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