in situ PeakForce Quantitative Nanomechanical (PF-QNM) characterization confirmed the adsorption of metal ions on the surface in the liquid medium. PF-QNM mapping of the freestanding biohybrid membranes also revealed the enhanced modulus of the biohybrid membrane compared with the TEMPO(2,2,6,6-tetramethylpiperidine-1-oxylradical)-mediated oxidation nanofibers (TOCNF) membrane, which explained the hydrolytic stability and recyclability of these membranes.

The established methodology, which combines advanced microscopy with spectroscopy and modelling techniques, can be extended to other biobased macromolecular systems to investigate the adsorption behaviour and/or surface interactions in bio nanotechnology.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry (MMK), Stockholm University, 2018. p. 23
Keywords
Atomic force microscopy, nanocellulose, water purification, surface interaction, biohybrids, self-assembly, metal ion clustering
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-155373 (URN)978-91-7797-260-0 (ISBN)978-91-7797-261-7 (ISBN)
Public defence
2018-06-08, Magnéli Hall, Arrhenius Laboratory, Svante Arrhenius väg 16 B, Stockholm, 09:30 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 4: Manuscript. Paper 5: Manuscript.

Available from: 2018-05-16 Created: 2018-04-19 Last updated: 2018-05-09Bibliographically approved

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