3D-Printable Room Temperature Phosphorescence Polymer Materials with On-Demand Modulation for Modulus Visualization and Anticounterfeiting Applications.

Conventional room temperature phosphorescence (RTP) polymer materials lack a dynamic structural change mechanism for on-demand phosphorescence emission, limiting their application in specific scenarios, such as smart devices. However, the development of RTP polymer materials with an on-demand emission capability is highly attractive yet rather challenging. Herein, we report a novel RTP polymer material that doped purely organic chromophores into a polymer network with numerous free hydroxyl side chains.

An Eight-Membered Ring Molecular Framework Based on Carbazole for the Development of Electroluminescent Materials.

The organic light-emitting diode (OLED) has been regarded as the most prominent product in the current market of organic electronics, which has attracted growing attention because of their applications in full-color displays and solid-state lighting. Organic materials that exhibit strong luminescence in the solid state constitute the core position of OLED. Extensive research efforts to probe the structure of organic luminescent materials have attracted considerable attention to the conjugated fusion ring architecture.

Tailoring CO Adsorption Configuration with Spatial Confinement Switches Electroreduction Product from Formate to Acetate.

Multi-proton-coupled electron transfer, multitudinous intermediates, and unavoidable competing hydrogen evolution reaction during CO electroreduction make it tricky to control high selectivity for specific products. Here, we present spatial confinement of Fe single atoms (FeNS) by adjacent FeS clusters (FeS) to orientate the transition of CO adsorption configuration from C,O-side to O-end, which triggers a shift of activated CO from first-step protonation to C-C coupling, thus switching the target product from HCOOH in high Faraday efficiency (FE: 90.6%) on FeNS to CHCOOH (FE: 82.

Overcoming Energy Storage-Loss Trade-Offs in Polymer Dielectrics Through the Synergistic Tuning of Electronic Effects in π-Conjugated Polystyrenes.

Achieving high-performance dielectric materials remains a significant challenge due to the inherent trade-offs between high energy storage density and low energy loss. A central difficulty lies in identifying a suitable dipolar unit that can enhance the polarity and dielectric constant of the material while effectively suppressing the high energy losses associated with polarization relaxation, charge injection, and conduction. To address this, a novel strategy is proposed that introduces electron-donating and electron-withdrawing substituents on the benzene ring of polystyrene-based polymers, creating bulky dipole groups that are resistant to reorientation under an electric field.

Spin State Modulation with Oxygen Vacancy Orientates C/N Intermediates for Urea Electrosynthesis of Ultrahigh Efficiency.

The co-electrolysis of CO and NO to synthesize urea has become an effective pathway to alternate the conventional Bosch-Meiser process, while the complexity of C-/N-containing intermediates for C-N coupling results in the urea electrosynthesis of unsatisfactory efficiency. In this work, an electronic spin state modulation maneuver with oxygen vacancies (Ov) is unveiled to effectively meliorate the oriented generation of key intermediates NH and CO for C-N coupling, furnishing urea in ultrahigh yield of 2175.47 µg mg h and Faraday efficiency of 70.

Efficient Bifunctional Electrocatalysts for Oxygen Evolution/Reduction Reactions in Two-Dimensional Metal-Organic Frameworks by a Constant Potential Method.

The evolution of bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts that are highly active, stable, and conductive is crucial for advancing metal-air batteries and fuel cells. We have here thoroughly explored the OER and ORR performance for a category of two-dimensional (2D) metal-organic frameworks (MOFs) called TM(HADQ), and Rh(HADQ) exhibits a promising bifunctional OER/ORR activity, with an overpotential of 0.31 V for both OER and ORR.

Interfacial Oxygen Vacancy-Copper Pair Sites on Inverse CeO/Cu Catalyst Enable Efficient CO Electroreduction to Ethanol in Acid.

Renewable electricity-driven electrochemical reduction of CO offers a promising route for the production of high-value ethanol. However, the current state of this technology is hindered by low selectivity and productivity, primarily due to a limited understanding of the atomic-level active sites involved in ethanol formation. Herein, we identify that the interfacial oxygen vacancy-neighboring Cu (O-Cu) pair sites are the active sites for CO electroreduction to ethanol.

Li Quasi-Grotthuss Topochemistry Transport Enables Direct Regeneration of Spent Lithium-Ion Battery Cathodes.

Direct regeneration of spent lithium-ion batteries offers economic benefits and a reduced CO footprint. Surface prelithiation, particularly through the molten salt method, is critical in enhancing spent cathode repair during high-temperature annealing. However, the sluggish Li transport kinetics, which predominantly relies on thermally driven processes in the traditional molten salt methods, limit the prelithiation efficiency and regeneration of spent cathodes.

Photoredox-Catalyzed Alkene Acylesterification with Acyloxime Esters via C-C and Tertiary C-O Bond Formation.

We describe an efficient acyl esterification method for alkenes utilizing acyloxime esters as bifunctional reagents featuring radical acylation and congested C-O bond formation. This approach is characterized by mild photoredox conditions, high step and atom economy, a broad substrate scope, and excellent regioselectivity. A variety of valuable α-acyl hindered alcohol esters, including those obtained via gram-scale synthesis and late-stage functionalization of pharmaceutical molecules, were presented, demonstrating its synthetic potential and practicability.

Engineering Air-Stable Triarylmethyl Radicals with One Pyrrole Ring.

Herein, seven air-stable triarylmethyl radicals (-), each featuring a pyrrole ring, were successfully synthesized. A comprehensive investigation into the linkages at the α-, β-, and -positions of the pyrrole ring, along with various substituents, revealed that the p-π conjugation between the central radical carbon and the pyrrole ring plays a crucial role in the distribution of spin density and overall stability. Notably, radicals to displayed excellent electrochemical and photostability.

Recent Advances in Wide-Range Temperature Metal-CO Batteries: A Mini Review.

The metal-carbon dioxide batteries, emerging as high-energy-density energy storage devices, enable direct CO utilization, offering promising prospects for CO capture and utilization, energy conversion, and storage. However, the electrochemical performance of M-CO batteries faces significant challenges, particularly at extreme temperatures. Issues such as high overpotential, poor charge reversibility, and cycling capacity decay arise from complex reaction interfaces, sluggish oxidation kinetics, inefficient catalysts, dendrite growth, and unstable electrolytes.

The SUMO (Singly Unoccupied Molecular Orbital)-LUMO (Lowest Unoccupied Molecular Orbital) Inversion Radicals.

Herein, SUMO-LUMO inversion (SLI) radicals - were designed by the combination of the tris(2,4,6-trichlorophenyl)methyl (TTM) radical and pyridinium derivatives (electron-withdrawing groups) for the first time. The energy of the LUMO lies below that of the SUMO, which deviated from the Aufbau principle as an alternative electronic configuration beyond the well-established SOMO-HOMO inversed system. Thus, for SLI radicals, the injection of one extra electron preferred to occupy the LUMO rather than the SUMO, giving diradicals, one of which had been fully confirmed by single crystal analysis, VT-NMR and VT-EPR experiments, as well as DFT calculations.

A Wet-Adhesion and Swelling-Resistant Hydrogel for Fast Hemostasis, Accelerated Tissue Injury Healing and Bioelectronics.

Hydrogel bioadhesives with adequate wet adhesion and swelling resistance are urgently needed in clinic. However, the presence of blood or body fluid usually weakens the interfacial bonding strength, and even leads to adhesion failure. Herein, profiting from the unique coupling structure of carboxylic and phenyl groups in one component (N-acryloyl phenylalanine) for interfacial drainage and matrix toughening as well as various electrostatic interactions mediated by zwitterions, a novel hydrogel adhesive (PAAS) is developed with superior tissue adhesion properties and matrix swelling resistance in challenging wet conditions (adhesion strength of 85 kPa, interfacial toughness of 450 J m, burst pressure of 514 mmHg, and swelling ratio of <4%).

Synthesis of fluorine-containing bicyclo[4.1.1]octenes photocatalyzed defluorinative (4 + 3) annulation of bicyclo[1.1.0]butanes with -difluoroalkenes.

Although bicyclo[4.1.1] systems are privileged scaffolds in many natural products and drug molecules, efficient synthetic approaches to these systems remain underdeveloped.

Tough Polyurethane Hydrogels with a Multiple Hydrogen-Bond Interlocked Bicontinuous Phase Structure Prepared by In Situ Water-Induced Microphase Separation.

Hydrogels with mechanical performances similar to load-bearing tissues are in demand for in vivo applications. In this work, inspired by the self-assembly behavior of amphiphilic polymers, polyurethane-based tough hydrogels with a multiple hydrogen-bond interlocked bicontinuous phase structure through in situ water-induced microphase separation strategy are developed, in which poly(ethylene glycol)-based polyurethane (PEG-PU, hydrophilic) and poly(ε-caprolactone)-based polyurethane (PCL-PU, hydrophobic) are blended to form dry films followed by water swelling. A multiple hydrogen bonding factor, imidazolidinyl urea, is introduced into the synthesis of the two polyurethanes, and the formation of multiple hydrogen bonds between PEG-PU and PCL-PU can promote homogeneous microphase separation for the construction of bicontinuous phase structures in the hydrogel network, by which the hydrogel features break strength of 12.

Low-Frequency Phonon Dispersion Relation Enabling Stable Cathode from Spent Lithium-Ion Batteries.

Direct recycling technology can effectively solve the environmental pollution and resource waste problems caused by spent lithium-ion batteries. However, the repaired LiNiCoMnO (NCM) black mass by direct recycling technology shows an unsatisfactory cycle life, which is attributed to the formation of spinel/rock salt phases and rotational stacking faults caused by the in-plane and out-of-plane migration of transition metal (TM) atoms during charge/discharge. Herein, local lattice stress is introduced into the regenerated cathode during repair.

Atmospheric Pressure Chemical Ionization Q-Orbitrap Mass Spectrometry Analysis of Gas-Phase High-Energy Dissociation Routes of Triarylamine Derivatives.

Triarylamine groups have been widely utilized in the development of high-performance charge-transporting or luminescent materials for fabricating organic light-emitting diodes (OLEDs). In this study, atmospheric pressure chemical ionization (APCI) Q-Orbitrap mass spectrometry was adopted to investigate the dissociation behaviors of these triarylamine derivatives. Specifically, taking [M+H] as the precursor ion, high-energy collision dissociation (HCD) experiments within the energy range from 0 to 80 eV were carried out.

Photoinduced Aromatization-Driven Deconstructive Fluorosulfonylation of Spiro Dihydroquinazolinones.

A catalyst-free photoinduced deconstructive fluorosulfonylation cascade of spiro dihydroquinazolinones with DABSO and NFSI is reported. This protocol features mild reaction conditions, good yields and excellent functional group tolerance, providing a practical approach to the quinazolin-4(1)-one-functionalized aliphatic sulfonyl fluorides. In addition, the ease of gram-scale synthesis and the versatility of the SuFEx exchange highlight the application potential of this protocol.

Miniaturized silicon-based capacitive six-axis force/torque sensor with large range, high sensitivity, and low crosstalk.

Miniaturized six-axis force/torque sensors have potential applications in robotic tactile sensing, minimally invasive surgery, and other narrow operating spaces, where currently available commercial sensors cannot meet the requirements because of their large size. In this study, a silicon-based capacitive six-axis force/torque sensing chip with a small size of 9.3 × 9.

Specific Adsorption of Alkaline Cations Enhances CO-CO Coupling in CO Electroreduction.

Electrolyte alkaline cations can significantly modulate the reaction selectivity of electrochemical CO reduction (eCOR), enhancing the yield of the valuable multicarbon (C) chemical feedstocks. However, the mechanism underlying this cation effect on the C-C coupling remains unclear. Herein, by performing constant-potential AIMD simulations, we studied the dynamic behavior of interfacial K ions over Cu surfaces during C-C coupling and the origin of the cation effect.

Bubbling Chemical Vapors in Molten Metal toward XIV-Group Nanosheets.

Two-dimensional (2D) XIV-group nanosheets (germanene, silicene, and stannene) possess unique physical and chemical features promising in fields of electronics, energy storage, and conversions. However, preparing these nanosheets is challenging owing to their non van der Waals structure with strong chemical bonds inside. Herein, a bubbling chemical-vapor growth method is proposed to synthesize these XIV-group nanosheets by bubbling XIV-group-element chlorides in molten sodium.