Modulatory spin-flip of triplet excitons diversiform electron-donating units for MR-TADF emitters towards solution-processed narrowband OLEDs.

Multiple resonance thermally activated delayed fluorescence (MR-TADF) molecules are emerging as promising candidates for high-resolution organic light-emitting diode (OLED) displays, but MR-TADF emitters always suffer from an unsatisfactory rate constant of reverse intersystem crossing ( ) due to inherently low spin orbital coupling strength between excited singlet and triplet states. Herein, we systematically investigate the long-range charge transfer (LRCT) and heavy-atom effects on modulating the excited state natures and energy levels integrating diversiform electron-donating units with the MR skeleton. Compared with unsubstituted analogues, newly designed MR-TADF emitters exhibit significantly boosted values and close-to-unity photoluminescence quantum yield especially for BuCzBN-PXZ (2.

π-extended pyrenes: from an antiaromatic buckybowl to doubly curved nanocarbons with gulf architectures.

The synthesis of π-extended pyrenes keeps attracting considerable attention. In particular, frameworks containing nonbenzenoid rings might display intriguing properties. Here, we report a practical synthetic pathway to access a new buckybowl (1), which is composed of four five-membered rings externally fused to a pyrene core.

A record-high EQE of 7.65%@3300 cd m achieved in non-doped near-ultraviolet OLEDs based on novel D'-D-A type bipolar fluorophores upon molecular configuration engineering.

Developing a high-performance near-ultraviolet (NUV) material and its simple non-doped device with a small efficiency roll-off and good color purity is a promising but challenging task. Here, we proposed a novel donor'-donor-acceptor (D'-D-A) type molecular strategy to largely solve the intrinsic contradictions among wide-bandgap NUV emission, fluorescence efficiency, carrier injection and transport. An efficient NUV fluorophore, 3,6-mPPICNC3, exhibiting a hybridized local and charge-transfer state, is achieved through precise molecular configuration engineering, realizing similar hole and electron mobilities at both low and high electric fields.

Revealing the synergistic effect of Ni single atoms and adjacent 3d metal doped Ni nanoparticles in electrocatalytic CO reduction.

Herein, we report the successful fabrication of a series of transition metal doped Ni nanoparticles (NPs) coordinated with Ni single atoms in nitrogen-doped carbon nanotubes (denoted as NiM-NCNTs, M = Mn, Fe, Co, Cu and Zn; Ni = Ni single atom). X-ray absorption fine structure reveals the coexistence of Ni single atoms with Ni-N coordination and NiM NPs. When applied for electrocatalytic CORR, the NiM-NCNT compounds show the Faradaic efficiency of CO (FE) with a volcano-like tendency of Mn < Fe ≈ Co < Zn < Cu, in which the NiCu-NCNT exhibits the highest FE of 96.

Expression of concern: Synthesis of a FeO@P4VP@metal-organic framework core-shell structure and studies of its aerobic oxidation reactivity.

Expression of concern for 'Synthesis of a FeO@P4VP@metal-organic framework core-shell structure and studies of its aerobic oxidation reactivity' by Zongcheng Miao , , 2017, , 2773-2779, https://doi.org/10.1039/C6RA25820D.

Fluorescent naphthalimide boronates as theranostics: structural investigations, confocal fluorescence and multiphoton fluorescence lifetime imaging microscopy in living cells.

New design and synthetic strategies were developed to generate functional phenyl boronic acid (BA)-based fluorescent probes incorporating the 1,8-naphthalimide (NI) tag. This fluorescent core was anchored onto the BA unit through small organic linkers consisting of nitrogen groups which can arrest, and internally stabilise the phenyl-boronate units. The newly synthesised fluorophores were characterised spectroscopically by NMR spectroscopy and mass spectrometry and evaluated for their ability to bind to a naturally occurring polysaccharide, β-d-glucan in DMSO and simultaneously as act as cell imaging reagents.

Buckybowl and its chiral hybrids featuring eight-membered rings and helicene units.

Here we report the synthesis of a novel buckybowl (7) with a high bowl-to-bowl inversion barrier (Δ = 38 kcal mol), which renders the rate of inversion slow enough at room temperature to establish two chiral polycyclic aromatic hydrocarbons (PAHs). By strategic fusion of eight-membered rings to the rim of 7, the chiral hybrids 8 and 9 are synthesized and display helicity and positive and negative curvature, allowing the enantiomers to be configurationally stable and their chiroptical properties are thoroughly examined. Computational and experimental studies reveal the enantiomerization mechanisms for the chiral hybrids and demonstrate that the eight-membered ring strongly affects the conformational stability.

Enhancing the quantum yield of singlet oxygen: photocatalytic degradation of mustard gas simulant 2-chloroethyl ethyl sulfide catalyzed by a hybrid of polyhydroxyl aluminum cations and porphyrin anions.

By combining the anionic salt meso-tetra(4-carboxyphenyl)porphyrin (TCPP) and the Keggin polyoxometalate cation cluster [AlO(OH)(HO)] a simple ion-exchange method, a hybrid (CHNO)[AlO(OH)(HO)](OH)·18HO (Al-TCPP) was prepared and thoroughly characterized as a prototype of polyoxometalate-porphyrin hybrids for the photocatalytic degradation of the mustard gas simulant 2-chloroethyl ethyl sulfide (CEES). The experimental results showed that the catalytic degradation rate of CEES in the presence of Al-TCPP reached 96.16 and 99.

Reverse atom transfer radical polymerization of dimethyl itaconate initiated by a new azo initiator: AIBME.

Reverse atom transfer radical polymerization (RATRP) was used to synthesize poly(dimethyl itaconate) (PDMI) using an AIBME/CuBr/dNbpy system. The number average molecular weight ( ) of PDMI was as high as = 15 000 g mol, the monomer conversion rate reached up to 70%, and the dispersity remained low ( = 1.06-1.

Direct oxidation of -ynylsulfonamides into -sulfonyloxoacetamides with DMSO as a nucleophilic oxidant.

-Arylethynylsulfonamides are oxidized into -sulfonyl-2-aryloxoacetamides directly and efficiently with dimethyl sulfoxide (DMSO) as both an oxidant and solvent with microwave assistance. DFT calculations indicate that DMSO nucleophilically attacks the ethylic triple bond and transfers its oxygen atom to the triple bond to form zwitterionic anionic -sulfonyliminiums to trigger the reaction. Then it nucleophilically attacks the generated iminium intermediates to accomplish the oxidation the second oxygen atom transfer.

Synergism of carbon quantum dots and Au nanoparticles with BiMoO for activity enhanced photocatalytic oxidative degradation of phenol.

Localized surface plasmon resonance (LSPR) offers an opportunity to enhance the efficiency of photocatalysis. However, the photocatalysts's plasmonic enhancement is still limited, as most metals/semiconductors depend on LSPR contribution of isolated metal nanoparticles. In the present work, carbon quantum dots (CQDs) and Au nanoparticles (NPs) were simultaneously assembled on the surface of a three-dimensional (3D) spherical BiMoO (BMO) nanostructure with surface oxygen vacancies (SOVs).

Metal-support interaction induced ZnO overlayer in Cu@ZnO/AlO catalysts toward low-temperature water-gas shift reaction.

The water-gas shift reaction (WGSR) plays a pivotal role in many important industrial processes as well as in the elimination of residual CO in feed gas for fuel cells. The development of a high-efficiency low-temperature WGSR (LT-WGSR) catalyst has attracted considerable attention. Herein, we report a ZnO-modified Cu-based nanocatalyst (denoted as Cu@ZnO/AlO) obtained an topological transformation from a CuZnAl-layered double hydroxide (CuZnAl-LDH) precursor at different reduction temperatures.

Stereodivergent synthesis of β-iodoenol carbamates with CO photocatalysis.

Photocatalytic conversion of carbon dioxide (CO) into value-added chemicals is of great significance from the viewpoint of green chemistry and sustainable development. Here, we report a stereodivergent synthesis of β-iodoenol carbamates through a photocatalytic three-component coupling of ethynylbenziodoxolones, CO and amines. By choosing appropriate photocatalysts, both - and -isomers of β-iodoenol carbamates, which are difficult to prepare using existing methods, can be obtained stereoselectively.

A pH-responsive ultrathin Cu-based nanoplatform for specific photothermal and chemodynamic synergistic therapy.

Noninvasive tumor therapy requires a new generation of bionanomaterials towards sensitive response to the unique tumor microenvironment to achieve accurate and effective treatment. Herein, we have developed a tumor therapy nanoplatform by immobilizing natural glucose oxidase (GOD) onto Cu-based layered double hydroxide (CuFe-LDH) nanosheets, which for the first time integrates acid-enhanced photothermal therapy (PTT), and pH-responsive and heat-facilitated chemodynamic therapy (CDT) simultaneously. As demonstrated by EXAFS and HRTEM, CuFe-LDH nanosheets possess a considerable number of defects caused by different acid conditions, resulting in a significantly acid-enhanced photothermal conversion efficiency (83.

Phase engineering of cobalt hydroxide toward cation intercalation.

Multi-cation intercalation in aqueous and neutral media is promising for the development of high-safety energy storage devices. However, developing a new host matrix for reversible cation intercalation as well as understanding the relationship between cation intercalation and the interlayer structure is still a challenge. In this work, we demonstrate layered cobalt hydroxides as a promising host for cation interaction, which exhibit high metal ion (Li, Na, K, Mg and Ca) storage capacities after phase transformation.

Phenol-like group functionalized graphene quantum dots structurally mimicking natural antioxidants for highly efficient acute kidney injury treatment.

Acute kidney injury (AKI) is a syndrome characterized by rapid loss of renal excretory function with high in-hospital mortality. The excess generation of reactive oxygen species (ROS) in the kidneys during AKI has been considered a major cause of renal failure. Currently available antioxidants for AKI treatment often lack the required antioxidative efficacy or renal accumulation rate.

Regiocontrolled dimerization of asymmetric diazaheptacene derivatives toward X-shaped porous semiconductors.

Conformationally rigid X-shaped PAHs are attracting interest due to their self-assembly into unique networks and as models to study through-space exciton and charge delocalization in one single molecule. We report here the synthesis of X-shaped PAHs by dimerization of diazaheptacene diimides. The diimide groups are employed to effectively direct the self-assembly into antiparallel dimer aggregates, which assist the compounds to undergo a regiocontrolled [4 + 4] dimerization, leading to an X-shaped conformation bearing electron-poor and -rich subunits.

Deep-red fluorescence from isolated dimers: a highly bright excimer and imaging .

Restricted by the energy-gap law, the development of bright near-infrared (near-IR) fluorescent luminophors in the solid state remains a challenge. Herein, we report a new design strategy for realizing high brightness and deep-red/near-IR-emissive organic molecules based on the incorporation of a hybridized local and charge-transfer (HLCT) state and separated dimeric stacks into one aggregate. Experimental and theoretical analyses show that this combination not only contributes to high photoluminescent quantum yields (PLQYs) but also significantly lessens the energy gap.

Reversible Treatment of Pressure Overload-Induced Left Ventricular Hypertrophy through Nucleic Acid Delivery Mediated by Functional Polyaminoglycoside.

Left ventricular hypertrophy and fibrosis are major risk factors for heart failure, which require timely and effective treatment. Genetic therapy has been shown to ameliorate hypertrophic cardiac damage. In this study, it is found that in mice, the dopamine D5 receptor (D5R) expression in the left ventricle (LV) progressively decreases with worsening of transverse aortic constriction-induced left ventricular hypertrophy.

Highly Accessible Atomically Dispersed Fe-N Sites Electrocatalyst for Proton-Exchange Membrane Fuel Cell.

Atomically dispersed transition metal-N sites have emerged as a frontier for electrocatalysis because of the maximized atom utilization. However, there is still the problem that the reactant is difficult to reach active sites inside the catalytic layer in the practical proton exchange membrane fuel cell (PEMFC) testing, resulting in the ineffective utilization of the deeply hided active sites. In the device manner, the favorite structure of electrocatalysts for good mass transfer is vital for PEMFC.

Quantitative evaluation of the non-thermal effect in microwave induced polymer curing.

Microwave irradiation is one of the most effective strategies to accelerate the curing of resin. However, the mechanism is still unclear. The debates mainly focus on how to quantitatively evaluate the 'non-thermal' effect of the microwave.

Excellent humidity sensor based on ultrathin HKUST-1 nanosheets.

The copper-based MOF, HKUST-1 has been applied for humidity sensing owing to hydrophilic ligands and open metal sites which are suitable for sensitively detecting moisture. However, most of the research on the sensor HKUST-1 focuses on the role of the central metal. There are few reports on the morphology-activity relationship of HKUST-1.

Multicomponent Transition Metal Dichalcogenide Nanosheets for Imaging-Guided Photothermal and Chemodynamic Therapy.

Transition metal dichalcogenides (TMDs) have received considerable attention due to their strong absorption in the near-infrared (NIR) region, strong spin-orbit coupling, and excellent photothermal conversion efficiency (PCE). Herein, CoFeMn dichalcogenide nanosheets (CFMS NSs) are prepared via facile vulcanization of a lamellar CoFeMn-layered double hydroxide (LDH) precursor followed by polyvinyl pyrrolidone modification (to give CFMS-PVP NSs), and found to show excellent photoacoustic (PA) imaging and synergistic photothermal/chemodynamic therapy (PTT/CDT) performance. The as-prepared CFMS-PVP NSs inherit the ultrathin morphology of the CoFeMn-LDH precursor and exhibit an outstanding photothermal performance with a of 89.