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1.
Synthesis and Photophysical Properties of a Sc3N@C80‐Corrole Electron Donor–Acceptor Conjugate
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Bin Liu Hongyun Fang Prof. Xiaofang Li Wenting Cai Lipiao Bao Marc Rudolf Fabian Plass Prof. Louzhen Fan Prof. Xing Lu Prof. Dirk M. Guldi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(2):746-752
Embedding endohdedral metallofullerenes (EMFs) into electron donor–acceptor systems is still a challenging task owing to their limited quantities and their still largely unexplored chemical properties. In this study, we have performed a 1,3‐dipolar cycloaddition reaction of a corrole‐based precursor with Sc3N@C80 to regioselectively form a [5,6]‐adduct ( 1 ). The successful attachment of the corrole moiety was confirmed by mass spectrometry. In the electronic ground state, absorption spectra suggest sizeable electronic communications between the electron acceptor and the electron donor. Moreover, the addition pattern occurring at a [5,6]‐bond junction is firmly proven by NMR spectroscopy and electrochemical investigations performed with 1 . In the electronically excited state, which is probed in photophysical assays with 1 , a fast electron‐transfer yields the radical ion pair state consisting of the one‐electron‐reduced Sc3N@C80 and of the one‐electron‐oxidized corrole upon its exclusive photoexcitation. As such, our results shed new light on the practical work utilizing EMFs as building blocks in photovoltaics. 相似文献
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Michiel Janssen Prof. Dirk E. De Vos 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(45):10724-10734
The practical application of Shilov-type Pt catalysis to the selective hydroxylation of terminal aliphatic C−H bonds remains a formidable challenge, due to difficulties in replacing PtIV with a more economically viable oxidant, particularly O2. We report the potential of employing FeCl2 as a suitable redox mediator to overcome the kinetic hurdles related to the direct use of O2 in the Pt reoxidation. For the selective conversion of butyric acid to γ-hydroxybutyric acid (GHB), a significantly enhanced catalyst activity and stability (turnover numbers (TON)>30) were achieved under 20 bar O2 in comparison to current state-of-the-art systems (TON<10). In this regard, essential reaction parameters affecting the overall activity were identified, along with specific additives to attain catalyst stability at longer reaction times. Notably, deactivation by reduction to Pt0 was prevented by the addition of monodentate pyridine derivatives, such as 2-fluoropyridine, but also by introducing varying partial pressures of N2 in the gaseous atmosphere. Finally, stability tests revealed the involvement of PtII and FeCl2 in catalyzing the non-selective overoxidation of GHB. Accordingly, in situ esterification with boric acid proved to be a suitable strategy to maintain enhanced selectivities at much higher conversions (TON>60). Altogether, a useful catalytic system for the selective hydroxylation of primary aliphatic C−H bonds with O2 is presented. 相似文献
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Anatomy of a gauge theory 总被引:4,自引:0,他引:4
We exhibit the role of Hochschild cohomology in quantum field theory with particular emphasis on gauge theory and Dyson–Schwinger equations, the quantum equations of motion. These equations emerge from Hopf- and Lie algebra theory and free quantum field theory only. In the course of our analysis, we exhibit an intimate relation between the Slavnov–Taylor identities for the couplings and the existence of Hopf sub-algebras defined on the sum of all graphs at a given loop order, surpassing the need to work on single diagrams. 相似文献
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We show how the Hopf algebra of rooted trees encodes the combinatorics of Epstein-Glaser renormalization and coordinate space renormalization in general. In particular, we prove that the Epstein-Glaser time-ordered products can be obtained from the Hopf algebra by suitable Feynman rules, mapping trees to operator-valued distributions. Twisting the antipode with a renormalization map formally solves the Epstein-Glaser recursion and provides local counterterms due to the Hochschild 1-closedness of the grafting operator B+.submitted 29/03/04, accepted 01/06/04 相似文献
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A. G. Milekhin A. I. Nikiforov M. Yu. Ladanov O. P. Pchelyakov S. Schulze D. R. T. Zahn 《Physics of the Solid State》2004,46(1):92-96
This paper reports on the results of resonant Raman scattering investigations of the fundamental vibrations in Ge/Si structures with strained and relaxed germanium quantum dots. Self-assembled strained Ge/Si quantum dots are grown by molecular-beam epitaxy on Si(001) substrates. An ultrathin SiO2 layer is grown prior to the deposition of a germanium layer with the aim of forming relaxed germanium quantum dots. The use of resonant Raman scattering (selective with respect to quantum dot size) made it possible to assign unambiguously the line observed in the vicinity of 300 cm?1 to optical phonons confined in relaxed germanium quantum dots. The influence of confinement effects and mechanical stresses on the vibrational spectra of the structures with germanium quantum dots is analyzed. 相似文献
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Viviane Van Hoof Hugo Cluckers Vera Verhaeghe An Hennebel Marleen Truyens Edith Van Loock Pierre Rombouts Dirk Maes Jan Van Elven Katrien Lesage Mark Flothmann Lieve Nijs Filip Colpaert Werner Vercammen Dominique Bolain 《Accreditation and quality assurance》2004,10(1-2):55-59
In response to a change of the Belgian National Directives whereby hospital laboratories became responsible for all point-of-care testing (POCT) performed within hospital walls a standardized and automated POC glucose-testing system was implemented in our hospital. The system consists of 50 AccuCheck Inform instruments (Roche Diagnostics, Vilvoorde, Belgium), 50 docking stations, a DataCare Server, and connections to the medical laboratory information system (MOLIS, Sysmex, Barchon, Belgium) and to the hospital information system. Implementation involved many parties and extensive preparation and communication. Key issues were bar-coded patient and user identification, training, and responsibilities. One year after the hospital wide implementation of this system the quality of POC glucose testing has significantly increased, thereby improving patient safety. This study describes a stepwise change over involving the medical laboratory and with a focus on hands-on quality.Presented at the ninth conference on Quality in the Spotlight, 18–19 March 2004, Antwerp, Belgium. 相似文献
10.
Using ultra-high vacuum scanning tunneling microscopy (UHV-STM), we show that copper-phthalocyanine (CuPc) grows in a well ordered manner on hydrogen passivated vicinal silicon surfaces. CuPc grows one-dimensionally parallel to the monatomic steps on the vicinal silicon surface. Surprisingly, elongated clusters of the CuPc parallel to the step directions are formed even on the middle of the terraces well away from the step edges. The one-dimensional growth mode continues even after the full monolayer coverage on the substrate which results in strongly oriented growth mode of a thin film of CuPc on the vicinal silicon surfaces. 相似文献