Browsing by Subject "Oxidation"

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  • Saarela, Taija; Rissanen, Antti J.; Ojala, Anne; Pumpanen, Jukka; Aalto, Sanni L.; Tiirola, Marja; Vesala, Timo; Jantti, Helena (2020)
    Freshwater ecosystems represent a significant natural source of methane (CH4). CH4 produced through anaerobic decomposition of organic matter (OM) in lake sediment and water column can be either oxidized to carbon dioxide (CO2) by methanotrophic microbes or emitted to the atmosphere. While the role of CH4 oxidation as a CH4 sink is widely accepted, neither the magnitude nor the drivers behind CH4 oxidation are well constrained. In this study, we aimed to gain more specific insight into CH4 oxidation in the water column of a seasonally stratified, typical boreal lake, particularly under hypoxic conditions. We used (CH4)-C-13 incubations to determine the active CH4 oxidation sites and the potential CH4 oxidation rates in the water column, and we measured environmental variables that could explain CH4 oxidation in the water column. During hypolimnetic hypoxia, 91% of available CH4 was oxidized in the active CH4 oxidation zone, where the potential CH4 oxidation rates gradually increased from the oxycline to the hypolimnion. Our results showed that in warm springs, which become more frequent, early thermal stratification with cold well-oxygenated hypolimnion delays the period of hypolimnetic hypoxia and limits CH4 production. Thus, the delayed development of hypolimnetic hypoxia may partially counteract the expected increase in the lacustrine CH4 emissions caused by the increasing organic carbon load from forested catchments.
  • Mäkelä, Noora; Maina, Ndegwa H.; Vikgren, Päivi; Sontag-Strohm, Tuula (2017)
    Viscosity of cereal beta-glucan during digestion is considered to be a vital factor for its health effects. Thus, studies on solution properties and gelation are essential for understanding the mechanisms of the beta-glucan functionality. The aim of this study was to investigate the effect of the dissolution temperature on gelation of cereal beta-glucan at low concentrations that are relevant for food products. The rheological properties of oat and barley beta-glucans (OBG and BBG) using three dissolution temperatures (37 degrees C, 57 degrees C and 85 degrees C) at low concentration (1.5% and 1%, respectively) were studied for 7 days. Additionally, the beta-glucans were oxidised with 70 mM H2O2 and 1 mM FeSO4 x 7H(2)O as a catalyst, to evaluate the consequence of oxidative degradation on the gelation properties. The study showed that dissolution at 85 degrees C did not result in gelation. The optimal dissolution temperature for gelation of OBG was 37 degrees C and for gelation of BBG 57 degrees C. At these temperatures, also the oxidised OBG and BBG gelled, although the gel strength was somewhat lower than in the non-oxidised ones. Gelation was suggested to require partial dissolution of beta-glucan, which depended on the molar mass and aggregation state of the beta-glucan molecule. Therefore, the state of beta-glucan in solution and its thermal treatment history may affect its technological and physiological functionality. (C) 2017 Elsevier Ltd. All rights reserved.
  • Zhu, Zhen; Sippola, Perttu; Ylivaara, Oili M E; Modanese, Chiara; Di Sabatino, Marisa; Mizohata, Kenichiro; Merdes, Saoussen; Lipsanen, Harri; Savin, Hele (Springer US, 2019)
    Abstract In this work, we report the successful growth of high-quality SiO2 films by low-temperature plasma-enhanced atomic layer deposition using an oxidant which is compatible with moisture/oxygen sensitive materials. The SiO2 films were grown at 90 °C using CO2 and Bis(tertiary-butylamino)silane as process precursors. Growth, chemical composition, density, optical properties, and residual stress of SiO2 films were investigated. SiO2 films having a saturated growth-per-cycle of ~ 1.15 Å/cycle showed a density of ~ 2.1 g/cm3, a refractive index of ~ 1.46 at a wavelength of 632 nm, and a low tensile residual stress of ~ 30 MPa. Furthermore, the films showed low impurity levels with bulk concentrations of ~ 2.4 and ~ 0.17 at. % for hydrogen and nitrogen, respectively, whereas the carbon content was found to be below the measurement limit of time-of-flight elastic recoil detection analysis. These results demonstrate that CO2 is a promising oxidizing precursor for moisture/oxygen sensitive materials related plasma-enhanced atomic layer deposition processes.
  • Mäkelä, Noora; Sontag-Strohm, Tuula; Schiehser, Sonja; Potthast, Antje; Maaheimo, Hannu; Maina, Ndegwa H. (2017)
    Oxidation of cereal beta-glucans may affect their stability in food products. Generally, polysaccharides oxidise via different pathways leading to chain cleavage or formation of oxidised groups within the polymer chain. In this study, oxidation pathways of oat and barley beta-glucans were assessed with different concentrations of hydrogen peroxide (H2O2) or ascorbic acid (Asc) with ferrous iron (Fe2+) as a catalyst. Degradation of beta-glucans was evaluated using high performance size exclusion chromatography and formation of carbonyl groups using carbazole-9-carbonyloxyamine labelling. Furthermore, oxidative degradation of glucosyl residues was studied. Based on the results, the oxidation with Asc mainly resulted in glycosidic bond cleavage. With H2O2, both glycosidic bond cleavage and formation of carbonyl groups within the beta-glucan chain was found. Moreover, H2O2 oxidation led to production of formic acid, which was proposed to result from Ruff degradation where oxidised glucose (gluconic acid) is decarboxylated to form arabinose. (C) 2016 Elsevier Ltd. All rights reserved.
  • Ahonen, Tiina J.; Rinne, Maiju; Grutschreiber, Peter; Mätlik, Kert; Airavaara, Mikko; Schaarschmidt, Dieter; Lang, Heinrich; Reiss, David; Xhaard, Henri; Gaveriaux-Ruff, Claire; Yli-Kauhaluoma, Jari; Moreira, Vania M. (2018)
    Despite extensive years of research, the direct oxidation of the 7,8-double bond of opioids has so far received little attention and knowledge about the effects of this modification on activity at the different opioid receptors is scarce. We herein report that potassium permanganate supported on iron(II) sulfate heptahydrate can be used as a convenient oxidant in the one-step, heterogeneous conversion of Delta(7.8)-opioids to the corresponding 7 beta-hydroxy-8-ketones. Details of the reaction mechanism are given and the effects of the substituent at position 6 of several opioids on the reaction outcome is discussed. The opioid hydroxy ketones prepared are antagonists at the mu- and delta-opioid receptors. Docking simulations and detailed structure-activity analysis revealed that the presence of the 7 beta-hydroxy-8-ketone functionality in the prepared compounds can be used to gain activity towards the delta opioid receptor. The 7 beta-hydroxy-8-ketones prepared with this method can also be regarded as versatile intermediates for the synthesis of other opioids of interest. (C) 2018 Elsevier Masson SAS. All rights reserved.
  • van Geenen, Fred A. M. G.; Franssen, Maurice C. R.; Miikkulainen, Ville; Ritala, Mikko; Zuilhof, Han; Kostiainen, Risto; Nielen, Michel W. F. (2019)
    In drug discovery, it is important to identify phase I metabolic modifications as early as possible to screen for inactivation of drugs and/or activation of prodrugs. As the major class of reactions in phase I metabolism is oxidation reactions, oxidation of drugs with TiO2 photocatalysis can be used as a simple non-biological method to initially eliminate (pro)drug candidates with an undesired phase I oxidation metabolism. Analysis of reaction products is commonly achieved with mass spectrometry coupled to chromatography. However, sample throughput can be substantially increased by eliminating pretreatment steps and exploiting the potential of ambient ionization mass spectrometry (MS). Furthermore, online monitoring of reactions in a time-resolved way would identify sequential modification steps. Here, we introduce a novel (time-resolved) TiO2-photocatalysis laser ablation electrospray ionization (LAESI) MS method for the analysis of drug candidates. This method was proven to be compatible with both TiO2-coated glass slides as well as solutions containing suspended TiO2 nanoparticles, and the results were in excellent agreement with studies on biological oxidation of verapamil, buspirone, testosterone, andarine, and ostarine. Finally, a time-resolved LAESI MS setup was developed and initial results for verapamil showed excellent analytical stability for online photocatalyzed oxidation reactions within the set-up up to at least 1h.
  • Calligaris, Sonia; Valoppi, Fabio; Barba, Luisa; Anese, Monica; Nicoli, Maria Cristina (2018)
    The aim of this research was to study beta-carotene degradation kinetics into lipid systems containing different fat crystal networks in the presence of increasing liquid oil amounts. To this purpose, fat blends containing liquid saturated medium chain triacylglycerols (MCT) with increasing content of saturated monoglycerides (MG), tripalmitin (PPP) and tristearin (SSS) were added with 0.6 mg/g beta-carotene. The fat crystal networks formed in the fat blends were characterized by using polarized light microscopy and synchrotron X-ray diffraction (XRD). In addition, A-carotene degradation was monitored during storage in the dark at 20 degrees C. Results highlighted that fat crystallization could differently affect beta-carotene stability. In bulk SSS and PPP, beta-carotene degradation proceeded at comparable rate, whereas when the saturated liquid oil MCT is included in the fat network, the rate of oxidation slightly decreased. Interestingly, the oxidation rate was not significantly affected by the solid/liquid ratio of the systems. A completely different behavior was observed in MG containing systems: the rate of beta-carotene oxidation was in every case significantly lower than that observed in SSS and PPP containing samples. Also in this case, the MG protective effect was independent on its content in the fat mixtures.