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Unsaturated Amide Chemistry Enables Ultralong‐Cycling Zn Anode
ABSTRACT Vigorous side reactions and uncontrolled Zn deposition compromise the interfacial stability of Zn anodes, severely impeding the implementation of rechargeable aqueous Zn metal batteries (RAZMBs). Developing facile and efficient strategies to mitigate these issues and achieve ultralong‐cycling Zn anodes remains challenging. Herein, an ultralong‐cycling Zn anode is realized via unsaturated amide chemistry. Specifically, amide‐based surfactants with polar groups (e.g., ─NH 2 ) and unsaturated bonds (e.g., C═C) served as electrolyte additives that specifically adsorb onto Zn anodes, reconstruct the inner Helmholtz plane (IHP) structure, and in situ form a dynamic polymer film (DPF) through electropolymerization during Zn deposition. The tailored IHP and in situ formed DPF synergistically enable a hybrid interphase integrating inorganic rigidity and organic flexibility, which not only effectively suppresses parasitic reactions, regulates Zn 2+ diffusion, and homogenizes Zn deposition, but also accommodates plating/stripping volume variations. Notably, with acrylamide (AAM) as a representative additive in ZnSO 4 ‐H 2 O electrolyte, the Zn||Zn symmetric cell delivers an ultralong cycle life of 5500 h (at 1.0 mA cm −2 and 1.0 mAh cm −2 ), outperforming most reports. These results suggest that the synergistically tailored IHP and in situ formed DPF driven by unsaturated amide chemistry can facilely and efficiently stabilize Zn anodes, providing a promising strategy for the practical application of RAZMBs.
A dual-layer hybrid path planning method for autonomous vehicles via multi-strategy enhanced GWO and adaptive DWA
Subcellular localization as a driver of protein function
Nitrogen‐Doped CeO <sub>2‐x</sub> Supports Accelerate Interfacial Water Dissociation at Surface Pt Sites for Durable Industrial Alkaline Hydrogen Evolution
ABSTRACT Surmounting the high kinetic barrier of water dissociation is a prerequisite for efficient alkaline hydrogen evolution reaction (HER). Herein, we present a nitrogen‐doping strategy for CeO 2‐x supports to tailor the interfacial water microenvironment at supported Pt sites. By leveraging distinct ligand‐directed metal–organic framework precursors, we construct well‐defined Pt−N/O−Ce interfacial coordination motifs. Nitrogen doping not only stabilizes ultrafine Pt clusters via enhanced metal–support interactions but also triggers pronounced interfacial electronic redistribution. Crucially, operando surface‐enhanced Raman spectroscopy reveals that the Pt−N/O−Ce interface promotes the accumulation of weakly hydrogen‐bonded K + ·H 2 O species, which disrupts the rigid interfacial water network and accelerates the rate‐determining water dissociation step. Consequently, the obtained catalyst with Pt−N/O−Ce interface delivers a remarkable mass activity of 13.6 A mg −1 Pt at 100 mV overpotential for HER, representing a 7.6‐fold enhancement over its N‐free counterpart. Demonstrating industrial viability, the Pt/N‐CeO 2‐x @NC achieves 1 A cm −2 at 1.73 V in a large‐area (25 cm 2 ) anion‐exchange membrane water electrolyzer, maintaining exceptional durability over 1600 h at 80°C (degradation rate of 87.5 µV h −1 ). This work elucidates the critical role of N‐mediated interfacial engineering in breaking the water dissociation bottleneck for robust industrial‐scale alkaline electrolysis.
Machine learning-assisted identification and validation of NRP1 inhibitors through molecular docking and dynamics simulations
Photocatalyzed Hydro‐acrylonitrilation of Alkenes
ABSTRACT The catalytic cyanation of alkene feedstocks is a powerful method for introducing highly versatile alkenyl nitrile moieties into organic molecules. These reactions have traditionally relied on transition metal catalysts, hazardous nitrile sources, or prefunctionalized alkenes, which have restricted their potential application in drug discovery. Here, we present the first photocatalytic hydro‐acrylonitrilation of free alkenes using stable 4‐cyano‐3‐oxotetrahydrothiophene (c‐THT) as the cyano source to produce fused alkenyl nitriles with broad substrate scope and excellent functional group tolerance. Unlike previous polar catalysis, c‐THT was first applied in visible‐light catalysis as an acrylonitrile surrogate, allowing this radical‐mediated reaction to occur under operationally simple and mild conditions and enabling numerous functionalized activated and nonactivated alkenes to proceed acrylonitrilation in a highly efficient manner. The synthetic utility was further demonstrated by the gram‐scale preparation and downstream synthetic elaboration toward various valuable building blocks.
A framework based on hybrid Suzuki-Abe and convex Hull approach for improved classification of skin lesions
Tandem Photoelectrochemical Cells for Hydrogen Peroxide With Glyceric Acid Production
ABSTRACT While photoelectrochemical (PEC) oxygen reduction for hydrogen peroxide (H 2 O 2 ) production offers a sustainable alternative to the energy‐intensive and detrimental anthraquinone process for industrial production, continuous and stable long‐term operation remains challenging due to sluggish charge transfer kinetics and poor corrosion resistance of the photoelectrode. Herein, we synthesized a heterojunction photocathode comprising CuO and W‐doped CuBi 2 O 4 decorated with Pd nanoparticles (Pd:CuO/W‐CBO) for efficient and stable PEC H 2 O 2 generation. The optimized photocathode achieves an average Faradaic efficiency exceeding 90% with a low onset potential of 1.08 V RHE , enabling a stable operation for over 50 h at 0.7 V RHE . The CuO overlayer effectively suppresses dissolution of Cu and Bi species, improving the stability of CuBi 2 O 4 ‐based photoelectrodes. More importantly, a bias‐free PEC system utilizing the Pd:CuO/W‐CBO photocathode and a Pt/TiO x anode was constructed for simultaneous solar‐driven H 2 O 2 production and electrochemical glycerol oxidation to high‐value chemicals. This unassisted system delivers a current density of 3.75 mA cm −2 under one sun illumination. Further employing a large‐scale photocathode (10 cm 2 ) enables H 2 O 2 and C 3 chemical production rates of 250.4 and 127.6 µmol h −1 , respectively. Regulating H 2 O 2 permeation using an anion exchange membrane considerably enhances the selectivity to 56% for oxidation of glycerol to glyceric acid, markedly outperforming systems using proton/cation exchange membranes (∼20%). Additionally, the cathodically generated H 2 O 2 enables rapid water disinfection, achieving >99.9% bacterial inactivation within 180 min. This work demonstrates a scalable PEC platform for stable concurrent solar‐driven H 2 O 2 generation and glycerol valorization while enabling energy conversion.
Direct comparison of mechanical circulatory support devices in porcine model of acute myocardial infarction complicated by ventricular septal defect and cardiogenic shock
Glycine‐Induced Unique Crystal Packing of Octacyanidetungstates With Strong Intermolecular Antiferromagnetic Interaction, Near‐Infrared Emission, and Second Harmonic Generation
ABSTRACT We report a supramolecular assembly of octacyanidetungstates ( S = 1/2) with glycine, Cs 3 [W V (CN) 8 ](glycine), featuring a one‐dimensional columnar structure with a remarkably strong intermolecular antiferromagnetic superexchange interaction of J = −42.41(2) K between adjacent octacyanidetungstates due to their effective packing close to van der Waals contacts. This represents the strongest intermolecular spin‐spin interaction reported to date among cyanidemetallates. When exposed to 470 nm light, this compound exhibits a near‐infrared emission with a peak at 763 nm originating from the ligand‐to‐metal charge‐transfer excited state of [W V (CN) 8 ] 3− . Such emission is notably rare for d 1 metal complexes. Additionally, the noncentrosymmetric crystal structure of this compound enables second harmonic generation, emitting second harmonic light at 650 nm when irradiated with 1300 nm incident light.
Multi-scale attention and collaborative fusion for enhanced RGB-D salient object detection in weld quality inspection
Unlocking Efficient Spontaneous Deracemization: A MOF‐Mediated Heterogeneous System Overcomes Catalytic Incompatibility in Cocrystallization
ABSTRACT Cocrystallization‐induced deracemization is a powerful route to enantiopure pharmaceuticals, yet is hindered by detrimental interactions between homogeneous catalysts and chiral components. Herein, we report a novel heterogeneous catalysis strategy using metal–organic frameworks (MOFs) to overcome this compatibility challenge. By encapsulating the base catalyst 1,8‐diazabicyclo[5.4.0]undec‐7‐ene (DBU) into ZIF‐8, we created a ZIF‐8@DBU composite catalyst, that effectively isolates the catalyst while preserving its racemization activity. This enabled the efficient deracemization of racemic DMY via cocrystallization, selectively yielding either the (2 R ,3 R )‐ or (2 S ,3 S )‐enantiomer simply by switching the handedness of the coformer, N‐benzyl‐1‐phenylethylamine (NBP). Remarkably, the product yield reached up to 52%, surpassing the 50% theoretical limit of conventional chiral resolution techniques. The strategy proved general, extending successfully to ZIF‐67@DBU and ZIF‐90@DBU. This work demonstrates the feasibility of using tailored MOF composites to overcome long‐standing compatibility barriers in deracemization and opens avenues for their broader application in asymmetric synthesis.
Deep learning-based semantic segmentation of night-sky clouds for operational telescope scheduling
Abstract Ground-based optical telescopes necessitate prompt and spatially detailed information regarding dome-scale cloud coverage to facilitate target-specific shuttering and scheduling decisions. When only coarse or delayed atmospheric data are available, observatories risk inefficient use of scarce dark time and the irreversible loss of scientific exposures. To address this, we introduce the WOANC dataset, a pixel-annotated nighttime full-dome dataset acquired at an operational observatory, alongside NightCloudSegNet, a fisheye-aware segmentation framework specifically designed for low-light astronomical imaging. Evaluated on the WOANC test set, NightCloudSegNet achieves a mean intersection-over-union (mIoU) of 86.6% and a pixel-level F1 score of 92.8%. Furthermore, when tested on the external SWINSEG dataset, the model attains an mIoU of 86.2% and an F1 score of 92.6%, thereby demonstrating robust performance under conditions of fisheye distortion and low illumination. By translating pixel-level segmentation masks into per-target observability indicators, this approach has the potential to support informed shuttering and scheduling decisions, which is expected to enhance observational efficiency in automated telescope operations.
Spontaneous, Catalyst‐Free Co‐Polymerization of Ionic Liquids With CO <sub>2</sub> Toward Polycarbonate
ABSTRACT The conversion of carbon dioxide (CO 2 ) into value‐added polymer is a cornerstone of sustainable chemistry, yet current strategies typically require high pressures, metal catalysts, and yield materials with limited functionality. Herein, we report a spontaneous, catalyst‐free polymerization that directly converts CO 2 and hydroxyl‐functionalized ionic liquids (ILs) into multifunctional ionic polycarbonates under ambient conditions (0.1 MPa, 60°C). Mechanism studies, combining spectroscopic analysis and density functional calculations, elucidate a synergistic process wherein IL cations function as CO 2 concentrators, while OH − anions drive the polymerization via a bicarbonate‐mediated nucleophilic pathway. This approach yields a well‐defined ionic polycarbonate that uniquely integrates high ionic conductivity (>10 − 4 S·m − 1 ), dual‐wavelength fluorescence, broad‐spectrum antibacterial activity (>99% inhibition against E. coli and S. aureus ), and performance as a multifunctional adhesive enhancer with self‐monitoring capability. Furthermore, these polymers undergo complete degradation into monomeric constituents, establishing a closed‐loop monomer‐polymer‐monomer lifecycle. This work provides a paradigm for sustainable CO 2 valorization into advanced multifunctional materials, with immediate potential in smart adhesives, wearable electronics, and information encryption.
Real-time dynamic monitoring of rockfalls with PTZ cameras
Metallaphotoredox‐Catalyzed Acceptorless Dehydrogenative Carbonylation Employing Benzylic C─H Bonds as Limiting Substrates
ABSTRACT We report a visible light‐driven, metallaphotoredox‐catalyzed acceptorless dehydrogenative carbonylation of benzylic C─H bonds with carbon monoxide and nucleophiles. Enabled by a long‐chain diphosphine ligated nickel(II) bromide complex, this protocol uniquely employs C(sp 3 )─H bonds as limiting reagents under ambient temperature and CO atmosphere, affording esters and related carbonyls under oxidant‐free conditions with H 2 as the sole byproduct. The reaction exhibits broad substrate scope, tolerating diverse functional groups and complex bioactive scaffolds. Mechanistic studies are consistent with a pathway involving photoinduced hydrogen atom transfer and nickel‐mediated carbonylation.
Reducing skin tone bias in dermatology AI via sketch-guided multimodal fusion
Abstract AI-driven skin lesion diagnosis systems are revolutionizing dermatology practice but perform worse on darker skin populations, which threatens diagnostic equity in dermatology. Existing debiasing strategies rely on explicit skin tone annotations or adversarial removal of demographic information, which may be unavailable in practice and can harm diagnostic accuracy. We aimed to design a dermatology AI system that reduces skin-tone-related performance disparities across diverse skin populations without using skin tone labels during training. We propose a novel sketch-guided multimodal fusion framework that combines color (RGB) images with algorithmically generated structural sketches. Separate encoders extract representations from each modality, which are integrated by a gated fusion module that adaptively weighs color and structure features. A feature distillation loss aligns color features with their sketch counterparts to encourage structure-aware representations while retaining clinically relevant color cues. We trained and evaluated the model on the Fitzpatrick17k and Diverse Dermatology Images (DDI) datasets. The fairness performance was assessed with Equalized Opportunity, Equalized Odds, and Predictive Quality Disparity across skin tone groups. Out-of-domain robustness was examined using a DermaAmin and Atlas Dermatologico split. On Fitzpatrick17k, the proposed model yielded competitive accuracy and F1-score, while showing lower mean disparity in fairness evaluation than baseline methods. It also demonstrated reduced subgroup disparity across skin tone groups on the evaluated fairness metrics. In the out-of-domain evaluation setup, the model also exhibited improved fairness. On the DDI dataset, the framework showed consistent performance across different skin tone groups with reduced variation. Our proposed model shows promise in reducing skin-tone-related bias in dermatology while preserving utility without relying on explicit skin tone annotations. The observed improvements in skin tone fairness across two datasets suggest that our approach may help reduce measured subgroup disparities in automated skin lesion assessment, although clinical utility and real-world impact remain to be established through prospective validation.
Wrinkled Strain‐Enriched High‐Entropy Metallene Enables Cross‐Site Tandem Nitrate‐to‐Ammonia
ABSTRACT High‐entropy alloys (HEAs) are interesting for sustainable electrocatalytic nitrate‐to‐ammonia but suffer from low atom utilization and insufficient exposure of active sites. Here, we report a wrinkled PdFeCoNiCuIn high‐entropy metallene (HEM) that leverages a structural‐electronic dual regulation strategy to transcend these limitations. The incorporation of the p‐block element indium (In) triggers a strong p‐d orbital hybridization that synergizes with the intrinsic metallene architecture to construct a broad adsorption energy landscape. This architecture enables a cross‐site tandem catalytic pathway that spatially decouples nitrate activation from ammonia desorption, thereby circumventing scaling constraints. Consequently, the PdFeCoNiCuIn‐HEM delivers a remarkable ammonia Faradaic efficiency of 99.3% and a yield rate of 4.55 mmol h −1 mg cat −1 . Furthermore, the rechargeable Zn‐NO 3 − battery assembled with the PdFeCoNiCuIn‐HEM as cathode achieves a high open‐circuit voltage of 1.48 V, a power density of 7.36 mW cm −2 , and stable cycling over 100 h. This work provides a practical and generalizable design strategy for developing efficient NRA catalysts.
Growth need strength promotes employee creativity through work reflection with visionary leadership as a moderator
Abstract Employee creativity is crucial for organizations to maintain competitiveness. Although existing research has explored the relationship between employees’ growth need strength and creativity, the underlying connection between the two remains unclear. Based on trait activation theory, this study examines how visionary leadership, as an environmental cue, activates employees’ growth need strength, thereby promoting work reflection and creativity. Data were collected from 516 full-time employees across 111 teams using a three-phase, time-lagged design. Multilevel path analysis and Monte Carlo simulations were used to test the hypotheses. The results showed that employees’ growth need strength is positively related to creativity. Work reflection mediates the relationship between growth need strength and creativity. Visionary leadership strengthens the positive relationship between employees’ growth need strength and work reflection. Visionary leadership also moderates the mediating role of work reflection in the relationship between employees’ growth need strength and creativity. These findings contribute to the employee creativity literature by highlighting work reflection as an important mechanism and visionary leadership as a key contextual condition through which growth need strength promotes creativity.
Supramolecular Modulation of Photoinduced Charge Transfer: Tuning Between Tunneling and Incoherent Hopping
ABSTRACT Photoinduced charge transfer (CT) underpins photosynthesis and solar energy conversion technologies. However, achieving comprehensive control over CT in traditional covalent donor−bridge−acceptor (D−B−A) systems remains challenging, hindered by tedious organic synthesis and limited tunability. In this investigation, we harness molecular recognition to regulate photoinduced CT—including charge separation and recombination—leveraging its facile preparation and dynamic reversibility. By integrating guest molecules with a wide range of frontier orbital energies into a rigid cyclophane host ( DAPPTTzBox 4+ ), which features directional photoinduced intramolecular CT through cofacially stacked chromophores, we achieve comprehensive modulation of CT within well‐defined supramolecular complexes. This modulation spans mechanisms from tunneling to incoherent hopping. Notably, molecular recognition accelerates charge separation in DAPPTTzBox 4+ by 5.9‐ to 230‐fold, shifting from single‐step superexchange to multistep incoherent charge shift, while charge recombination rates are decreased (from 1.3‑ to 2.8‑fold) in superexchange systems. Additionally, guest‐induced charge trapping was also successfully demonstrated. This research exemplifies a fresh strategy for manipulating CT dynamics via noncovalent interactions, opening new avenues for the design of advanced artificial light‐harvesting materials.