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  • 1. Abdala, Paula M
    et al.
    Safonova, Olga V
    Wiker, Geir
    van Beek, Wouter
    Emerich, Herman
    van Bokhoven, Jeroen A
    Sá, Jacinto
    Szlachetko, Jakub
    Nachtegaal, Maarten
    Scientific opportunities for heterogeneous catalysis research at the SuperXAS and SNBL beam lines.2012In: Chimia (Basel), ISSN 0009-4293, Vol. 66, no 9, p. 699-705Article in journal (Refereed)
    Abstract [en]

    In this short review, we describe the complementary experimental capabilities for catalysis research at two beam lines available to the Swiss community, SuperXAS at SLS (Swiss Light Source, Villigen) and SNBL (Swiss Norwegian Beam lines) at ESRF (European Synchrotron Radiation Facility, Grenoble). Over the years, these two facilities have been developed to provide powerful techniques for structural studies under in situ and operando conditions. These techniques, X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and X-ray emission spectroscopy (XES) in combination with Raman or infrared spectroscopy provide new avenues for structure-performance studies of catalysts. Several exemplary studies are used to demonstrate the capability of these facilities.

  • 2.
    Antila, Liisa J.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Santomauro, Fabio G.
    Hammarström, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Fernandes, Daniel L. A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sa, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Hunting for the elusive shallow traps in TiO2 anatase2015In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 51, no 54, p. 10914-10916Article in journal (Refereed)
    Abstract [en]

    Understanding electron mobility on TiO2 is crucial because of its applications in photocatalysis and solar cells. This work shows that shallow traps believed to be involved in electron migration in TiO2 conduction band are formed upon band gap excitation, i.e., are not pre-existing states. The shallow traps in TiO2 results from large polarons and are not restricted to surface.

  • 3. Barrabes, Noelia
    et al.
    Foettinger, Karin
    Llorca, Jordi
    Dalinov, Anton
    Medina, Francesc
    Sa, Jacinto
    Hardacre, Christopher
    Rupprechter, Guenther
    Pretreatment Effect on Pt/CeO2 Catalyst in the Selective Hydrodechlorination of Trichloroethylene2010In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 114, no 41, p. 17675-17682Article in journal (Refereed)
  • 4. Barrabes, Noelia
    et al.
    Sa, Jacinto
    Catalytic nitrate removal from water, past, present and future perspectives2011In: Applied Catalysis B: Environmental, ISSN 0926-3373, E-ISSN 1873-3883, Vol. 104, no 1-2, p. 1-5Article in journal (Refereed)
  • 5. Berger, Gilles
    et al.
    Fusaro, Luca
    Luhmer, Michel
    Czapla-Masztafiak, Joanna
    Lipiec, Ewelina
    Szlachetko, Jakub
    Kayser, Yves
    Fernandes, Daniel L. A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sa, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Dufrasne, Francois
    Bombard, Sophie
    Insights into the structure-activity relationships of chiral 1,2-diaminophenylalkane platinum(II) anticancer derivatives2015In: Journal of Biological Inorganic Chemistry, ISSN 0949-8257, E-ISSN 1432-1327, Vol. 20, no 5, p. 841-853Article in journal (Refereed)
    Abstract [en]

    The structure-activity relationships of chiral 1,2-diaminophenylalkane platinum(II) anticancer derivatives are studied, including interactions with telomeric- and genomic-like DNA sequences, the pKa of their diaqua species, structural properties obtained from DFT calculations and resonant X-ray emission spectroscopy. The binding modes of the compounds to telomeric sequences were elucidated, showing no major differences with conventional cis-platinum(II) complexes like cisplatin, supporting that the cis-square planar geometry governs the binding of small Pt(II) complexes to G4 structures. Double-stranded DNA platination kinetics and acid-base constants of the diaqua species of the compounds were measured and compared, highlighting a strong steric dependence of the DNA-binding kinetics, but independent to stereoisomerism. Structural features of the compounds are discussed on the basis of dispersion-corrected DFT, showing that the most active series presents conformers for which the platinum atom is well devoid of steric hindrance. If reactivity indices derived from conceptual DFT do not show evidences for different reactivity between the compounds, RXES experiments provide new insight into the availability of platinum orbitals for binding to nucleophiles.

  • 6.
    Bhunia, Asamanjoy
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. Natl Inst Technol Puducherry, Dept Chem, Karaikal 609609, India.
    Johnson, Ben A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Czapla-Masztafiak, Joanna
    Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Ott, Sascha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Formal water oxidation turnover frequencies from MIL-101(Cr) anchored Ru(bda) depend on oxidant concentration2018In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 54, p. 7770-7773Article in journal (Refereed)
    Abstract [en]

    The molecular water oxidation catalyst [Ru(bda)(L)(2)] has been incorporated into pyridine-decorated MIL-101(Cr) metal-organic frameworks. The resulting MIL-101@Ru materials exhibit turnover frequencies (TOFs) up to ten times higher compared to the homogenous reference. An unusual dependence of the formal TOFs on oxidant concentration is observed that ultimately arises from differing amounts of catalysts in the MOF crystals being active.

  • 7.
    Blachucki, W.
    et al.
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Kayser, Y.
    Phys Tech Bundesanstalt, D-10587 Berlin, Germany.
    Czapla-Masztafiak, J.
    Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland.
    Guo, Meiyuan
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Theoretical Chemistry.
    Juranic, P.
    Paul Scherrer Inst, CH-5232 Villigen, Switzerland.
    Kavcic, M.
    Jozef Stefan Inst, SI-1000 Ljubljana, Slovenia.
    Källman, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Theoretical Chemistry.
    Knopp, G.
    Paul Scherrer Inst, CH-5232 Villigen, Switzerland.
    Lundberg, Marcus
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Theoretical Chemistry.
    Milne, C.
    Paul Scherrer Inst, CH-5232 Villigen, Switzerland.
    Rehanek, J.
    Paul Scherrer Inst, CH-5232 Villigen, Switzerland.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Szlachetko, J.
    Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland.
    Inception of electronic damage of matter by photon-driven post-ionization mechanisms2019In: Structural Dynamics, ISSN 2329-7778, Vol. 6, no 2, article id 024901Article in journal (Refereed)
    Abstract [en]

    "Probe-before-destroy" methodology permitted diffraction and imaging measurements of intact specimens using ultrabright but highly destructive X-ray free-electron laser (XFEL) pulses. The methodology takes advantage of XFEL pulses ultrashort duration to outrun the destructive nature of the X-rays. Atomic movement, generally on the order of >50 fs, regulates the maximum pulse duration for intact specimen measurements. In this contribution, we report the electronic structure damage of a molecule with ultrashort X-ray pulses under preservation of the atoms' positions. A detailed investigation of the X-ray induced processes revealed that X-ray absorption events in the solvent produce a significant number of solvated electrons within attosecond and femtosecond timescales that are capable of coulombic interactions with the probed molecules. The presented findings show a strong influence on the experimental spectra coming from ionization of the probed atoms' surroundings leading to electronic structure modification much faster than direct absorption of photons. This work calls for consideration of this phenomenon in cases focused on samples embedded in, e.g., solutions or in matrices, which in fact concerns most of the experimental studies.

  • 8.
    Blachucki, Wojciech
    et al.
    Polish Acad Sci, Inst Phys Chem, 44-52 Kasprzaka St, PL-01224 Warsaw, Poland.
    Czapla-Masztafiak, Joanna
    Polish Acad Sci, Inst Nucl Phys, 152 Radzikowskiego St, PL-31342 Krakow, Poland.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, 44-52 Kasprzaka St, PL-01224 Warsaw, Poland.
    Szlachetko, Jakub
    Polish Acad Sci, Inst Nucl Phys, 152 Radzikowskiego St, PL-31342 Krakow, Poland.
    A laboratory-based double X-ray spectrometer for simultaneous X-ray emission and X-ray absorption studies2019In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 34, no 7, p. 1409-1415Article in journal (Refereed)
    Abstract [en]

    X-ray spectroscopy studies are usually performed using synchrotron radiation sources, which offer bright, coherent, energy-tuneable and monochromatic light. However, the application of synchrotron-based Xray emission spectroscopy (XES) and X-ray absorption spectroscopy (XAS) is directly constrained by the limited, infrequent access to central facilities. With the advent of new technological solutions in the field of X-ray sources, optics and detectors, the development of efficient and compact laboratory X-ray spectroscopy systems is possible. A permanent laboratory-based setup offers the advantages of low cost and easy accessibility and, therefore, more flexibility in the preparation and scheduling of measurements. Herein, we report a laboratory X-ray setup allowing simultaneous XES and XAS measurements. The double von Hamos spectrometer performances are demonstrated by concurrent K beta XES and K-edge XAS measurements done for 3d elements.

  • 9. Blachucki, Wojciech
    et al.
    Szlachetko, Jakub
    Kayser, Yves
    Dousse, Jean-Claude
    Hoszowska, Joanna
    Fernandes, Daniel L. Abreu
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sa, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Study of the reactivity of silica supported tantalum catalysts with oxygen followed by in situ HEROS2015In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 17, no 28, p. 18262-18264Article in journal (Refereed)
    Abstract [en]

    We report on the reactivity of grafted tantalum organometallic catalysts with molecular oxygen. The changes in the local Ta electronic structure were followed by in situ high-energy resolution off-resonant spectroscopy (HEROS). The results revealed agglomeration and formation of Ta dimers, which cannot be reversed. The process occurs independently of starting grafted complex.

  • 10.
    Blachucki, Wojciech
    et al.
    Univ Fribourg, Dept Phys, Chemin Musee 3, CH-1700 Fribourg, Switzerland..
    Szlachetko, Jakub
    Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland.;Jan Kochanowski Univ Humanities & Sci, Inst Phys, PL-25406 Kielce, Poland..
    Kayser, Yves
    Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland..
    Dousse, Jean-Claude
    Univ Fribourg, Dept Phys, Chemin Musee 3, CH-1700 Fribourg, Switzerland..
    Hoszowska, Joanna
    Univ Fribourg, Dept Phys, Chemin Musee 3, CH-1700 Fribourg, Switzerland..
    Zeeshan, Faisal
    Univ Fribourg, Dept Phys, Chemin Musee 3, CH-1700 Fribourg, Switzerland..
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Warsaw, Poland.
    In situ high energy resolution off-resonant spectroscopy applied to a time-resolved study of single site Ta catalyst during oxidation2017In: Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, ISSN 0168-583X, E-ISSN 1872-9584, Vol. 411, p. 63-67Article in journal (Refereed)
    Abstract [en]

    In the present work high energy resolution off-resonant X-ray spectroscopy (HEROS) was employed at a synchrotron to study a silica supported Ta(V) bisalkyl catalyst activated in hydrogen. The Ta L alpha(1) HEROS spectra were measured during oxidation of the starting complex and the relative species' concentration was successfully retrieved as a function of time using the fingerprint HEROS spectra measured for the unoxidized and the oxidized catalyst. Based on the experimental data and theory-based calculations, it was shown that oxidation of the active Ta catalyst leads to the formation of mono- and di-meric species on the SiO2 surface. The obtained results were compared to those of the previously reported time resolved HEROS study on an inactive silica supported Ta(V) bisalkyl catalyst's concentration evolution during its oxidation Blachucki et al. (2015). The study allowed observation of an immediate transition of the active Ta catalyst from its unoxidized form to the oxidized one. This finding is dissimilar to the result of the study on the inactive Ta catalyst, where the oxidation led through an intermediate step.

  • 11.
    Bonarowska, Magdalena
    et al.
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Matus, Krzysztof
    Silesian Tech Univ, Inst Engn Mat & Biomat, PL-44100 Gliwice, Poland.
    Srebowata, Anna
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Application of silica-supported Ir and Ir-M (M=Pt, Pd, Au) catalysts for low-temperature hydrodechlorination of tetrachloromethane2018In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 644, p. 287-297Article in journal (Refereed)
    Abstract [en]

    Herein, it is presented a catalytic system for gas-phase hydrodechlorination of tetrachloromethane at low temperature and atmospheric pressure, using iridium supported on silica as parent catalyst. Iridium electronic configuration is suitable to catalyse the hydrodechlorination reactions, however, it has been rarely used in this reaction to date. The catalytic abilities were significantly improved when a second transition metal was added. Catalysts' stability and selectivity to the desired products (i.e. C-1-C-4 hydrocarbons) improved compared to conventional activation in hydrogen when catalysts were activated shortly with microwave irradiation. Microwave irradiation of catalysts favourably influences the homogeneity of the metallic active phase, both in terms of the size of metal crystals and the homogeneity of bimetallic systems. Addition of platinumto the 'parent' iridium catalyst improved its catalytic properties and decreased deactivation. Fresh and spent catalysts were comprehensively characterized using several techniques (BET, CO-chemisorption, XRD, XPS, electron microscopy and mass spectrometry) to determine structure-activity relationships and potential causes for catalyst deactivation. No significant changes in crystalline size or bimetallic phase composition were observed for spent catalysts (with the exception of Ir-Pd catalysts which underwent bulk carbide during the reaction).

  • 12.
    Bonarowska, Magdalena
    et al.
    Polish Acad Sci, Inst Phys Chem, Warsaw, Poland.
    Zielinski, Maciej
    Polish Acad Sci, Inst Phys Chem, Warsaw, Poland.
    Matus, Krzysztof
    Silesian Tech Univ, Inst Engn Mat & Biomat, Gliwice, Poland.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Warsaw, Poland.
    Srebowata, Anna
    Polish Acad Sci, Inst Phys Chem, Warsaw, Poland.
    Influence of microwave activation on the catalytic behavior of Pd-Au/C catalysts employed in the hydrodechlorination of tetrachloromethane2018In: Reaction Kinetics, Mechanisms and Catalysis, ISSN 1878-5190, E-ISSN 1878-5204, Vol. 124, no 1, p. 375-388Article in journal (Refereed)
    Abstract [en]

    This work investigates the influence of activation by microwave irradiation on the catalytic properties of Pd-Au/C-Sibunit catalysts in the hydrodechlorination of CCl4. Pd and Pd-Au samples were thoroughly characterized by CO chemisorption, X-ray diffraction, TPHD and STEM, and used in gas phase hydrodechlorination of tetrachloromethane. The studies showed that homogenous Pd-Au alloys are formed more efficiently if short-time microwave activation is applied instead of conventional activation by H-2 reduction at 380 A degrees C. These catalysts show higher activity, stability and higher selectivity towards the desired products (C1-C5 hydrocarbons) than the catalysts activated by conventional reduction in 10%H-2/Ar flow.

  • 13.
    Błachucki, Wojciech
    et al.
    Institute of Physical Chemistry, Polish Academy of Sciences, Warsaw 01-224, Poland.
    Hoszowska, Joanna
    Department of Physics, University of Fribourg, Chemin du Musée 3, CH-1700 Fribourg, Switzerland.
    Dousse, Jean-Claude
    Department of Physics, University of Fribourg, Chemin du Musée 3, CH-1700 Fribourg, Switzerland.
    Kayser, Yves
    Physikalisch-Technische Bundesanstalt (PTB), Abbestr. 2-12, Berlin 10587,Germany.
    Stachura, Regina
    Institute of Physics, Jan Kochanowski University, Kielce 25-406, Poland.
    Tyrała, Krzysztof
    Institute of Physics, Jan Kochanowski University, Kielce 25-406, Poland.
    Wojtaszek, Klaudia
    Institute of Physics, Jan Kochanowski University, Kielce 25-406, Poland.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Institute of Physical Chemistry, Polish Academy of Sciences, Warsaw 01-224, Poland.
    Szlachetko, Jakub
    Institute of Physical Chemistry, Polish Academy of Sciences, Warsaw 01-224, Poland.;Institute of Physics, Jan Kochanowski University, Kielce 25-406, Poland.
    High energy resolution off-resonant spectroscopy: A review2017In: Spectrochimica Acta Part B - Atomic Spectroscopy, ISSN 0584-8547, E-ISSN 1873-3565, Vol. 136, no Supplement C, p. 23-33Article, review/survey (Refereed)
    Abstract [en]

    We review the high energy resolution off-resonant spectroscopy (HEROS) technique. HEROS probes the unoccupied electronic states of matter in a single-shot manner thanks to the combination of off-resonant excitation around atomic core states using wavelength dispersive X-ray detection setups. In this review we provide a general introduction to the field of X-ray spectroscopy together with the specification of the available X-ray techniques and X-ray methodologies. Next, the theoretical description of the HEROS approach is introduced with a special focus on the derivation of the X-ray emission and X-ray absorption correspondence relation at off-resonant excitation conditions. Finally, a number of experimental HEROS reports are reviewed in the field of chemistry and material science. We emphasize the applicability of HEROS to pulsed X-ray sources, like X-ray free electron lasers, and support the review with experimental examples. The review is complemented with perspectives on and possible further applications of the HEROS technique to the field of X-ray science.

  • 14. Cairns, Marie-Louise
    et al.
    Dickson, Glenn R
    Orr, John F
    Farrar, David
    Hardacre, Christopher
    Sa, Jacinto
    Lemoine, Patrick
    Mughal, Muhammad Zeeshan
    Buchanan, Fraser J
    The potential of electron beam radiation for simultaneous surface modification and bioresorption control of PLLA.2012In: Journal of Biomedical Materials Research. Part A, ISSN 1549-3296, E-ISSN 1552-4965, Vol. 100, no 9, p. 2223-9Article in journal (Refereed)
    Abstract [en]

    Bioresorbable polymers have been widely investigated as materials exhibiting significant potential for successful application in the fields of tissue engineering and drug delivery. Further to the ability to control degradation, surface engineering of polymers has been highlighted as a key method central to their development. Previous work has demonstrated the ability of electron beam (e-beam) technology to control the degradation profiles and bioresorption of a number of commercially relevant bioresorbable polymers (poly-l-lactic acid (PLLA), L-lactide/DL-lactide co-polymer (PLDL) and poly(lactic-co-glycolic acid (PLGA)). This work investigates the further potential of e-beam technology to impart added biofunctionality through the manipulation of polymer (PLLA) surface properties. PLLA samples were subjected to e-beam treatments in air, with varying beam energies and doses. Surface characterization was then performed using contact angle analysis, X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and atomic force microscopy. Results demonstrated a significant increase in surface wettability post e-beam treatment. In correlation with this, XPS data showed the introduction of oxygen-containing functional groups to the surface of PLLA. Raman spectroscopy indicated chain scission in the near surface region of PLLA (as predicted). However, e-beam effects on surface properties were not shown to be dependent on beam energy or dose. E-beam irradiation did not seem to affect the surface roughness of PLLA as a direct consequence of the treatment.

  • 15. Campbell, Paul S.
    et al.
    Santini, Catherine C.
    Bayard, Francois
    Chauvin, Yves
    Colliere, Vincent
    Podgorsek, Ajda
    Gomes, Margarida F. Costa
    Sa, Jacinto
    Olefin hydrogenation by ruthenium nanoparticles in ionic liquid media: Does size matter?2010In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 275, no 1, p. 99-107Article in journal (Refereed)
  • 16.
    Cieslak, Anna M.
    et al.
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland..
    Pavliuk, Mariia V.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    D'Amario, Luca
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Abdellah, Mohamed
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sokolowski, Kamil
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland..
    Rybinska, Urszula
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Fernandes, Daniel L. A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Leszczynski, Michal K.
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland..
    Mamedov, Fikret
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    El-Zhory, Ahmed M.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Föhlinger, Jens
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Budinska, Alena
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Wolska-Pietkiewicz, Malgorzata
    Warsaw Univ Technol, Fac Chem, PL-00661 Warsaw, Poland..
    Hammarström, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Lewinski, Janusz
    Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.;Warsaw Univ Technol, Fac Chem, PL-00661 Warsaw, Poland..
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland..
    Ultra long-lived electron-hole separation within water-soluble colloidal ZnO nanocrystals: Prospective Applications For Solar Energy Production2016In: Nano Energy, ISSN 2211-2855, Vol. 30, p. 187-192Article in journal (Refereed)
    Abstract [en]

    Zinc oxide was one of the first semiconductors used in dye-sensitized solar cells but its instability in aqueous media precludes its use for large-scale applications. Herein, we report on a novel ZnO nanocrystal material derived by an organometallic approach that is simultaneously stable and soluble in water due to its carboxylate oligoethylene glycol shell strongly anchored to the inorganic core by the head groups. The resulting unique inorganic core-organic shell interface also stabilizes the photo-generated hole, leading to a dramatic slowing down of charge recombination, which otherwise is a major hurdle in using nanostructured ZnO.

  • 17.
    Czapla-Masztafiak, Joanna
    et al.
    Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland.;PSI, CH-5232 Villigen, Switzerland..
    Nogueira, Juan J.
    Univ Vienna, Inst Theoret Chem, Fac Chem, Wahringer Str 17, A-1090 Vienna, Austria..
    Lipiec, Ewelina
    Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland.;Swiss Fed Inst Technol, Vladimir Prelog Weg 1-5-10, CH-8093 Zurich, Switzerland..
    Kwiatek, Wojciech M.
    Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland..
    Wood, Bayden R.
    Monash Univ, Sch Chem, Ctr Biospectroscopy, Victoria 3800, Australia..
    Deacon, Glen B.
    Monash Univ, Sch Chem, Fac Sci, Clayton, Vic 3800, Australia..
    Kayser, Yves
    PSI, CH-5232 Villigen, Switzerland..
    Fernandes, Daniel L. A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Pavliuk, Mariia V.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Szlachetko, Jakub
    PSI, CH-5232 Villigen, Switzerland.;Jan Kochanowski Univ Humanities & Sci, Inst Phys, Swietokrzyska 15 St, PL-25406 Kielce, Poland..
    Gonzalez, Leticia
    Univ Vienna, Inst Theoret Chem, Fac Chem, Wahringer Str 17, A-1090 Vienna, Austria..
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Direct Determination of Metal Complexes' Interaction with DNA by Atomic Telemetry and Multiscale Molecular Dynamics2017In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 8, no 4, p. 805-811Article in journal (Refereed)
    Abstract [en]

    The lack of molecular mechanistic understanding of the interaction between metal complexes and biomolecules hampers their potential medical use. Herein we present a robust procedure combining resonant X-ray emission spectroscopy and multiscale molecular dynamics simulations, which allows for straightforward elucidation of the precise interaction mechanism at the atomic level. The report unveils an unforeseen hydrolysis process and DNA binding of [Pt{N(p-HC6F4)CH2}(2)py(2)] (Pt103), which showed potential cytotoxic activity in the past. Pt103 preferentially coordinates to adjacent adenine sites, instead of guanine sites as in cisplatin, because of its hydrogen bond ability. Comparison with previous research on cisplatin suggests that selective binding to guanine or adenine may be achieved by controlling the acidity of the compound.

  • 18.
    Czapla-Masztafiak, Joanna
    et al.
    Paul Scherrer Inst, Villigen, Switzerland.;Polish Acad Sci, Inst Nucl Phys, Krakow, Poland..
    Szlachetko, Jakub
    Paul Scherrer Inst, Villigen, Switzerland.;Jan Kochanowski Univ Humanities & Sci, Inst Phys, Kielce, Poland..
    Milne, Christopher J.
    Paul Scherrer Inst, Villigen, Switzerland..
    Lipiec, Ewelina
    Sa, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Warsaw, Poland..
    Penfold, Thomas J.
    Newcastle Univ, Dept Chem, Bedson Bldg, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England..
    Huthwelker, Thomas
    Paul Scherrer Inst, Villigen, Switzerland..
    Borca, Camelia
    Paul Scherrer Inst, Villigen, Switzerland..
    Abela, Rafael
    Paul Scherrer Inst, Villigen, Switzerland..
    Kwiatek, Wojciech M.
    Polish Acad Sci, Inst Nucl Phys, Krakow, Poland..
    Investigating DNA Radiation Damage Using X-Ray Absorption Spectroscopy2016In: Biophysical Journal, ISSN 0006-3495, E-ISSN 1542-0086, Vol. 110, no 6, p. 1304-1311Article in journal (Refereed)
    Abstract [en]

    The biological influence of radiation on living matter has been studied for years; however, several questions about the detailed mechanism of radiation damage formation remain largely unanswered. Among all biomolecules exposed to radiation, DNA plays an important role because any damage to its molecular structure can affect the whole cell and may lead to chromosomal rearrangements resulting in genomic instability or cell death. To identify and characterize damage induced in the DNA sugar-phosphate backbone, in this work we performed x-ray absorption spectroscopy at the P K-edge on DNA irradiated with either UVA light or protons. By combining the experimental results with theoretical calculations, we were able to establish the types and relative ratio of lesions produced by both UVA and protons around the phosphorus atoms in DNA.

  • 19.
    Fernandes, Daniel L. A.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Budinska, Alena
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Pavliuk, Mariia V.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland..
    Novel photo-reactor for fast screening of photo-catalytic systems2017In: Journal of Photochemistry and Photobiology A: Chemistry, ISSN 1010-6030, E-ISSN 1873-2666, Vol. 335, p. 36-39Article in journal (Refereed)
    Abstract [en]

    Photo-catalysis is an emerging technology for clean energy production, organic synthesis and environmental protection, etc. While there is a hydrogen of systems and schemes to attain these objectives, there is a paucity of photo-reactors capable of determine catalytic abilities in real time with reduce amounts of samples, i.e., fast-screening of catalyst and reaction parameters. Herein, we report a novel photo-reactor for simultaneous online monitoring of gaseous products with quadrupole mass spectrometry and photo-physics with fibre optic UV/Vis with millisecond time resolution on 4 mL cuvettes.

  • 20.
    Fernandes, Daniel L. A.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Paun, Cristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Pavliuk, Mariia V.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Fernandes, Arthur B.
    Univ Sao Paulo, Inst Chem, Dept Fundamental Chem, BR-05508000 Sao Paulo, Brazil..
    Bastos, Erick L.
    Univ Sao Paulo, Inst Chem, Dept Fundamental Chem, BR-05508000 Sao Paulo, Brazil..
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland..
    Green microfluidic synthesis of monodisperse silver nanoparticles via genetic algorithm optimization2016In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 6, no 98, p. 95693-95697Article in journal (Refereed)
    Abstract [en]

    A scalable and green procedure for the microfluidic flow synthesis of monodisperse silver nanoparticles is reported. Beetroot extract is used both as a reducing and growth-regulating agent. A multi-objective genetic algorithm was used to automate the optimization of the reaction and reduce sample polydispersity observed in previous reports. The proposed methodology ensures high-quality nanoparticles in a rapidly manner and devoid of human skill or intuition, essential for method standardization and implementation.

  • 21.
    Fernandes, Daniel L. A.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Pavliuk, Maria V.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sa, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    A 3D printed microliquid jet with an adjustable nozzle diameter2015In: The Analyst, ISSN 0003-2654, E-ISSN 1364-5528, Vol. 140, no 18, p. 6234-6238Article in journal (Refereed)
    Abstract [en]

    Microliquid jets have many applications, in particular in the fields of spectroscopy/analysis of samples susceptible to beam damage. Herein, we report a microliquid jet, manufactured with 3D printing technology, with a tuneable nozzle diameter output. This strategy increases the breadth of techniques that can be covered with a single microliquid jet.

  • 22. Friedli, Peter
    et al.
    Sigg, Hans
    Sá, Jacinto
    Dye-injected electron trapping in TiO2 determined by broadband transient infrared spectroscopy.2014In: Photochemical and Photobiological Sciences, ISSN 1474-905X, E-ISSN 1474-9092, Vol. 13, no 10, p. 1393-6Article in journal (Refereed)
    Abstract [en]

    We report the dynamics of electrons injected into TiO2 due to the excitation of Ru-N719 dye at 532 nm. The synchrotron based broadband transient mid-IR spectroscopy revealed that the injected electrons are quickly confined to a trap state with an average energy of ca. 240 meV below the conduction band. The average energy of the trapping states did not change with the increase of the delay time, suggesting a singular electronic identity of the trap states.

  • 23.
    Garlisi, Corrado
    et al.
    Khalifa Univ Sci & Technol, Dept Chem Engn, Masdar Inst, POB 54224, Abu Dhabi, U Arab Emirates..
    Szlachetko, Jakub
    Jan Kochanowski Univ Humanities & Sci, Inst Phys, Kielce, Poland.;Polish Acad Sci, Inst Phys Chem, Warsaw, Poland..
    Aubry, Cyril
    Khalifa Univ Sci & Technol, Dept Mech Engn, Masdar Inst, POB 54224, Abu Dhabi, U Arab Emirates..
    Fernandes, Daniel L. A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Hattori, Yocefu
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Paun, Cristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Pavliuk, Mariia V.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Rajput, Nitul S.
    Khalifa Univ Sci & Technol, Dept Mech Engn, Masdar Inst, POB 54224, Abu Dhabi, U Arab Emirates..
    Lewin, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Warsaw, Poland.
    Palmisano, Giovanni
    Khalifa Univ Sci & Technol, Dept Chem Engn, Masdar Inst, POB 54224, Abu Dhabi, U Arab Emirates..
    N-TiO2/Cu-TiO2 double-layer films: Impact of stacking order on photocatalytic properties2017In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 353, p. 116-122Article in journal (Refereed)
    Abstract [en]

    In this work, we report for the first time a unique configuration of N-doped and Cu-doped TiO2 bilayer. The activity of TiO2 was improved by combining Cu- and N-doping in a layered thin-film structure. The impact of the stacking order was studied, pointing out how the best arrangement is by far the one with Cu-TiO2 as the top layer. The results reveal a unique and simple way to enhance the photocatalytic response of TiO2 in the visible domain.

  • 24.
    Gizinski, Damian
    et al.
    Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Blachucki, Wojciech
    Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Srebowata, Anna
    Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Zienkiewicz-Machnik, Malgorzata
    Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Goszewska, Ilona
    Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Matus, Krzysztof
    Silesian Tech Univ, Inst Engn Mat & Biomat, Konarskiego 18 A, PL-44100 Gliwice, Poland.
    Lisovytskiy, Dmytro
    Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Pisarek, Marcin
    Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Szlachetko, Jakub
    Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland;Polish Acad Sci, Inst Nucl Phys, Ul Radzikowskiego 152, PL-31342 Krakow, Poland.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Ul Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    On-the-fly Catalyst Accretion and Screening in Chemoselective Flow Hydrogenation2018In: ChemCatChem, ISSN 1867-3880, E-ISSN 1867-3899, Vol. 10, no 17, p. 3641-3646Article in journal (Refereed)
    Abstract [en]

    Herein, it is reported an on-the-fly accretion/reaction protocol to evaluate the structure-performance relationship in the chemoselective flow citral hydrogenation over Ni-based catalysts. Based on the methodology one was able to determine Ni nanoparticles ideal average size (ca. 9nm), in a rapid and facile manner. The methodology offers a simple workflow, cost-effective and adaptable strategy for process intensification and optimization.

  • 25.
    Gizinski, Damian
    et al.
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Goszewska, Ilona
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Zielinski, Maciej
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Lisovytskiy, Dmytro
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Nikiforov, Kostiantyn
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Masternak, Joanna
    Jan Kochanowski Univ Humanities & Sci, Inst Chem, Swietokrzyska 15G, PL-25406 Kielce, Poland..
    Zienkiewicz-Machnik, Malgorzata
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Srebowata, Anna
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    Chemoselective flow hydrogenation of alpha,beta - Unsaturated aldehyde with nano-nickel2017In: Catalysis communications, ISSN 1566-7367, E-ISSN 1873-3905, Vol. 98, p. 17-21Article in journal (Refereed)
    Abstract [en]

    Herein, it is presented a novel catalytic system for the continuous flow chemoselective hydrogenation of a,alpha,beta- unsaturated aldehydes used in the production of high value cosmetics and pharmaceuticals precursors. The reaction was catalyzed by nano nickel particles grafted on polymeric support, synthesized via a simple, adaptable and green methodology. The system was highly active and very selective to C=C bond saturation.

  • 26.
    Gizinski, Damian
    et al.
    Polish Acad Sci, Inst Phys Chem, Warsaw, Poland..
    Sa, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Warsaw, Poland.;Ecole Polytech Fed Lausanne, Lab Ultrafast Spect, CH-1015 Lausanne, Switzerland..
    Hydrogenation by Copper Catalysts2016In: Hydrogenation With Low-Cost Transition Metals, CRC PRESS-TAYLOR & FRANCIS GROUP , 2016, p. 79-117Chapter in book (Refereed)
    Abstract [en]

    This chapter deals with hydrogenation mediated by copper metal present as supported and unsupported nanoparticles. In the chapter, we highlight synthetic procedures for the preparation of metallic copper nanoparticles and their applications in catalysis. The main target is reactions carried out for fine and pharmaceutical chemicals' production.

  • 27. Goguet, Alexandre
    et al.
    Ace, Matthew
    Saih, Youssef
    Sa, Jacinto
    Kavanagh, Joy
    Hardacre, Christopher
    Remarkable stability of ionic gold supported on sulfated lanthanum oxide.2009In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, no 32, p. 4889-91Article in journal (Refereed)
    Abstract [en]

    Isolated cationic gold deposited on sulfated lanthanum oxide has been shown to exhibit remarkable stability opening a promising way of stabilising ionic gold for catalytic reactions.

  • 28. Goguet, Alexandre
    et al.
    Hardacre, Christopher
    Harvey, Ian
    Narasimharao, Katabathini
    Saih, Youssef
    Sa, Jacinto
    Increased dispersion of supported gold during methanol carbonylation conditions.2009In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 131, no 20, p. 6973-5Article in journal (Refereed)
    Abstract [en]

    The active site in supported gold catalysts for the carbonylation of methanol has been identified as dimers/trimers of gold which are formed from large gold particles >10 nm in diameter. Methyl iodide was found to be critical for this dispersion process and to maintain the catalyst in the active form. This study also shows that it may be possible to redisperse gold catalysts, in general, after reaction.

  • 29. Goguet, Alexandre
    et al.
    Partridge, William P.
    Aiouche, Farid
    Hardacre, Christopher
    Morgan, Kevin
    Stere, Cristina
    Sa, Jacinto
    Comment on "The Critical evaluation of in situ probe techniques for catalytic honeycomb monoliths" by Hettel et al.2014In: Catalysis Today, ISSN 0920-5861, E-ISSN 1873-4308, Vol. 236, p. 206-208Article in journal (Refereed)
  • 30.
    Goncalves, Leticia C. P.
    et al.
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9 163, A-1060 Vienna, Austria.
    Mansouri, Hamid R.
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9 163, A-1060 Vienna, Austria.
    PourMehdi, Shads
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9 163, A-1060 Vienna, Austria.
    Abdellah, Mohamed
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Department of Chemistry, Qena Faculty of Science, South Valley University, 83523 Qena, Egypt.
    Fadiga, Bruna S.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Univ Sao Paulo, Inst Chem, Dept Fundamental Chem, BR-03178200 Sao Paulo, Brazil.
    Bastos, Erick L.
    Univ Sao Paulo, Inst Chem, Dept Fundamental Chem, BR-03178200 Sao Paulo, Brazil.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Mihovilovic, Marko D.
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9 163, A-1060 Vienna, Austria.
    Rudroffe, Florian
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9 163, A-1060 Vienna, Austria.
    Boosting photobioredox catalysis by morpholine electron donors under aerobic conditions2019In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 9, no 10, p. 2682-2688Article in journal (Refereed)
    Abstract [en]

    Light-driven reduction of flavins, e.g. FAD or FMN, by sacrificial electron donors emerged as a convenient method to promote biocatalytic transformations. However, flavin activation has been restricted to oxygen-free conditions to prevent enzyme deactivation caused by reactive oxygen species (ROS). Herein, we show that the photoreduction of FMN by morpholines, including 3-(N-morpholino)propanesulfonic acid (MOPS), lessens the deactivation of the enoate reductase XenB from Pseudomonas sp. during the stereoselective asymmetric enzymatic reduction of a model ,-unsaturated diketone under aerobic conditions, leading to a 91% GC-yield and a stereoselectivity greater than 94%. The kinetic stability of the thermolabile XenB was increased by more than 20-fold in MOPS buffer compared to that in Tris-HCl buffer, and a pronounced positive effect on the transition midpoint temperature was observed. The reactive form of the FMN photocatalyst is stabilized by the formation of a (3)[FMN--MOPS+] ensemble, which reduces the formation of hydrogen peroxide and other ROS in the presence of oxygen. These results contribute to broaden the application of photobiocatalytic transformations using flavin-dependent reductases.

  • 31.
    Goncalves, Leticia C. P.
    et al.
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9-163, A-1060 Vienna, Austria.
    Mansouri, Hanild R.
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9-163, A-1060 Vienna, Austria.
    Bastos, Erick L.
    Univ Sao Paulo, Inst Chem, Dept Fundamental Chem, BR-03178200 Sao Paulo, Brazil.
    Abdellah, Mohamed
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt.
    Fadiga, Bruma S.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Univ Sao Paulo, Inst Chem, Dept Fundamental Chem, BR-03178200 Sao Paulo, Brazil.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Rudroff, Florian
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9-163, A-1060 Vienna, Austria.
    Mihovilovic, Marko D.
    TU Wien, Inst Appl Synthet Chem, Getreidemarkt 9-163, A-1060 Vienna, Austria.
    Morpholine-based buffers activate aerobic photobiocatalysis via spin correlated ion pair formation2019In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 9, no 6, p. 1365-1371Article in journal (Refereed)
    Abstract [en]

    The use of enzymes for synthetic applications is a powerful and environmentally-benign approach to increase molecular complexity. Oxidoreductases selectively introduce oxygen and hydrogen atoms into myriad substrates, catalyzing the synthesis of chemical and pharmaceutical building blocks for chemical production. However, broader application of this class of enzymes is limited by the requirements of expensive cofactors and low operational stability. Herein, we show that morpholine-based buffers, especially 3-(N-morpholino)propanesulfonic acid (MOPS), promote photoinduced flavoenzyme-catalyzed asymmetric redox transformations by regenerating the flavin cofactor via sacrificial electron donation and by increasing the operational stability of flavin-dependent oxidoreductases. The stabilization of the active forms of flavin by MOPS via formation of the spin correlated ion pair (3)[flavin(-)-MOPS+] ensemble reduces the formation of hydrogen peroxide, circumventing the oxygen dilemma under aerobic conditions detrimental to fragile enzymes.

  • 32.
    Goszewska, Ilona
    et al.
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Gizinski, Damian
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Zienkiewicz-Machnik, Malgorzata
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Lisovytskiy, Dmytro
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Nikiforov, Kostyantyn
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Masternak, Joanna
    Jan Kochanowski Univ Humanities & Sci, Inst Chem, Swietokrzyska 15G, PL-25406 Kielce, Poland..
    Srebowata, Anna
    Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland..
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Kasprzaka 44-52, PL-01224 Warsaw, Poland.
    A novel nano-palladium catalyst for continuous-flow chemoselective hydrogenation reactions2017In: Catalysis communications, ISSN 1566-7367, E-ISSN 1873-3905, Vol. 94, p. 65-68Article in journal (Refereed)
    Abstract [en]

    Herein, we report a catalyst composed of palladium nanoparticles immobilized on polymeric resin for chemoselective hydrogenation reactions under flow conditions. The catalyst exhibits high activity and selectivity towards hydrogenation of C=C double bond, as confirmed in the hydrogenation of 2-heptene and 6-methyl-5-hepten-2-one.

  • 33.
    Hattori, Yocefu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Abdellah, Mohamed
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt.
    Meng, Jie
    Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark.
    Zheng, Kaibo
    Tech Univ Denmark, Dept Chem, DK-2800 Lyngby, Denmark;Lund Univ, Chem Phys & NanoLund, Box 124, S-22100 Lund, Sweden.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Simultaneous Hot Electron and Hole Injection upon Excitation of Gold Surface Plasmon2019In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 10, no 11, p. 3140-3146Article in journal (Refereed)
    Abstract [en]

    We have successfully investigated the simultaneous injection of hot electrons and holes upon excitation of gold localized surface plasmon resonance (LSPR). The studies were performed on all-solid-state plasmonic system composed of titanium dioxide (TiO2)/poly(3,4-ethylenedioxythiophene) :poly(styrenesulfonic acid) (PEDOT:PSS) p-n junctions with gold nanoparticles (Au NPs). The study revealed that both charge carriers are transferred within 200 fs to the respective charge acceptors, exhibiting a free carrier transport behavior. We also confirmed that the transfer of charge carriers are accompanied by change in the initial relaxation dynamics of Au NPs.

  • 34.
    Hattori, Yocefu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Abdellah, Mohamed
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt.
    Rocha, Igor
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Pavliuk, Mariia V.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Fernandes, Daniel L. A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.
    Light-induced ultrafast proton-coupled electron transfer responsible for H-2 evolution on silver plasmonics2018In: Materials Today, ISSN 1369-7021, E-ISSN 1873-4103, Vol. 21, no 6, p. 590-593Article in journal (Refereed)
    Abstract [en]

    Light-driven proton-coupled electron transfer (PCET) reactions on nanoplasmonics would bring temporal control of their reactive pathways, in particular, prolong their charge separation state. Using a silver nano-hybrid plasmonic structure, we observed that optical excitation of Ag-localized surface plasmon instigated electron injection into TiO2 conduction band and oxidation of isopropanol alcoholic functionality. Femtosecond transient infrared absorption studies show that electron transfer from Ag to TiO2 occurs in ca. 650 fs, while IPA molecules near the Ag surface undergo an ultrafast bidirectional PCET step within 400 fs. Our work demonstrates that ultrafast PCET reaction plays a determinant role in prolonging charge separation state, providing an innovative strategy for visible-light photocatalysis with plasmonic nanostructures.

  • 35. Kartusch, Christiane
    et al.
    Krumeich, Frank
    Safonova, Olga
    Hartfelder, Urs
    Makosch, Martin
    Sa, Jacinto
    van Bokhoven, Jeroen A.
    Redispersion of Gold Multiple-Twinned Particles during Liquid-Phase Hydrogenation2012In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 2, no 7, p. 1394-1403Article in journal (Refereed)
  • 36. Kartusch, Christiane
    et al.
    Makosch, Martin
    Sa, Jacinto
    Hungerbuehler, Konrad
    van Bokhoven, Jeroen A.
    The Dynamic Structure of Gold Supported on Ceria in the Liquid Phase Hydrogenation of Nitrobenzene2012In: ChemCatChem, ISSN 1867-3880, E-ISSN 1867-3899, Vol. 4, no 2, p. 236-242Article in journal (Refereed)
  • 37.
    Kayser, Yves
    et al.
    Paul Scherrer Inst, CH-5232 Villigen, Switzerland..
    Sa, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland..
    Szlachetko, Jakub
    Paul Scherrer Inst, CH-5232 Villigen, Switzerland.;Jan Kochanowski Univ Humanities & Sci, Inst Phys, PL-25406 Kielce, Poland..
    Depth-Resolved X-ray Absorption Spectroscopy by Means of Grazing Emission X-ray Fluorescence2015In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 87, no 21, p. 10815-10821Article in journal (Refereed)
    Abstract [en]

    Grazing emission X-ray fluorescence (GEXRF) is well suited for nondestructive elemental-sensitive depth-profiling measurements on samples with nanometer-sized features. By varying the grazing emission angle under which the X-ray fluorescence signal is detected, the probed depth range can be tuned from a few to several hundred nanometers. The dependence of the XRF intensity on the grazing emission angle can be assessed in a sequence of measurements or in a scanning-free approach using a position-sensitive area detector. Hereafter, we will show that the combination of scanning-free GEXRF and fluorescence detected X-ray absorption spectroscopy (XAS) allows for depth-resolved chemical speciation measurements with nanometer-scale accuracy. While the conventional grazing emission geometry is advantageous to minimize self-absorption effects, the use of a scanning-free setup makes the sequential scanning of the grazing emission angles obsolete and paves the way toward time-resolved depth-sensitive XAS measurements. The presented experimental approach was applied to study the surface oxidation of an Fe layer on the top of bulk Si and of a Ge bulk sample. Thanks to the penetrating properties and the insensitivity toward the electric conduction properties of the incident and emitted X-rays, the presented experimental approach is well suited for in situ sample surface studies in the nanometer regime.

  • 38. Kayser, Yves
    et al.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Szlachetko, Jakub
    Nanoparticle characterization by means of scanning free grazing emission X-ray fluorescence.2015In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 7, no 20, p. 9320-9330Article in journal (Refereed)
    Abstract [en]

    Nanoparticles are considered for applications in domains as various as medical and pharmaceutical sciences, opto- and microelectronics, catalysis, photovoltaics, spintronics or nano- and biotechnology. The applications realized with nanocrystals depend strongly on the physical dimensions (shape and size) and elemental constitution. We demonstrate here that grazing emission X-ray fluorescence (GEXRF) is an element sensitive technique that presents the potential for a reliable and accurate determination of the morphology of nanoparticles deposited on a flat substrate (ready-to-use devices). Thanks to the scanning-free approach of the used GEXRF setup, the composition, shape and average size of nanoparticles are determined in short time intervals, minimizing the exposure to radiation. The (scanning-free) GEXRF technique allows for in situ investigations of the nanoparticulate systems thanks to the penetration properties of both the probe X-ray beam and the emitted X-ray fluorescence signal.

  • 39. Kleymenov, Evgeny
    et al.
    Sa, Jacinto
    Abu-Dahrieh, Jehad
    Rooney, David
    Van Bokhoven, Jeroen A.
    Troussard, Ekaterina
    Szlachetko, Jakub
    Safonova, Olga V.
    Nachtegaal, Maarten
    Structure of the methanol synthesis catalyst determined by in situ HERFD XAS and EXAFS2012In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 2, no 2, p. 373-378Article in journal (Refereed)
  • 40. Kowalewski, Emil
    et al.
    Zienkiewicz-Machnik, Malgorzata
    Lisovytskiy, Dmytro
    Nikiforov, Kostiantyn
    Matus, Krzysztof
    Srebowata, Anna
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Turbostratic carbon supported palladium as an efficient catalyst for reductive purification of water from trichloroethylene2017In: AIMS Materials Science, ISSN 2372-0468, Vol. 4, no 6, p. 1276-1288Article in journal (Refereed)
    Abstract [en]

    This work investigates the catalytic properties of turbostratic carbon supported Pd catalyst in hydrodechlorination of trichloroethylene (TCE HDC) in aqueous phase. 1.57 wt% Pd/C was thoroughly characterized by BET, TPHD, CO chemisorption, PXRD, STEM, XPS and used as the catalyst in removal of trichloroethylene from drinking water in batch and continuous - flow reactors. The studies showed that catalytic performance of Pd/C depended on the hydrophobicity and textural properties of carbon support, which influenced noble metal dispersion and increased catalyst tolerance against deactivation by chlorination. Palladium in the form of uniformly dispersed small (~3.5 nm) nanoparticles was found to be very active and stable in purification of water from TCE both in batch and continuous - flow operation.   

  • 41. Legagneux, Nicolas
    et al.
    Basset, Jean-Marie
    Thomas, Amélie
    Lefebvre, Frédéric
    Goguet, Alexandre
    Sá, Jacinto
    Hardacre, Christopher
    Characterization of silica-supported dodecatungstic heteropolyacids as a function of their dehydroxylation temperature.2009In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, no 12, p. 2235-40Article in journal (Refereed)
    Abstract [en]

    Dodecatungsto-silicic H(4)SiW(12)O(40) and -phosphoric acids H(3)PW(12)O(40) were deposited on silica by a classical impregnation technique. The resulting materials were studied by in situ Raman and infrared spectroscopy, XPS and by solid-state (1)H MAS NMR as a function of their dehydroxylation temperature. The data show that in the case of H(3)PW(12)O(40) three silanol groups are protonated while in the case of H(4)SiW(12)O(40) at least one acidic proton remains. Upon heating this proton reacts leading to a disordered structure and a broadening of the W-O Raman bands.

  • 42. Lipiec, Ewelina
    et al.
    Czapla, Joanna
    Szlachetko, Jakub
    Kayser, Yves
    Kwiatek, Wojciech
    Wood, Bayden
    Deacon, Glen B
    Sá, Jacinto
    Novel in situ methodology to observe the interactions of chemotherapeutical Pt drugs with DNA under physiological conditions.2014In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 43, no 37, p. 13839-44Article in journal (Refereed)
    Abstract [en]

    The binding of the antitumor drug cisplatin with DNA was determined by means of in situ resonant inelastic X-ray scattering (RIXS) spectroscopy. Because of the penetrating properties of hard X-rays, we could determine, under physiological conditions, the identity and number of platinum complexes present. In situ RIXS revealed that under physiological conditions, water molecules replace chloride ligands owing to drug hydration. The subsequent interaction with DNA, led to the bonding of the aqua complexes into the DNA structure with simultaneous loss of the coordinating water and chloride ion. The data analysis reveals that Pt is coordinated by two adjacent guanines giving cis-[Pt(NH3)2{d(GpG)-N7(1),-N7(2)}] upon losing its coordinating water or chloride ligands.

  • 43.
    Lojewska, Tomila
    et al.
    Polish Acad Sci, Inst Phys Chem, Warsaw, Poland..
    Sa, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Polish Acad Sci, Inst Phys Chem, Warsaw, Poland.;Ecole Polytech Fed Lausanne, Lab Ultrafast Spect, CH-1015 Lausanne, Switzerland..
    Hydrogenation by Iron Catalysts2016In: Hydrogenation With Low-Cost Transition Metals, CRC PRESS-TAYLOR & FRANCIS GROUP , 2016, p. 119-154Chapter in book (Refereed)
    Abstract [en]

    This chapter deals with hydrogenation mediated by iron metal present as supported and unsupported nanoparticles. Inspired by nature, design scientists have developed homogeneous and heterogeneous systems to perform selective hydrogenation. In the chapter, we highlight synthetic procedures for the preparation of metallic iron nanoparticles and their applications to fine and pharmaceutical chemical production.

  • 44. Makosch, Martin
    et al.
    Bumbalek, Vaclav
    Sa, Jacinto
    van Bokhoven, Jeroen A.
    Alternative preparation of size-controlled thiol-capped gold colloids2013In: Gold Bulletin, ISSN 0017-1557, Vol. 46, no 3, p. 161-164Article in journal (Refereed)
  • 45. Makosch, Martin
    et al.
    Kartusch, Christiane
    Sá, Jacinto
    Duarte, Renata Bessa
    van Bokhoven, Jeroen A
    Kvashnina, Kristina
    Glatzel, Pieter
    Fernandes, Daniel L A
    Nachtegaal, Maarten
    Kleymenov, Evgeny
    Szlachetko, Jakub
    Neuhold, Bobby
    Hungerbühler, Konrad
    HERFD XAS/ATR-FTIR batch reactor cell.2012In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 14, no 7, p. 2164-70Article in journal (Refereed)
    Abstract [en]

    An autoclave reactor was modified to perform simultaneously high energy resolution fluorescence detected X-ray absorption spectroscopy (HERFD XAS) and attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy measurements without altering the reactor design. This operando cell allows one to follow changes in the electronic and geometric structure of the catalyst with HERFD XAS and relate them to the simultaneously detected activity and reaction species with ATR-FTIR formed during the reaction in the liquid phase. The capability of the cell is demonstrated by two studies. The first shows the reduction of Au/CeO(2) precursors in different solvents. The second shows that mainly Au(0) is present in the hydrogenation of nitrobenzene over Au/CeO(2).

  • 46. Makosch, Martin
    et al.
    Lin, Wan-Ing
    Bumbalek, Viclav
    Sa, Jacinto
    Medlin, J. Will
    Hungerbuehler, Konrad
    van Bokhoven, Jeroen A.
    Organic Thiol Modified Pt/TiO2 Catalysts to Control Chemoselective Hydrogenation of Substituted Nitroarenes2012In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 2, no 10, p. 2079-2081Article in journal (Refereed)
  • 47. Makosch, Martin
    et al.
    Sa, Jacinto
    Kartusch, Christiane
    Richner, Gilles
    van Bokhoven, Jeroen A.
    Hungerbuehler, Konrad
    Hydrogenation of Nitrobenzene Over Au/MeOx CatalystsuA Matter of the Support2012In: ChemCatChem, ISSN 1867-3880, E-ISSN 1867-3899, Vol. 4, no 1, p. 59-63Article in journal (Refereed)
  • 48. Manyar, Haresh G.
    et al.
    Morgan, Richard
    Morgan, Kevin
    Yang, Bo
    Hu, P.
    Szlachetko, Jakub
    Sa, Jacinto
    Hardacre, Christopher
    High energy resolution fluorescence detection XANES - an in situ method to study the interaction of adsorbed molecules with metal catalysts in the liquid phase2013In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 3, no 6, p. 1497-1500Article in journal (Refereed)
  • 49.
    Meier de Andrade, Ageo
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Kullgren, Jolla
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Broqvist, Peter
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Insights into reactive nanoparticles2018Conference paper (Other academic)
  • 50.
    Meier de Andrade, Ageo
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Kullgren, Jolla
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Structural Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sá, Jacinto
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Broqvist, Peter
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Insights into reactive nanoparticles2019Conference paper (Other academic)
123 1 - 50 of 112
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