Objective: Vitamin D deficiency (VDD) is emerging as a predictor of poor prognosis in various neurological conditions, where clinical outcomes are often worse in stroke patients with VDD. This study aimed to provide experimental evidence on whether and how pre-existing VDD would affect survival and neurofunctional outcomes in intracerebral haemorrhage (ICH), and to evaluate whether acute vitamin D (VD) supplementation would improve post-stroke outcomes.
Methods: Experimental ICH models were induced in mice with and without VDD.
Proc Natl Acad Sci U S A
June 2024
Many cancer-driving protein targets remain undruggable due to a lack of binding molecular scaffolds. In this regard, octahedral metal complexes with unique and versatile three-dimensional structures have rarely been explored as inhibitors of undruggable protein targets. Here, we describe antitumor iridium(III) pyridinium-N-heterocyclic carbene complex , which profoundly reduces the viability of lung and breast cancer cells as well as cancer patient-derived organoids at low micromolar concentrations.
View Article and Find Full Text PDFDescribed here are sterically hindered tetradentate [Pt(O^N^C^N)] emitters (Pt-1, Pt-2, and Pt-3) developed for stable and high-performance green phosphorescent organic light-emitting diodes (OLEDs). These Pt(II) emitters exhibit strong saturated green phosphorescence (λ = 517-531 nm) in toluene and mCP thin films with emission quantum yields as high as 0.97, radiative rate constants (k) as high as 4.
View Article and Find Full Text PDFBackground: Chemoresistant cancer cells frequently exhibit a state of chronically activated endoplasmic reticulum (ER) stress. Engaged with ER stress, the unfolded protein response (UPR) is an adaptive reaction initiated by the accumulation of misfolded proteins. Protein disulfide isomerase (PDI) is a molecular chaperone known to be highly expressed in glioblastomas with acquired resistance to temozolomide (TMZ).
View Article and Find Full Text PDFAcceleration of singlet-triplet intersystem crossings (ISC) is instrumental in bolstering triplet exciton harvesting of multi-resonance thermally activated delayed fluorescent (MR-TADF) emitters. This work describes a simple gold(I) coordination strategy to enhance the spin-orbit coupling of green and blue BN(O)-based MR-TADF emitters, which results in a notable increase in rate constants of the spectroscopically observed ISC process to 3×10 s with nearly unitary ISC quantum yields. Accordingly, the resultant thermally-stable Au emitters attained large values of delayed fluorescence radiative rate constant up to 1.
View Article and Find Full Text PDFDemyelination due to oligodendrocytes loss occurs after traumatic spinal cord injury (TSCI). Several studies have suggested the therapeutic potential of vitamin D (VitD) in demyelinating diseases. However, experimental evidence in the context of TSCI is limited, particularly in the presence of prior VitD-deficiency.
View Article and Find Full Text PDFA critical step in advancing the practical application of copper-based organic light-emitting diodes (OLEDs) is to bridge the large gap between device efficiency and operational stability at practical luminance. Described is a panel of air- and thermally stable two-coordinate Cu emitters featuring bulky pyrazine- (PzIPr) or pyridine-fused N-heterocyclic carbene (PyIPr*) and carbazole (Cz) ligands with enhanced amide-Cu-carbene bonding interactions. These Cu emitters display thermally activated delayed fluorescence (TADF) from the LL'CT(Cz→PzIPr/PyIPr*) excited states across the blue to red regions with exceptional radiative rate constants of 1.
View Article and Find Full Text PDFVoltage-dependent, color-tunable organic light-emitting diodes (OLEDs) are appealing tools that can be used for the visualization of electronic output signal of sensors. Nonetheless, the literature-reported color-tunable OLEDs that have a simple single-cell device structure suffer from relatively low efficiency, pronounced efficiency roll-off, color-aging, and short operation lifetime, all of which limit their practical applications. Here, a novel co-host-in-double-emissive-layer (CHIDEL) device, designed to enhance the performance of color-tunable OLEDs with the use of a single tetradentate Pt[O N C N] emitter, is described.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2021
Photoinduced hydroarylation of alkenes is an appealing synthetic strategy for arene functionalization. Herein, we demonstrated that aryl radicals generated from electron-deficient aryl chlorides/bromides could be trapped by an array of terminal/internal aryl alkenes in the presence of [Pt(O^N^C^N)] under visible-light (410 nm) irradiation, affording anti-Markovnikov hydroarylated compounds in up to 95 % yield. Besides, a protocol for [Pt(O^N^C^N)]-catalyzed intramolecular photocyclization of acrylanilides to give structurally diverse 3,4-dihydroquinolinones has been developed.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2019
The realization of high-efficiency solution-processed organic light-emitting diodes (OLEDs) using phosphorescent tetradentate Pt(II) emitters and bipolar organic hosts is demonstrated in this work. To investigate the effect of organic host on the platinum dopant, the performances of solution-processed Pt-OLEDs with various combinations between four tetradentate Pt(II) emitters, including two newly developed and and three bipolar organic hosts , , and , have been analyzed and compared. Among the tetradentate Pt(II) complexes studied in this work, exhibited the best electroluminescent performance attributable to its bulky molecular scaffold structure, high emission quantum yield, and good solubility in common organic solvents.
View Article and Find Full Text PDFMetal-TADF (thermally activated delayed fluorescence) emitters hold promise in the development of next generation light-emitting materials for display and lighting applications, examples of which are, however, largely confined to Cu and recently Au , Ag , and Au emitters. Herein is described the design strategy for an unprecedented type of metal-TADF emitter based on inexpensive tungsten metal chelated with Schiff base ligand that exhibit high emission quantum yields of up to 56 % in solutions and 84 % in thin-film (5 wt % in 1,3-bis(N-carbazolyl)benzene, mCP) at room temperature. Femtosecond time-resolved emission (fs-TRE) spectroscopy and DFT calculations were undertaken to decipher the TADF properties.
View Article and Find Full Text PDFA panel of iridium(iii) porphyrin complexes containing axial N-heterocyclic carbene (NHC) ligand(s) were synthesized and characterized. X-ray crystal structures of the bis-NHC complexes [Ir(ttp)(IMe)] (), [Ir(oep)(BIMe)] (), [Ir(oep)(I Pr)] () and [Ir(Ftpp)(IMe)] () display ruffled porphyrin rings with mesocarbon displacements of 0.483-0.
View Article and Find Full Text PDFThe development of novel luminescent iridium(III) complexes with highly tunable emission energy and versatile applications is of particular importance. In this Communication, a series of luminescent iridium(III) complexes supported by chromophoric pyridinium-derived N-heterocyclic carbene (NHC) ligands that display tunable emission from 516 to 682 nm were prepared. These complexes can be used as photocatalysts in photooxidation and photoreduction reactions and could have potential applications in pH sensing.
View Article and Find Full Text PDFCopper(I) complexes of tris(thioimidazolyl)borates (R'Tm), including [Cu(Tm)(PR″)] (R″ = Ph, Cu1; Cy, Cu2) and [Cu(R'Tm)(PR″)] (R' = N-methylimidazole; R″ = Ph, Cy) were prepared and characterized by spectroscopic methods. The X-ray crystal structures of Cu1 and Cu2 feature a tripodal Tm ligand coordinated in κ-S,S,S mode. Using Cu2 as a catalyst (loading: 1 mol %), the aziridination of styrenes and sulfimidation of thioanisoles with PhI═NTs at RT for 3 and 0.
View Article and Find Full Text PDFA new class of cyclometalated Ir(iii) complexes supported by various bidentate C-deprotonated (C^N) and -chelating bis(N-heterocyclic carbene) (bis-NHC) ligands has been synthesized. These complexes display strong emission in deaerated solutions at room temperature with photoluminescence quantum yields up to 89% and emission lifetimes up to 96 μs. A photo-stable complex containing C-deprotonated fluorenyl-substituted C^N shows no significant decomposition even upon irradiation for over 120 h by blue LEDs (12 W).
View Article and Find Full Text PDFWe report herein the synthesis and application of a novel tetradentate ruthenium(II) complex 1 containing a tris(2-pyridylmethyl)amine (tpa) ligand as an inhibitor of β-amyloid fibrillogenesis. [Ru(tpa)(bt)]ClO(4) 1 (bt =2-acetylbenzo[b]thiophene-3-olate) showed significant inhibition of Aβ(1-40) peptide aggregation in vitro, which was confirmed by a Thioflavin T assay and transmission electron microscopy imaging.
View Article and Find Full Text PDFVisible-light driven CO2 reduction is considered to be a sustainable energy source. However, earth-abundant molecular catalysts with high efficiency and robustness towards solar-driven CO2 reduction are limited. Herein, we report a cobalt complex supported by a tetradentate tripodal ligand, which demonstrates catalytic solar-driven CO2 reduction with TON(CO) > 900 over 70 h in the presence of a photosensitizer.
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