Ultralow Coordination Copper Sites Compartmentalized within Ordered Pores for Highly Efficient Electrosynthesis of -Propanol from CO.

Coordinatively unsaturated copper (Cu) has been demonstrated to be effective for electrifying CO reduction into C products by adjusting the coupling of C-C intermediates. Nevertheless, the intuitive impacts of ultralow coordination Cu sites on C products are scarcely elucidated due to the lack of synthetic recipes for Cu with low coordination numbers and its vulnerability to aggregation under reductive potentials. Herein, computational predictions revealed that Cu sites with higher levels of coordinative unsaturation favored the adsorption of C and C intermediates.

Atomically Dispersed Co-P Moieties via Direct Thermal Exfoliation for Alkaline Hydrogen Electrosynthesis.

The development of highly active and stable cathodes in alkaline solutions is crucial for promoting the commercialization of anion exchange membrane (AEM) electrolyzers, yet it remains a significant challenge. Herein, we synthesized atomically dispersed CoP moieties (CoP-SSC) immobilized on ultrathin carbon nanosheets via a phosphidation exfoliation strategy at medium temperature. The thermodynamic formation process of the Co-P moieties was elucidated using X-ray absorption spectroscopy (XAS) and theoretical calculations.

Low-Cost Preparation of Wafer-Scale Au(111) Single Crystals for the Epitaxy of Two-Dimensional Layered Materials.

Single-crystal Au(111), renowned for its chemically inert surface, long-range "herringbone" reconstruction, and high electrical conductivity, has long served as an exemplary template in diverse fields, , crystal epitaxy, electronics, and electrocatalysis. However, commercial Au(111) products are high-priced and limited to centimeter sizes, largely restricting their broad applications. Herein, a low-cost, high-reproducible method is developed to produce 4 in.

Nanomaterials-Induced Pyroptosis: Advancing Novel Therapeutic Pathways in Nanomedicine.

Pyroptosis, a form of programmed cell death characterized by cell lysis and inflammation, has significant implications for disease treatment. Nanomaterials (NMs), with their unique physicochemical properties, can precisely modulate pyroptosis, offering novel and intelligent therapeutic strategies for cancer, infectious diseases, and chronic inflammatory conditions with targeted activation and reduced systemic toxicity. This review explores the mechanisms by which NMs regulate pyroptosis, comparing molecular and NM inducers, and examines the role of intrinsic properties such as size, shape, surface charge, and chemical composition in these processes.

Mechanism of Water Freezing in Solutions: Solutes Affect the Formation of Critical Ice Nuclei.

The microscopic mechanisms by which solutes modulate water freezing are fundamental for controlling the freezing of various environmental and cryobiotic systems. Although our understanding of the initiation mechanisms of pure water freezing is becoming clearer, the microscopic pictures regarding ice nucleation in complex systems such as solutions still rely on theory assumption and empirical formulation. Here, we experimentally demonstrate that solutes modulate water freezing through affecting critical ice nucleus formation.

Synergistic Enhancement of Ferroptosis via Mitochondrial Accumulation and Photodynamic-Controlled Release of an Organogold(I) Cluster Prodrug.

Effective delivery and controlled release of metallo-prodrugs with sustained activation and rapid response feed the needs of precise medicine in metal chemotherapeutics. However, gold-based anticancer drugs often suffer from detoxification binding and extracellular transfer by sulfur-containing peptides. To address this challenge, we integrate a thiol-activated prodrug strategy of newly prepared hypercoordinated carbon-centered gold(I) clusters (HCGCs) with their photosensitization character to augment the mitochondrial release of Au(I) in tumors.

Coherent Exciton Spin Relaxation Dynamics and Exciton Polaron Character in Layered Two-Dimensional Lead-Halide Perovskites.

The quantum-well-like two-dimensional lead-halide perovskites exhibit strongly confined excitons due to the quantum confinement and reduced dielectric screening effect, which feature intriguing excitonic effects. The ionic nature of the perovskite crystal and the "softness" of the lattice induce the complex lattice dynamics. There are still open questions about how the soft lattices decorate the nature of excitons in these hybrid materials.

Intrinsic Mechanical Effects on the Activation of Carbon Catalysts.

The mechanical effects on carbon-based metal-free catalysts (C-MFCs) have rarely been explored, despite the global interest in C-MFCs as substitutes for noble metal catalysts. Stress is ubiquitous, whereas its dedicated study is severely restricted due to its frequent entanglement with other structural variables, such as dopants, defects, and interfaces in catalysis. Herein, we report a proof-of-concept study by establishing a platform to continuously apply strain to a highly oriented pyrolytic graphite (HOPG) lamina, simultaneously collecting electrochemical signals.

Descriptor for electro-oxidation of glycerol with high-efficiency bifunctional Cu-N single atom catalyst and coupled with hydrogen evolution/carbon dioxide reduction.

Electrochemical glycerol oxidation reaction (GOR) presents a promising approach for converting excess glycerol (GLY) into high-value-added products. However, the complex mechanism and the challenge of achieving selectivity for diverse products make GOR difficult to address in both experimental and theoretical studies. In this work, three nitrogen-doped graphene-supported copper single-atom catalysts (CuN@Gra SACs, x = 2-4) were selected as the model system due to their simple structure, excellent conductivity and high structural stability.

Modulation of Molecular Quadrupole Moments by Phenyl Side-Chain Fluorination for High-Voltage and High-Performance Organic Solar Cells.

The ground-state charge generation (GSCG) in photoactive layers determines whether the photogenerated carriers occupy the deep trap energy levels, which, in turn, affects the device performance of organic solar cells (OSCs). In this work, charge-quadrupole electrostatic interactions are modulated to achieve GSCG through a molecular strategy of introducing different numbers of F atom substitutions on the BTA3 side chain. The results show that 8F substitution (BTA3-8F) and 16F substitution (BTA3-16F) lead to different patterns of highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energy level changes.

Mechanically Resilient and Highly Efficient Flexible Perovskite Solar Cells with Octylammonium Acetate for Surface Adhesion and Stress Relief.

Flexible perovskite solar cells (FPSCs) have advanced significantly because of their excellent power-per-weight performance and affordable manufacturing costs. The unsatisfactory efficiency and mechanical stability of FPSCs are bottleneck challenges that limit their application. Here, we explore the use of octylammonium acetate (OAAc) with a long, intrinsic, flexible molecular chain on perovskite films for surface adhesion and mechanical releasing.

Harnessing Adsorbate-adsorbate Interaction to Activate C-N Bond for Exceptional Photoelectrochemical Urea Oxidation.

The photoelectrochemical (PEC) urea oxidation reaction (UOR) presents a promising half-reaction for green hydrogen production, but the stable resonance structure of the urea molecule results in sluggish kinetics for breaking the C-N bond. Herein, we realize the record PEC UOR performance on a NiO-modified n-Si photoanode (NiO@Ni/n-Si) by harnessing the adsorbate-adsorbate interaction. We quantificationally unveil a dependence of the UOR activation barrier on the coverage of photogenerated surface high-valent Ni-oxo species (NiIV=O) by employing operando PEC spectroscopic measurements and theoretical simulations.

Resonantly Enhanced Hybrid Wannier-Mott-Frenkel Excitons in Organic-Inorganic Van Der Waals Heterostructures.

Hybrid excitons formed via resonant hybridization in 2D material heterostructures feature both large optical and electrical dipoles, providing a promising platform for many-body exciton physics and correlated electronic states. However, hybrid excitons at organic-inorganic interface combining the advantages of both Wannier-Mott and Frenkel excitons remain elusive. Here, hybrid excitons are reported in the copper phthalocyanine/molybdenum diselenide (CuPc/MoSe) heterostructure (HS) featuring strong molecular orientation dependence by low-temperature photoluminescence and absorption spectroscopy.

Exciton Emission Enhancement in Two-Dimensional Monolayer Tungsten Disulfide on a Silicon Substrate via a Fabry-Pérot Microcavity.

Exciton emitters in two-dimensional monolayer transition-metal dichalcogenides (TMDs) provide a boulevard for the emerging optoelectronic field, ranging from miniaturized light-emitting diodes to quantum emitters and optical communications. However, the low quantum efficiency from limited light-matter interactions and harmful substrate effects seriously hinders their applications. In this work, we achieve a ∼438-fold exciton photoluminescence enhancement by constructing a Fabry-Pérot cavity consisting of monolayer WS and a micron-scale hole on the SiO/Si substrate.

t2 Occupancy as an Effective and Predictive Descriptor for the Design of High-Performance Spinel Oxide Peroxidase-like Nanozymes.

Nanozymes are next generation of enzyme mimics. Due to the lack of activity descriptors, most nanozymes were discovered through trial-and-error strategies or by accident. While eg occupancy in an octahedral crystal field was proven as an effective descriptor, the t2 in a tetrahedral crystal field has rarely been explored.

Endogenous hydrogen sulfide persulfidates endothelin type A receptor to inhibit pulmonary arterial smooth muscle cell proliferation.

Background: The binding of endothelin-1 (ET-1) to endothelin type A receptor (ETAR) performs a critical action in pulmonary arterial smooth muscle cell (PASMC) proliferation leading to pulmonary vascular structural remodeling. More evidence showed that cystathionine γ-lyase (CSE)-catalyzed endogenous hydrogen sulfide (HS) was involved in the pathogenesis of cardiovascular diseases. In this study, we aimed to explore the effect of endogenous HS/CSE pathway on the ET-1/ETAR binding and its underlying mechanisms in the cellular and animal models of PASMC proliferation.

Zinc nanoparticles from oral supplements accumulate in renal tumours and stimulate antitumour immune responses.

A successful therapeutic outcome in the treatment of solid tumours requires efficient intratumoural drug accumulation and retention. Here we demonstrate that zinc gluconate in oral supplements assembles with plasma proteins to form ZnO nanoparticles that selectively accumulate into papillary Caki-2 renal tumours and promote the recruitment of dendritic cells and cytotoxic CD8 T cells to tumour tissues. Renal tumour targeting is mediated by the preferential binding of zinc ions to metallothionein-1X proteins, which are constitutively overexpressed in Caki-2 renal tumour cells.

A nanoparticle-based wireless deep brain stimulation system that reverses Parkinson's disease.

Deep brain stimulation technology enables the neural modulation with precise spatial control but requires permanent implantation of conduits. Here, we describe a photothermal wireless deep brain stimulation nanosystem capable of eliminating α-synuclein aggregates and restoring degenerated dopamine neurons in the substantia nigra to treat Parkinson's disease. This nanosystem (ATB NPs) consists of gold nanoshell, an antibody against the heat-sensitive transient receptor potential vanilloid family member 1 (TRPV1), and β-synuclein (β-syn) peptides with a near infrared-responsive linker.

Synergetic Interface and Bulk Defects Modification with Identical Organic Molecule for Efficient Inverted Perovskite Solar Cells.

Recent progress in inverted perovskite solar cells (IPSCs) mainly focused on NiO modification and perovskite (PVK) regulation to enhance efficiency and stability. However, most works address only monofunctional modifications, and identical molecules with the ability to simultaneously optimize NiO interface and perovskite bulk phase have been rarely reported. This work proposes a dual modification approach using 4-amino-3,5-dichlorobenzotrifluoride (DCTM) to optimize both NiO upper interfaces and reduction of bulk defects in perovskite.

An OMV-Based Nanovaccine as Antigen Presentation Signal Enhancer for Cancer Immunotherapy.

Antigen-presenting cells (APCs) process tumor vaccines and present tumor antigens as the first signals to T cells to activate anti-tumor immunity, which process requires the assistance of co-stimulatory second signals on APCs. The immune checkpoint programmed death ligand 1 (PD-L1) not only mediates the immune escape of tumor cells but also acts as a co-inhibitory second signal on APCs. The serious dysfunction of second signals due to the high expression of PD-L1 on APCs in the tumor body results in the inefficiency of tumor vaccines.

Genetically Encoded Nucleic Acid Nanostructures for Biological Applications.

Nucleic acid, as a carrier of genetic information, has been widely employed as a building block for the construction of versatile nanostructures with pre-designed sizes and shapes through complementary base pairing. With excellent programmability, addressability, and biocompatibility, nucleic acid nanostructures are extensively applied in biomedical researches, such as bio-imaging, bio-sensing, and drug delivery. Notably, the original gene-encoding capability of the nucleic acids themselves has been utilized in these structurally well-defined nanostructures.

Fluoride binding-modulated supramolecular chirality of urea-containing triarylamine and its photo-manifestation.

In recent years, the regulation of anion-mediated chiral assemblies has gained significant interest. This study investigated the modulation of supramolecular chiroptical signals and chiral assembled structures in a triarylamine system containing a urea moiety through fluoride ion-urea bond interactions, aiming to understand the chiral sense amplification in supramolecular assemblies. Chiral triarylamine derivatives containing urea or amide units were synthesized and the self-assemblies were examined in the absence and presence of fluoride ions.

Rapid Preparation of Collagen/Red Blood Cell Membrane Tubes for Stenosis-Free Vascular Regeneration.

Extracellular matrix (ECM)-based small-diameter vascular grafts (SDVGs, inner diameter (ID) < 6 mm) hold great promise for clinical applications. However, existing ECM-based SDVGs suffer from limited donor availability, complex purification, high cost, and insufficient mechanical properties. SDVGs with ECM-like structure and function, and good mechanical properties were rapidly prepared by optimizing common materials and preparation, which can improve their clinical prospects.

Safe Production of Rice ( L.) in Arsenic-Contaminated Soil: a Remedial Strategy using Micro-Nanostructured Bone Biochar.

This study investigated the effects of fine-sized pork bone biochar particles on remediating As-contaminated soil and alleviating associated phytotoxicity to rice in 50-day short-term and 120-day full-life-cycle pot experiments. The addition of micro-nanostructured pork bone biochar (BC) pyrolyzed at 400 and 600 °C (BC400 and BC600) significantly increased the As-treated shoot and root fresh weight by 24.4-77.

Phosphorescent Liquid Crystalline Polymer-based Circularly Polarized Luminescence Optical Waveguides for Enhanced Photonic Signal Processing and Information Encryption.

Efficient circularly polarized luminescence (CPL) optical waveguides have significant potential for advancing photonic and optoelectronic devices. However, the development of CPL optical waveguides materials (OWMs) with low optical loss coefficient remains a considerable challenge. To overcome this, we design and synthesize CPL OWMs based on room-temperature phosphorescent liquid crystalline polymers (LCPs).