Nature Communications最新文献

Aryl thiols have proven to be a useful class of electron donors and hydrogen atom sources in photochemical processes. However, the direct activation and functionalization of C(sp²)–S bonds in aryl thiols remains elusive in the field of photochemistry. Herein, a photochemical carboxylation of C(sp²)–S bonds in aryl thiols with CO₂ is reported, providing a synthetic route to important aryl carboxylic acids. Moreover, different kinds of aryl thiol derivatives, benzeneselenol and diphenyl diselenide also show moderate-to-high reactivity in this transformation. Mechanistic studies, including DFT calculations, suggest that the in situ generated carbon dioxide radical anion (CO₂^•−) and disulfide might be the key intermediates, which undergo radical substitution to yield products. This reaction features mild and catalyst-free conditions, good functional group tolerance and wide substrate scope. Furthermore, the efficient degradation of polyphenylene sulfide highlights the usefulness of this methodology.

Brain region- and cell-specific transcriptomic and epigenomic features are associated with heritability for neuropsychiatric traits, but a systematic view, considering cortical and subcortical regions, is lacking. Here, we provide an atlas of chromatin accessibility and gene expression profiles in neuronal and non-neuronal nuclei across 25 distinct human cortical and subcortical brain regions from 6 neurotypical controls. We identified extensive gene expression and chromatin accessibility differences across brain regions, including variation in alternative promoter-isoform usage and enhancer-promoter interactions. Genes with distinct promoter-isoform usage across brain regions were strongly enriched for neuropsychiatric disease risk variants. Moreover, we built enhancer-promoter interactions at promoter-isoform resolution across different brain regions and highlighted the contribution of brain region-specific and promoter-isoform-specific regulation to neuropsychiatric disorders. Including promoter-isoform resolution uncovers additional distal elements implicated in the heritability of diseases, thereby increasing the power to fine-map risk genes. Our results provide a valuable resource for studying molecular regulation across multiple regions of the human brain and underscore the importance of considering isoform information in gene regulation.

Pigs play a central role in human livelihoods in China, but a lack of systematic large-scale whole-genome sequencing of Chinese domestic pigs has hindered genetic studies. Here, we present the 1000 Chinese Indigenous Pig Genomes Project sequencing dataset, comprising 1011 indigenous individuals from 50 pig populations covering approximately two-thirds of China’s administrative divisions. Based on the deep sequencing (~25.95×) of these pigs, we identify 63.62 million genomic variants, and provide a population-specific reference panel to improve the imputation performance of Chinese domestic pig populations. Using a combination of methods, we detect an ancient admixture event related to a human immigration climax in the 13^th century, which may have contributed to the formation of southeast-central Chinese pig populations. Analyzing the haplotypes of the Y chromosome shows that the indigenous populations residing around the Taihu Lake Basin exhibit a unique haplotype. Furthermore, we find a 13 kb region in the THSD7A gene that may relate to high-altitude adaptation, and a 0.47 Mb region on chromosome 7 that is significantly associated with body size traits. These results highlight the value of our genomic resource in facilitating genomic architecture and complex traits studies in pigs.

Ab-initio methods such as density functional theory (DFT) is useful for fundamental atomistic-level study and is widely used across many scientific fields, including for the discovery of electrochemical reaction byproducts. However, many DFT steps may be needed to discover rare electrochemical reaction byproducts, which limits DFT’s scalability. In this work, we demonstrate that it is possible to generate many elementary electrochemical reaction byproducts in-silico using just a small number of ab-initio energy minimization steps if it is done in a multi-scale manner, such as via previously reported tiered tensor transform (3T) method. We first demonstrate the algorithm through a simple example of a complex floppy organic molecule passivator binding onto perovskite solar cell surface defect site. We then demonstrate more complex examples by generating hundreds of electrochemical reaction byproducts in lithium-ion battery liquid electrolyte (many are verified in previous experimental studies), with most trajectories completed within 50–100 DFT steps as opposed to more than 10,000 steps typically utilized in an ab-initio molecular dynamics trajectory. This approach requires no machine learning training data generation and can be directly applied on any new chemistries, making it suitable for ab-initio elementary chemical reaction byproduct investigation when temperature dependence is not required.

In the era of synthetic biology, design, construction, and utilization of synthetic chromosomes with unique features provide a strategy to study complex cellular processes such as aging. Herein, we successfully construct the 884 Kb synXIII of Saccharomyces cerevisiae to investigate replicative aging using these synthetic strains. We verify that up-regulation of a rRNA-related transcriptional factor, RRN9, positively influence replicative lifespan. Using SCRaMbLE system that enables inducible whole-genome rearrangement on synXIII, we obtain 20 SCRaMbLEd synXIII strains with extended lifespan. Transcriptome analysis reveal the expression of genes involve in global protein synthesis is up-regulated in longer-lived strains. We establish causal links between genotypic change and the long-lived phenotype via reconstruction of some key structural variations observed in post-SCRaMbLE strains and further demonstrate combinatorial effects of multiple aging regulators on lifespan extension. Our findings underscore the potential of synthetic yeasts in unveiling the function of aging-related genes.

The pulverization of silicon (Si) anode materials is recognized as a major cause of their poor cycling performance, yet a mechanistic understanding of this degradation from a full cell perspective remains elusive. Here, we identify an overlooked contributor to Si anode failure: mechanical shutdown of separators. Through mechano-structural characterization of Si full cells, combined with digital-twin simulation, we demonstrate that the volume expansion of Si exerts localized compressive stress on commercial polyethylene separators, leading to pore collapse. This structural disruption impairs ion transport across the separator, exacerbating redox nonuniformity and Si pulverization. Compression simulation reveals that a Young’s modulus greater than 1 GPa is required for separators to withstand the volume expansion of Si. To fulfill this requirement, we design a high modulus separator, enabling a high-areal-capacity pouch-type Si full cell to retain 88% capacity after 400 cycles at a fast charge rate of 4.5 mA cm⁻².

Perovskite solar cells (PSCs) offer an efficient, inexpensive alternative to current photovoltaic technologies, with the potential for manufacture via high-throughput coating methods. However, challenges for commercial-scale solution-processing of metal-halide perovskites include the use of harmful solvents, the expense of maintaining controlled atmospheric conditions, and the inherent instabilities of PSCs under operation. Here, we address these challenges by introducing a high volatility, low toxicity, biorenewable solvent system to fabricate a range of 2D perovskites, which we use as highly effective precursor phases for subsequent transformation to α-formamidinium lead triiodide (α-FAPbI₃), fully processed under ambient conditions. PSCs utilising our α-FAPbI₃ reproducibly show remarkable stability under illumination and elevated temperature (ISOS-L-2) and “damp heat” (ISOS-D-3) stressing, surpassing other state-of-the-art perovskite compositions. We determine that this enhancement is a consequence of the 2D precursor phase crystallisation route, which simultaneously avoids retention of residual low-volatility solvents (such as DMF and DMSO) and reduces the rate of degradation of FA⁺ in the material. Our findings highlight both the critical role of the initial crystallisation process in determining the operational stability of perovskite materials, and that neat FA⁺-based perovskites can be competitively stable despite the inherent metastability of the α-phase.

The development of efficient and robust catalysts for hydrogen evolution reaction is crucial for advancing the hydrogen economy. In this study, we demonstrate that ultra-low coordinated hollow PtRuNi-O_x nanocages exhibit superior catalytic activity and stability across varied conditions, notably surpassing commercial Pt/C catalysts. Notably, the PtRuNi-O_x catalysts achieve current densities of 10 mA cm⁻² at only 19.6 ± 0.1, 20.9 ± 0.1, and 21.0 ± 0.1 mV in alkaline freshwater, chemical wastewater, and seawater, respectively, while maintaining satisfied stability with minimal activity loss after 40,000 cycles. In situ experiments and theoretical calculations reveal that the ultra-low coordination of Pt, Ru, and Ni atoms creates numerous dangling bonds, which lower the water dissociation barrier and optimizing hydrogen adsorption. This research marks a notable advancement in the precise engineering of atomically dispersed multi-metallic centers in catalysts for energy-related applications.

Extracellular matrix (ECM) stiffness influences cancer cell fate by altering gene expression. Previous studies suggest that stiffness-induced nuclear deformation may regulate gene expression through YAP nuclear localization. We investigated the role of the nuclear lamina in this process. We show that the nuclear lamina exhibits mechanical threshold behavior: once unwrinkled, the nuclear lamina is inextensible. A computational model predicts that the unwrinkled lamina is under tension, which is confirmed using a lamin tension sensor. Laminar unwrinkling is caused by nuclear flattening during cell spreading on stiff ECM. Knockdown of lamin A/C eliminates nuclear surface tension and decreases nuclear YAP localization. These findings show that nuclear deformation in cells conforms to the nuclear drop model and reveal a role for lamin A/C tension in controlling YAP localization in cancer cells.

Nanoporous solids, including metal-organic frameworks (MOFs), have long been known to capture small molecules by adsorption on their pore surfaces. Liquids are also known to accommodate small molecules by dissolution. These two processes have been recognized as fundamentally distinct phenomena because of the different nature of the medium—solids and liquids. Here, we report a dissolution-like gas accommodation so-called “adsorptive-dissolution” behavior in a MOF (PFAC-2) with pores densely filled with perfluoroalkyl chains. PFAC-2 does not have solvent-accessible voids; nevertheless, it captures oxygen molecules without changing the framework structure, analogous to molecular dissolution into liquids. Moreover, we demonstrate the selective capture of O₂ by PFAC-2 in a mixture of O₂ and Ar, which are difficult to separate due to their similarities such as boiling point and molecular size. Our results show the integration of molecular adsorption into nanospaces and dissolution into fluorous solvents, which can guide the design of crystalline adsorbents for selective molecular trapping and gas separation.