Selenium-induced anion vacancy and active site migration stimulating remarkable sulfide Na-Ion storage.

Heterojunctions and controllable anionic vacancies are perceived to be powerful means of ameliorating the performance of sodium-ion batteries assignable to their unique physical and chemical properties. However, the mechanism by which heterojunction and vacancy structures affect sodium-ion battery storage remains to be systemically explored. In this study, the Se doped CoS@CoS@Carbon (Se-CoS@CoS@C) heterostructure with anion vacancy was synthesized by a one-step calcination.

Metal-free, photoredox-catalyzed aromatization-driven deconstructive functionalization of spiro-dihydroquinazolinones with α-CF alkenes.

Metal-free, photoredox-catalyzed aromatization-driven deconstructive functionalization of spiro-dihydroquinazolinones with α-CF alkenes is presented. The readily available spiro-dihydroquinazolinones reacted efficiently with α-CF alkenes during photocatalysis to give the -difluoroallylated and the CF-containing quinazolin-4(3)-ones in good yields with excellent chemoselectivity. The selectivity depends on the electron effect of substituents in α-CF alkenes.

Photoredox-Catalyzed Sequential Decarboxylative/Defluorinative Aminoalkylation of CF-Alkenes with -Arylglycines.

A photoredox-catalyzed sequential decarboxylative/defluorinative aminoalkylation of CF-alkenes with -arylglycines is described. This metal-free and redox-neutral protocol provided efficient access to the monofluoroalkenyl-1,5-diamines in good yields with excellent functional group compatibility. Mechanistic studies revealed that the reaction proceeds via a radical pathway with the -difluoroalkenyl amine as an intermediate.

Revealing the Limitation Induced by Hydroxyl in Regulating Solvation Structure of Zn and Overcoming Challenges with Hybrid Additives towards Highly Stable Zinc Anodes.

In the field of electrolyte design for aqueous zinc-ion batteries (AZIBs), additives containing hydroxyl have been demonstrated to effectively modulate the solvation structure of Zn. However, reported studies typically focus solely on the effectiveness of hydroxyl while neglecting the issues that emerge during solvation structure regulation. The strong electron-attracting capability of Zn attracts electrons from the oxygen in hydroxyl, thereby weakening the strength of hydroxyl, the hydrogen evolution reaction (HER) is also pronounced.

Overcoming challenges of protonation effects induced by high isoelectric point amino acids through a synergistic strategy towards highly stable and reversible zinc electrode-electrolyte interface.

Amino acids are among the most commercially promising additive solutions for achieving stable zinc anodes. However, greater attention should be given to the limitation arising from the protonation effects induced by high isoelectric point amino acids in the weakly acidic electrolytes of aqueous zinc-ion batteries (AZIBs). In this study, we introduce histidine (HIS) and ethylenediaminetetraacetic acid (EDTA) as hybrid additives into the aqueous electrolyte.

Computational Studies of Reactions of 1,2,4,5-Tetrazines with Enamines in MeOH and HFIP.

The reaction between 1,2,4,5-tetrazines and alkenes in polar solvents proceeds through a Diels-Alder cycloaddition along the C-C axis (C3/C6 cycloaddition) of the tetrazine, followed by dinitrogen loss. By contrast, the reactions of 1,2,4,5-tetrazines with enamines in hexafluoroisopropanol (HFIP) give 1,2,4-triazine products stemming from a formal Diels-Alder addition across the N-N axis (N1/N4 cycloaddition). We explored the mechanism of this interesting solvent effect through DFT calculations in detail and revealed a novel reaction pathway characterized by C-N bond formation, deprotonation, and a 3,3-sigmatropic rearrangement.

Microporous Materials in Polymer Electrolytes: The Merit of Order.

Solid-state batteries (SSBs) have garnered significant attention in the critical field of sustainable energy storage due to their potential benefits in safety, energy density, and cycle life. The large-scale, cost-effective production of SSBs necessitates the development of high-performance solid-state electrolytes. However, the manufacturing of SSBs relies heavily on the advancement of suitable solid-state electrolytes.

Achieving pure room temperature phosphorescence (RTP) in phenoselenazine-based organic emitters through synergism among heavy atom effect, enhanced n → π* transitions and magnified electron coupling by the A-D-A molecular configuration.

The weak spin-orbit coupling (SOC) in metal-free organic molecules poses a challenge in achieving phosphorescence emission. To attain pure phosphorescence in RTP organic emitters, a promising molecular design concept has been proposed. This involves incorporating n → π* transitions and leveraging the heavy atomic effect within the spin-orbit charge transfer-induced intersystem crossing (SOCT-ISC) mechanism of bipolar molecules.

Flexible iontronics with super stretchability, toughness and enhanced conductivity based on collaborative design of high-entropy topology and multivalent ion-dipole interactions.

All-solid-state ionic conductive elastomers (ASSICEs) are emerging as a promising alternative to hydrogels and ionogels in flexible electronics. Nevertheless, the synthesis of ASSICEs with concomitant mechanical robustness, superior ionic conductivity, and cost-effective recyclability poses a formidable challenge, primarily attributed to the inherent contradiction between mechanical strength and ionic conductivity. Herein, we present a collaborative design of high-entropy topological network and multivalent ion-dipole interaction for ASSICEs, and successfully mitigate the contradiction between mechanical robustness and ionic conductivity.

Tough and elastic hydrogels based on robust hydrophobicity-assisted metal ion coordination for flexible wearable devices.

Flexible wearable sensors that combine excellent flexibility, high elasticity, sensing capabilities, and outstanding biocompatibility are gaining increasing attention. In this study, we successfully develop a robust and elastic hydrogel-based flexible wearable sensor by modulating molecular structures combined with metal ion coordination. We leverage three -acryloyl amino acid monomers, including -acryloyl glycine (AG), -acryloyl alanine (AA), and -acryloyl valine (AV) with different hydrophobic groups adjacent to the carboxyl group, to copolymerize with acrylamide (AM) in the presence of Zr for hydrogel preparation in one step (P(AM-AG/AA/AV)-Zr hydrogels).

The Selectivity Origins in Ag-Catalyzed CO Electroreduction.

Ag exhibits high selectivity of electrochemical CO reduction (COR) toward C products, while the hydrogenation involving the concerted proton-electron transfer (CPET) or sequential electron-proton transfer (SEPT) mechanism is still in debate. Toward a better understanding of the Ag-catalyzed electrochemical COR, we employed a microkinetic model based on the Marcus electron transfer theory to thoroughly investigate the selectivity of C products of electrochemical COR over the Ag(111) surface. We found that at an acidic condition of pH = 1.

A gradient-distributed binder with high energy dissipation for stable silicon anode.

Silicon is considered as a promising alternative to traditional graphite anode for lithium-ion batteries. Due to the dramatic volume expansion of silicon anode generated from the insertion of Li ions, the binder which can suppress the severe volume change and repeated massive stress impact during cycling is required greatly. Herein, we design a gradient-distributed two-component binder (GE-PAA) to achieve excellent cyclic stability, and reveal the mechanism of high energy dissipative binder stabilized silicon electrodes.

Aromatization-driven deconstructive functionalization of spiro dihydroquinazolinones dual photoredox/nickel catalysis.

Aromatization-driven deconstruction and functionalization of spiro dihydroquinazolinones dual photoredox/nickel catalysis is developed. The aromatization effect was introduced to synergistically drive unstrained cyclic C-C bond cleavage, with the aim of overcoming the ring-size limitation of nitrogen-centered radical induced deconstruction of carbocycles. Herein, we demonstrate the synergistic photoredox/nickel catalyzed deconstructive cross-coupling of spiro dihydroquinazolinones with organic halides.

The third strategy: modulating emission colors of organic light-emitting diodes with UV light during the device fabrication process.

The modulation of emission color is one of the most critical topics in the research field of organic light-emitting diodes (OLEDs). Currently, only two ways are commonly used to tune the emission colors of OLEDs: one is to painstakingly synthesize different emitters with diverse molecular structures, the other is to precisely control the degree of aggregation or doping concentration of one emitter. To develop a simpler and less costly method, herein we demonstrate a new strategy in which the emission colors of OLEDs can be continuously changed with UV light during the device fabrication process.

Oxidative Tandem Cyclization of Aromatic Acids with (Benzo)thiophenes: One-Pot Access to Planar Sulfur-Containing Polycyclic Heteroarenes for Lipid-Droplet-Targeted Probes.

The efficient construction of π-conjugated polycyclic heteroarenes represents a significant task in the field of functional materials. A one-step oxidative tandem cyclization of aromatic acids with (benzo)thiophenes was developed to access planar sulfur-containing polycyclic heteroarenes. This protocol undergoes intermolecular cross-dehydrogenative coupling followed by intramolecular Friedel-Crafts acylation and provides a facile pathway to planar polycyclic compounds from inexpensive reactants.

Elevating Discharge Voltage of LiCO-Routine Li-CO Battery over 2.9 V at an Ultra-Wide Temperature Window.

The Li-CO batteries utilizing greenhouse gas CO possess advantages of high energy density and environmental friendliness. However, these batteries following LiCO-product route typically exhibit low work voltage (<2.5 V) and energy efficiency.

Regulating Zn Migration-Diffusion Behavior by Spontaneous Cascade Optimization Strategy for Long-Life and Low N/P Ratio Zinc Ion Batteries.

Parasitic side reactions and dendrite growth on zinc anodes are formidable issues causing limited lifetime of aqueous zinc ion batteries (ZIBs). Herein, a spontaneous cascade optimization strategy is first proposed to regulate Zn migration-diffusion behavior. Specifically, PAPE@Zn layer with separation-reconstruction properties is constructed in situ on Zn anode.

Surface Redox Chemistry Regulates the Reaction Microenvironment for Efficient Hydrogen Peroxide Generation.

Electrosynthesis has emerged as an enticing solution for hydrogen peroxide (HO) production. However, efficient HO generation encounters challenges related to the robust gas-liquid-solid interface within electrochemical reactors. In this work, we introduce an effective hydrophobic coating modified by iron (Fe) sites to optimize the reaction microenvironment.

Suppressed Dissolution of Fluorine-Rich SEI Enables Highly Reversible Zinc Metal Anode for Stable Aqueous Zinc-Ion Batteries.

The instability of the solid electrolyte interface (SEI) is a critical challenge for the zinc metal anodes, leading to an erratic electrode/electrolyte interface and hydrogen evolution reaction (HER), ultimately resulting in anode failure. This study uncovers that the fluorine species dissolution is the root cause of SEI instability. To effectively suppress the F dissolution, an introduction of a low-polarity molecule, 1,4-thioxane (TX), is proposed, which reinforces the stability of the fluorine-rich SEI.

Merging of Palladium and Organocatalysis Enabled Asymmetric Decarboxylative (2+1) Cycloadditions toward Cyclopropanes.

A cascade reaction enabling enantio- and diastereoselective construction of strained cyclopropanes is described. This asymmetric (2+1) annulation process uses vinyl methylene carbonate and 2-cyanoacrylate as reaction partners in the presence of Pd(PPh) as a precatalyst and an enantioenriched phosphoramidite ligand featuring a morpholine functionality. Mechanistic investigations unveil that the PPh derived from the Pd(PPh) and the morpholine-containing phosphoramidite work as cooperative phosphorus and Brønsted base catalysts to promote the reaction.

Notch-Targeted Therapeutic in Colorectal Cancer by Notch1 Attenuation Via Tumor Microenvironment-Responsive Cascade DNA Delivery.

The Notch signaling is a key molecular pathway that regulates cell fate and development. Aberrant Notch signaling can lead to carcinogenesis and progression of malignant tumors. However, current therapies targeting Notch pathway lack specificity and induce high toxicity.

pH-responsive bioadhesive with robust and stable wet adhesion for gastric ulcer healing.

Development of bioadhesives that can be facilely delivered by endoscope and exhibit instant and robust adhesion with gastric tissues to promote gastric ulcer healing remains challenging. In this study, an advanced bioadhesive is prepared through free radical polymerization of ionized N-acryloyl phenylalanine (iAPA) and N-[tris (hydroxymethyl) methyl] acrylamide (THMA). The precursory polymer solution exhibits low viscosity with the capability for endoscope delivery, and the hydrophilic-hydrophobic transition of iAPA upon exposure to gastric acid can trigger gelation through phenyl groups assisted multiple hydrogen bonds formation and repel water molecules on tissue surface to establish favorable environment for interfacial interactions between THMA and functional groups on tissues.

Revealing the interaction forms between Hg(II) and group types (-Cl, -CN, -NH, -OH, -COOH) in functionalized Poly(pyrrole methane)s for efficient mercury removal.

To explore the impact of different functional groups on Hg(II) adsorption, a range of poly(pyrrole methane)s functionalized by -Cl, -CN, -NH, -OH and -COOH were synthesized and applied to reveal the interaction between different functional groups and mercury ions in water, and the adsorption mechanism was revealed through combined FT-IR, XPS, and DFT calculations. The adsorption performance can be improved to varying degrees by the incorporation of functional groups. Among them, the oxygen-containing functional groups (-OH and -COOH) exhibit stronger affinity for Hg(II) and can increase the adsorption capacity from 180 mg g to more than 1400 mg g at 318 K, with distribution coefficient (K) exceeding 10 mL g.

Luminescent Perovskite-Cross-Linked Polymer with Low Shrinkage and Excellent Stability.

When organic cross-linked polymers are combined with metal halide perovskite nanocrystals (PNCs) for realizing luminescent perovskite-polymer display materials, the stability of PNCs is enhanced and their shrinkage is suppressed. This work presents a feasible strategy for preparing CsPbBr nanocrystals (NCs) within a polydicyclopentadiene (PDCPD) thermosetting cross-linked resin matrix simultaneously via a one-step reaction. The obtained PDCPD@PNCs composite exhibits narrow peak half-widths (15-20 nm), high light transmittance (80%), low curing volume shrinkage (1.