Angewandte Chemie最新文献

Heterogeneous Catalysis. In their Research Article (e202405641), Gang Wu, Gao Li et al. report a MnRuO_x catalyst exhibiting a unique structure, combining microcrystalline and amorphous regions. This design enables the catalyst to showcase excellent performance in water electrolysis.

Asymmetric Catalysis. The design and evolution of an enzyme for the asymmetric Michael addition of cyclic ketones to nitroolefins by enamine catalysis is reported by Zhi Zhou et al. in their Communication (e202404312).

Perylene diimide (PDI) dimers and higher aggregates are key components in organic molecular photonics and photovoltaic devices, supporting singlet fission and symmetry breaking charge separation. Detailed understanding of their excited states is thus important. This has proven challenging because interchromophoric coupling is a strong function of dimer architecture. Recently, a macrocyclic PDI dimer was reported in which excitonic coupling could be turned on and off simply by changing the solvent. This presents a useful case where coupling is modified without synthetic changes to tune supramolecular structure. Here we present a detailed study of solvent dependent excited state dynamics in this dimer by means of coherent multidimensional spectroscopy. Spectral analysis resolves the different coupling strengths, which are consistent with solvent dependent changes in dimer conformation. The strongly coupled conformer forms an excimer within 300 fs. The low-frequency Raman active modes recovered from two-dimensional electronic spectra reveal frequencies characteristic of exciton coupling. These are assigned to modes modulating the coupling from the corresponding DFT calculations. Further analysis reveals a time dependent frequency during excimer formation. Analysis of two-dimensional “beatmaps” reveals features in the coupled dimer which are not predicted by the displaced harmonic oscillator model and are assigned to vibronic coupling.

A strategy for transition metal-free cross-coupling of alkyl nitroso-carbamates and boronic acids is reported. The N-nitroso carbamates are easily prepared from the corresponding amine in two simple steps. This method allows for the synthesis of a wide variety of secondary boronates, benzylic boronates and formal Csp³−Csp² cross-coupling products under operationally simple conditions. Functional group tolerance is also demonstrated and applied in the modification of lysine to make non-canonical amino acids.

Droplets dancing to non-classical tunes. Nishant Singh and co-workers (e202406220) show in their Communication how phase-separated amino acid droplets can non-classically evolve into poly-crystals and fibrous hydrogels. Several complex and direct pathways are explored to achieve transient or stable soft materials, single- or poly-crystals by provoking disordered droplets.

Direct evidence differentiating the chiroptical signals originating from either topological or Euclidean chirality in topologically chiral [2]catenane by time-resolved circularly polarized luminescence (TRCPL) spectroscopy combined with transient absorption (TA) spectroscopy, is reported by Jinquan Chen et al. in their Research Article (e202407929).

An acknowledgement was accidentally omitted from this publication. With this Corrigendum, the authors acknowledge that: “Financial support was also provided by the U.S. Department of Energy under Award Number DE-SC0024448.”

Supramolecular hetero-self-assembly is more challenging and meaningful compared to homo-self-assembly in many areas. In their Research Article (e202410130), Xu-Man Chen, Hong Yang, Quan Li et al. present a cucurbit[8]uril-mediated heterodimerization, which enables the occurrence of a rare cucurbit[8]uril-mediated [2+2] heterocycloaddition under UV irradiation. The final product is found to be an unexpected [2]rotaxane, developing into a novel photochemical template synthesis of mechanically interlocked molecules.

In the Table of Content, Scheme 1, Figure 1A, Figure 2A, Figure 3G, an inadvertent mistake was made in the stereocenters of the galactose units in the peptides or the modified serine, as firstly noticed by Dr Sebastien Vidal. The correct figures are shown below. In addition, the stereocenter information of galactose units in Figures S1, S4, and S14 was also shown in an opposite fashion and was revised appropriately as well. This Corrigendum does not affect the results and the conclusions of the paper. We apologize for any inconvenience.

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