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Work‐Function‐Modulated Ag Single‐Atom Catalysts for Amino Alcohol Oxidation
ABSTRACT We report Ag single‐atom catalysts for amino alcohol oxidation into amino acids. Using a surface defect trapping strategy, we fabricate a series of Ag 1 /MO x catalysts (M = Ce, Fe, Ti, Zn, Nb) featuring atomic dispersion and tunable electronic states of Ag. Oxygen vacancies on coordinatively unsaturated MO x act as high‐affinity trapping sites to anchor isolated Ag atoms. The electron density of Ag 1 is regulated by the work function of the reducible oxide: low‐work‐function supports induce stronger electron transfer to Ag, generating electron‐enriched Ag δ+ species (0 < δ < 1), while high‐work‐function supports suppress charge transfer and stabilize more electron‐deficient Ag sites. Together with adjacent oxygen vacancies, these tunable Ag δ+ sites enable O 2 activation and subsequent amino alcohol oxidation, delivering an initial rate of 0.81 mol h −1 g metal −1 and 95.1% glycine selectivity in monoethanolamine oxidation. This work establishes a work‐function‐modulated strategy for designing Ag‐based single‐atom oxidation catalysts, demonstrating that amino alcohol oxidation can be efficiently achieved beyond the conventional reliance on Au‐based systems.
Discrete element simulation and dimensionless parameter-based optimization of near-wellbore fracture propagation during perforation fracturing of tight sandstone
Two distinct Okazaki fragment failure modes dominate mutagenesis in the absence of flap endonuclease 1
Abstract The yeast RAD27 gene encodes the Rad27/Fen1 nuclease, which contributes to genome stability during Okazaki fragment maturation (OFM), DNA mismatch repair (MMR), base excision repair, and other processes. Here, we analyze whole genome mutation accumulation in Saccharomyces cerevisiae lacking RAD27 and show that its loss elevates diverse mutation classes arising through multiple mechanistic pathways. Overall mutation rates in rad27 Δ cells are over 60-fold higher than in wild type and only modestly lower than in MMR-deficient strains. However, most mutations in rad27 Δ cells cannot be explained by defective MMR, elevated translesion synthesis, or defects in other Rad27-associated repair processes. Instead, mutation spectra implicate aberrant processing of Okazaki fragment intermediates via DNA terminus slippage before ligation (SBL) and template switching (TS). The latter may arise through replication-associated processes such as transient primer relocation (TPR) or through recombination-mediated mechanisms including homoeologous recombination. SBL accounts for the majority of insertion mutations in rad27 Δ cells, while TS explains substantial fractions of substitutions, insertions, deletions, and copy number variants, often involving non-local templates. Our results indicate that Rad27 suppresses genome instability through multiple mechanistically distinct roles. Together, these findings reveal Rad27/Fen1 to be a determinant of replication-associated genome stability on par with MMR.
Theoretical Screening and Structural Optimization of High‐Performing Li <sub>2</sub> S/Alkaline‐Earth Metal Sulfides Cathodes for Advanced Anode‐Free Li−S Batteries
ABSTRACT Anode‐fre Li−S batteries can achieve extremely high energy density and excellent intrinsic safety by circumventing the direct use of metallic Li. However, the actual output performance is largely constrained by sluggish reaction kinetics and severe structural deterioration of Li 2 S cathode. Here, we report an anchor‐encapsulated nanostructure cooperated with alkaline‐earth metal sulfides’ catalysis to promote Li 2 S kinetics and simultaneously stabilize sulfur species. DFT calculations are first implemented to screen out an optimized MgS electrocatalyst, then a synthetic paradigm of metallothermic‐sulfidation‐carbonization via burning LiMg alloy in CS 2 vapor is proposed to in situ construct Li 2 S‐MgS@graphene nanocapsules. Systematic studies reveal its integrated anchor‐encapsulated structure and synergistic physicochemical interactions among three key components: robust C−S bonding facilitates fast electron/ion transport and stable interface, compact graphene encapsulation alleviates volume change and electrolyte's erosion, and symbiotic MgS bears excellent electrocatalytic effect on Li 2 S dissociation, greatly reducing activation barrier. Owing to the improvement on electrical, catalytic and volumetric properties, this cathode design enables promising electrochemical performance. It demonstrates a great potential for anode‐free Li−S battery and Li 2 S‐MgS@graphene//Cu cell exhibits 823 mAh g −1 initial specific capacity and 73% capacity retention after 100 cycles. Findings in this work are expected to spark a promising direction for designing high‐performing anode‐free batteries.
Elicitor effects of silver nanoparticles (AgNPs) on secondary metabolite–related gene expression in different tissues and differentiation conditions of saffron (Crocus sativus L.)
Charge-spin dichotomy in the kagome metal CsCr3Sb5
Encoding and Encryption via Dual‐Wavelength 3D Digital Light Processing
ABSTRACT Additive manufacturing of multi‐responsive materials is opening new opportunities in a wide range of applications, including information storage, security, and sensing. Herein, complex structures enabling both the encoding and encryption of information in three dimensions (3D) are achieved by combining photo‐ and pH‐responsive chromophores, spiropyran and phenolphthalein derivatives, respectively, within a single ink formulation. To this end, a multi‐wavelength digital light processing (DLP) system is employed to fabricate initially colorless structures using a 405 nm wavelength LED to trigger the photopolymerization process. In parallel, a 365 nm wavelength LED integrated into the same system can induce locally controlled isomerization of spiropyran to the colored merocyanine, enabling information encoding in 3D in a layer‐by‐layer fashion. The stored information can be reversibly encrypted on demand via pH variation. The pH‐responsive chromophore, phenolphthalein, enables modulation of optical contrast, rendering the encoded patterns temporarily unreadable. This work opens new pathways toward engineering multi‐responsive functionality in complex 3D architectures.
Validity and feasibility of the simplified dietary inflammatory index in Chinese older adults
Targeted polar entropy regulation enables superior energy-storage in tungsten bronze multilayer capacitors
Protonation‐Gated Orthogonal Control of Highly Efficient Molecular Motors With Broad Visible‐Light Responsiveness
ABSTRACT Molecular motors with red‐shifted absorption are highly attractive for biomedical applications, yet remain challenging to realize because conventional strategies for extending excitation wavelengths often compromise photochemical efficiency and directional motor function. Here, we report a protonation‐gated strategy in which reversible modulation of conjugation topology enables state‐dependent molecular motor operation across a broad visible‐light window. Modifying coumarin‐derived overcrowded alkenes with benzazole substituents, the resulting motors undergo efficient photoisomerization under blue–green light irradiation. Photophysical studies supported by DFT calculations reveal that protonation induces a pronounced conformational inversion with the formation of intramolecular hydrogen bonds, thereby promoting molecular planarization and enhanced electronic delocalization, leading to the efficient photoisomerization under 530–600 nm irradiation while quantitative photoconversion is retained. Overall, these findings establish reversible protonation as a powerful chemical gating strategy to expand the visible‐light responsiveness of the motor without permanent structural modification, paving the way for its application in multimodal responsive bioimaging and advanced optical devices.
General semantic, personal semantic and episodic details when thinking about the past and the future in moderate-to-severe traumatic brain injury
IL-26-driven epigenetic remodeling promotes immune evasion in colorectal cancer
Reactant‐Sustained Dynamically Stable Interfacial Hydrogen‐Bond Network for Highly Selective, Ampere‐Level Ethylene Glycol Electrooxidation
ABSTRACT The catalyst‐electrolyte interfacial microenvironment fundamentally governs the activity and selectivity of electrochemical reactions. However, engineering a dynamically stable interface capable of sustaining continuous reactant delivery and facilitating proton‐coupled electron transfer remains challenging, particularly under ampere‐level current densities. Herein, a reactant‐enhanced hydrogen‐bond network constructed on an ultrathin metal‐organic framework (MOF)‐derived electrocatalyst (Co‐PET@NF) enables highly selective ethylene glycol electrooxidation (EGOR). Mechanistic investigations reveal that abundant exposed unsaturated Co sites promote preferential EG adsorption for increased EG surface coverage and accelerated replenishment dynamics, ensuring the connectivity and integrity of the interfacial hydrogen‐bond network. This dynamically reinforced network facilitates rapid proton transfer from the catalyst surface into the bulk electrolyte, stabilizing the dehydrogenated active sites while preserving a localized alkaline surface microenvironment. Consequently, Co‑PET@NF achieves a high Faradaic efficiency for formate (FE FA ) of 92.8% at 1.0 A cm −2 . In a coupled hydrogen co‑production system, the cell voltage is reduced by 260 mV at 1.0 A cm −2 compared to water electrolysis, with stable operation over 120 h while delivering an FE FA of 96.9%. Moreover, this mechanism can be extended to other alcohol‐based substances (e.g., methanol and glycerol), elucidating the importance of reactant‐catalyst interfacial hydrogen‐bond interactions in steering alcohol oxidation selectivity and providing a sustainable strategy for biomass and plastic upgrading.
Human precursor labeling in situ reveals a conveyor belt differentiation trajectory and a 6-day neutrophil life span
The kinetics of neutrophil development in human bone marrow remain largely unclear, despite the large implications for the mechanisms underlying host defense and inflammatory responses. Here, in situ DNA labeling was used to follow human neutrophil precursor maturation in bone marrow and blood. Human bone marrow samples were obtained by aspiration from healthy volunteers after short-term (6 hrs) labeling of dividing cells via oral intake of glucose containing the stable isotope deuterium. Mature and precursor populations were isolated at different times by fluorescence-activated cell sorting, and the deuterium incorporation in DNA was measured by GC/MS. Promyelocytes quickly incorporated deuterium in their DNA, whereas in mature neutrophils deuterium was only found from 6 days after intake. The enrichment curves of myelocytes, metamyelocytes, banded, and mature neutrophils mirrored that of the promyelocytes, shifted in time. This pattern indicated that neutrophil development in the bone marrow is well described with a linear conveyor belt model, i.e. following the "first-in/first-out" principle. In contrast to the current dogma, myelocytes did not divide, placing them in the postmitotic pool. Furthermore, the deuterium enrichment curves suggested that mature neutrophils constantly exchange between the bone marrow, blood, and tissue. Our unique labeling data of all stages of the neutrophil life cycle allowed us to estimate the lifespan of the mature neutrophil, deriving a value of at least 6 days. This study provides new insights into neutrophil development kinetics, informing the design and application of therapeutic strategies targeting granulopoiesis and the recruitment of mature neutrophils.
Schizotypy and subclinical depression relate to specific trait curiosity dimensions
Abstract Curiosity promotes human development, but its link to subclinical psychological variations remains poorly understood. In two online experiments, we examined associations of trait and state curiosity with schizotypal characteristics (experiment 1, n = 238) and subclinical depressive symptoms (experiment 2, n = 264) in samples from the general population. In addition to an established multidimensional curiosity framework that allowed us to quantify specific trait curiosity facets, such as Joyous Exploration, Stress Tolerance and Deprivation Sensitivity, we also employed a previously established test to assess state epistemic curiosity. Both schizotypal characteristics and subclinical depressive symptoms were associated with lower Joyous Exploration and Stress Tolerance, while higher Deprivation Sensitivity showed more selective associations with schizotypy. In contrast, state epistemic curiosity did not significantly correlate with schizotypy or depressive symptoms. Together, these findings suggest that trait curiosity dimensions show both shared and selective associations with subclinical depression and schizotypy, potentially reflecting distinct motivational and affective processes. From a broader perspective, this underscores the value of a multidimensional approach to curiosity in mental health.
Bound water as a kinetic crosslinker for bio-inspired impact-stiffening polymers
Engineered Substrates for a Sulfurtransferase Enhance Endogenous Hydropersulfides and Inhibit Ferroptosis
ABSTRACT Cellular hydropersulfides (RS‐SH) derived from hydrogen sulfide (H 2 S) such as glutathione hydropersulfide (GS‐SH) are excellent hydrogen atom transfer agents, and quench radicals to protect cells from ferroptosis, a form of iron‐mediated cell death associated with an unchecked build‐up of lipid radicals. Here, using principles of enzyme‐inhibitor design, a series of new artificial substrates for the endogenous hydropersulfide‐generating enzyme, 3‐mercaptopyruvate sulfurtransferase (3‐MST) was developed. We find that the lead molecules generated GS‐SH, catalyzed by 3‐MST, permeated cells to enhance endogenous hydropersulfides, protected cells from ferroptosis, and reduced systemic inflammation in an animal model. Together, this calibrated approach to promote cell's own radical trapping antioxidants using its biosynthetic machinery to prevent ferroptosis has tremendous implications in redox biology and therapeutics.
Temporal dependency modeling of data inconsistencies in AI-driven ETL systems using graph-based embeddings
Antiretroviral therapy in the peripartum period impairs post pregnancy cardiac reverse remodeling in a rodent model
Abstract Cardiovascular (CV) disease is the leading cause of maternal mortality worldwide and has been partially linked to the cardiometabolic remodeling required to support fetal growth. In healthy pregnancies, these adaptations reverse postpartum without long-term consequences; however, impaired reverse remodeling (RR) increases future CV risk. Pregnant women living with HIV face additional risk, though it remains unclear whether this is driven by chronic low-level viremia or continuous antiretroviral therapy (ART). ART used during pregnancy often includes nucleoside reverse transcriptase inhibitors (NRTIs), which can affect mitochondria - organelles essential for maintaining cardiac function. Here, we tested the hypothesis that NRTI-containing ART negatively impacts the maternal heart. Using a rat model, we show that ART impairs pregnancy-associated cardiac RR. Mechanistically, ART induced mitochondrial alterations in both the heart and the liver, leading to dyslipidemia that collectively compromised cardiac function. These findings emphasize the importance of maternal cardiovascular health research and the need for further studies on the long-term effects of ART.
Interstitial fluid N-glycans serve as a proxy for serum biomarker discovery in a pilot study
Abstract Protein glycosylation is the most prevalent post-translational modification and is known to undergo profound alterations in disease. While serum N -glycosylation has been extensively studied, interstitial fluid is gaining prominence as a minimally invasive biomarker source, underscored by the widespread clinical adoption of wearable glucose monitors in diabetic patients. However, the glycomic landscape of interstitial fluid remains largely unexplored. Here, we have performed a comparative analysis of the N -glycome from interstitial fluid and matched plasma from five healthy volunteers using liquid chromatography, mass spectrometry and exoglycosidase digestions. Strikingly, the interstitial fluid N -glycome closely shows overlapping profiles with the plasma of each individual, with only subtle differences that did not reach statistical significance. Glycosylation profiles were highly individualised, reinforcing the biological specificity of the glycome of each person. These findings demonstrate that interstitial fluid closely reflects systemic N -glycosylation and therefore may represent a powerful, accessible matrix for glycan biomarker discovery. They further support the development of minimally invasive or wearable technologies for monitoring glycosylation-based indicators of disease onset, progression and treatment response.