In Situ Welding Ionic Conductive Breakpoints for Highly Reversible All-Solid-State Lithium-Sulfur Batteries.

Poly(ethylene oxide) (PEO)-based solid-state lithium-sulfur batteries (SSLSBs) have garnered considerable interest owing to their impressive energy density and high safety. However, the dissolved lithium polysulfide (LiPS) together with sluggish reaction kinetics disrupts the electrolyte network, bringing about ionic conductive breakpoints and severely limiting battery performance. To cure this, we propose an in situ welding strategy by introducing phosphorus pentasulfide (PS) as the welding filler into PEO-based solid cathodes.

Achieving Significant Multilevel Modulation in Superior-quality Organic Spin Valve.

Organic semiconductors, characterized by their exceptionally long spin relaxation times (≈ms) and unique spinterface effects, are considered game-changers in spintronics. However, achieving high-performance and wide-range tunable magnetoresistance (MR) in organic spintronic devices remains challenging, severely limiting the development of organic spintronics. This work combines straintronic multiferroic heterostructures with organic spin valve (OSV) to develop a three-terminal OSV device with a gate structure.

Ultrasound-Responsive Carbon Monoxide Microneedle for Enhanced Healing of Infected Diabetic Wounds.

Efficient management of difficult-to-heal diabetic wounds remains a clinical challenge owing to bacterial infections, as well as oxidative and hyperglycemic complex pathology. Therefore, developing intelligent strategies for diabetic wound healing is urgently needed. Herein, an ultrasound (US)-responsive microneedle (MN) patch (MN@GOX@TiO@CO) capable of controlled delivery of carbon monoxide (CO) gas within the skin for effective treatment of diabetic infected wounds is developed.

Recent advances in peptide macrocyclization strategies.

Recently, owing to their special spatial structures, peptide-based macrocycles have shown tremendous promise and aroused great interest in multidisciplinary research ranging from potent antibiotics against resistant strains to functional biomaterials with novel properties. Besides traditional monocyclic peptides, many fascinating polycyclic and remarkable higher-order cyclic, spherical and cylindric peptidic systems have come into the limelight owing to breakthroughs in various chemical (, native chemical ligation and transition metal catalysis), biological (, post-translational enzymatic modification and genetic code reprogramming), and supramolecular (, mechanically interlocked, metal-directed folding and self-assembly noncovalent interactions) macrocyclization strategies developed in recent decades. In this tutorial review, diverse state-of-the-art macrocyclization methodologies and techniques for peptides and peptidomimetics are surveyed and discussed, with insights into their practical advantages and intrinsic limitations.

Vertically Expanded Crystalline Porous Covalent Organic Frameworks.

Covalent organic frameworks (COFs) can be developed for molecular confinement and separation. However, their proximate π stacks limit the interlayer distance to be only 3-6 Å, which is too small for guests to enter. As a result, COFs block access to the - space and limit guest entry/exit strictly to only the pores along the direction.

Phosphorylated Covalent Organic Framework Membranes Toward Ultrafast Single Lithium-Ion Transport.

Developing all-solid-state electrolytes, the chips for lithium-metal batteries, with superior electrochemical and mechanical properties awaits the disruptive materials. Herein, ionic covalent organic framework membranes are explored as solid-state electrolytes for single Li conduction. In the membrane, the anion groups act as Li transporter, determining Li binding capacity and releasing ability, whereas the oxygen-containing groups act as Li co-transporter, creating relay sites between adjacent Li transporters for rapid hopping.

Bubble Drainage Assisted Fabrication of Polyamide Membranes with Crater-like Structures for Efficient Desalination.

Bubble drainage (BD) occurs in various natural phenomena and industrial activities, in which bubbles rise toward the water surface and create a progressively thinned two-sided liquid film, called a lamella. Surfactant, as an important regulator in the BD process, not only assembles on both sides of the lamellae, generating a configuration of lamellae sandwiched by monolayers of surfactants (lamellae/MS), but also induces interfacial deformation by lowering interfacial tension. Herein, we developed a strategy of BD assisted interfacial polymerization for the fabrication of polyamide (PA) membranes.

Molecular Interactions in Atomically Precise Metal Nanoclusters.

For nanochemistry, precise manipulation of nanoscale structures and the accompanying chemical properties at atomic precision is one of the greatest challenges today. The scientific community strives to develop and design customized nanomaterials, while molecular interactions often serve as key tools or probes for this atomically precise undertaking. In this Perspective, metal nanoclusters, especially gold nanoclusters, serve as a good platform for understanding such nanoscale interactions.

Electrothermal Conversion of Methane to Methanol at Room Temperature with Phosphotungstic Acid.

Traditional methods for the aerobic oxidation of methane to methanol frequently require the use of noble metal catalysts or flammable H-O mixtures. While electrochemical methods enhance safety and may avoid the use of noble metals, these processes suffer from low yields due to limited current density and/or low selectivity. Here, we design an electrothermal process to conduct aerobic oxidation of methane to methanol at room temperature using phosphotungstic acid (PTA) as a redox mediator.

Selective Reduction of Nitroarenes via Noncontact Hydrogenation.

In traditional hydrogenation, where H and substrates with unsaturated bonds are activated on the same catalyst (contact mode), competitive hydrogenation of multiple reducible groups often occurs. We employ an unbiased H-cell for selective hydrogenation of the nitro group when multiple reducible groups are present. The setup spatially separates H and nitroarenes into two chambers connected by a proton-exchange membrane, thus adding barriers for a Langmuir-Hinshelwood-type mechanism that is common in thermocatalytic hydrogenation.

n-ZrS/p-ZrOS Photoanodes with NiOOH/FeOOH Oxygen Evolution Catalysts for Photoelectrochemical Water Oxidation.

Photoelectrochemical water splitting offers a promising approach for carbon neutrality, but its commercial prospects are still hampered by a lack of efficient and stable photoelectrodes with earth-abundant materials. Here, we report a strategy to construct an efficient photoanode with a coaxial nanobelt structure, comprising a buried-ZrS/ZrOS n-p junction, for photoelectrochemical water splitting. The p-type ZrOS layer, formed on the surface of the n-type ZrS nanobelt through a pulsed-ozone-treatment method, acts as a hole collection layer for hole extraction and a protective layer to shield the photoanode from photocorrosion.

Modular alkene synthesis from carboxylic acids, alcohols and alkanes via integrated photocatalysis.

Alkenes serve as versatile building blocks in diverse organic transformations. Despite notable advancements in olefination methods, a general strategy for the direct conversion of carboxylic acids, alcohols and alkanes into alkenes remains a formidable challenge owing to their inherent reactivity disparities. Here we demonstrate an integrated photochemical strategy that facilitates a one-pot conversion of these fundamental building blocks into alkenes through a sequential C(sp)-C(sp) bond formation-fragmentation process, utilizing an easily accessible and recyclable phenyl vinyl ketone as the 'olefination reagent'.

Atomically Isolated Pd Sites Promote Electrochemical CO Reduction to Acetate through a Protonation-Regulated Mechanism.

Electrochemical CO reduction reaction (CORR) offers a promising approach for sustainable acetate production, the promotion of which requires the control of multiple protonation steps. This paper describes the synthesis of atomically isolated Pd sites onto Cu nanoflakes to regulate the protonation of key intermediates. The Pd sites with moderate water activation capability are found to enhance the protonation of *CO at the neighboring Cu site to *COH, which is confirmed to be the rate-determining step through kinetic isotope effect studies.

Dynamic Asymmetric Diamination of Allylic Alcohols through Borrowing Hydrogen Catalysis: Diastereo-Divergent Synthesis of Tetrahydrobenzodiazepines.

We present herein a catalytic enantioconvergent diamination of racemic allylic alcohols with the construction of two C-N bonds and 1,3-nonadjacent stereocenters. This iridium/chiral phosphoric acid cooperative catalytic system operates through an atom-economical borrowing hydrogen amination/aza-Michael cascade, and converts readily available phenylenediamines and racemic allylic alcohols to 1,5-tetrahydrobenzodiazepines in high enantioselectivity. An intriguing solvent-dependent switch of diastereoselectivity was also observed.

Tumor Microenvironment-Activated In Situ Synthesis of Peroxynitrite for Enhanced Chemodynamic Therapy.

Chemodynamic therapy (CDT) can induce cancer cell death through hydroxyl radicals (·OH) generated from Fenton or Fenton-like reactions. Compared with traditional therapies, CDT effectively overcomes inevitable drug resistance and exhibits low side effects. However, clinical application still faces challenges, primarily due to insufficient ·OH generation and the short-lifetime of ·OH in vivo.

Stable and homogeneous intermetallic alloys by atomic gas-migration for propane dehydrogenation.

Intermetallic nanoparticles (NPs) possess significant potentials for catalytic applications, yet their production presents challenges as achieving the disorder-to-order transition during the atom ordering process involves overcoming a kinetic energy barrier. Here, we demonstrate a robust approach utilizing atomic gas-migration for the in-situ synthesis of stable and homogeneous intermetallic alloys for propane dehydrogenation (PDH). This approach relies on the physical mixture of two separately supported metal species in one reactor.

Machine learning-assisted dual-atom sites design with interpretable descriptors unifying electrocatalytic reactions.

Low-cost, efficient catalyst high-throughput screening is crucial for future renewable energy technology. Interpretable machine learning is a powerful method for accelerating catalyst design by extracting physical meaning but faces huge challenges. This paper describes an interpretable descriptor model to unify activity and selectivity prediction for multiple electrocatalytic reactions (i.