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Saeedi Garakani, Sadaf
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Publikationer (9 of 9) Visa alla publikationer
Saeedi Garakani, S. (2024). Heteroatom-doped porous carbon materials derived from poly(ionic liquid)s and their composites for battery and catalytic applications. (Doctoral dissertation). Stockholm: Department of Materials and Environmental Chemistry, Stockholm University
Öppna denna publikation i ny flik eller fönster >>Heteroatom-doped porous carbon materials derived from poly(ionic liquid)s and their composites for battery and catalytic applications
2024 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
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.

Ort, förlag, år, upplaga, sidor
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University, 2024. s. 60
Nyckelord
Heteroatom doped carbon, Porous carbon membrane, Poly(ionic liquid)-derived carbon, Wood-derived carbon, Catalytic activity, Peroxidase-like activity, lithium sulfur battery
Nationell ämneskategori
Materialkemi
Forskningsämne
materialkemi
Identifikatorer
urn:nbn:se:su:diva-225583 (URN)978-91-8014-639-5 (ISBN)978-91-8014-640-1 (ISBN)
Disputation
2024-03-01, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 13:00 (Engelska)
Opponent
Handledare
Tillgänglig från: 2024-02-07 Skapad: 2024-01-17 Senast uppdaterad: 2024-02-15Bibliografiskt granskad
Saeedi Garakani, S., Sikdar, A., Pang, K. & Yuan, J. (2024). Poly(ionic liquid)-derived metal-free heteroatom co-doped porous carbons with peroxidase-like activity. Applied Materials Today, 37, Article ID 102081.
Öppna denna publikation i ny flik eller fönster >>Poly(ionic liquid)-derived metal-free heteroatom co-doped porous carbons with peroxidase-like activity
2024 (Engelska)Ingår i: Applied Materials Today, ISSN 2352-9407, Vol. 37, artikel-id 102081Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Development of affordable, efficient 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 problems 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.

Nyckelord
Heteroatom co-doped carbon, Metal-free carbonaceous catalyst, Poly(ionic liquid)-derived carbon, Artificial enzyme, Peroxidase-like activity
Nationell ämneskategori
Materialkemi Organisk kemi
Identifikatorer
urn:nbn:se:su:diva-228193 (URN)10.1016/j.apmt.2024.102081 (DOI)001176572300001 ()2-s2.0-85184007619 (Scopus ID)
Tillgänglig från: 2024-04-10 Skapad: 2024-04-10 Senast uppdaterad: 2024-04-10Bibliografiskt granskad
Pang, K., Tang, Y., Qiu, C., Zhang, M., Tayal, A., Feng, S., . . . Yuan, J. (2024). Redirecting configuration of atomically dispersed selenium catalytic sites for efficient hydrazine oxidation. Matter, 7(2), 655-667
Öppna denna publikation i ny flik eller fönster >>Redirecting configuration of atomically dispersed selenium catalytic sites for efficient hydrazine oxidation
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2024 (Engelska)Ingår i: Matter, ISSN 2590-2393, E-ISSN 2590-2385, Vol. 7, nr 2, s. 655-667Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Understanding the reconstruction of surface sites is crucial for gaining insights into the true active sites and catalytic mechanisms. While extensive research has been conducted on reconstruction behaviors of atomically dispersed metallic catalytic sites, limited attention has been paid to non-metallic ones despite their potential catalytic activity comparable or even superior to their noble-metal counterpart. Herein, we report a carbonaceous, atomically dispersed non-metallic selenium catalyst that displayed exceptional catalytic activity in the hydrazine oxidation reaction (HzOR) in alkaline media, outperforming the noble-metal Pt catalysts. In situ X-ray absorption spectroscopy (XAS) and Fourier transform infrared spectroscopy revealed that the pristine SeC4 site pre-adsorbs an ∗OH ligand, followed by HzOR occurring on the other side of the OH–SeC4. Theoretical calculations proposed that the pre-adsorbed ∗OH group pulls electrons from the Se site, resulting in a more positively charged Se and a higher polarity of Se–C bonds, thereby enhancing surface reactivity toward HzO/R.

Nationell ämneskategori
Materialkemi
Forskningsämne
materialvetenskap
Identifikatorer
urn:nbn:se:su:diva-225579 (URN)10.1016/j.matt.2023.12.001 (DOI)001182393300001 ()2-s2.0-85184059651 (Scopus ID)
Tillgänglig från: 2024-01-17 Skapad: 2024-01-17 Senast uppdaterad: 2024-03-26Bibliografiskt granskad
Saeedi Garakani, S., Zhang, M., Xie, D., Sikdar, A., Pang, K. & Yuan, J. (2023). Facile Fabrication of Wood-Derived Porous Fe3C/Nitrogen-Doped Carbon Membrane for Colorimetric Sensing of Ascorbic Acid. Nanomaterials, 13(20), Article ID 2786.
Öppna denna publikation i ny flik eller fönster >>Facile Fabrication of Wood-Derived Porous Fe3C/Nitrogen-Doped Carbon Membrane for Colorimetric Sensing of Ascorbic Acid
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2023 (Engelska)Ingår i: Nanomaterials, E-ISSN 2079-4991, Vol. 13, nr 20, artikel-id 2786Artikel i tidskrift (Refereegranskat) 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.

Nyckelord
iron carbide nanoparticles, nitrogen-doped carbon, wood-derived carbon, colorimetric detection, ascorbic acid
Nationell ämneskategori
Materialkemi
Identifikatorer
urn:nbn:se:su:diva-223976 (URN)10.3390/nano13202786 (DOI)001092601900001 ()37887937 (PubMedID)2-s2.0-85175081396 (Scopus ID)
Tillgänglig från: 2023-11-24 Skapad: 2023-11-24 Senast uppdaterad: 2024-01-18Bibliografiskt granskad
Zhang, M., Dong, K., Saeedi Garakani, S., Khorsand Kheirabad, A., Manke, I., Wu, M., . . . Yuan, J. (2022). Bridged Carbon Fabric Membrane with Boosted Performance in AC Line-Filtering Capacitors. Advanced Science, 9(7), Article ID 2105072.
Öppna denna publikation i ny flik eller fönster >>Bridged Carbon Fabric Membrane with Boosted Performance in AC Line-Filtering Capacitors
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2022 (Engelska)Ingår i: Advanced Science, E-ISSN 2198-3844, Vol. 9, nr 7, artikel-id 2105072Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

High-frequency responsive capacitors with lightweight, flexibility, and miniaturization are among the most vital circuit components because they can be readily incorporated into various portable devices to smooth out the ripples for circuits. Electrode materials no doubt are at the heart of such devices. Despite tremendous efforts and recent advances, the development of flexible and scalable high-frequency responsive capacitor electrodes with superior performance remains a great challenge. Herein, a straightforward and technologically relevant method is reported to manufacture a carbon fabric membrane “glued” by nitrogen-doped nanoporous carbons produced through a polyelectrolyte complexation-induced phase separation strategy. The as-obtained flexible carbon fabric bearing a unique hierarchical porous structure, and high conductivity as well as robust mechanical properties, serves as the free-standing electrode materials of electrochemical capacitors. It delivers an ultrahigh specific areal capacitance of 2632 µF cm−2 at 120 Hz with an excellent alternating current line filtering performance, fairly higher than the state-of-the-art commercial ones. Together, this system offers the potential electrode material to be scaled up for AC line-filtering capacitors at industrial levels. 

Nyckelord
alternating current line filtering, phase angle, poly(ionic liquid), porous carbon membrane
Nationell ämneskategori
Kemi
Identifikatorer
urn:nbn:se:su:diva-201831 (URN)10.1002/advs.202105072 (DOI)000744694800001 ()35060354 (PubMedID)2-s2.0-85123168721 (Scopus ID)
Tillgänglig från: 2022-02-08 Skapad: 2022-02-08 Senast uppdaterad: 2022-05-11Bibliografiskt granskad
Kheirabad, A. K., Garakani, S. S., Tan, L. & Yuan, J. (2021). Ferrocene-Containing Porous Poly(Ionic Liquid) Membranes: Synthesis and Application as Sacrificial Template for Porous Iron Oxide Films. Macromolecular rapid communications, 42(13), Article ID 2100077.
Öppna denna publikation i ny flik eller fönster >>Ferrocene-Containing Porous Poly(Ionic Liquid) Membranes: Synthesis and Application as Sacrificial Template for Porous Iron Oxide Films
2021 (Engelska)Ingår i: Macromolecular rapid communications, ISSN 1022-1336, E-ISSN 1521-3927, Vol. 42, nr 13, artikel-id 2100077Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Herein, the fabrication of iron-containing porous polyelectrolyte membranes (PPMs) via ionic complexation between an imidazolium-based poly(ionic liquid) (PIL) and 1,1-ferrocenedicarboxylic acid is reported. The key parameters to control the microstructure of porous hybrid membranes are investigated in detail. Further aerobic pyrolysis of such porous hybrid membranes at 900 °C can transfer the ferrocene-containing PPMs into freestanding porous iron oxide films. This process points out a sacrificial template function of porous poly(ionic liquid) membranes in the fabrication of porous metal oxide films.

Nyckelord
ferrocene, poly(ionic liquid), porous iron oxide films, porous polyelectrolyte membranes
Nationell ämneskategori
Kemi
Identifikatorer
urn:nbn:se:su:diva-195764 (URN)10.1002/marc.202100077 (DOI)000656569100001 ()34061421 (PubMedID)
Tillgänglig från: 2021-08-26 Skapad: 2021-08-26 Senast uppdaterad: 2023-02-27Bibliografiskt granskad
Garakani, S. S., Xie, D., Kheirabad, A. K., Lu, Y. & Yuan, J. (2021). Template-synthesis of a poly(ionic liquid)-derived Fe1−xS/nitrogen-doped porous carbon membrane and its electrode application in lithium–sulfur batteries. Materials Advances, 2(15), 5203-5212
Öppna denna publikation i ny flik eller fönster >>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 (Engelska)Ingår i: Materials Advances, E-ISSN 2633-5409, Vol. 2, nr 15, s. 5203-5212Artikel i tidskrift (Refereegranskat) 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.

Nationell ämneskategori
Kemi
Identifikatorer
urn:nbn:se:su:diva-196521 (URN)10.1039/d1ma00441g (DOI)000672780600001 ()34382003 (PubMedID)
Tillgänglig från: 2021-09-07 Skapad: 2021-09-07 Senast uppdaterad: 2024-01-18Bibliografiskt granskad
Guiver, M. D., Yahia, M., Dal-Cin, M. M., Robertson, G. P., Saeedi Garakani, S., Du, N. & Tavajohi, N. (2020). Gas Transport in a Polymer of Intrinsic Microporosity (PIM-1) Substituted with Pseudo-Ionic Liquid Tetrazole-Type Structures. Macromolecules, 53(20), 8951-8959
Öppna denna publikation i ny flik eller fönster >>Gas Transport in a Polymer of Intrinsic Microporosity (PIM-1) Substituted with Pseudo-Ionic Liquid Tetrazole-Type Structures
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2020 (Engelska)Ingår i: Macromolecules, ISSN 0024-9297, E-ISSN 1520-5835, Vol. 53, nr 20, s. 8951-8959Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

We report a side group modification strategy to tailor the structure of a polymer of intrinsic microporosity (PIM-1). PIM-1 with an average of similar to 50% of the repeat units converted to tetrazole is prepared, and a subsequent reaction then introduces three types of pseudo-ionic liquid tetrazole-like structures (PIM-1-ILx). The presence of pseudo-ionic liquid functional groups in the PIM-1 structure increases gas selectivities for O-2/N-2 and CO2/N-2, while it decreases pure-gas permeabilities. The overall gas separation performance of PIM-1-ILx is close to the 2008 Robeson upper bound. Since the tetrazoles are versatile groups for building a wide variety of ionic liquids, the modification method can be expanded to explore a broad spectrum of functional groups.

Nationell ämneskategori
Kemi
Identifikatorer
urn:nbn:se:su:diva-188901 (URN)10.1021/acs.macromol.0c01321 (DOI)000586789500023 ()33132419 (PubMedID)
Tillgänglig från: 2021-01-14 Skapad: 2021-01-14 Senast uppdaterad: 2022-02-25Bibliografiskt granskad
Saeedi Garakani, S., Pang, K., Pradip Nawadkar, A. & Yuan, J.Synthesis of Poly(ionic liquids)/wood composite-derived boron and nitrogen co-doped porous carbons with peroxidase-like activity.
Öppna denna publikation i ny flik eller fönster >>Synthesis of Poly(ionic liquids)/wood composite-derived boron and nitrogen co-doped porous carbons with peroxidase-like activity
(Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
Nationell ämneskategori
Materialkemi
Forskningsämne
materialvetenskap
Identifikatorer
urn:nbn:se:su:diva-225578 (URN)
Tillgänglig från: 2024-01-17 Skapad: 2024-01-17 Senast uppdaterad: 2024-02-26Bibliografiskt granskad
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