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Cellulose Nanofibril-based Hybrid Materials: Eco-friendly design towards separation and packaging applications
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0001-6572-7460
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Nanocellulose has been lately considered as the “Holy-Grail” in the design of sustainable materials due to its bio-origin and an unprecedented combination of prominent features, including good mechanical properties, anisotropy and versatile surface chemistry. In addition, nanocellulose in the form of cellulose nanofibrils, can adopt variable structures and morphologies depending on the processing technique, such as aerogels, films and monoliths.

However, there are limitations that hinder the implementation of cellulose nanofibrils in “real-life applications”, such as inherent interaction with bacteria and proteins, thus leading to surface-fouling; and loss of integrity due to water-induced swelling. A way to overcome these challenges, and provide further functionality, is through hybridization strategies, at which the multiple components act synergistically towards specific properties and applications. In this thesis, the aim is to present multiple strategies for the synthesis of novel cellulose nanofibril-based hybrid materials, in the form of 2D-films and 3D-foams, towards their employment for separation applications or active food packaging.

A novel strategy to surface-functionalize cellulose nanofibril-membranes is proposed via grafting zwitterionic polymer brushes of poly (cysteine methacrylate). The modification can suppress the absorption of proteins in an 85%, as well as decreasing the adhesion of bacteria in an 87%, while introducing antimicrobial properties, as demonstrated against S. aureus.

The spontaneous formation of functional metal oxide nanoparticles occurring in situ on cellulose nanofibrils-films during the adsorption of metal ions from water is investigated, which occurs without the additional use of chemicals or temperature. Notably, this process not only enables the upcycling of materials through multi-stage applications, but also provides a cost-effective method to prepare multifunctional hybrid materials with enhanced dye-removal/antimicrobial activity.

The processing of functional composite films from cellulose nanofibril-stabilized Pickering emulsions and their suitability to be used as active edible barriers was demonstrated. The presence of oil in the films fine-tuned the properties of the films, as well as acted as the medium to encapsulate bio-active hydrophobic compounds, providing further functionality such as antioxidant and antimicrobial properties.

Anisotropic porous hybrid foams with ultra-high loading capacity of sorbents (e.g., zeolites and metal-organic frameworks) were produced via unidirectional freeze-casting method using cellulose nanofibrils/gelatin as template material. The foams indeed exhibited ultra-high loading capacity of sorbent nanomaterials, a linear relationship between sorbent content and CO2 adsorption capacity, and high CO2/N2 selectivity.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University , 2019. , p. 35
Keywords [en]
Cellulose nanofibrils, hybrid materials, membranes, aerogels, separation, food packaging
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-175622ISBN: 978-91-7797-927-2 (print)ISBN: 978-91-7797-928-9 (electronic)OAI: oai:DiVA.org:su-175622DiVA, id: diva2:1368268
Public defence
2019-12-09, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 13:00 (English)
Opponent
Supervisors
Note

At the time of the doctoral defense, the following paper was unpublished and had a status as follows: Paper 2: Submitted.

Available from: 2019-11-14 Created: 2019-11-06 Last updated: 2019-11-08Bibliographically approved
List of papers
1. Fully bio-based zwitterionic membranes with superior antifouling and antibacterial properties prepared via surface-initiated free-radical polymerization of poly(cysteine methacrylate)
Open this publication in new window or tab >>Fully bio-based zwitterionic membranes with superior antifouling and antibacterial properties prepared via surface-initiated free-radical polymerization of poly(cysteine methacrylate)
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2018 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 6, no 34Article in journal (Refereed) Published
Abstract [en]

This article proposes a strategy to prepare membranes that combine the network characteristics of micro/nanocellulose with grafted zwitterionic poly(cysteine methacrylate) (PCysMA) to develop fully bio-based membranes with antifouling properties. The surface characteristics of the membranes were studied, together with static adsorption of bovine serum albumin (BSA) and S. aureus for evaluating the antifouling properties of the membranes. Experimental data revealed a homogeneous modification that resulted in excellent antifouling properties with a reduction of 85% in biofilm formation and enhanced antimicrobial activity. Moreover, we introduced a novel method to determine the pore size of membranes in the wet-state and assess the antifouling performance in situ by synchrotron-based SAXS. This allowed us to observe in real-time the decrease in pore size upon adsorption of BSA during filtration, and how this phenomenon is strongly suppressed by grafting of PCysMA. The importance of this work lies in introducing a simple method to yield cellulosic membranes with superior antifouling properties, which could significantly increase their potential for water treatment applications.

National Category
Chemical Sciences
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-161075 (URN)10.1039/c8ta06095a (DOI)000444698200010 ()
Available from: 2018-11-01 Created: 2018-11-01 Last updated: 2019-12-09Bibliographically approved
2. Unravelling the spontaneous formation of metal oxide nanoparticles on cellulose nanofibrils during adsorption of metal ions: A green alternative towards multifunctional hybrid materials
Open this publication in new window or tab >>Unravelling the spontaneous formation of metal oxide nanoparticles on cellulose nanofibrils during adsorption of metal ions: A green alternative towards multifunctional hybrid materials
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2019 (English)In: Article in journal (Refereed) Submitted
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-175621 (URN)
Available from: 2019-11-06 Created: 2019-11-06 Last updated: 2019-12-09Bibliographically approved
3. Biobased Cellulose Nanofibril–Oil Composite Films for Active Edible Barriers
Open this publication in new window or tab >>Biobased Cellulose Nanofibril–Oil Composite Films for Active Edible Barriers
2019 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 11, no 17, p. 16040-16047Article in journal (Refereed) Published
Abstract [en]

Low-concentration oil-in-water emulsions stabilized by cellulose nanofibrils (CNFs) extracted from primary plant cell wall materials are used to prepare thin biobased CNF–oil composite films by solvent casting. Flexible, transparent, and biodegradable composite films are obtained, with increased thermal stability (up to 300 °C) as the oil concentration increases. Examination of the microstructure demonstrates a clear dependency on the oil content, as a multilayered structure where the oil phase trapped between two layers of CNFs is appreciated at high oil concentrations. The embedded oil significantly influences the mechanical and wetting properties of the films, confirming their potential for use in packaging systems. Encapsulation of curcumin in the composite films leads to an increased antioxidant (up to 30% radical scavenging activity) and antimicrobial activity, inhibiting the growth of foodborne bacteria such as Escherichia coli. The resulting composite films show promising results in the field of active packaging for applications in the food, pharmaceutical, and cosmetic industries.

Keywords
active packaging, edible barrier, emulsion, nanocellulose, oleofilm
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-168658 (URN)10.1021/acsami.9b02649 (DOI)000466988800096 ()
Available from: 2019-05-02 Created: 2019-05-02 Last updated: 2019-11-06Bibliographically approved
4. Bio-based Micro-/Meso-/Macroporous Hybrid Foams with Ultrahigh Zeolite Loadings for Selective Capture of Carbon Dioxide
Open this publication in new window or tab >>Bio-based Micro-/Meso-/Macroporous Hybrid Foams with Ultrahigh Zeolite Loadings for Selective Capture of Carbon Dioxide
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2019 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 11, no 43, p. 40424-40431Article in journal (Refereed) Published
Abstract [en]

Microporous (<2 nm) crystalline aluminosilicates in the form of zeolites offer a great potential as efficient adsorbents for atmospheric CO2 in the eminent battle against global warming and climate change. The processability of conventional zeolite powders is, however, poor, which limits their implementation in many applications, such as in gas filtration industrial systems. In this work, we overcome this issue through the preparation of hybrid foams using mesoporous/macroporous supporting materials based on the strong network properties of gelatin/nanocellulose, which can support ultrahigh loadings of silicalite-1, used as a model sorbent nanomaterial. We achieved up to 90 wt % of zeolite content and a microporous/mesoporous/macroporous hybrid material. The application of hybrid foams for selective CO2 sorption exhibits a linear relationship between the zeolite content and CO2 adsorption capacity and high selectivity over N2, where the gelatin/nanocellulose foam efficiently supports the zeolite crystals without apparently blocking their pores.

Keywords
hybrid foams, nanocellulose, gelatin, zeolites, selective capture, CO2 adsorption
National Category
Chemical Sciences
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-175620 (URN)10.1021/acsami.9b11399 (DOI)000493869700104 ()
Available from: 2019-11-06 Created: 2019-11-06 Last updated: 2019-12-09Bibliographically approved
5. Nanocellulose leaf-like zeolitic imidazolate framework (ZIF-L) foams for selective capture of carbon dioxide
Open this publication in new window or tab >>Nanocellulose leaf-like zeolitic imidazolate framework (ZIF-L) foams for selective capture of carbon dioxide
2019 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 213, p. 338-345Article in journal (Refereed) Published
Abstract [en]

The last decades have been witness of an ever-growing interests for the synthesis and application of metal-organic frameworks (MOFs). However, most of the current synthetic procedures produce MOFs in powder state. In this work, hybrid foams were fabricated via in situ synthesis of leaf-like zeolitic imidazolate frameworks (ZIF-L) into nanocellulose at room temperature using water as solvent, followed by a gelatin matrix incorporation and freeze-drying. The foams are ultralight weight and are highly porous with densities ranging from 19.18 to 37.4 kg.m(-3). The shapeability, hierarchical porosity, and low density of the formed foams offer promising potentials for applications such as CO2 sorption. The dispersion of ZIF-L into the cellulose network increases the material accessibility and may open new venues for further MOFs processing.

Keywords
Nanocellulose, Foams, Metal-organic frameworks, Zeolitic imidazolate frameworks, CO2 adsorption
National Category
Chemical Sciences
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-167552 (URN)10.1016/j.carbpol.2019.03.011 (DOI)000461316200037 ()30879677 (PubMedID)
Available from: 2019-04-12 Created: 2019-04-12 Last updated: 2019-11-06Bibliographically approved

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