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Affronte M Troiani F Ghirri A Carretta S Santini P Corradini V Schuecker R Muryn C Timco G Winpenny RE 《Dalton transactions (Cambridge, England : 2003)》2006,(23):2810-2817
We report on real molecular complexes and propose strategies that explore the possibility of implementation of specific quantum computation architectures with molecular spin systems. We focus on Cr3+ carboxylate derivatives and use the Loss-DiVincenzo scheme as reference. 相似文献
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Raffael Davenport Mattia Silvi Adam Noble Zied Hosni Natalie Fey Varinder K. Aggarwal 《Angewandte Chemie (International ed. in English)》2020,59(16):6525-6528
There are a limited number of ring‐contraction methodologies which convert readily available five‐membered rings into strained four‐membered rings. Here we report a photo‐induced radical‐mediated ring contraction of five‐membered‐ring alkenyl boronate complexes into cyclobutanes. The process involves the addition of an electrophilic radical to the electron‐rich alkenyl boronate complex, leading to an α‐boryl radical. Upon one‐electron oxidation, ring‐contractive 1,2‐metalate rearrangement occurs to give a cyclobutyl boronic ester. A range of radical precursors and vinyl boronates can be employed, and chiral cyclobutanes can be accessed with high levels of stereocontrol. The process was extended to the preparation of benzofused cyclobutenes and the versatility of the boronic ester was demonstrated by conversion to other functional groups. 相似文献
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Yuriy Yusim Enrico Trevisanello Dr. Raffael Ruess Dr. Felix H. Richter Dr. Alexander Mayer Dr. Dominic Bresser Prof. Dr. Stefano Passerini Prof. Dr. Dr. h.c. Jürgen Janek Dr. Anja Henss 《Angewandte Chemie (International ed. in English)》2023,62(12):e202218316
Solid-state batteries (SSBs) with high-voltage cathode active materials (CAMs) such as LiNi1−x−yCoxMnyO2 (NCM) and poly(ethylene oxide) (PEO) suffer from “noisy voltage” related cell failure. Moreover, reports on their long-term cycling performance with high-voltage CAMs are not consistent. In this work, we verified that the penetration of lithium dendrites through the solid polymer electrolyte (SPE) indeed causes such “noisy voltage cell failure”. This problem can be overcome by a simple modification of the SPE using higher molecular weight PEO, resulting in an improved cycling stability compared to lower molecular weight PEO. Furthermore, X-ray photoelectron spectroscopy analysis confirms the formation of oxidative degradation products after cycling with NCM, for what Fourier transform infrared spectroscopy is not suitable as an analytical technique due to its limited surface sensitivity. Overall, our results help to critically evaluate and improve the stability of PEO-based SSBs. 相似文献
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Viktor Paczelt Dr. Raffael C. Wende Prof. Dr. Peter R. Schreiner Dr. André K. Eckhardt 《Angewandte Chemie (International ed. in English)》2023,62(11):e202218548
Simple unhindered aldimines tend to hydrolyze or oligomerize and are therefore spectroscopically not well characterized. Herein we report the formation and spectroscopic characterization of the simplest imino acid, namely glycine imine, by cryogenic matrix isolation IR and UV/Vis spectroscopy. Glycine imine forms after UV irradiation of 2-azidoacetic acid by N2 extrusion in anti-(E,E)- and anti-(Z,Z)-conformation that can be photochemically interconverted. In matrix isolation pyrolysis experiments with 2-azidoacetic acid, glycine imine cannot be trapped as it further decarboxylates to aminomethylene. In aqueous solution glycine imine is hydrolyzed to hydroxy glycine and hydrated glyoxylic acid. At higher concentrations or in the presence of FeIISO4 as a reducing agent glycine imine undergoes self-reduction by oxidative decarboxylation chemistry. Glycine imine may be seen as one of the key reaction intermediates connecting prebiotic amino acid and sugar formation chemistry. 相似文献
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Dr. Tong-Tong Zuo Dr. Felix Walther Jun Hao Teo Dr. Raffael Rueß Yubo Wang Prof. Marcus Rohnke Prof. Daniel Schröder Prof. Linda F. Nazar Prof. Jürgen Janek 《Angewandte Chemie (International ed. in English)》2023,62(7):e202213228
Lithium argyrodite-type electrolytes are regarded as promising electrolytes due to their high ionic conductivity and good processability. Chemical modifications to increase ionic conductivity have already been demonstrated, but the influence of these modifications on interfacial stability remains so far unknown. In this work, we study Li6PS5Cl and Li5.5PS4.5Cl1.5 to investigate the influence of halogenation on the electrochemical decomposition of the solid electrolyte and the chemical degradation mechanism at the cathode interface in depth. Electrochemical measurements, gas analysis and time-of-flight secondary ion mass spectrometry indicate that the Li5.5PS4.5Cl1.5 shows pronounced electrochemical decomposition at lower potentials. The chemical reaction at higher voltages leads to more gaseous degradation products, but a lower fraction of solid oxygenated phosphorous and sulfur species. This in turn leads to a decreased interfacial resistance and thus a higher cell performance. 相似文献
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The reaction of the 10-I-3 hypervalent iodine electrophilic trifluoromethylation reagent 1-trifluoromethyl-1,2-benziodoxol-3-(1H)-one (2) with 2,4,6-trimethylphenol, after deprotonation with NaH and in the presence of 18-crown-6 in a polar, nonprotic solvent, affords 1,3,5-trimethyl-2-(trifluoromethoxy)benzene (4) only as a byproduct. Trifluoromethylation occurs preferentially at the ortho- and para-positions of the aromatic core, giving the corresponding trifluoromethylcyclohexadienones 5 and 6. In case the ortho- and/or para-positions are not substituted, the corresponding products of an aromatic, electrophilic substitution are obtained in moderate yield, for example, 2-trifluoromethyl-4-tert-butylphenol (10a) from 4-tert-butylphenol (10). 相似文献
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