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Sökning: L773:1433 7851

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  • Achenbach, Bastian, et al. (författare)
  • Porous Salts Containing Cationic Al24-Hydroxide-Acetate Clusters from Scalable, Green and Aqueous Synthesis Routes
  • 2023
  • Ingår i: Angewandte Chemie International Edition. - 1433-7851 .- 1521-3773. ; 62:29
  • Tidskriftsartikel (refereegranskat)abstract
    • 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). 
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  • Agarwala, Hemlata, et al. (författare)
  • Alternating Metal-Ligand Coordination Improves Electrocatalytic CO2 Reduction by a Mononuclear Ru Catalyst**
  • 2023
  • Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 62:17
  • Tidskriftsartikel (refereegranskat)abstract
    • 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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  • Agosta, Lorenzo, et al. (författare)
  • Origin of the Hydrophobic Behaviour of Hydrophilic CeO2
  • 2023
  • Ingår i: Angewandte Chemie International Edition. - : Wiley-VCH Verlagsgesellschaft. - 1433-7851 .- 1521-3773. ; 62:35
  • Tidskriftsartikel (refereegranskat)abstract
    • 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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  • Ahlquist, Mårten, et al. (författare)
  • Dispersion and Back-Donation Gives Tetracoordinate [Pd(PPh3)4]
  • 2011
  • Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 50:49, s. 11794-11797
  • Tidskriftsartikel (refereegranskat)abstract
    • 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.
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