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Dr. Peiyu Ge Dr. Mohamad Hojeij Dr. Micheál D. Scanlon Prof. Hubert H. Girault 《Chemphyschem》2020,21(24):2630-2633
H2 may be evolved biphasically using a polarised liquid|liquid interface, acting as a “proton pump”, in combination with organic soluble metallocenes as electron donors. Sustainable H2 production requires methodologies to recycle the oxidised donor. Herein, the photo-recycling of decamethylferrocenium cations (DcMFc+) using aqueous core-shell semiconductor CdSe@CdS nanoparticles is presented. Negative polarisation of the liquid|liquid interface is required to extract DcMFc+ to the aqueous phase. This facilitates the efficient capture of electrons by DcMFc+ on the surface of the photo-excited CdSe@CdS nanoparticles, with hydrophobic DcMFc subsequently partitioning back to the organic phase and resetting the system. TiO2 (P25) and CdSe semiconductor nanoparticles failed to recycle DcMFc+ due to their lower conduction band energy levels. During photo-recycling, CdS (on CdSe) may be self-oxidised and photo-corrode, instead of water acting as the hole scavenger. 相似文献
3.
Lukas Lohmeyer Dr. Elisabeth Kaifer Prof. Hubert Wadepohl Prof. Hans-Jörg Himmel 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(26):5834-5845
New redox-active 1,2,5,6-tetrakis(guanidino)-naphthalene compounds, isolable and storable in the neutral and deep-green dicationic redox states and oxidisable further in two one-electron steps to the tetracations, are reported. Protonation switches on blue fluorescence, with the fluorescence intensity (quantum yield) increasing with the degree of protonation. Reactions with N-halogenosuccinimides or N-halogenophthalimides led to a series of new redox-active halogeno- and succinimido-/phthalimido-substituted derivatives. These highly selective reactions are proposed to proceed via the tri- or tetracationic state as the intermediate. The derivatives are oxidised reversibly at slightly higher potentials than that of the unsubstituted compounds to dications and further to tri- and tetracations. The integration of redox-active ligands in the transition-metal complexes shifts the redox potentials to higher values and also allows reversible oxidation in two potentially separated one-electron steps. 相似文献
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Explicit and partly sharp estimates are given of integrals over the square of Bessel functions with an integrable weight which can be singular at the origin. They are uniform with respect to the order of the Bessel functions and provide explicit bounds for some smoothing estimates as well as for the L2 restrictions of Fourier transforms onto spheres in which are independent of the radius of the sphere. For more special weights these restrictions are shown to be Hölder continuous with a Hölder constant having this independence as well. To illustrate the use of these results a uniform resolvent estimate of the free Dirac operator with mass in dimensions is derived. 相似文献
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Roksana Kordala-Markiewicz Hubert Rodak Bartosz Markiewicz Filip Walkiewicz Agata Sznajdrowska Katarzyna Materna Katarzyna Marcinkowska Tadeusz Praczyk Juliusz Pernak 《Tetrahedron》2014
Ammonium ionic liquids with the 4-chloro-2-methylphenoxyacetate anion were synthesized and characterized. Physicochemical properties, such as thermal stability, phase transition temperatures, viscosity, density, refractive index, as well as surface activity and herbicidal activity were determined. Improved physicochemical properties suggest a reduced environmental impact of newly formed group of herbicidal ionic liquids (HILs). HILs with a longer substituent can be characterized with better herbicidal activity in comparison with commercial products. 相似文献
8.
Torsten Roth Vladislav Vasilenko Callum G. M. Benson Hubert Wadepohl Dominic S. Wright Lutz H. Gade 《Chemical science》2015,6(4):2506-2510
A simple, “click” synthetic approach to a new type of hybrid phosph(III)azane/NHC system is described. The presence of the phosphazane P2N2 ring unit, with P atoms flanking the NCN fragment and with this ring perpendicular to the binding site of the NHC, provides unique opportunities for modifying the electronic and steric character of these carbenes. 相似文献
9.
Qiang Liu Hubert Meissel Ilia Sadykov Simon Jones Nick Van Dijk Przemyslaw Rzepka Luca Artiglia Marco Ranocchiari Jeroen A. van Bokhoven 《Helvetica chimica acta》2021,104(7):e2100082
Stability studies on supported metal nanoparticles are essential for gaining insight into the design and optimization of high-performance materials. In this work, the dissolutions of Pt-based catalysts in HBr/Br2 mixture of various concentration regimes were studied and correlated with material structural properties. The dissolution of metal nanoparticles was enhanced by adding Br2 to the HBr solution. Comparing with commercial Pt/C catalyst, the well-alloyed PtIr/C catalyst was observed to exhibit high resistance towards dissolution. In addition, regulating the accessibility of the metal sites to dissolution-inducing species contributed to the marked stability of the nanoparticles in HBr/Br2 solutions, as shown for the surface-modified PtIr/C catalysts with organic diamine molecules. 相似文献
10.
Freia Ruegenberg Dr. Markus Seibald Dr. Dominik Baumann Dr. Simon Peschke Dr. Frauke Philipp Prof. Dr. Hubert Huppertz 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(45):11701-11706
In order to expand the field of alkali lithosilicates, a new representative of the substance class with a previously unknown structure type was found based on solid-state synthesis. The novel compound with the sum formula Rb[Li5Si2O7] crystallizes in the orthorhombic space group Pbcm (no. 57) with a=7.6269(3), b=9.5415(4), and c=9.4095(3) Å by means of single-crystal X-ray diffraction. The structure consists of a highly condensed lithosilicate framework, built up of corner- and edge-linked [LiO4]-tetrahedra and [Si2O7]-units, and the rubidium ions aligned in channels. Suitable crystals of the material were obtained using sealed tantalum ampoules as reaction tube at a temperature of 750 °C. The new compound was further characterized via powder diffraction, Rietveld analysis, and EDX measurements. At first glance, Eu2+-doped Rb[Li5Si2O7] reveals an intense green luminescence. In-depth crystal analysis shows that a core-shell formation is present even for apparently high quality single-crystals. As a minority phase, the known green phosphor RbLi[Li3SiO4]2:Eu2+ is the origin of the luminescence, representing a tiny core inside of the particles surrounded by a large matrix of transparent Rb[Li5Si2O7] dominating the single-crystal diffraction pattern. 相似文献