43 research outputs found

    Polymer-Induced Emission-Active Fluorine-Embedded Carbon Dots for the Preparation of Warm WLEDs with a High Color Rendering Index

    No full text
    Exploration of many strategies has continuously contributed to producing aggregation-induced red-emissive carbon dots (CDs). In this work, we designed fluorine-embedded (F-embedded) CDs from 1,2,4-triaminobenzene, thiourea, and ammonium fluoride (NH4F) exhibiting polymer-induced emission (PIE). The PIE phenomenon of fluorescent CDs is obtained in poly­(vinyl alcohol) (PVA), showing emissions at 611 and 617 nm in the dispersed and solid states, respectively. The CDs exhibited a red shift of 28 nm in the PVA solution because PVA hydroxyl groups formed a robust bridge-like H-bonding network between CDs. The fluorine embedded in CDs enhanced the H-bond affinity toward PVA. It showed that this H-bond restricted the coupling of CDs’ surface states and inhibited the nonirradiation transfer. For the solid state, surface PVA chains eliminated the π–π interaction of the conjugated core and constructed a self-quenching resistance polymeric system around CDs. As a result, CDs showed an unexpected red shift of fluorescence emission in PVA. Furthermore, white light-emitting diodes (WLEDs) have a correlated color temperature (CCT) of 5232 K, and a high color rendering index of 95 has been fabricated by integrating the red- and green-emissive films over the UV LEDs. Interestingly, the as-synthesized CDs showed room temperature phosphorescence (RTP), which enabled us to employ the CDs in double-security protection. Simultaneously, CDs have been used in fingerprint detection

    Polymer-Induced Emission-Active Fluorine-Embedded Carbon Dots for the Preparation of Warm WLEDs with a High Color Rendering Index

    No full text
    Exploration of many strategies has continuously contributed to producing aggregation-induced red-emissive carbon dots (CDs). In this work, we designed fluorine-embedded (F-embedded) CDs from 1,2,4-triaminobenzene, thiourea, and ammonium fluoride (NH4F) exhibiting polymer-induced emission (PIE). The PIE phenomenon of fluorescent CDs is obtained in poly­(vinyl alcohol) (PVA), showing emissions at 611 and 617 nm in the dispersed and solid states, respectively. The CDs exhibited a red shift of 28 nm in the PVA solution because PVA hydroxyl groups formed a robust bridge-like H-bonding network between CDs. The fluorine embedded in CDs enhanced the H-bond affinity toward PVA. It showed that this H-bond restricted the coupling of CDs’ surface states and inhibited the nonirradiation transfer. For the solid state, surface PVA chains eliminated the π–π interaction of the conjugated core and constructed a self-quenching resistance polymeric system around CDs. As a result, CDs showed an unexpected red shift of fluorescence emission in PVA. Furthermore, white light-emitting diodes (WLEDs) have a correlated color temperature (CCT) of 5232 K, and a high color rendering index of 95 has been fabricated by integrating the red- and green-emissive films over the UV LEDs. Interestingly, the as-synthesized CDs showed room temperature phosphorescence (RTP), which enabled us to employ the CDs in double-security protection. Simultaneously, CDs have been used in fingerprint detection

    Polymer-Induced Emission-Active Fluorine-Embedded Carbon Dots for the Preparation of Warm WLEDs with a High Color Rendering Index

    No full text
    Exploration of many strategies has continuously contributed to producing aggregation-induced red-emissive carbon dots (CDs). In this work, we designed fluorine-embedded (F-embedded) CDs from 1,2,4-triaminobenzene, thiourea, and ammonium fluoride (NH4F) exhibiting polymer-induced emission (PIE). The PIE phenomenon of fluorescent CDs is obtained in poly­(vinyl alcohol) (PVA), showing emissions at 611 and 617 nm in the dispersed and solid states, respectively. The CDs exhibited a red shift of 28 nm in the PVA solution because PVA hydroxyl groups formed a robust bridge-like H-bonding network between CDs. The fluorine embedded in CDs enhanced the H-bond affinity toward PVA. It showed that this H-bond restricted the coupling of CDs’ surface states and inhibited the nonirradiation transfer. For the solid state, surface PVA chains eliminated the π–π interaction of the conjugated core and constructed a self-quenching resistance polymeric system around CDs. As a result, CDs showed an unexpected red shift of fluorescence emission in PVA. Furthermore, white light-emitting diodes (WLEDs) have a correlated color temperature (CCT) of 5232 K, and a high color rendering index of 95 has been fabricated by integrating the red- and green-emissive films over the UV LEDs. Interestingly, the as-synthesized CDs showed room temperature phosphorescence (RTP), which enabled us to employ the CDs in double-security protection. Simultaneously, CDs have been used in fingerprint detection

    La<sub>1–<i>x</i></sub>K<i><sub>x</sub></i>FeO<sub>3−δ</sub>: An Anion Intercalative Pseudocapacitive Electrode for Supercapacitor Application

    No full text
    The green energy alternative to a fossil fuel-based economy can be provided only by coupling renewable energy solution solutions such as solar or wind energy plants with large-scale electrochemical energy storage devices. Enabling high-energy storage coupled with high-power delivery can be envisaged though high-capacitive pseudocapacitor electrodes. A pseudocapacitor electrode with multiple oxidation state accessibility can enable more than 1e– charge/transfer per molecule to facilitate superior energy storage. K-doped LaFeO3 (La1–xKxFeO3−δ) is presented here as an electrode having a high pseudocapacitance storage, equivalent to 1.32e– charge/transfer per molecule, resulting in a capacity equivalent of 662 F/g at 1 mV/s scan rate by introduction of a layered potential over the Fe-ion octahedral to utilize higher redox state energies (Fe4+→ Fe2+). La/K ordering in orthorhombic perovskite (La1–xKxFeO3−δ) made the Fe4+ oxidation state accessible, and a systematic shift in the redox energies of Fe4+/3+ and Fe3+/2+ redox couples was observed with K+ ion doping in the A site of the LaFeO3 perovskite, which resulted in a high faradic contribution to the capacitance, coupled with anionic intercalation of H2O/OH– in the host perovskite lattice. The surface capacitive and diffusion control contributions for capacitance are about 42 and 58%, respectively, at −0.6 V, with a scan rate of 1  mV/s. A high gravimetric capacitance, equivalent to 619, 347, 188, 121, and 65 F/g, respectively, at 1, 2, 3, 5, and 10 A/g constant current, was observed for the La0.5K0.5FeO3−δ electrode. Up to 88.9% capacitive retention and 97% Coulombic efficacy were obtained for continuous 5000 cycles of charge/discharge for the La0.5K0.5FeO3−δ electrode. The gravimetric capacitance values of ASCs (activated carbon//La0.5K0.5FeO3−δ) are 348, 290, 228, and 147 F/g at current densities of 1, 2, 3, and 5 A/g, respectively. A maximum specific power of ∼3594 W/kg was obtained when the specific energy reached ∼117 Wh/kg at 5 A/g of current density

    Methylene Thiazolidinediones as Alkylation Reagents in Catalytic C–H Functionalization: Rapid Access to Glitazones

    No full text
    The straightforward and rapid incorporation of a thiazolidinedione scaffold into prefunctionalized (hetero)aromatic compounds is in demand for the development of antidiabetic glitazones and other pharmaceuticals. Herein, we report the unprecedented N- and O-directed C–H alkylation of various (hetero)arenes with methylene thiazolidinediones under rhodium(III) catalysis. The applicability of the developed protocol in challenging contexts is exhibited by the late-stage installation of a methylene thiazolidinedione moiety on the C–H bond of commercially available drug molecules. Combined mechanistic investigations aided the elucidation of a plausible reaction mechanism

    Methylene Thiazolidinediones as Alkylation Reagents in Catalytic C–H Functionalization: Rapid Access to Glitazones

    No full text
    The straightforward and rapid incorporation of a thiazolidinedione scaffold into prefunctionalized (hetero)aromatic compounds is in demand for the development of antidiabetic glitazones and other pharmaceuticals. Herein, we report the unprecedented N- and O-directed C–H alkylation of various (hetero)arenes with methylene thiazolidinediones under rhodium(III) catalysis. The applicability of the developed protocol in challenging contexts is exhibited by the late-stage installation of a methylene thiazolidinedione moiety on the C–H bond of commercially available drug molecules. Combined mechanistic investigations aided the elucidation of a plausible reaction mechanism

    Methylene Thiazolidinediones as Alkylation Reagents in Catalytic C–H Functionalization: Rapid Access to Glitazones

    No full text
    The straightforward and rapid incorporation of a thiazolidinedione scaffold into prefunctionalized (hetero)aromatic compounds is in demand for the development of antidiabetic glitazones and other pharmaceuticals. Herein, we report the unprecedented N- and O-directed C–H alkylation of various (hetero)arenes with methylene thiazolidinediones under rhodium(III) catalysis. The applicability of the developed protocol in challenging contexts is exhibited by the late-stage installation of a methylene thiazolidinedione moiety on the C–H bond of commercially available drug molecules. Combined mechanistic investigations aided the elucidation of a plausible reaction mechanism

    Transition-Metal-Free Alkylation and Acylation of Benzoxazinones with 1,4-Dihydropyridines

    No full text
    The direct functionalization of N-heterocycles is a vital transformation for the development of pharmaceuticals, functional materials, and other chemical entities. Herein, the transition-metal-free alkylation and acylation of C­(sp2)–H bonds in biologically relevant 2-benzoxazinones with 1,4-dihydropyridines as readily accessible radical surrogates is described. Excellent functional group compatibility and a broad substrate scope were attained. Gram-scale reaction and transformations of the synthesized adducts via Suzuki coupling with heteroaryl boronic acids demonstrated the synthetic potential of the developed protocol

    Cobalt(II)-Catalyzed C–H Alkylation of <i>N</i>‑Heterocycles with 1,4-Dihydropyridines

    No full text
    The rapid incorporation of alkyl and acyl groups into C–H bonds of N-heterocycles is in demand for the development of lead candidates in drug discovery. Herein, we report the cobalt(II)-catalyzed C–H alkylation and acylation of N-heterocycles with 1,4-dihydropyridines (DHPs) as alkylating and acylating agents. Notably, a combination of KBrO3 and a Co(II) catalyst was successfully employed for the generation of alkyl and acyl radicals from DHPs. A series of heterocycles, including azauracils, quinoxalinones, pyrazinones, pyridones, quinolones, quinazolinones, xanthines, chromones, and azine N-oxides, were compatible under the developed conditions. The applicability of the developed protocol in challenging contexts is highlighted by the selective modification of drug candidates as well as the gram-scale synthesis of bioactive molecules. Combined mechanistic investigations aided the elucidation of a plausible reaction mechanism

    Ruthenium(II)-Catalyzed Tandem C–H Allylation and [3 + 2] Dipolar Cycloaddition to Construct Bridged Tetracycles

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    The ruthenium­(II)-catalyzed tandem C–H allylation and intramolecular dipolar cycloaddition between azomethine imines and 2-methylidenetrimethylene carbonate is described herein. The initially formed β-substituted allyl fragment could trigger the exotype [3 + 2] cycloaddition with the polar azomethine group, resulting in the formation of bridged tetracycles bearing a hydroxymethylene group at a bridgehead carbon center. A wide substrate scope and broad functional group compatibility were observed. The gram-scale synthesis and synthetic transformations demonstrate the synthetic utility of this process
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