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  • 1.
    Boily, Jean-Francois
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Song, Xiaowei
    Direct identification of reaction sites on ferrihydrite2020In: Communications Chemistry, E-ISSN 2399-3669, Vol. 3, no 1, article id 79Article in journal (Refereed)
    Abstract [en]

    Hydroxyl groups are the cornerstone species driving catalytic reactions on mineral nanoparticles of Earth's crust, water, and atmosphere. Here we directly identify populations of these groups on ferrihydrite, a key yet misunderstood iron oxyhydroxide nanomineral in natural sciences. This is achieved by resolving an enigmatic set of vibrational spectroscopic signatures of reactive hydroxo groups and chemisorbed water molecules embedded in specific chemical environments. We assist these findings by exploring a vast array of configurations of computer-generated nanoparticles. We find that these groups are mainly disposed along rows at edges of sheets of iron octahedra. Molecular dynamics of nanoparticles as large as 10 nm show that the most reactive surface hydroxo groups are predominantly free, yet are hydrogen bond acceptors in an intricate network formed with less reactive groups. The resolved vibrational spectroscopic signatures open new possibilities for tracking catalytic reactions on ferrihydrite, directly from the unique viewpoint of its reactive hydroxyl groups. Ferrihydrite nanoparticles have many hydroxyl sites which can react with environmental contaminants and nutrients, but the surface structure of this common mineral is still not fully understood. Here, a combination of vibrational spectroscopy and molecular simulations identify hydroxyl groups exposed along rows at the edges of sheets of iron octahedra.

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  • 2.
    Deiana, Marco
    et al.
    Umeå University, Faculty of Medicine, Department of Medical Biochemistry and Biophysics.
    Josse, Pierre
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France.
    Dalinot, Clément
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France.
    Osmolovskyi, Artem
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France.
    Marqués, Pablo Simón
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France.
    Castán, José María Andrés
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France.
    Abad Galán, Laura
    Univ Lyon, ENS de Lyon, CNRS UMR 5182, Université Claude Bernard Lyon 1, Lyon, France.
    Allain, Magali
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France.
    Khrouz, Lhoussain
    Univ Lyon, ENS de Lyon, CNRS UMR 5182, Université Claude Bernard Lyon 1, Lyon, France.
    Maury, Olivier
    Univ Lyon, ENS de Lyon, CNRS UMR 5182, Université Claude Bernard Lyon 1, Lyon, France.
    Le Bahers, Tangui
    Univ Lyon, ENS de Lyon, CNRS UMR 5182, Université Claude Bernard Lyon 1, Lyon, France.
    Blanchard, Philippe
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France.
    Dabos-Seignon, Sylvie
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France.
    Monnereau, Cyrille
    Univ Lyon, ENS de Lyon, CNRS UMR 5182, Université Claude Bernard Lyon 1, Lyon, France.
    Sabouri, Nasim
    Umeå University, Faculty of Medicine, Department of Medical Biochemistry and Biophysics.
    Cabanetos, Clément
    Univ Angers, CNRS, MOLTECH-ANJOU, SFR MATRIX, Angers, France; IRL CNRS 2002, 2BFUEL, CNRS -Yonsei University, Seoul, South Korea.
    Site-selected thionated benzothioxanthene chromophores as heavy-atom-free small-molecule photosensitizers for photodynamic therapy2022In: Communications Chemistry, E-ISSN 2399-3669, Vol. 5, article id 142Article in journal (Refereed)
    Abstract [en]

    Photodynamic therapy is a clinically approved anticancer modality that employs a light-activated agent (photosensitizer) to generate cytotoxic reactive oxygen species (ROS). There is therefore a growing interest for developing innovative photosensitizing agents with enhanced phototherapeutic performances. Herein, we report on a rational design synthetic procedure that converts the ultrabright benzothioxanthene imide (BTI) dye into three heavy-atom-free thionated compounds featuring close-to-unit singlet oxygen quantum yields. In contrast to the BTI, these thionated analogs display an almost fully quenched fluorescence emission, in agreement with the formation of highly populated triplet states. Indeed, the sequential thionation on the BTI scaffold induces torsion of its skeleton reducing the singlet-triplet energy gaps and enhancing the spin-orbit coupling. These potential PSs show potent cancer-cell ablation under light irradiation while remaining non-toxic under dark condition owing to a photo-cytotoxic mechanism that we believe simultaneously involves singlet oxygen and superoxide species, which could be both characterized in vitro. Our study demonstrates that this simple site-selected thionated platform is an effective strategy to convert conventional carbonyl-containing fluorophores into phototherapeutic agents for anticancer PDT.

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  • 3.
    El Omari, Kamel
    et al.
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom; Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom.
    Duman, Ramona
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom; Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom.
    Mykhaylyk, Vitaliy
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom; Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom.
    Orr, Christian M.
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom; Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom.
    Latimer-Smith, Merlyn
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom.
    Winter, Graeme
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom.
    Grama, Vinay
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom.
    Qu, Feng
    Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom; Department of Life Sciences, Imperial College London, London, United Kingdom; Department of Biochemistry, University of Oxford, Oxford, United Kingdom.
    Bountra, Kiran
    Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom; Department of Life Sciences, Imperial College London, London, United Kingdom.
    Kwong, Hok Sau
    Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom; Department of Life Sciences, Imperial College London, London, United Kingdom.
    Romano, Maria
    Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom; Department of Life Sciences, Imperial College London, London, United Kingdom; Institute of Biostructures and Bioimaging, IBB, CNR, Naples, Italy; Department of Pharmacy, University of Naples “Federico II”, Naples, Italy.
    Reis, Rosana I.
    National Physical Laboratory, Hampton Road, Teddington, United Kingdom.
    Vogeley, Lutz
    Charles River Discovery Research Services UK, Chesterford Research Park, Saffron Walden, United Kingdom; Max Planck Institute of Molecular Cell Biology and Genetics (MPI-CBG), Dresden, Germany.
    Vecchia, Luca
    Division of Structural Biology, Wellcome Centre for Human Genetics, University of Oxford, Oxford, United Kingdom; Friedrich Miescher Institute for Biomedical Research, Basel, Switzerland.
    Owen, C. David
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom; Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom.
    Wittmann, Sina
    Department of Biochemistry, University of Oxford, Oxford, United Kingdom; Institute of Molecular Biology (IMB), Ackermannweg 4, Mainz, Germany.
    Renner, Max
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Division of Structural Biology, Wellcome Centre for Human Genetics, University of Oxford, Oxford, United Kingdom.
    Senda, Miki
    Structural Biology Research Center, Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK), Ibaraki, Tsukuba, Japan.
    Matsugaki, Naohiro
    Structural Biology Research Center, Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK), Ibaraki, Tsukuba, Japan; Department of Materials Structure Science, School of High Energy Accelerator Science, The Graduate University of Advanced Studies (Soken-dai), 1-1 Oho, Ibaraki, Tsukuba, Japan.
    Kawano, Yoshiaki
    Advanced Photon Technology Division, RIKEN SPring-8 Center, Hyogo, Japan.
    Bowden, Thomas A.
    Division of Structural Biology, Wellcome Centre for Human Genetics, University of Oxford, Oxford, United Kingdom.
    Moraes, Isabel
    National Physical Laboratory, Hampton Road, Teddington, United Kingdom.
    Grimes, Jonathan M.
    Division of Structural Biology, Wellcome Centre for Human Genetics, University of Oxford, Oxford, United Kingdom.
    Mancini, Erika J.
    School of Life Sciences, University of Sussex, Falmer, Brighton, United Kingdom.
    Walsh, Martin A.
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom; Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom.
    Guzzo, Cristiane R.
    Department of Microbiology, Institute of Biomedical Sciences, University of São Paulo, São Paulo, Brazil.
    Owens, Raymond J.
    Division of Structural Biology, Wellcome Centre for Human Genetics, University of Oxford, Oxford, United Kingdom; The Rosalind Franklin Institute, Harwell Campus, Oxford, United Kingdom.
    Jones, E. Yvonne
    Division of Structural Biology, Wellcome Centre for Human Genetics, University of Oxford, Oxford, United Kingdom.
    Brown, David G.
    Charles River Discovery Research Services UK, Chesterford Research Park, Saffron Walden, United Kingdom.
    Stuart, Dave I.
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom; Division of Structural Biology, Wellcome Centre for Human Genetics, University of Oxford, Oxford, United Kingdom.
    Beis, Konstantinos
    Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom; Department of Life Sciences, Imperial College London, London, United Kingdom.
    Wagner, Armin
    Diamond Light Source, Harwell Science and Innovation Campus, United Kingdom; Research Complex at Harwell, Rutherford Appleton Laboratory, Didcot, United Kingdom.
    Experimental phasing opportunities for macromolecular crystallography at very long wavelengths2023In: Communications Chemistry, E-ISSN 2399-3669, Vol. 6, no 1, article id 219Article in journal (Refereed)
    Abstract [en]

    Despite recent advances in cryo-electron microscopy and artificial intelligence-based model predictions, a significant fraction of structure determinations by macromolecular crystallography still requires experimental phasing, usually by means of single-wavelength anomalous diffraction (SAD) techniques. Most synchrotron beamlines provide highly brilliant beams of X-rays of between 0.7 and 2 Å wavelength. Use of longer wavelengths to access the absorption edges of biologically important lighter atoms such as calcium, potassium, chlorine, sulfur and phosphorus for native-SAD phasing is attractive but technically highly challenging. The long-wavelength beamline I23 at Diamond Light Source overcomes these limitations and extends the accessible wavelength range to λ = 5.9 Å. Here we report 22 macromolecular structures solved in this extended wavelength range, using anomalous scattering from a range of elements which demonstrate the routine feasibility of lighter atom phasing. We suggest that, in light of its advantages, long-wavelength crystallography is a compelling option for experimental phasing.

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  • 4.
    Haziri, Veton
    et al.
    Department of Chemistry, University of Prishtina, Prishtina, Serbia.
    Nha, Tu Pham Tran
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Berisha, Avni
    Department of Chemistry, University of Prishtina, Prishtina, Serbia.
    Boily, Jean-Francois
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    A gateway for ion transport on gas bubbles pinned onto solids2021In: Communications Chemistry, E-ISSN 2399-3669, Vol. 4, no 1, article id 43Article in journal (Refereed)
    Abstract [en]

    Gas bubbles grown on solids are more than simple vehicles for gas transport. They are charged particles with surfaces populated with exchangeable ions. We here unveil a gateway for alkali metal ion transport between oxygen bubbles and semi-conducting (iron oxide) and conducting (gold) surfaces. This gateway was identified by electrochemical impedance spectroscopy using an ultramicroelectrode in direct contact with bubbles pinned onto these solid surfaces. We show that this gateway is naturally present at open circuit potentials, and that negative electric potentials applied through the solid enhance ion transport. In contrast, positive potentials or contact with an insulator (polytetrafluoroethylene) attenuates transport. We propose that this gateway is generated by overlapping electric double layers of bubbles and surfaces of contrasting (electro)chemical potentials. Knowledge of this ion transfer phenomenon is essential for understanding electric shielding and reaction overpotential caused by bubbles on catalysts. This has especially important ramifications for predicting processes including mineral flotation, microfluidics, pore water geochemistry, and fuel cell technology.

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1 - 4 of 4
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