A recyclable dynamic semiconducting polymer consisting of Pauli-paramagnetic diradicaloids promoted and stabilized by catechol-boron coordination.

Coordination between 5,5',6,6'-tetrahydroxyindigo (4OH-ID) and boron tribromide unexpectedly affords a novel dynamic covalent polymer, namely P(ID-O-B), consisting of alternating indigo and indigo diradicaloid units. The catechol-boron dynamic bond plays a vital role in promoting the diradicaloid formation and stabilizing the formed diradicaloid segments. The diradicaloid segment in the polymer has a triplet ground state and a thermally populated doublet state, which has been confirmed by the EPR study.

A high entropy metallic-high entropy nonmetallic community as a high performance electrocatalyst for the oxygen evolution reaction and oxygen reduction reaction.

The multi-element synergism in high-entropy materials (HEMs) provides great opportunities as multi-functional catalysts or for the promotion of tandem reactions. Herein, a strategy that utilizes a high entropy precursor is proposed to realize the formation of a unique high entropy metallic-high entropy non-metallic community (HEM-HENMC). Aminotriazole acts as a "bonding agent" for the high entropy precursor, and not only binds the five metals Cr, Mn, Fe, Co and Ni together, but also introduces nitrogen and carbon .

An electrochemiluminescence device for visualized detection of lead in practical samples.

Lead (Pb) pollution poses a significant threat to human health due to its potential accumulation through the food chain. In response to this challenge, an array of electrochemiluminescence (ECL) devices has been developed for the accurate and visualized detection of trace Pb, achieving an ultra-low limit of detection (LOD) of 9.8 pg L.

Efficient helical columnar emitters of chiral homoleptic Pt(ii) metallomesogens for circularly polarized electroluminescence.

Chiral organometallic Pt(ii) complexes have been demonstrated to be excellent circularly polarized luminescence (CPL) materials due to their rich phosphorescence and strong self-assembly characteristics. However, it remains a formidable task to simultaneously achieve high luminance () and electroluminescence dissymmetry factor ( ) values for circularly polarized electroluminescence (CP-EL) devices of Pt(ii) complex-based emitters. In this study, we carry out a straightforward and efficient protocol to construct highly CPL-active helical columnar () emitters by using chiral homoleptic triazolatoplatinum(ii) metallomesogens (/-HPt).

Efficient circularly polarized multiple resonance thermally activated delayed fluorescence from B,N-embedded hetero[8]helicene enantiomers.

Helicene-based circularly polarized multiple resonance thermally activated delayed fluorescence (CP-MR-TADF) materials are promising for ultra-high-definition and 3D displays, but most of them encounter potential problems such as easy racemization during the thermal deposition process, low luminous efficiency, and low luminescence dissymmetry factor ( ), making the development of efficient circularly polarized organic light-emitting diodes (CP-OLEDs) a significant challenge. Here, we report a pair of CP-MR-TADF enantiomers with high-order B,N-embedded hetero[8]helicene, (/)-BN-TP-ICz, by fusing two MR chromophores, DtCzB and indolo[3,2,1-]carbazole (ICz). BN-TP-ICz exhibits green emission in toluene with a peak of 531 nm and a full-width at half-maximum (FWHM) of 36 nm.

Rational design of CT-coupled J-aggregation platform based on Aza-BODIPY for highly efficient phototherapy.

Supramolecular engineering is exceptionally appealing in the design of functional materials, and J-aggregates resulting from noncovalent interactions offer intriguing features. However, building J-aggregation platforms remains a significant challenge. Herein, we report 3,5-dithienyl Aza-BODIPYs with a donor-acceptor-donor (D-A-D) architecture as the first charge transfer (CT)-coupled J-aggregation BODIPY-type platform.

Ultrafast C-C and C-N bond formation reactions in water microdroplets facilitated by the spontaneous generation of carbocations.

Carbocations are important electrophilic intermediates in organic chemistry, but their formation typically requires harsh conditions such as extremely low pH, elevated temperature, strong oxidants and/or expensive noble-metal catalysts. Herein, we report the spontaneous generation of highly reactive carbocations in water microdroplets by simply spraying a diarylmethanol aqueous solution. The formation of transient carbocations as well as their ultrafast in-droplet transformations through carbocation-involved C-C and C-N bond formation reactions are directly characterized by mass spectrometry.

Macroscopic handedness inversion of terbium coordination polymers achieved by doping homochiral ligand analogues.

Inspired by natural biological systems, chiral or handedness inversion by altering external and internal conditions to influence intermolecular interactions is an attractive topic for regulating chiral self-assembled materials. For coordination polymers, the regulation of their helical handedness remains little reported compared to polymers and supramolecules. In this work, we choose the chiral ligands -pempH (pempH = (1-phenylethylamino)methylphosphonic acid) and -XpempH (X = F, Cl, Br) as the second ligand, which can introduce C-H⋯π and C-H⋯X interactions, doped into the reaction system of the Tb(-cyampH)·3HO (cyampH = (1-cyclohexylethylamino)methylphosphonic acid) coordination polymer, which itself can form a right-handed superhelix by van der Waals forces, and a series of superhelices -1H-, -2F-, -3Cl-, and -4Br- with different doping ratios were obtained, whose handedness is related to the second ligand and its doping ratio, indicating the decisive role of interchain interactions of different strengths in the helical handedness.

Site-selective heat boosting electrochemiluminescence for single cell imaging.

visualization of local electrochemical reactions provides mechanical insights into the dynamic transport of interfacial charge and reactant/product. Electrochemiluminescence is a crossover technique that quantitatively determines Faraday current and mass transport in a straightforward manner. However, the sensitivity is hindered by the low collision efficiency of radicals and side reactions at high voltage.

Regulating tumor glycometabolism and the immune microenvironment by inhibiting lactate dehydrogenase with platinum(iv) complexes.

Lactate dehydrogenase (LDH) is a key enzyme involved in the process of glycolysis, assisting cancer cells to take in glucose and generate lactate, as well as to suppress and evade the immune system by altering the tumor microenvironment (TME). Platinum(iv) complexes MDP and DDP were prepared by modifying cisplatin with diclofenac at the axial position(s). These complexes exhibited potent antiproliferative activity against a panel of human cancer cell lines.

Catalytic asymmetric indolization by a desymmetrizing [3 + 2] annulation strategy.

A new catalytic asymmetric indolization reaction by a desymmetrizing [3 + 2] annulation strategy is developed. The reaction proceeds a rhodium-catalyzed enantioposition-selective addition/5--trig cyclization/dehydration cascade between -amino arylboronic acids and 2,2-disubstituted cyclopentene-1,3-diones to produce -unprotected cyclopenta[]indoles bearing an all-carbon quaternary stereocenter in high yields with good enantioselectivities. A quantitative structure-selectivity relationship (QSSR) model was established to identify the optimal chiral ligand, which effectively controlled the formation of the stereocenter away from the reaction site.

Manganese(ii) complexes stimulate antitumor immunity aggravating DNA damage and activating the cGAS-STING pathway.

Activating the cyclic GMP-AMP synthase-stimulator of the interferon gene (cGAS-STING) pathway is a promising immunotherapeutic strategy for cancer treatment. Manganese(ii) complexes MnPC and MnPVA (P = 1,10-phenanthroline, C = chlorine, and VA = valproic acid) were found to activate the cGAS-STING pathway. The complexes not only damaged DNA, but also inhibited histone deacetylases (HDACs) and poly adenosine diphosphate-ribose polymerase (PARP) to impede the repair of DNA damage, thereby promoting the leakage of DNA fragments into cytoplasm.

An enzyme-powered microRNA discriminator for the subtype-specific diagnosis of breast cancer.

Breast cancer, a disease with highly heterogeneous features, is the most common malignancy diagnosed in people worldwide. Early diagnosis of breast cancer is crucial for improving its cure rate, and accurate classification of the subtype-specific features is essential to precisely treat the disease. An enzyme-powered microRNA (miRNA, RNA = ribonucleic acid) discriminator was developed to selectively distinguish breast cancer cells from normal cells and further identify subtype-specific features.

From amorphous to crystalline: a universal strategy for structure regulation of high-entropy transition metal oxides.

High-entropy materials (HEMs) exhibit extensive application potential owing to their unique structural characteristics. Structure regulation is an effective strategy for enhancing material performance. However, the fabrication of HEMs by integrating five metal elements into a single crystalline phase remains a grand challenge, not to mention their structure regulation.

BOINPYs: facile synthesis and photothermal properties triggered by photoinduced nonadiabatic decay.

Photothermal agents (PTAs) represent a core component of photothermal therapy (PTT). However, the current photothermal dyes are almost derived from well-known chromophores such as porphyrins, cyanine, and BODIPYs, and the design of new chromophores as versatile building blocks for PTA is considerably challenging because of the complexity of the modulation of excited-states. Herein, we adopted the concept of photoinduced nonadiabatic decay (PIND) to develop a photothermal boron-containing indoline-3-one-pyridyl chromophore (.

Single-atom engineering of hemicyanine and its amphiphilic derivative for optimized near infrared phototheranostics.

Near-infrared (NIR) dyes are widely used in the field of phototheranostics. Hemicyanine dyes (HDs) have recently received tremendous attention due to their easy synthesis and excellent NIR features. However, HDs can easily form non-fluorescent aggregates and their potential for phototherapy still needs further exploration due to their poor ability to generate reactive oxygen species (ROS).

High-efficiency and durable V-Ti-Nb ternary catalyst prepared by a wet-solid mechanochemical method for sustainably producing acrylic acid acetic acid-formaldehyde condensation.

Based on the precise phase control V species adjustment of vanadium phosphorus oxides (VPOs), a series of metal oxides (NbO, MoO, WO, and BiO) were selected as modification agents to further enhance the catalytic activity and retain the excellent durability of VPO-TiO-based catalysts for the new procedure of producing acrylic acid acetic acid-formaldehyde condensation. At an elevated liquid hourly space velocity (LHSV), the (AA + MA) selectivity reached 92.3% with a (MA + AA) formation rate of 63.

A temperature-tuned electrochemiluminescence layer for reversibly imaging cell topography.

Investigating electrochemiluminescence (ECL) scenarios under different temperatures is important to expand its imaging scope near an electrode surface. Here, we develop a temperature-tuned ECL layer by recording the evolution of shadow regions of adherent cells. Finite element simulation and experimental results demonstrate that the thickness of the ECL layer (TEL) is reversibly regulated by electrode temperature ( ), so that single cell topography at different heights is imaged.

A self-powered and drug-free diabetic wound healing patch breaking hyperglycemia and low HO limitations and precisely sterilizing driven by electricity.

Accelerating diabetes-related chronic wound healing is a long-sought-after goal in diabetes management. However, therapeutic strategies based on antibiotics or catalysts still face great challenges to break the limitations of antimicrobial resistance, low HO and the blocking effect of bacterial biofilms on antibiotic/catalyst penetration. Herein, we reported a glucose biofuel cell-powered and drug-free antibacterial patch, which consisted of an MAF-7 protected glucose oxidase/horseradish peroxidase anode and a horseradish peroxidase cathode, for treating diabetic wounds.

Correction: An engineered third electrostatic constriction of aerolysin to manipulate heterogeneously charged peptide transport.

[This corrects the article DOI: 10.1039/D1SC06459B.].

Insights into electrochemiluminescence dynamics by synchronizing real-time electrical, luminescence, and mass spectrometric measurements.

Electrochemiluminescence (ECL) comprises a sophisticated cascade of reactions. Despite advances in mechanistic studies by electrochemistry and spectroscopy, a lack of access to dynamic molecular information renders many plausible ECL pathways unclear or unproven. Here we describe the construction of a real-time ECL mass spectrometry (MS) platform (RT-Triplex) for synchronization of dynamic electrical, luminescent, and mass spectrometric outputs during ECL events.

Profiling single-molecule reaction kinetics under nanopore confinement.

The study of a single-molecule reaction under nanoconfinement is beneficial for understanding the reactive intermediates and reaction pathways. However, the kinetics model of the single-molecule reaction under confinement remains elusive. Herein we engineered an aerolysin nanopore reactor to elaborate the single-molecule reaction kinetics under nanoconfinement.