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Adsorption Behavior of Cellulose and Its Derivatives toward Ag(I) in Aqueous Medium: An AFM, Spectroscopic, and DFT Study
Luleå University of Technology, Sweden.
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Number of Authors: 62015 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 31, no 45, p. 12390-12400Article in journal (Refereed) Published
Abstract [en]

The aim of this study was to develop a fundamental understanding of the adsorption behavior of metal ions on cellulose surfaces using experimental techniques supported by computational modeling, taking Ag(I) as an example. Force interactions among three types of cellulose microspheres (native cellulose and its derivatives with sulfate and phosphate groups) and the silica surface in AgNO3 solution were studied with atomic force microscopy (AFM) using the colloidal probe technique. The adhesion force between phosphate cellulose microspheres (PCM) and the silica surface in the aqueous AgNO3 medium increased significantly with increasing pH while the adhesion force slightly decreased for sulfate cellulose microspheres (SCM), and no clear adhesion force was observed for native cellulose microspheres (CM). The stronger adhesion enhancement for the PCM system is mainly attributed to the electrostatic attraction between Ag(I) and the negative silica surface. The observed force trends were in good agreement with the measured zeta potentials. The scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR) analyses confirmed the presence of silver on the surface of cellulose microspheres after adsorption. This study showed that PCM with a high content of phosphate groups exhibited a larger amount of adsorbed A(I) than CM and SCM and possible clustering of Ag(I) to nanoparticles. The presence of the phosphate group and a wavenumber shift of the P-OH vibration caused by the adsorption of silver ions on the phosphate groups were further confirmed with computational studies using density functional theory (DFT), which gives support to the above findings regarding the adsorption and clustering of Ag(I) on the cellulose surface decorated with phosphate groups as well as IR spectra.

Place, publisher, year, edition, pages
2015. Vol. 31, no 45, p. 12390-12400
National Category
Chemical Sciences
Research subject
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-124757DOI: 10.1021/acs.langmuir.5b03228ISI: 000365150700009PubMedID: 26501836OAI: oai:DiVA.org:su-124757DiVA, id: diva2:892146
Available from: 2016-01-08 Created: 2016-01-04 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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