| 1. |
- Artemenko, A., et al.
(författare)
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Reference XPS spectra of amino acids
- 2021
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Konferensbidrag (refereegranskat)abstract
- In this report we present XPS data for five amino acids (AAs) (tryptophan, methionine, glutamine, glutamic acid, and arginine) with different side chain groups measured in solid state (powder form). The theoretically and experimentally obtained chemical structure of AAs are compared. Here, we analyse and discuss C 1 s, N 1 s, O 1s and S 2p core level binding energies, FWHMs, atomic concentrations of the functional groups in AAs. The experimentally obtained and theoretically calculated ratio of atomic concentrations are compared. The zwitterionic nature of methionine and glutamine in solid state was determined from protonated amino groups in N 1s peak and deprotonated carboxylic groups in the C 1s spectrum. The obtained XPS results for AAs well correspond with previously reported data.
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| 2. |
- Barišić, Antun, et al.
(författare)
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Experimental Data Contributing to the Elusive Surface Charge of Inert Materials in Contact with Aqueous Media
- 2021
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Ingår i: Colloids and interfaces. - : MDPI. - 2504-5377. ; 5:1
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Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
- We studied the charging of inert surfaces (polytetrafluoroethylene, i.e., PTFE; graphite; graphene; and hydrophobic silica) using classical colloid chemistry approaches. Potentiometric titrations showed that these surfaces acquired less charge from proton-related reactions than oxide minerals. The data from batch-type titrations for PTFE powder did not show an effect of ionic strength, which was also in contrast with results for classical colloids. In agreement with classical colloids, the electrokinetic results for inert surfaces showed the typical salt level dependence. In some cases, the point of zero net proton charge as determined from mass and tentatively from acid–base titration differed from isoelectric points, which has also been previously observed, for example by Chibowski and co-workers for ice electrolyte interfaces. Finally, we found no evidence for surface contaminations of our PTFE particles before and after immersion in aqueous solutions. Only in the presence of NaCl-containing solutions did cryo-XPS detect oxygen from water. We believe that our low isoelectric points for PTFE were not due to impurities. Moreover, the measured buffering at pH 3 could not be explained by sub-micromolar concentrations of contaminants. The most comprehensive explanation for the various sets of data is that hydroxide ion accumulation occurred at the interfaces between inert surfaces and aqueous solutions.
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| 3. |
- Bottone, Anna, et al.
(författare)
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Sodium hypochlorite as an oxidizing agent for removal of soil organic matter before microplastics analyses
- 2021
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Ingår i: Journal of Environmental Quality. - : John Wiley & Sons. - 0047-2425 .- 1537-2537. ; 51:1, s. 112-122
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Tidskriftsartikel (refereegranskat)abstract
- The omnipresence of microplastics (MPs) across Earth's surface has raised concerns about their environmental impact and created an urgent need for methods to identify them in complex soil and sedimentary matrices. However, detecting MPs in the O horizons of soils is difficult because plastic polymers share many physical and chemical properties with natural soil organic matter (SOM). In this study, we assessed whether sodium hypochlorite (NaOCl), a reagent that can oxidize SOM and simultaneously preserve mineral constituents, can be used for MP analysis and characterization in soil environments. In addition, we scrutinized how factors such as MP size, polymer type, extraction methods, and soil matrix affect the recovery of microplastic particles. We used both hydrophobic and density-dependent separation methods to assess the effects of our oxidation treatment on the recovery of MP. We observed that NaOCl effectively removed SOM without greatly altering the surface properties of resistant MP polymers (polypropylene, polylactic acid, low-density polyethylene, and polyethylene terephthalate), which were characterized using scanning electron microscopy and Fourier-transform infrared spectroscopy after SOM removal. The NaOCl treatment caused some chlorination and formation of additional C–OH bonds on polymer surfaces, which likely contributed to the reduced efficiency of the hydrophobic-based (oil) extraction. We conclude that NaOCl treatment can improve detection of MPs in SOM-rich soil and that recovery of MPs from soils is influenced by MP size, polymer type, extraction method, and soil type, which makes it challenging to develop a universal analytical method.
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| 4. |
- Cant, David J. H., et al.
(författare)
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Cryo-XPS for surface characterization of nanomedicines
- 2023
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 127:39, s. 8220-8227
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Tidskriftsartikel (refereegranskat)abstract
- Nanoparticles used for medical applications commonly possess coatings or surface functionalities intended to provide specific behavior in vivo, for example, the use of PEG to provide stealth properties. Direct, quantitative measurement of the surface chemistry and composition of such systems in a hydrated environment has thus far not been demonstrated, yet such measurements are of great importance for the development of nanomedicine systems. Here we demonstrate the first use of cryo-XPS for the measurement of two PEG-functionalized nanomedicines: a polymeric drug delivery system and a lipid nanoparticle mRNA carrier. The observed differences between cryo-XPS and standard XPS measurements indicate the potential of cryo-XPS for providing quantitative measurements of such nanoparticle systems in hydrated conditions.
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| 5. |
- Cheng, Wei, et al.
(författare)
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Nanoscale hydration in layered manganese oxides
- 2021
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Ingår i: Langmuir. - : American Chemical Society (ACS). - 0743-7463 .- 1520-5827. ; 37:2, s. 666-674
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Tidskriftsartikel (refereegranskat)abstract
- Birnessite is a layered MnO2 mineral capable of intercalating nanometric water films in its bulk. With its variable distributions of Mn oxidation states (MnIV, MnIII, and MnII), cationic vacancies, and interlayer cationic populations, birnessite plays key roles in catalysis, energy storage solutions, and environmental (geo)chemistry. We here report the molecular controls driving the nanoscale intercalation of water in potassium-exchanged birnessite nanoparticles. From microgravimetry, vibrational spectroscopy, and X-ray diffraction, we find that birnessite intercalates no more than one monolayer of water per interlayer when exposed to water vapor at 25 °C, even near the dew point. Molecular dynamics showed that a single monolayer is an energetically favorable hydration state that consists of 1.33 water molecules per unit cell. This monolayer is stabilized by concerted potassium–water and direct water–birnessite interactions, and involves negligible water–water interactions. Using our composite adsorption–condensation–intercalation model, we predicted humidity-dependent water loadings in terms of water intercalated in the internal and adsorbed at external basal faces, the proportions of which vary with particle size. The model also accounts for additional populations condensed on and between particles. By describing the nanoscale hydration of birnessite, our work secures a path for understanding the water-driven catalytic chemistry that this important layered manganese oxide mineral can host in natural and technological settings.
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| 6. |
- Gojkovic, Zivan, et al.
(författare)
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Cryogenic X-ray photoelectron spectroscopy determines surface composition of algal cells and gives insights into their spontaneous sedimentation
- 2020
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Ingår i: Algal Research. - : Elsevier. - 2211-9264. ; 47
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Tidskriftsartikel (refereegranskat)abstract
- The flotation properties of two green microalgal species isolated from Northern Sweden, Chlorella vulgaris 13-1 and Coelastrella sp. 3-4, were investigated. C. vulgaris 13-1 is a flotating alga that remains suspended in solution during culturing, while Coelastrella sp. 3-4 is readily sedimenting in the stationary growth phase. We were the first to use cryogenic X-ray photoelectron spectroscopy (Cryo-XPS) to gain information on the chemical composition of the algal cell surface and added to these data results obtained from diffuse reflectance - Fourier Transform infrared spectroscopy (DR-FTIR) and classical chemical extractions of carbohydrates, lipids and proteins. Based on the Cryo-XPS data the surface of the sedimenting Coelastrella sp. 3-4 strain is rich in proteins and lipids, while the cell surface of non-flocculating C. vulgaris 13-1 is predominated by carbohydrates, but is poor in lipids. The Zeta-potential of both strains was equally negative. Cell size and the amount of carbohydrates on the algal cell surface, but not the negative surface charge, therefore indicate colloidal stability of microalgae in solutions and can be applied to predict flotation properties of green microalgae.
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| 7. |
- Kumar Raul, Prasanta, et al.
(författare)
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Microwave assisted and in-situ generated palladium nanoparticles catalysed desulfitative synthesis of cross-biphenyls from arylsulfonyl chlorides and phenylboronic acids
- 2021
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Ingår i: Results in Chemistry. - : Elsevier. - 2211-7156. ; 3
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Tidskriftsartikel (refereegranskat)abstract
- A microwave assisted reaction protocol for Suzuki–Miyaura cross-coupling has been developed. Substituted arylboronic acids and arylsulfonyl chlorides coupled under microwave irradiation (MWI) to produce cross-biphenyls in high yields under aerobic condition. The principal advantage of this protocol is that formation of cross-biphenyls was achieved within shorter time along with desulfurization of arylsulfonyl chloride. In-situ generated Pd nanoparticles (NPs) act as catalyst in the reaction. Substituents like methyl, halogens, cyano, amino and t-butyl groups in arylboronic acids tolerate the reaction condition. Pd NPs could be reused several times under chosen reaction conditions without losing its activity significantly. The product formation and the role of the catalyst for the cross-coupling reaction has been rationalised with the help of a proposed mechanism. This reaction is one of the examples of In-situ generated Nanoparticles-catalyzed Organic Synthesis Enhancement (i-NOSE) approach. The approach derives its importance in terms of catalyst’s (i) simple preparation method, (ii) stability under the chosen reaction condition, (iii) substrate specificity, (iv) simple filtration to recover the catalyst and (v) easy regeneracy which clearly indicate that the approach could be applicable for various types of catalytic transformations.
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| 8. |
- Luong, N. Tan, et al.
(författare)
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Water film-driven Mn (oxy)(hydr)oxide nanocoating growth on rhodochrosite
- 2022
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Ingår i: Geochimica et Cosmochimica Acta. - : Elsevier. - 0016-7037 .- 1872-9533. ; 329, s. 87-105
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Tidskriftsartikel (refereegranskat)abstract
- Minerals exposed to moist air stabilize thin water films that drive a score of chemical reactions of great importance to water-unsaturated terrestrial environments. In this study, we identified Mn (oxy)(hydr)oxide nanocoatings formed by the dissolution, oxidation and precipitation of Mn in oxygenated water films grown on rhodochrosite (MnCO3) microparticles. Nanocoatings that could be identified by vibrational spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and (scanning and transmission) electron microscopy formed in water films containing the equivalent of at least 7 monolayers (∼84 H2O/nm2). These films were formed by exposing microparticles to moist air with at least 50% relative humidity (RH). Films of neutral pH reacted up to 14% of the MnII located in the topmost ∼5 nm region of the microparticles in atmospheres of up to 90% RH for 7 d. These reactions produced MnOOH, birnessite (MnO2) and hausmannite (Mn3O4) nanoparticles of low crystallinity, while exposure to atmospheric air for 1 yr. converted only 2% of MnII in this region to MnOOH. In contrast, reactions in alkaline water films converted up to ∼75% of the MnII but only after 16 d of reaction. These films produced MnOOH and MnO2 of low crystallinity, as well as crystalline hausmannite. Kinetic modeling of the time-resolved growth of the Mn[sbnd]O stretching vibrational bands of these nanocoatings revealed two concurrent reaction processes. A 1rst-order process was assigned to nucleation events terminating only after a few hours, and a 0-order process was assigned to the sustained growth of nanocoatings from these nuclei over longer reaction time. By identifying nanocoatings formed by water film-driven reactions on rhodochrosite, our study adds new insight into mineralogical transformations relevant to anoxic–oxic boundaries in water-unsaturated environments.
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| 9. |
- Martínez-Klimov, Mark E., et al.
(författare)
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Hydrodeoxygenation of Isoeugenol over Carbon-Supported Pt and Pt-Re Catalysts for Production of Renewable Jet Fuel
- 2021
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Ingår i: Energy & Fuels. - : American Chemical Society (ACS). - 0887-0624 .- 1520-5029. ; 35:21, s. 17755-17768
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Tidskriftsartikel (refereegranskat)abstract
- A series of monometallic platinum and bimetallic platinum–rhenium catalysts supported on mesoporous carbon Sibunit, which is a type of mesoporous, microcrystalline carbon, were investigated for hydrodeoxygenation (HDO) of isoeugenol (IE) at 200–300 °C and 30 bar of H2, using dodecane as a solvent. Catalytic activity was tested in a batch reactor to screen the catalysts and, for comparison, also in the continuous mode. For batch experiments, complete conversion, and a high yield of the desired product, propylcyclohexane (PCH), were obtained for all bimetallic PtRe/Sibunit in 240 min, with the highest yield of PCH when Pt:Re ratio was 1:1 or 1:3. The results for Pt–Re (1:1) were reproducible, in terms of catalytic activity and reusability of catalysts, which showed no deactivation. Monometallic Pt catalysts displayed low activity. Continuous experiments were performed with PtRe(1:1)/Sibunit at 30 bar H2, 0.5 mL/min of the liquid flow, and temperatures between 75 °C and 200 °C. The distribution of products showed deoxygenation at higher temperatures, while at lower temperatures, mainly oxygenated products were formed. XPS results confirmed the presence of ReOx species, where an increase in the platinum loading resulted in a decrease in the fraction of ReOx species and subsequently lower PCH yield.
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| 10. |
- Phal, Sereilakhena, et al.
(författare)
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Electrografting of 4-Carboxybenzenediazonium on Glassy Carbon Electrode : The Effect of Concentration on the Formation of Mono and Multilayers
- 2020
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Ingår i: Molecules. - Basel : MDPI. - 1431-5157 .- 1420-3049. ; 25:19
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Tidskriftsartikel (refereegranskat)abstract
- Grafting of electrodes with diazonium salts using cyclic voltammetry (CV) is a well-established procedure for surface modification. However, little is known about the effect of the concentration of the diazonium salt on the number of layers grafted on the electrode surface. In this work, the impact of concentration on the grafting of 4-carboxybenzenediazonium (4-CBD) onto a glassy carbon electrode (GCE) is elucidated. The number of layers grafted on the GCE was linearly dependent on the concentration of 4-CBD and varied between 0.9 and 4.3 when the concentration was varied between 0.050 and 0.30 mmol/L at 0.10 V.s−1. Characterization of modified glassy carbon surface with X-ray photoelectron spectroscopy (XPS) confirmed the grafting of carboxyphenyl layer on the surface. Grafting with 0.15 mmol/L 4-CBD (1 CV cycle) did not form a detectable amount of carboxyphenyl (CP) moieties at the surface, while a single scan with higher concentration (2.5 mmol/L) or multiple scans (22 cycles) gave detectable signals, indicating formation of multilayers. We also demonstrate the possibility of removing the thin layer grafted on a glassy carbon electrode by applying high oxidation potential +1.40 V.
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| 11. |
- Ramstedt, Madeleine, et al.
(författare)
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Cryo-XPS spectra from bacterial reference strain Pseudomonas fluorescens DSM50090
- 2022
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Ingår i: Surface Science Spectra. - : AVS Science and Technology Society. - 1055-5269 .- 1520-8575. ; 29:1
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Tidskriftsartikel (refereegranskat)abstract
- Cryogenic x-ray photoelectron spectroscopy was used to analyze the cell envelope of intact and hydrated Gram-negative bacteria of the species Pseudomonas fluorescens. We used a reference strain, DSM50090, from the German microbial culture collection, which we previously have suggested would function well as a reference strain for future XPS analyses of Gram-negative bacteria. Bacteria were grown on nutrient agar plates at room temperature, collected with a cultivation loop, and washed using phosphate buffered saline. An aliquot of the cell pellet was fast-frozen on the sample holder in the sample introduction chamber to a temperature of 103 K and kept frozen throughout the measurement. Survey spectra and high-resolution spectra of Na 1s, O 1s, N 1s, C 1s, Cl 2p, S 2p, and P 2p are reported. The spectra obtained from the analyzed cells represent a combined signal from O, N, C, and S atoms in proteins, lipids, and polysaccharides at the cell surface. Furthermore, signal from P, Na, K, and Cl atoms was present both originating from processes in the cell envelope and remnants from the wash buffer.
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| 12. |
- Ramstedt, Madeleine, et al.
(författare)
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XPS spectra from nucleobases, DNA, and RNA
- 2023
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Ingår i: Surface Science Spectra. - : American Institute of Physics (AIP). - 1055-5269 .- 1520-8575. ; 30:1
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Tidskriftsartikel (refereegranskat)abstract
- X-ray photoelectron spectroscopy was used to analyze commercially available powders of thymine, uracil, cytosine, guanine, adenine, as well as DNA isolated from salmon testes and RNA from torula yeast. The powders were pressed onto a sample holder and analyzed as received from the manufacturer. Survey spectra and high-resolution spectra of O 1s, N 1s, C 1s of all nucleobases are reported, including a small Na 1s contamination in cytosine. Spectra of DNA and RNA are also included for comparison. Furthermore, the presented data are compared with previously published results, as well as theoretical values, and differences are discussed.
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| 13. |
- Saeid, Soudabeh, et al.
(författare)
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Advanced Oxidation Process for Degradation of Carbamazepine from Aqueous Solution : Influence of Metal Modified Microporous, Mesoporous Catalysts on the Ozonation Process
- 2020
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Ingår i: Catalysts. - : MDPI. - 2073-4344. ; 10:1
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Tidskriftsartikel (refereegranskat)abstract
- Carbamazepine (CBZ), a widely used pharmaceutical compound, is one of the most detected drugs in surface waters. The purpose of this work was to identify an active and durable catalyst, which, in combination with an ozonation process, could be used to remove CBZ and its degradation products. It was found that the CBZ was completely transformed after ozonation within the first minutes of the treatment. However, the resulting degradation products, 1-(2-benzaldehyde)-4-hydro-(1H,3H)-quinazoline-2-one (BQM) and 1-(2-benzaldehyde)-(1H,3H)-quinazoline-2,4-dione (BQD), were more resistant during the ozonation process. The formation and degradation of these products were studied in more detail and a thorough catalytic screening was conducted to reveal the reaction kinetics of both the CBZ and its degradation products. The work was performed by non-catalytic ozonation and with six different heterogeneous catalysts (Pt-MCM-41-IS, Ru-MCM-41-IS, Pd-H-Y-12-EIM, Pt-H-Y-12-EIM, Pd-H-Beta-300-EIM and Cu-MCM-41-A-EIM) operating at two temperatures 20 °C and 50 °C. The influence of temperature on degradation kinetics of CBZ, BQM and BQD was studied. The results exhibited a notable difference in the catalytic behavior by varying temperature. The higher reactor temperature (50 °C) showed a higher activity of the catalysts but a lower concentration of dissolved ozone. Most of the catalysts exhibited higher removal rate for BQM and BQD compared to non-catalytic experiments in both temperatures. The Pd-H-Y-12-EIM catalyst illustrated a higher degradation rate of by-products at 50 °C compared to other catalysts.
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| 14. |
- Saeid, Soudabeh, et al.
(författare)
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Pt Modified Heterogeneous Catalysts Combined with Ozonation for the Removal of Diclofenac from Aqueous Solutions and the Fate of by-Products
- 2020
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Ingår i: Catalysts. - : MDPI. - 2073-4344. ; 10:3
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Tidskriftsartikel (refereegranskat)abstract
- The degradation of the pharmaceutical compound diclofenac in an aqueous solution was studied with an advanced oxidation method, catalytic ozonation. Diclofenac was destroyed in a few minutes by ozonation but several long-lasting degradation by-products were formed. For this reason, the combination of heterogeneous catalysts and ozonation was applied to eliminate them completely. The kinetics of the diclofenac degradation and the formation of by-products were thoroughly investigated. Loading of Pt on the catalysts resulted in an improvement of the activity. The Mesoporous Molecular Sieves (MCM) were one of the promising catalysts for the degradation of organic pollutants. In this study, six heterogeneous catalysts were screened, primarily MCM-22-100 catalysts with different Pt concentrations loaded via the evaporation-impregnation (EIM) method, and they were applied on the degradation of diclofenac. It was found that the presence of Pt improved the degradation of diclofenac and gave lower concentrations of by-products. The 2 wt % Pt-H-MCM-22-100-EIM demonstrated the highest degradation rate compared to the proton form, 1% or 5 wt % Pt concentration, i.e., an optimum was found in between. Pt-H-Y-12-IE and Pt-γ-Al2O3 (UOP)-IMP catalysts were applied and compared with the MCM-22 structure. Upon use of both of these catalysts, an improvement in the degradation of diclofenac and by-products was observed, and the 2 wt % Pt-H-MCM-22-100-EIM illustrated the maximum activity. All important characterization methods were applied to understand the behavior of the catalysts (X-ray powder diffraction, transmission electron microscopy, nitrogen physisorption, scanning electron microscopy, energy dispersive X-ray micro-analyses, pyridine adsorption-desorption with FTIR spectroscopy, X-ray photoelectron spectroscopy). Finally, leaching of Pt and Al were analyzed by inductively coupled optical emission spectrometry.
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| 15. |
- Samikannu, Ajaikumar, et al.
(författare)
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Highly dispersed NbOPO4/SBA-15 as a versatile acid catalyst upon production of renewable jet-fuel from bio-based furanics via hydroxyalkylation-alkylation (HAA) and hydrodeoxygenation (HDO) reactions
- 2020
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Ingår i: Applied Catalysis B. - : Elsevier. - 0926-3373 .- 1873-3883. ; 272
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Tidskriftsartikel (refereegranskat)abstract
- Herein, we report the synthesis of a highly active and mesoporous Brønsted acidic NbOPO4/SBA-15 catalyst. The prepared catalysts were thoroughly characterized by means of analytical techniques such as XRD, FT-IR, XPS, NH3-TPD, SEM-EDS, TEM, TGA, 31P-MAS-NMR and N2-physisorption. The H3PO4 free deposition method was found to be effective for preserving the structure of Silica based carrier. In terms of catalytic performance, these materials demonstrated high activity upon C-C coupling of 2-methyl furan with carbonyl compounds and outperforming bulk NbOPO4, Nb2O5/SBA-15 and traditional solid acid catalysts (Al-MCM-41, Si/Al and H-ZSM-5). The NbOPO4/SBA-15 catalysts were stable and maintained high activity upon reuse and continuous operation (∼65 h). Furthermore, the Pd loaded counterparts (Pd/NbOPO4/SBA-15 and Pd/Nb2O5/SBA-15) also functioned as bifunctional catalysts and exhibited excellent activity upon subsequent hydrodeoxygenation of C-C coupling products. Most importantly, in terms of jet-fuel range hydrocarbons selectivity, these catalysts outperformed monofunctional Pd/carbon and aluminosilicate based bifunctional catalysts.
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| 16. |
- Shchukarev, Andrey, et al.
(författare)
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Applying Cryo-X-ray Photoelectron Spectroscopy to Study the Surface Chemical Composition of Fungi and Viruses
- 2021
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Ingår i: Frontiers in Chemistry. - : Frontiers Media S.A.. - 2296-2646. ; 9
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Tidskriftsartikel (refereegranskat)abstract
- Interaction between microorganisms and their surroundings are generally mediated via the cell wall or cell envelope. An understanding of the overall chemical composition of these surface layers may give clues on how these interactions occur and suggest mechanisms to manipulate them. This knowledge is key, for instance, in research aiming to reduce colonization of medical devices and device-related infections from different types of microorganisms. In this context, X-ray photoelectron spectroscopy (XPS) is a powerful technique as its analysis depth below 10Â nm enables studies of the outermost surface structures of microorganism. Of specific interest for the study of biological systems is cryogenic XPS (cryo-XPS). This technique allows studies of intact fast-frozen hydrated samples without the need for pre-treatment procedures that may cause the cell structure to collapse or change due to the loss of water. Previously, cryo-XPS has been applied to study bacterial and algal surfaces with respect to their composition of lipids, polysaccharides and peptide (protein and/or peptidoglycan). This contribution focuses onto two other groups of microorganisms with widely different architecture and modes of life, namely fungi and viruses. It evaluates to what extent existing models for data treatment of XPS spectra can be applied to understand the chemical composition of their very different surface layers. XPS data from model organisms as well as reference substances representing specific building blocks of their surface were collected and are presented. These results aims to guide future analysis of the surface chemical composition of biological systems.
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| 17. |
- Shchukarev, Andrey, et al.
(författare)
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Cryo-XPS analysis reveals surface composition of microalgae
- 2020
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Ingår i: Applied Surface Science. - : Elsevier. - 0169-4332 .- 1873-5584. ; 526
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Tidskriftsartikel (refereegranskat)abstract
- Green microalgae are widely used for wastewater treatment, food/feed and pigment production, as well as for aquaculture. However, very little is known about their surface composition, which can determine algae behavior in nature and influence their processing. In this work, we use cryo-XPS to characterize the surface chemical composition of three different microalgae species. We investigate the applicability of a data treatment method, developed for bacteria, deconvoluting C 1s with respect to protein, lipid and polysaccharide. We discuss how substances unique to algae contribute to the C 1s spectra and how this affects the transferability of the method to microalgae. Two species of green microalgae isolated from Northern Sweden, Chlorella vulgaris 13-1 and Coelastrella sp. 3-4, were compared to reference culture collection strain, Scenedesmus obliquus RISE (UTEX 417). Cryo-XPS data indicate that surfaces of Coelastrella sp. 3-4 and C. vulgaris 13-1 cells are dominated by protein and carbohydrates. However, the carbohydrate content was higher for C. vulgaris. The reference strain shows the highest content of proteins and has an increased amount of lipids compared to the other two. Estimation of the cell surface hydrophobicity suggests that the hydrophobicity increases in the order: C. vulgaris < Coelastrella sp. < S. obliquus.
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| 18. |
- Škvarla, Jiří, et al.
(författare)
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Cryo-XPS : A new technique for the quantitative analysis of the structure of electric double layer at colloidal particles?
- 2020
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Ingår i: Colloids and Surfaces A. - : Elsevier. - 0927-7757 .- 1873-4359. ; 586
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Tidskriftsartikel (refereegranskat)abstract
- There is a long-lasting uncertainty as to the structure of the metal oxide/water interface. Various structures have especially been invoked to rationalize the seemingly anomalous silica/water interface. But, none of them seems to be approved in a quantitative and systematic way. We show that the concentration ratio of monovalent counterions and coions around colloidal silica spheres, as detected by the cryo-XPS technique, follows fundamental theoretical predictions of either Boltzmann or Donnan distribution. It is suggested that the reason of the dual response is the formation of the swelling gel layer on the silica surface due to its longer contact with water.
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| 19. |
- Slavinskaya, E. M., et al.
(författare)
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Thermal activation of Pd/CeO2-SnO2 catalysts for low-temperature CO oxidation
- 2020
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Ingår i: Applied Catalysis B. - : Elsevier. - 0926-3373 .- 1873-3883. ; 277
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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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| 20. |
- Vucetic, Nemanja, et al.
(författare)
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Competing commercial catalysts: Unprecedented catalyst activity and stability of Mizoroki-Heck reaction in a continuous packed bed reactor
- 2022
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Ingår i: Chemical Engineering Journal. - : Elsevier. - 1385-8947 .- 1873-3212. ; 433
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Tidskriftsartikel (refereegranskat)abstract
- Main obstacle for adopting continuous processes as a standard technology for Mizoroki-Heck reaction usually lies in its specific reaction mechanism. Here we present an important step forward answering the challenges unraveled through a comprehensive study that provides deeper understanding on the Mizoroki-Heck reaction, in particular the case when iodobenzene and butyl acrylate react in a continuous packed bed reactor in the presence of a Pd Supported Ionic Liquid Catalyst (SILCA). On-line UV–VIS spectrometry supported by ICP-OES, TEM and XPS measurements were carried out and the catalyst leaching was minimized. Finally, simple continuous flow process was proposed resulting in a high catalytic activity (up to 1470 molArI molPd−1h−1) and reaching productivity in the range of 12,000 to 16,000 molArI molPd−1 thus competing with the performance of commercial catalysts.
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| 21. |
- Vucetic, Nemanja, et al.
(författare)
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Tuned Bis-Layered Supported Ionic Liquid Catalyst (SILCA) for Competitive Activity in the Heck Reaction of Iodobenzene and Butyl Acrylate
- 2020
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Ingår i: Catalysts. - : MDPI. - 2073-4344. ; 10:9
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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.
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| 22. |
- Yu, Changxun, 1983-, et al.
(författare)
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Manganese cycling and transport in boreal estuaries impacted by acidic Mn-rich drainage
- 2024
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Ingår i: GEOCHIMICA ET COSMOCHIMICA ACTA. - : Elsevier. - 0016-7037 .- 1872-9533 .- 0046-564X. ; 365, s. 136-157
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Tidskriftsartikel (refereegranskat)abstract
- As critical transition zones between the land and the sea, estuaries are not only hotspots of hydrogeochemical and microbial processes/reactions, but also play a vital role in processing and transferring terrestrial fluxes of metals and nutrients to the sea. This study focused on three estuaries in the Gulf of Bothnia. All of them expe-rience frequent inputs of acidic and Mn/metal-rich creek waters due to flushing of acid sulfate soils that are widespread in the creeks catchments. Analyzing existing long-term water chemistry data revealed a strong sea-sonal variation of Mn loads, with the highest values in spring (after snow melt) and autumn (after heavy rains). We sampled surface waters, suspended particulate matter (SPM), and sediments from the estuarine mixing zones and determined the loads and solid-phase speciation of Mn as well as the composition and metabolic potentials of microbial communities. The results showed that the removal, cycling, and lateral transport of Mn were governed by similar phases and processes in the three estuaries. Manganese X-ray absorption spectroscopy data of the SPM suggested that the removal of Mn was regulated by silicates (e.g., biotite), organically complexed Mn(II), and MnOx (dominated by groutite and phyllomanganates). While the fractional amounts of silicate-bound Mn(II) were overall low and constant throughout the estuaries, MnOx was strongly correlated with the Mn loadings of the SPM and thus the main vector for the removal of Mn in the central and outer parts of the estuaries, along with organically complexed Mn(II). Down estuary, both the fractional amounts and average Mn oxidation state of the MnOx phases increased with (i) the total Mn loads on the SPM samples and (ii) the relative abundances of several potential Mn-oxidizing bacteria (Flavobacterium, Caulobacter, Mycobacterium, and Pedobacter) in the surface waters. These features collectively suggested that the oxidation of Mn, probably mediated by the potential Mn-oxidizing microorganisms, became more extensive and complete towards the central and outer parts of the es-tuaries. At two sites in the central parts of one estuary, abundant phyllomanganates occurred in the surface sediments, but were converted to surface-sorbed Mn(II) phases at deeper layers (>3-4 cm). The occurrence of phyllomanganates may have suppressed the reduction of sulfate in the surface sediments, pushing down the methane sulfate transition zone that is typically shallow in estuarine sediments. At the outermost site in the estuary, deposited MnOx were reduced immediately at the water-sediment interface and converted most likely to Mn carbonate. The mobile Mn species produced by the Mn reduction processes (e.g., aqueous Mn(II) and ligand complexed Mn(III)) could partly diffuse into the overlying waters and, together with the estuarine Mn loads carried by the surface waters, transfer large amounts of reactive Mn into open coastal areas and subsequently contribute to Mn shuttling and inter-linked biogeochemical processes over the seafloor. Given the widespread occurrence of acid sulfate soils and other sulfidic geological materials on many coastal plains worldwide, the identified Mn attenuation and transport mechanisms are relevant for many estuaries globally.
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| 23. |
- Yun, Jingwei, et al.
(författare)
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Effects of Inorganic Acids and Organic Solutes on the Ice Nucleating Ability and Surface Properties of Potassium-Rich Feldspar
- 2021
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Ingår i: ACS Earth and Space Chemistry. - : American Chemical Society (ACS). - 2472-3452. ; 5:5, s. 1212-1222
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Tidskriftsartikel (refereegranskat)abstract
- Mineral dust particles can initiate the freezing of cloud droplets in the atmosphere. The freezing efficiency of these particles can, however, be strongly affected by solutes, such as inorganic acids, polyols, and carboxylic acids. Here, we report the effects of inorganic acids (HNO3 and HCl), polyols, and carboxylic acids at low concentrations on the ice nucleating ability of potassium-rich feldspar (K-rich feldspar) using the droplet freezing technique. The inorganic acids and carboxylic acids decreased the median freezing temperature of droplets containing K-rich feldspar by up to 7 °C, while the polyols had no significant effect on the median freezing temperature. For the inorganic acids and carboxylic acids, the median freezing temperature was a strong function of the pH of the droplets, with the median freezing temperature decreasing as the pH decreased. By examining the surface properties of K-rich feldspar exposed to different concentrations of HCl with cryogenic X-ray photoelectron spectroscopy, we show that the decrease in the ice nucleating ability of K-rich feldspar by the inorganic acids and carboxylic acids was likely caused by ion exchange (H3O+ with parent K+ in microcline) and the incongruent dissolution of Al with respect to Si at K-rich feldspar surfaces. The decrease in the ice nucleating ability of K-rich feldspar by the carboxylic acids only related to the pH of the droplets rather than the type of carboxylic acid and their expected binding mechanisms on K-rich feldspar. This study focuses on rare ice nucleating active sites (with an ice nucleating active site density of 10-600 cm-2) of the K-rich feldspar and short exposure times between the solutes and the K-rich feldspar. Further studies are needed to investigate more abundant ice nucleating active sites and longer exposure times, as well as K-rich feldspar samples from different sources.
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| 24. |
- Yun, Jingwei, et al.
(författare)
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Surface Composition Dependence on the Ice Nucleating Ability of Potassium-Rich Feldspar
- 2020
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Ingår i: ACS Earth and Space Chemistry. - : American Chemical Society (ACS). - 2472-3452. ; 4:6, s. 873-881
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Tidskriftsartikel (refereegranskat)abstract
- Mineral dust particles are one of the most abundant types of ice nucleating particles in the atmosphere. During atmospheric transport, these particles can be coated with water-soluble solutes, which can modify their ice nucleating ability. Although previous studies have shown that even low concentrations of water-soluble solutes can modify the ice nucleating properties of mineral dust particles, our understanding of this topic is far from complete. We examined the effects of a series of alkali metal nitrates at low concentrations (5 × 10–5 M to 5 × 10–3 M) on the surface composition and immersion freezing of potassium-rich feldspar (K-rich feldspar). Immersion freezing was investigated with the droplet freezing technique, and the surface composition was investigated with cryogenic X-ray photoelectron spectroscopy. K+ increased the median freezing temperature of the droplets, while the other alkali metal cations either had no effect or decreased the median freezing temperature. The changes in the median freezing temperature of the droplets due to the presence of nitrates followed the order K+ ≥ Li+ ≥ Na+ ≥ Rb+ ≥ Cs+ and, except for Cs+, were correlated to the K/Al ratio at the surface of K-rich feldspar. The K/Al ratio is possibly an indicator of the abundance of certain types of K-bearing microcline surfaces that drive the immersion freezing of K-rich feldspar, while Cs+ likely influences the immersion freezing of K-rich feldspar by an additional mechanism, possibly blocking ice nucleation sites by adsorption. Our work also shows that the cation charge density (charge density over the surface area of a single cation) is not a good predictor of the effects of cations on the immersion freezing of K-rich feldspar in our experiments.
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