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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
2.
3.
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
4.
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
5.
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
6.
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
7.
S. Heinze P. Kurz D. Wortmann G. Bihlmayer S. Blügel 《Applied Physics A: Materials Science & Processing》2002,75(1):25-36
In this paper we present a density functional theory investigation of complex magnetic structures in ultra-thin films. The
focus is on magnetically frustrated antiferromagnetic Cr and Mn monolayers deposited on a triangular lattice provided by a
Ag (111) substrate. This involves non-collinear magnetic structures, which we treat by first-principles calculations on the
basis of the vector spin-density formulation of the density functional theory. We find for Cr/Ag (111) a coplanar non-collinear
periodic 120° Néel structure, for Mn/Ag (111) a row-wise antiferromagnetic structure, and for Fe/Ag (111) a ferromagnetic
structure as magnetic ground states. The spin-polarized scanning tunneling microscope (SP–STM) operated in the constant-current
mode is proposed as a powerful tool to investigate complex atomic-scale magnetic structures of otherwise chemically equivalent
atoms. We discuss a recent application of this operation mode of the SP–STM on Mn/W (110), which led to the first observation
of a two-dimensional antiferromagnet on a non-magnetic metal. The future potential of this approach is demonstrated by calculating
SP–STM images for different magnetic structures of Cr/Ag (111). The results show that the predicted non-collinear magnetic
ground state structure can clearly be discriminated from competing magnetic structures. A general discussion of the application
of different operation modes of the SP–STM is presented on the basis of the model of Tersoff and Hamann.
Received: 07 May 2001 / Accepted: 23 July 2001 / Published online: 3 April 2002 相似文献
8.
V Ravindran Pankaj Agrawal Rahul Basu Satyaki Bhattacharya J Blümlein V Del Duca R Harlander D Kosower Prakash Mathews Anurag Tripathi 《Pramana》2006,67(5):983-992
This is the report of the subgroup QCD of Working Group-4 at WHEPP-9. We present the activities that had taken place in the
subgroup and report some of the partial results arrived at following the discussion at the working group meetings. 相似文献
9.
Dirk P. Kroese Sergey Porotsky Reuven Y. Rubinstein 《Methodology and Computing in Applied Probability》2006,8(3):383-407
In recent years, the cross-entropy method has been successfully applied to a wide range of discrete optimization tasks. In
this paper we consider the cross-entropy method in the context of continuous optimization. We demonstrate the effectiveness
of the cross-entropy method for solving difficult continuous multi-extremal optimization problems, including those with non-linear
constraints.
相似文献
10.
An acoustic pulse propagating on a two-mode fiber can act as a beam splitter in a scanning interferometer. When this device
is employed in white-light interferometry, the effects of distributed coupling and dispersive interferometer arms need to
be considered. A theory suitable for treating acousto-optic interaction of partially coherent light in a moving interaction
region was developed. It was found that differential optical dispersion should be negligible and the acoustic pulse length
short. Also the coherence time should be short but long compared to the intermodal group delay difference over a pulse length.
Experiments with long acoustic pulses were performed, and fairly good agreement with theory was obtained. 相似文献