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1.
Engineering of functional nanosnowflakes from gold nanocarriers capped with amino-modified DNA oligonucleotides
Alexandre Loukanov, Velichka Arahangelova, Saim Emin, Chavdar Filipov, 2023, izvirni znanstveni članek

Opis: Abstract The design, engineering and electron microscopic characterization of anisotropic nanosized snowflake‐like structural assemblies (nanosnowflakes) is reported. They were fabricated through immobilization of double stranded amine‐modified and thiol‐terminated DNA oligonucleotides on the surface of ultra‐small isotropic gold nanoparticles used as nanocarriers. The transmission electron microscopy images combined with spectrophotometric data revealed the formation of self‐assembled structural aggregation between individual ligands‐coated nanoparticles. They act as seeds for the further spontaneous dendritic growth in different directions. Their anisotropic morphology is formed due to the occurrence of facilitated electrostatic interactions between positive charged amino‐groups and the negative sugar‐phosphate backbone of oligonucleotides. Thus, nanosnowflakes with size distribution between 40 and 80 nm were obtained. The microscopic analysis demonstrated also that the stable nanosnowflakes structure was highly dependent on the solution ionic strength, which effect the charge fluctuation within the assembly. The reported DNA functionalized nanostructures have potential to be applied as a platform for development of therapeutic materials, as well as drug delivery nanosystems. Research Highlights The engineering, fabrication, and microscopic characterization of DNA nanosnowflakes is reported. The electron microscopy analysis revealed formation of self‐assemblies with anisotropic morphology. The nanosnowflakes size distribution was between 40 and 80 nm.
Ključne besede: DNA, nanocarrier, functionalization, drug delivery
Objavljeno v RUNG: 18.03.2024; Ogledov: 152; Prenosov: 0
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2.
Photoelectrochemical activation of peroxymonosulfate using Sn-doped ▫$α-Fe_2O_3$▫ thin film for degradation of anti-inflammatory pharmaceutical drug
Manel Machreki, Georgi Tyuliev, Dušan Žigon, Qian Guo, Takwa Chouki, Ana Belén Jorge Sobrido, Stoichko Dimitrov, Saim Emin, 2024, izvirni znanstveni članek

Opis: Introduction of oxygen vacancies (OVs) has been investigated as a promising way to improve the electrical and catalytic characteristics of a hematite (α-Fe2O3) based photoelectrode. In this work, we develop a novel method for preparing porous Sn-doped α-Fe2O3 (Sn:Fe2O3) thin films with intrinsic OVs. The procedure included spin- coating an iron precursor onto a fluorine-doped tin oxide (FTO) substrate, followed by thermal treatment at elevated temperatures. The influence of Sn dopant on the optoelectronic properties of α-Fe2O3 was demonstrated by X-ray photoelectron spectroscopy and photoelectrochemical (PEC) measurements. The combined effect of OVs and Sn doping was found to play a synergistic role in reducing the charge recombination’s. The Sn:Fe2O3 photoanodes were used as a dual catalyst to oxidise water and break down an anti-inflammatory drug called 2-(4- isobutylphenyl)propanoic acid (IBPA). The Sn:Fe2O3 thin film with a 30-minute heat treatment time displayed the highest incident photon-to-current efficiency. For the first time, Sn:Fe2O3 thin films were utilised in the effective PEC degradation of IBPA employing peroxymonosulfate (PMS) under visible light illumination. The hydroxyl radicals (•OH), singlet oxygen (1O2), photogenerated holes (h+), and sulfate radicals (SO4 • ) were discovered to be the main reactive species during PEC degradation. IBPA degradation and the formation of new compounds were verified using liquid chromatography-mass spectrometry. The Lepidium sativum L phytotoxicity test reveals that PEC-treated wastewater with IBPA exhibits decreased toxicity.
Ključne besede: Sn-doped Fe2O3, oxygen vacancies, photoelectrochemical degradation, 2-(4-isobutylphenyl)propanoic acid, peroxymonosulfate
Objavljeno v RUNG: 10.01.2024; Ogledov: 356; Prenosov: 6
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3.
Materials for sustainable electrochemical energy conversion
Saim Emin, Takwa Chouki, Manel Machreki, 2023, objavljeni povzetek znanstvenega prispevka na konferenci (vabljeno predavanje)

Opis: The process of hydrogen evolution reaction (HER) through water electrolysis is an important technology for establishing the so called "hydrogen economy". Here we will cover different systems for electrocatalytic HER. Transition metal carbides and metal phosphides are alternative to platinum (Pt) and offer excellent electrocatalytic activity for HER. Pyrolysis of hexacarbonyl tungsten, W(CO)6, in 1-octadecene has been used to prepare colloidal tungsten, W, nanoparticles (NPs) [1]. The obtained W NPs has been spin-coated on graphite (C) electrodes. Heat treatment of the W/C electrodes at elevated temperatures (≥ 900°C) allows the preparation of metallic W and tungsten carbide (W2C@WC) thin films. The obtained W2C@WC electrodes were used for hydrogen evolution studies (HER) in 0.5M H2SO4. Cyclic voltammetry tests for 1000 cycles showed that W2C@WC exhibit long term stability without significant drop in current density. The overpotential defined at 10 mA/cm2 is 310 mV vs. RHE giving an excellent catalytic activity for HER. Iron phosphide electrocatalysts were synthesized using a triphenylphosphine (TPP) precursor. Different iron phosphide phases were synthesized at 300°C (Fe2P) and at 350°C ( FeP ) [2]. To enhance the catalytic activities of obtained iron phosphide particles heat-treatments were carried out at elevated temperatures. Annealing at 500°C under reductive atmosphere induced structural changes in the samples: (i) Fe2P provided a pure Fe3P phase (Fe3P−500°C) and (ii) FeP transformed into a mixture of iron phosphide phases (Fe2P/FeP−500°C). The lowest electrode potential of 110 mV vs. a reversible hydrogen electrode (RHE) at 10 mA cm−2 was achieved with Fe2P/FeP−500°C catalyst
Ključne besede: Fe2P, electrocatalysis, hydrogen, ammonia
Objavljeno v RUNG: 13.12.2023; Ogledov: 481; Prenosov: 3
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4.
The role of lattice defects on the optical properties of TiO[sub]2 nanotube arrays for synergistic water splitting
Manel Machreki, Takwa Chouki, Georgi Tyuliev, Mattia Fanetti, Matjaž Valant, Denis Arčon, Matej Pregelj, Saim Emin, 2023, izvirni znanstveni članek

Opis: In this study, we report a facile one-step chemical method to synthesize reduced titanium dioxide (TiO2) nanotube arrays (NTAs) with point defects. Treatment with NaBH4 introduces oxygen vacancies (OVs) in the TiO2 lattice. Chemical analysis and optical studies indicate that the OV density can be significantly increased by changing reduction time treatment, leading to higher optical transmission of the TiO2 NTAs and retarded carrier recombination in the photoelectrochemical process. A cathodoluminescence (CL) study of reduced TiO2 (TiO2–x) NTAs revealed that OVs contribute significantly to the emission bands in the visible range. It was found that the TiO2 NTAs reduced for a longer duration exhibited a higher concentration of OVs. A typical CL spectrum of TiO2 was deconvoluted to four Gaussian components, assigned to F, F+, and Ti3+ centers.
Ključne besede: TiO2 nanotubes, defects, cathodoluminescence
Objavljeno v RUNG: 13.12.2023; Ogledov: 285; Prenosov: 7
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5.
Tuning the activity of iron phosphide electrocatalysts for sustainable energy conversion
Saim Emin, Takwa Chouki, Manel Machreki, 2023, objavljeni povzetek znanstvenega prispevka na konferenci (vabljeno predavanje)

Opis: Electrocatalysis is a promising approach for the sustainable conversion of renewable energy sources, such as solar and wind power, into chemical energy that can be stored and used on demand. By harnessing renewable electricity to drive electrochemical reactions, we can produce fuels and chemicals in a way that is both clean and cost-effective. As we continue to develop new electrocatalytic materials and improve the efficiency of existing processes, the potential for electrocatalysis to transform our energy system will only continue to grow. We report the use of iron phosphide (Fe2P, FeP) in several electrocatalytic applications, such as reduction of nitrate ions (NO3), hydrogen and oxygen evolution studies. The electrochemical reduction of the nitrate ion (NO3), a widespread water pollutant, to valuable ammonia (NH3) is a promising approach to achieving green energy conservation. Particularly, FeP and Fe2P phases were successfully demonstrated as efficient catalysts for NH3 generation. Detection of the in-situ formed product using a bi-potentiostat was achieved by electrooxidation of NH3 to nitrogen (N2) on a Pt electrode. The Fe2P catalyst exhibits the highest Faradaic efficiency (96%) for NH3 generation with a yield (0.25 mmol h−1 cm-−2 or 2.10 mg h−1 cm−2) at −0.55 V vs. reversible hydrogen electrode (RHE). To get relevant information about the reaction mechanisms and the fundamental origins behind the better performance of Fe2P, density functional theory (DFT) calculations were performed.
Ključne besede: Fe2P, FeP, electrocatalysis, NH3 reduction, counter electrode
Objavljeno v RUNG: 04.12.2023; Ogledov: 418; Prenosov: 4
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6.
A novel multi-functional thiophene-based organic cation as passivation, crystalline orientation, and organic spacer agent for low-dimensional 3D/1D perovskite solar cells
Ali Semerci, Ali Buyruk, Saim Emin, Rik Hooijer, Daniela Kovacheva, Peter Mayer, Manuel A. Reus, Dominic Blätte, Marcella Günther, Nicolai F. Hartmann, 2023, izvirni znanstveni članek

Opis: Recently, the mixed-dimensional (3D/2D or 3D/1D) perovskite solar cellsusing small organic spacers have attracted interest due to their outstandinglong-term stability. Here, a new type of thiophene-based organic cation2-(thiophene-2yl-)pyridine-1-ium iodide (ThPyI), which is used to fabricatemixed-dimensional 3D/1D perovskite solar cells, is presented. TheThPyI-based 1D perovskitoid is applied as a passivator on top of a 3D methylammonium lead iodide (MAPI) to fabricate surface-passivated 3D/1Dperovskite films or added alone into the 3D perovskite precursor to generatebulk-passivated 3D MAPI. The 1D perovskitoid acts as a passivating agent atthe grain boundaries of surface-passivated 3D/1D, which improves the powerconversion efficiency (PCE) of the solar cells. Grazing incidence wide-angleX-ray scattering (GIWAXS) studies confirm that ThPyI triggers the preferentialorientation of the bulk MAPI slabs, which is essential to enhance chargetransport. Champion bulk-passivated 3D and surface-passivated 3D/1Ddevices yield 14.10% and 19.60% PCE, respectively. The bulk-passivated 3Doffers favorable stability, with 84% PCE retained after 2000 h withoutencapsulation. This study brings a new perspective to the design of organicspacers having a different binding motif and a passivation strategy to mitigatethe impact of defects in hybrid 3D/1D perovskite solar cells.A. Semerci, A. Buyruk, R. Hooijer, P. Mayer, D. Blätte, M. Günther, T. Bein,T. AmeriDepartment of Chemistry and Center for NanoScience (CeNS)Ludwig-Maximilians-Universität MünchenButenandtstrasse 5–13 (E), 81377 Munich, GermanyE-mail:tayebeh.ameri@ed.ac.ukS.EminMaterialsResearchLaboratoryUniversityofNovaGoricaVipavska13c,Ajdovšˇcina5270,SloveniaThe ORCID identification number(s) for the author(s) of this articlecan be found under https://doi.org/10.1002/adom.202300267© 2023 The Authors. Advanced Optical Materials published byWiley-VCH GmbH. This is an open access article under the terms of theCreative Commons Attribution-NonCommercial License, which permitsuse, distribution and reproduction in any medium, provided the originalwork is properly cited and is not used for commercial purposes.DOI: 10.1002/adom.2023002671. IntroductionDuring the last decade, 3D organic–inorganic halide perovskites (OIHPs) haveemerged as promising absorber materialsfor photovoltaic applications due to theirsuperior properties such as high absorp-tion coefficient, long diffusion length ofthe charge carriers, fast charge transport,and tunable bandgap. The 3D OIHPs havedemonstrated rapid increase in powerconversion efficiency (PCE) from 3.8% to25.2%.[1–9]On the other hand, their mod-erate intrinsic stability against moistureand heat still has been a concern with aview on possible commercialization.[10–14]Instability of the 3D methyl ammoniumlead iodide (MAPI) perovskite is assumedto be due to its crystalline structure. Ionicmigration is now well recognized to affectthe photovoltaic properties of perovskitesolar cells. Especially, the ionic migrationcauses the generation and displacement ofvacancies in perovskite materials. OIHPsare mixed ionic–electronic conductors withiodide ions as the majority of ionic carriers.D. KovachevaInstitute of General and Inorganic ChemistryBulgarian Academy of SciencesSofia 1113, BulgariaM. A. Reus, P. Müller-BuschbaumTUM School of Natural SciencesDepartment of PhysicsChair for Functional MaterialsTechnical University of MunichJames-Franck-Str. 1, 85748 Garching, GermanyN. F. HartmannAttocube systems AGNanoscale AnalyticsneaspecEglfinger Weg 2, 85540 Haar, GermanyS. Lotfi, J. P. HofmannSurface Science LaboratoryDepartment of Materials and Earth SciencesTechnical University of DarmstadtOtto-Berndt-Str. 3, 64287 Darmstadt, GermanyAdv. Optical Mater.2023,11, 23002672300267 (1 of 13)© 2023 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
Ključne besede: perovskites, solar cells, passivation
Objavljeno v RUNG: 04.12.2023; Ogledov: 382; Prenosov: 2
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7.
Efficient electrochemical nitrogen fixation at iron phosphide (Fe_2P) catalyst in alkaline medium
Beata Rytelewska, Anna Chmielnicka, Takwa Chouki, Magdalena Skunik-Nuckowka, Shaghayegh Naghdi, Dominik Eder, Aleksandra Michalowska, Tomasz Ratajczyk, Egon Pavlica, Saim Emin, 2023, izvirni znanstveni članek

Opis: A catalytic system based on iron phosphide (Fe2P) has exhibited electrocatalytic activity toward N2-reduction reaction in alkaline medium (0.5 mol dm−3 NaOH). Based on voltammetric stripping-type electroanalytical measurements, Raman spectroscopic and spectrophotometric data, it can be stated that the Fe2P catalyst facilitates conversion of N2 to NH3, and the process is fairly selective with respect to the competing hydrogen evolution. A series of diagnostic electrocatalytic experiments (utilizing platinum nanoparticles and HKUST-1) have been proposed and performed to control purity of nitrogen gas and to probe presence of potential contaminants such as ammonia, nitrogen oxo-species and oxygen. On the whole, the results are consistent with the view that the interfacial reduced-iron (Fe0) centers, while existing within the network of P sites, induce activation and reduction of nitrogen, parallel to the water splitting (reduction) to hydrogen. It is apparent from Tafel plots and impedance measurements that mechanism and dynamics of nitrogen reduction depends on the applied electroreduction potential. The catalytic system exhibits certain tolerance with respect to the competitive hydrogen evolution and gives (during electrolysis at -0.4 V vs. RHE) the Faradaic efficiency, namely, the selectivity (molar) efficiency, toward production of NH3 on the level of 60%. Under such conditions, the NH3-yield rate has been found to be equal to 7.5 µmol cm−2 h−1 (21 µmol m−2 s−1). By referring to classic concepts of electrochemical kinetic analysis, the rate constant in heterogeneous units has been found to be on the moderate level of 1-2*10−4 cm s−1 (at -0.4 V). The above mentioned iron-phosphorous active sites, which are generated on surfaces of Fe2P particles, have also been demonstrated to exhibit strong catalytic properties during reductions of other electrochemically inert reactants, such as oxygen, nitrites and nitrates.
Ključne besede: nitrogen reduction, alkaline medium, iron phosphide catalyst, ammonia, electrochemical determinations
Objavljeno v RUNG: 30.11.2023; Ogledov: 511; Prenosov: 3
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8.
9.
Defective ▫$TiO_2$▫ nanotube arrays for efficient photoelectrochemical degradation of organic pollutants
Manel Machreki, Takwa Chouki, Georgi Tyuliev, Dušan Žigon, Bunsho Ohtani, Alexandre Loukanov, Plamen Stefanov, Saim Emin, 2023, izvirni znanstveni članek

Opis: Oxygen vacancies (OVs) are one of the most critical factors that enhance the electrical and catalytic characteristics of metal oxide-based photo-electrodes. In this work, a simple procedure was applied to prepare reduced TiO 2 nanotube arrays (NTAs) (TiO 2−x) via a one-step reduction method using NaBH 4. A series of characterization techniques were used to study the structural, optical, and electronic properties of TiO 2−x NTAs. X-ray photoelectron spectroscopy confirmed the presence of defects in TiO 2−x NTAs. Photoacoustic measurements were used to estimate the electron-trap density in the NTAs. Photoelectrochemical studies show that the photocurrent density of TiO 2−x NTAs was nearly 3 times higher than that of pristine TiO 2. It was found that increasing OVs in TiO 2 affects the surface recombination centers, enhances electrical conductivity, and improves charge transport. For the first time, a TiO 2−x photoanode was used in the photo-electrochemical (PEC) degradation of a textile dye (basic blue 41, B41) and ibuprofen (IBF) pharmaceutical using in situ generated reactive chlorine species (RCS). Liquid chromatography coupled with mass spectrometry was used to study the mechanisms for the degradation of B41 and IBF. Phytotoxicity tests of B41 and IBF solutions were performed using Lepidium sativum L. to evaluate the potential acute toxicity before and after the PEC treatment. The present work provides efficient PEC degradation of the B41 dye and IBF in the presence of RCS without generating harmful products.
Ključne besede: TiO2, nanotube arrays, photoelectrochemical degradation, organic pollutants
Objavljeno v RUNG: 12.06.2023; Ogledov: 917; Prenosov: 7
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