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71.
Jannik Brückmann Dr. Carolin Müller Ilse Friedländer Dr. Alexander K. Mengele Prof. Kalina Peneva Prof. Benjamin Dietzek-Ivanšić Prof. Sven Rau 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(61):e202201931
The ambitious goal of artificial photosynthesis is to develop active systems that mimic nature and use light to split water into hydrogen and oxygen. Intramolecular design concepts are particularly promising. Herein, we firstly present an intramolecular photocatalyst integrating a perylene-based light-harvesting moiety and a catalytic rhodium center ( RhIIIphenPer ). The excited-state dynamics were investigated by means of steady-state and time-resolved absorption and emission spectroscopy. The studies reveal that photoexcitation of RhIIIphenPer yields the formation of a charge-separated intermediate, namely RhIIphenPer ⋅ + , that results in a catalytically active species in the presence of protons. 相似文献
72.
Sebastian Wöllner Timothy Nowak Dr. Gui-Rong Zhang Dr. Nils Rockstroh Dr. Hanadi Ghanem Prof. Dr. Stefan Rosiwal Prof. Dr. Angelika Brückner Prof. Dr. Bastian J. M. Etzold 《ChemistryOpen》2021,10(5):600-606
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) offers a renewable approach to produce the value-added platform chemical 2,5-furandicarboxylic acid (FDCA). The key for the economic viability of this approach is to develop active and selective electrocatalysts. Nevertheless, a reliable catalyst evaluation protocol is still missing, leading to elusive conclusions on criteria for a high-performing catalyst. Herein, we demonstrate that besides the catalyst identity, secondary parameters such as materials of conductive substrates for the working electrode, concentration of the supporting electrolyte, and electrolyzer configurations have profound impact on the catalyst performance and thus need to be optimized before assessing the true activity of a catalyst. Moreover, we highlight the importance of those secondary parameters in suppressing side reactions, which has long been overlooked. The protocol is validated by evaluating the performance of free-standing Cu-foam, and CuCoO modified with NaPO2H2 and Ni, which were immobilized on boron-doped diamond (BDD) electrodes. Recommended practices and figure of merits in carefully evaluating the catalyst performance are proposed. 相似文献
73.
J. Brüning 《The European physical journal. Special topics》2007,145(1):181-189
We describe the main lines of mathematical research dealing
with nodal sets of eigenfunctions since the days of Chladni. We
present the material in a form hopefully suited to a nonspecialized
but mathematically educated audience. 相似文献
74.
We propose what we believe to be a novel, refined model of the angular sensitivity function of artificial apposition compound eyes. Compared with the formerly used Gaussian approximation that was derived for natural compound eyes, our model is better suited to describe the resolution capacity of artificial compound eyes accounting for the cylindrical sensitivity function of technical receptors. It is shown that this analytic model is valid over a broad range of parameters of the optical system, which was not fulfilled by one of the previous models. Finally, an analytic approach is used to derive the modulation transfer function of these multichannel imaging systems. 相似文献
75.
Ekta Mishra Jill L. Worlinsky Christian Brückner Victor Ryzhov 《Journal of the American Society for Mass Spectrometry》2014,25(1):18-29
Free base and cobalt(II) complexes of six meso-tetraphenylporphyrinoids containing nonpyrrolic heterocycles and of three meso-thienylporphyrins were investigated using electrospray ionization tandem mass spectrometry (ESI-MS/MS). Their fragmentation was studied in a quadrupole ion trap as a function of the porphyrinoid macrocycle structure and compared with the fragmentation behavior of the benchmark compound meso-tetraphenylporphyrin. In situ oxidation of the neutral cobalt(II) complexes under ESI conditions produced singly charged cobalt(III) porphyrinoid ions; the free bases were ionized by protonation. For the porphyrinoids with an intact porphyrin core, the major fragmentation pathways observed were the losses of the meso-substituent (for meso-phenyl groups) and characteristic fragmentations of one or more meso-substituents (for the meso-thienyl group). Complex fragmentation pathways were observed for porphyrinoids with modifications to the porphyrin core but chemically reasonable structures could be assigned to most fragments, thus delineating general patterns for the behavior of pyrrole-modified porphyrins under CID conditions. Figure
? 相似文献
76.
Mono‐ and Bis(pyrrolo)tetrathiafulvalene Derivatives Tethered to C60: Synthesis,Photophysical Studies,and Self‐Assembled Monolayers 下载免费PDF全文
Dr. Marta Vico Solano Dr. Eduardo Antonio Della Pia Dr. Martyn Jevric Christina Schubert Xintai Wang Dr. Cornelia van der Pol Prof. Dr. Anders Kadziola Prof. Dr. Kasper Nørgaard Prof. Dr. Dirk M. Guldi Prof. Dr. Mogens Brøndsted Nielsen Prof. Dr. Jan O. Jeppesen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(32):9918-9929
A series of mono‐ (MPTTF) and bis(pyrrolo)tetrathiafulvalene (BPTTF) derivatives tethered to one or two C60 moieties was synthesized and characterized. The synthetic strategy for these dumbbell‐shaped compounds was based on a 1,3‐dipolar cycloaddition reaction between aldehyde‐functionalized MPTTF/BPTTF derivatives, two different tailor‐made amino acids, and C60. Electronic communication between the MPTTF/BPTTF units and the C60 moieties was studied by a variety of techniques including cyclic voltammetry and absorption spectroscopy. These solution‐based studies indicated no observable electronic communication between the MPTTF/BPTTF units and the C60 moieties. In addition, femtosecond and nanosecond transient absorption spectroscopy revealed, rather surprisingly, that no charge transfer from the MPTTF/BPTTF units to the C60 moieties takes place on excitation of the fullerene moiety. Finally, it was shown that the MPTTF–C60 and C60–BPTTF‐C60 dyad and triad molecules formed self‐assembled monolayers on a Au(111) surface by anchoring to C60. 相似文献
77.
Steffen M. Brülls Dr. Valentina Cantatore Zhenping Wang Dr. Pui Lam Tam Dr. Per Malmberg Jessica Stubbe Prof. Dr. Biprajit Sarkar Prof. Dr. Itai Panas Prof. Dr. Jerker Mårtensson Prof. Dr. Siegfried Eigler 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(29):6694-6702
Hybridizing graphene and molecules possess a high potential for developing materials for new applications. However, new methods to characterize such hybrids must be developed. Herein, the wet-chemical non-covalent functionalization of graphene with cationic π-systems is presented and the interaction between graphene and the molecules is characterized in detail. A series of tricationic benzimidazolium salts with various steric demand and counterions was synthesized, characterized and used for the fabrication of graphene hybrids. Subsequently, the doping effects were studied. The molecules are adsorbed onto graphene and studied by Raman spectroscopy, XPS as well as ToF-SIMS. The charged π-systems show a p-doping effect on the underlying graphene. Consequently, the tricationic molecules are reduced through a partial electron transfer process from graphene, a process which is accompanied by the loss of counterions. DFT calculations support this hypothesis and the strong p-doping could be confirmed in fabricated monolayer graphene/hybrid FET devices. The results are the basis to develop sensor applications, which are based on analyte/molecule interactions and effects on doping. 相似文献
78.
Stephan Schaumüller Doris Cristurean Stephan Haudum George S. Pappas Markus Himmelsbach Matthias Bechmann Oliver Brüggemann Ian Teasdale 《Journal of polymer science. Part A, Polymer chemistry》2021,59(24):3161-3166
We report a facile post-polymerization modification route to functionalized aromatic polyimides via Diels-Alder cycloaddition. Aromatic polyimides are important, versatile high-performance polymers; however, their structural diversity is restricted by the requirements of the step-growth polymerization. We prepared polyimides with alkynes in their main-chain as macromolecular dienophiles and quantitatively grafted tetraphenylcyclopentadienone based dienes. The resulting solution-processable, wholly aromatic polyimides show a considerable increase in surface area due to the induced conformational changes and bulky, rigid, and contorted molecular structures. The orthogonality of the reaction is exploited to insert functional groups, namely bromine and sulfonates, along the polymer backbone. In a further extension, the phenylene segments undergo cyclodehydrogenation to form nanographene segments within the polymer chains. The Diels-Alder cycloaddition onto polyimides is therefore demonstrated to be an effective, widely applicable route to tunable high-performance polymers with value-added functionality and thus considerable potential in a wide range of advanced materials. 相似文献
79.
80.
O. Kavatsyuk C. Mazzocchi Z. Janas A. Banu L. Batist F. Becker A. Blazhev W. Brüchle J. Döring T. Faestermann M. Górska H. Grawe A. Jungclaus M. Karny M. Kavatsyuk O. Klepper R. Kirchner M. La Commara K. Miernik I. Mukha C. Plettner A. Płochocki E. Roeckl M. Romoli K. Rykaczewski M. Schädel K. Schmidt R. Schwengner J. Żylicz 《The European Physical Journal A - Hadrons and Nuclei》2007,31(3):319-325
The β decay of the very neutron-deficient isotope 101Sn was studied at the GSI on-line mass separator using silicon detectors for recording charged particles and germanium detectors
for γ-ray spectroscopy. Based on the β-delayed proton data the production cross-section of 101Sn in the 50Cr + 58Ni fusion-evaporation reaction was determined to be about 60nb. The half-life of 101Sn was measured to be 1.9(3)s. For the first time β-delayed γ-rays of 101Sn were tentatively identified, yielding weak evidence for a cascade of 352 and 1065keV transitions in 101In. The results for the 101Sn decay as well as those from previous work on the 103Sn decay are discussed by comparing them to predictions obtained from shell model calculations employing a new interaction
in the 88Sr to 132Sn model space. 相似文献