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Sustained Delivery of Cu (II)-Based DNA Intercalators by Nanometer-sized Cyclodextrin-based Porous Polymers
Tina Skorjanc, Julian Heinrich, Damjan Makuc, Nora Kulak, Matjaz Valant, 2023, izvirni znanstveni članek

Opis: DNA intercalators are small molecules that insert between adjacent DNA base pairs and thus disturb DNA replication and transcription, which can lead to cell death. Certain metal complexes are excellent DNA intercalators, and have shown promise in chemotherapy. Here, a cyclodextrin porous polymer was prepared, characterized, exfoliated to form nanometer-sized particles, and used as a delivery vehicle for metal-free and Cu(II)-metalated anthraquinone-based DNA intercalators with a goal to minimize side effects of the highly toxic DNA intercalators. NMR experiments, including DOSY NMR, have shown the interaction between the cyclodextrin building block and the studied DNA intercalators. Porous nature of the delivery vehicle provided ample surface area for interaction with the drug candidates, resulting in encapsulation rates of up to 56%. Sustained cargo release from the polymer was achieved over eight days, and time-dependent cytotoxicity was observed. Furthermore, optical microscopy images indicated delivery vehicle internalization as well as disturbed cellular morphology within 24 hours of incubation. We anticipate that this study will stimulate further interest in the development of polymeric delivery systems for metal complexes.
Ključne besede: Porous organic polymers, cyclodextrin, DNA intercalators, Cu(II) complexes, metal complexes, drug delivery, anthraquinone
Objavljeno v RUNG: 10.11.2023; Ogledov: 229; Prenosov: 2
.pdf Celotno besedilo (5,10 MB)

Crystallizing covalent organic frameworks from metal organic framework through chemical induced‑phase engineering
Abdul Khayum Mohammed, Safa Gaber, Jesus Raya, Tina Skorjanc, Nada Elmerhi, Sasi Stephen, Pilar Pena Sanchez, Felipe Gandara, Steven J. 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: 245; Prenosov: 3
.pdf Celotno besedilo (3,64 MB)
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In vitro tumor hypoxia imaging with fluorescent covalent organic frameworks
Tina Skorjanc, Dinesh Shetty, Damjan Makuc, Gregor Mali, Martina Bergant Marušič, Matjaz Valant, 2023, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: Hypoxia refers to a condition where cells and tissues experience low, inadequate levels of O2. While healthy tissues are typically supplied with sufficient O2 (normoxia), cancerous tissues commonly face hypoxia due to the tumor’s extraordinarily high demand for oxygen. Various fluorescent small-molecule probes have been designed for selective detection of hypoxia in living cells, but few nanomaterials have been investigated for this type of bioimaging. Herein, we prepare a fluorescent covalent organic framework (COF) with β-ketoenamine linkages and post-synthetically modify it to conjugate hypoxia-sensitive nitroimidazole moieties into its pores (NI-COF). Stacks of sheets in NI-COF observed under electron microscopy were exfoliated by ultrasonication, and dynamic light scattering measurements confirmed particle size of less than 200 nm. Thus-prepared material exhibited good stability in physiological conditions and low cytotoxicity in in vitro experiments. NI-COF also showed useful fluorescence properties with an emission peak at 490 nm (λex = 420 nm) at both neutral and mildly acidic pH levels that are characteristic of tumor tissues. Encouraged by the favorable properties of the material, we incubated HeLa cells pre-treated in either hypoxic or normoxic conditions with NI-COF. Fluorescence microscopy images demonstrated that the material was preferentially taken up by hypoxic cells, which showed higher fluorescence signal in their interior than cells cultured under normoxia conditions. It is anticipated that this study will stimulate further developments of COFs for imaging various biological conditions.
Ključne besede: hypoxia, fluorescence, covalent organic frameworks, imaging, tumor cells
Objavljeno v RUNG: 19.09.2023; Ogledov: 354; Prenosov: 3
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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 Skorjanc, Felipe Gandara, Jesus Raya, Simon Pascal, Olivier Siri, Ali Trabolsi, Iltaf Shah, Dinesh Shetty, Syed Salman Ashraf, 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: 432; Prenosov: 2
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Changes in exhaled volatile organic compounds following indirect bronchial challenge in suspected asthma
Adam Peel, Ran Wang, Waqar Ahmed, Iain R White, Max Wilkinson, Yoon K Loke, Andrew M Wilson, Stephen J Fowler, 2023, izvirni znanstveni članek

Opis: Background Inhaled mannitol provokes bronchoconstriction via mediators released during osmotic degranulation of inflammatory cells, and, hence represents a useful diagnostic test for asthma and model for acute attacks. We hypothesised that the mannitol challenge would trigger changes in exhaled volatile organic compounds (VOCs), generating both candidate biomarkers and novel insights into their origin. Methods Participants with a clinical diagnosis of asthma, or undergoing investigation for suspected asthma, were recruited. Inhaled mannitol challenges were performed, followed by a sham challenge after 2 weeks in participants with bronchial hyper-responsiveness (BHR). VOCs were collected before and after challenges and analysed using gas chromatography–mass spectrometry. Results Forty-six patients (mean (SD) age 52 (16) years) completed a mannitol challenge, of which 16 (35%) were positive, and 15 of these completed a sham challenge. Quantities of 16 of 51 identified VOCs changed following mannitol challenge (p<0.05), of which 11 contributed to a multivariate sparse partial least square discriminative analysis model, with a classification error rate of 13.8%. Five of these 16 VOCs also changed (p<0.05) in quantity following the sham challenge, along with four further VOCs. In patients with BHR to mannitol distinct postchallenge VOC signatures were observed compared with post-sham challenge. Conclusion Inhalation of mannitol was associated with changes in breath VOCs, and in people with BHR resulted in a distinct exhaled breath profile when compared with a sham challenge. These differentially expressed VOCs are likely associated with acute airway inflammation and/or bronchoconstriction and merit further investigation as potential biomarkers in asthma.
Ključne besede: Asthma, Exhaled volatile organic compounds, Pulmonology, Breath metabolomics
Objavljeno v RUNG: 31.07.2023; Ogledov: 427; Prenosov: 2
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Biological applications of porous polymers and covalent organic frameworks
Tina Škorjanc, 2023, predavanje na tuji univerzi

Opis: Porous organic polymers (POPs) and covalent organic frameworks (COFs) have gained significant attention in the scientific community for a wide array of applications because of their attractive physical and chemical properties. Porosity of these materials provides ample surface area for interaction with targets, while crystallinity allows for highly specific structural tuning. In this seminar, I will present two strategies of utilizing these features of newly prepared materials in biosensing. Firstly, a cationic POP was synthesized, deposited onto interdigitated electrode arrays via a nontraditional electrophoresis technique, and utilized for electrochemical sensing of bacterial cells. As the principle of detection relied on electrostatic interactions between the cationic POP and the anionic bacterial surface, the sensor operated for both Gram-positive and Gram-negative bacteria. Secondly, a small-molecule nitroimidazole target for hypoxia, a low oxygen environment present in tumors, was post-synthetically conjugated to the pores of a fluorescent COF. This material served as a useful hypoxia imaging agent in cancerous cells. The seminar will conclude with some future perspectives on POPs and COFs in biological applications followed by Q & A.
Ključne besede: Porous organic polymers, covalent organic frameworks, biosensors, hypoxia
Objavljeno v RUNG: 13.07.2023; Ogledov: 472; Prenosov: 0
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Modulation of charge transfer exciton dynamics in organic semiconductors using different structural arrangements : none
Cristian Soncini, Abhishek Kumar, Federica Bondino, Elena Magnano, Matija Stupar, Barbara Ressel, Giovanni De Ninno, Antonis Papadopoulos, Efthymis Serpetzoglou, Emmanuel Stratakis, Maddalena Pedio, 2023, izvirni znanstveni članek

Opis: In devices based on organic semiconductors, aggregation and inter-molecular interactions play a key role in affecting the photo-physical and dynamical carrier properties of the material, potentially becoming a limiting factor to achieving high efficiency. As a consequence, a detailed understanding of the interplay between the film molecular structure and the material properties is essential to properly design devices with optimized performance. Here we demonstrate how different molecular structural arrangements modulate the charge transfer (CT) dynamics in cobalt phthalocyanine (CoPc) thin films. By transient absorption spectroscopy and time-resolved photoemission spectroscopy, we study the influence of different CoPc structures on the dynamical electronic properties, the CoPc intra and inter- molecular de-excitation pathways up to 7 ns. We rationalize the ultrafast formation of triplet states in the CoPc through an electron exchange process between the single-occupied Co3dz2 orbital and p orbitals of the macrocycle, which obviate for an energetically unfavourable spin-flip. We found enhanced CT exciton lifetime in the case of the herringbone structure with respect to the brickwork one, possibly explainable by a more efficient CT exciton delocalization along the stacking axis.
Ključne besede: Charge transfer, organic molecules, time resolved spectroscopies
Objavljeno v RUNG: 30.06.2023; Ogledov: 587; Prenosov: 2
.pdf Celotno besedilo (1,30 MB)
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