Nature Communications最新文献

Photothermal catalysis is a promising strategy to combine the advantages of both thermal-catalysis and photocatalysis. Herein we achieve the protolignin conversion to aromatics via the photothermal catalytic transfer hydrogenolysis process intensified by the in-situ protection strategy. The Pd/TiO₂ at 140 °C with UV irradiation can catalyze the reforming of primary alcohols to aldehydes and active H* species, which further participate in the acetalation protection of the 1,3-diol group of β-O-4 linkage and mediate the hydrogenolysis of C_β–OAr bonds, respectively. The conversion of birch sawdust with ethanol as the hydrogen donor provides a 40 wt% yield of phenolic monomers, compared with an 11 wt% monomer yield obtained from the conversion of extracted 1,3-diol-protected lignin under the same conditions. The synergistic effect of photocatalysis and thermal-catalysis contributes to the prior cleavage of the C_β–OAr bond before other C–O bonds. The feasibility of solar-light-driven photothermal catalytic system is demonstrated.

SmCo₄B-based alloys with high magnetocrystalline anisotropy are expected to be used as raw materials or constituent phases for new permanent magnets. In this work, we develop Sm(Co, Fe, Ni)₄B alloys with excellent hard magnetic properties by tuning the contents of Fe, Co, and Ni. The addition of Fe enhances the amorphous formation ability of the as-spun ribbons, whereas Ni addition improves the structural stability of the crystalline phases. During annealing, the amorphous phase crystallizes into different Sm-Co-B phases in stages. A high coercivity of 5.68–6.71 MA·m⁻¹ is obtained in the annealed SmCo_4–x–yFe_xNi_yB (x = 1.0–2.0, y = 0.8–1.0) ribbons composed of platelet-shaped and equiaxed grains in comparison with the coercivity of 2.89–5.18 MA·m⁻¹ in the x = 1.0–1.2 and y = 0–0.8 ribbons with equiaxed grains. Here, we show the strong correlations between the microstructure and magnetic properties and provide insights for the future development of high-performance SmCo₄B-based magnets.

Residue-free and highly efficient techniques for drinking water disinfection are urgently needed. Herein, we report an electrochemical water disinfection system equipped with atomically precise Ag₂₈ nanoclusters (NCs) as electrode materials. The deployment of these Ag₂₈ NCs not only provides sufficient electrosorption sites for intelligent microbe enrichment but also ensures high-efficiency dual-mode microbial killing through the in situ electrocatalytic production of residue-free reactive oxygen species (ROS) and the inherent antimicrobial activity of Ag₂₈ NCs. Moreover, the design of the system enables a cyclical “alive microbe capture–killing–dead microbe desorption” process for continuous water disinfection. On this basis, this water disinfection system is efficient against broad-spectrum microbes (with >99.99% antimicrobial activity), durable (with a performance reduction of only 0.75% over 40 cycles and 99.90% antimicrobial efficiency for over 5 h of continuous operation), versatile (i.e., other NCs can be used), scalable (with water productivity of 213.33 L h⁻¹ m⁻²), energy efficient (with a low energy consumption of 4.91 Wh m⁻³; 1.04 Wh m⁻³ without the pumping cost) and applicable for various real water samples. This study may open new avenues for global water disinfection techniques.

Coronavirus Disease 2019 (COVID-19) emerged in December 2019, prompting the implementation of a “zero-COVID” policy in Mainland China. The easing of this policy in December 2022 led to a surge in COVID cases, which was believed to significantly increase antibiotic usage, potentially due to antibiotic misuse or increased coinfections. Our study aimed to compare antibiotic consumption and patterns before and after this policy adjustment. We utilised wastewater-based epidemiology (WBE) to analyse antibiotic levels in samples collected from five wastewater treatment plants in Eastern China during January and February of 2021 and 2023. 27 antibiotics were quantified using ultra-high performance liquid chromatography coupled with triple quadrupole tandem mass spectrometry (UPLC-MS/MS) and analysed via WBE, with the resulting estimates compared with catchment-specific prescription data. 23 antibiotics were detected in wastewater samples, with a substantial increase in usage in 2023 (ranging from 531% to 3734%), consistent with prescription data. Here, we show a significant rise in antibiotic consumption during the COVID-19 surge and this underscores the need for further investigation into the impacts of inappropriate antibiotic use in China.

Semiconductor quantum dots (QDs) in planar germanium (Ge) heterostructures have emerged as front-runners for future hole-based quantum processors. Here, we present strong coupling between a hole charge qubit, defined in a double quantum dot (DQD) in planar Ge, and microwave photons in a high-impedance (Z_r = 1.3 kΩ) resonator based on an array of superconducting quantum interference devices (SQUIDs). Our investigation reveals vacuum-Rabi splittings with coupling strengths up to g₀/2π = 260 MHz, and a cooperativity of C ~ 100, dependent on DQD tuning. Furthermore, utilizing the frequency tunability of our resonator, we explore the quenched energy splitting associated with strong Coulomb correlation effects in Ge QDs. The observed enhanced coherence of the strongly correlated excited state signals the presence of distinct symmetries within related spin functions, serving as a precursor to the strong coupling between photons and spin-charge hybrid qubits in planar Ge. This work paves the way towards coherent quantum connections between remote hole qubits in planar Ge, required to scale up hole-based quantum processors.

Non-homologous end joining (NHEJ) is the predominant pathway that repairs DNA double-stranded breaks (DSBs) in vertebrates. However, due to challenges in detecting DSBs in living cells, the repair capacity of the NHEJ pathway is unknown. The DNA termini of many DSBs must be processed to allow ligation while minimizing genetic changes that result from break repair. Emerging models propose that DNA termini are first synapsed ~115 Å apart in one of several long-range synaptic complexes before transitioning into a short-range synaptic complex that juxtaposes DNA ends to facilitate ligation. The transition from long-range to short-range synaptic complexes involves both conformational and compositional changes of the NHEJ factors bound to the DNA break. Importantly, it is unclear how NHEJ proceeds in vivo because of the challenges involved in analyzing recruitment of NHEJ factors to DSBs over time in living cells. Here, we develop an approach to study the temporal and compositional dynamics of NHEJ complexes using live cell single-molecule imaging. Our results provide direct evidence for stepwise maturation of the NHEJ complex, pinpoint key regulatory steps in NHEJ progression, and allowed us to estimate the overall repair capacity of the NHEJ pathway in living cells.

Contrary to common chemical intuition, cation-π interactions can persist in polar, aqueous reaction solutions, rather than in dry non-coordinative solvent systems. This account highlights how alkali ion-π interactions impart distinctive structure-influencing supramolecular forces that can be exploited in the preparation of nanoscopic metal-organic capsules. The incorporation of alkali ions from polar solutions into molecular pockets promotes the assembly of otherwise inaccessible capsular entities whose structures are distinctive to those of common polyoxovanadate clusters in which {V=O} moieties usually point radially to the outside, shielding the molecular entities. The applied concept is exemplified by homologous {V₂₀} and {V₃₀} cages, composed of inverted, hemispherical {V₅O₉} units. The number and geometrical organization of these {V₅O₉} sub-units in these cages are associated with prevailing cation-(pi) interactions and competing steric effects. The stereoisomers of these resulting nano-sized objects are comparable to Alfred Werner-type structural isomers of simple mononuclear complexes in-line with fundamental coordination chemistry principles.

Psychological stress contributes to cardiovascular disease (CVD) and sudden cardiac death, yet its molecular basis remains obscure. RNA binding protein RBM24 plays a critical role in cardiac development, rhythm regulation, and cellular stress. Here, we show that psychological stress activates RBM24 S181 phosphorylation through eIF4E2-GSK3β signaling, which causally links psychological stress to CVD by promoting APOE translation (apolipoprotein E). Using an Rbm24 S181A KI mouse model, we show that impaired S181 phosphorylation leads to cardiac contractile dysfunction, atrial fibrillation, dyslipidemia, reduced muscle strength, behavioral abnormalities, and sudden death under acute and chronic psychological stressors. The impaired S181 phosphorylation of RBM24 inhibits cardiac translation, including APOE translation. Notably, cardiomyocyte-specific expression of APOE rescues cardiac electrophysiological abnormalities and contractile dysfunction, through preventing ROS stress and mitochondrial dysfunction. Moreover, RBM24-S181 phosphorylation acts as a serum marker for chronic stress in human. These results provide a functional link between RBM24 phosphorylation, eIF4E-regulated APOE translation, and psychological-stress-induced CVD.

Chromothripsis is a frequent form of genome instability, whereby a presumably single catastrophic event generates extensive genomic rearrangements of one or multiple chromosome(s). However, little is known about the heterogeneity of chromothripsis across different clones from the same tumour, as well as changes in response to treatment. Here we analyse single-cell genomic and transcriptomic alterations linked with chromothripsis in human p53-deficient medulloblastoma and neural stem cells (n = 9). We reconstruct the order of somatic events, identify early alterations likely linked to chromothripsis and depict the contribution of chromothripsis to malignancy. We characterise subclonal variation of chromothripsis and its effects on extrachromosomal circular DNA, cancer drivers and putatively druggable targets. Furthermore, we highlight the causative role and the fitness consequences of specific rearrangements in neural progenitors.

Despite the significant potential of generative models, low synthesizability of many generated molecules limits their real-world applications. In response to this issue, we develop ClickGen, a deep learning model that utilizes modular reactions like click chemistry to assemble molecules and incorporates reinforcement learning along with inpainting technique to ensure that the proposed molecules display high diversity, novelty and strong binding tendency. ClickGen demonstrates superior performance over the other reaction-based generative models in terms of novelty, synthesizability, and docking conformation similarity for existing binders targeting the three proteins. We then proceeded to conduct wet-lab validation on the ClickGen’s proposed molecules for poly adenosine diphosphate-ribose polymerase 1. Due to the guaranteed high synthesizability and model-generated synthetic routes for reference, we successfully produced and tested the bioactivity of these novel compounds in just 20 days, much faster than typically expected time frame when handling sufficiently novel molecules. In bioactivity assays, two lead compounds demonstrated superior anti-proliferative efficacy against cancer cell lines, low toxicity, and nanomolar-level inhibitory activity to PARP1. We demonstrate that ClickGen and related models may represent a new paradigm in molecular generation, bringing AI-driven, automated experimentation and closed-loop molecular design closer to realization.