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Crystallizing covalent organic frameworks from metal organic framework through chemical induced-phase engineering
Abdul Khayum Mohammed, Safa Gaber, Jesus Raya, Tina Škorjanc, Nada Elmerhi, Sasi Stephen, Pilar Pena-Sánchez, Felipe Gándara, Steven Hinder, Mark A. Baker, Kyriaki Polychronopoulou, Dinesh Shetty, 2023, izvirni znanstveni članek

Opis: The ordered porous frameworks like MOFs and COFs are generally constructed using the monomers through distinctive metal-coordinated and covalent linkages. Meanwhile, the inter-structural transition between each class of these porous materials is an under-explored research area. However, such altered frameworks are expected to have exciting features compared to their pristine versions. Herein, we have demonstrated a chemical-induction phase-engineering strategy to transform a two dimensional conjugated Cu-based SA-MOF (Cu-Tp) into 2D-COFs (Cu-TpCOFs). The structural phase transition offered in-situ pore size engineering from 1.1 nm to 1.5–2.0 nm. Moreover, the Cu-TpCOFs showed uniform and low percentage-doped (~ 1–1.5%) metal distribution and improved crystallinity, porosity, and stability compared to the parent Cu-Tp MOF. The construction of a framework from another framework with new linkages opens interesting opportunities for phase-engineering.
Ključne besede: metal organic framework, covalent organic framework, phase engineering, chemical transformation, porous materials
Objavljeno v RUNG: 10.11.2023; Ogledov: 851; Prenosov: 5
.pdf Celotno besedilo (3,64 MB)
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Enzyme-immobilized hierarchically porous covalent organic framework biocomposite for catalytic degradation of broad-range emerging pollutants in water
Nada Elmerhi, Khadega Al-Maqdi, Khawlah Athamneh, Abdul Khayum Mohammed, Tina Škorjanc, Felipe Gándara, Jesus Raya, Pascal Simon, Olivier Siri, Ali Trabolsi, 2023, izvirni znanstveni članek

Opis: Efficient enzyme immobilization is crucial for the successful commercialization of large-scale enzymatic water treatment. However, issues such as lack of high enzyme loading coupled with enzyme leaching present challenges for the widespread adoption of immobilized enzyme systems. The present study describes the development and bioremediation application of an enzyme biocomposite employing a cationic macrocycle-based covalent organic framework (COF) with hierarchical porosity for the immobilization of horseradish peroxidase (HRP). The intrinsic hierarchical porous features of the azacalix[4]arene-based COF (ACA-COF) allowed for a maximum HRP loading capacity of 0.76 mg/mg COF with low enzyme leaching (<5.0%). The biocomposite, HRP@ACA-COF, exhibited exceptional thermal stability (~200% higher relative activity than the free enzyme), and maintained ~60% enzyme activity after five cycles. LCMSMS analyses confirmed that the HRP@ACA-COF system was able to achieve >99% degradation of seven diverse types of emerging pollutants (2-mercaptobenzothiazole, paracetamol, caffeic acid, methylparaben, furosemide, sulfamethoxazole, and salicylic acid)in under an hour. The described enzyme-COF system offers promise for efficient wastewater bioremediation applications.
Ključne besede: covalent organic frameworks, enzymes, emerging pollutants, water purification, biocomposite
Objavljeno v RUNG: 11.08.2023; Ogledov: 990; Prenosov: 6
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Taming the topology of calix[4]arene-based 2D-covalent organic frameworks : interpenetrated vs noninterpenetrated frameworks and their selective removal of cationic dyes
Bikash Garai, Dinesh Shetty, Tina Škorjanc, Felipe Gándara, Nawavi Naleem, Sabu Varghese, Sudhir Kumar Sharma, Maria Baias, Ramesh Jagannathan, Mark Anthony Olson, 2021, izvirni znanstveni članek

Opis: A bowl-shaped calix[4]arene with its exciting host–guest chemistry is a versatile supramolecular building block for the synthesis of distinct coordination cages or metal–organic frameworks. However, its utility in the synthesis of crystalline covalent organic frameworks (COFs) remains challenging, presumably due to its conformational flexibility. Here, we report the synthesis of a periodic 2D extended organic network of calix[4]arenes joined by a linear benzidine linker via dynamic imine bonds. By tuning the interaction among neighboring calixarene units through varying the concentration in the reaction mixture, we show the selective formation of interpenetrated (CX4-BD-1) and non-interpenetrated (CX4-BD-2) frameworks. The cone-shaped calixarene moiety in the structural backbone allows for the interweaving of two neighboring layers in CX4-BD-1, making it a unique example of interpenetrated 2D layers. Due to the high negative surface charge from calixarene units, both COFs have shown high performance in charge-selective dye removal and an exceptional selectivity for cationic dyes irrespective of their molecular size. The charge distribution of the COFs and the resulting selectivity for the cationic dyes were further investigated using computational methods.
Ključne besede: dyes and pigments, covalent organic frameworks, adsorption, layers, chemical structure
Objavljeno v RUNG: 16.03.2021; Ogledov: 2286; Prenosov: 0
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Highly efficient carcinogenic bromate removal from water by a cationic covalent organic framework
Tina Skorjanc, Dinesh Shetty, Felipe Gandara, Liaqat Ali, Ali Trabolsi, 2019, objavljeni povzetek znanstvenega prispevka na konferenci

Ključne besede: bromate, covalent organic frameworks, Zincke reaction, adsorption, water purification
Objavljeno v RUNG: 03.09.2020; Ogledov: 2870; Prenosov: 0
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