Subtle Modifications in Interface Configurations of Iron/Cobalt Phthalocyanine-Based Electrocatalysts Determine Molecular CO Reduction Activities.

Strain engineering has emerged as a powerful approach in steering material properties. However, the mechanism and potential limitations remain poorly understood. Here we report that subtle changes in molecular configurations can profoundly affect, conducively or adversely, the catalytic selectivity and product turnover frequencies (TOFs) of CO reduction reaction.

Deciphering the electronic and structural origin of chiroptical activity of chiral 2D perovskites.

Understanding the structure-chiroptical activity relationship in chiral perovskites is of great significance as it provides a pathway to control light-matter interactions. Although many reports have shown various chiral structures with distinctive chiroptical responses, a clear structure-property relationship is still missing, partially stemming from the poor understanding of the optical activity mechanism. For instance, it remains unclear if and how the chiroptical activity is related to exciton spin splitting.

Exploring efficient and air-stable d Re(v) alkylidyne catalysts: toward room temperature alkyne metathesis.

Transition metal-catalyzed alkyne metathesis has become a useful tool in synthetic chemistry. Well-defined alkyne metathesis catalysts comprise alkylidyne complexes of tungsten, molybdenum and rhenium. Non-d Re(v) alkylidyne catalysts exhibit advantages such as remarkable tolerance to air and moisture as well as excellent functional group compatibility.

A numerical platform for predicting the performance of paper-based analytical devices.

This article presents a numerical platform for predicting the performance of paper-based analytical devices. The capillary flow, reaction, dissolution, and other physicochemical phenomena associated with device operation are accounted for using Darcy's law, Richard's equation and other transport equations. The platform can be used for different paper substrates, biorecognition methods, detection systems (such as optical and electrochemical detection), device patterns and dimensions, and ways in which the device is operated such as the input method of the body fluid.

A rhodamine-based fluorescent probe bearing 8-hydroxyquinoline group for the highly selective detection of Hg and its practical application in cell imaging.

A highly selective and sensitive fluorescent probe, RHOQ, was designed for the detection of Hg by incorporating an 8-hydroxyquinoline moiety onto a rhodamine molecular platform with a suitable linker. In MeOH-Tris (20 mM, pH = 7.4, 1 : 9, v/v) buffer solution, RHOQ exhibited 550-fold fluorescence enhancement at 594 nm upon addition of Hg, with a fast response and a low detection limit (9.

Meso/Microporous Single-Atom Catalysts Featuring Curved Fe-N Sites Boost the Oxygen Reduction Reaction Activity.

Zeolitic-imidazolate frameworks (ZIFs) are among the most efficient precursors for the synthesis of atomically dispersed Fe-N/C materials, which are promising catalysts for enhancing the performance of Zn-air batteries (ZABs) and proton exchange fuel cells (PEMFCs). However, existing ZIF-derived Fe-N/C electrocatalysts mostly consist of microporous materials, leading to insufficient mass transport and inadequate battery/cell performance. In this study, we synthesize an atomically dispersed meso/microporous Fe-N/C material with curved Fe-N active sites, denoted as FeSA-N/TC, through the pyrolysis of hemin-modified ZIF films on ZnO nanorods, obtained from the self-assembly reaction between Zn from ZnO hydrolysis and 2-methylimidazole.

Organocatalytic enantio- and diastereoselective assembly of cyclopropane-incorporated polycyclic molecules isobenzopyrylium ions.

A highly enantio- and diastereoselective organocatalytic formation of cyclopropanes embedded in a complex bridged polycyclic architecture is disclosed. In the presence of a chiral phosphoric acid catalyst, this reaction generates four new stereogenic centers and three new C-C bonds efficiently from isochromene acetals and vinylboronic acids under mild conditions. Different from conventional asymmetric cyclopropanation strategies, this process does not involve carbenes or carbenoids.

Red-Shifting B-Dependent Photoreceptor Protein via Optical Coupling for Inducible Living Materials.

Cobalamin (B)-dependent photoreceptors are gaining traction in materials synthetic biology, especially for optically controlling cell-to-cell adhesion in living materials. However, these proteins are mostly responsive to green light, limiting their deep-tissue applications. Here, we present a general strategy for shifting photoresponse of B-dependent photoreceptor CarH from green to red/far-red light via optical coupling.

Two-Photon Clusteroluminescence Enabled by Through-Space Conjugation for In Vivo Bioimaging.

Clusteroluminescence (CL) materials without largely conjugated structures have gained significant attention due to their unique photophysical properties and potential in bioimaging. However, low luminescence efficiency and short emission wavelength limit their development. This work designs three luminogens with CL properties (CLgens) by introducing n-electron-involved through-space conjugation (TSC) into diarylmethane.

NIR-II AIEgens for Infectious Diseases Phototheranostics.

Pathogenic infectious diseases have persistently posed significant threats to public health. Phototheranostics, which combines the functions of diagnostic imaging and therapy, presents an extremely promising solution to block the spread of pathogens as well as the outbreak of epidemics owing to its merits of a wide-spectrum of activity, high controllability, non-invasiveness, and difficult to acquire resistance. Among multifarious phototheranostic agents, second near-infrared (NIR-II, 1000-1700 nm) aggregation-induced emission luminogens (AIEgens) are notable by virtue of their deep penetration depth, excellent biocompatibility, balanced radiative and nonradiative decay and aggregation-enhanced theranostic performance, making them an ideal option for combating pathogens.

Polyarylene-Based Anion Exchange Membranes for Fuel Cells.

Anion exchange membrane fuel cell (AEMFC) is an emerging and promising technology that can help realize a carbon-neutral, sustainable economy. Also, compared to the proton exchange membrane counterpart, AEMFC can achieve comparable cell outputs with lower costs due to the applicability of non-platinum group metal electrocatalysts for the reaction on the electrodes' surfaces. However, the wide application of the AEMFCs has been impeded by the unsatisfactory stability and performance of the hydroxide-conductive membranes in the past.

Metallaaromaticity involving a d early transition metal centre: synthesis, structure, and aromaticity of tantallapyridinazirine complexes.

Though late transition metal aromatic metallabenzenes and related heteroatom-containing analogues have been well studied, the corresponding aromatic early transition metal complexes remain elusive. Herein, we demonstrate the synthesis of aromatic, planar, and delocalised organotantallapyridinium complexes a simple one-pot process by sequential treatment of tantalum methyl complex [η:σ-MeC(CH)(CBH)]TaMe with alkynes and isocyanide. Single-crystal X-ray analyses, NMR spectroscopic data and DFT calculations suggest that they are aromatic tantallapyridinium complexes, a class of long-sought-after molecules.

Toward robust lithium-sulfur batteries advancing LiS deposition.

Lithium-sulfur batteries (LSBs) with two typical platforms during discharge are prone to the formation of soluble lithium polysulfides (LiPS), leading to a decrease in the cycling life of the battery. Under practical working conditions, the transformation of S into LiS is cross-executed rather than a stepwise reaction, where the liquid LiPS to solid LiS conversion can occur at a high state of charge (SOC) to maintain the current requirement. Therefore, advancing LiS deposition can effectively reduce the accumulation of LiPSs and ultimately improve the reaction kinetics.

Pattern-Matched Polymer Ligands Toward Near-Perfect Synergistic Passivation for High-Performance and Stable Br/Cl Mixed Perovskite Light-Emitting Diodes.

Mixed Br/Cl perovskite nanocrystals (PeNCs) exhibit bright pure-blue emission benefiting for fulfilling the Rec. 2100 standard. However, phase segregation remains a significant challenge that severely affects the stability and emission spectrum of perovskite light-emitting diodes (PeLEDs).

Exciting Bacteria to a Hypersensitive State for Enhanced Aminoglycoside Therapy by a Rationally Constructed AIE Luminogen.

The diminishing effectiveness of existing aminoglycoside antibiotics (AGs) compels scientists to seek new approaches to enhance the sensitivity of current AGs. Despite ongoing efforts, currently available approaches remain restricted. Herein, a novel strategy involving the rational construction of an aggregation-induced-emission luminogen (AIEgen) is introduced to significantly enhance Gram-positive bacteria's susceptibility to AGs.

A planar electronic acceptor motif contributing to NIR-II AIEgen with combined imaging and therapeutic applications.

Designing molecules with donor-acceptor-donor (D-A-D) architecture plays an important role in obtaining second near-infrared region (NIR-II, 1000-1700 nm) fluorescent dyes for biomedical applications; however, this always comes with a challenge due to very limited electronic acceptors. On the other hand, to endow NIR-II fluorescent dyes with combined therapeutic applications, trivial molecular design is indispensable. Herein, we propose a pyrazine-based planar electronic acceptor with a strong electron affinity, which can be used to develop NIR-II fluorescent dyes.

Photochemical three-component assembly of tri-substituted oxazoles through a carbenic phosphorus-nitrile hybrid ylide formation/trapping cascade.

Construction of complex molecular skeletons with ubiquitous chemical feedstocks in a single transformation is highly appealing in organic synthesis. We report a novel visible-light-induced three-component reaction for the construction of complex 2,4,5-trisubstituted oxazoles, which are valuable in medicinal chemistry, from simple and readily available iodonium-phosphonium hybrid ylides, carboxylic acids, and nitriles. This reaction features a carbenic phosphorus-nitrile hybrid ylide formation/trapping cascade, in which a photo-generated α-phosphonium carbene acts as a sequence trigger.

Avenue to novel -carboranyl boron compounds - reactivity study of -carborane-fused aminoborirane towards organic azides.

Herein we report the reactivity study of -carborane-fused bis(trimethylsilyl)aminoborirane towards three different types of organic azides, , aryl, alkyl, and silyl azides. The reaction with ArN (Ar = 2,6-iPrCH, 2,6-CHCl, 2,4,6-CHBr, CF) resulted in the cycloaddition of ArN to the borirane BN unit accompanied by silyl migration. Conversely, in the reaction with BnN, only the BnN : borirane 1 : 2 ring expansion product was obtained.

Organocatalytic enantioselective synthesis of C-N atropisomers formal C-O bond amination.

Compared with well-developed construction of C-C atropisomers, the synthesis of C-N atropisomers remains in its infancy, which is recognized as both appealing and challenging. Herein, we achieved the first organocatalyzed asymmetric synthesis of C-N atropisomers by formal C-O amination. With the aid of a suitable acid, 3-alkynyl-3-hydroxyisoindolinones reacted smoothly with 1-methylnaphthalen-2-ols to afford a wide range of atropisomers by selective formation of the C-N axis.

Boryls, their compounds and reactivity: a structure and bonding perspective.

Boryls and their compounds are important due to their diverse range of applications in the fields of materials science and catalysis. They are an integral part of boron chemistry, which has attracted tremendous research interest over the past few decades. In this perspective, we provide an in-depth analysis of the reaction chemistry of boryl compounds from a structure and bonding perspective.

Tailoring the Position of Ester Group on N-Alkyl Chains of Benzotriazole-based Small Molecule Acceptors for High-Performance Organic Solar Cells.

Side chain engineering plays a vital role in exploring high-performance small molecule acceptors (SMAs) for organic solar cells (OSCs). In this work, we designed and synthesized a series of A-DA'D-A type SMAs by introducing different N-substituted alkyl and ester alkyl side chains on benzotriazole (BZ) central unit and aimed to investigate the effect of different ester substitution positions on photovoltaic performances. All the new SMAs with ester groups exhibit lower the lowest unoccupied molecular orbital (LUMO) energy levels and more blue-shifted absorption, but relatively higher absorption coefficients than alkyl chain counterpart.

Asymmetric edge supercurrents in MoTe Josephson junctions.

To investigate the higher order topology in MoTe, the supercurrent interference phenomena in Nb/MoTe/Nb planar Josephson junctions have been systematically studied. By analyzing the obtained interference pattern of the critical supercurrents and performing a comparative study of the edge-touched and untouched junctions, it's found that the supercurrent is dominated by the edges, rather than the bulk or surfaces of MoTe. An asymmetric Josephson effect with a field-tunable sign is also observed, indicating the nontrivial origin of the edge states.

Primary activation of -quinone methides by chiral phosphoric acid for enantioselective construction of tetraarylmethanes.

Demonstrated here is an asymmetric nucleophilic addition primary activation of -quinone methides (-QMs) based on a chiral phosphoric acid catalytic system. In sharp contrast to previous CPA-based bifunctional activation processes that all required the nucleophiles to have an effective hydrogen bond donor unit (, OH, NH), here no such unit is required in the nucleophile. -protected indole nucleophiles were successfully utilized for the synthesis of chiral tetraarylmethanes with high efficiency and enantioselectivity under mild conditions.

Borirenes and Boriranes: Development and Perspectives.

Strained compounds constitute a highly topical area of research in chemistry. Borirene and borirane both feature a BC three-membered ring. They can be viewed as the structural analogues of cyclopropane and cyclopropene, where a CH unit of the carbonaceous counterparts is replaced with BH, respectively.