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Year 2024
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Advancing sustainable hybrid bitumen systems: A compatibilization solution by functionalized polyolefins for enhanced crumb rubber content in bitumen
PublicationPolymer waste pollution has a profound effect on the environment and, consequently, on the lifestyle of hu- mankind. The massive production and disposal of cross-linked polymers clearly exemplify the challenges of recycling. Increasing efforts are being undertaken to introduce recycled polymers, especially crumb rubber (CR), into asphalt formulations. Due to the rather poor processability and phase separation associated with CR- modified...
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Fluorescence of p-hydroxyazobenzocrowns – Tautomeric equilibrium effect
PublicationThe spectroscopic properties of a series of para-hydroxyazobenzocrowns, including three novel compounds, were investigated using UV–Vis absorption and emission spectroscopy. This study presents, for the first time, determined quantum yield (QY) values for macrocycles of this category, ranging between 0.122 and 0.195. The highest values were obtained for crowns bearing two phenyl substituents in benzene rings. The impact of aromatic...
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Macrocyclic derivatives of imidazole as chromoionophores for bismuth(III)/lead(II) pair
Publication18-membered diazomacrocycles with imidazole or 4-methylimidazole residue as a part of macrocycle were used as chromoionophores in bismuth(III) and lead(II) dual selective optodes for the first time. Cellulose triacetate membranes doped with macrocyclic chromoionophores are bismuth(III) and lead(II) selective with color change from orange/red to different shades of blue and violet, respectively. Results obtained for model and real...
Year 2023
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Chromogenic azomacrocycles with imidazole residue: Structure vs. properties
PublicationNew diazo macrocycles linked by hydrocarbon chain bearing imidazole or 4-methylimidazole residue have been synthetized with satisfactory yield (24–55%). The structure of macrocycles was confirmed by X-ray analysis and spectroscopic methods (1H NMR, MS, FTIR). Metal cation complexation studies were carried out in acetonitrile and acetonitrile-water system. It was found that azomacrocyles form triple-decker complexes with lead(II)....
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Controlling crystallites orientation and facet exposure for enhanced electrochemical properties of polycrystalline MoO3 films
PublicationThis study focuses on the development and optimization of MoO3 films on commercially available FTO substrates using the pulsed laser deposition (PLD) technique. By carefully selecting deposition conditions and implementing post-treatment procedures, precise control over crystallite orientation relative to the substrate is achieved. Deposition at 450 °C in O2 atmosphere results in random crystallite arrangement, while introducing...
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Do Phenyl Substituents Affect the Properties of Azobenzocrown Derivatives?
PublicationNew products of photo- and thermal rearrangements of 19-membered azoxybenzocrown with phenyl substituents in benzene rings in the para positions to oligooxyethylene fragments are characterized. The yields of photochemical transformations depend on the solvent. Para-hydroxyazocrown is formed with yields over 50% in propan-2-ol. Ortho-hydroxyazobenzocrown is obtained with yields up to 70% in toluene/acetic acid mixture. Macrocyclic...
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Enhanced supercapacitor materials from pyrolyzed algae and graphene composites
PublicationThis study focuses on the synthesis and characterization of supercapacitor materials derived from pyrolyzed natural compounds. Four compounds were investigated: methylcellulose with lysine (ML), methylcellulose with lysine-graphene composite (MLG), algae (A), and algae-graphene composite (AG). The pyrolysis process was utilized to convert these natural compounds into carbon-based materials suitable for supercapacitor applications....
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Exfoliated graphite with spinel oxide as an effective hybrid electrocatalyst for water splitting
PublicationThe aim of the conducted research was to develop hybrid nanostructures formed from MnCo2O4 and exfoliated graphite. Carbon added during the synthesis allowed for obtaining a well-distributed MnCo2O4 particle size with exposed active sites contributing to the increased electric conductivity. The influence of the weight ratios of carbon to a catalyst for hydrogen and oxygen evolution reactions was investigated. The new bifunctional...
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Influence of hydrochloric acid concentration and type of nitrogen source on the electrochemical performance of TiO2/N-MoS2 for energy storage applications
PublicationIn this work, nitrogen-doped molybdenum sulfide was directly deposited on titanium dioxide nanotubes substrate (TiO2/N-MoS2) during hydrothermal synthesis. The study focuses on the influence of hydrochloric acid concentration used for the synthesis, with the results indicating its essential role in thioacetamide hydrolysis and thus in the effectiveness of the N-MoS2 deposition. The electrode material itself is characterized by...
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M-BDC (M = Co and/ or Fe) MOFs as effective catalysts for hydrogen generation via hydrolysis of sodium borohydride
PublicationMono- (Co-BDC, Fe-BDC) and bimetallic FeCo-BDC Metal-Organic Frameworks are successfully synthesized by the solvothermal method in DMF at 150 °C within 15 h and tested as catalysts for sodium borohydride hydrolysis. The materials are characterized by FTIR, PXRD, TGA, ICP-OES, H2-TPR, BET model, and SEM-EDS. The catalytic activity of these materials is studied for dehydrogenation of sodium borohydride in water at various temperatures...
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New light on the photocatalytic performance of NH4V4O10 and its composite with rGO
PublicationSolar-driven photocatalysis has shown great potential as a sustainable wastewater treatment technology that utilizes clean solar energy for pollutant degradation. Consequently, much attention is being paid to the development of new, efficient and low-cost photocatalyst materials. In this study, we report the photocatalytic activity of NH4V4O10 (NVO) and its composite with rGO (NVO/rGO). Samples were synthesized via a facile one-pot...
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Recent advancements in molecularly imprinted polymers for the removal of heavy metal ions and dyes
PublicationContamination set off by highly toxic metal ions and dyes is a big threat to the environment and living beings. Various industries like metal plating, mining, pesticides, battery manufacturing, and dyeing release metal ions and toxic dyes directly into the water. It is necessary to remove these toxic substances from the environment. Molecular imprinting technology (MIT) got a lot of attention in the last two decades because of...
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Simple colorimetric copper(II) sensor – spectral characterization and possible applications
PublicationNew o-hydroxyazocompound L bearing pyrrole residue was obtained in the simple synthetic protocol. The structure of L was confirmed and analyzed by X-ray diffraction. It was found that new chemosensor can be successfully used as copper(II) selective spectrophotometric regent in solution and can be also applied for the preparation of sensing materials generating selective color signal upon interaction with copper(II). Selective colorimetric...
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Structurally well-defined functionalized polyolefins and graft copolymers thereof as bitumen modifiers
PublicationHere we demonstrate the application of hydroxyl-functionalized propylene-based copolymers, poly(propylene-co-1-hexene-co-10-undecen-1-ol) (FPP) and poly(styrene-co-maleic anhydride) (SMA) graft copolymers derived thereof, poly(propylene-co-1- hexene-graft-styrene-co-maleic anhydride) (FPP-g-SMA) as bitumen modifiers. The FPP samples were synthesized via solution copolymerization, while FPP-g-SMA products were obtained via transesterification...
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Succinite, Baltic Amber: A Chemical Masterpiece of Nature
PublicationSuccinite, Baltic amber, is one of the most appreciated fossil resins. Its beauty has fascinated people since prehistoric times. It is a substance, and also gemstone, whose uniqueness is due to its compelling, though still not fully understood, physicochemical nature. In this article, some facts about the physical and chemical properties of succinite in order to find an answer for questions about the unique properties of this resin,...
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Synergistic effects of nitrogen-doped carbon and praseodymium oxide in electrochemical water splitting
PublicationHybrid materials featuring perovskite-type metal oxide in conjunction with heteroatom-doped graphene hold immense promise as alternatives to costly noble metal catalysts for electrochemical water splitting, facilitating the generation of environmentally friendly hydrogen. In this study, perovskite-type oxide containing praseodymium, barium, strontium, cobalt, and iron atoms dispersed in a carbon matrix as a catalyst is synthesized...
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The influence of magnetic particle incorporation on bisphenol A removal by β-cyclodextrin-derived sorbent
PublicationA novel, biomass-derived hybrid sorbent Ban-CD-EPI-Fe was successfully synthesized in a coprecipitation method, in which β-cyclodextrin copolymerized with banana peel extract and epichlorohydrin was grafted onto an iron oxide surface. The composition, presence of functional groups, morphology, thermal stability, and magnetic properties of the obtained material were characterized by Powder X-Ray Diffraction (XRD), X-Ray Photoelectron...
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The new method of ZnIn2S4 synthesis on the titania nanotubes substrate with enhanced stability and photoelectrochemical performance
PublicationThe new method of ZnIn2S4 synthesis on the titania nanotubes substrate with enhanced stability and photoelectrochemical performance
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Ti-Fe2O3/In2O3 as photoactive material: The role of the substrate in photoelectrochemical water oxidation
PublicationThe layers of Ti-Fe2O3/In2O3 were prepared on the different substrates using hydrothermal method: Ti/TiO2 nanotubes, Ti foil, FTO and FTO/TiO2. Materials were characterized using scanning electron microscopy, XRD, Raman, UV-Vis, and X-ray photoelectron spectroscopy and tested as photoanodes for water oxidation under illumination. The formation of heterojunction on the TiO2 nanotubes increases photocurrent of water oxidation at...
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Unprecedented Adhesive Performance of Propylene-Based Hydroxyl Functionalized Terpolymers
PublicationThe synthesis of hydroxyl functionalized propylene-based terpolymers and their performance as hot melt adhesives were investigated. The products comprise uniformly distributed butyl and 4-hydroxyl-butyl branches along the polypropylene backbone. Despite the low hydroxyl-functionality level of ≤ 0.5 mol%, hydroxyl functionalized terpolymers show formidable adhesion to aluminum and steel providing an adhesive strength exceeding 16...
Year 2022
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Cellulose and its derivatives, coffee grounds, and cross-linked, β-cyclodextrin in the race for the highest sorption capacity of cationic dyes in accordance with the principles of sustainable development
PublicationIn this study, seven different materials were analyzed and includes coffee grounds (CG), two types of cellulose (CGC and CC), two types of modified cellulose (CT and CTCD), and cross-linked β-cyclodextrin (CD-1 and CD-2) were tested as adsorbents for the removal of dyes from the wastewater. The composition, morphology, and presence of functional groups in the obtained sorption materials were characterized by elemental analysis,...
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Electrochemical synthesis of 2D copper coordination-polymers: Layer-stacking deviation induced by the solvent and its effect on the adsorptive properties
PublicationA 2D Cu-based Metal-Organic Framework (MOF), namely copper-terephthalate (Cu(1,4-BDC)), was successfully synthesized by electrochemical method for effective methylene blue (MB) sorption from aqueous solutions. The composition, morphology, and the presence of functional groups in the obtained material were verified by Fourier Transform Infrared spectroscopy (FTIR), Powder X-Ray Diffraction (PXRD), Thermal (TGA), and Elemental (EA)...
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Hydrogen Storage in Geological Formations—The Potential of Salt Caverns
PublicationHydrogen-based technologies are among the most promising solutions to fulfill the ze- ro-emission scenario and ensure the energy independence of many countries. Hydrogen is considered a green energy carrier, which can be utilized in the energy, transport, and chemical sectors. However, efficient and safe large-scale hydrogen storage is still challenging. The most frequently used hydrogen storage solutions in industry, i.e., compression...
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Hydrothermal modification of TiO2 nanotubes in water and alkali metal electrolytes (LiNO3, NaNO3, KNO3) – Direct evidence for photocatalytic activity enhancement
PublicationThe influence of hydrothermal annealing (HA) of TiO2 nanotubes (TiO2-NTs) in various baths (H2O, LiNO3, NaNO3, KNO3 performed for 4 h, 24 h, 64 h), on their photocatalytic and photoelectrocatalytic properties, was studied. The use of electrolytes was to enable the monitoring of photoactivity changes as a result of the expected impact on the population of hydroxyl groups on the surface. The assumption turned out to be correct and...
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In-Reactor Polypropylene Functionalization─The Influence of Catalyst Structures and Reaction Conditions on the Catalytic Performance
PublicationTo unravel the relationship between silylene-bridged metallocene catalyst structures and polymerization conditions and their effect on the performance in in-reactor functionalization of polypropylene, the behaviors of rac-Me2Si(2-Me-4-Ph-Ind)2ZrCl2/MMAO, rac-Me2Si(Ind)2ZrCl2, rac-Me2Si(2-Me-4-Ph-Ind)2HfCl2, and rac-Me2Si(Ind)2HfCl2 in propylene/aluminum alkyl-passivated 10-undecen-1-ol copolymerization were compared. Kinetic analysis...
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Insight into Potassium Vanadates as Visible-Light-Driven Photocatalysts: Synthesis of V(IV)-Rich Nano/Microstructures for the Photodegradation of Methylene Blue
PublicationPhotocatalysis is regarded as a promising tool for wastewater remediation. In recent years, many studies have focused on investigating novel photocatalysts driven by visible light. In this study, K2V6O16·nH2O nanobelts and KV3O8 microplatelets were synthesized and investigated as photocatalysts. Samples were obtained via the facile method based on liquid-phase exfoliation with ion exchange. By changing the synthesis temperature...
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Modification of TiO2 nanotubes by graphene–strontium and cobalt molybdate perovskite for efficient hydrogen evolution reaction in acidic medium
PublicationHerein, we demonstrate that modification of TiO2 nanotubes with graphene–strontium and cobalt molybdate perovskite can turn them into active electrocatalysts for hydrogen evolution reaction (HER). For this purpose, a simple method of hydrothermal synthesis of perovskites was developed directly on the TiO2 nanotubes substrate. Moreover, the obtained hybrids were also decorated with graphene oxide (GO) during one-step hydrothermal...
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N-doped carbon materials as electrodes for highly stable supercapacitors
PublicationThis article reports a strategy to use nitrogen-doped carbon materials as electrodes for supercapacitors. Depending on the carbon precursor, the porous structure is changed with specific surface area reached up to 2270 m2 g−1. The capacitance of carbon materials used as electrodes is related strictly to pore size. The microstructure and nitrogen functionalities enable a high capacitance (327 F g−1) and cycle durability. The nanoporous...
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Poly(hydroxybutyrate-co-hydroxyvalerate) as a biodegradable binder in a negative electrode material for lithium-ion batteries
PublicationIn this work, graphite-based negative electrode for lithium-ion battery consisting a novel and biodegradable binder poly(hydroxybutyrate-co-hydroxyvalerate) (PHBV) is compared with standard graphite electrode with polyvinylidene fluoride (PVDF) as a binder. The rate and cycling performance of lithium ion insertion/extraction of electrodes with PHBV in a half-cell configuration are evaluated. Moreover, on the basis of the electrochemical...
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Products of Photo- and Thermochemical Rearrangement of 19-Membered di-tert-Butyl-Azoxybenzocrown
PublicationThe preparation and characterization of products of the photochemical and thermochemical rearrangements of 19-membered azoxybenzocrowns with two, bulky, tert-butyl substituents in benzene rings in the para positions to oligooxyethylene fragments (meta positions to azoxy group, i.e., t-Bu-19-Azo-O have been presented. In photochemical rearrangement, two colored typical products were expected, i.e., 19-membered o-hydroxy-m,m′-di-tert-butyl-azobenzocrown...
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Provenance studies on Late Neolithic amber ornaments from North-East Poland
PublicationThe area of North-East Poland was in prehistory, and still is today, an area with easy access to amber as a raw material, as is evidenced in part by numerous Late Neolithic (3rd millennium) amber workshops located in the Gulf of Gdańsk and Żuławy Wiślane (Vistula Fens). Given this fact, it is surprising that only a few finished amber products have been recovered from this area. Among them are unique ornaments from the Late Neolithic...
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Pyrrole bearing diazocrowns: Selective chromoionophores for lead(II) optical sensing
PublicationDiazocrowns of 18-, 21- and 23-membered rings with pyrrole residue as a part of macrocycle were for the first time used as chromoionophores in lead(II) selective optodes. Sensing properties of optodes depend on the type of macrocycle, namely its size and the type of linker: oligoether or hydrocarbon chain. The best results were obtained for optode bearing 18-membered crown with oligoether linker showing linear response range of...
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Recent Advancements in Cyclodextrin-Based Adsorbents for the Removal of Hazardous Pollutants from Waters
PublicationWater is an essential substance for the survival on Earth of all living organisms. However, population growth has disturbed the natural phenomenon of living, due to industrial growth to meet ever expanding demands, and, hence, an exponential increase in environmental pollution has been reported in the last few decades. Moreover, water pollution has drawn major attention for its adverse effects on human health and the ecosystem....
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Recent Progress on Hydrogen Storage and Production Using Chemical Hydrogen Carriers
PublicationDepleting fossil fuel resources and anthropogenic climate changes are the reasons for the intensive development of new, sustainable technologies based on renewable energy sources. One of the most promising strategies is the utilization of hydrogen as an energy vector. However, the limiting issue for large-scale commercialization of hydrogen technologies is a safe, efficient, and economical method of gas storage. In industrial practice,...
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Removal of nonsteroidal anti-inflammatory drugs and analgesics from wastewater by adsorption on cross-linked β-cyclodextrin
PublicationWe present a method using the material in the form of cross-linked β-cyclodextrin (CD) showing high efficiency in the simultaneous removal of hazardous pollutants from sewage, such as diclofenac (DIC), ibuprofen (IBU), ketoprofen (KETO), naproxen (NAPR), salicylic acid (SALI) and tramadol (TRAM). The material is stable and particularly easy to regenerate. The sorbent probably remembers the shape of the contaminants, which increases...
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Self-Organization of Graft Copolymers and Retortable iPP-Based Nanoporous Films Thereof
PublicationPolyolefins might become inexpensive alternatives to the existing membranes based on polyethersulfone. Here we disclose the production of retortable, well-defined PP-based nanoporous membranes derived from amphiphilic graft copolymer precursors. The graft copolymers, containing a polypropylene backbone and polyester grafts, were obtained by grafting lactones, specifically δ-valerolactone and ε-caprolactone, from well-defined randomly...
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SnO2 nanoparticles embedded onto MoS2 nanoflakes - An efficient catalyst for photodegradation of methylene blue and photoreduction of hexavalent chromium
PublicationIn this work, a molybdenum disulfide/tin oxide (MoS2/SnO2) composite was successfully prepared via a hydrothermal method. The MoS2/SnO2 composite was used as a photocatalyst for photoreduction of hexavalent chromium and photodecomposition of methylene blue. It exhibited higher photocatalytic performance under simulated solar light irradiation than MoS2 itself. The obtained material was characterized by several spectroscopic and...
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The phenomenon of increasing capacitance induced by 1T/2H-MoS2 surface modification with Pt particles – Influence on composition and energy storage mechanism
PublicationIn this paper, several approaches to the synthesis of molybdenum-based electrode materials for supercapacitors are presented, including anodization, hydrothermal process and annealing. For the material prepared via anodization of a molybdenum plate, followed by a hydrothermal process in thiourea aqueous solution, a thorough study of the Pt-surface modification through repetitive cycling in 1 M sulfuric acid with Pt acting as a...
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The valance state of vanadium-key factor in the flexibility of potassium vanadates structure as cathode materials in Li-ion batteries
PublicationPotassium hexavanadate (K2V6O16·nH2O) nanobelts have been synthesized by the LPE-IonEx method, which is dedicated to synthesis of transition metal oxide bronzes with controlled morphology and structure. The electrochemical performance of K2V6O16·nH2O as a cathode material for lithium-ion batteries has been evaluated. The KVO nanobelts demonstrated a high discharge capacity of 260 mAh g−1, and long-term cyclic stability up to 100...
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Theoretical designing of selenium heterocyclic non-fullerene acceptors with enhanced power conversion efficiency for organic solar cells: a DFT/TD-DFT-based prediction and understanding
PublicationIn this study, we have designed and explored a new series of non-fullerene acceptors for possible applications in organic solar cells. We have designed four molecules named as APH1 to APH4 after end-capped modification of recently synthesized Y6-Se-4Cl molecule. Density functional theory and time dependent-density functional theory have been employed for computing geometric and photovoltaic parameters of the designed molecules....
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Towards spectroscopic monitoring of photoelectrodes: In-situ Raman photoelectrochemistry of a TiO2/prussian blue photoanode
PublicationHere, novel in-situ Raman photoelectrochemical measurements are performed. The obtained results have proved that it is possible to track the progress of a photoelectrochemical reaction that takes place on a semiconducting electrode using the spectroscopic method. As an exemplary system, the Ti/TiO2/Prussian blue electrode is investigated. Since TiO2 is an n-type semiconductor, it cannot act as an efficient anode in dark conditions....
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Ultrasound-Assisted Dispersive Liquid-Liquid Microextraction Using Deep Eutectic Solvents (DESs) for Neutral Red Dye Spectrophotometric Determination
PublicationDeep eutectic solvents (DES), which have low toxicity and are low cost, biodegradable, and easily synthesized, were used for the extraction of neutral red (NR) dye before its spectrophotometric analysis. DES, containing choline chloride as a hydrogen bond acceptor and phenol as a hydrogen bond donor with a molar ratio of 1:2, was used for the extraction of NR dye from aqueous media. The possible interaction of different DESs with...
Year 2021
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A MEASUREMENT SYSTEM FOR MONITORING CARDIOVASCULAR EVENTS IN SYNCOPE PATIENTS
PublicationSyncope phenomena is an abrupt and transient loss of consciousness leading to interruption of awareness of one’s surroundings and falls with risk of injury. Syncope is often followed by complete and usually rapid spontaneous recovery. It is said that half of all individuals experience syncopal event at least once during their life. The condition can occur at any age and happens in people with and without other medical problems....
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Combined effect of nitrogen-doped functional groups and porosity of porous carbons on electrochemical performance of supercapacitors
PublicationIn this work, nitrogen-doped porous carbons obtained from chitosan, gelatine, and green algae were investigated in their role as supercapacitor electrodes. The effects of three factors on electrochemical performance have been studied— of the specific surface area, functional groups, and a porous structure. Varying nitrogen contents (from 5.46 to 10.08 wt.%) and specific surface areas (from 532 to 1095 m2g−1) were obtained by modifying...
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Deep learning for ultra-fast and high precision screening of energy materials
PublicationSemiconductor materials for energy storage are the core and foundation of modern information society and play important roles in photovoltaic system, integrated circuit, spacecraft technology, lighting applications, and other fields. Unfortunately, due to the long experiment period and high calculation cost, the high-precision band gap (the basic characteristic parameter) of semiconductor is difficult to obtain, which hinders the...
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Detoxification of the tricyclic antidepressant opipramol and its analog – IS-noh by UGT enzymes before and after activation by phase I enzymes in rat liver microsomes
PublicationThe present studies were carried out to evaluate the simultaneous one-pot metabolism of opipramol (IS-opi) and analog (IS-noh) by phase I and phase II enzymes present in rat liver microsomes (RLM) as an alternative to separate testing with recombinant enzymes. This approach allows for more time-saving and cost-effective screening of the metabolism of newly discovered drugs. We also considered that the lack of results for phase...
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Dipodal Tetraamide Derivatives of 1,10-Diaza-18-Crown-6 and Alkylmalonic Acids—Synthesis and Use as Ionophores in Ion Selective Membrane Electrodes
PublicationNovel dipodal derivatives of an 18-membered diaza-crown ether with two diamide chains featuring methylmalonic or butylmalonic acid residues were obtained and tested as ionophores in ion-selective plasticized membrane electrodes. The objective of the study was to identify measurement conditions which ensure the most favorable performance for magnesium ion-selective electrodes. The relationship between the molar lipophilic anion...
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Hydrothermal Cobalt Doping of Titanium Dioxide Nanotubes towards Photoanode Activity Enhancement
PublicationDoping and modification of TiO2 nanotubes were carried out using the hydrothermal method. The introduction of small amounts of cobalt (0.1 at %) into the structure of anatase caused an increase in the absorption of light in the visible spectrum, changes in the position of the flat band potential, a decrease in the threshold potential of water oxidation in the dark, and a significant increase in the anode photocurrent. The material...
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Influence of alkali metal cations on the photoactivity of crystalline and exfoliated amorphous WO3 – photointercalation phenomenon
PublicationIn order to investigate the effect of photointercalation on photoelectrochemical properties, two types of WO3-based photoanodes, bulk and exfoliated have been prepared and investigated. An aqueous exfoliation method is introduced for the simple fabrication of amorphous and hydrated WO3 nanomaterial using commercial bulk WO3 precursor. The comparison of obtained material with bulk WO3 was performed using Raman, UV–vis, and XPS as...
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Materiały sorpcyjne wykorzystywane w maskach ochronnych
PublicationOd zarania dziejów ludzie starają się chronić przed chorobami zakaźnymi, stosując środki ochrony osobistej, do których należą maski ochronne. Z uwagi na obecnie panującą pandemię wirusa SARS-CoV-2, noszenie masek stało się normą w walce z koronawirusem. Jednak zagrożenia dla górnych dróg oddechowych nie stanowią wyłącznie wirusy, lecz również cząstki stałe zawieszone w powietrzu. Szczególnie w krajach wysoko uprzemysłowionych,...