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61.
3D DNA Origami Nanoparticles: From Basic Design Principles to Emerging Applications in Soft Matter and (Bio‐)Nanosciences
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Sebastian Loescher Saskia Groeer Prof. Andreas Walther 《Angewandte Chemie (International ed. in English)》2018,57(33):10436-10448
Scaffold‐based lattice‐engineered 3D DNA origami is a powerful and versatile technique for the rational design and build‐up of arbitrarily structured and monodisperse DNA‐based 3D nanoobjects. Relying on the unsurpassed molecular programmability of sequence‐specific DNA hybridization, a long DNA single strand (termed scaffold) is assembled with many short single‐stranded oligomers (termed staples), which organize the scaffold into a 3D lattice in a single step, thereby leading to 3D nanoparticulate structures of the highest precision in high yields. Applications of 3D DNA origami are increasingly wide‐spread and interface with numerous fields of sciences, for example, anisometric or anisotropically functionalized nanoparticles, fundamental investigations of superstructure formation, biomedicine, (bio)physics, sensors, and optical materials. This Minireview discusses the fundamentals and recent advances from structure formation to selected applications, with a mission to promote cross‐disciplinary exchange. 相似文献
62.
Cobalt‐Bridged Ionic Liquid Polymer on a Carbon Nanotube for Enhanced Oxygen Evolution Reaction Activity
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Dr. Yuxiao Ding Dr. Alexander Klyushin Dr. Xing Huang Travis Jones Detre Teschner Dr. Frank Girgsdies Dr. Tania Rodenas Prof. Dr. Robert Schlögl Dr. Saskia Heumann 《Angewandte Chemie (International ed. in English)》2018,57(13):3514-3518
By taking inspiration from the catalytic properties of single‐site catalysts and the enhancement of performance through ionic liquids on metal catalysts, we exploited a scalable way to place single cobalt ions on a carbon‐nanotube surface bridged by polymerized ionic liquid. Single dispersed cobalt ions coordinated by ionic liquid are used as heterogeneous catalysts for the oxygen evolution reaction (OER). Performance data reveals high activity and stable operation without chemical instability. 相似文献
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Performing numerous analyses of tire/road noise measurements on low-noise pavements during the last several years, the authors observed significant inhomogeneity of the wearing course in numerous cases, while similar problems were almost non-existent when dense pavements were measured. 相似文献
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Dr. Johannes Preindl Saskia Schulthoff Conny Wirtz M. Sc. Julia Lingnau Prof. Alois Fürstner 《Angewandte Chemie (International ed. in English)》2017,56(26):7525-7530
Orevactaene and epipyrone A were previously thought to comprise the same polyunsaturated tail but notably different C-glycosylated 4-hydroxy-2-pyrone head groups. Total synthesis now shows that the signature bicyclic framework assigned to orevactaene is a chimera; the compound is almost certainly identical with epipyrone A, whose previously unknown stereochemistry has also been established during this study. Key to success was the ready formation of the bicyclic core of putative orevactaene by a sequence of two alkyne cycloisomerization reactions using tungsten and gold catalysis. Equally important was the flexibility in the assembly process gained by the use of heterobimetallic polyunsaturated modules whose termini could be selectively and consecutively addressed in a practical one-pot cross-coupling sequence. 相似文献
66.
Dr. Mariusz Jaremko Dr. Łukasz Jaremko Dr. Saskia Villinger Christian D. Schmidt Prof. Dr. Christian Griesinger Dr. Stefan Becker Prof. Dr. Markus Zweckstetter 《Angewandte Chemie (International ed. in English)》2016,55(35):10518-10521
15N spin‐relaxation rates are demonstrated to provide critical information about the long‐range structure and internal motions of membrane proteins. Combined with an improved calculation method, the relaxation‐rate‐derived structure of the 283‐residue human voltage‐dependent anion channel revealed an anisotropically shaped barrel with a rigidly attached N‐terminal helix. Our study thus establishes an NMR spectroscopic approach to determine the structure and dynamics of mammalian membrane proteins at high accuracy and resolution. 相似文献
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Prof. Dr. Oliver Trapp Dr. Saskia Lamour Dr. Frank Maier Dr. Alexander F. Siegle Dr. Kerstin Zawatzky Prof. Dr. Bernd F. Straub 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(68):15871-15880
Chemical reactions that lead to a spontaneous symmetry breaking or amplification of the enantiomeric excess are of fundamental interest in explaining the formation of a homochiral world. An outstanding example is Soai's asymmetric autocatalysis, in which small enantiomeric excesses of the added product alcohol are amplified in the reaction of diisopropylzinc and pyrimidine-5-carbaldehydes. The exact mechanism is still in dispute due to complex reaction equilibria and elusive intermediates. In situ high-resolution mass spectrometric measurements, detailed kinetic analyses and doping with in situ reacting reaction mixtures show the transient formation of hemiacetal complexes, which can establish an autocatalytic cycle. We propose a mechanism that explains the autocatalytic amplification involving these hemiacetal complexes. Comprehensive kinetic experiments and modelling of the hemiacetal formation and the Soai reaction allow the precise prediction of the reaction progress, the enantiomeric excess as well as the enantiomeric excess dependent time shift in the induction period. Experimental structural data give insights into the privileged properties of the pyrimidyl units and the formation of diastereomeric structures leading to an efficient amplification of even minimal enantiomeric excesses, respectively. 相似文献
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Dr. Thomas N. Snaddon Dr. Philipp Buchgraber Saskia Schulthoff Conny Wirtz Dr. Richard Mynott Prof. Dr. Alois Fürstner 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(40):12133-12140
A productive total synthesis of both enantiomers of berkelic acid ( 1 ) is outlined that takes the structure revision of this bioactive fungal metabolite previously proposed by our group into account. The successful route relies on a fully optimized triple‐deprotection/1,4‐addition/spiroacetalization cascade reaction sequence, which delivers the tetracyclic core 32 of the target as a single isomer in excellent yield. The required cyclization precursor 31 is assembled from the polysubstituted benzaldehyde derivative 20 and methyl ketone 25 by an aldol condensation, in which the acetyl residue in 20 transforms from a passive protecting group into an active participant. Access to fragment 25 takes advantage of the Collum–Godenschwager variant of the ester enolate Claisen rearrangement, which clearly surpasses the classical Ireland–Claisen procedure in terms of diastereoselectivity. Although it is possible to elaborate 32 into the target without any additional manipulations of protecting groups, a short detour consisting in the conversion of the phenolic ? OH into the corresponding TBS‐ether is beneficial. It tempers the sensitivity of the compound toward oxidation and hence improves the efficiency and reliability of the final stages. Orthogonal ester groups for the benzoate and the aliphatic carboxylate terminus of the side chain secure an efficient liberation of free berkelic acid in the final step of the route. 相似文献