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Poly(ionic liquid)-derived metal-free heteroatom co-doped porous carbons with peroxidase-like activity
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). (Yuan group)
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
(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 [en]
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: urn:nbn:se:su:diva-225573OAI: oai:DiVA.org:su-225573DiVA, id: diva2:1829004
Available from: 2024-01-17 Created: 2024-01-17 Last updated: 2024-01-25
In thesis
1. Heteroatom-doped porous carbon materials derived from poly(ionic liquid)s and their composites for battery and catalytic applications
Open this publication in new window or tab >>Heteroatom-doped porous carbon materials derived from poly(ionic liquid)s and their composites for battery and catalytic applications
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
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:nbn:se:su:diva-225583 (URN)978-91-8014-639-5 (ISBN)978-91-8014-640-1 (ISBN)
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

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