RESUMO
For Tb3+-doped green phosphors, the energy transfer from Ce3+ to Tb3+ can largely enhance the absorption of excitation; however, obtaining phosphors that exhibit both high quantum efficiency and thermal stability continues to pose a significant challenge. Herein, we established a paradigm to achieve novel silicate BaY4Si5O17 (BYSO):Ce3+,Tb3+. The near-ultraviolet light efficiently excites the BYSO:Ce3+ material, causing it to emit light at a wavelength of 408 nm. The photoluminescence of BYSO:0.12Ce3+ exhibits a relatively small Stokes shift and a thermal stability of 89.8% of the 303 K emission intensity at 423 K (89.8%@423 K). The energy transfer (ET) from Ce3+ to Tb3+ ions can be readily constructed in BYSO:Ce3+,Tb3+ utilizing the overlap between the Ce3+ emission and the Tb3+ excitation. The ET efficiency from the Ce3+ to Tb3+ ions reached 83.8% at y = 1.2 and a maximum of 94.6%. Finally, the optimized phosphor BYSO:0.12Ce3+,1.2Tb3+ had an internal quantum efficiency of 94.4% and had excellent thermal stability (96.1%@423 K). Our work pointed out the avenue to novel green phosphors with high efficiency and thermal stability by choosing appropriate host and construct efficient ET.
RESUMO
In an increasing manner, near-infrared phosphor-converted light-emitting diodes (NIR pc-LEDs) are considered to be exemplary light sources owing to their notable attributes of elevated output power, economical nature, and exceptional portability. NIR phosphors are critical components of NIR pc-LEDs. Herein, we report a novel blue light excitable NIR phosphor CaLu2ZrScAl3O12:Cr3+ (CLZSA:Cr3+) as a crucial and efficient broadband NIR emitter. The CLZSA:Cr3+ phosphor displays an intense NIR broadband emission peaking at 776 nm and with a full width at half-maximum (fwhm) of 140 nm. The designed material also exhibits superior resistance to thermal quenching, as the intensity of emission at 423 K remains at 80% of that at room temperature. The constructed NIR pc-LED device based on CLZSA:Cr3+ demonstrates a high total output power of 68.4 mW at a drive current of 100 mA, along with a high photoelectric conversion efficiency of 23.0%. Impressively, the high-power NIR pc-LEDs are utilized as light sources for remote control and non-invasive detection, resulting in the excellent performance and remarkable achievement.
RESUMO
The cation-equivalent substitution strategy has the ability to manipulate the luminescence color of phosphors and enhance their overall luminescence performance. A series of novel yellow feldspar-type 3D layered phosphors (Ca1-ySry)4MgAl2Si3O14:xEu2+ were synthesized using a high-temperature solid-state reaction. The solid solution phosphors belong to a tetragonal crystal system with a space group of P4Ì 21m and cell parameters of a = b = 7.75407-7.91794 Å, c = 5.04299-5.22543 Å, and V = 303.166-327.602 Å3. Under near-ultraviolet (n-UV) excitation, the luminescence color of the phosphor undergoes modulation from yellow-green (530 nm) to blue (467 nm) as the Sr2+ ion substitution ratio increases. This modulation is attributed to the gradual decrease in crystal field splitting energy. Additionally, both the Stokes shift and the full width of the luminescence spectra decrease. Furthermore, there is an increase in the quantum yield (QY) from 45.50 to 60.73%. Finally, the fabricated white-light-emitting diode devices emitted warm white light and achieved high Ra (Ra = 94, 96.6, 92.7) and low correlated color temperature (CCT = 3486, 3430, 3788 K), indicating that the prepared solid solution phosphors can be used as candidate materials for WLED lighting.
RESUMO
Ornithine aminotransferase (OAT) is overexpressed in hepatocellular carcinoma (HCC), and we previously showed that inactivation of OAT inhibits the growth of HCC. Recently, we found that (3S,4S)-3-amino-4-fluorocyclopentenecarboxylic acid (5) was a potent inactivator of γ-aminobutyric acid aminotransferase (GABA-AT), proceeding by an enamine mechanism. Here we describe our investigations into the activity and mechanism of 5 as an inactivator of human OAT. We have found that 5 exhibits 10-fold less inactivation efficiency (kinact/KI) against hOAT than GABA-AT. A comprehensive mechanistic study was carried out to understand its inactivation mechanism with hOAT. pKa and electrostatic potential calculations were performed to further support the notion that the α,ß-unsaturated alkene of 5 is critical for enhancing acidity and nucleophilicity of the corresponding intermediates and ultimately responsible for the improved inactivation efficiency of 5 over the corresponding saturated analogue (4). Intact protein mass spectrometry and the crystal structure complex with hOAT provide evidence to conclude that 5 mainly inactivates hOAT through noncovalent interactions, and that, unlike with GABA-AT, covalent binding with hOAT is a minor component of the total inhibition which is unique relative to other monofluoro-substituted derivatives. Furthermore, based on the results of transient-state measurements and free energy calculations, it is suggested that the α,ß-unsaturated carboxylate group of PLP-bound 5 may be directly involved in the inactivation cascade by forming an enolate intermediate. Overall, compound 5 exhibits unusual structural conversions which are catalyzed by specific residues within hOAT, ultimately leading to an enamine mechanism-based inactivation of hOAT through noncovalent interactions and covalent modification.
Assuntos
Carcinoma Hepatocelular , Neoplasias Hepáticas , Humanos , Aminoácidos/farmacologia , Inibidores Enzimáticos/farmacologia , Ornitina-Oxo-Ácido Transaminase/química , Ornitina-Oxo-Ácido Transaminase/metabolismo , Ácido gama-Aminobutírico , Ácidos Carboxílicos/farmacologia , Ácidos Carboxílicos/química , OrnitinaRESUMO
Non-rare earth doped oxide phosphors with far-red emission have become one of the hot spots of current research due to their low price and excellent physicochemical stability as the red component in white light-emitting diodes (W-LEDs) and plant growth. Herein, we report novel Mn4+-doped La2CaSnO6 and La2MgSnO6 phosphors by high-temperature solid-phase synthesis and analyzed their crystal structures by XRD and Rietveld refinement. Their excitation spectra consist of two distinct excitation bands with the dominant excitation range from 250 to 450 nm, indicating that they possess strong absorption of near-ultraviolet light. Their emission is located around 693 and 708 nm, respectively, and can be absorbed by the photosensitive pigments Pr and Pfr, proving their great potential for plant growth. Finally, the prepared samples were coated with 365 nm UV chips to fabricate far-red LEDs and W-LEDs with low correlation color temperature (CCT = 4958 K/5275 K) and high color rendering index (Ra = 96.4/96.6). Our results indicate that La2CaSnO6:Mn4+ and La2MgSnO6:Mn4+ red phosphors could be used as candidate materials for W-LED lighting and plant growth.
Assuntos
Compostos de Cálcio , Raios Ultravioleta , Óxidos/química , LuzRESUMO
The inhibition of human ornithine δ-aminotransferase (hOAT) is a potential therapeutic approach to treat hepatocellular carcinoma. In this work, (S)-3-amino-4,4-difluorocyclopent-1-enecarboxylic acid (SS-1-148, 6) was identified as a potent mechanism-based inactivator of hOAT while showing excellent selectivity over other related aminotransferases (e.g., GABA-AT). An integrated mechanistic study was performed to investigate the turnover and inactivation mechanisms of 6. A monofluorinated ketone (M10) was identified as the primary metabolite of 6 in hOAT. By soaking hOAT holoenzyme crystals with 6, a precursor to M10 was successfully captured. This gem-diamine intermediate, covalently bound to Lys292, observed for the first time in hOAT/ligand crystals, validates the turnover mechanism proposed for 6. Co-crystallization yielded hOAT in complex with 6 and revealed a novel noncovalent inactivation mechanism in hOAT. Native protein mass spectrometry was utilized for the first time in a study of an aminotransferase inactivator to validate the noncovalent interactions between the ligand and the enzyme; a covalently bonded complex was also identified as a minor form observed in the denaturing intact protein mass spectrum. Spectral and stopped-flow kinetic experiments supported a lysine-assisted E2 fluoride ion elimination, which has never been observed experimentally in other studies of related aminotransferase inactivators. This elimination generated the second external aldimine directly from the initial external aldimine, rather than the typical E1cB elimination mechanism, forming a quinonoid transient state between the two external aldimines. The use of native protein mass spectrometry, X-ray crystallography employing both soaking and co-crystallization methods, and stopped-flow kinetics allowed for the detailed elucidation of unusual turnover and inactivation pathways.
Assuntos
Ornitina-Oxo-Ácido Transaminase/metabolismo , Humanos , Estrutura Molecular , Ornitina-Oxo-Ácido Transaminase/químicaRESUMO
Human ornithine aminotransferase (hOAT), a pyridoxal 5'-phosphate-dependent enzyme, plays a critical role in the progression of hepatocellular carcinoma (HCC). Pharmacological selective inhibition of hOAT has been shown to be a potential therapeutic approach for HCC. Inspired by the discovery of the nonselective aminotransferase inactivator (1R,3S,4S)-3-amino-4-fluoro cyclopentane-1-carboxylic acid (1), in this work, we rationally designed, synthesized, and evaluated a novel series of fluorine-substituted cyclohexene analogues, thereby identifying 8 and 9 as novel selective hOAT time-dependent inhibitors. Intact protein mass spectrometry and protein crystallography demonstrated 8 and 9 as covalent inhibitors of hOAT, which exhibit two distinct inactivation mechanisms resulting from the difference of a single fluorine atom. Interestingly, they share a similar turnover mechanism, according to the mass spectrometry-based analysis of metabolites and fluoride ion release experiments. Molecular dynamics (MD) simulations and electrostatic potential (ESP) charge calculations were conducted, which elucidated the significant influence of the one-fluorine difference on the corresponding intermediates, leading to two totally different inactivation pathways. The novel addition-aromatization inactivation mechanism for 9 contributes to its significantly enhanced potency, along with excellent selectivity over other aminotransferases.
Assuntos
Ácidos Cicloexanocarboxílicos/química , Cicloexilaminas/química , Inibidores Enzimáticos/química , Hidrocarbonetos Fluorados/química , Ornitina-Oxo-Ácido Transaminase/antagonistas & inibidores , Ácidos Cicloexanocarboxílicos/síntese química , Ácidos Cicloexanocarboxílicos/metabolismo , Cicloexilaminas/síntese química , Cicloexilaminas/metabolismo , Inibidores Enzimáticos/síntese química , Inibidores Enzimáticos/metabolismo , Humanos , Hidrocarbonetos Fluorados/síntese química , Hidrocarbonetos Fluorados/metabolismo , Modelos Químicos , Simulação de Acoplamento Molecular , Simulação de Dinâmica Molecular , Estrutura Molecular , Ornitina-Oxo-Ácido Transaminase/química , Ornitina-Oxo-Ácido Transaminase/metabolismo , Ligação Proteica , Fosfato de Piridoxal/química , Ácido gama-Aminobutírico/análogos & derivadosRESUMO
Recently, the development of multifunctional theranostic nanoplatforms to realize tumor-specific imaging and enhanced cancer therapy via responding or modulating the tumor microenvironment (TME) has attracted tremendous interests in the field of nanomedicine. Herein, tungsten disulfide (WS2 ) nanoflakes with their surface adsorbed with iron oxide nanoparticles (IONPs) via self-assembly are coated with silica and then subsequently with manganese dioxide (MnO2 ), on to which polyethylene glycol (PEG) is attached. The obtained WS2 -IO/S@MO-PEG appears to be highly sensitive to pH, enabling tumor pH-responsive magnetic resonance imaging with IONPs as the pH-inert T2 contrast probe and MnO2 as the pH-sensitive T1 contrast probe. Meanwhile, synergistic combination tumor therapy is realized with such WS2 -IO/S@MO-PEG, by utilizing the strong near-infrared light and X-ray absorbance of WS2 for photothermal therapy (PTT) and enhanced cancer radiotherapy (RT), respectively, as well as the ability of MnO2 to decompose tumor endogenous H2 O2 and relieve tumor hypoxia to further overcome hypoxia-associated radiotherapy resistance. The combination of PTT and RT with WS2 -IO/S@MO-PEG results in a remarkable synergistic effect to destruct tumors. This work highlights the promise of developing multifunction nanocomposites for TME-specific imaging and TME modulation, aiming at precision cancer synergistic treatment.
RESUMO
A novel series of N-aryl-N'-pyrimidin-4-yl ureas has been optimized to afford potent and selective inhibitors of the EGFR L858R/T790M. The most representative compound 28 showed high activity against EGFR L858R/T790M kinase (IC50â¯=â¯4â¯nM) and 22-fold selectivity against wild type EGFR. Moreover, compound 28 potently inhibited EGFR L858R/T790M phosphorylation (IC50â¯=â¯41â¯nM) and cellular proliferation (IC50â¯=â¯37â¯nM) in the H1975 cell line, while being significantly less toxic to A431 cells. Further, compound 28 exhibited a great selectivity in a mini-panel of kinases.
Assuntos
Antineoplásicos/farmacologia , Descoberta de Drogas , Inibidores de Proteínas Quinases/farmacologia , Ureia/farmacologia , Antineoplásicos/síntese química , Antineoplásicos/química , Linhagem Celular Tumoral , Proliferação de Células/efeitos dos fármacos , Relação Dose-Resposta a Droga , Ensaios de Seleção de Medicamentos Antitumorais , Receptores ErbB/antagonistas & inibidores , Receptores ErbB/genética , Receptores ErbB/metabolismo , Humanos , Simulação de Acoplamento Molecular , Estrutura Molecular , Mutação , Fosforilação/efeitos dos fármacos , Inibidores de Proteínas Quinases/síntese química , Inibidores de Proteínas Quinases/química , Relação Estrutura-Atividade , Ureia/análogos & derivados , Ureia/químicaRESUMO
Sodium-ion batteries are potential low-cost alternatives to current lithium-ion technology, yet their performances still fall short of expectation due to the lack of suitable electrode materials with large capacity, long-term cycling stability, and high-rate performance. In this work, we demonstrated that ultrasmall (â¼5 nm) iron selenide (FeSe2) nanoparticles exhibited a remarkable activity for sodium-ion storage. They were prepared from a high-temperature solution method with a narrow size distribution and high yield and could be readily redispersed in nonpolar organic solvents. In ether-based electrolyte, FeSe2 nanoparticles exhibited a large specific capacity of â¼500 mAh/g (close to the theoretical limit), high rate capability with â¼250 mAh/g retained at 10 A/g, and excellent cycling stability at both low and high current rates by virtue of their advantageous nanosizing effect. Full sodium-ion batteries were also constructed from coupling FeSe2 with NASICON-type Na3V2(PO4)3 cathode and demonstrated impressive capacity and cycle ability.
RESUMO
Multifunctional theranostic agents have become rather attractive to realize image-guided combination cancer therapy. Herein, we develop a novel method to synthesize Bi2Se3 nanosheets decorated with mono-dispersed FeSe2 nanoparticles (FeSe2/Bi2Se3) for tetra-modal image-guided combined photothermal & radiation tumor therapy. Interestingly, upon addition of Bi(NO3)3, pre-made FeSe2 nanoparticles via cation exchange would be gradually converted into Bi2Se3 nanosheets, on which remaining FeSe2 nanoparticles are decorated. The yielded FeSe2/Bi2Se3 composite-nanostructures were then modified with polyethylene glycol (PEG). Taking advantages of the high r2 relaxivity of FeSe2, the X-ray attenuation ability of Bi2Se3, the strong near-infrared (NIR) optical absorbance of the whole nanostructure, as well as the chelate-free radiolabeling of 64Cu on FeSe2/Bi2Se3-PEG, in vivo magnetic resonance (MR)/computer tomography (CT)/photoacoustic (PA)/position emission tomography (PET) multimodal imaging was carried out, revealing efficient tumor homing of FeSe2/Bi2Se3-PEG after intravenous injection. Utilizing the intrinsic physical properties of FeSe2/Bi2Se3-PEG, in vivo photothermal & radiation therapy to achieve synergistic tumor destruction was then realized, without causing obvious toxicity to the treated animals. Our work presents a unique method to synthesize composite-nanostructures with highly integrated functionalities, promising not only for nano-biomedicine, but also potentially for other different nanotechnology fields.
RESUMO
While position emission tomography (PET) is an important molecular imaging technique for both preclinical research and clinical disease diagnosis/prognosis, chelator-free radiolabeling has emerged as a promising alternative approach to label biomolecules or nanoprobes in a facile way. Herein, starting from bottom-up synthesized WS2 nanoflakes, this study fabricates a unique type of WS2 /WOx nanodots, which can function as inherent hard oxygen donor for stable radiolabeling with Zirconium-89 isotope (89 Zr). Upon simply mixing, 89 Zr can be anchored on the surface of polyethylene glycol (PEG) modified WS2 /WOx (WS2 /WOx -PEG) nanodots via a chelator-free method with surprisingly high labeling yield and great stability. A higher degree of oxidation in the WS2 /WOx -PEG sample (WS2 /WOx (0.4)) produces more electron pairs, which would be beneficial for chelator-free labeling of 89 Zr with higher yields, suggesting the importance of surface chemistry and particle composition to the efficiency of chelator-free radiolabeling. Such 89 Zr-WS2 /WOx (0.4)-PEG nanodots are found to be an excellent PET contrast agent for in vivo imaging of tumors upon intravenous administration, or mapping of draining lymph nodes after local injection.
Assuntos
Quelantes/química , Nanopartículas/química , Óxidos/química , Tomografia por Emissão de Pósitrons/métodos , Radioisótopos/química , Sulfetos/química , Zircônio/química , Animais , Linhagem Celular Tumoral , Feminino , Linfonodos/patologia , Camundongos Endogâmicos BALB C , Nanopartículas/ultraestruturaRESUMO
A series of AKBA derivatives were synthesized, and evaluated as potent VEGFR-2 inhibitors. The initial biological evaluation indicated that the introduction of C-24 amide group or a heterocycle at C-2,3 position effectively improved the potency. Further structure-activity relationship analysis showed that amide (7, 23, 25, and 26) and heterocycle (19, 34, and 36) substituted AKBA derivatives displayed more potential anti-proliferation activities than AKBA (1) on HUVECs that express high levels of VEGFR-2. Among all tested compounds, compounds 7 and 19 exhibited the best potency (IC50: 2.36 and 2.13 µM) and obvious inhibitory activities with VEGFR-2 inhibition rates of 96% and 94% at 50 µM, respectively.
Assuntos
Inibidores de Proteínas Quinases/farmacologia , Triterpenos/farmacologia , Receptor 2 de Fatores de Crescimento do Endotélio Vascular/antagonistas & inibidores , Proliferação de Células/efeitos dos fármacos , Relação Dose-Resposta a Droga , Células Endoteliais da Veia Umbilical Humana/efeitos dos fármacos , Humanos , Estrutura Molecular , Inibidores de Proteínas Quinases/síntese química , Inibidores de Proteínas Quinases/química , Relação Estrutura-Atividade , Triterpenos/síntese química , Triterpenos/química , Receptor 2 de Fatores de Crescimento do Endotélio Vascular/metabolismoRESUMO
The pursuit of high-quality phosphors exhibiting swift response to near-ultraviolet (n-UV) excitation, elevated quantum efficiency (QE), superior thermal stability, and impeccable light quality has been a focal point of investigation. In this research, we synthesized a novel K2La2B2O7:Ce3+,Tb3+ (KLBO:Ce3+,Tb3+) color-tunable phosphor that meets these requirements. KLBO:Ce3+ can be stimulated efficiently by the n-UV light and shows an intense blue emission centered at 437 nm. Notably, KLBO:0.04Ce3+ exhibits exceptional internal QE (IQE = 94%) and outstanding thermal stability (I423 K/I303 K = 88%). Optimization of doping compositions enables efficient Ce3+ â Tb3+ energy transfer, resulting in substantial enhancements in QE and thermal stability. Specifically, KLBO:0.04Ce3+,0.28Tb3+ achieves an IQE of 98% and a thermal stability of 97%, higher than those of most phosphors of the same type. White light-emitting diodes fabricated using phosphor samples emit warm white light characterized by high Ra (Ra = 96.6 and 93.4) and low CCT (CCT = 4886 and 4400 K). This study underscores the feasibility of enhancing phosphor QE and thermal stability through energy transfer mechanisms.
RESUMO
NIR luminescent materials have garnered widespread attention because of their exceptional properties, with high tissue penetration, low absorption and high signal-to-noise ratio in the field of optical imaging. However, producing nanophosphors with high quantum yields of emitting infrared light with wavelengths above 1000 nm remains a significant challenge. Here, we prepared a nanoscale ZnGa2O4:xCr3+,yNi2+ phosphor with good luminescence performance in near-infrared emission, which was synthesized via a hydrothermal method and subsequent calcination process. By co-doping with Cr3+ and Ni2+, the ZnGa2O4 phosphor shows a strong broadband emission of 1100-1600 nm in the second near-infrared (NIR-II) region, owing to the energy transfer from Cr3+ to Ni2+ with an efficiency up to 90%. Meanwhile, a near-infrared phosphor-conversion LED (NIR pc-LED) device is fabricated based on the ZnGa2O4:0.8%Cr3+,0.4%Ni2+ nanophosphor, which has under 100 mA input current, an output power of 23.99 mW, and a photoelectric conversion efficiency of 7.53%, and can be effectively applied in imaging and non-destructive testing. Additionally, the intensity ratio of INi/ICr of ZnGa2O4:0.8% Cr3+,0.4%Ni2+ with its high sensitivity value of 4.21% K-1 at 453 K under 410 nm excitation, indicates its potential for thermometry application.
RESUMO
Phosphors with intrinsic white light emission are of great potential in constructing high-quality white LEDs (WLEDs). In this work, we propose the use of energy transfer from Bi3+ to Eu3+ ions for white light emission. A unique Bi3+-activated phosphor LaGdO3 (LGO):Bi3+ was generated using the conventional high-temperature solid-state process. An energy transfer was established by introducing Eu3+ into the phosphor composition. The emission colour of LGO:Bi3+,Eu3+ phosphors changes from cyan to white to orange-red depending on the Bi3+/Eu3+ doping proportion. The energy transfer between the Bi3+ and Eu3+ ions results from the dipole-dipole interaction. The LGO:Bi3+,Eu3+ phosphors were combined with a near-ultraviolet chip to successfully create a single-component WLED device with a colour-rendering index of 92.4. Our work demonstrates the energy transfer as a route for single-component white light emission and makes LGO:Bi3+,Eu3+ phosphors one of the candidate materials for near-ultraviolet lighting.
RESUMO
A series of new arctigenin and 9-deoxy-arctigenin derivatives bearing different ester and ether side chains at the phenolic hydroxyl positions are designed, synthesized, and evaluated for activating AMPK potency in L6 myoblasts. Initial biological evaluation indicates that some alkyl ester and phenethyl ether arctigenin derivatives display potential activities in AMPK phosphorylation improvement. Further structure-activity relationship analysis shows that arctigenin ester derivatives 3a, 3h and 9-deoxy-arctigenin phenethyl ether derivatives 6a, 6c, 6d activate AMPK more potently than arctigenin. Moreover, the 2-(3,4-dimethoxyphenyl)ethyl ether moiety of 6c has been demonstrated as a potential functional group to improve the effect of AMPK phosphorylation. The structural optimization of arctigenin leads to the identification of 6c as a promising lead compound that exhibits excellent activity in AMPK activation.
Assuntos
Proteínas Quinases Ativadas por AMP/antagonistas & inibidores , Furanos/química , Furanos/farmacologia , Lignanas/química , Lignanas/farmacologia , Mioblastos/efeitos dos fármacos , Mioblastos/enzimologia , Proteínas Quinases Ativadas por AMP/metabolismo , Animais , Linhagem Celular , Ésteres , Furanos/síntese química , Lignanas/síntese química , Fosforilação/efeitos dos fármacos , Relação Estrutura-AtividadeRESUMO
In this work, a series of BaSrGd4O8:xBi3+ blue phosphors was synthesized employing the high-temperature solid-state method. Phase purity of the samples was verified by X-ray diffraction and Rietveld refinement. Time-resolved photoluminescence spectra revealed the existence of two distinct Bi sites. Subsequent optimization of dopant types and doping levels in the batch led to an almost twofold increase in quantum efficiency. The introduction of Eu3+ into the phosphors facilitated the construction of an energy transfer pathway. As the concentration of Eu3+ was increased, the emission color changed from blue to purple and finally to red. In addition, the thermal stability and potential applications of the phosphors were extensively investigated. Finally, two WLED devices were successfully fabricated with color rendering indices of 96.27 and 92.18, and correlated color temperatures of 5198 and 2475 K. This underscores the prospective application of these phosphors in the field of high-quality warm WLEDs.
RESUMO
Most commercial phosphor-converted white light-emitting diodes (pc-WLEDs) are manufactured with blue LED chips and yellow-emitting Y3Al5O12:Ce3+ (YAG:Ce3+) garnet phosphor, but the lack of blue-green light in the spectrum results in a low color rendering index (CRI). In this paper, we synthesized Y3ScAl4O12:Ce3+ (YSAG:Ce3+) by replacing Al3+ in YAG:Ce3+ with Sc3+. The introduction of Sc3+ with a larger ionic radius through a cation substitution strategy causes lattice expansion, elongation of the Y-O bond, and ultimately a decrease in Ce3+ 5d level crystal field splitting. As a consequence, the emission spectrum undergoes a blue-shift of 10 nm. Furthermore, the YSAG:Ce3+ phosphor exhibits good thermal stability, and its emission intensity at 423 K is about 58% of that at 303 K. Moreover, the analysis of Eu3+ emission spectra demonstrates that the introduction of Sc3+ resulted in a slight reduction of the dodecahedral lattice symmetry. YSAG:Ce3+ effectively compensates for the lack of the blue-green region, and WLEDs with high color rendering index (90.1), low color temperature (4566 K) and high luminous efficiency (133.59 lm W-1) were prepared using the combination of YSAG:0.08Ce3+, CaAlSiN3:Eu2+ and 450 nm blue chips. These findings indicate that YSAG:Ce3+ garnet phosphor has potential to be used in high quality WLEDs.
RESUMO
Na2MgScF7 (NMSF) was experimentally obtained for the first time by combining hydrothermal and high-temperature solid-state reactions. X-ray powder diffraction (XRD) combined with Rietveld refinement confirms that NMSF is crystallized in the space group Imma with the cell parameters a = 10.40860(18), b = 7.32804(12) and c = 7.52879(11) Å, α = ß = γ = 90° and V = 574.256(24) Å3. Through doping with Tb3+ or Eu3+ ions, downshifting yellow-green or red emission could be achieved in NMSF-based phosphors, respectively. Upconversion emission could also be designed by doping with Yb3+-Er3+, Yb3+-Tm3+, Yb3+-Ho3+ or Er3+. Moreover, the NMSF:Er3+ phosphor exhibited green upconversion emission upon excitation at 980 nm, and it exhibited red emission upon excitation at 1532 nm. Finally, recognizable patterns were obtained under excitation at 254, 365 and 980 nm, indicating that the as-prepared phosphors can be applied to multicolor anti-counterfeiting. Moreover, our synthesis strategy opens up new avenues for the synthesis of novel fluorides.