In Situ Electrochemical Oxidation for High-Energy-Density Aqueous Batteries: Mechanisms, Materials, and Prospects.

To advance the commercial utilization of aqueous electrochemical devices for grid-scale energy storage, it is crucial to address the current limitations related to energy density and cycle stability. Indeed, the lack of high-performance cathodes is still an obstructive issue, not to mention the limited capacities related to the monotonic cation intercalation/deintercalation mechanism. Fortunately, conversion chemistries with redox reactions bring a new dimension, where materials with multiple valence states facilitate multi-electron redox reactions, offering the potential for high-energy-density storage.

Semiconductor Cluster with High Reduction Potential and Efficient Charge Transfer Enables Visible-Light-Driven Activation of Inert Organic Substrates.

Photoredox catalysis is an essential component of modern organic synthesis. However, current photocatalysts face the challenge of simultaneously requiring strong redox potentials and efficient charge transfer to meet the thermodynamic and kinetic demands of photoinduced electron transfer processes. Herein, we present an excellent reactivity mode for photocatalysis based on semiconductor clusters, exploiting the ideal Marcus parabola to couple potential and kinetic requirements.

Selenolated Copper Hydride Clusters for Visible-Light Photocatalytic Iodofluoroalkylation of Alkynes.

The photocatalytic iodofluoroalkylation of unsaturated systems is of great interest, with significant potential in the synthesis of fluorinated compounds. Herein, we introduce a selenate-protected hydride cluster, [CuH(dppy)(PhCHSe)](PF) (dppy = diphenyl-2-pyridylphosphine, PhCHSe = benzylselenate), that enables visible light-mediated iodofluoroalkylative difunctionalization of alkynes. Single crystal X-ray structural analysis reveals that the cluster comprises a hydride-embedded hexagonal close-packed Cu kernel of the symmetry, coprotected by benzylselenate and dppy ligands.

Universal Artificial Urinary Biomarker Probe Enabled by an Aptamer-DNAzyme-Nanozyme Construct.

Artificial urinary biomarker probes (AUBPs) have recently emerged as a new class of diagnostic tools. However, they are applicable only to the biomarkers with catalytic activities or high reactivities. Here, we present a general modular design of AUBPs, integrating an aptamer for target recognition, DNAzyme for triggerable signal transduction, and nanozyme as a urinary artificial biomarker.

A novel damage detection method based on sequential iteration and Gaussian mixture model for structural health monitoring under environmental effects.

Environmental effects often cause variability in dynamic features, obscuring actual damage indicators and leading to false alarms in damage detection. The Gaussian mixture model (GMM) based method is an effective solution, but challenges such as selecting initial model parameters and determining the optimal number of Gaussian components can hinder its performance. To address these challenges, we propose a two-step method that combines sequential iteration with the GMM approach.

Spatial-Interactive Synergistic Confinement in Isoreticular Metal-Organic Frameworks for Facilitating CH Separation from CO with Record Packing Density.

The synchronous implementation of precise molecule recognition and efficient gas accumulation in porous materials is highly desirable but challenging for physisorptive separation/storage applications. Here, we demonstrate the feasibility of achieving effective acetylene (CH) purification from a CH/CO mixture with record-high gas packing density by modulating the pore size and interpenetrating symmetry in three isomorphic pillar-layered MOFs (CTGU-41/42/43). The 1D rectangular narrow channels and regularly arranged paired binding sites trigger spatial-interactive synergistic confinement (SISC), enabling suitable molecular orientation and spacing distances during CH adsorption within these MOFs.

A Porous MOF Containing Accessible Open Metal Sites with Low Steric Hindrance for Selective Separation of Hydrocarbons.

Conventional hydrocarbon production yields impure products, while solvent-based purification techniques emit volatile pollutants and are energy-intensive. Metal-organic frameworks (MOFs) with open metal sites (OMSs) offer an energy-efficient and eco-friendly alternative, yet steric hindrance from OMSs with traditional geometries restricts multimolecule adsorption. Herein, a stable incorporating novel seesaw-geometry OMSs was constructed using a 1,3,5-tris(pyrazolyl)benzene ligand.

Somatostatin receptor 2 targeting peptide modifications for peptide-drug conjugate treatment of small cell lung cancer.

Peptide-drug conjugate (PDC) represents a special therapeutic strategy to enhance drug delivery by targeting tumor cell receptors while minimizing off-target effects. Comparing the antibody-drug conjugate (ADC), the targeting peptide constitutes the pivotal component of PDC, especially with easy optimization of peptides to promote their in vivo stability, and with the agonist stimulated GPCR internalization to facilitate drug distribution into tumor cell plasma. Herein, we have optimized a highly stable peptide molecule LanTC targeting somatostatin receptor 2 (SSTR2), through amino acid substitution and disulfide bond modification from an FDA proved peptide drug Lanreotide.

Hemoporfin-Mediated Photodynamic Therapy-Caused Skin Barrier Damage and Triggered Dermatitis in Port-Wine Stains.

Background: Hemoporfin-mediated photodynamic therapy (PDT) is a high efficacy treatment alternative for port-wine stains (PWS) patients, and PDT also induced eczematous dermatitis in treated areas. However, the effect of PDT treatment on the prevalence and risk of dermatitis in patients with PWS have not been reported.

Purpose: To assess the association between PDT and dermatitis incidence and to investigate the mechanism of PDT-triggered dermatitis in PWS patients.

Valence Electron Fluctuation in a High-Entropy Oxide Heterojunction Enables Collaborative Photodynamic and Mild-Thermal Therapy for Cutaneous Biofilm Infections.

Mild photothermal therapy combined with photodynamic therapy has emerged as an effective treatment for antibiotic-resistant infection. However, controlling operation temperature within a safe range during reactive oxygen species (ROS) production remains a challenge. Herein, we present a functional heterojunction consisting of TiCT-MXene and (CoCrFeMnNi)O high-entropy oxide (HEO) featuring a valence electron fluctuation effect, achieving a highly efficient treatment of biofilm-associated infections in wounds and abscesses under mild conditions where skin temperature remains below 42.

Interweaving Covalent Organic Polymer Chains Into Two-Dimensional Networks: Synthesis, Single Crystal Structure, and Application for Stabilizing Lithium Metal Anode.

Macroscopic weaving has been proven to be the most enduring and effective method for manufacturing fabrics to meet the practical needs of humanity for thousands of years. However, the construction of molecular structures with exquisite topologies and specific properties based on molecular weaving is still in its infancy. Herein, we designed and fabricated a two-dimensional (2D) woven covalent organic polymer (COP) network (named as CityU-46) driven by the dative N→B bonds between the 1,4-bis(benzodioxa-borole)benzene (BACT) and 2,5-bis(4-pyridyl)-1,3,4-thiadiazole (BPT).

Core-Shell MIL-125-NH@FeOOH Nanocomposites for Highly Selective Photocatalytic Oxidation of Methane to Formaldehyde in Water Vapor.

Formaldehyde (HCHO), a crucial industrial chemical, finds extensive applications across diverse sectors, including household products, commercial materials, aviation, and medical supplies. Methane (CH), as an abundant C1 resource, presents a promising feedstock for HCHO synthesis. However, the direct conversion of CH to HCHO remains challenging due to its inherent chemical inertness, characterized by low polarizability and high C-H bond dissociation energy (439 kJ mol), coupled with the high reactivity of intermediate products.

Partial normalization of microbiota dysbiosis in condyloma acuminatum patients following treatment.

Introduction: Condyloma acuminatum (CA) is the most common sexually transmitted disease and the presence of microbiota dysbiosis has been observed to promote the progress of the disease. However, the explicit characteristics of microbiota dysbiosis in CA patients have not been well elucidated yet.

Methods: We recruited 40 CA patients who received QYXJ (an in-hospital prescription that has been used to treat CA for many years) treatment and 40 healthy controls (HC) in the current study.

Utilizing Photothermal Effect Enhances Photocatalytic Water Splitting Coupled with Selective Benzyl Alcohol Oxidation over Schottky Junctions.

As is well known, there are problems such as low utilization rate of photogenerated holes and resource consumption of sacrificial agent in solar-driven photocatalytic water splitting to hydrogen technology. Herein, WC quantum dots decorated defective ZnInS nanosheets (DZIS/WCQDs) dual-functional photocatalysts are fabricated. Its unique Schottky junctions and photothermal effect significantly promote the separation and transport efficiency of photogenerated carriers, as well as achieving synergistic enhancement of photocatalytic water splitting coupled with selective oxidation of benzyl alcohol (BA).

Construction of Local-Ion Trap in Phase-Reversed Mixed Matrix COF Membranes for Ultrahigh Ion Selectivity.

Artificial molecular/ion traps afford grand potential in membrane-based separation processes. However, the existing trap-based architectures often confer over-strong binding forces, which severely impede the release of bound solutes during their transmembrane diffusion processes. Herein, we propose an unprecedented local-ion trap bearing moderate binding force and additional repulsion force in a type of phase-reversed mixed matrix covalent organic framework (PRCOF) membrane.

An Electrochemically-Driven Reconstruction Strategy to Realize Highly Crystalline Covalent Organic Frameworks for Enhanced Hydrogen Evolution Reaction.

Developing diverse methods to approach highly crystalline covalent organic frameworks (COFs) for improvement of their electrocatalytic hydrogen evolution reaction (HER) activity is important but very challenging. Herein, for the first time, an electrochemically-driven reconstruction strategy is demonstrated to convert semi-polymerized low-crystalline COFs into highly crystalline, structurally ordered COFs with enhanced HER activity. In situ and ex situ characterizations reveal that cyclic voltammetry (CV) cycles can promote crystallinity, thereby leading to improved conductivity, increased active site density, and superior stability.

Opto-digital molecular analytics.

In contrast to conventional ensemble-average-based methods, opto-digital molecular analytic approaches digitize detection by physically partitioning individual detection events into discrete compartments or directly locating and analyzing the signals from single molecules. The sensitivity can be enhanced by signal amplification reactions, signal enhancement interactions, labelling by strong signal emitters, advanced optics, image processing, and machine learning, while specificity can be improved by designing target-selective probes and profiling molecular dynamics. With the capabilities to attain a limit of detection several orders lower than the conventional methods, reveal intrinsic molecular information, and achieve multiplexed analysis using a small-volume sample, the emerging opto-digital molecular analytics may be revolutionarily instrumental to clinical diagnosis, molecular chemistry and science, drug discovery, and environment monitoring.

Significantly enhanced NIR emission of solid-state clusters based on CuPt triggered with volatile organic compounds.

Near-infrared (NIR) emitting metal clusters, recognized for their low toxicity, large Stokes shift, and exceptional photostability, hold considerable promise as stimuli-responsive luminescent materials for applications including organic vapor sensing, pollutant detection, and photoluminescent thermometers. However, their limited quantum yield (QY) for NIR emission poses a challenge, highlighting the need for developing light-up sensors with NIR emitting metal clusters to broaden the scope of applications. Herein, the carbazole-alkyne ligand-incorporated novel bimetallic cluster, CuPt(CZ-PrA)(dppy)(PF) (CZ-Cu4Pt2, CZ-PrAH = 9-(Prop-2-yn-1-yl)-9-carbazole; dppy = diphenyl-2-pyridylphosphine), was synthesized, which exhibits NIR emission centered at 740 nm in the solid state and shows a significant blue shift compared to the previously reported analogues.

Photoinduced Cobaloxime-Catalyzed Regio- and Diastereoselective Hydrogen-Evolution C(sp)-H Phosphorylation of Bicyclo[1.1.0]butanes.

Radical-initiated functionalization of bicyclo[1.1.0]butanes (BCBs) is a straightforward approach to accessing diverse cyclobutane derivatives.

Multiscale Understanding of Anion Exchange Membrane Fuel Cells: Mechanisms, Electrocatalysts, Polymers, and Cell Management.

Anion exchange membrane fuel cells (AEMFCs) are among the most promising sustainable electrochemical technologies to help solve energy challenges. Compared to proton exchange membrane fuel cells (PEMFCs), AEMFCs offer a broader choice of catalyst materials and a less corrosive operating environment for the bipolar plates and the membrane. This can lead to potentially lower costs and longer operational life than PEMFCs.

Severe interstitial lung disease risk prediction in anti-melanoma differentiation-associated protein 5 positive dermatomyositis: the STRAD-Ro52 model.

Objective: Anti-melanoma differentiation-associated gene 5-positive dermatomyositis-associated interstitial lung disease (MDA5DM-ILD) often leads to acute respiratory failure and endangers lives. This study quantitatively analysed chest high-resolution computed tomography (HRCT) images to assess MDA5DM-ILD and establish a risk prediction model for severe ILD within six months.

Methods: We developed a 'Standardized Threshold Ratio Analysis & Distribution' (STRAD) to analyse lung HRCT images.

Photothermally-enhanced ferroptotic-chemo therapy enabled by ZIF-derived multizyme.

A multi-functional single-Fe-atom nanozyme (Fe-SAzyme) is designed, integrating the near-infrared photothermal property, the ability to carry chemoagent (doxorubicin - DOX), and nanocatalytic activities mimicking peroxidase, oxidase, and glutathione oxidase. The nanocatalytic activities act cooperatively to effectively produce cytotoxic radicals in the tumor microenvironment (TME), thereby leading to ferroptosis of cancer cells. The photothermal effect not only enhances the nanocatalytic therapy but also enables photothermal therapy.