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  • Vucetic, Nemanja, et al. (författare)
  • Tuned Bis-Layered Supported Ionic Liquid Catalyst (SILCA) for Competitive Activity in the Heck Reaction of Iodobenzene and Butyl Acrylate
  • 2020
  • Ingår i: Catalysts. - : MDPI. - 2073-4344. ; 10:9
  • Tidskriftsartikel (refereegranskat)abstract
    • A thorough experimental optimization of supported ionic liquid catalyst (SILCA) was performed in order to obtain a stable and efficient catalyst for the Heck reaction. Out of fifteen proposed structures, propyl imidazolium bromide-tetramethylguanidinium pentanoate modified SiO2 loaded with PdCl2 appeared to be the most stable and to have a good activity in the reaction between butylacrylate and iodobezene, resulting in a complete conversion in 40 min at 100 °C, in four consecutive experiments. This study elucidated on the stability of the catalytic system with an ionic liquid layer during the catalyst synthesis but also under reaction conditions. In the bis-layered catalyst, the imidazolium moiety as a part of internal layer, brought rigidity to the structure, while in external layer pentanoic acid gave sufficiently acidic carboxylic group capable to coordinate 1,1,3,3-tetramethylguanidine (TMG) and thus, allow good dispersion of Pd nanoparticles. The catalyst was characterized by means of XPS, FT-IR, TEM, ICP-OES, ζ-potential, EDX, TGA, and 13C NMR. The release and catch mechanism was observed, whereas Pd re-deposition can be hindered by catalyst poisoning and eventual loss of palladium.
  • Guo, Y., et al. (författare)
  • Reversible Structural Isomerization of Nature's Water Oxidation Catalyst Prior to O-O Bond Formation
  • 2022
  • Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 144:26, s. 11736-11747
  • Tidskriftsartikel (refereegranskat)abstract
    • Photosynthetic water oxidation is catalyzed by a manganese-calcium oxide cluster, which experiences five "S-states" during a light-driven reaction cycle. The unique "distorted chair"-like geometry of the Mn4CaO5(6)cluster shows structural flexibility that has been frequently proposed to involve "open" and "closed"-cubane forms from the S1 to S3states. The isomers are interconvertible in the S1 and S2states, while in the S3state, the open-cubane structure is observed to dominate inThermosynechococcus elongatus (cyanobacteria) samples. In this work, using density functional theory calculations, we go beyond the S3+Yzstate to the S3nYz•→ S4+Yzstep, and report for the first time that the reversible isomerism, which is suppressed in the S3+Yzstate, is fully recovered in the ensuing S3nYz•state due to the proton release from a manganese-bound water ligand. The altered coordination strength of the manganese-ligand facilitates formation of the closed-cubane form, in a dynamic equilibrium with the open-cubane form. This tautomerism immediately preceding dioxygen formation may constitute the rate limiting step for O2formation, and exert a significant influence on the water oxidation mechanism in photosystem II. 
  • Björn van Praagh, Helena, et al. (författare)
  • Metabolic fate of C-14-labelled chlorinated and non-chlorinated fatty acids in goldfish (Carassius auratus)
  • 2004
  • Ingår i: Fish Physiology & Biochemistry. - : Springer. - 0920-1742 .- 1573-5168. ; 30:1, s. 13-20
  • Tidskriftsartikel (refereegranskat)abstract
    • In order to study the metabolic fate of chlorinated fatty acids in fish, goldfish were fed either 9,10-dichlorostearic acid or oleic acid, chosen as the unchlorinated analogue, both radiolabelled at either the carboxyl (1st) or the terminal (18th) carbon of the fatty acid chain. By keeping the fish in hermetically closed aquaria, all the respired, assimilated and excreted radioactivity could be accounted for. Fish fed 9,10-dichlorostearic acid labelled in the terminal end respired radioactive CO2 to a much lower degree than fish fed the other test compounds. As a consequence, the radioactivity bound in lipids was higher in the group of fish fed dichlorostearic acid labelled in the terminal end. It is suggested that the chlorine atoms in the middle of the carbon chain obstruct the metabolic turn-over of 9,10-dichlorostearic acid, which may have an impact on the residence time of these compounds in the ecosystem.
  • Khokarale, Santosh G., et al. (författare)
  • One-Pot, Metal-Free Synthesis of Dimethyl Carbonate from CO2 at Room Temperature
  • 2020
  • Ingår i: Sustainable Chemistry. - : MDPI. - 2673-4079. ; 1:3, s. 298-314
  • Tidskriftsartikel (refereegranskat)abstract
    • Herein, we report on the metal-free, one-pot synthesis of industrially important dimethyl carbonate (DMC) from molecular CO2 under ambient conditions. In this process, initially the CO2 was chemisorbed through the formation of a switchable ionic liquid (SIL), [DBUH] [CH3CO3], by the interaction of CO2 with an equivalent mixture of organic superbase 1,8-diazabicyclo-[5.4.0]-undec-7-ene (DBU) and methanol. The obtained SIL further reacted with methyl iodide (CH3I) to form DMC. The synthesis was carried out in both dimethyl sulfoxide (DMSO) and methanol. Methanol is preferred, as it not only served as a reagent and solvent in CO2 capture and DMC synthesis, but it also assisted in controlling the side reactions between chemical species such as CH3I and [DBUH]+ cation and increased the yield of DMC. Hence, the use of methanol avoided the loss of captured CO2 and favored the formation of DMC with high selectivity. Under the applied reaction conditions, 89% of the captured CO2 was converted to DMC. DBU was obtained, achieving 86% recovery of its salts formed during the synthesis. Most importantly, in this report we describe a simple and renewable solvent-based process for a metal-free approach to DMC synthesis under industrially feasible reaction conditions.
  • Mousavinejad, Atiyeh, et al. (författare)
  • Nickel-Based Metal–Organic Frameworks to Improve the CO2/CH4 Separation Capability of Thin-Film Pebax Membranes
  • 2020
  • Ingår i: Industrial & Engineering Chemistry Research. - : American Chemical Society (ACS). - 0888-5885 .- 1520-5045. ; 59:28, s. 12834-12844
  • Tidskriftsartikel (refereegranskat)abstract
    • Incorporating metal–organic frameworks (MOFs) into the thin layer of thin-film composite (TFC) membranes is an effective way of improving the CO2/CH4 separation performance. In this study, porous polyethersulfone (PES) membranes were surface-coated with a novel CO2-permeable layer consisting of CO2-philic Pebax and nickel-based MOF particles. The MOF particles were synthesized using nickel(II) acetate tetrahydrate as a metal source and 2-amino-1,4-dicarboxybenzene (NH2-BDC) as an organic linker. The properties and performance of the MOFs and synthesized membranes were assessed using analytical techniques including differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), field-emission scanning electron microscopy (FE-SEM), and dynamic light scattering (DLS). DLS analysis showed that the MOF particle size range was in a range of 350–650 nm. Moreover, cross-sectional FE-SEM images depicted that a uniform and dense Pebax layer was shaped on top of the PES substrate. Well dispersion of the particles was demonstrated by surface FE-SEM imaging. DSC analysis showed that embedding Ni-NH2-BDC MOF particles into the Pebax-1657 film increased the crystallinity degree and the glass-transition temperature (Tg) of resulted membranes. To evaluate the membrane’s separation performance, permeation experiments were performed with CO2, CH4, and CO2/CH4 mixtures at ambient temperature. Embedding 5 wt % Ni-based MOF particles improved the CO2 permeability and CO2/CH4 selectivity from 19.05 Barrer and 32.2 to 31.55 Barrer and 94, respectively, compared to MOF-free membranes. Loading MOF particles into the Pebax matrix also improved the real gas separation factor. The obtained results demonstrate the great potential of the fabricated TFC membranes for gas separation.
  • Rickaby, Rosalind E. M., et al. (författare)
  • Perturbing phytoplankton : response and isotopic fractionation with changing carbonate chemistry in two coccolithophore species
  • 2010
  • Ingår i: Climate of the Past. - : Copernicus Publications on behalf of the European Geosciences Union. - 1814-9324 .- 1814-9332. ; 6, s. 771-785
  • Tidskriftsartikel (refereegranskat)abstract
    • All species of coccolithophore appear to respond to perturbations of carbonate chemistry in a different way. Here, we show that the degree of malformation, growthrate and stable isotopic composition of organic matter and carbonate produced by two contrasting species of coccolithophore (Gephyrocapsa oceanica and Coccolithus pelagicusssp. braarudii) are indicative of differences between their photosynthetic and calcification response to changing DIC levels (ranging from 1100 to 7800 μmol kg−1) at constant pH (8.13±0.02). Gephyrocapsa oceanica thrived under all conditions of DIC, showing evidence of increased growth rates at higher DIC, but C. braarudii was detrimentally affected at high DIC showing signs of malformation, and decreased growth rates. The carbon isotopic fractionation into organic matter and the coccoliths suggests that C. braarudii utilises a common internal pool of carbon for calcification and photosynthesis but G. oceanica relies on independent supplies for each process. All coccolithophores appear to utilize bicarbonate as their ultimate source of carbon for calcification resulting in the release of a proton. But, we suggest that this proton can be harnessed to enhance the supply of CO2(aq) for photosynthesis either from a large internal HCO−3 pool which acts as a pH buffer (C. braarudii), or pumped externally to aid the diffusive supply of CO2 across the membrane from the abundant HCO−3 (G. oceanica), likely mediated by an internal and external carbonic anhydrase respectively. Our simplified hypothetical spectrum of physiologies may provide a context to understand different species response to changing pH and DIC, the species specific Ep and calcite “vital effects”, as well as accounting for geological trends in coccolithophore cell size.
  • Kylin, Henrik, et al. (författare)
  • Evaluating threats to an endangered species by proxy : air pollution as threat to the blue swallow (Hirundo atrocaerulea) in South Africa
  • 2011
  • Ingår i: Environmental Science and Pollution Research. - : Springer. - 0944-1344 .- 1614-7499. ; 18:2, s. 282-290
  • Tidskriftsartikel (refereegranskat)abstract
    • Background, aim, and scope: The blue swallow (Hirundo atrocaerulea) is one of the most threatened bird species in southern Africa. Among terrestrial birds, its plumage is known to be the most water repellent, an adaptation to foraging on the wing in dense fog. Despite this uniqueadaptation, the nesting success of the blue swallow at the Blue Swallow Natural Heritage Site (BSNHS) is lower during years with high incidence of fog. As the phenomenon is not observed at other nesting sites, we hypothesized that this is due to changes in the air chemistry at the BSNHS. In the immediate proximity of the BSNHS, plantations of exotic trees (e.g., pines and eucalypts), rich in volatile organic compounds (VOCs), are dominant features. In addition, air pollution from the Johannesburg area is transported with the surface winds and mix withVOCs released from exotic trees. Together with the high humidity and high elevation, these conditions may result in the formation of sulphonates. Sulphonates are strong detergents, and the presence of these in the fog could lead to decreased water repellence of the plumage. This study was performed in order to determine the occurrence and distribution of sulphonates in the BSNHS and to compare these with sulphonates formed in other locations in South Africa. Because the blue swallow is endangered, pine needles were used as proxy to detect formation of sulphonates.Methods: We sampled pine needles with different exposure to air pollutants, in climates with different humidity, and at different elevation and analyzed these for sulphonates using mass spectrometry.Results: Pine needles from high elevations and the BSNHS, with high humidity, and exposure to air pollution contained significantly higher concentrations of sulphonates than pine needles from low elevations or from high elevations with a dryer climate or a different combination of air pollutants.Conclusions: These findings lead to two conclusions. First, the occurrence and distribution of sulphonates may be explained by chemical reactions between sulphur dioxide and organic compounds in the humid air induced by ultraviolet radiation. Second, elevated concentrations of sulphonates in the fog could affect the water repellence of the blue swallow plumage, possibly decreasing their capacity to forage in the fog. We cannot prove conclusively that this is the reason why the number of blue swallows atthe BSNHS has decreased dramatically, but for endangered species, we may have to rely on proxies to draw conclusions about outside threats. All such information should be valuable in devising protection plans for species under threat.Recommendations and perspectives: The use of proxies to elucidate threats to endangered species should be evaluated in a broad scale. The mist-belt habitat in general is threatened by many human activities. These findings indicate that air pollution and the proximity of volatile organic compound (VOC) sources close to mist-belt habitat refuges may be an unrecognised conservation threat to the animals inhabiting them.
  • Bui, Thai Q., et al. (författare)
  • Mesoporous Melamine-Formaldehyde Resins as Efficient Heterogeneous Catalyst for Continuous Synthesis of Cyclic Carbonates from Epoxides and gaseous CO2
  • 2020
  • Ingår i: ACS Sustainable Chemistry and Engineering. - : American Chemical Society (ACS). - 2168-0485. ; 8:34, s. 12852-12869
  • Tidskriftsartikel (refereegranskat)abstract
    • Herein we report the application of inexpensive mesoporous melamine-formaldehyde resins (MMFR and MMFR250) obtained by a novel template-free and organosolvent-free hydrothermal method as efficient heterogeneous catalysts for direct synthesis of cyclic carbonates from CO2 and epoxides (epichlorohydrin, butylene oxide and styrene oxide). The catalytic activity of the melamine resins was attributed to the abundant Lewis basic N-sites capable of activating CO2 molecules. Based on CO2-Temperature programmed desorption, the concentration of surface basic sites for MMFR and MMFR250 were estimated to be 172 and 56 µmol/g, while the activation energy of CO2 desorption (strength of basic sites) were calculated to be 92.1 and 64.5 kJ/mol. We also observed considerable differences in the catalytic activity and stability of polymeric catalysts in batch and in continuous-flow mode; due to the existence of a synergism between adsorption of CO2 and cyclic carbonates (poison). Our experiments also revealed important role of catalyst surface chemistry and CO2 partial pressure upon catalyst poisoning. Nevertheless, owing to their unique properties (large specific surface area, large mesoporous and CO2 basicity) melamine resins presented excellent activity (turnover frequency 207-2147 h-1), selectivity (>99%) for carbonation of epoxides with CO2 (20 bar initial CO2 or CO2:epoxide mole ratio ~1.5) under solvent-free and co-catalyst-free conditions at 100-120 oC. Most importantly, these low-cost polymeric catalysts were reusable and demonstrated exceptional stability in a flow reactor (tested upto 13 days time on stream, weight hourly space velocity 0.26-1.91 h-1) for continuous cyclic carbonate production from gaseous CO2 with different epoxides (conversion 76-100% and selectivity >99%) under industrially relevant conditions (120 oC, 13 bar, solvent-free/co-catalyst-free) confirming their superiority over the previously reported catalytic materials.
  • Saeid, Soudabeh, et al. (författare)
  • Synthesis and Characterization of Metal Modified Catalysts for Decomposition of Ibuprofen from Aqueous Solutions
  • 2020
  • Ingår i: Catalysts. - : MDPI. - 2073-4344. ; 10:7
  • Tidskriftsartikel (övrigt vetenskapligt)abstract
    • The presence of pharmaceuticals in surface water, drinking water, and wastewater has attracted significant concern because of the non-biodegradability, resistance, and toxicity of pharmaceutical compounds. The catalytic ozonation of an anti-inflammatory pharmaceutical, ibuprofen was investigated in this work. The reaction mixture was analyzed and measured by high-performance liquid chromatography (HPLC). Liquid chromatography-mass spectrometry (LC-MS) was used for the quantification of by-products during the catalytic ozonation process. Ibuprofen was degraded by ozonation under optimized conditions within 1 h. However, some intermediate oxidation products were detected during the ibuprofen ozonation process that were more resistant than the parent compound. To optimize the process, nine heterogeneous catalysts were synthesized using different preparation methods and used with ozone to degrade the ibuprofen dissolved in aqueous solution. The aim of using several catalysts was to reveal the effect of various catalyst preparation methods on the degradation of ibuprofen as well as the formation and elimination of by-products. Furthermore, the goal was to reveal the influence of various support structures and different metals such as Pd-, Fe-, Ni-, metal particle size, and metal dispersion in ozone degradation. Most of the catalysts improved the elimination kinetics of the by-products. Among these catalysts, Cu-H-Beta-150-DP synthesized by the deposition–precipitation process showed the highest decomposition rate. The regenerated Cu-H-Beta-150-DP catalyst preserved the catalytic activity to that of the fresh catalyst. The catalyst characterization methods applied in this work included nitrogen adsorption–desorption, scanning electron microscopy, transmission electron microscopy, and Fourier-transform infrared spectroscopy. The large pore volume and small metal particle size contributed to the improved catalytic activity.
  • Slavinskaya, E. M., et al. (författare)
  • Thermal activation of Pd/CeO2-SnO2 catalysts for low-temperature CO oxidation
  • 2020
  • Ingår i: Applied Catalysis B. - : Elsevier. - 0926-3373 .- 1873-3883. ; 277
  • Tidskriftsartikel (refereegranskat)abstract
    • In this work, the counter precipitation method was used to synthesise Pd/CeO2-SnO2 catalysts, which possess excellent low-temperature activity and high thermal stability. It was revealed that calcination of Pd/CeO2-SnO2 catalysts at 800−1000 °C induces significant growth of catalytic activity in CO oxidation at T<150 °C. This effect of thermal activation for Pd/CeO2-SnO2 catalysts was enhanced when water was admitted to the reaction mixture. In the presence of water the T50 value for the Pd/CeO2-SnO2 catalyst calcined at 900 °C becomes 45 °C lower than for the Pd/CeO2 catalyst. It was found that calcination of the catalysts at T<600 °C leads to the formation of solid solutions based on the fluorite and rutile structures. As the calcination temperature is raised above 600 °C, the solid solutions decompose with formation of catalytically active PdxCe1-xO2-δdispersed phase on the surface of SnO2 nanoparticles. The formed nanoheterogeneous structure provides both high thermal stability and high water resistance of Pd/CeO2-SnO2 catalysts.
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