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Microwave carbonized cellulose for trace pharmaceutical adsorption
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.ORCID iD: 0000-0002-5850-8873
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Industrial Biotechnology.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Polymer Technology.ORCID iD: 0000-0002-7790-8987
2018 (English)In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 346, p. 557-566Article in journal (Refereed) Published
Abstract [en]

A promising sustainable strategy to valorize cellulose to high-value adsorbents for trace pharmaceuticals, like diclofenac sodium (DCF), in the water is demonstrated. Carbon nanospheres (CN) as the DCF adsorbent were derived from cellulose through a one-pot microwave-assisted hydrothermal carbonization method. CN exhibited efficient DCF removal (100% removal of 0.001 mg/mL DCF in 30 s and 59% removal of 0.01 mg/mL DCF in 1 h). The adsorption kinetics and isotherm data were well-fitted with the pseudo-second-order kinetic model and Langmuir model, respectively. The adsorption process was endothermic and spontaneous as confirmed by the thermodynamic parameters. Multiple characterization techniques including SEM/EDS, FTIR, FTIR-imaging and zeta potential were applied to qualitatively investigate the adsorption process. π-π stacking and hydrogen bonding were proposed as the dominant adsorption interactions. CN also demonstrated effective adsorption capacity towards three other commonly-detected contaminants in the wastewater including ketoprofen (KP), benzophenone (BZP), and diphenylamine (DPA), each bearing partial structural similarity with DCF. The affinity of the contaminants towards CN followed the order DPA > BZP > DCF > KP, which could be explained by the different configurations and chemical units. It was speculated that for DCF and KP, the steric hindrance and electrostatic repulsion produced by dissociated carboxyl groups can impede the adsorption process as compared to DPA and BZP. This methodology could offer further insights into the drug adsorption on the cellulose-derived carbon adsorbents and the use of bioderived carbons for treatment of wastewaters contaminated with pharmaceuticals.

Place, publisher, year, edition, pages
Elsevier, 2018. Vol. 346, p. 557-566
Keywords [en]
Adsorption, Carbon nanosphere, Carbonization, Cellulose, Diclofenac, Microwave
National Category
Chemical Sciences Polymer Technologies
Identifiers
URN: urn:nbn:se:kth:diva-227509DOI: 10.1016/j.cej.2018.04.014ISI: 000432878400057Scopus ID: 2-s2.0-85045434362OAI: oai:DiVA.org:kth-227509DiVA, id: diva2:1207013
Note

QC 20180518

Available from: 2018-05-18 Created: 2018-05-18 Last updated: 2019-04-10Bibliographically approved
In thesis
1. From Polysaccharides to Functional Materials for Trace Pharmaceutical Adsorption
Open this publication in new window or tab >>From Polysaccharides to Functional Materials for Trace Pharmaceutical Adsorption
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The transition to bioeconomy will reduce our dependency on fossil fuels as well as contribute to a more sustainable society. Within this framework, exploitation and development of renewable substitutes to petroleum-based products provides feasible roadmap for the material design. Here a perspective is provided to how the natural polysaccharides chitosan (CS) and/or cellulose (CL) could be elaborated and transformed to high-performance materials with the explicit aim of removing trace pharmaceutical contaminants from the wastewater, thus facilitating the sustainable development. In the first part of the thesis, chitosan and cellulose were converted to the carbon spheres (C-sphere) through a microwave-assisted hydrothermal carbonization process, and C-sphere was further broken down to the nanographene oxide (nGO) via a simple oxidation route. On this foundation, a green pathway was developed for fabrication of biobased materials for wastewater purification. First, macroporous chitosan-based composite hydrogels with controllable properties were developed, where chitosan-derived nGO worked as a functional property enhancer. Second, a further development changing from the bulky hydrogels to microgels consisting of CS composite particles in the microscopic size was achieved by a fast one-pot spraying-drying process. The crosslinking reaction occurred in situ during the spray-drying. Last, the C-sphere by-itself was also believed to be a potential adsorbent for wastewater contaminants. In the next step the prepared systems were evaluated for their capacity to adsorb pharmaceutical contaminants. Diclofenac sodium (DCF) was utilized as the model drug, and the three fabricated bio-adsorbents all demonstrated effective DCF adsorption performance, with the adsorption efficiency varying from 65.6 to 100%. Moreover, the DCF adsorption kinetics, isotherms and thermodynamic study were also investigated to reveal the nature of the adsorption process with the different materials. Finally, chitosan-based microspheres were selected for the reusability study, with the adsorption efficiency above 70% retained after six adsorption-desorption cycles, thus further endowing the promising potential of the fabricated bio-adsorbents for commercial applications.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2019. p. 48
Series
TRITA-CBH-FOU ; 2019:21
Keywords
Chitosan, cellulose, nanographene oxide, carbon spheres, hydrogel, microsphere, adsorbent, pharmaceutical, microwave, spray-drying
National Category
Environmental Engineering Nano Technology Textile, Rubber and Polymeric Materials Physical Chemistry Polymer Chemistry
Research subject
Fibre and Polymer Science
Identifiers
urn:nbn:se:kth:diva-248454 (URN)978-91-7873-167-1 (ISBN)
Public defence
2019-05-23, F3, Lindstedtsvägen 26, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 20190411

Available from: 2019-04-11 Created: 2019-04-09 Last updated: 2019-05-27Bibliographically approved

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Feng, ZhaoxuanOdelius, KarinRajarao, Gunaratna KuttuvaHakkarainen, Minna

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