Angewandte Chemie最新文献

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Solid polymer electrolytes (SPEs) are promising ionic conductors for developing high-specific-energy solid-state lithium metal batteries. However, developing SPEs with both high ionic conductivity and interfacial compatibility remains a challenge. Here, we propose a design concept of an anion-modulated polymer electrolyte (termed AMPE) for high-voltage Li metal batteries. Specifically, we design the AMPE by incorporating high-voltage-resistant and high charge density units with an anion receptor unit. The high-voltage-resistant and high charge density segments contribute to achieving a decent voltage tolerance of the polymer chains and ensure sufficient carrier ions. The anion receptor, represented by a boron-containing molecule, promotes the generation of free Li⁺ by dissociating anion-cation pairs. More importantly, the strong interaction between the electron-deficient B and the TFSI⁻ in the matrix promotes the anion reduction to form a stable anion-derived mosaic-like solid electrolyte interphase on the Li-metal anode. As a result, the AMPE exhibits a high ionic conductivity of 3.80×10⁻⁴ S cm⁻¹ and effectively suppresses lithium dendrites, enabling an all-solid-state Li|AMPE|LiCoO₂ cell to achieve a cycle life of 700 cycles at an operating voltage of 4.40 V. This design concept would inspire efforts to develop high-performance SPEs for high-specific-energy solid-state lithium metal batteries.

Core fucosylation, catalyzed by α-1,6-fucosyltransferase (FUT8), is implicated in various diseases, making FUT8 inhibitors highly desirable. In their Research Article (e202414682), Yoshiyuki Manabe, Koichi Fukase et al. developed FUT8 inhibitors with potent cellular activity. Through high-throughput screening and structural optimization, potent FUT8 inhibitors were identified. Additionally, prodrug derivatization enhanced the stability of these inhibitors, enabling the suppression of core fucose expression in cell-based assays.

Highly efficient solar thermal conversion (STC) at catalytic active sites is critical for harnessing solar energy to boost catalytic reactions. In their Communication (e202412049), Dehui Deng, Liang Yu and co-workers report direct integration of full-spectrum STC and electrocatalytic oxygen evolution activity on a “Chainmail” catalyst by constructing a hierarchical nanocage architecture, achieving a near complete 98 % solar absorptivity and a remarkable potential decrease of over 240 mV for the oxygen evolution reaction.

Thiosilvatins are a class of biologically active dithiodiketopiperazine natural products. In their Research Article (e202412397), Daniel Strand and co-workers describe a first, collective, synthesis of thiosilvatins, introducing methods and tactics to overcome stereochemical issues in dithiodiketopiperazine synthesis. The artwork depicts thiosilvatins emerging from and escaping an abyss of inaccessibility and structural ambiguity.

An innovative upcycling process transforms unsorted daily plastic waste into hydrogen and valuable carbon materials. In their Research Article (e202404196), Guoxing Chen, Zeai Huang, Ying Zhou, Anke Weidenkaff et al. develop a novel plasma-enabled method using single-atom catalysts to rapidly decompose various types of plastic waste, including mixed plastics, into high-value carbon nanomaterials and hydrogen. This efficient and cost-effective approach represents a breakthrough in sustainable waste management, providing a promising solution for large-scale recycling of mixed post-consumer plastics.

Dynamic boroxine linkers were incorporated into the mesoporous metal–organic framework (MOF) PCN-333, which creates defects and expands pore sizes, enabling the encapsulation of enzymes larger than the intrinsic MOF pores. As reported by Xing Zhang, Shuai Yuan et al in their Research Article (e202409951), this strategy facilitates the immobilization of glycoenzymes for synthesizing complex oligosaccharides and polysaccharides, demonstrating both high activity and enhanced enzyme stability.

While functionalized polyethylenes (PEs) exhibit valuable characteristics, the constraints of existing synthetic approaches limit the variety of readily incorporated functionality. New methods to generate functionalized PEs are required to afford new applications of this common material. We report 100 % atom economic tantalum-catalyzed hydroaminoalkylation of vinyl-terminated polyethylene (VTPE) as a method to produce amine-terminated PE. VTPEs with molecular weights between 2200–16800 g/mol are successfully aminated using solvent-free conditions. Our catalytic system is efficient for the installation of both aromatic and aliphatic amines, and can be carried out on multigram scale. The associating amine functional groups afford modified material properties, as measured by water contact angle, differential scanning calorimetry (DSC) and polymer rheology. The basic amine functionality offers the opportunity to convert inert PE into stimuli-responsive materials, such that the protonation of aminated PE affords the generation of functional antibacterial PE films.

Tryptophan nitration chemistry of an economically impactful heme enzyme, TxtE, has been modeled utilizing synthetic heme mimics by Sam P. de Visser, Gayan B. Wijeratne et al. in their Research Article (e202409430). Therein, spectroscopic and theoretical characterizations strongly suggest the occurrence of a heme peroxynitrite active species, closely paralleling mechanistic propositions put forward for TxtE enzyme. Precise mechanistic details and key structure–activity relationships present important findings to be implemented in next generation therapeutic and synthetic applications.

Die 57. SCS-Konferenz über Stereochemie, besser bekannt als Bürgenstock-Konferenz, brachte in Brunnen (Schweiz) ein breites Spektrum an Fachwissen aus der Chemie zusammen.