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Heteroatom-doped porous carbon materials derived from poly(ionic liquid)s and their composites for battery and catalytic applications
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
2024 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In the past decade, there has been significant interest in heteroatom-doped porous carbons, driven by the distinctive and adjustable physical and chemical properties that they exhibit across scales, from the atomic to the macroscopic level. Particularly, attributes such as conductivity, electron density, high specific surface area, hierarchical pore structure, and oxidation resistance offer a wide range of characteristics for diverse applications. The development of multimodal, hierarchical pore sizes, ranging from micropores to macropores, ensures balanced diffusion resistance and a high surface area for active site accommodation. However, their synthesis usually involves multiple steps or complicated processing to incorporate both hierarchically porous structures and heteroatoms in carbon materials.

This PhD thesis explores poly(ionic liquid)s (PILs) for preparation of heteroatom-doped porous carbon materials, driven by the growing demand for functional carbons in industry and academia. The aim of this thesis is to develop straightforward synthetic approaches to introduce various heteroatoms and different pore sizes in the carbonous structure and study their diverse functions. Here, we propose and explore fabrication methods based on two precursors. First, PILs were examined as both the carbon and heteroatom source, serving as a sacrificial template for porous carbons. Second, the delicate structure of wood was employed as a carbon source to generate macropores, while being coated with PILs to introduce heteroatoms or iron-based nanoparticles and create additional micropores. Moreover, the application of these carbonaceous materials was studied in two areas, i.e., batteries and artificial enzymes. This research is likely to contribute to a deeper understanding of synthetic methodologies of heteroatom-doped porous carbon materials and their physiochemical properties for various applications.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University , 2024. , p. 60
Keywords [en]
Heteroatom doped carbon, Porous carbon membrane, Poly(ionic liquid)-derived carbon, Wood-derived carbon, Catalytic activity, Peroxidase-like activity, lithium sulfur battery
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-225583ISBN: 978-91-8014-639-5 (print)ISBN: 978-91-8014-640-1 (electronic)OAI: oai:DiVA.org:su-225583DiVA, id: diva2:1829069
Public defence
2024-03-01, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2024-02-07 Created: 2024-01-17 Last updated: 2024-02-15Bibliographically approved
List of papers
1. Template-synthesis of a poly(ionic liquid)-derived Fe1−xS/nitrogen-doped porous carbon membrane and its electrode application in lithium–sulfur batteries
Open this publication in new window or tab >>Template-synthesis of a poly(ionic liquid)-derived Fe1−xS/nitrogen-doped porous carbon membrane and its electrode application in lithium–sulfur batteries
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2021 (English)In: Materials Advances, E-ISSN 2633-5409, Vol. 2, no 15, p. 5203-5212Article in journal (Refereed) Published
Abstract [en]

This study deals with the facile synthesis of Fe1−xS nanoparticle-containing nitrogen-doped porous carbon membranes (denoted as Fe1−xS/N-PCMs) via vacuum carbonization of hybrid porous poly(ionic liquid) (PIL) membranes, and their successful use as a sulfur host material to mitigate the shuttle effect in lithium–sulfur (Li–S) batteries. The hybrid porous PIL membranes as the sacrificial template were prepared via ionic crosslinking of a cationic PIL with base-neutralized 1,1′-ferrocenedicarboxylic acid, so that the iron source was molecularly incorporated into the template. The carbonization process was investigated in detail at different temperatures, and the chemical and porous structures of the carbon products were comprehensively analyzed. The Fe1−xS/N-PCMs prepared at 900 °C have a multimodal pore size distribution with a satisfactorily high surface area and well-dispersed iron sulfide nanoparticles to physically and chemically confine the LiPSs. The sulfur/Fe1−xS/N-PCM composites were then tested as electrodes in Li–S batteries, showing much improved capacity, rate performance and cycle stability, in comparison to iron sulfide-free, nitrogen-doped porous carbon membranes.

National Category
Chemical Sciences
Identifiers
urn:nbn:se:su:diva-196521 (URN)10.1039/d1ma00441g (DOI)000672780600001 ()34382003 (PubMedID)
Available from: 2021-09-07 Created: 2021-09-07 Last updated: 2024-01-18Bibliographically approved
2. Facile Fabrication of Wood-Derived Porous Fe3C/Nitrogen-Doped Carbon Membrane for Colorimetric Sensing of Ascorbic Acid
Open this publication in new window or tab >>Facile Fabrication of Wood-Derived Porous Fe3C/Nitrogen-Doped Carbon Membrane for Colorimetric Sensing of Ascorbic Acid
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2023 (English)In: Nanomaterials, E-ISSN 2079-4991, Vol. 13, no 20, article id 2786Article in journal (Refereed) Published
Abstract [en]

Fe3C nanoparticles hold promise as catalysts and nanozymes, but their low activity and complex preparation have hindered their use. Herein, this study presents a synthetic alternative toward efficient, durable, and recyclable, Fe3C-nanoparticle-encapsulated nitrogen-doped hierarchically porous carbon membranes (Fe3C/N–C). By employing a simple one-step synthetic method, we utilized wood as a renewable and environmentally friendly carbon precursor, coupled with poly(ionic liquids) as a nitrogen and iron source. This innovative strategy offers sustainable, high-performance catalysts with improved stability and reusability. The Fe3C/N–C exhibits an outstanding peroxidase-like catalytic activity toward the oxidation of 3,3′,5,5′-tetramethylbenzidine in the presence of hydrogen peroxide, which stems from well-dispersed, small Fe3C nanoparticles jointly with the structurally unique micro-/macroporous N–C membrane. Owing to the remarkable catalytic activity for mimicking peroxidase, an efficient and sensitive colorimetric method for detecting ascorbic acid over a broad concentration range with a low limit of detection (~2.64 µM), as well as superior selectivity, and anti-interference capability has been developed. This study offers a widely adaptable and sustainable way to synthesize an Fe3C/N–C membrane as an easy-to-handle, convenient, and recoverable biomimetic enzyme with excellent catalytic performance, providing a convenient and sensitive colorimetric technique for potential applications in medicine, biosensing, and environmental fields.

Keywords
iron carbide nanoparticles, nitrogen-doped carbon, wood-derived carbon, colorimetric detection, ascorbic acid
National Category
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-223976 (URN)10.3390/nano13202786 (DOI)001092601900001 ()37887937 (PubMedID)2-s2.0-85175081396 (Scopus ID)
Available from: 2023-11-24 Created: 2023-11-24 Last updated: 2024-01-18Bibliographically approved
3. Poly(ionic liquid)-derived metal-free heteroatom co-doped porous carbons with peroxidase-like activity
Open this publication in new window or tab >>Poly(ionic liquid)-derived metal-free heteroatom co-doped porous carbons with peroxidase-like activity
(English)In: Applied materials today, ISSN 2352-9407Article in journal (Refereed) Submitted
Abstract [en]

Development of affordable, efficacious and metal-free heterogeneous catalytic systems has been a persistent challenge in academia and industry. Heteroatom-doped metal-free carbon materials are increasingly recognized as valuable heterogeneous catalysts, and if well-designed, can present comparable performance to, or even surpass transition metal-containing catalysts. Their physicochemical properties and structural characteristics are  tunable in a wide range, plus being free of leakage of transition metal species into the environment. Herein, three types of hierarchically porous N/X co-doped carbon materials (X denotes B, P or S)  were synthesized via using poly(ionic liquid)s (PILs) as carbon precursors and source of heteroatom dopants. The incorporation of sacrificial pore-inducing templating agents which created abundant edge defects, in combination with a heteroatom co-doping strategy enhanced the number of active sites and their peroxidase-like catalytic activities. Comparison with only nitrogen single-doped porous carbons as reference demonstrated that co-doping with nitrogen and another heteroatom exhibits higher peroxidase-like activity and affinity towards substrates. Among the three types of heteroatom co-doped porous carbonaceous artificial enzymes, the N/B co-doped carbonaceous catalyst displayed the highest specific activities and Vmax values. These observations suggest a synergistic effect of the co-dopants, here N and B in the enzyme that holds a promising potential to further enhance peroxidase-like activity.

Keywords
Heteroatom co-doped carbon, Metal-free carbonaceous catalyst, Poly(ionic liquid)-derived carbon, Artificial enzyme, Peroxidase-like activity
National Category
Materials Chemistry
Research subject
Materials Science
Identifiers
urn:nbn:se:su:diva-225573 (URN)
Available from: 2024-01-17 Created: 2024-01-17 Last updated: 2024-01-25
4. Synthesis of Poly(ionic liquids)/wood composite-derived boron and nitrogen co-doped porous carbons with peroxidase-like activity
Open this publication in new window or tab >>Synthesis of Poly(ionic liquids)/wood composite-derived boron and nitrogen co-doped porous carbons with peroxidase-like activity
(English)Manuscript (preprint) (Other academic)
National Category
Materials Chemistry
Research subject
Materials Science
Identifiers
urn:nbn:se:su:diva-225578 (URN)
Available from: 2024-01-17 Created: 2024-01-17 Last updated: 2024-02-26Bibliographically approved

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Saeedi Garakani, Sadaf

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