Nature Communications最新文献

Manipulating the selectivity-determining step in the hydrogenation of nitrogen-containing intermediates is critical to achieving high ammonia selectivity in electrocatalytic nitrate reduction. Here, we propose a molecular interface engineering strategy that functionalized with thiol-anchored aromatic ligands to regulate the interfacial binding affinity and activation of key nitrogen-containing intermediates on silver nanocube surfaces. By systematically varying the electronic properties of the substituents, we identify 4-(methylthio)benzaldehyde as the most effective ligand, increasing the ammonia Faradaic efficiency from 50.8% to 98.9% and achieving a yield rate of 14,366.1 μg h^-1 cm_geo^-2 at -0.63 V versus reversible hydrogen electrode. In situ electrochemical characterizations combined with theoretical simulations further reveal that 4-(methylthio)benzaldehyde modification promotes the activation of weakly hydrogen-bonded water molecules and accelerates the hydrogenation of *HNO intermediates. This targeted modulation of interfacial binding affinity offers an effective strategy for selectivity control in electrocatalytic nitrate reduction. The enhanced performance is further validated in a membrane electrode assembly electrolyser, underscoring the practical viability of this molecular design strategy for selective nitrate conversion.

Soft and conducting organic materials are ideal candidates for stretchable bioelectronics and wearable devices. Despite recent advances, our understanding of conducting polymer nanostructures and how they arise remains incomplete, given the limited high-resolution studies and molecular-level descriptions of these systems. Here, we employ cryogenic transmission electron microscopy (cryo-EM) to investigate the evolution of poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) morphology in solution and the resulting solid state structure in the presence of ionic and molecular additives. Our results reveal the formation of heterostructural elongated fibers consisting of PEDOT:PSS micelles in solution. Cryo-EM further reveals that additives increase the number of fibrils, in addition to inducing the formation of crystalline domains. We observe that fibril and crystalline phases in solutions act as a template for the growth of these nanostructures in the solid state. Furthermore, exploiting cryo-EM reveals the role of solid-liquid interactions in PEDOT:PSS through the imaging of PEDOT:PSS nanostructures after the hydration of thin films. Hydration leads to the swelling of heterostructural fibers while reducing the crystalline domain size. Such behavior explains the mechanical robustness of PEDOT:PSS thin films processed with various additives as well as the high electrical conductivity of PEDOT:PSS in applications such as organic electorchemical transistors.

Protected areas (PAs) are central to China's forest conservation strategy, yet their effectiveness for carbon storage across governance and management contexts remains unclear. A clearer understanding of their current and future carbon benefits is essential for informing conservation and climate policy. Here, using 1-km GEDI satellite data, we show that forests within China's PAs store on average 68.29 ± 0.17 Mg C ha⁻¹ - about 13% more than matched unprotected forests. Carbon gains are highest in national parks (18.19 ± 0.69 Mg C ha⁻¹) and in managed naturally regenerating forests (9.85 ± 0.36 Mg C ha⁻¹), although some PA categories underperform. To assess future potential, we integrate GEDI observations with CMIP6 climate projections and find that under the high-emission SSP5-8.5 climate scenario, strongly protected areas could retain an additional ~600 ± 36.39 Tg C by 2100. These results show that strong protection and optimized management substantially enhance China's carbon sink, offering major opportunities for climate mitigation and biodiversity conservation.

Influenza A viruses (FLUAV) utilize sialic acid to enter host cells via the envelope's hemagglutinin (HA), and its affinity for host-specific sialic acid linkage configuration is a major host range determinant. However, some FLUAV subtypes (H17, H18, H19) use the major histocompatibility complex class II (MHCII) as an entry receptor instead of sialic acid (SA), challenging our knowledge about FLUAV tropism and interspecies transmission potential. Here, we show that H3N2 viruses can use MHCII as an alternative entry receptor in a host-specific manner, and adaptation of human viruses to pigs increases affinity for the MHCII swine leukocyte antigen (SLA). By using two prototypic human-seasonal (hVIC/11) and swine-adapted (sOH/04) H3N2 viruses we found that expression of the human (HLA) but not the swine MHCII conferred replication of hVIC/11 in desialylated, non-susceptible cells. Further, expression of SLA in non-susceptible cells conferred susceptibility to infection by sOH/04. Introduction of point mutations near the hVIC/11 HA receptor-binding site (RBS) allowed the use of both human and swine MHCII. Our findings revealed that MHCII can serve as a sialic acid-independent entry receptor to H3N2 FLUAV in a host-specific manner, with potential implications for the viral pathogenesis and adaptation to a new species.

Autonomous motion in a persistent manner such as spinning of Euler's disk is long-sought-after by natural or artificial microsystems due to their limited energy loading and is particularly challenging for Marangoni motors as inhomogeneity of active molecules is difficult to sustain. Here we show that by releasing a droplet containing hydrogel precursor and non-small active molecules on a diluted crosslinking-agent solution, the droplet self-propels with a lifetime 300-to-1000-fold longer. It is found that continuously crosslinking hydrogel shell cuts rapid surfactant diffusion and accompanying volumetric contraction perforates the shell and generates a vent through which active molecules are unidirectionally released. The mechanism echoes squid's jet propulsion wherein water is expelled out of a siphon by contracting mantle. Such self-generated contracting mantle-siphon configuration of a gelling droplet maximizes the localized concentration inhomogeneity and protracts adsorption saturation on water surface, improving the efficiency and lifetime of Marangoni motors for sustained powering of interfacial machines. The unfolded strategy potentially provides solutions for microscale release control which will be of interest to microrobots, materials assembly, and biomolecules transport.

Bioorthogonal chemistry has become a robust toolbox with growing applications in biology and medicine. To meet diverse needs in research, new types of on-demand bioorthogonal reactions capable of responding to biological triggers or exogenous stimuli are highly valuable, to achieve spatial and temporal control over reactions in living systems. Elevated levels of reactive oxygen species have been implicated in aging and multiple diseases, serving as remarkable endogenous triggers for prodrugs, probes and materials, however ROS-activated bioorthogonal ligation remains as a challenge. Here we report a reactive oxygen species activated tetrazine ligation enabled by boronate-caged dihydrotetrazines. Bioorthogonal handle tetrazines can be in situ generated from boronate-caged dihydrotetrazines upon the elevated level of hydrogen peroxide, resulting in spatiotemporal control of subsequent reactions with dienophiles. Using this strategy, a reactive oxygen species triggered construction of proteolysis targeting chimera for targeted degradation of the protein of interest bromodomain-containing protein 4 (BRD4) is successfully established by tagging boronate-caged dihydrotetrazines with a cereblon E3 ligase recruiter. Furthermore, we demonstrate a reactive oxygen species triggered tetrazine ligation enabled tumor-selective drug delivery in both living cells and mice. The present reactive oxygen species responsive delivery of cytotoxin doxorubicin via a click-to-release reaction between boronate-caged dihydrotetrazines and trans-cyclooctene modified doxorubicin shows excellent chemotherapeutic efficacy and safety in suppressing the growth of some tumors, superior to both direct administration of doxorubicin and reactive oxygen species sensitive prodrug of boronate-caged doxorubicin. We expect this reactive oxygen species responsive bioorthogonal reaction will offer compelling opportunities for precision therapy and provide approaches for studying pathogenesis.

Commercial shipping is a cornerstone of global trade. Its impact on the marine environment, however, remains underexplored. This study combines hydroacoustic data, sediment samples, propeller-induced shear stress calculations and vessel tracking information to assess the effects of shipping in one of the busiest maritime regions in the Baltic Sea, the Bay of Kiel. We unveil substantial seafloor erosion, including up to 1.5 m variation in water depths, over 10 years that clearly relates to vessel traffic. By imaging water column disturbance behind passing ships, we trace wake turbulence to the seafloor and show the breakdown of a strongly stratified water column and a possible excitement of internal waves, likely increasing the mixing of oxygen, nutrients, and greenhouse gases. While the environmental consequences of this anthropogenic stressor are unquantified, our findings leave little doubt that they include modifications to marine ecosystems and element budgets on a Baltic-wide scale.

Pretraining on a large number of unlabeled 3D molecules has showcased superiority in various scientific applications. However, prior efforts typically focus on pretraining models in a specific domain, missing the opportunity to leverage cross-domain knowledge. To mitigate this gap, we introduce Equivariant Pretrained Transformer, an all-atom foundation model that can be pretrained from multiple domain 3D molecules. Built upon an E(3)-equivariant transformer, the model learns both atom-level interactions and graph-level structural features (e.g. residuals in proteins), allowing it to generalize across diverse tasks. The model achieves strong gains in ligand binding affinity prediction, while also performing competitively in predicting properties of proteins and small molecules. We further show that the model can help identify potential antiviral compounds against the main protease of the COVID-19 virus, and validate promising candidates through computational and experimental studies.

Creating a catalogue of early diverged genome variation is critical to determine the true extent of human diversity and associated medical impact. Generating deep whole genome data for 150 Khoe-San (12 groups, 1 unclassified), and 40 regionally comparative Southern Africans (3 groups), we identify ~30 million small-to-large variants - over 1.3 million unknown single nucleotide variants. Representing shared traditionally forager lifestyles and click-speaking languages, we identify San and Damara as separate phylogenetic lineages, contributing two admixture waves to Nama. While San represented modern humans' deep divergence (~115 thousand years ago), Damara divergence is recent, with both showing high effective population sizes between 45-150 thousand years ago. Developing an assembly-based test we report 1,376 genes under positive selection (dN/dS = 19.46) of which 479 are significantly associated with forager peoples and, therefore, maintained ancestral alleles that differ from derived genetic variation observed in non-African biomedical resources.

Although cobalt spinel oxide-based catalysts have demonstrated promising performance for the oxygen evolution reaction in acid, strategies reported have largely focused on manipulating the binding energies of reaction intermediates through tailoring the inherent electronic structures. The role of interfacial water structures on the electrode surface in promoting the acidic oxygen evolution reaction performance through controlled water activation has been largely overlooked. Here we show that introducing chromium dopant into cobalt spinel oxide can simultaneously increase the activity and stability by promoting interfacial water dissociation and dynamic electron transfer. The chromium dopant can not only dynamically regulate the electronic structure of cobalt and mitigate the over-oxidation of active cobalt sites at high overpotential, but also enhance the coverage of hydroxyl species on the catalyst surface, thereby optimizing the interfacial water structure, accelerating the reactant free-water supply and promoting subsequent interfacial water dissociation. Consequently, the obtained catalyst demonstrates enhanced performance in both solution electrocatalysis and device electrocatalysis. This work provides a comprehensive understanding of enhancing the acidic oxygen evolution reaction performance by promoting interfacial water dissociation.