Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Stimuli-Responsive Materials Derived from Cellulose Nanofibrils: Synthesis, characterization, and performance evaluation
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0003-3334-9076
2024 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis presents a comprehensive study on stimuli-responsive materials derived from cellulose nanofibrils (CNFs), focusing on their synthesis, characterization, and performance evaluation in various applications. Renowned for their biodegradability, renewability, and robust mechanical properties, CNFs are explored in three primary contexts: moisture-responsive actuators, voltage-responsive actuators, and CO2-responsive sensors.

The unique properties of CNFs, such as high tensile strength and surface area, are leveraged to achieve effective motion in response to moisture exposure. Specifically, CNFs are utilized to create bilayer, torsional, and tensile actuators. These actuators exhibit controllable and dynamic responses, making them suitable for applications in soft robotics and wearable technology.

In the realm of voltage-responsive actuators, this study investigates the impact of various electrolytes and counteranions on positively charged CNFs. It uncovers the critical role of electrolyte choice, ion migration and the plasticization effect within the CNFs matrix, resulting in volumetric expansion, which is pivotal to the actuation mechanism. These insights pave the way for CNFs applications requiring precise control of motion and flexibility in shape, such as in soft robotics.

The third area of application involves the development of a capacitive CO2 sensor using CNFs-based foams functionalized with primary amines to enhance CO2 capture through chemisorption. This functionalization turns the CNFs-based foam into an efficient dielectric layer (DE) for sensor applications. The addition of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) to the DE further expands the scope of sensor's capacitance change in response to CO2 exposure, underscoring its potential in environmental monitoring and CO2 detection.

Overall, this thesis emphasizes the versatility and adaptability of CNFs as a sustainable biomaterial for developing stimuli-responsive devices. The insights gained from studying CNFs in these varied applications contribute significantly to materials science and open new avenues for research in sustainable, bio-based materials.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University , 2024. , p. 45
Keywords [en]
bio-based materials, cellulose nanofibrils, CO2 sorption, soft actuators, stimuli-responsive materials
National Category
Materials Chemistry Biomaterials Science
Research subject
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-224538ISBN: 978-91-8014-627-2 (print)ISBN: 978-91-8014-628-9 (electronic)OAI: oai:DiVA.org:su-224538DiVA, id: diva2:1820259
Public defence
2024-02-16, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2024-01-24 Created: 2023-12-17 Last updated: 2024-01-16Bibliographically approved
List of papers
1. Nanodancing with Moisture: Humidity-Sensitive Bilayer Actuator Derived from Cellulose Nanofibrils and Reduced Graphene Oxide
Open this publication in new window or tab >>Nanodancing with Moisture: Humidity-Sensitive Bilayer Actuator Derived from Cellulose Nanofibrils and Reduced Graphene Oxide
Show others...
2022 (English)In: Advanced Intelligent Systems, E-ISSN 2640-4567, Vol. 4, no 1, article id 2100084Article in journal (Refereed) Published
Abstract [en]

Bilayer actuators, traditionally consisting of two laminated materials, are the most common types of soft or hybrid actuators. Herein, a nanomaterial-based organic–inorganic humidity-sensitive bilayer actuator composed of TEMPO-oxidized cellulose nanofibrils (TCNF-Na+) and reduced graphene oxide (rGO) sheets is presented. The hybrid actuator displays a large humidity-driven locomotion with an atypical fast unbending. Cationic exchange of the anionically charged TCNF-Na+ and control of the layer thickness is used to tune and dictate the locomotion and actuator's response to humidity variations. Assembly of a self-oscillating electrical circuit, that includes a conductive rGO layer, displays autonomous on-and-off lighting in response to actuation-driven alternating electrical heating.

Keywords
bilayer actuators, cellulose nanofibrils, humidity sensors, reduced graphene oxide, smart materials
National Category
Chemical Sciences
Identifiers
urn:nbn:se:su:diva-198677 (URN)10.1002/aisy.202100084 (DOI)000700058800001 ()
Available from: 2021-11-15 Created: 2021-11-15 Last updated: 2023-12-17Bibliographically approved
2. Cationic cellulose Nanofibrils-based electro-actuators: The effects of counteranion and electrolyte
Open this publication in new window or tab >>Cationic cellulose Nanofibrils-based electro-actuators: The effects of counteranion and electrolyte
2023 (English)In: Sensors and Actuators Reports, E-ISSN 2666-0539, Vol. 5, article id 100142Article in journal (Refereed) Published
Abstract [en]

Cellulose-based electro-actuators have enormous potential in various applications, e.g. artificial muscles, soft grippers, medical devices, just to name a few, owing to their high mechanical strength, lightness and natural abundance. However, significant challenges remain in the fabrication of such electro-actuators featuring low operating voltage and fast response kinetics. We report here a facile fabrication route towards high-performance electro-actuators composed of CNFs films doped with ionic liquids or lithium salts and sandwiched by two thin film gold electrodes. Large bending motion at voltages as low as 3.0 V could be observed. The size effect of both anions and cations on the actuation was comprehensively investigated. CNF-TFSI@LiTFSI and CNF-BF4@EMIM-BF4 electro-actuators presented the best bending strain under an AC voltage of 3.0 V. This work provides new inspiration in the design of natural polymer-based high-performance electro-actuators.

Keywords
Electro-actuators, Cellulose nanofibrils, Ionic liquids, Soft robotics, Anion influence
National Category
Textile, Rubber and Polymeric Materials
Identifiers
urn:nbn:se:su:diva-216348 (URN)10.1016/j.snr.2023.100142 (DOI)000945690100001 ()2-s2.0-85147605788 (Scopus ID)
Available from: 2023-04-18 Created: 2023-04-18 Last updated: 2023-12-17Bibliographically approved
3. Capacitive CO2 sensor made of aminated cellulose nanofibrils: Development and optimization
Open this publication in new window or tab >>Capacitive CO2 sensor made of aminated cellulose nanofibrils: Development and optimization
(English)Manuscript (preprint) (Other academic)
Keywords
soft actuator, cellulose nanofibrils, smart materials, CO2 capture, CO2-responsive materials
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-224537 (URN)
Available from: 2023-12-16 Created: 2023-12-16 Last updated: 2023-12-17
4. Humidity-responsive fiber actuators based on cellulose nanofibrils
Open this publication in new window or tab >>Humidity-responsive fiber actuators based on cellulose nanofibrils
Show others...
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Fiber actuators, particularly valuable in soft robotics and environmental sensing, are at the forefront of smart materials and materials innovation. Torsional and tensile biofiber actuators, notable for their cost-effectiveness and biodegradability, mark a critical gap in the development of next-generation functional materials and devices. To address this gap, this study showcases moisture-responsive actuators made from cellulose nanofibrils (CNFs). It introduces a pioneering torsional actuator, leveraging the hydrophilic nature of CNFs filaments produced through wet-spinning processes. These robust filaments exhibit a mechanical strength of 237.0 MPa, and are twisted to form the high-performance torsional actuator. This torsional actuator demonstrates rapid rotations, achieving up to 1180 revolutions per minute (rpm) within merely 10 seconds of moisture exposure and being durable across multiple cycles. The research here further explores critical factors such as filament morphology and twist density, which significantly impact the performance of this torsional actuator. Additionally, a sheath-run tensile actuator is unveiled, ingeniously combining a moisture-sensitive CNFs layer with a supercoiled nylon core to enhance structural support. 

Keywords
fiber actuator, tensile actuator, tensile actuator, Wet spinning, cellulose nanofibrils
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-224539 (URN)
Available from: 2023-12-16 Created: 2023-12-16 Last updated: 2023-12-17
5. A transport channel-regulated MXene membrane via organic phosphonic acids for efficient water permeation
Open this publication in new window or tab >>A transport channel-regulated MXene membrane via organic phosphonic acids for efficient water permeation
Show others...
2021 (English)In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 57, no 51, p. 6245-6248Article in journal (Refereed) Published
Abstract [en]

A series of organic phosphonic acids (OPAs) were applied as multifunctional spacers to enlarge the inner space of carbide MXene (Ti3C2Tx) laminates. A synergistic improvement in permeance, rejection and stability is achieved via introducing OPA to create pillared laminates. This strategy provides a universal way to regulate transport channels of MXene-based membranes.

National Category
Chemical Sciences
Identifiers
urn:nbn:se:su:diva-195078 (URN)10.1039/d1cc01464a (DOI)000656480000001 ()34059863 (PubMedID)
Available from: 2021-08-09 Created: 2021-08-09 Last updated: 2023-12-17Bibliographically approved
6. Multitasking tartaric-acid-enabled, highly conductive, and stable MXene/conducting polymer composite for ultrafast supercapacitor
Open this publication in new window or tab >>Multitasking tartaric-acid-enabled, highly conductive, and stable MXene/conducting polymer composite for ultrafast supercapacitor
2021 (English)In: Cell Reports Physical Science, E-ISSN 2666-3864, Vol. 2, no 6, article id 100449Article in journal (Refereed) Published
Abstract [en]

Ti3C2Tx (MXene), a thriving member of the two-dimensional (2D) materials family, has shown increasing potential in a myriad of applications, ranging from printable electronics to energy storage and separation membranes. Nevertheless, the dilemma of its oxidative instability and the easy disintegration of its assemblies in contact with water has been restricting its real-life use. Here, we report the benefits of tartaric acid, a natural source, as a non-innocent additive in the MXene composite. In water, it can, above all, inhibit oxidation of Ti3C2Tx and hold individual components in the composite Ti3C2Tx/poly(3,4-ethylenedioxy thiophene):polystyrene sulfonate) (Ti3C2Tx/PEDOT:PSS) firmly together; equally important, it can boost 4-fold the composite’s electron conductivity in comparison to the additive-free equivalent. To showcase its practical value, a tartaric-acid-treated, water-stable MXene/PEDOT:PSS conductive coating is made, which serves as electrodes for an ultrafast supercapacitor; among all 2D materials-based assemblies, the designed supercapacitor delivers, to our knowledge, the record-high performance in an alternating-current filtering application.

National Category
Chemical Sciences
Identifiers
urn:nbn:se:su:diva-196180 (URN)10.1016/j.xcrp.2021.100449 (DOI)000665056400011 ()
Available from: 2021-09-07 Created: 2021-09-07 Last updated: 2023-12-17Bibliographically approved
7. Vacancy-Rich MXene-Immobilized Ni Single Atoms as a High-Performance Electrocatalyst for the Hydrazine Oxidation Reaction
Open this publication in new window or tab >>Vacancy-Rich MXene-Immobilized Ni Single Atoms as a High-Performance Electrocatalyst for the Hydrazine Oxidation Reaction
Show others...
2022 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 34, no 36, article id 2204388Article in journal (Refereed) Published
Abstract [en]

Single-atom catalysts (SACs), on account of their outstanding catalytic potential, are currently emerging as high-performance materials in the field of heterogeneous catalysis. Constructing a strong interaction between the single atom and its supporting matrix plays a pivotal role. Herein, Ti3C2Tx-MXene-supported Ni SACs are reported by using a self-reduction strategy via the assistance of rich Ti vacancies on the Ti3C2Tx MXene surface, which act as the trap and anchor sites for individual Ni atoms. The constructed Ni SACs supported by the Ti3C2Tx MXene (Ni SACs/Ti3C2Tx ) show an ultralow onset potential of −0.03 V (vs reversible hydrogen electrode (RHE)) and an exceptional operational stability toward the hydrazine oxidation reaction (HzOR). Density functional theory calculations suggest a strong coupling of the Ni single atoms and their surrounding C atoms, which optimizes the electronic density of states, increasing the adsorption energy and decreasing the reaction activation energy, thus boosting the electrochemical activity. The results presented here will encourage a wider pursuit of 2D-materials-supported SACs designed by a vacancy-trapping strategy. 

Keywords
electronic density of states, hydrazine oxidation reaction, Ni single-atom electrocatalysts, Ti vacancies, Ti3C2Tx MXene
National Category
Materials Engineering Chemical Sciences
Identifiers
urn:nbn:se:su:diva-209778 (URN)10.1002/adma.202204388 (DOI)000837009000001 ()35839429 (PubMedID)2-s2.0-85135530791 (Scopus ID)
Available from: 2022-09-30 Created: 2022-09-30 Last updated: 2024-01-22Bibliographically approved
8. Polypeptide-based vapor-responsive porous poly(ionic liquid) actuators: From reversible to unexpectedly irreversible actuation
Open this publication in new window or tab >>Polypeptide-based vapor-responsive porous poly(ionic liquid) actuators: From reversible to unexpectedly irreversible actuation
Show others...
2023 (English)In: Materials Today Communications, ISSN 2352-4928, Vol. 35, article id 105878Article in journal (Refereed) Published
Abstract [en]

Soft actuators capable of large and swift locomotion in combination with biocompatibility hold great potential in medicine and healthcare applications. In this contribution, a polypeptide-type poly(ionic liquid) (termed “PLL-PMIM-Tf2N”) was designed and synthesized by post-polymerization modification of poly-L-lysine; Next, via controlled electrostatic complexation with poly(acrylic acid) (PAA) or poly(L-glutamic acid) (PLG), porous membrane actuators termed PLL-PMIM-Tf2N/PAA or PLL-PMIM-Tf2N/PLG, respectively, were tailor-made. Hemolytic tests support excellent blood cell compatibility of the fully polypeptide-based PLL-PMIM-Tf2N/PLG actuator. The as-made soft actuators could bend significantly up to 500°with a maximum curvature of 7 cm−1 in response to solvent vapor in a fast actuation process within 2 s. Their high sensitivity towards solvent molecules equips them with skills to distinguish solvent isomers, as exemplified by butanol isomers, in terms of bending curvature due to varied molecular interactions between the actuator and the isomer. To be highlighted is an unusual irreversible actuated tubular state of the fully polypeptide-based PLL-PMIM-Tf2N/PLG actuator that is stable in shape and resembles bionic blood vessels. Such polypeptide-type poly(ionic liquid) actuators are of significant value in future development of biocompatible devices for medical and healthcare applications.

Keywords
Soft actuators, Polypeptide, Solvent vapor, Bionic blood vessel, Poly(ionic liquid)
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:su:diva-219279 (URN)10.1016/j.mtcomm.2023.105878 (DOI)2-s2.0-85151471603 (Scopus ID)
Funder
EU, European Research Council, PARIS-101043485Stockholm University
Available from: 2023-07-21 Created: 2023-07-21 Last updated: 2023-12-17Bibliographically approved
9. Assembly of Hierarchically Porous Holey-MXene Hydrogels for Ultrafast Pseudocapacitive Energy Storage
Open this publication in new window or tab >>Assembly of Hierarchically Porous Holey-MXene Hydrogels for Ultrafast Pseudocapacitive Energy Storage
Show others...
(English)Manuscript (preprint) (Other academic)
National Category
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-224546 (URN)
Available from: 2023-12-16 Created: 2023-12-16 Last updated: 2023-12-17

Open Access in DiVA

fulltext(14589 kB)103 downloads
File information
File name FULLTEXT01.pdfFile size 14589 kBChecksum SHA-512
35ed63097094c675e98e0b928ffc3d6faf481dff527d8ec429d7990553f1ca56d90bc0c34df61545425efa2b387a139d8b2cd40bd6f19662a1897585a03ed97b
Type fulltextMimetype application/pdf

Authority records

Héraly, Frédéric

Search in DiVA

By author/editor
Héraly, Frédéric
By organisation
Department of Materials and Environmental Chemistry (MMK)
Materials ChemistryBiomaterials Science

Search outside of DiVA

GoogleGoogle Scholar
Total: 103 downloads
The number of downloads is the sum of all downloads of full texts. It may include eg previous versions that are now no longer available

isbn
urn-nbn

Altmetric score

isbn
urn-nbn
Total: 948 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf