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Lignin nanoparticle-decorated nanocellulose cryogels as adsorbents for pharmaceutical pollutants
Univ Helsinki, Fac Agr & Forestry, Dept Food & Nutr, POB 66, FI-00014 Helsinki, Finland..ORCID iD: 0000-0001-9189-0851
Univ Helsinki, Fac Agr & Forestry, Dept Food & Nutr, POB 66, FI-00014 Helsinki, Finland..
Univ Helsinki, Fac Sci, Dept Chem, POB 55, FI-00014 Helsinki, Finland..ORCID iD: 0000-0002-3583-2064
VTT Tech Res Ctr Finland, POB 1000, FIN-02044 Espoo, Finland..
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2023 (English)In: Journal of Environmental Management, ISSN 0301-4797, E-ISSN 1095-8630, Vol. 330, article id 117210Article in journal (Refereed) Published
Abstract [en]

Adsorption is a relatively simple wastewater treatment method that has the potential to mitigate the impacts of pharmaceutical pollution. This requires the development of reusable adsorbents that can simultaneously remove pharmaceuticals of varying chemical structure and properties. Here, the adsorption potential of nanostructured wood-based adsorbents towards different pharmaceuticals in a multi-component system was investigated. The adsorbents in the form of macroporous cryogels were prepared by anchoring lignin nanoparticles (LNPs) to the nanocellulose network via electrostatic attraction. The naturally anionic LNPs were anchored to cationic cellulose nanofibrils (cCNF) and the cationic LNPs (cLNPs) were combined with anionic TEMPO-oxidized CNF (TCNF), producing two sets of nanocellulose-based cryogels that also differed in their overall surface charge density. The cryogels, prepared by freeze-drying, showed layered cellulosic sheets randomly decorated with spherical lignin on the surface. They exhibited varying selectivity and efficiency in removing pharmaceuticals with differing aromaticity, polarity and ionic characters. Their adsorption potential was also affected by the type (unmodified or cationic), amount and morphology of the lignin nanomaterials, as well as the pH of the pharmaceutical solution. Overall, the findings revealed that LNPs or cLNPs can act as functionalizing and crosslinking agents to nanocellulose-based cryogels. Despite the decrease in the overall positive surface charge, the addition of LNPs to the cCNF-based cryogels showed enhanced adsorption, not only towards the anionic aromatic pharmaceutical diclofenac but also towards the aromatic cationic metoprolol (MPL) and tramadol (TRA) and neutral aromatic carbamazepine. The addition of cLNPs to TCNF-based cryogels improved the adsorption of MPL and TRA despite the decrease in the net negative surface charge. The improved adsorption was attributed to modes of removal other than electrostatic attraction, and they could be 7C-7C aromatic ring or hydrophobic interactions brought by the addition of LNPs or cLNPs. However, significant improvement was only found if the ratio of LNPs or cLNPs to nanocellulose was 0.6:1 or higher and with spherical lignin nanomaterials. As crosslinking agents, the LNPs or cLNPs affected the rheological behavior of the gels, and increased the firmness and decreased the water holding capacity of the corresponding cryogels. The resistance of the cryogels towards disintegration with exposure to water also improved with crosslinking, which eventually enabled the cryogels, especially the TCNF-based one, to be regenerated and reused for five cycles of adsorption-desorption experiment for the model pharmaceutical MPL. Thus, this study opened new opportunities to utilize LNPs in providing nanocellulose-based adsorbents with additional functional groups, which were otherwise often achieved by rigorous chemical modifications, at the same time, crosslinking the nanocellulose network.

Place, publisher, year, edition, pages
Elsevier BV , 2023. Vol. 330, article id 117210
Keywords [en]
Nanocellulose, Lignin nanoparticles, Cryogels, Adsorption, Pharmaceutical pollutants, Multi-component
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-323770DOI: 10.1016/j.jenvman.2022.117210ISI: 000914964400001PubMedID: 36608603Scopus ID: 2-s2.0-85146025995OAI: oai:DiVA.org:kth-323770DiVA, id: diva2:1736995
Note

QC 20230215

Available from: 2023-02-15 Created: 2023-02-15 Last updated: 2023-02-15Bibliographically approved

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Oliaei, Erfan

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