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  • 1. Achenbach, Bastian
    et al.
    Svensson Grape, Erik
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Wahiduzzaman, Mohammad
    Pappler, Sandra K.
    Meinhart, Marcel
    Siegel, Renée
    Maurin, Guillaume
    Senker, Jürgen
    Inge, A. Ken
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Stock, Norbert
    Porous Salts Containing Cationic Al24-Hydroxide-Acetate Clusters from Scalable, Green and Aqueous Synthesis Routes2023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 29, article id e202218679Article in journal (Refereed)
    Abstract [en]

    The solution chemistry of aluminum is highly complex and various polyoxocations are known. Here we report on the facile synthesis of a cationic Al24 cluster that forms porous salts of composition [Al24(OH)56(CH3COO)12]X4, denoted CAU-55-X, with X=Cl, Br, I, HSO4. Three-dimensional electron diffraction was employed to determine the crystal structures. Various robust and mild synthesis routes for the chloride salt [Al24(OH)56(CH3COO)12]Cl4 in water were established resulting in high yields (>95 %, 215 g per batch) within minutes. Specific surface areas and H2O capacities with maximum values of up to 930 m2 g−1 and 430 mg g−1 are observed. The particle size of CAU-55-X can be tuned between 140 nm and 1250 nm, permitting its synthesis as stable dispersions or as highly crystalline powders. The positive surface charge of the particles, allow fast and effective adsorption of anionic dye molecules and adsorption of poly- and perfluoroalkyl substances (PFAS). 

  • 2. Afshar, Majid Ghahraman
    et al.
    Crespo, Gaston A.
    Bakker, Eric
    Thin-Layer Chemical Modulations by a Combined Selective Proton Pump and pH Probe for Direct Alkalinity Detection2015In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 54, no 28, p. 8110-8113Article in journal (Refereed)
  • 3.
    Agarwala, Hemlata
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Synthetic Molecular Chemistry. Tech Univ Munich TUM, Campus Straubing Biotechnol & Sustainabil,Uferstr, D-94315 Straubing, Germany..
    Chen, Xiaoyu
    KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth CBH, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden..
    Lyonnet, Julien R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Barcelona Inst Sci & Technol, Inst Chem Res Catalonia ICIQ, Tarragona 43007, Spain..
    Johnson, Ben A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Tech Univ Munich TUM, Campus Straubing Biotechnol & Sustainabil,Uferstr, D-94315 Straubing, Germany..
    Ahlquist, Marten
    KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth CBH, Dept Theoret Chem & Biol, S-10691 Stockholm, Sweden..
    Ott, Sascha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Alternating Metal-Ligand Coordination Improves Electrocatalytic CO2 Reduction by a Mononuclear Ru Catalyst2023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 17Article in journal (Refereed)
    Abstract [en]

    Molecular electrocatalysts for CO2-to-CO conversion often operate at large overpotentials, due to the large barrier for C-O bond cleavage. Illustrated with ruthenium polypyridyl catalysts, we herein propose a mechanistic route that involves one metal center that acts as both Lewis base and Lewis acid at different stages of the catalytic cycle, by density functional theory in corroboration with experimental FTIR. The nucleophilic character of the Ru center manifests itself in the initial attack on CO2 to form [Ru-CO2](0), while its electrophilic character allows for the formation of a 5-membered metallacyclic intermediate, [Ru-CO2CO2](0,c), by addition of a second CO2 molecule and intramolecular cyclization. The calculated activation barrier for C-O bond cleavage via the metallacycle is decreased by 34.9 kcal mol(-1) as compared to the non-cyclic adduct in the two electron reduced state of complex 1. Such metallacyclic intermediates in electrocatalytic CO2 reduction offer a new design feature that can be implemented consciously in future catalyst designs.

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  • 4.
    Agarwala, Hemlata
    et al.
    Department of Chemistry - Ångström Laboratories, Uppsala University Box 523, 75120, Uppsala, Sweden; Present address: Technical University of Munich (TUM), Campus Straubing for Biotechnology and Sustainability, Uferstraße 53, 94315, Straubing, Germany.
    Chen, Xiaoyu
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Theoretical Chemistry and Biology.
    Lyonnet, Julien R.
    Department of Chemistry - Ångström Laboratories, Uppsala University Box 523, 75120, Uppsala, Sweden; Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Tarragona, 43007, Spain.
    Johnson, Ben A.
    Department of Chemistry - Ångström Laboratories, Uppsala University Box 523, 75120, Uppsala, Sweden; Present address: Technical University of Munich (TUM), Campus Straubing for Biotechnology and Sustainability, Uferstraße 53, 94315, Straubing, Germany.
    Ahlquist, Mårten S. G.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Theoretical Chemistry and Biology.
    Ott, Sascha
    Department of Chemistry - Ångström Laboratories, Uppsala University Box 523, 75120, Uppsala, Sweden.
    Alternating Metal-Ligand Coordination Improves Electrocatalytic CO2 Reduction by a Mononuclear Ru Catalyst**2023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 17, article id e202218728Article in journal (Refereed)
    Abstract [en]

    Molecular electrocatalysts for CO2-to-CO conversion often operate at large overpotentials, due to the large barrier for C−O bond cleavage. Illustrated with ruthenium polypyridyl catalysts, we herein propose a mechanistic route that involves one metal center that acts as both Lewis base and Lewis acid at different stages of the catalytic cycle, by density functional theory in corroboration with experimental FTIR. The nucleophilic character of the Ru center manifests itself in the initial attack on CO2 to form [Ru-CO2]0, while its electrophilic character allows for the formation of a 5-membered metallacyclic intermediate, [Ru-CO2CO2]0,c, by addition of a second CO2 molecule and intramolecular cyclization. The calculated activation barrier for C−O bond cleavage via the metallacycle is decreased by 34.9 kcal mol−1 as compared to the non-cyclic adduct in the two electron reduced state of complex 1. Such metallacyclic intermediates in electrocatalytic CO2 reduction offer a new design feature that can be implemented consciously in future catalyst designs.

  • 5.
    Aggarwal, Varinder K.
    et al.
    Bristol University.
    Olofsson, Berit
    Stockholm University, Faculty of Science, Department of Organic Chemistry. University of Bristol, Bristol, UK.
    Enantioselective α-arylation of cyclohexanones with diaryl iodonium salts: Application to the synthesis of (-)-epibatidine.2005In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 44, no 34, p. 5516-5519Article in journal (Refereed)
    Abstract [en]

    The direct asym. α-arylation of prochiral ketones has been effected using chiral lithium amide bases and diaryl iodonium salts. The methodol. has been employed in a short total synthesis of the alkaloid (-)-epibatidine. [on SciFinder(R)]

  • 6.
    Agosta, Lorenzo
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Arismendi-Arrieta, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Dzugutov, Mikhail
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Hermansson, Kersti
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Origin of the Hydrophobic Behaviour of Hydrophilic CeO22023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 35, article id e202303910Article in journal (Refereed)
    Abstract [en]

    The nature of the hydrophobicity found in rare-earth oxides is intriguing. The CeO2 (100) surface, despite its strongly hydrophilic nature, exhibits hydrophobic behaviour when immersed in water. In order to understand this puzzling and counter-intuitive effect we performed a detailed analysis of the water structure and dynamics. We report here an ab-initio molecular dynamics simulation (AIMD) study which demonstrates that the first water layer, in immediate contact with the hydroxylated CeO2 surface, is responsible for the effect behaving as a hydrophobic interface with respect to the rest of the liquid water. The hydrophobicity is manifested in several ways: a considerable diffusion enhancement of the confined liquid water as compared with bulk water at the same thermodynamic condition, a weak adhesion energy and few H-bonds above the hydrophobic water layer, which may also sustain a water droplet. These findings introduce a new concept in water/rare-earth oxide interfaces: hydrophobicity mediated by specific water patterns on a hydrophilic surface.

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  • 7.
    Ahlquist, Mårten
    et al.
    KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.
    Norrby, Per-Ola
    Department of Chemistry, University of Gothenburg, Sweden.
    Dispersion and Back-Donation Gives Tetracoordinate [Pd(PPh3)4]2011In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 50, no 49, p. 11794-11797Article in journal (Refereed)
    Abstract [en]

    18e R.I.P. The apparent compliance of [Pd(PPh3)4] ("tetrakis") with the 18-electron rule is not due to an electronic preference on the central metal. Pd is valence-saturated already by two ligands. Further ligand addition gives a minor energy gain, and is only possible due to strong back-bonding. Dispersion corrections are needed for properly describing the interactions between the ligands.

  • 8.
    Ahlsten, Nanna
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Bermejo Gomez, Antonio
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Martin-Matute, Belen
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Iridium-Catalyzed 1,3-Hydrogen Shift/Chlorination of Allylic Alcohols2013In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 52, no 24, p. 6273-6276Article in journal (Refereed)
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  • 9.
    Aili, Daniel
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Sensor Science and Molecular Physics . Linköping University, The Institute of Technology.
    Tai, Feng-I
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, The Institute of Technology.
    Enander, Karin
    Linköping University, Department of Physics, Chemistry and Biology, Sensor Science and Molecular Physics . Linköping University, The Institute of Technology.
    Baltzer, Lars
    Department of Biochemistry andOrganic Chemistry Uppsala University, BMC, Box 576, 75123 Uppsala, Sweden.
    Liedberg, Bo
    Linköping University, Department of Physics, Chemistry and Biology, Sensor Science and Molecular Physics . Linköping University, The Institute of Technology.
    Self-Assembly of Fibers and Nanorings from Disulfide-Linked Helix–Loop–Helix Polypeptides2008In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 47, no 30, p. 5554-5556Article in journal (Refereed)
  • 10. Aili, Daniel
    et al.
    Tai, Feng-I
    Enander, Karin
    Baltzer, Lars
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Biochemistry and Organic Chemistry.
    Liedberg, Bo
    Self-assembly of fibers and nanorings from disulfide-linked helix-loop-helix polypeptides2008In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 47, no 30, p. 5554-5556Article in journal (Refereed)
  • 11. Akkarasamiyo, Sunisa
    et al.
    Samec, Joseph S. M.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Intermolecular Stereospecific Substitution of Underivatized Enantioenriched Secondary Alcohols by Organocatalysis2019In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 58, no 50, p. 17908-17910Article in journal (Refereed)
    Abstract [en]

    The stereospecific substitution of non-derivatized and non-allylic enantioenriched alcohols with only water as a by-product would enable the use of readily available alcohols as substrates for green and sustainable transformations. However, the poor leaving group ability of the OH group has hampered the development of such a process. Denton and co-workers recently described the use of (2-hydroxybenzyl)diphenylphosphine oxide as a catalyst of a redox-neutral and zero-waste-generating Mitsunobu reaction. This innovative process constitutes the first intermolecular stereospecific substitution of non-allylic alcohols, and might find industrial applications.

  • 12.
    Alam, Rauful
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Diner, Colin
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Jonker, Sybrand
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Eriksson, Lars
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Szabó, Kálmán J.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Catalytic Asymmetric Allylboration of Indoles and Dihydroisoquinolines with Allylboronic Acids: Stereodivergent Synthesis of up to Three Contiguous Stereocenters2016In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 55, no 46, p. 14417-14421Article in journal (Refereed)
    Abstract [en]

    The catalytic asymmetric allylboration of cyclic imines with gamma,gamma-disubstituted allylboronic acids provides products with adjacent stereocenters in high yield and stereoselectivity. Various electrophiles, including 3,4-dihydroisoquinolines and indoles, were prenylated in a fully stereodivergent fashion by switching the E/Z geometry of the allylboronate and/or the enantiomer of the BINOL catalyst. 3-Methylindole provided products with three adjacent stereocenters with high stereoselectivity in one synthetic operation.

  • 13.
    Alamsetti, Santosh Kumar
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Persson, Andreas K. A.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Jiang, Tuo
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Bäckvall, Jan-E.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Scalable Synthesis of Oxazolones from Propargylic Alcohols through Multistep Palladium(II) Catalysis: beta-Selective Oxidative Heck Coupling of Cyclic Sulfonyl Enamides and Aryl Boroxines2013In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 52, no 51, p. 13745-13750Article in journal (Refereed)
  • 14.
    Alsufyani, Maryam
    et al.
    Univ Oxford, England.
    Stoeckel, Marc-Antoine
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Chen, Xingxing
    King Abdullah Univ Sci & Technol KAUST, Saudi Arabia.
    Thorley, Karl
    Univ Kentucky, KY 40506 USA.
    Hallani, Rawad K.
    King Abdullah Univ Sci & Technol KAUST, Saudi Arabia.
    Puttisong, Yuttapoom
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Ji, Xudong
    Northwestern Univ, IL 60208 USA.
    Meli, Dilara
    Northwestern Univ, IL 60208 USA.
    Paulsen, Bryan D.
    Northwestern Univ, IL 60208 USA.
    Strzalka, Joseph
    Argonne Natl Lab, IL 60439 USA.
    Regeta, Khrystyna
    King Abdullah Univ Sci & Technol KAUST, Saudi Arabia.
    Combe, Craig
    King Abdullah Univ Sci & Technol KAUST, Saudi Arabia.
    Chen, Hu
    King Abdullah Univ Sci & Technol KAUST, Saudi Arabia.
    Tian, Junfu
    Univ Oxford, England.
    Rivnay, Jonathan
    Northwestern Univ, IL 60208 USA; Northwestern Univ, IL 60611 USA.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    McCulloch, Iain
    Univ Oxford, England; King Abdullah Univ Sci & Technol KAUST, Saudi Arabia.
    Lactone Backbone Density in Rigid Electron-Deficient Semiconducting Polymers Enabling High n-type Organic Thermoelectric Performance2022In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 61, no 7, article id e202113078Article in journal (Refereed)
    Abstract [en]

    Three lactone-based rigid semiconducting polymers were designed to overcome major limitations in the development of n-type organic thermoelectrics, namely electrical conductivity and air stability. Experimental and theoretical investigations demonstrated that increasing the lactone group density by increasing the benzene content from 0 % benzene (P-0), to 50 % (P-50), and 75 % (P-75) resulted in progressively larger electron affinities (up to 4.37 eV), suggesting a more favorable doping process, when employing (N-DMBI) as the dopant. Larger polaron delocalization was also evident, due to the more planarized conformation, which is proposed to lead to a lower hopping energy barrier. As a consequence, the electrical conductivity increased by three orders of magnitude, to achieve values of up to 12 S cm and Power factors of 13.2 mu Wm(-1) K-2 were thereby enabled. These findings present new insights into material design guidelines for the future development of air stable n-type organic thermoelectrics.

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  • 15.
    Andersen, Thomas L.
    et al.
    Aarhus Univ, Carbon Dioxide Activat Ctr CADIAC, Dept Chem, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark.;Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark..
    Nordeman, Patrik
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Medicinal Chemistry, Division of Molecular Imaging.
    Christoffersen, Heidi F.
    Aarhus Univ, Carbon Dioxide Activat Ctr CADIAC, Dept Chem, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark.;Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark..
    Audrain, Helene
    Aarhus Univ Hosp, Dept Nucl Med, DK-8000 Aarhus, Denmark.;Aarhus Univ Hosp, PET Ctr, DK-8000 Aarhus, Denmark..
    Antoni, Gunnar
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Medicinal Chemistry, Division of Molecular Imaging.
    Skrydstrup, Troels
    Aarhus Univ, Carbon Dioxide Activat Ctr CADIAC, Dept Chem, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark.;Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, Gustav Wieds Vej 14, DK-8000 Aarhus C, Denmark..
    Application of Methyl Bisphosphine-Ligated Palladium Complexes for Low Pressure N-C-11-Acetylation of Peptides2017In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 56, no 16, p. 4549-4553Article in journal (Refereed)
    Abstract [en]

    A mild and effective method is described for C-11-labeling of peptides selectively at the N-terminal nitrogen or at internal lysine positions. The presented method relies on the use of specific biphosphine palladium-methyl complexes and their high reactivity towards amino-carbonylation of amine groups in the presence [C-11] carbon monoxide. The protocol facilitates the production of native N-C-11-acetylated peptides, without any structural modifications and has been applied to a selection of bioactive peptides.

  • 16.
    Andersson, Hans
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Gustafsson, Magnus
    Boström, Dan
    Umeå University, Faculty of Science and Technology, Department of Applied Physics and Electronics.
    Olsson, Roger
    Almqvist, Fredrik
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    The Regio- and Stereoselective Synthesis of trans-2,3-Dihydropyridine N-oxides and Piperidines2009In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 48, no 18, p. 3288-3291Article in journal (Refereed)
    Abstract [en]

    No Abstract

  • 17. Andrews, Lester
    et al.
    Wang, Xuefeng
    Lindh, Roland
    Department of Theoretical Chemistry, Lund University.
    Roos, Bjoern O
    Marsden, Colin J.
    Simple N UF3 and P UF3 molecules with triple bonds to uranium2008In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 47, no 29, p. 5366-5370Article in journal (Refereed)
  • 18.
    Antoni, Per
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Hed, Yvonne
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Nordberg, Axel
    KTH, School of Technology and Health (STH), Neuronic Engineering.
    Nyström, Daniel
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    von Holst, Hans
    KTH, School of Technology and Health (STH), Neuronic Engineering.
    Hult, Anders
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Malkoch, Michael
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Bifunctional Dendrimers: From Robust Synthesis and Accelerated One-Pot Postfunctionalization Strategy to Potential Applications2009In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 48, no 12, p. 2126-2130Article in journal (Refereed)
  • 19.
    Antzutkin, Oleg
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Sustainable Process Engineering.
    Iuga, Dino
    Department of Physics, Warwick University, Coventry.
    Filippov, Andrei
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Sustainable Process Engineering.
    Kelly, Robert T.
    Department of Physics, Warwick University, Coventry.
    Becker-Baldus, Johanna
    Department of Physics, Warwick University, Coventry.
    Brown, Steven P.
    Department of Physics, Warwick University, Coventry.
    Dupree, Ray
    Department of Physics, Warwick University, Coventry.
    Hydrogen bonding in Alzheimer’s amyloid-β fibrils probed by 15N{17O} REAPDOR solid-state NMR spectroscopy2012In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 51, no 41, p. 10289-10292Article in journal (Refereed)
    Abstract [en]

    An exclusive label: 15N{17O} REAPDOR NMR was used to validate intermolecular C17O⋅⋅⋅H15N hydrogen bonding in Ac-Aβ(16–22)-NH2 (see scheme) and Aβ(11–25) amyloid fibrils, which are associated with Alzheimer’s disease, by selectively labeling them with 17O and 15N. This method was effective for confirming the structure of these fibrils, and could be useful for a number of other biological samples.

  • 20.
    Arkhypchuk, Anna I.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Santoni, Marie-Pierre
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Ott, Sascha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Cascade Reactions Forming Highly Substituted, Conjugated Phospholes and 1,2-Oxaphospholes2012In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 51, no 31, p. 7776-7780Article in journal (Refereed)
    Abstract [en]

    The reaction of a phospha-Wittig–Horner reagent with diacetylenic ketones (see scheme) results in a cascade of reactions that can lead to both an oxaphosphole-terminated cumulene system and an alkene-bridged bis-phosphole. The reaction outcome is determined by the nature of the acetylene termini, with phenyl groups stabilizing a carbene intermediate that dimerizes to give the bis-phosphole product.

  • 21.
    Arkhypchuk, Anna
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Svyaschenko, Yurii
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Orthaber, Andreas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Ott, Sascha
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Mechanism of the Phospha-Wittig-Horner Reaction2013In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 52, no 25, p. 6484-6487Article in journal (Refereed)
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  • 22.
    Aslandukov, Andrey
    et al.
    Univ Bayreuth, Germany.
    Jurzick, Pascal L.
    Univ Cologne, Germany.
    Bykov, Maxim
    Univ Cologne, Germany.
    Aslandukova, Alena
    Univ Bayreuth, Germany.
    Chanyshev, Artem
    Univ Bayreuth, Germany.
    Laniel, Dominique
    Univ Edinburgh, Scotland; Univ Edinburgh, Scotland.
    Yin, Yuqing
    Univ Bayreuth, Germany.
    Akbar, Fariia I.
    Univ Bayreuth, Germany.
    Khandarkhaeva, Saiana
    Univ Bayreuth, Germany.
    Fedotenko, Timofey
    Deutsch Elektronen Synchrotron DESY, Germany.
    Glazyrin, Konstantin
    Deutsch Elektronen Synchrotron DESY, Germany.
    Chariton, Stella
    Univ Chicago, IL 60637 USA.
    Prakapenka, Vitali
    Univ Chicago, IL 60637 USA.
    Wilhelm, Fabrice
    European Synchrotron Radiat Facil, France.
    Rogalev, Andrei
    European Synchrotron Radiat Facil, France.
    Comboni, Davide
    European Synchrotron Radiat Facil, France.
    Hanfland, Michael
    European Synchrotron Radiat Facil, France.
    Doubrovinckaia, Natalia
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering. Univ Bayreuth, Germany.
    Dubrovinsky, Leonid
    Univ Bayreuth, Germany.
    Stabilization Of The CN35− Anion In Recoverable High-pressure Ln3O2(CN3) (Ln=La, Eu, Gd, Tb, Ho, Yb) Oxoguanidinates2023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773Article in journal (Refereed)
    Abstract [en]

    A series of isostructural Ln(3)O(2)(CN3) (Ln=La, Eu, Gd, Tb, Ho, Yb) oxoguanidinates was synthesized under high-pressure (25-54 GPa) high-temperature (2000-3000 K) conditions in laser-heated diamond anvil cells. The crystal structure of this novel class of compounds was determined via synchrotron single-crystal X-ray diffraction (SCXRD) as well as corroborated by X-ray absorption near edge structure (XANES) measurements and density functional theory (DFT) calculations. The Ln(3)O(2)(CN3) solids are composed of the hitherto unknown CN35- guanidinate anion-deprotonated guanidine. Changes in unit cell volumes and compressibility of Ln(3)O(2)(CN3) (Ln=La, Eu, Gd, Tb, Ho, Yb) compounds are found to be dictated by the lanthanide contraction phenomenon. Decompression experiments show that Ln(3)O(2)(CN3) compounds are recoverable to ambient conditions. The stabilization of the CN35- guanidinate anion at ambient conditions provides new opportunities in inorganic and organic synthetic chemistry.

  • 23.
    Aslandukov, Andrey
    et al.
    University of Bayreuth: Universitat Bayreuth Laboratory of Crystallography, Bayreuth, GERMANY.
    Trybel, Florian
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Aslandukova, Alena
    University of Bayreuth: Universitat Bayreuth Bayerisches Geoinstitut, GERMANY.
    Laniel, Dominique
    The University of Edinburgh Centre for Science at Extreme Conditions and School of Physics and Astronomy, UNITED KINGDOM.
    Fedotenko, Timofey
    DESY: Deutsches Elektronen-Synchrotron Photon Science, Deutsches Elektronen-Synchrotron, GERMANY.
    Khandarkhaeva, Saiana
    University of Bayreuth: Universitat Bayreuth Material Physics and Technology at Extreme Conditions, Laboratory of Crystallography, GERMANY.
    Aprilis, Georgios
    ESRF European Synchrotron Radiation Facility, FRANCE.
    Giacobbe, Carlotta
    ESRF European Synchrotron Radiation Facility, FRANCE.
    Lawrence Bright, Eleanor
    ESRF European Synchrotron Radiation Facility, FRANCE.
    Abrikosov, Igor A.
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Dubrovinsky, Leonid
    University of Bayreuth: Universitat Bayreuth Bayerisches Geoinstitut, GERMANY.
    Dubrovinskaia, Natalia
    University of Bayreuth: Universitat Bayreuth Material Physics and Technology at Extreme Conditions, Laboratory of Crystallography, GERMANY.
    Anionic N18 Macrocycles and a Polynitrogen Double Helix in Novel Yttrium Polynitrides YN6 and Y2N11 at 100 GPa2022In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 61, no 34, article id e202207469Article in journal (Refereed)
    Abstract [en]

    Two novel yttrium nitrides, YN6 and Y2N11, were synthesized by direct reaction between yttrium and nitrogen at 100 GPa and 3000 K in a laser-heated diamond anvil cell. High-pressure synchrotron single-crystal X-ray diffraction revealed that the crystal structures of YN6 and Y2N11 feature a unique organization of nitrogen atoms-a previously unknown anionic N-18 macrocycle and a polynitrogen double helix, respectively. Density functional theory calculations, confirming the dynamical stability of the YN6 and Y2N11 compounds, show an anion-driven metallicity, explaining the unusual bond orders in the polynitrogen units. As the charge state of the polynitrogen double helix in Y2N11 is different from that previously found in Hf2N11 and because N-18 macrocycles have never been predicted or observed, their discovery significantly extends the chemistry of polynitrides.

  • 24. Baber, Ashleigh E.
    et al.
    Yang, Xiaofang
    Kim, Hyun You
    Mudiyanselage, Kumudu
    Soldemo, Markus
    KTH.
    Weissenrieder, Jonas
    KTH.
    Senanayake, Sanjaya D.
    Al-Mahboob, Abdullah
    Sadowski, Jerzy T.
    Evans, Jaime
    Rodriguez, Jose A.
    Liu, Ping
    Hoffmann, Friedrich M.
    Chen, Jingguang G.
    Stacchiola, Dario J.
    Stabilization of Catalytically Active Cu plus Surface Sites on TitaniumCopper Mixed-Oxide Films**2014In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 53, no 21, p. 5336-5340Article in journal (Refereed)
    Abstract [en]

    The oxidation of CO is the archetypal heterogeneous catalytic reaction and plays a central role in the advancement of fundamental studies, the control of automobile emissions, and industrial oxidation reactions. Copper-based catalysts were the first catalysts that were reported to enable the oxidation of CO at room temperature, but a lack of stability at the elevated reaction temperatures that are used in automobile catalytic converters, in particular the loss of the most reactive Cu+ cations, leads to their deactivation. Using a combined experimental and theoretical approach, it is shown how the incorporation of titanium cations in a Cu2O film leads to the formation of a stable mixed-metal oxide with a Cu+ terminated surface that is highly active for CO oxidation.

  • 25. Baber, Ashleigh E.
    et al.
    Yang, Xiaofang
    Kim, Hyun You
    Mudiyanselage, Kumudu
    Soldemo, Markus
    KTH, School of Information and Communication Technology (ICT), Materials- and Nano Physics, Material Physics, MF.
    Weissenrieder, Jonas
    KTH, School of Information and Communication Technology (ICT), Materials- and Nano Physics, Material Physics, MF.
    Senanayake, Sanjaya D.
    Al-Mahboob, Abdullah
    Sadowski, Jerzy T.
    Evans, Jaime
    Rodriguez, Jose A.
    Liu, Ping
    Hoffmann, Friedrich M.
    Chen, Jingguang G.
    Stacchiola, Dario J.
    Stabilization of Catalytically Active Cu plus Surface Sites on TitaniumCopper Mixed-Oxide Films**2014In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 53, no 21, p. 5336-5340Article in journal (Refereed)
    Abstract [en]

    The oxidation of CO is the archetypal heterogeneous catalytic reaction and plays a central role in the advancement of fundamental studies, the control of automobile emissions, and industrial oxidation reactions. Copper-based catalysts were the first catalysts that were reported to enable the oxidation of CO at room temperature, but a lack of stability at the elevated reaction temperatures that are used in automobile catalytic converters, in particular the loss of the most reactive Cu+ cations, leads to their deactivation. Using a combined experimental and theoretical approach, it is shown how the incorporation of titanium cations in a Cu2O film leads to the formation of a stable mixed-metal oxide with a Cu+ terminated surface that is highly active for CO oxidation.

  • 26. Bach, Anders
    et al.
    Chi, Celestine N.
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Medicine, Department of Medical Biochemistry and Microbiology.
    Pang, Gar F.
    Olsen, Lars
    Kristensen, Anders S.
    Jemth, Per
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Medicine, Department of Medical Biochemistry and Microbiology.
    Strømgaard, Kristian
    Design and synthesis of highly potent and plasma-stable dimeric inhibitors of the PSD-95-NMDA receptor interaction2009In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 48, no 51, p. 9685-9689Article in journal (Refereed)
    Abstract [en]

    On the double: Dimerization of monomeric peptide ligands towards the PDZ domains of the protein PSD-95 (postsynaptic density 95) leads to potent inhibitors of protein-protein interactions with stability in blood plasma. Optimization of the length of the polyethylene glycol linker results in unprecedented affinity for inhibitors of the PDZ1-2 domain.

  • 27. Bae, Juna
    et al.
    Cichocka, Magdalena O.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Zhang, Yi
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Bacsik, Zoltan
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Bals, Sara
    Zou, Xiaodong
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Willhammar, Tom
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Hong, Suk Bong
    Phase Transformation Behavior of a Two-Dimensional Zeolite2019In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 58, no 30, p. 10230-10235Article in journal (Refereed)
    Abstract [en]

    Understanding the molecular-level mechanisms of phase transformation in solids is of fundamental interest for functional materials such as zeolites. Two-dimensional (2D) zeolites, when used as shape-selective catalysts, can offer improved access to the catalytically active sites and a shortened diffusion length in comparison with their 3D analogues. However, few materials are known to maintain both their intralayer microporosity and structure during calcination for organic structure-directing agent (SDA) removal. Herein we report that PST-9, a new 2D zeolite which has been synthesized via the multiple inorganic cation approach and fulfills the requirements for true layered zeolites, can be transformed into the small-pore zeolite EU-12 under its crystallization conditions through the single-layer folding process, but not through the traditional dissolution/recrystallization route. We also show that zeolite crystal growth pathway can differ according to the type of organic SDAs employed.

  • 28. Bai, Licheng
    et al.
    Wang, Xin
    Chen, Qiang
    Ye, Yifan
    Zheng, Haoquan
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Guo, Jinghua
    Yin, Yadong
    Gao, Chuanbo
    Explaining the Size Dependence in Platinum-Nanoparticle-Catalyzed Hydrogenation Reactions2016In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 55, no 50, p. 15656-15661Article in journal (Refereed)
    Abstract [en]

    Hydrogenation reactions are industrially important reactions that typically require unfavorably high H-2 pressure and temperature for many functional groups. Herein we reveal surprisingly strong size-dependent activity of Pt nanoparticles (PtNPs) in catalyzing this reaction. Based on unambiguous spectral analyses, the size effect has been rationalized by the size-dependent d-band electron structure of the PtNPs. This understanding enables production of a catalyst with size of 1.2 nm, which shows a sixfold increase in turnover frequency and 28-fold increase in mass activity in the regioselective hydrogenation of quinoline, compared with PtNPs of 5.3 nm, allowing the reaction to proceed under ambient conditions with unprecedentedly high reaction rates. The size effect and the synthesis strategy developed herein may provide a general methodology in the design of metal-nanoparticle-based catalysts for a broad range of organic syntheses.

  • 29. Bai, Pu
    et al.
    Dong, Zhuoya
    Wang, Shuang
    Wang, Xiangyu
    Li, Yue
    Wang, Yunzheng
    Ma, Yanhang
    Yan, Wenfu
    Zou, Xiaodong
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Yu, Jihong
    A Layered Cationic Aluminum Oxyhydroxide as a Highly Efficient and Selective Trap for Heavy Metal Oxyanions2020In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 59, no 44, p. 19539-19544Article in journal (Refereed)
    Abstract [en]

    Cationic framework materials, especially pure inorganic cationic frameworks that can efficiently and selectively capture harmful heavy metal oxyanions from aqueous solution are highly desired yet scarcely reported. Herein, we report the discovery of a 2D cationic aluminum oxyhydroxide, JU-111, which sets a new benchmark for heavy metal oxyanion sorbents, especially for Cr-VI. Its structure was solved based on 3D electron diffraction tomography data. JU-111 shows fast sorption kinetics (ca. 20 min), high capture capacity (105.4 mg g(-1)), and broad working pH range (3-10) toward Cr(VI)oxyanions. Unlike layered double hydroxides (LDHs), which are poorly selective in the presence of CO32-, JU-111 retains excellent selectivity for Cr(VI)even under a large excess of CO32-. These superior features coupled with the ultra-low cost and environmentally benign nature make JU-111 a promising candidate for toxic metal oxyanion remediation as well as other potential applications.

  • 30.
    Bally, Marta
    et al.
    Chalmers, Sweden .
    Rydell, Gustaf E.
    Institute Curie, France .
    Zahn, Raphael
    University of Zurich, Switzerland Swiss Federal Institute Technology, Switzerland .
    Nasir, Waqas
    University of Gothenburg, Sweden .
    Eggeling, Christian
    Max Planck Institute Biophys Chemistry, Germany .
    Breimer, Michael E.
    University of Gothenburg, Sweden .
    Svensson, Lennart
    Linköping University, Department of Clinical and Experimental Medicine, Molecular Virology. Linköping University, Faculty of Health Sciences.
    Hook, Fredrik
    Chalmers, Sweden .
    Larson, Gran
    University of Gothenburg, Sweden .
    Norovirus GII.4 Virus-like Particles Recognize Galactosylceramides in Domains of Planar Supported Lipid Bilayers2012In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 51, no 48, p. 12020-12024Article in journal (Refereed)
    Abstract [en]

    n/a

  • 31.
    Barragan, Ana
    et al.
    IMDEA Nanosci Inst, Spain.
    Nicolas-Garcia, Tomas
    IMDEA Nanosci Inst, Spain.
    Lauwaet, Koen
    IMDEA Nanosci Inst, Spain.
    Sanchez-Grande, Ana
    IMDEA Nanosci Inst, Spain; Czech Acad Sci, Czech Republic.
    Urgel, Jose I
    IMDEA Nanosci Inst, Spain.
    Björk, Jonas
    Linköping University, Department of Physics, Chemistry and Biology, Materials design. Linköping University, Faculty of Science & Engineering.
    Perez, Emilio M.
    IMDEA Nanosci Inst, Spain.
    Ecija, David
    IMDEA Nanosci Inst, Spain.
    Design and Manipulation of a Minimalistic Hydrocarbon Nanocar on Au(111)2023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 6, article id e202212395Article in journal (Refereed)
    Abstract [en]

    Nanocars are carbon-based single-molecules with a precise design that facilitates their atomic-scale control on a surface. The rational design of these molecules is important in atomic and molecular-scale manipulation to advance the development of molecular machines, as well as for a better understanding of self-assembly, diffusion and desorption processes. Here, we introduce the molecular design and construction of a collection of minimalistic nanocars. They feature an anthracene chassis and four benzene derivatives as wheels. After sublimation and adsorption on an Au(111) surface, we show controlled and fast manipulation of the nanocars along the surface using the tip of a scanning tunneling microscope (STM). The mechanism behind the successful displacement is the induced dipole created over the nanocar by the STM tip. We utilized carbon monoxide functionalized tips both to avoid decomposition and accidentally picking the nanocars up during the manipulation. This strategy allowed thousands of maneuvers to successfully win the Nanocar Race II championship.

  • 32.
    Bartholomeyzik, Teresa
    et al.
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Mazuela, Javier
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Pendrill, Robert
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Deng, Youqian
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Bäckvall, Jan-Erling
    Stockholm University, Faculty of Science, Department of Organic Chemistry.
    Palladium-Catalyzed Oxidative Arylating Carbocyclization of Allenynes: Control of Selectivity and Role of H2O2014In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 53, no 33, p. 8696-8699Article in journal (Refereed)
    Abstract [en]

    Highly selective protocols for the carbocyclization/arylation of allenynes using arylboronic acids are reported. Arylated vinylallenes are obtained with the use of BF3 center dot Et2O as an additive, whereas addition of water leads to arylated trienes. These conditions provide the respective products with excellent selectivities (generally > 97:3) for a range of boronic acids and different allenynes. It has been revealed that water plays a crucial role for the product distribution.

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  • 33. Bassan, A.
    et al.
    Zou, W. B.
    Reyes, E.
    Himo, Fahmi
    KTH, School of Biotechnology (BIO), Theoretical Chemistry.
    Cordova, A.
    The origin of stereoselectivity in primary amino acid catalyzed intermolecular Aldol reactions2005In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 44, no 43, p. 7028-7032Article in journal (Refereed)
  • 34. Beahm, Brendan J
    et al.
    Dehnert, Karen W
    Derr, Nicolas L
    Kuhn, Joachim
    Eberhart, Johann K
    Spillmann, Dorothe
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Medicine, Department of Medical Biochemistry and Microbiology.
    Amacher, Sharon L
    Bertozzi, Carolyn R
    A visualizable chain-terminating inhibitor of glycosaminoglycan biosynthesis in developing zebrafish2014In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 53, no 13, p. 3347-3352Article in journal (Refereed)
    Abstract [en]

    Heparan sulfate (HS) and chondroitin sulfate (CS) glycosaminoglycans (GAG) are proteoglycan-associated polysaccharides with essential functions in animals. They have been studied extensively by genetic manipulation of biosynthetic enzymes, but chemical tools for probing GAG function are limited. HS and CS possess a conserved xylose residue that links the polysaccharide chain to a protein backbone. Here we report that, in zebrafish embryos, the peptide-proximal xylose residue can be metabolically replaced with a chain-terminating 4-azido-4-deoxyxylose (4-XylAz) residue by administration of UDP-4-azido-4-deoxyxylose (UDP-4-XylAz). UDP-4-XylAz disrupted both HS and CS biosynthesis and caused developmental abnormalities reminiscent of GAG biosynthesis and laminin mutants. The azide substituent of protein-bound 4-XylAz allowed for rapid visualization of the organismal sites of chain termination in vivo through bioorthogonal reaction with fluorescent cyclooctyne probes. UDP-4-XylAz therefore complements genetic tools for studies of GAG function in zebrafish embryogenesis.

  • 35.
    Behren, Sandra
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Leibniz-Institut für Analytische Wissenschaften, Dortmund, Germany.
    Yu, Jin
    Leibniz-Institut für Analytische Wissenschaften, Dortmund, Germany; Glycosciences Laboratory, Imperial College London, London, United Kingdom.
    Pett, Christian
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Leibniz-Institut für Analytische Wissenschaften, Dortmund, Germany.
    Schorlemer, Manuel
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Leibniz-Institut für Analytische Wissenschaften, Dortmund, Germany.
    Heine, Viktoria
    Laboratory for Biomaterials, Institute of Biotechnology and Helmholtz-Institute for Biomedical Engineering, RWTH Aachen University, Aachen, Germany.
    Fischöder, Thomas
    Laboratory for Biomaterials, Institute of Biotechnology and Helmholtz-Institute for Biomedical Engineering, RWTH Aachen University, Aachen, Germany.
    Elling, Lothar
    Laboratory for Biomaterials, Institute of Biotechnology and Helmholtz-Institute for Biomedical Engineering, RWTH Aachen University, Aachen, Germany.
    Westerlind, Ulrika
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Leibniz-Institut für Analytische Wissenschaften, Dortmund, Germany.
    Fucose binding motifs on mucin core glycopeptides impact bacterial lectin recognition2023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 62, no 32, article id e202302437Article in journal (Refereed)
    Abstract [en]

    Mucin glycoproteins are essential components of the mucosal barrier, which protects the host from pathogens. Throughout evolution, bacteria have developed strategies to modulate and penetrate this barrier, and cause virulence by interacting with mucin O-glycans at the epithelial cell-surface. O-fucosylated glycan epitopes on mucins are key ligands of many bacterial lectins. Here, a chemoenzymatic synthesis strategy is described to prepare a library of fucosylated mucin core glycopeptides to enable studies of mucin-interacting and fucose-binding bacterial lectins. Glycan cores with biologically important Lewis and H-antigens were prepared decorating the peptide backbone at different sites and densities. The fucosylated mucin glycopeptides were applied in microarray binding studies to explore the importance of glycan core and peptide backbone presentation of these antigens in binding interactions with the P. aeruginosa lectin LecB and the C. difficile toxin A.

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  • 36. Bello-Jurado, Estefanía
    et al.
    Schwalbe-Koda, Daniel
    Nero, Mathias
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Paris, Cecilia
    Uusimäki, Toni
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Román-Leshkov, Yuriy
    Corma, Avelino
    Willhammar, Tom
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Gómez-Bombarelli, Rafael
    Moliner, Manuel
    Tunable CHA/AEI Zeolite Intergrowths with A Priori Biselective Organic Structure-Directing Agents: Controlling Enrichment and Implications for Selective Catalytic Reduction of NOx2022In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 61, no 28, article id e202201837Article in journal (Refereed)
    Abstract [en]

    A novel ab initio methodology based on high-throughput simulations has permitted designing unique biselective organic structure-directing agents (OSDAs) that allow the efficient synthesis of CHA/AEI zeolite intergrowth materials with controlled phase compositions. Distinctive local crystallographic ordering of the CHA/AEI intergrowths was revealed at the nanoscale level using integrated differential phase contrast scanning transmission electron microscopy (iDPC STEM). These novel CHA/AEI materials have been tested for the selective catalytic reduction (SCR) of NOx, presenting an outstanding catalytic performance and hydrothermal stability, even surpassing the performance of the well-established commercial CHA-type catalyst. This methodology opens the possibility for synthetizing new zeolite intergrowths with more complex structures and unique catalytic properties. 

  • 37. Benninger, Richard K. P.
    et al.
    Hofmann, Oliver
    Önfelt, Björn
    Munro, Ian
    Dunsby, Chris
    Davis, Daniel M.
    Neil, Mark A. A.
    French, Paul M. W.
    de Mello, Andrew J.
    Fluorescence-lifetime imaging of DNA-dye interactions within continuous-flow microfluidic systems2007In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 46, no 13, p. 2228-2231Article in journal (Refereed)
  • 38.
    Berg, Lotta
    et al.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Niemiec, Moritz S.
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Qian, Weixing
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Andersson, C. David
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Wittung-Stafshede, Pernilla
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Ekström, Fredrik
    Umeå University, Faculty of Science and Technology, Department of Chemistry. Umeå University, Faculty of Science and Technology, European CBRNE Center.
    Linusson, Anna
    Umeå University, Faculty of Science and Technology, Department of Chemistry.
    Similar but Different: Thermodynamic and Structural Characterization of a Pair of Enantiomers Binding to Acetylcholinesterase2012In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 51, no 51, p. 12716-12720Article in journal (Refereed)
    Abstract [en]

    Take a closer look: Unexpectedly, a pair of enantiomeric ligands proved to have similar binding affinities for acetylcholinesterase. Further studies indicated that the enantiomers exhibit different thermodynamic profiles. Analyses of the noncovalent interactions in the protein-ligand complexes revealed that these differences are partly due to nonclassical hydrogen bonds between the ligands and aromatic side chains of the protein.

  • 39.
    Berglund, Per
    KTH, School of Biotechnology (BIO), Biochemistry.
    Asymmetric Organic Synthesis with Enzymes: Edited by Vicente Gotor, Ignacio Alfonso and Eduardo Garcia-Urdiales2008In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 47, no 35, p. 6514-6515Article, book review (Other academic)
  • 40.
    Bernhardt, Peter
    et al.
    KTH, School of Biotechnology (BIO), Biochemistry.
    Hult, Karl
    KTH, School of Biotechnology (BIO), Biochemistry.
    Kazlauskas, R. J.
    Molecular basis of perhydrolase activity in serine hydrolases2005In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 44, no 18, p. 2742-2746Article in journal (Refereed)
    Abstract [en]

    (Chemical Equation Presented) Changing substrates: A mutation that forms a cis-proline-peptide bond in a loop structure close to the active site of an aryl esterase from Pseudomonas fluorescens converts the enzyme into a perhydrolase (see picture). The switch in activity is explained by a new hydrogen bond formed between a backbone carbonyl oxygen atom and the peroxy deacylation intermediate.

  • 41. Bhagi-Damodaran, Ambika
    et al.
    Kahle, Maximilian
    Stockholm University, Faculty of Science, Department of Biochemistry and Biophysics.
    Shi, Yelu
    Zhang, Yong
    Ädelroth, Pia
    Stockholm University, Faculty of Science, Department of Biochemistry and Biophysics.
    Lu, Yi
    Insights Into How Heme Reduction Potentials Modulate Enzymatic Activities of a Myoglobin-based Functional Oxidase2017In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 56, no 23, p. 6622-6626Article in journal (Refereed)
    Abstract [en]

    Heme-copper oxidase (HCO) is a class of respiratory enzymes that use a heme-copper center to catalyze O-2 reduction to H2O. While heme reduction potential (E degrees') of different HCO types has been found to vary >500 mV, its impact on HCO activity remains poorly understood. Here, we use a set of myoglobin-based functional HCO models to investigate the mechanism by which heme E degrees' modulates oxidase activity. Rapid stopped-flow kinetic measurements show that increasing heme E degrees' by ca. 210 mV results in increases in electron transfer (ET) rates by 30-fold, rate of O-2 binding by 12-fold, O-2 dissociation by 35-fold, while decreasing O-2 affinity by 3-fold. Theoretical calculations reveal that E degrees' modulation has significant implications on electronic charge of both heme iron and O-2, resulting in increased O-2 dissociation and reduced O-2 affinity at high E degrees' values. Overall, this work suggests that fine-tuning E degrees' in HCOs and other heme enzymes can modulate their substrate affinity, ET rate and enzymatic activity.

  • 42.
    Björk, Jonas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Materials design. Linköping University, Faculty of Science & Engineering.
    Sanchez-Sanchez, Carlos
    Swiss Fed Labs Mat Sci & Technol, Switzerland; Inst Mat Sci Madrid ICMM CSIC, Spain.
    Chen, Qiang
    Max Planck Inst Polymer Res, Germany; Univ Oxford, England.
    Pignedoli, Carlo A.
    Swiss Fed Labs Mat Sci & Technol, Switzerland.
    Rosén, Johanna
    Linköping University, Department of Physics, Chemistry and Biology, Materials design. Linköping University, Faculty of Science & Engineering.
    Ruffieux, Pascal
    Swiss Fed Labs Mat Sci & Technol, Switzerland.
    Feng, Xinliang
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany.
    Narita, Akimitsu
    Max Planck Inst Polymer Res, Germany; Okinawa Inst Sci & Technol Grad Univ, Japan.
    Mullen, Klaus
    Max Planck Inst Polymer Res, Germany.
    Fasel, Roman
    Swiss Fed Labs Mat Sci & Technol, Switzerland; Univ Bern, Switzerland.
    The Role of Metal Adatoms in a Surface-Assisted Cyclodehydrogenation Reaction on a Gold Surface2022In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 61, no 49, article id e202212354Article in journal (Refereed)
    Abstract [en]

    Dehydrogenation reactions are key steps in many metal-catalyzed chemical processes and in the on-surface synthesis of atomically precise nanomaterials. The principal role of the metal substrate in these reactions is undisputed, but the role of metal adatoms remains, to a large extent, unanswered, particularly on gold substrates. Here, we discuss their importance by studying the surface-assisted cyclodehydrogenation on Au(111) as an ideal model case. We choose a polymer theoretically predicted to give one of two cyclization products depending on the presence or absence of gold adatoms. Scanning probe microscopy experiments observe only the product associated with adatoms. We challenge the prevalent understanding of surface-assisted cyclodehydrogenation, unveiling the catalytic role of adatoms and their effect on regioselectivity. The study adds new perspectives to the understanding of metal catalysis and the design of on-surface synthesis protocols for novel carbon nanomaterials.

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  • 43. Björling, T.
    et al.
    Noréus, D.
    Jansson, K.
    Andersson, Magnus
    KTH, School of Information and Communication Technology (ICT), Microelectronics and Information Technology, IMIT.
    Leonova, E.
    Edén, M.
    Hålenius, U.
    Häussermann, U.
    SrAlSiH: A polyanionic semiconductor hydride2005In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 44, no 44, p. 7269-7273Article in journal (Refereed)
    Abstract [en]

    (Chemical Equation Presented) Stable and semiconducting: Polyanionic hydrides represent a new class of main-group-metal hydrides with unforeseen hydrogen-coordination environments. The hydrogen atom in SrAlSiH is attached exclusively to Al and forms part of a layered [AlHSi]2- polyanion (see figure). This material is the first narrow bandgap semiconductor hydride and combines the high thermal stability of saline hydrides with the air and moisture stability of interstitial transition-metal hydrides.

  • 44.
    Björling, Thomas
    et al.
    Stockholms universitet.
    Noréus, Dag
    Stockholms universitet.
    Jansson, Kjell
    Stockholms universitet.
    Andersson, Magnus
    Kungliga Tekniska Högskolan.
    Leonova, Ekaterina
    Stockholms universitet.
    Edén, Mattias
    Stockholms universitet.
    Hålenius, Ulf
    Swedish Museum of Natural History, Department of Geology.
    Häussermann, Ulrich
    Stockholms universitet.
    SrAlSiH: A polyanionic semiconductor hydride2005In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 44, p. 7269-7273Article in journal (Refereed)
  • 45. Bolla, Jani Reddy
    et al.
    Corey, Robin A.
    Sahin, Cagla
    Gault, Joseph
    Hummer, Alissa
    Hopper, Jonathan T. S.
    Lane, David P.
    Drew, David
    Stockholm University, Faculty of Science, Department of Biochemistry and Biophysics.
    Allison, Timothy M.
    Stansfeld, Phillip J.
    Robinson, Carol
    Landreh, Michael
    A Mass-Spectrometry-Based Approach to Distinguish Annular and Specific Lipid Binding to Membrane Proteins2020In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 59, no 9, p. 3523-3528Article in journal (Refereed)
    Abstract [en]

    Membrane proteins engage in a variety of contacts with their surrounding lipids, but distinguishing between specifically bound lipids, and non-specific, annular interactions is a challenging problem. Applying native mass spectrometry to three membrane protein complexes with different lipid-binding properties, we explore the ability of detergents to compete with lipids bound in different environments. We show that lipids in annular positions on the presenilin homologue protease are subject to constant exchange with detergent. By contrast, detergent-resistant lipids bound at the dimer interface in the leucine transporter show decreased k(off) rates in molecular dynamics simulations. Turning to the lipid flippase MurJ, we find that addition of the natural substrate lipid-II results in the formation of a 1:1 protein-lipid complex, where the lipid cannot be displaced by detergent from the highly protected active site. In summary, we distinguish annular from non-annular lipids based on their exchange rates in solution.

  • 46. Brandau, Sven
    et al.
    Landa, Aitor
    Franzen, Johan
    Marigo, Mauro
    Jorgensen, Karl Anker
    Organocatalytic conjugate addition of malonates to alpha,beta-unsaturated aldehydes: Asymmetric formal synthesis of (-)-paroxetine, chiral lactams, and lactones2006In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 45, no 26, p. 4305-4309Article in journal (Refereed)
  • 47.
    Bruening, Lukas
    et al.
    Univ Cologne, Germany.
    Jena, Nityasagar
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Medicine and Health Sciences.
    Bykova, Elena
    Goethe Univ Frankfurt, Germany.
    Jurzick, Pascal L.
    Univ Cologne, Germany.
    Flosbach, Niko T.
    Univ Cologne, Germany.
    Mezouar, Mohamed
    European Synchrotron Radiat Facil, France.
    Hanfland, Michael
    European Synchrotron Radiat Facil, France.
    Giordano, Nico
    Deutsch Elektronen Synchrotron DESY, Germany.
    Fedotenko, Timofey
    Deutsch Elektronen Synchrotron DESY, Germany.
    Winkler, Bjoern
    Goethe Univ Frankfurt, Germany.
    Abrikosov, Igor
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Bykov, Maxim
    Univ Cologne, Germany.
    Stabilization of Guanidinate Anions [CN3]5− in Calcite-Type SbCN32023In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773Article in journal (Refereed)
    Abstract [en]

    The stabilization of nitrogen-rich phases presents a significant chemical challenge due to the inherent stability of the dinitrogen molecule. This stabilization can be achieved by utilizing strong covalent bonds in complex anions with carbon, such as cyanide CN- and NCN(2- )carbodiimide, while more nitrogen-rich carbonitrides are hitherto unknown. Following a rational chemical design approach, we synthesized antimony guanidinate SbCN3 at pressures of 32-38 GPa using various synthetic routes in laser-heated diamond anvil cells. SbCN3, which is isostructural to calcite CaCO3, can be recovered under ambient conditions. Its structure contains the previously elusive guanidinate anion [CN3](5-), marking a fundamental milestone in carbonitride chemistry. The crystal structure of SbCN3 was solved and refined from synchrotron single-crystal X-ray diffraction data and was fully corroborated by theoretical calculations, which also predict that SbCN3 has a direct band gap with the value of 2.20 eV. This study opens a straightforward route to the entire new family of inorganic nitridocarbonates.

  • 48. Bueno-Alejo, Carlos J.
    et al.
    Villaescusa, Luis A.
    Garcia-Bennett, Alfonso E.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Supramolecular Transcription of Guanosine Monophosphate into Mesostructured Silica2014In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 53, no 45, p. 12106-12110Article in journal (Refereed)
    Abstract [en]

    There is large interest in replicating biological supramolecular structures in inorganic materials that are capable of mimicking biological properties. The use of 5-guanosine monophosphate in the presence of Na+ and K+ ions as a supramolecular template for the synthesis of well-ordered mesostructured materials is reported here. Mesostructured particles with the confined template exhibit high structural order at both meso-and atomic scales, with a lower structural symmetry in the columnar mesophase. Although a chiral space group can not be deduced from X-ray diffraction, analysis by electron microscopy and circular dichroism confirms a chiral stacking arrangement along the c-axis. Guanosine monophosphate based mesophases thus illustrate the possibility for specific molecular imprinting of mesoporous materials by genetic material and the potential for higher definition in molecular recognition.

  • 49.
    Bykov, Maxim
    et al.
    Univ Bayreuth, Germany.
    Bykova, Elena
    Deutsch Elektronen Synchrotron DESY, Germany.
    Koemets, Egor
    Univ Bayreuth, Germany.
    Fedotenko, Timofey
    Univ Bayreuth, Germany.
    Aprilis, Georgios
    Univ Bayreuth, Germany.
    Glazyrin, Konstantin
    Deutsch Elektronen Synchrotron DESY, Germany.
    Liermann, Hanns-Peter
    Deutsch Elektronen Synchrotron DESY, Germany.
    Ponomareva, Alena V.
    Natl Univ Sci and Technol MISIS, Russia.
    Tidholm, Johan
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Tasnadi, Ferenc
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Abrikosov, Igor A.
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Dubrovinskaia, Natalia
    Univ Bayreuth, Germany.
    Dubrovinsky, Leonid
    Univ Bayreuth, Germany.
    High-Pressure Synthesis of a Nitrogen-Rich Inclusion Compound ReN8·xN2 with Conjugated Polymeric Nitrogen Chains2018In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 57, no 29, p. 9048-9053Article in journal (Refereed)
    Abstract [en]

    A nitrogen-rich compound, ReN(8)xN(2), was synthesized by a direct reaction between rhenium and nitrogen at high pressure and high temperature in a laser-heated diamond anvil cell. Single-crystal X-ray diffraction revealed that the crystal structure, which is based on the ReN8 framework, has rectangular-shaped channels that accommodate nitrogen molecules. Thus, despite a very high synthesis pressure, exceeding 100GPa, ReN(8)xN(2) is an inclusion compound. The amount of trapped nitrogen (x) depends on the synthesis conditions. The polydiazenediyl chains [-N=N-] that constitute the framework have not been previously observed in any compound. Abinitio calculations on ReN(8)xN(2) provide strong support for the experimental results and conclusions.

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  • 50.
    Bykov, Maxim
    et al.
    Howard Univ, DC 20059 USA; Carnegie Inst Sci, DC 20015 USA.
    Bykova, Elena
    Carnegie Inst Sci, DC 20015 USA.
    Ponomareva, Alena V.
    Natl Univ Sci & Technol MISIS, Russia.
    Abrikosov, Igor
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Chariton, Stella
    Univ Chicago, IL 60437 USA.
    Prakapenka, Vitali B.
    Univ Chicago, IL 60437 USA.
    Mahmood, Mohammad F.
    Howard Univ, DC 20059 USA.
    Dubrovinsky, Leonid
    Bayer Geoinst, Germany.
    Goncharov, Alexander F.
    Carnegie Inst Sci, DC 20015 USA.
    Stabilization of Polynitrogen Anions in Tantalum-Nitrogen Compounds at High Pressure2021In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 60, no 16, p. 9003-9008Article in journal (Refereed)
    Abstract [en]

    The synthesis of polynitrogen compounds is of great importance due to their potential as high-energy-density materials (HEDM), but because of the intrinsic instability of these compounds, their synthesis and stabilization is a fundamental challenge. Polymeric nitrogen units which may be stabilized in compounds with metals at high pressure are now restricted to non-branched chains with an average N-N bond order of 1.25, limiting their HEDM performances. Herein, we demonstrate the synthesis of a novel polynitrogen compound TaN5 via a direct reaction between tantalum and nitrogen in a diamond anvil cell at circa 100 GPa. TaN5 is the first example of a material containing branched all-single-bonded nitrogen chains [N-5(5-)](infinity). Apart from that we discover two novel Ta-N compounds: TaN4 with finite N-4(4-) chains and the incommensurately modulated compound TaN2-x, which is recoverable at ambient conditions.

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