Merging SOMO activation with transition metal catalysis: Deoxygenative functionalization of amides to β-aryl amines.

Singly occupied molecular orbital (SOMO) activation of in situ generated enamines has achieved great success in (asymmetric) α-functionalization of carbonyl compounds. However, examples on the use of this activation mode in the transformations of other functional groups are rare, and the combination of SOMO activation with transition metal catalysis is still less explored. In the area of deoxygenative functionalization of amides, intermediates such as iminium ions and enamines were often generated in situ to result in the formation of α-functionalized amines.

Mesoporous Single-Crystal FeFe(CN)6 Microspheres for Superior Potassium-Ion Storage.

Metal hexacyanoferrates (HCFs), also known as Prussian blue analogues, are ideal cathodes for potassium-ion batteries (PIBs) due to their nontoxicity and cost-effectiveness. Nevertheless, obtaining metal HCF cathode materials with both long-term cycling stability and high rate performance remains a daunting challenge. In this study, we present mesoporous single-crystalline iron hexacyanoferrate (MSC-FeHCF) microspheres, featuring a single-crystalline structure that contains interconnected pores spanning the entire crystal lattice.

A temperature-sensitive and fluorescent Tr-CD/AuNP-based catalyst for efficient, monitorable, and recyclable catalytic reactions.

Gold nanoparticles (AuNPs) have been widely used as efficient and environmentally friendly catalysts due to their high specific surface area and abundant active sites. However, AuNP-based catalytic systems face several challenges, including the instability of AuNPs during the reaction, the difficulty in monitoring the process, which can easily result in insufficient reaction due to short reaction time or waste of resources due to long reaction time, as well as issues of catalyst recovery. This study proposes a novel catalyst integrating various functions, such as high stability, the capacity for real-time monitoring of the catalytic process, and rapid recycling.

High-performance solid-state proton gating membranes based on two-dimensional hydrogen-bonded organic framework composites.

Biological ion channels exhibit strong gating effects due to their zero-current closed states. However, the gating capabilities of artificial nanochannels have typically fallen short of biological channels, primarily owing to the larger nanopores that fail to completely block ion transport in the off-states. Here, we demonstrate solid-state hydrogen-bonded organic frameworks-based membranes to achieve high-performance ambient humidity-controlled proton gating, accomplished by switching the proton transport pathway instead of relying on conventional ion blockage/activation effects.

Biodegradable Vanadium-Based Nanomaterials for Photothermal-Enhanced Tumor Ferroptosis and Pyroptosis.

The designability and high reactivity of nanotechnology provide strategies for antitumor therapy by regulating the redox state in tumor cells. Here, we synthesize a kind of vanadium dioxide nanoparticle encapsulated in bovine serum albumin and containing disulfide bonds (VSB NPs) for photothermal-enhanced ferroptosis and pyroptosis effects. Mechanism studies show that disulfide bonds can effectively consume overexpressed glutathione (GSH) in the tumor microenvironment, leading to a decrease in glutathione peroxidase 4 (GPX4) activity.

Remote epitaxial crystalline perovskites for ultrahigh-resolution micro-LED displays.

The miniaturization of light-emitting diodes (LEDs) is pivotal in ultrahigh-resolution displays. Metal-halide perovskites promise efficient light emission, long-range carrier transport and scalable manufacturing for bright microscale LED (micro-LED) displays. However, thin-film perovskites with inhomogeneous spatial distribution of light emission and unstable surface under lithography are incompatible with the micro-LED devices.

PSMA-Targeted Intracellular Self-Assembled Probe for Enhanced PET Imaging.

Positron-emission tomography (PET) offers high sensitivity for cancer diagnosis. However, small-molecule-based probes often exhibit insufficient accumulation in tumor sites, while nanoparticle-based agents typically have limited delivery efficiency. To address this challenge, this study proposes a novel PET imaging probe, Ga-CBT-PSMA, designed for prostate cancer.

Solar-driven production of renewable chemicals via biomass hydrogenation with green methanol.

Solar-driven, selective biomass hydrogenation is recognized as a promising route to renewable chemicals production, but remains challenging. Here, we report a TiO supported Cu single-atom catalyst with a four-coordinated Cu-O structure, which can be universally applied for solar-driven production of various renewable chemicals from lignocellulosic biomass-derived platform molecules with good yields using green methanol as a hydrogen donor, to address this challenge. It is significant that the biomass upgrading driven by natural sunlight on a gram scale demonstrates the great practical potential.

Olfactory-Inspired Separation-Sensing Nanochannel-Based Electronics for Wireless Sweat Monitoring.

Human sweat has the potential to be sufficiently utilized for noninvasive monitoring. Given the complexity of sweat secretion, the sensitivity and selectivity of sweat monitoring should be further improved. Here, we developed an olfactory-inspired separation-sensing nanochannel-based electronic for sensitive and selective sweat monitoring, which was simultaneously endowed with interferent separation and target detection performances.

N-oxide-Functionalized Bipyridines as Strong Electron-Deficient Units to Construct High-Performance n-Type Conjugated Polymers.

Developing low-cost unipolar n-type organic thin-film transistors (OTFTs) is necessary for logic circuits. To achieve this objective, the usage of new electron-deficient building blocks with simple structure and easy synthetic route is desirable. Among all electron-deficient building units, N-oxide-functionalized bipyridines can be prepared through a simple oxidized transformation of bipyridines.

Lanthanide-polyoxometalate-based self-erasing luminescent hydrogels with time-dependent and resilient properties for advanced information encryption.

In such an era of information explosion, improving the level of information security is still a challenging task. Self-erasing luminescent hydrogels are becoming ideal candidates for improving the level of information security with simple encryption and decryption methods. Herein, a lanthanide-polyoxometalate-based self-erasing luminescent hydrogel with time-dependent and resilient properties was constructed through a covalent crosslinked network constructed with polyacrylamide and a non-covalent crosslinked network constructed with [2-(methacryloyloxy)ethyl]trimethyl ammonium chloride/NaDyWO, along with doping urease.

Deciphering the endogenous SUMO-1 landscape: a novel combinatorial peptide enrichment strategy for global profiling and disease association.

Small ubiquitin-like modifier (SUMO) plays a pivotal role in diverse cellular processes and is implicated in diseases such as cancer and neurodegenerative disorders. However, large-scale identification of endogenous SUMO-1 faces challenges due to limited enrichment methods and its lower abundance compared to SUMO-2/3. Here we propose a novel combinatorial peptide strategy, combined with anti-adhesive polymer development, to enrich endogenous SUMO-1 modified peptides, revealing a comprehensive SUMOylation landscape.

Accessing renewable magnetic cellulose nanofiber adsorbent to enhance separation efficiency for adsorption and recovery of Cd.

To address the issue of toxic cadmium pollution and meet the need for rapid separation from water body, a magnetic bio-composite material, marked as CFeMg, was prepared via a facile method. It explicitly includes components of cellulose nanofiber (CNF), FeO and Mg (OH). The microstructures and morphology were characterized and analyzed using XRD, FT-IR, SEM, and TEM.

High-Strength Ultrafine-Grained Al-Mg-Si Alloys Exposed to Mechanical Alloying and Press-Forming: A Comparison with Cast Alloys.

A high-strength Al-Mg-Si alloy was prepared using mechanical alloying (MA) combined with press-forming (PF) technology, achieving a strength of up to 715 MPa and a hardness of 173 HB. The microstructures were comparatively analyzed with conventional cast Al-Mg-Si alloys using XRD, TKD, and TEM. The XRD results showed that the full width at half maximum (FWHM) of the alloy prepared by MA+PF was significantly broadened and accompanied by a shift in the diffraction peak.

Prediction of Thermodynamic Properties of C-Based Fullerenols Using Machine Learning.

Traditional machine learning methods face significant challenges in predicting the properties of highly symmetric molecules. In this study, we developed a machine learning model based on graph neural networks (GNNs) to accurately and swiftly predict the thermodynamic and photochemical properties of fullerenols, such as C(OH) ( = 1 to 30). First, we established a global method for generating fullerenol isomers through isomer fingerprinting, which can generate all possible isomers or produce diverse structural types on demand.

Recent Advances in Ruddlesden-Popper Phase-Layered Perovskite SrTiO Photocatalysts.

SrTiO, a prominent member of the Ruddlesden-Popper (RP) perovskite family, has garnered significant interest in photocatalysis, primarily owing to its distinctive two-dimensional (2D) layered structure. In this review, we provide an insightful and concise summary of the intrinsic properties of SrTiO, focusing on the electronic, optical, and structural characteristics that render it a promising candidate for photocatalytic applications. Moreover, we delve into the innovative strategies that have been developed to optimize the structural attributes of SrTiO.

Nonconventional Full-Color Luminescent Polyurethanes: Luminescence Mechanism at the Molecular Orbital Level.

The study of structure-activity relationships is a top priority in the development of nontraditional luminescent materials. In this work, nonconjugated polyurethanes (PUs) with full-color emission (red, green, and blue) are easily obtained by control of the diol monomer structure and the polymerization conditions. Selected diol monomers introduced single, double, or triple bond repeating units into the main chain of the PUs, in order to understand how unsaturated bonds and H-bonds affect their luminescence from a molecular orbital viewpoint.

Visual Location of Oxygen Vacancies on Bismuth Titanate Nanosheets with Periodic Quantum Well and Promoting HO Photosynthesis.

Oxygen vacancy (OV) defect engineering plays a crucial role in enhancing photocatalytic efficiency. However, the direct visual characterization of oxygen vacancies still remains technically limited. Herein, a bismuth titanate (BiTiO, BTO-OV) model photocatalyst containing oxygen vacancies is constructed through density functional theory (DFT) calculations to reveal the influence mechanism of distinctive periodic quantum well and oxygen vacancies on the charge transfer behavior in BTO.

Solvent induced self-assembly of a dinuclear Eu(III) helicate and emergent strong CPL.

Herein, we report the influence of solvent on the self-assembly of a dinuclear helicate, (NMe)[Eu(LR)]. A multiple species mixture with the chemical composition of [Eu(LR)] present in CHCN can be transformed into a helicate upon increasing the content of CHCl, accompanied by a significant enhancement in circularly polarized luminescence activity.

g-CN S-Scheme Homojunction through Van der Waals Interface Regulation by Intrinsic Polymerization Tailoring for Enhanced Photocatalytic H Evolution and CO Reduction.

The effective S-scheme homojunction relies on the precise regulation of band structure and construction of advantaged charge migration interfaces. Here, the electronic structural properties of g-CN were modulated through meticulous polymerization of self-assembled supramolecular precursors. Experimental and DFT results indicate that both the intrinsic bandgap and surface electronic characteristics were adjusted, leading to the formation of an in-situ reconstructed homojunction interface facilitated by intrinsic van der Waals forces.

Carrier-Induced Room-Temperature Half-Metallicity in an Exfoliable Two-Dimensional Cr(TCNB) Metal-Organic Framework.

Half-metallicity, enabling 100% spin polarization, is pivotal for spintronics but remains challenging to achieve in low-dimensional materials. Using first-principles calculations, we theoretically propose an experimentally feasible two-dimensional (2D) metal-organic framework (MOF) magnetic semiconductor, Cr(TCNB) (TCNB = 1,2,4,5-tetracyanobenzene). This monolayer can be exfoliated from a Ag(100) substrate due to its low exfoliation energy of 0.

New insights in the low-temperature-dependent formation of amorphous titania-coated magnetic polydopamine nanocomposites for the adsorption of methylene blue.

Removal of accumulated dyes from the environment water bodies is essential to prevent further harm to humans. The development and design of new alternative nanoadsorbents that can conveniently, quickly, and efficiently improve the adsorption and removal efficiency of dyes from wastewater remains a huge challenge. An amorphous TiO with a magnetic core-shell-shell structure (FeO@PDA@a-TiO, denoted as FPaT) was constructed through a series of steps.

Oligosaccharide-assisted resolution of holothurian fucosylated chondroitin sulfate for fine structure and P-selectin inhibition.

Fucosylated chondroitin sulfate (FCS) from Holothuria mexicana (FCS) was selected for investigation because of its intriguing branch features. Selective β-eliminative depolymerization and the bottom-up assembly were performed to unravel that FCS consisted of a {D-GlcA-β1,3-D-GalNAc} backbone and branches of alternating Fuc (55 %) and D-GalNAc-α1,2-L-Fuc (45 %), the highest proportion of disaccharide branch reported to date. In branches, sulfation could occur at every free -OH site except O-3 of GalNAc, being the most complex and various structure features of natural FCS.

Construction of naphthalimide-based fluorescent probe for sequential detection of Al and NOR and its application in tea and honey.

Metal aluminum ions and the antibiotic NOR have both benefited humanity and due to improper use, posed significant threats to the environment and human health. Although the correct and rational use of these substances is crucial, developing real-time, rapid, and highly sensitive detection of trace aluminum ions and NOR in the environment and organisms is more important for early diagnosis of potential related diseases. After several decades of development, fluorescence analysis has become a mainstream research method due to its ability to meet these requirements.