Nature Communications最新文献

Trifluoromethylation remains a fundamental transformation in drug discovery, underpinning many top-selling pharmaceuticals. Emerging developments in iron ligand-to-metal charge transfer (LMCT) catalysis have redefined fluoroalkylation chemistry by unlocking the repurposing of readily available trifluoroacetates as radical trifluoromethyl sources. Recent (hetero)arene trifluoromethylation methods generally require stoichiometric inorganic oxidants to turnover photoactive iron catalysts, thereby limiting their broader applicability. Herein, we present an integrated photoelectrocatalytic strategy employing in situ-generated multifunctional iron species to achieve C(sp²)-H trifluoromethylation without stoichiometric oxidants and generating only traceless byproducts. Mechanistic studies identify catalytically active iron species exhibiting a dual synergistic function: promoting the photodecarboxylation of trifluoroacetates and mediating catalytic redox turnover. This protocol offers mild, tunable, and scalable conditions powered by visible light and electric current. It features a broad substrate scope, enabling the functionalization of diverse (hetero)cyclic scaffolds, including challenging electron-rich and easily oxidizable substrates, thus demonstrating its potential for sustainable late-stage modification in pharmaceutical synthesis.

The stereoselective synthesis of glycosidic bonds can be promoted by the addition of stereodirecting solvents. In particular, nitrile and ether based solvents are known to promote the selective production of β- or α-glycosides, respectively. Even though the application of co-solvents in glycosylation protocols is well-established, the understanding of their impact on the glycosylation mechanism as well as the reaction intermediates formed upon their addition, remains incomplete. As the exact mechanism of solvent stereo direction remains debated, this limits the ability to develop stereoselective glycosylation methods. Herein, we report the application of relaxation and exchange NMR techniques to establish that acetonitrile and tetrahydrofuran form covalent glycosyl-nitrilium and glycosyl-oxonium ions, respectively. In contrast, other ethereal solvents such as diethyl ether and 1,4-dioxane were not able to do so. This work highlights the potential of exchange NMR to study reaction mechanisms, provides evidence for the formation of glycosyl-solvent adducts despite their very low populations, and improves our ability to develop better stereoselective glycosylation protocols.

The human gut is colonized by trillions of microbes that influence the health of their human host. Whereas many bacterial species have now been linked to a variety of different diseases, the involvement of Archaea, an evolutionarily distinct group of microbes, in human disease remains elusive. By analyzing 19 independent clinical studies, we demonstrate that associations between Archaea and human diseases are widespread yet highly heterogeneous, with a pronounced and consistent enrichment of Methanobrevibacter smithii in colorectal cancer (CRC) patients. Metabolic modelling and in vitro co-culture identified distinct mutualistic interactions of M. smithii with CRC-causing bacteria such as Fusobacterium nucleatum, including metabolic enhancement. Metabolomics further reveal archaeal-derived compounds with tumor-modulating properties. Together, our results provide mechanistic insights into how the human gut archaeome may participate in CRC-associated microbial networks through metabolic cooperation with bacteria.

Two-dimensional (2D) materials, including graphene and MXenes, have garnered significant interest for enhancing both the mechanical and multifunctional properties of advanced structural ceramics. These materials encounter operational limitations under high temperatures, particularly due to oxidative degradation of 2D reinforcement architectures that induces composition instability and property deterioration. In this study, we developed a processing methodology for fabricating 2D Al₂O₃ platelet-reinforced yttria-stabilized zirconia (YSZ) composites, which can be stable up to 1300 ^oC in an atmosphere. Through a multi-field coupling strategy combining gravitational field modulation, high-intensity vibrational alignment, and controlled pressure densification, we achieved densified composites with parallel-aligned Al₂O₃ platelet array in YSZ matrix.‌ The composite demonstrates reduced near-infrared (NIR) transmittance below 10%, effectively blocking radiative thermal transfer. Meanwhile, The YSZ-Al₂O₃ platelet composite (YSZ-Al₂O₃-PL) simultaneously demonstrates enhanced resistance to CaO-MgO-AlO_1.5-SiO₂ (CMAS) molten salts and improved fracture toughness. The cost-effective 2D oxide/ceramic composites possess exceptional thermo-mechanical stability, promising for harsh environments.