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排序方式: 共有791条查询结果,搜索用时 93 毫秒
1.
Simen Gjelseth Antonsen Arne Joakim C. Bunkan Tomas Mikoviny Yngve Stenstrøm Armin Wisthaler 《Molecular physics》2020,118(15)
The kinetics of the O3, OH and NO3 radical reactions with diazomethane were studied in smog chamber experiments employing long-path FTIR and PTR-ToF-MS detection. The rate coefficients were determined to be k CH2NN+O3?=?(3.2?±?0.4)?×?10?17 and k CH2NN+OH?=?(1.68?±?0.12)?×?10?10 cm3 molecule?1 s?1 at 295?±?3?K and 1013?±?30 hPa, whereas the CH2NN?+?NO3 reaction was too fast to be determined in the static smog chamber experiments. Formaldehyde was the sole product observed in all the reactions. The experimental results are supported by CCSD(T*)-F12a/aug-cc-pVTZ//M062X/aug-cc-pVTZ calculations showing the reactions to proceed exclusively via addition to the carbon atom. The atmospheric fate of diazomethane is discussed. 相似文献
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Dr. Dinar Abdullin Dr. Hideto Matsuoka Dr. Maxim Yulikov Nico Fleck Dr. Christoph Klein Dr. Sebastian Spicher Dr. Gregor Hagelueken Prof. Dr. Stefan Grimme Prof. Dr. Arne Lützen Prof. Dr. Olav Schiemann 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(37):8820-8828
Pulsed EPR dipolar spectroscopy (PDS) offers several methods for measuring dipolar coupling and thus the distance between electron-spin centers. To date, PDS measurements to metal centers were limited to ions that adhere to the high-field approximation. Here, the PDS methodology is extended to cases where the high-field approximation breaks down on the example of the high-spin Fe3+/nitroxide spin-pair. First, the theory developed by Maryasov et al. (Appl. Magn. Reson. 2006 , 30, 683–702) was adapted to derive equations for the dipolar coupling constant, which revealed that the dipolar spectrum does not only depend on the length and orientation of the interspin distance vector with respect to the applied magnetic field but also on its orientation to the effective g-tensor of the Fe3+ ion. Then, it is shown on a model system and a heme protein that a PDS method called relaxation-induced dipolar modulation enhancement (RIDME) is well-suited to measuring such spectra and that the experimentally obtained dipolar spectra are in full agreement with the derived equations. Finally, a RIDME data analysis procedure was developed, which facilitates the determination of distance and angular distributions from the RIDME data. Thus, this study enables the application of PDS to for example, the highly relevant class of high-spin Fe3+ heme proteins. 相似文献
5.
Prasenjit Das Jérôme Roeser Arne Thomas 《Angewandte Chemie (International ed. in English)》2023,62(29):e202304349
A chemically stable 2D microporous COF ( PMCR-1 ) was synthesized via the multicomponent Povarov reaction. PMCR-1 exhibits a remarkable and long-term stable photocatalytic H2O2 production rate (60 h) from pure and sea water under visible light. The H2O2 production is markedly enhanced when benzyl alcohol (BA) is added as reductant, which is also due to a strong π–π interaction of BA with dangling phenyl moieties in the COF pores introduced by the multicomponent Povarov reaction. Motivated by the concomitant BA oxidation to benzaldehyde during H2O2 formation, the photocatalytic oxidation of various organic substrates such as benzyl amine and methyl sulfide derivatives was investigated. It is shown that the well-defined micropores of PMCR-1 enable size-selective photocatalytic oxidation. 相似文献
6.
Vincent Weigelt Dr. Sarah Vogl Dr. Johannes Schmidt Prof. Arne Thomas 《Angewandte Chemie (International ed. in English)》2023,62(39):e202307818
The Wittig reaction is a key step in industrial processes to synthesise large quantities of vitamin A and various other important chemicals that are used in daily life. This article presents a pathway to achieve the Wittig reaction in a solid network. A highly porous triphenylphosphine-based polymer was applied as a solid Wittig reagent that undergoes, in a multi-step cycle, in total six post-synthetic modifications. This allowed for regeneration of the solid Wittig reagent and reuse for the same reaction cycle. Of particular industrial relevance is that the newly developed material also enables a simple way of separating the product by filtration. Therefore, additional costly and difficult separation and purification steps are no longer needed. 相似文献
7.
Gioria Esteban Signorini Chiara Taleb María C. Thomas Arne Mihályi Magdolna R. Gutierrez Laura 《Cellulose (London, England)》2021,28(14):9135-9147
Cellulose - Palladium was incorporated into carboxymethylated cellulose fibers as a support, thereby becoming an efficient and stable catalyst for low temperature gas phase reaction. Thus, NO was... 相似文献
8.
Asymmetric Synthesis of Fully Substituted Cyclopentane‐Oxindoles through an Organocatalytic Triple Michael Domino Reaction 下载免费PDF全文
Dr. Liang‐Hua Zou Arne R. Philipps Prof. Dr. Gerhard Raabe Prof. Dr. Dieter Enders 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(3):1004-1008
An efficient, highly stereoselective asymmetric synthesis of fully functionalized cyclopentanes bearing an oxindole moiety and several other functional groups in one pot has been developed. Key step is an organocatalytic triple Michael domino reaction forming three C?C bonds and six stereocenters, including a quaternary one. Starting from equimolar amounts of simple substrates, a high molecular complexity can be reached after a Wittig olefination in one pot. The new protocol can easily be scaled up to gram amounts. 相似文献
9.
Dr. Dinar Abdullin Nico Fleck Christoph Klein Philipp Brehm Sebastian Spicher Prof. Dr. Arne Lützen Prof. Dr. Stefan Grimme Prof. Dr. Olav Schiemann 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(10):2586-2596
Iron(III) porphyrins have the propensity to form μ2-oxo-dimers, the structures of which resemble two wheels on an axle. Whereas their crystal structure is known, their solution structure and internal dynamics is not. In the present work, the structure and dynamics of such dimers were studied by means of electron paramagnetic resonance (EPR) spectroscopy and quantum chemistry based molecular dynamics (MD) simulations by using the semiempirical tight-binding method (GFN-xTB). To enable EPR investigation of the dimers, a nitroxide was attached to each of the tetraphenylporphyrin cores through a linear and a bent linker. The inter-nitroxide distance distributions within the dimers were determined by continuous-wave (cw)-EPR and pulsed electron–electron double resonance (PELDOR or DEER) experiments and, with the help of MD, interpreted in terms of the rotation of the porphyrin planes with respect to each other around the Fe–O–Fe axis. It was found that such rotation is restricted to the four registers defined by the phenyl substituents. Within the registers, the rotation angle swings between 30° and 60° in the proximal and between 125° and 145° in the distal register. With EPR, all four angles were found to be equally populated, whereas the 30° and 145° angles are strongly favored to the expense of the 60° and 125° angles in the MD simulation. In either case, the internal dynamics of these dimers thus resemble the motion of a step motor. 相似文献
10.
Arne Van Antwerpen 《Journal of Pure and Applied Algebra》2018,222(11):3379-3394
In this paper, we show that all Coleman automorphisms of a finite group with self-central minimal non-trivial characteristic subgroup are inner; therefore the normalizer property holds for these groups. Using our methods we show that the holomorph and wreath product of finite simple groups, among others, have no non-inner Coleman automorphisms. As a further application of our theorems, we provide partial answers to questions raised by M. Hertweck and W. Kimmerle. Furthermore, we characterize the Coleman automorphisms of extensions of a finite nilpotent group by a cyclic p-group. Finally, we note that class-preserving Coleman automorphisms of p-power order of some nilpotent-by-nilpotent groups are inner, extending a result by J. Hai and J. Ge, where p is a prime number. 相似文献