Development of a β-cyclodextrin-chitosan polymer as active coating for cellulosic surfaces and capturing of microcystin-LR

Diego Gomez-Maldonado; Ilari Filpponen; Iris Beatriz Vega Erramuspe; Leena-Sisko Johansson; María Fernanda Mori; R. Jayachandra Babu; Matthew N. Waters; Maria S. Peresin

doi:10.1016/j.surfin.2022.102192

Development of a β-cyclodextrin-chitosan polymer as active coating for cellulosic surfaces and capturing of microcystin-LR

Diego Gomez-Maldonado
, Ilari Filpponen
, Iris Beatriz Vega Erramuspe
, Leena-Sisko Johansson
, María Fernanda Mori
, R. Jayachandra Babu
, Matthew N. Waters
, Maria S. Peresin^*

^*Corresponding author for this work

Auburn University
Universidad Nacional del Litoral

Research output: Contribution to journal › Article › Scientific › peer-review

21 Citations (Scopus)

Abstract

In the search for more environmentally friendly adsorbent materials, the use of polysaccharides results attractive. Especially, as they can be used as coatings to add functionality to common materials as a new avenue to explore. Their inherent tendency to adsorb into each other is valuable as it adds a variety of functional groups on the outmost surface layer. Our project focuses on the pre-modification of the bio-polymer chitosan (Ch) with a 2,2,6,6-Tetramethylpiperidine-1-oxyl (TEMPO) oxidized β-cyclodextrin (Ch-TOCD), which was then adsorbed onto the cellulose nanofibrils (CNF) surface. Furthermore, the mechanism driving the adsorption of the modified chitosan onto the cellulose backbone was studied by using three different Ch-TOCD conjugates possessing different degrees of substitutions. This was conducted to evaluate whether the adsorption was guided by the change of the available electrostatic interactions between the amino (Ch) and the residual carboxyl groups of cellulose or if the adsorption was driven by the dispersive forces of the hydroxyl groups from both polysaccharides. Finally, to assess the viability of the added hydrophobic cavities (Ch-TOCD conjugate), the capture of an amphipathic toxin categorized as a monitored pollutant (microcystin-LR) was followed by Quartz Crystal Microbalance with Dissipation monitoring (QCM-D) on a surface level and by High-performance liquid chromatography (HPLC) when the Ch-TOCD coating was applied in CNF beads. Results showed that the adsorption of Ch-TOCD was accomplished at similar levels independent of the degree of substitution. The highest adsorbed amounts of microcystin-LR were 20.5 mg/g on the model coated CNF surface, and 2.36 mg/g on the CNF coated beads. The successful coating of two nanocellulose systems and the positive adsorption of the microcystin suggest a broad-scale application of this bio-based, low energy input coating in high-end fields such as drug delivery, textile, and water restoration.

Original language	English
Article number	102192
Number of pages	12
Journal	Surfaces and Interfaces
Volume	33
Early online date	18 Jul 2022
DOIs	https://doi.org/10.1016/j.surfin.2022.102192
Publication status	Published - Oct 2022
MoE publication type	A1 Journal article-refereed

Funding

This work was supported by the National Science Foundation CAREER award 2119809 through the BMAT program in the Division of Materials Research and the EPSCoR program. Support was also provided by the USDA National Institute of Food and Agriculture, Hatch Program (ALA013-17003) and McIntire-Stennis Program (1022526). The School of Forestry and Wildlife Sciences at Auburn University's financial support to complete this work is much appreciated. This work made use of Aalto University Bioeconomy Facilities (the XPS statement), the FinnCERES - Competence Centre for the Materials Bioeconomy support is highly appreciated. This work was supported by the National Science Foundation CAREER award 2119809 through the BMAT program in the Division of Materials Research and the EPSCoR program. Support was also provided by the USDA National Institute of Food and Agriculture, Hatch Program ( ALA013-17003 ) and McIntire-Stennis Program ( 1022526 ). The School of Forestry and Wildlife Sciences at Auburn University's financial support to complete this work is much appreciated. This work made use of Aalto University Bioeconomy Facilities (the XPS statement), the FinnCERES - Competence Centre for the Materials Bioeconomy support is highly appreciated.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 6 Clean Water and Sanitation

Keywords

Active coatings
Cellulose beads
Green chemistry
Model surfaces
Physical adsorption
Water remediation

Access to Document

10.1016/j.surfin.2022.102192

Cite this

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title = "Development of a β-cyclodextrin-chitosan polymer as active coating for cellulosic surfaces and capturing of microcystin-LR",

abstract = "In the search for more environmentally friendly adsorbent materials, the use of polysaccharides results attractive. Especially, as they can be used as coatings to add functionality to common materials as a new avenue to explore. Their inherent tendency to adsorb into each other is valuable as it adds a variety of functional groups on the outmost surface layer. Our project focuses on the pre-modification of the bio-polymer chitosan (Ch) with a 2,2,6,6-Tetramethylpiperidine-1-oxyl (TEMPO) oxidized β-cyclodextrin (Ch-TOCD), which was then adsorbed onto the cellulose nanofibrils (CNF) surface. Furthermore, the mechanism driving the adsorption of the modified chitosan onto the cellulose backbone was studied by using three different Ch-TOCD conjugates possessing different degrees of substitutions. This was conducted to evaluate whether the adsorption was guided by the change of the available electrostatic interactions between the amino (Ch) and the residual carboxyl groups of cellulose or if the adsorption was driven by the dispersive forces of the hydroxyl groups from both polysaccharides. Finally, to assess the viability of the added hydrophobic cavities (Ch-TOCD conjugate), the capture of an amphipathic toxin categorized as a monitored pollutant (microcystin-LR) was followed by Quartz Crystal Microbalance with Dissipation monitoring (QCM-D) on a surface level and by High-performance liquid chromatography (HPLC) when the Ch-TOCD coating was applied in CNF beads. Results showed that the adsorption of Ch-TOCD was accomplished at similar levels independent of the degree of substitution. The highest adsorbed amounts of microcystin-LR were 20.5 mg/g on the model coated CNF surface, and 2.36 mg/g on the CNF coated beads. The successful coating of two nanocellulose systems and the positive adsorption of the microcystin suggest a broad-scale application of this bio-based, low energy input coating in high-end fields such as drug delivery, textile, and water restoration.",

keywords = "Active coatings, Cellulose beads, Green chemistry, Model surfaces, Physical adsorption, Water remediation",

author = "Diego Gomez-Maldonado and Ilari Filpponen and \{Vega Erramuspe\}, \{Iris Beatriz\} and Leena-Sisko Johansson and Mori, \{Mar{\'i}a Fernanda\} and Babu, \{R. Jayachandra\} and Waters, \{Matthew N.\} and Peresin, \{Maria S.\}",

note = "Funding Information: This work was supported by the National Science Foundation CAREER award 2119809 through the BMAT program in the Division of Materials Research and the EPSCoR program. Support was also provided by the USDA National Institute of Food and Agriculture, Hatch Program (ALA013-17003) and McIntire-Stennis Program (1022526). The School of Forestry and Wildlife Sciences at Auburn University's financial support to complete this work is much appreciated. This work made use of Aalto University Bioeconomy Facilities (the XPS statement), the FinnCERES - Competence Centre for the Materials Bioeconomy support is highly appreciated. Funding Information: This work was supported by the National Science Foundation CAREER award 2119809 through the BMAT program in the Division of Materials Research and the EPSCoR program. Support was also provided by the USDA National Institute of Food and Agriculture, Hatch Program ( ALA013-17003 ) and McIntire-Stennis Program ( 1022526 ). The School of Forestry and Wildlife Sciences at Auburn University's financial support to complete this work is much appreciated. This work made use of Aalto University Bioeconomy Facilities (the XPS statement), the FinnCERES - Competence Centre for the Materials Bioeconomy support is highly appreciated. Publisher Copyright: {\textcopyright} 2022",

year = "2022",

month = oct,

doi = "10.1016/j.surfin.2022.102192",

language = "English",

volume = "33",

journal = "Surfaces and Interfaces",

issn = "2468-0230",

publisher = "Elsevier",

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T1 - Development of a β-cyclodextrin-chitosan polymer as active coating for cellulosic surfaces and capturing of microcystin-LR

AU - Gomez-Maldonado, Diego

AU - Filpponen, Ilari

AU - Vega Erramuspe, Iris Beatriz

AU - Johansson, Leena-Sisko

AU - Mori, María Fernanda

AU - Babu, R. Jayachandra

AU - Waters, Matthew N.

AU - Peresin, Maria S.

N1 - Funding Information: This work was supported by the National Science Foundation CAREER award 2119809 through the BMAT program in the Division of Materials Research and the EPSCoR program. Support was also provided by the USDA National Institute of Food and Agriculture, Hatch Program (ALA013-17003) and McIntire-Stennis Program (1022526). The School of Forestry and Wildlife Sciences at Auburn University's financial support to complete this work is much appreciated. This work made use of Aalto University Bioeconomy Facilities (the XPS statement), the FinnCERES - Competence Centre for the Materials Bioeconomy support is highly appreciated. Funding Information: This work was supported by the National Science Foundation CAREER award 2119809 through the BMAT program in the Division of Materials Research and the EPSCoR program. Support was also provided by the USDA National Institute of Food and Agriculture, Hatch Program ( ALA013-17003 ) and McIntire-Stennis Program ( 1022526 ). The School of Forestry and Wildlife Sciences at Auburn University's financial support to complete this work is much appreciated. This work made use of Aalto University Bioeconomy Facilities (the XPS statement), the FinnCERES - Competence Centre for the Materials Bioeconomy support is highly appreciated. Publisher Copyright: © 2022

PY - 2022/10

Y1 - 2022/10

N2 - In the search for more environmentally friendly adsorbent materials, the use of polysaccharides results attractive. Especially, as they can be used as coatings to add functionality to common materials as a new avenue to explore. Their inherent tendency to adsorb into each other is valuable as it adds a variety of functional groups on the outmost surface layer. Our project focuses on the pre-modification of the bio-polymer chitosan (Ch) with a 2,2,6,6-Tetramethylpiperidine-1-oxyl (TEMPO) oxidized β-cyclodextrin (Ch-TOCD), which was then adsorbed onto the cellulose nanofibrils (CNF) surface. Furthermore, the mechanism driving the adsorption of the modified chitosan onto the cellulose backbone was studied by using three different Ch-TOCD conjugates possessing different degrees of substitutions. This was conducted to evaluate whether the adsorption was guided by the change of the available electrostatic interactions between the amino (Ch) and the residual carboxyl groups of cellulose or if the adsorption was driven by the dispersive forces of the hydroxyl groups from both polysaccharides. Finally, to assess the viability of the added hydrophobic cavities (Ch-TOCD conjugate), the capture of an amphipathic toxin categorized as a monitored pollutant (microcystin-LR) was followed by Quartz Crystal Microbalance with Dissipation monitoring (QCM-D) on a surface level and by High-performance liquid chromatography (HPLC) when the Ch-TOCD coating was applied in CNF beads. Results showed that the adsorption of Ch-TOCD was accomplished at similar levels independent of the degree of substitution. The highest adsorbed amounts of microcystin-LR were 20.5 mg/g on the model coated CNF surface, and 2.36 mg/g on the CNF coated beads. The successful coating of two nanocellulose systems and the positive adsorption of the microcystin suggest a broad-scale application of this bio-based, low energy input coating in high-end fields such as drug delivery, textile, and water restoration.

AB - In the search for more environmentally friendly adsorbent materials, the use of polysaccharides results attractive. Especially, as they can be used as coatings to add functionality to common materials as a new avenue to explore. Their inherent tendency to adsorb into each other is valuable as it adds a variety of functional groups on the outmost surface layer. Our project focuses on the pre-modification of the bio-polymer chitosan (Ch) with a 2,2,6,6-Tetramethylpiperidine-1-oxyl (TEMPO) oxidized β-cyclodextrin (Ch-TOCD), which was then adsorbed onto the cellulose nanofibrils (CNF) surface. Furthermore, the mechanism driving the adsorption of the modified chitosan onto the cellulose backbone was studied by using three different Ch-TOCD conjugates possessing different degrees of substitutions. This was conducted to evaluate whether the adsorption was guided by the change of the available electrostatic interactions between the amino (Ch) and the residual carboxyl groups of cellulose or if the adsorption was driven by the dispersive forces of the hydroxyl groups from both polysaccharides. Finally, to assess the viability of the added hydrophobic cavities (Ch-TOCD conjugate), the capture of an amphipathic toxin categorized as a monitored pollutant (microcystin-LR) was followed by Quartz Crystal Microbalance with Dissipation monitoring (QCM-D) on a surface level and by High-performance liquid chromatography (HPLC) when the Ch-TOCD coating was applied in CNF beads. Results showed that the adsorption of Ch-TOCD was accomplished at similar levels independent of the degree of substitution. The highest adsorbed amounts of microcystin-LR were 20.5 mg/g on the model coated CNF surface, and 2.36 mg/g on the CNF coated beads. The successful coating of two nanocellulose systems and the positive adsorption of the microcystin suggest a broad-scale application of this bio-based, low energy input coating in high-end fields such as drug delivery, textile, and water restoration.

KW - Active coatings

KW - Cellulose beads

KW - Green chemistry

KW - Model surfaces

KW - Physical adsorption

KW - Water remediation

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DO - 10.1016/j.surfin.2022.102192

M3 - Article

AN - SCOPUS:85134599097

SN - 2468-0230

VL - 33

JO - Surfaces and Interfaces

JF - Surfaces and Interfaces

M1 - 102192

ER -

Development of a β-cyclodextrin-chitosan polymer as active coating for cellulosic surfaces and capturing of microcystin-LR

Abstract

Funding

UN SDGs

Keywords

Access to Document

Other files and links

Fingerprint

FinnCERES: Competence Center for the Materials Bioeconomy: A Flagship for our Sustainable Future

Bioeconomy Research Infrastructure

Cite this

Development of a β-cyclodextrin-chitosan polymer as active coating for cellulosic surfaces and capturing of microcystin-LR

Abstract

Funding

UN SDGs

Keywords

Access to Document

Other files and links

Fingerprint

Projects

FinnCERES: Competence Center for the Materials Bioeconomy: A Flagship for our Sustainable Future

Equipment

Bioeconomy Research Infrastructure

Cite this