Highly Efficient Ru-VO/TiO Catalysts for Hydrodeoxygenation of Amides to Amines: The Promotion Effect of Monolayer Dispersed VO on Rutile TiO.

The hydrodeoxygenation of amide to amine is one of the most important amine synthetic approaches in chemical engineering. However, low amide reactivity and poor amine selectivity remain big challenges for catalytic hydrodeoxygenation of amides. Here, Ru-VO/TiO catalysts with different V/Ru atomic ratios were prepared with the sequential impregnation method.

Bioinspired Spatial Compartment of Substrate Molecules and Catalytic Counting Entities in Hierarchical MOFs Initiated for a Dual-Mode Glycoprotein Assay.

Living cell systems possess multiple isolated compartments that can spatially confine complex substances and shield them from each other to allow for feedback reactions. In this work, a bioinspired design of metal-organic frameworks (MOFs) with well-defined multishelled matrices was fabricated as a hierarchical host for multiple guest substances including fluorogenic molecules and catalytic nanoparticles (NPs) at the separated locations for the development of a dual-mode glycoprotein assay. The multispatial-compartmental zeolitic imidazolate framework-8 (ZIF-8) constituents were synthesized via epitaxial shell-by-shell overgrowth to guide the integration and spatial organization of host guests.

Self-Assembled Covalent Triazine Frameworks Derived N, S Co-Doped Carbon Nanoholes with Facilitating Ions Transportation Toward Remarkably Enhanced Oxygen Reduction Reaction and for Zinc-Air Batteries.

3D assembled carbon materials, featuring unique hierarchical porosity and interconnected channels, are essential for the advancement of emerging zinc-air batteries (ZABs). In this study, nitrogen (N) and sulfur (S) co-doped 3D carbon nanoholes (N/S-CNHs) are synthesized through a straightforward procedure involving self-assembly followed by carbonization. This process utilizes a hybrid of self-assembled covalent triazine framework and sodium lignosulphonate (CTF@LS) as a multifunctional precursor.

Insights Into the Role of π-Electrons of Aromatic Aldehydes in Passivating Perovskite Defects.

Carbonyl-containing aromatic ketones or aldehydes have been demonstrated to be effective defect passivators for perovskite films to improve performances of perovskite solar cells (PSCs). It has been claimed that both π-electrons within aromatic units and carbonyl groups can, separately, interact with ionic defects, which, however, causes troubles in understanding the passivation mechanism of those aromatic ketone/aldehyde molecules. Herein, we clarify the effect of both moieties in one molecule on the defect passivation by investigating three aromatic aldehydes with varied conjugation planes, namely, biphenyl-4-carbaldehyde (BPCA), naphthalene-2-carbaldehyde (NACA) and pyrene-1-carbaldehyde (PyCA).

Pressure aging: An effective process to liberate the power of high-pressure materials research.

High pressure can create extreme conditions that enable the formation of novel materials and the discovery of new phenomena. However, the ability to preserve the desirable characteristics of materials obtained under high pressure has remained an elusive challenge, as the pressure-induced changes are typically reversible, except for the pressure-induced chemical reactions such as polymerization of hydrocarbons. Here, we propose the concept of "pressure aging" (PA) that enables the permanent locking-in of high-pressure structures and their associated enhanced properties in functional materials.

Regulating Charge Separation Via Periodic Array Nanostructures for Plasmon-Enhanced Water Oxidation.

Plasmonic resonance intensity in metallic nanostructures plays a crucial role in charge generation and separation, directly affecting plasmon-induced photocatalytic activity. Engineering strategies to enhance plasmonic effects involve designing specific nanostructures, such as triangular nanoplates with sharp corners or dimer nanostructures with hot spots. However, these approaches often lead to a trade-off between enhanced plasmonic intensity and resonance energy, which ultimately determines local charge density and photocatalytic performance.

π-HuB: the proteomic navigator of the human body.

The human body contains trillions of cells, classified into specific cell types, with diverse morphologies and functions. In addition, cells of the same type can assume different states within an individual's body during their lifetime. Understanding the complexities of the proteome in the context of a human organism and its many potential states is a necessary requirement to understanding human biology, but these complexities can neither be predicted from the genome, nor have they been systematically measurable with available technologies.

Non-Radical Mediated Photocatalytic HO Synthesis in Conjugate-Enhanced Phenolic Resins with Ultrafast Charge Separation.

It is essential for the development of highly efficient polymeric photocatalysts for hydrogen peroxide (HO) production. Nevertheless, the non-uniform molecular structures and sluggish reaction pathway of polymeric photocatalysts lead to low conversion efficiency. In this work, we report sulfur-contained phenolic resins with regulated conjugation for photocatalytic HO production.

A peptide-centric local stability assay enables proteome-scale identification of the protein targets and binding regions of diverse ligands.

By using a limited-proteolysis strategy that employs a large amount of trypsin to generate peptides directly from native proteins, we found that ligand-induced protein local stability shifts can be sensitively detected on a proteome-wide scale. This enabled us to develop the peptide-centric local stability assay, a modification-free approach that achieves unprecedented sensitivity in proteome-wide target identification and binding-region determination. We demonstrate the broad applications of the peptide-centric local stability assay by investigating interactions across various biological contexts.

One-Pot Production of Cinnamonitriles from Lignin β-O-4 Segments Induced by Selective Oxidation of the γ-OH Group.

The construction of N-containing aromatic compounds from lignin is of great importance to expanding the boundary of the biorefinery and meeting the demand for value-added biorefinery. However, it remains a huge challenge due to the complex lignin structure and the incompatible catalysis for C-O/C-C bond cleavage and C-N formation. Herein, sustainable synthesis of cinnamonitrile derivatives from lignin β-O-4 model compounds in the presence of 2,2,6,6-tetramethylpiperidine oxide (TEMPO), (diacetoxyiodo)benzene (BAIB), and a strong base has been achieved in a one-pot, two-step fashion under transition-metal-free conditions.

Synthesis, anticancer and antibacterial evaluation of novel spiramycin-acylated derivatives.

Spiramycin and its derivatives are commonly used antimicrobials, and its derivative, carrimycin, has recently been found to have good anticancer potential. Here, we found that the 4''-OH of spiramycin can be selectively acylated, resulting in a series of novel spiramycin derivatives with a structure similar to carrimycin. Anticancer studies showed that most of the derivatives exhibited moderate to good anti-proliferative activity against four cancer cell lines, including HGC-27, HT-29, HCT-116 and HeLa, especially compound 14, which has the strongest activity against HGC-27 cells with an IC value of 0.

Amplified Detection of Threading Dislocations in n-Type 4H-SiC Epilayers Enabled by Time-Resolved Photoluminescence Mapping.

Threading dislocations (TDs) in epitaxial layers of silicon carbide (SiC) exert a negative impact on the device performance, thereby hampering the commercialization of SiC power devices. Therefore, inspection of TD defects is a crucial step in the fabrication of SiC wafers. In this work, we reported a time-resolved photoluminescence (PL) mapping technique for detecting TDs by extracting PL images at different delay times after pulse excitation along the lifetime decay curve.

Palladium-Catalyzed Carbonylative Sonogashira Coupling of Aliphatic Alkynes and Aryl Thianthrenium Salts to Alkynones and Furanones.

Herein, we developed a mild and efficient palladium-catalyzed carbonylative Sonogashira coupling of aryl thianthrenium salts with aliphatic alkynes and benzyl acetylene toward alkynones and furanones. Various desired products were prepared in good yields with broad functional group tolerance including the bromide group. In the case of using benzyl acetylene, the corresponding furanones can be obtained in good yields under the same conditions with two molecules of CO inserted.

Spatial Conformation Engineering of Aromatic Ketones for Highly Efficient and Stable Perovskite Solar Cells.

Carbonyl-containing materials employed in state-of-the-art hybrid lead halide perovskite solar cells (PSCs) exhibit a strong structure-dependent electron donor effect that predominates in defect passivation. However, the impact of the molecular spatial conformation on the efficacy of carbonyl-containing passivators remains ambiguous, hindering the advancement of molecular design for passivating materials. Herein, we show that altering the spatial torsion angle of aromatic ketones from twisted to planar configurations, as seen in benzophenone (BP, 27.

Hollow Mo/MoS Nanoreactors with Tunable Built-in Electric Fields for Sustainable Hydrogen Production.

Constructing built-in electric field (BIEF) in heterojunction catalyst is an effective way to optimize adsorption/desorption of reaction intermediates, while its precise tailor to achieve efficient bifunctional electrocatalysis remains great challenge. Herein, the hollow Mo/MoS nanoreactors with tunable BIEFs are elaborately prepared to simultaneously promote hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) for sustainable hydrogen production. The BIEF induced by sulfur vacancies can be modulated from 0.

Improved Efficiency and Stability in Pure-Red CdSe Nanoplatelet LEDs Enabled by Gradient Alloyed CdSeS/CdZnS Crown/Shell.

Anisotropic nanoplatelets (NPLs) possess strong in-plane transition dipole moments and out-of-plane emission, which enable a maximum photon out-coupling efficiency of 40% and a high gain coefficient, making them ideal candidates for light-emitting diodes (LEDs) and lasers. However, the unbalanced surface energy between the side and top facets of NPLs results in poor thermal stability and high susceptibility to ripening at elevated temperatures, which complicates the growth of the shell. To address this issue, a gradient crown (CdSeS) around the CdSe NPLs is designed to stabilize the high energy side facets.

Polysaccharides isolated from Ampelopsis grossedentata and their immunomodulatory activity.

To explore the immunomodulatory activity of polysaccharides from Ampelopsis grossedentata, two polysaccharides named AGP1 and AGP2 were isolated and purified by DEAE-cellulose 52 column and Sephacryl S-300HR chromatography. AGP1 and AGP2 were composed of fucose, arabinose, rhamnose, galactose, glucose, mannose, galacturonic acid, and glucuronic acid, with a ratio of 0.5: 10.

Microparticle-assisted protein capture method facilitates proteomic and glycoproteomic analysis of urine samples.

Serum tests have become a partial alternative to renal biopsy for diagnosing primary membranous nephropathy (pMN). However, urine tests, due to their non-invasive nature and ability to more accurately reflect glomerular diseases, hold great promise for the detection of pMN. However, the low protein concentration and the time-consuming sample preparation procedure of urine samples challenges the proteomic and glycoproteomic analysis to find urine-derived signatures associated with pMN.

Atomically Dispersed Mn-Doped Ru@RuO Core/Shell Nanostructure with High Acidic Water Oxidation Performance Arising from Multiple Synergies.

The high overpotential and unsatisfactory stability of RuO-based catalysts seriously hinder their application in acidic oxygen evolution reaction (OER). Herein, a Ru@RuO core/shell catalyst doped with atomically dispersed Mn species, denoted as Ru@Mn-RuO, is reported, which is prepared by a facile one-pot method. Detailed structural characterizations confirm that Mn is homogeneously and atomically distributed in RuO shell, which causes lattice contraction of RuO.

Mechanism of Ampicillin Hydrolysis by New Delhi Metallo-β-Lactamase 1: Insight From QM/MM MP2 Calculation.

The New Delhi metallo-β-lactamase 1 (NDM-1) can hydrolyze nearly all clinically important β-lactam antibiotics, narrowing the options for effective treatment of bacterial infections. QM/MM MP2 calculations are performed to reveal the mechanism of ampicillin hydrolysis catalyzed by NDM-1. It is found that the rate-determining step is the dissociation of hydrolyzed ampicillin from the NDM-1 active site, which requires a proton transfer from the bridging neutral water molecule to the newly formed carboxylate group.

Characterization of two new alginate lyases from Pseudomonas mendocina E03.

Alginate lyases, which degrade alginate into oligosaccharides, have broad applications in biorefinery, biomedical, and industrial fields. The Polysaccharide Lyase Family 7 (PL7) is particularly notable for its alginate lyase activity. In this study, two novel alginate lyases, PmAlg7A and PmAlg7B, from Pseudomonas mendocina E03 were cloned, heterologously expressed, and characterized.

Carbon Monoxide and Alkoxycarbonyl Radical Enabled Migration Strategy for the Carbonylative Functionalization of Unactivated Alkenes.

Herein we report a "carbonylative migration" strategy for the acylation-esterification type double functionalization of unactivated alkenes using alkyloxalkyl chlorides and CO as the reagents. The transformation is proceeded by the alkoxycarbonyl radical addition to unactivated alkenes, followed by the insertion of carbon monoxide to induce intramolecular migration of heteroaryl groups, which is different from the traditional reaction modes. The reaction conditions were mild and well tolerated with varieties of functional groups.

Low-valence platinum single atoms in sulfur-containing covalent organic frameworks for photocatalytic hydrogen evolution.

This study focuses on optimizing catalytic activity in photocatalytic hydrogen evolution reaction by precisely designing and modulating the electronic structure of metal single atoms. The catalyst, denoted as PtSA@S-TFPT, integrates low-valence platinum single atoms into sulfur-containing covalent organic frameworks. The robust asymmetric four-coordination between sulfur and platinum within the framework enables a high platinum loading of 12.