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1.
Adv Mater ; : e2406164, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38924614

RESUMO

The quest for artificial light sources mimicking sunlight has been a long-standing endeavor, particularly for applications in anticounterfeiting, agriculture, and color hue detection. Conventional sunlight simulators are often cost-prohibitive and bulky. Therefore, the development of a series of single-phase phosphors Ca9LiMg1-xAl2x/3(PO4)7:0.1Eu2+ (x = 0-0.75) with sunlight-like emission represents a welcome step towards compact and economical light source alternatives. The phosphors are obtained by an original heterovalent substitution method and emit a broad spectrum   spanning from violet to deep red. Notably, the phosphor with x = 0.5 exhibits an impressive full width at half-maximum of 330 nm. A synergistic interplay of experimental investigations and theory unveils the mechanism behind sunlight-like emission due to the local structural perturbations introduced by the heterovalent substitution of Al3+ for Mg2+, leading to a varied distribution of Eu2+ within the lattice. Subsequent characterization of a series of organic dyes combining absorption spectroscopy with convolutional neural network analysis convincingly demonstrates the potential of this phosphor in portable photodetection devices. Broad-spectrum light source testing empowers the model to precisely differentiate dye patterns. This points to the phosphor being ideal for mimicking sunlight. Beyond this demonstrated application, the phosphor's utility is envisioned in other relevant domains, including visible light communication and smart agriculture.

2.
Nat Commun ; 15(1): 3209, 2024 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-38615033

RESUMO

The manipulation of excitation modes and resultant emission colors in luminescent materials holds pivotal importance for encrypting information in anti-counterfeiting applications. Despite considerable achievements in multimodal and multicolor luminescent materials, existing options generally suffer from static monocolor emission under fixed external stimulation, rendering them vulnerability to replication. Achieving dynamic multimodal luminescence within a single material presents a promising yet challenging solution. Here, we report the development of a phosphor exhibiting dynamic multicolor photoluminescence (PL) and photo-thermo-mechanically responsive multimodal emissions through the incorporation of trace Mn2+ ions into a self-activated CaGa4O7 host. The resulting phosphor offers adjustable emission-color changing rates, controllable via re-excitation intervals and photoexcitation powers. Additionally, it demonstrates temperature-induced color reversal and anti-thermal-quenched emission, alongside reproducible elastic mechanoluminescence (ML) characterized by high mechanical durability. Theoretical calculations elucidate electron transfer pathways dominated by intrinsic interstitial defects and vacancies for dynamic multicolor emission. Mn2+ dopants serve a dual role in stabilizing nearby defects and introducing additional defect levels, enabling flexible multi-responsive luminescence. This developed phosphor facilitates evolutionary color/pattern displays in both temporal and spatial dimensions using readily available tools, offering significant promise for dynamic anticounterfeiting displays and multimode sensing applications.

3.
Phys Chem Chem Phys ; 25(42): 29303-29309, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37876211

RESUMO

Near-infrared (NIR) phosphors with high thermal stability are significant for NIR light-emitting diodes (LEDs). For a decade, Debye temperature has been a successful indicator of structural rigidity and thermal stability for phosphors, but some exceptions exist due to its dependence on atomic mass. Inspired by the Debye temperature model that relates the elastic properties of solids, our density functional theory calculations revealed that the Vickers hardness of Cr3+-doped NIR phosphors was negatively correlated with Stokes shifts (Pearson's R = -0.81) and positively correlated with thermal stabilities (Pearson's R = 0.85) within a set of 13 distinct material types. Highlighting the predictive power of Vickers hardness, two new NIR phosphors were investigated: KMg(PO3)3:Cr3+ showed low thermal stability, correlating with its lower Vickers hardness, in contrast to the high thermal stability and correspondingly higher Vickers hardness of La2MgSnO6:Cr3+. Vickers hardness can be used to screen potential hosts for Cr3+-doped NIR phosphors with high thermal stabilities, due to the advantages of the predictable feature by density functional theory calculation and low independence on atomic mass.

4.
Pestic Biochem Physiol ; 195: 105543, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37666614

RESUMO

The rapid evolution of pest resistance threatens the sustainable utilization of bioinsecticides such as abamectin, and so deciphering the molecular mechanisms affecting toxicity and resistance is essential for their long-term application. Historical studies of abamectin resistance in arthropods have mainly focused on mechanisms involving the glutamate-gated chloride channel (GluCl) targets, with the role of metabolic processes less clear. The two-spotted spider mite, Tetranychus urticae, is a generalist herbivore notorious for rapidly developing resistance to pesticides worldwide, and abamectin has been widely used for its control in the field. After reanalyzing previous transcriptome and RNA-seq data, we here identified an ABC transporter subfamily C gene in T. urticae named multidrug resistance-associated protein 1 (TuMRP1), whose expression differed between susceptible and resistant populations. Synergism bioassays with the inhibitor MK-571, the existence of a genetic association between TuMRP1 expression and susceptibility to abamectin, and the effect of RNA interference mediated silencing of TuMRP1 were all consistent with a direct role of this transporter protein in the toxicity of abamectin. Although ABC transporters are often involved in removing insecticidal compounds from cells, our data suggest either an alternative role for these proteins in the mechanism of action of abamectin or highlight an indirect association between their expression and abamectin toxicity.


Assuntos
Tetranychidae , Animais , Tetranychidae/genética , Proteínas Associadas à Resistência a Múltiplos Medicamentos , Ivermectina/toxicidade
5.
Nanomaterials (Basel) ; 13(13)2023 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-37446426

RESUMO

To develop novel luminescent materials for optical temperature measurement, a series of Yb3+- and Er3+-doped Ca3Sc2Si3O12 (CSS) upconversion (UC) phosphors were synthesized by the sol-gel combustion method. The crystal structure, phase purity, and element distribution of the samples were characterized by powder X-ray diffraction and a transmission electron microscope (TEM). The detailed study of the photoluminescence emission spectra of the samples shows that the addition of Yb3+ can greatly enhance the emission of Er3+ by effective energy transfer. The prepared Yb3+ and Er3+ co-doped CSS phosphors exhibit green emission bands near 522 and 555 nm and red emission bands near 658 nm, which correspond to the 2H11/2→4I15/2, 4S3/2→4I15/2, and 4F9/2→4I15/2 transitions of Er3+, respectively. The temperature-dependent behavior of the CSS:0.2Yb3+,0.02Er3+ sample was carefully studied by the fluorescence intensity ratio (FIR) technique. The results indicate the excellent sensitivity of the sample, with a maximum absolute sensitivity of 0.67% K-1 at 500 K and a relative sensitivity of 1.34% K-1 at 300 K. We demonstrate here that the temperature measurement performance of FIR technology using the CSS:Yb3+,Er3+ phosphor is not inferior to that of infrared thermal imaging thermometers. Therefore, CSS:Yb3+,Er3+ phosphors have great potential applications in the field of optical thermometry.

6.
Neuroreport ; 34(13): 655-663, 2023 09 06.
Artigo em Inglês | MEDLINE | ID: mdl-37506317

RESUMO

This study was designed to see the expression of toll-like receptor 4 (TLR4) and downstream molecules including myeloid differentiation factor 88 (MyD88) and interleukin 1-ß (IL-1ß) in the spinal cord as peripheral nerve injury recovered in mice. We established a model of femoral nerve injury (FNI) in C57BL/6 mice by transection of the motor branch of the femoral nerve, followed by retrograde labeling to show the according motor neurons in the anterior horn of the spinal cord pars lumbar. We observed the motor function recovery of the injured hind limbs using behavioral tests. The expression of TLR4, MyD88, and IL-1ß was examined by immunofluorescent staining and western blot. According to the behavior test, the FNI animals fully recovered within 6-8 weeks. TLR4, MyD88, and IL-1ß were expressed in the ventral horn of the spinal cord both at 72 h till 6 weeks after the femoral nerve transection surgery, and these proteins were mostly co-localized with neurons. IL-1ß also tended to rise in the same surgery groups, but more intimate with microglia surrounding nearby retrograde labeled neurons. And western blot results were consistent with histological findings. The results indicate that peripheral nerve injury may induce innate immune reactions of the central neurons and critical signaling like TLR4/MyD88 in the spinal cord may reflect the recovery of the injury. These findings suggest that peripheral nerve injury triggered the TLR4/MyD88 signal in the soma of spinal neurons may be involved in function and nerve restoration through neuron-glia crosstalk.


Assuntos
Fator 88 de Diferenciação Mieloide , Traumatismos dos Nervos Periféricos , Camundongos , Animais , Fator 88 de Diferenciação Mieloide/metabolismo , Receptor 4 Toll-Like/metabolismo , Nervo Femoral/metabolismo , Camundongos Endogâmicos C57BL , Neurônios Motores/metabolismo
7.
Adv Mater ; 35(42): e2302771, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37278254

RESUMO

Increasing sulfur mass loading and minimizing electrolyte amount remains a major challenge for the development of high-energy-density Li-S batteries, which needs to be tackled with combined efforts of materials development and mechanistic analysis. This work, following the same team's most recent identification of the potential-limiting step of Li-S batteries under lean electrolyte conditions, seeks to advance the understanding by extending it to a new catalyst and into the high-sulfur-mass-loading region. CeOx nanostructures are integrated into cotton-derived carbon to develop a multifunctional 3D network that can host a large amount of active material, facilitate electron transport, and catalyze the sulfur lithiation reaction. The resulting S/CeOx /C electrode can deliver a stable areal capacity of 9 mAh cm-2 with a high sulfur loading of 14 mg cm-2 at a low electrolyte/sulfur ratio of 5 µL mg-1 . This study discovers that Li||S/CeOx /C cells usually fail during charging at high current density, as a consequence of local short circuiting caused by electrochemically deposited Li dendrites penetrating through the separator, a previously overlooked failure pattern distinctive to cells operating under lean electrolyte conditions. This work highlights the importance of developing new material structures and analyzing failure mechanisms in the advancement of Li-S batteries.

8.
Angew Chem Int Ed Engl ; 62(35): e202307868, 2023 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-37366547

RESUMO

Orange Eu2+ -doped phosphors are essential for light-emitting diodes for cornering lights to prevent fatal road accidents at night, but such phosphors require features of high thermal, chemical stability and facile synthesis. This study reports a series of yellow-orange-red emitting SrAl2 Si3 ON6 :Eu2+ oxynitride phosphors, derived from the SrAlSi4 N7 nitride iso-structure by replacing Si4+ -N3- with Al3+ -O2- . The introduction of a certain amount of oxygen enabled the facile synthesis under atmospheric pressure using the air-stable raw materials SrCO3 , Eu2 O3 , AlN and Si3 N4 . SrAl2 Si3 ON6 has a smaller band gap and lower structure rigidity than SrAlSi4 N7 (5.19 eV vs 5.50 eV, Debye temperature 719 K vs 760 K), but exhibits higher thermal stability with 100 % of room temperature intensity remaining at 150 °C compared to 85 % for SrAlSi4 N7 . Electron paramagnetic resonance, thermoluminescence and density functional theory revealed that the oxygen vacancy electron traps compensated the thermal loss. Additionally, no decrease in emission intensity was found after either being heated at 500 °C for 2 hours or being immersed in water for 20 days, implying both of the thermal and chemical stability of SrAl2 Si3 ON6 :Eu2+ phosphors. The strategy of oxynitride-introduction from nitride promotes the development of low-cost thermally and chemically stable luminescent materials.

9.
Small ; 19(26): e2207919, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36938911

RESUMO

Constructing active heterointerfaces is powerful to enhance the electrochemical performances of transition metal dichalcogenides, but the interface density regulation remains a huge challenge. Herein, MoO2 /MoS2 heterogeneous nanorods are encapsulated in nitrogen and sulfur co-doped carbon matrix (MoO2 /MoS2 @NSC) by controllable sulfidation. MoO2 and MoS2 are coupled intimately at atomic level, forming the MoO2 /MoS2 heterointerfaces with different distribution density. Strong electronic interactions are triggered at these MoO2 /MoS2 heterointerfaces for enhancing electron transfer. In alkaline media, the optimal material exhibits outstanding hydrogen evolution reaction (HER) performances that significantly surpass carbon-covered MoS2 nanorods counterpart (η10 : 156 mV vs 232 mV) and most of the MoS2 -based heterostructures reported recently. First-principles calculation deciphers that MoO2 /MoS2 heterointerfaces greatly promote water dissociation and hydrogen atom adsorption via the O-Mo-S electronic bridges during HER process. Moreover, benefited from the high pseudocapacitance contribution, abundant "ion reservoir"-like channels, and low Na+ diffusion barrier appended by high-density MoO2 /MoS2 heterointerfaces, the material delivers high specific capacity of 888 mAh g-1 , remarkable rate capability and cycling stability of 390 cycles at 0.1 A g-1 as the anode of sodium ion battery. This work will undoubtedly light the way of interface density engineering for high-performance electrochemical energy conversion and storage systems.

10.
Dalton Trans ; 52(15): 4808-4818, 2023 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-36939174

RESUMO

A Sm3+-doped YGa1.5Al1.5(BO3)4 (abbreviated as YGAB) phosphor was synthesized via a solid-state reaction with mechanical activation assistance in a high-energy density stirred bead mill. The samples were characterized by laser particle size analysis, specific surface area analysis, powder X-ray diffraction (XRD), scanning electron microscopy (SEM), differential scanning calorimetry (DSC), and fluorescence spectroscopy. In addition, the photoluminescence characteristics, luminescence decay, thermal stability, and LED application of the phosphors were also investigated. The results show that the mechanical activation of mixed raw materials before calcination can reduce the particle size and the activation energy of crystallization, resulting in the formation of the YGAB crystal phase at a lower calcination temperature. The mechanical activation in grinding can accelerate the subsequent solid-phase reaction, make Sm3+ ions more easily diffuse into the YGAB lattice, and improve the crystal structure of the synthesized phosphor, thus enhancing the optical properties of the phosphor. According to the photoluminescence emission (PL) and excitation (PLE) spectra, Sm3+ doped in the YGAB lattice can provide an efficient emission under 405 nm excitation. The optimum doping concentration of Sm3+ ions is 0.03 mol%. The optimum photoluminescence intensity, quantum yield, and fluorescence lifetime of the phosphor synthesized from mixed raw materials ground for 45 min can be obtained. The temperature-dependent PL spectra show that the emission intensity of the YGAB:0.03Sm3+ phosphor at 425 K is 84.7% of its initial intensity at room temperature. It is indicated that the YGAB:0.03Sm3+ phosphor synthesized could be used as one of the promising LED lighting materials.

11.
RSC Adv ; 12(45): 29338-29345, 2022 Oct 11.
Artigo em Inglês | MEDLINE | ID: mdl-36329764

RESUMO

Concentration quenching, which generally originates from serious energy migrations among the uniformly distributed luminescent centers in the host matrix, is a key factor to influence the luminescence properties of materials. Different from previous reports, we demonstrate a novel fluorescence-quenching mechanism attributable to the second-phase Eu2W2O9 in non-equivalent substituted SrWO4:xEu3+ phosphors. The crystal structure, elemental distribution, and luminescence properties of the as-prepared SrWO4:xEu3+ phosphors are systematically investigated. A second-phase Eu2W2O9 is confirmed when the Eu3+-doping concentration exceeds 20%, which produces the new structure defects and energy-transfer paths, resulting in fluorescence quenching in this material. This finding gives a new perspective to analyze the concentration-quenching mechanism of the non-equivalent substituted phosphors and can help in the design of new, efficient luminescence materials. In addition, the as-prepared SrWO4:xEu3+ phosphors exhibit a strong intrinsic excitation in the range of 355-425 nm, which is accompanied by the Commission Internationale de I'Eclairage (CIE) coordinates at (0.653, 0.347) and stable color purity of up to 94.52%. A packaged white light-emitting diode with CIE chromaticity coordinates of (0.398, 0.335), correlated color temperature of 3132 K, and color rendering index of 84.3 is fabricated by SrWO4:20%Eu3+ phosphors with blue BAM:Eu2+ and green YAGB:Tb3+ phosphors in a near-ultraviolet chip.

12.
Brain Behav ; 12(6): e2623, 2022 06.
Artigo em Inglês | MEDLINE | ID: mdl-35587519

RESUMO

BACKGROUND: Neuromyelitis optica spectrum disorder (NMOSD) is a central and acute demyelinating disease of the central nervous system with unusual clinical course. The development of novel biomarkers for NMOSD is critical for implementing effective clinical treatment. CD226 is known to be expressed on many types of peripheral lymphoid cells. However, the expression level and function of CD226 on type 1 T regulatory (Tr1) cells during NMOSD is unknown. METHODS: Eighteen patients with NMOSD and 10 healthy volunteers were enrolled in the test group to probe the difference of CD226 expression on Tr1 cells using flow cytometric analysis. RESULTS: The expression of CD226 on Tr1 cells exhibited significantly increased tendency in NMOSD patients. Additionally, methylprednisolone and rituximab treatment decreased the expression of CD226 on Tr1 cells. Furthermore, the expression of CD226 on Tr1 cells was correlated with disease severity. CONCLUSION: This study provides a new basic insight into CD226 expression pattern on Tr1 cells, which have great potential to be biomarkers for monitoring the development and treatment of NMOSD.


Assuntos
Neuromielite Óptica , Biomarcadores , Humanos , Neuromielite Óptica/tratamento farmacológico , Índice de Gravidade de Doença , Linfócitos T Reguladores , Resultado do Tratamento
13.
Angew Chem Int Ed Engl ; 61(28): e202204411, 2022 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-35481661

RESUMO

The minimization of thermal quenching, which leads to luminescence loss at high temperatures, is one of the most important issues for near-infrared phosphors. In the present work, we investigated the properties of near-infrared Ca(Sc,Mg)(Al, Si)O6 : Cr3+ phosphors with a pyroxene-type structure under blue light excitation. The CaScAlSiO6 : Cr3+ end member of Ca(Sc,Mg)(Al,Si)O6 : Cr3+ phosphor led to broadband emission at a full-width half maximum of 215 nm, whereas the CaMgSi2 O6 : Cr3+ end member exhibited high thermal stability at 150 °C, with an intensity of 88.4 % of that at room temperature. The structural analysis and density functional theory calculations revealed the absence of soft conformations and local space confinement contributed to the high structural rigidity and weakened the thermal quenching effect.

14.
Dalton Trans ; 51(4): 1378-1383, 2022 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-34985065

RESUMO

We report an organic solvent-assisted (OSA) co-precipitation strategy for the production of Mn4+-activated K2TiF6 phosphor. The phosphor particle size was controlled through the selection of organic solvents with an alcohol functional group and different carbon chain lengths used in the synthesis. The synergistic effect of the organic solvent and hydrofluoric acid results in large smoothed hexagonal-shaped crystal sheets of particles that become larger as the carbon chain length of the organic solvent increases. The photoluminescence (PL) properties of K2TiF6:Mn powders strongly depend on the size and thickness of the particles. The addition of n-butanol during the synthesis increases the emission intensity of K2TiF6:Mn by 208%. The PL quantum efficiency of phosphors prepared using the n-butanol-assisted strategy is much higher (98.2%) than that of conventionally prepared phosphors (89.9%). Our findings demonstrate a way to prepare the K2TiF6:Mn phosphor with targeted morphology and very high quantum efficiency and also provide the route for the optimization of all Mn4+-activated fluoride phosphors used in white light-emitting diodes.

15.
Arch Gynecol Obstet ; 305(1): 139-147, 2022 01.
Artigo em Inglês | MEDLINE | ID: mdl-34528140

RESUMO

PURPOSE: The aim of this study was to investigate differentially expressed proteins (DEPs) and their functions in the uteruses of primary dysmenorrhea (PD) rats using label-free quantitative proteomics analysis. METHODS: The PD rat model was induced by injecting both estradiol benzoate and oxytocin. Twenty rats were equally divided into two groups: a control group (normal rats), a PD model group (PD rats). Writhing scores and serum levels of Prostaglandin E2 (PGE2) and Prostaglandin F2α (PGF2α) were used to evaluate the success of the rat PD model. The DEPs were identified and analyzed by label-free quantitative proteomics and bioinformatics analyses. RESULTS: A total of 276 DEPs were identified, including 119 up-regulated DEPs and 157 down-regulated DEPs. Bioinformatics revealed that the DEPs were mainly associated with 'protein binding', 'metabolism', 'signal conduction' and 'focal adhesion'. The proteomic findings were verified by western blot analysis, which confirmed that myosin light-chain kinase (MLCK), heat shock protein 90 AB1 (HSP90AB1), apolipoprotein A1 (Apoa1), p38 MAP kinase, c-Jun N-terminal kinase (JNK), and extracellular signal-related kinase 1/2 (ERK1/2) were significantly differentially expressed in the control and PD samples. CONCLUSIONS: These results provide a deeper understanding of the molecular pathogenesis of PD. The DEPs found in the present study may provide new ideas for further study of the mechanism of PD and aid the search for biomarkers for early diagnosis and treatment.


Assuntos
Dismenorreia , Proteômica , Animais , Biologia Computacional , Dinoprostona , Dismenorreia/terapia , Feminino , Humanos , Ratos , Útero
16.
Angew Chem Int Ed Engl ; 60(8): 3940-3945, 2021 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-33200499

RESUMO

A solvent-vapor transport route produces centimeter-sized single-crystal red phosphors. The epitaxial growth route to yield its core-shell structure at ambient temperature was adopted. These red phosphors could be applied in all-inorganic WLED devices. Cs2 TiF6 :Mn4+ (CTFM) single crystal provides enhancement of quantum efficiency, moisture resistance, and thermal stability compared to polycrystalline powders. The internal quantum efficiency can reach as high as 98.7 %. To further improve waterproof stability, the Cs2 TiF6 (CTF) shell with tunable thickness has been epitaxially grown on the CTFM single crystal surface and a unique three-step photoluminescence intensity evolution mechanism has been proposed. By combining as-prepared CTFM@CTF core-shell structured single crystal, YAG:Ce single crystal and blue-chip, warm WLEDs with excellent color rendition (Ra =90, R9 =94), low correlated color temperature (CCT=3155 K), and high luminous efficacy were fabricated without any organic resins.

17.
Chem Commun (Camb) ; 56(75): 11142, 2020 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-32929425

RESUMO

Correction for 'Cu2O template synthesis of high-performance PtCu alloy yolk-shell cube catalysts for direct methanol fuel cells' by Sheng-Hua Ye et al., Chem. Commun., 2014, 50, 12337-12340, DOI: 10.1039/C4CC04108A.

18.
Angew Chem Int Ed Engl ; 59(47): 20909-20913, 2020 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-32761724

RESUMO

The practical applications of non-aqueous lithium-oxygen batteries are impeded by large overpotentials and unsatisfactory cycling durability. Reported here is that commonly encountered fatal problems can be efficiently solved by using a carbon- and binder-free electrode of titanium coated with TiO2 nanotube arrays (TNAs) and gold nanoparticles (AuNPs). Ultraviolet irradiation of the TNAs generates positively charged holes, which efficiently decompose Li2 O2 and Li2 CO3 during recharging, thereby reducing the overpotential to one that is near the equilibrium potential for Li2 O2 formation. The AuNPs promote Li2 O2 formation, resulting in a large discharge capacity. The electrode exhibits excellent stability with about 100 % coulombic efficiency during continuous cycling of up to 200 cycles, which is due to the carbon- and binder-free composition. This work reveals a new strategy towards the development of highly efficient oxygen electrode materials for lithium-oxygen batteries.

19.
Adv Sci (Weinh) ; 7(14): 2000407, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32714753

RESUMO

The rational design of electrode structure with catalysts adequately utilized is of vital importance for future fuel cells. Herein, a novel 3D oriented wholly integrated electrode comprising core-shell Fe3O4@N-doped-C (Fe3O4@NC) nanoparticles embedded into N-doped ordered interconnected hierarchical porous carbon (denoted as Fe3O4@NC/NHPC) is developed for the oxygen reduction reaction (ORR). The as-prepared catalyst possesses novel structure and efficient active sites. In rotating disk electrode measurements, the Fe3O4@NC/NHPC exhibits almost identical ORR electrocatalytic activity, superior durability, and much better methanol tolerance compared with the commercial Pt/C in acidic media. To the authors' knowledge, this is among the best non-precious-metal ORR catalysts reported so far. Importantly, the Fe3O4@NC/NHPC is successfully in situ assembled onto carbon paper by the electrophoresis method to obtain a well-designed 3D-ordered electrode. With improved mass transfer and maximized active sites for ORR, the 3D-oriented wholly integrated electrode shows superior performance to the one fabricated by the traditional method.

20.
Small ; 16(28): e2000040, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32519511

RESUMO

Structures comprising high capacity active material are highly desirable in the development of advanced electrodes for energy storage devices. However, the structure degradation of such material still remains a challenge. The construction of amorphous and crystalline heterostructure appears to be a novel and effectual strategy to figure out the problem, owing to the distinct properties of the amorphous protective layer. Herein, crystalline-Co3 O4 @amorphous-TiO2 core-shell nanoarrays directly grown on the carbon cloth substrate are rationally designed to construct the free-standing electrode. In the unique structure, the 3D porous nanoarrays provide increased availability of electrochemical active sites, and the array with a unique heterostructure of crystalline Co3 O4 core and amorphous TiO2 shell exhibits intriguing synergistic properties. Besides, the amorphous TiO2 protective layer shows elastic behavior to mitigate the volume effect of Co3 O4 . Benefiting from these structural advantages, the as-prepared free-standing electrode exhibits superior lithium storage properties, including high coulombic efficiency, outstanding cyclic stability, and rate capability. Pouch cells with high flexibility are also fabricated and show remarkable electrochemical performances, holding great potential for flexible electronic devices in the future.

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