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1.
Nature ; 2024 May 08.
Artículo en Inglés | MEDLINE | ID: mdl-38720080

RESUMEN

Light-emitting diodes (LEDs) based on perovskite quantum dots (QDs) have produced external quantum efficiencies (EQEs) of more than 25% with narrowband emission1,2, but these LEDs have limited operating lifetimes. We posit that poor long-range ordering in perovskite QD films-variations in dot size, surface ligand density and dot-to-dot stacking-inhibits carrier injection, resulting in inferior operating stability because of the large bias required to produce emission in these LEDs. Here we report a chemical treatment to improve the long-range order of perovskite QD films: the diffraction intensity from the repeating QD units increases three-fold compared with that of controls. We achieve this using a synergistic dual-ligand approach: an iodide-rich agent (aniline hydroiodide) for anion exchange and a chemically reactive agent (bromotrimethylsilane) that produces a strong acid that in situ dissolves smaller QDs to regulate size and more effectively removes less conductive ligands to enable compact, uniform and defect-free films. These films exhibit high conductivity (4 × 10-4 S m-1), which is 2.5-fold higher than that of the control, and represents the highest conductivity recorded so far among perovskite QDs. The high conductivity ensures efficient charge transportation, enabling red perovskite QD-LEDs that generate a luminance of 1,000 cd m-2 at a record-low voltage of 2.8 V. The EQE at this luminance is more than 20%. Furthermore, the stability of the operating device is 100 times better than previous red perovskite LEDs at EQEs of more than 20%.

2.
Small ; : e2402371, 2024 Apr 10.
Artículo en Inglés | MEDLINE | ID: mdl-38597692

RESUMEN

Quantum dot (QD) light-emitting diodes (QLEDs) are promising for next-generation displays, but suffer from carrier imbalance arising from lower hole injection compared to electron injection. A defect engineering strategy is reported to tackle transport limitations in nickel oxide-based inorganic hole-injection layers (HILs) and find that hole injection is able to enhance in high-performance InP QLEDs using the newly designed material. Through optoelectronic simulations, how the electronic properties of NiOx affect hole injection efficiency into an InP QD layer, finding that efficient hole injection depends on lowering the hole injection barrier and enhancing the acceptor density of NiOx is explored. Li doping and oxygen enriching are identified as effective strategies to control intrinsic and extrinsic defects in NiOx, thereby increasing acceptor density, as evidenced by density functional theory calculations and experimental validation. With fine-tuned inorganic HIL, InP QLEDs exhibit a luminance of 45 200 cd m-2 and an external quantum efficiency of 19.9%, surpassing previous inorganic HIL-based QLEDs. This study provides a path to designing inorganic materials for more efficient and sustainable lighting and display technologies.

3.
Nano Lett ; 24(9): 2765-2772, 2024 Mar 06.
Artículo en Inglés | MEDLINE | ID: mdl-38393855

RESUMEN

Alloying lanthanide ions (Yb3+) into perovskite quantum dots (Yb3+:CsPb(Cl1-xBrx)3) is an effective method to achieve efficient near-infrared (NIR) luminescence (>950 nm). Increasing the Yb3+ alloying ratio in the perovskite matrix enhances the luminescence intensity of Yb3+ emission at 990 nm. However, high Yb3+ alloying (>15%) results in vacancy-induced inferior material stability. In this work, we developed a polarity-mediated antisolvent manipulation strategy to resolve the incompatibility between a high Yb3+ alloying ratio and inferior stability of Yb3+:CsPb(Cl1-xBrx)3. Precise control of solution polarity enables increased uniformity of the perovskite matrix with fewer trap densities. Employing this strategy, we obtain Yb3+:CsPb(Cl1-xBrx)3 with the highest Yb3+ alloying ratio of 30.2% and a 2-fold higher electroluminescence intensity at 990 nm. We lever the engineered Yb3+:CsPb(Cl1-xBrx)3 to fabricate NIR-LEDs, achieving a peak external quantum efficiency (EQE) of 8.5% at 990 nm: this represents the highest among perovskite NIR-LEDs with an emission wavelength above 950 nm.

4.
Sci Bull (Beijing) ; 68(23): 2954-2961, 2023 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-37919156

RESUMEN

In terms of tunable luminescence and high quantum efficiency, colloidal quantum dots (CQDs) are promising semiconductors for constructing near-infrared light-emitting diodes (NIR-LEDs). However, currently available NIR-LEDs are susceptible to variations in the emission layer thickness (EMLT), the highest external quantum efficiency (EQE) decreases to below 50% (relative to peak EQE) when the EMLT varies out of a narrow range of (±30 nm). This is due to the thickness-dependent carrier recombination rate and current density variation, resulting in batch-to-batch EQE fluctuations that limit LED reproducibility. Here we report efficient NIR-LEDs that exhibit EQE variations of less than 15% (relative to the champion EQE) over an EMLT range of 40-220 nm; the highest achievable EQE of ∼11.5% was obtained by encapsulating a 212 nm-thick CQD within a type-I inorganic shell to enhance the radiative recombination in the dots, resulting in a high photoluminescence quantum yield of 80%, and by post-treating the films with a bifunctional linking agent to improve and balance the hole and electron mobilities in the entire film (electron mobility: 8.23 × 10-3 cm2 V-1 s-1; hole mobility: 7.0 × 10-3 cm2 V-1 s-1). This work presents the first NIR-LEDs that exhibit EMLT-invariant EQE over an EMLT range of 40-220 nm, which represents the highest EQE among reported CQD NIR-LEDs with a QD thickness exceeding 100 nm.

5.
BMC Med Imaging ; 23(1): 167, 2023 10 26.
Artículo en Inglés | MEDLINE | ID: mdl-37884901

RESUMEN

BACKGROUND: To investigate the association between CT signs and clinicopathological features and disease recurrence in patients with hepatoid adenocarcinoma of stomach (HAS). METHODS: Forty nine HAS patients undergoing radical surgery were retrospectively collected. Association between CT and clinicopathological features and disease recurrence was analyzed. Multivariate logistic model was constructed and evaluated for predicting recurrence by using receiver operating characteristic (ROC) curve. Survival curves between model-defined risk groups was compared using Kaplan-Meier method. RESULTS: 24(49.0%) patients developed disease recurrence. Multivariate logistic analysis results showed elevated serum CEA level, peritumoral fatty space invasion and positive pathological vascular tumor thrombus were independent factors for disease recurrence. Odds ratios were 10.87 (95%CI, 1.14-103.66), 6.83 (95%CI, 1.08-43.08) and 42.67 (95%CI, 3.66-496.85), respectively. The constructed model showed an area under ROC of 0.912 (95%CI,0.825-0.999). The model-defined high-risk group showed poorer overall survival and recurrence-free survival than the low-risk group (both P < 0.001). CONCLUSIONS: Preoperative CT appearance of peritumoral fatty space invasion, elevated serum CEA level, and pathological vascular tumor thrombus indicated poor prognosis of HAS patients.


Asunto(s)
Adenocarcinoma , Neoplasias Gástricas , Trombosis , Neoplasias Vasculares , Humanos , Estudios Retrospectivos , Pronóstico , Neoplasias Vasculares/patología , Recurrencia Local de Neoplasia/diagnóstico por imagen , Recurrencia Local de Neoplasia/patología , Adenocarcinoma/diagnóstico por imagen , Adenocarcinoma/cirugía , Neoplasias Gástricas/diagnóstico por imagen , Neoplasias Gástricas/cirugía , Tomografía Computarizada por Rayos X , Estadificación de Neoplasias
6.
Huan Jing Ke Xue ; 44(10): 5718-5726, 2023 Oct 08.
Artículo en Chino | MEDLINE | ID: mdl-37827787

RESUMEN

Phosphorus exerts a good stabilization effect on soil lead. In this study, the findings of 90 papers were summarized using the Meta-analysis method. These papers described the immobilization of soil lead using phosphorus from 1997 to 2022. The effects of phosphorus materials on the stabilization rate and speciation transformation of soil Pb and soil pH were quantitatively analyzed based on soil properties, stabilization process conditions, and types of phosphorus materials. The results revealed that the stronger the soil alkalinity (pH ≥ 7.5), the lower is the content of lead (≤ 500 mg·kg-1), and the higher the content of soil organic matter (>0.5%), the more conducive it is to the phosphorus-based stabilization of soil lead; the stabilization rates are 75.21%, 34.97% and 93.12%, respectively. In terms of stabilization process conditions, the higher the addition amount of phosphorus (≥ 10%), the higher is the water content (>50%)and longer is the curing time (≥ 30 days), and the higher the curing temperature (≥ 40℃), the more conducive it is to the stabilization of soil lead, and the stabilization rates are 80.65%, 84.98%, 79.39%, and 41.44%, respectively. According to the types of phosphorus, soluble phosphorus had a high stabilization rate of soil lead (96.24%). The conversion rate of exchangeable lead and carbonate-bound lead to residual lead was 95.93%. Soluble phosphorus was majorly acidic, reducing the soil pH by 7.27%, whereas insoluble phosphorus was majorly alkaline, increasing the soil pH by 3.63%. In conclusion, when the soil pH ≥ 7.5, soil lead content ≤ 500 mg·kg-1, soil organic matter content >0.5%, soluble phosphorus addition ≥ 10%, water content >50%, curing time ≥ 30 days, and curing temperature ≥ 40℃, phosphorus had a better effect on soil Pb stabilization. In the actual remediation process of lead-contaminated soil, to improve the lead stabilization rate, it is necessary to comprehensively consider the effects of soil properties, stabilization process conditions, phosphorus, and other factors.

7.
Angew Chem Int Ed Engl ; 62(46): e202311089, 2023 Nov 13.
Artículo en Inglés | MEDLINE | ID: mdl-37770413

RESUMEN

Resurfacing perovskite nanocrystals (NCs) with tight-binding and conductive ligands to resolve the dynamic ligands-surface interaction is the fundamental issue for their applications in perovskite light-emitting diodes (PeLEDs). Although various types of surface ligands have been proposed, these ligands either exhibit weak Lewis acid/base interactions or need high polar solvents for dissolution and passivation, resulting in a compromise in the efficiency and stability of PeLEDs. Herein, we report a chemically reactive agent (Iodotrimethylsilane, TMIS) to address the trade-off among conductivity, solubility and passivation using all-inorganic CsPbI3 NCs. The liquid TMIS ensures good solubility in non-polar solvents and reacts with oleate ligands and produces in situ HI for surface etching and passivation, enabling strong-binding ligands on the NCs surface. We report, as a result, red PeLEDs with an external quantum efficiency (EQE) of ≈23 %, which is 11.2-fold higher than the control, and is among the highest CsPbI3 PeLEDs. We further demonstrate the universality of this ligand strategy in the pure bromide system (CsPbBr3 ), and report EQE of ≈20 % at 640, 652, and 664 nm. This represents the first demonstration of a chemically reactive ligand strategy that applies to different systems and works effectively in red PeLEDs spanning emission from pure-red to deep-red.

8.
Sci Adv ; 9(36): eadh2140, 2023 Sep 08.
Artículo en Inglés | MEDLINE | ID: mdl-37683007

RESUMEN

Blue perovskite light-emitting diodes (LEDs) have shown external quantum efficiencies (EQEs) of more than 10%; however, devices that emit in the true blue-those that accord with the emission wavelength required for Rec. 2100 primary blue-have so far been limited to EQEs of ~6%. We focused here on true blue emitting CsPbBr3 colloidal nanocrystals (c-NCs), finding in early studies that they suffer from a high charge injection barrier, a problem exacerbated in films containing multiple layers of nanocrystals. We introduce a self-assembled monolayer (SAM) active layer that improves charge injection. We identified a bifunctional capping ligand that simultaneously enables the self-assembly of CsPbBr3 c-NCs while passivating surface traps. We report, as a result, SAM-based LEDs exhibit a champion EQE of ~12% [CIE of (0.132, 0.069) at 4.0 V with a luminance of 11 cd/m2], and 10-fold-enhanced operating stability relative to the best previously reported Rec. 2100-blue perovskite LEDs.

9.
Artículo en Inglés | MEDLINE | ID: mdl-37591053

RESUMEN

The sea cucumber Holothuria leucospilota, a nutritive and commercial marine species, has a high protein and low lipid content. To date, the mechanisms underlying gender determination and differentiation in sea cucumbers remain unclear. Identifying gender-specific molecular markers is an effective method of revealing the genetic basis of gender determination and differentiation. The inability to distinguish between male and female individuals causes reproductive efficiency to decline in aquaculture. In this study, we used the gonads of the sea cucumber H. leucospilota as samples to conduct the experiment. The differentially abundant metabolites (DAMs) detected by liquid chromatography-mass spectrometry were enriched in pathways associated with prolactin metabolism, insulin metabolism, hypoxia-inducible factor-1 signaling, and calcium signaling. At the transcriptome level, Illumina sequencing was performed on H. leucospilota, demonstrating that gender-specific expression genes were enriched in the retinoic acid-inducible gene I-like receptor signaling pathway, C-type lectin receptor signaling pathway, alpha-linolenic acid metabolism, and ether lipid metabolism by the Kyoto Encyclopedia of Genes and Genomes (KEGG) analysis. By analyzing the common pathways between DAMs and differentially expressed genes, we found that gender-related genes of H. leucospilota were mostly enriched in the necroptosis pathway and the cysteine and methionine metabolism pathways. According to the common pathways, uch-sc1 and uch-sc2 are male-specific expression genes, and uch-sc3 and bhmt are female-specific expression genes at the mRNA level. These results provide information on gender differences in H. leucospilota.


Asunto(s)
Holothuria , Pepinos de Mar , Humanos , Animales , Femenino , Masculino , Transcriptoma , Metaboloma , Señalización del Calcio
10.
Adv Mater ; 35(45): e2303528, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37450343

RESUMEN

Addition of aqueous hydrohalic acids during the synthesis of colloidal quantum dots (QDs) is widely employed to achieve high-quality QDs. However, this reliance on the use of aqueous solutions is incompatible with oxygen- and water-sensitive precursors such as those used in the synthesis of Te-alloyed ZnSe QDs. Herein, it is shown that this incompatibility leads to phase segregation into Te-rich and Te-poor regions, causing spectral broadening and luminescence peak shifting under high laser irradiation and applied electrical bias. Here, a synthetic strategy to produce anhydrous-HF in situ by using benzenecarbonyl fluoride (BF) as a chemical additive is reported. Through in situ 19 F NMR spectroscopy, it is found that BF reacts with surfactants in tandem, ultimately producing intermediary F···H···trioctylamine adducts. These act as a pseudo-HF source that releases anhydrous HF. The controlled release of HF during nucleation and growth steps homogenizes Te distribution in ZnSeTe lattice, leading to spectrally stable blue-emitting QDs under increasing laser flux from ≈3 µW to ≈12 mW and applied bias from 2.6 to 10 V. Single-dot photoluminescence (PL) spectroscopy and analyses of the absorption, PL and transient absorption spectra together with density functional theory point to the role of anhydrous HF as a Te homogenizer.

11.
Nanomaterials (Basel) ; 13(10)2023 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-37242111

RESUMEN

Quantum dot light-emitting diodes (QLEDs) have been identified as a next-generation display technology owing to their low-cost manufacturing, wide color gamut, and electrically driven self-emission properties. However, the efficiency and stability of blue QLEDs still pose a significant challenge, limiting their production and potential application. This review aims to analyse the factors leading to the failure of blue QLEDs and presents a roadmap to accelerate their development based on the progress made in the synthesis of II-VI (CdSe, ZnSe) quantum dots (QDs), III-V (InP) QDs, carbon dots, and perovskite QDs. The proposed analysis will include discussions on material synthesis, core-shell structures, ligand interactions, and device fabrication, providing a comprehensive overview of these materials and their development.

12.
J Am Chem Soc ; 145(11): 6428-6433, 2023 Mar 22.
Artículo en Inglés | MEDLINE | ID: mdl-36897963

RESUMEN

Indium phosphide (InP) quantum dots have enabled light-emitting diodes (LEDs) that are heavy-metal-free, narrow in emission linewidth, and physically flexible. However, ZnO/ZnMgO, the electron-transporting layer (ETL) in high-performance red InP/ZnSe/ZnS LEDs, suffers from high defect densities, quenches luminescence when deposited on InP, and induces performance degradation that arises due to trap migration from the ETL to the InP emitting layer. We posited that the formation of Zn2+ traps on the outer ZnS shell, combined with sulfur and oxygen vacancy migration between ZnO/ZnMgO and InP, may account for this issue. We synthesized therefore a bifunctional ETL (CNT2T, 3',3'″,3'″″-(1,3,5-triazine-2,4,6-triyl)tris(([1,1'-biphenyl]-3-carbonitrile)) designed to passivate Zn2+ traps locally and in situ and to prevent vacancy migration between layers: the backbone of the small molecule ETL contains a triazine electron-withdrawing unit to ensure sufficient electron mobility (6 × 10-4 cm2 V-1 s-1), and the star-shaped structure with multiple cyano groups provides effective passivation of the ZnS surface. We report as a result red InP LEDs having an EQE of 15% and a luminance of over 12,000 cd m-2; this represents a record among organic-ETL-based red InP LEDs.

13.
ACS Nano ; 17(4): 3696-3704, 2023 Feb 28.
Artículo en Inglés | MEDLINE | ID: mdl-36745006

RESUMEN

Given the synergy of optogenetics and bioimaging in neuroscience, it is possible for light to simultaneously modulate and visualize synaptic events of optoelectronic synaptic devices, which are building blocks of a neuromorphic computing system with optoelectronic integration. Here we demonstrate the realization of the simultaneous modulation and visualization of synaptic events by using optically stimulated synaptic devices based on the heterostructure of fluorescent silicon quantum dots (Si QDs) and monolayer molybdenum disulfide (MoS2). The charge-transfer-enabled photogating effect of the Si QDs/MoS2 heterostructure leads to the nonvolatility of the synaptic devices, which exhibit important synaptic functionalities and synchronous fluorescence upon optical stimulation. An array of the Si QDs/MoS2 optoelectronic synaptic devices is well-employed to mimic robust neural population coding. Defective devices in this array may be pinpointed by the absence of their fluorescence. This work has an important implication for the development of synaptic devices facilitating the system-level diagnosis and device-level positioning of a neuromorphic computing system.

14.
Exp Biol Med (Maywood) ; 248(3): 201-208, 2023 02.
Artículo en Inglés | MEDLINE | ID: mdl-36598065

RESUMEN

This study set out to investigate the clinical significance of serum tumor necrosis factor receptor-associated protein 1 (TRAP1) in diagnosing small cell lung cancer (SCLC) with different clinical stages, and to compare the diagnostic efficiency with neuron-specific enolase (NSE), carcinoembryonic antigen (CEA) and carbohydrate antigen 19-9 (CA19-9). Besides, to analyze the role of serum TRAP1 in tumor immunity. A total of 91 patients with SCLC, 99 patients with non-small cell lung cancer (NSCLC), 102 patients with pulmonary nodules (PN), and 75 healthy people were included. The concentrations of serum TRAP1 was detected by enzyme-linked immunosorbent assay (ELISA). NSE, CEA, and CA19-9 were detected by chemiluminescence. The results showed that level of TRAP1 in Group SCLC was lower than other three groups (P < 0.01), whereas NSE in SCLC was significantly higher than the others (P < 0.01), and the levels of CEA and CA19-9 were higher than healthy people and PN patients (P < 0.01). There was a significant difference in TRAP1 levels between patients with limited-stage disease SCLC (LD-SCLC) and extensive-stage disease SCLC (ED-SCLC) (P < 0.0001). The sensitivity and specificity of TRAP1 in diagnosing LD-SCLC were 0.964 and 0.560, respectively, and the area under the curve (AUC) was 0.819. The sensitivity and specificity in diagnosing ED-SCLC were 0.810 and 0.868, respectively, and the AUC was 0.933, which showed high diagnostic value. The AUC of these two groups can be increased to 0.946 and 0.947 in combination of four biomarkers, effectively improving the diagnosis rate of SCLC. Our findings have revealed that serum TRAP1 has high diagnostic value for SCLC and high diagnostic sensitivity for LD-SCLC. It is a potential biomarker for SCLC. Combined detection can effectively improve the diagnosis rate of SCLC. TRAP1 may be secreted into the circulation by mature immune cells and participates in tumor immunity as a carrier of tumor antigens.


Asunto(s)
Carcinoma de Pulmón de Células no Pequeñas , Neoplasias Pulmonares , Humanos , Antígeno Carcinoembrionario , Carcinoma de Pulmón de Células no Pequeñas/patología , Neoplasias Pulmonares/patología , Antígeno CA-19-9 , Biomarcadores de Tumor/análisis , Proteínas HSP90 de Choque Térmico
15.
Br J Clin Pharmacol ; 89(4): 1491-1494, 2023 04.
Artículo en Inglés | MEDLINE | ID: mdl-36440759

RESUMEN

Ceftriaxone is widely used in children with community-acquired pneumonia. Currently, there are no available data regarding epithelial lining fluid (ELF) concentrations of ceftriaxone in children. Thus, blood and bronchoalveolar lavage fluids samples were collected by using an opportunistic sampling design, then we determined plasma and ELF concentrations in 22 children (0.5-11.7 years), with a total of 36 plasma and 22 ELF samples available for analysis. Ceftriaxone plasma and ELF concentrations ranged from 1.07 to 138.71 mg/L and from 0.61 to 26.69 mg/L, respectively. Ceftriaxone concentration in ELF was 12.18 ± 5.15 (mean ± standard deviation) times higher than that in plasma, ranging from 1.29 to 20.44.


Asunto(s)
Ceftriaxona , Neumonía , Humanos , Niño , Neumonía/tratamiento farmacológico , Líquido del Lavado Bronquioalveolar , Antibacterianos
16.
J Am Chem Soc ; 144(45): 20923-20930, 2022 Nov 16.
Artículo en Inglés | MEDLINE | ID: mdl-36327099

RESUMEN

InP-based quantum dot (QD) light-emitting diodes (QLEDs) provide a heavy-metal-free route to size-tuned LEDs having high efficiency. The stability of QLEDs may be enhanced by replacing organic hole-injection layers (HILs) with inorganic layers. However, inorganic HILs reported to date suffer from inefficient hole injection, the result of their shallow work functions. Here, we investigate the tuning of the work function of nickel oxide (NiOx) HILs using self-assembled molecules (SAMs). Density functional theory simulations and near-edge X-ray absorption fine structure put a particular focus onto the molecular orientation of the SAMs in tuning the work function of the NiOx HIL. We find that orientation plays an even stronger role than does the underlying molecular dipole itself: SAMs having the strongest electron-withdrawing nitro group (NO2), despite having a high intrinsic dipole, show limited work function tuning, something we assign to their orientation parallel to the NiOx surface. We further find that the NO2 group─which delocalizes electrons over the molecule by resonance─induces a deep lowest unoccupied molecular orbital level that accepts electrons from QDs, producing luminescence quenching. In contrast, SAMs containing a trifluoromethyl group exhibit an angled orientation relative to the NiOx surface, better activating hole injection into the active layer without inducing luminescence quenching. We report an external quantum efficiency (EQE) of 18.8%─the highest EQE among inorganic HIL-based QLEDs (including Cd-based QDs)─in InP QLEDs employing inorganic HILs.

17.
ACS Appl Mater Interfaces ; 14(15): 17691-17697, 2022 Apr 20.
Artículo en Inglés | MEDLINE | ID: mdl-35411769

RESUMEN

Perovskite quantum dots (PQDs) are applicable in light-emitting diodes (LEDs) owing to their color tunability, high color purity, and excellent photoluminescence quantum yield (PLQY) in the solution state. However, a PQD film obtained through nonradiative recombination by concentration quenching and the formation of surface defects exhibited a low PLQY. In this study, we focused on the energy transfer between PQDs with different energy gaps (Eg) to reduce nonradiative recombination in the film state and consequently achieve high device performance. We prepared size-controlled PQDs measuring 10.7 nm (large-size QD; LQD) and 7.9 nm (small-size QD; SQD) with different Eg values and observed a spectral overlap between SQD emission and LQD absorption. To investigate the Förster resonance energy transfer (FRET) from SQDs to LQDs, we prepared SQD-LQD mixed QDs (MQDs). The MQD film enhanced LQD emission and exhibited a higher PLQY (52%) with a longer PL decay time (7.4 ns) than those exhibited by the neat LQD film (38% and 6.2 ns). This energy transfer was determined to be FRET by photoluminescence excitation and PL decay times. Moreover, the external quantum efficiency of an MQD-based LED increased to 15%, indicating that the FRET process can enhance the PLQY of the film and LED efficiency.

18.
ACS Appl Mater Interfaces ; 14(11): 13722-13732, 2022 Mar 23.
Artículo en Inglés | MEDLINE | ID: mdl-35274932

RESUMEN

Metal organic frameworks (MOFs) have unique advantages in optimizing the ionic conductivity of battery separators because of their rich cavity structure and highly ordered and connected pores. In this study, we used a hydrothermal method to synthesize a functional material, Ag-MOF crystal, as a separator coating content, and then studied the properties and application effect of the MOF-Al2O3-blended coating applying to a polyethylene (PE) separator (MOFxAl1-x/PE). Results show that MOF0.08Al0.92/PE (MOF/Al2O3 = 0.08:0.92) used in NCM811||Li cells significantly not only improves the fast charge-discharge performance of the cells but also inhibits the growth of lithium dendrites during long-term charge-discharge cycling; the Li+ transference number (tLi+) of the MOF0.08Al0.92/PE composite separator is 0.61; the Li||separator||Li half-cell circulates stably for 1000 h at varying current density from 0.5 to 10 mA cm-2 and only produces low overpotentials, indicating that MOF0.08Al0.92 stabilizes lithium. The initial capacity of the NCM811||Li cell using the MOF0.08Al0.92/PE separator is 165.0 mA h g-1, its capacity retention is 70.67% after 300 cycles at 5 C, and the interface resistance of the cells only increases from 13.8 to 31.5 Ω, whereas the capacity retention of Al2O3/PE separator batteries is only 40.41% (62.2 mA h g-1) under the same conditions. During the charge-discharge cycling, the MOF-Al2O3 coating induces the lithium anode to quickly form a stable and dense solid-electrolyte interphase layer, promotes the uniform deposition of Li+, and inhibits the growth of lithium dendrites as well.

19.
Adv Mater ; 34(21): e2200854, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-35297516

RESUMEN

Instability in mixed-halide perovskites (MHPs) is a key issue limiting perovskite solar cells and light-emitting diodes (LEDs). One form of instability arises during the processing of MHP quantum dots using an antisolvent to precipitate and purify the dots forming surface traps that lead to decreased luminescence, compromised colloidal stability, and emission broadening. Here, the introduction of inorganic ligands in the antisolvents used in dot purification is reported in order to overcome this problem. MHPs that are colloidally stable for over 1 year at 25 °C and 40% humidity are demonstrated and films that are stable under 100 W cm-2 photoirradiation, 4× longer than the best previously reported MHPs, are reported. In LEDs, the materials enable an EQE of 24.4% (average 22.5 ± 1.3%) and narrow emission (full-width at half maximum of 30 nm). Sixfold-enhanced operating stability relative to the most stable prior red perovskite LEDs having external quantum efficiency >20% is reported.

20.
Nature ; 599(7886): 594-598, 2021 11.
Artículo en Inglés | MEDLINE | ID: mdl-34819678

RESUMEN

Light-emitting diodes (LEDs) based on perovskite quantum dots have shown external quantum efficiencies (EQEs) of over 23% and narrowband emission, but suffer from limited operating stability1. Reduced-dimensional perovskites (RDPs) consisting of quantum wells (QWs) separated by organic intercalating cations show high exciton binding energies and have the potential to increase the stability and the photoluminescence quantum yield2,3. However, until now, RDP-based LEDs have exhibited lower EQEs and inferior colour purities4-6. We posit that the presence of variably confined QWs may contribute to non-radiative recombination losses and broadened emission. Here we report bright RDPs with a more monodispersed QW thickness distribution, achieved through the use of a bifunctional molecular additive that simultaneously controls the RDP polydispersity while passivating the perovskite QW surfaces. We synthesize a fluorinated triphenylphosphine oxide additive that hydrogen bonds with the organic cations, controlling their diffusion during RDP film deposition and suppressing the formation of low-thickness QWs. The phosphine oxide moiety passivates the perovskite grain boundaries via coordination bonding with unsaturated sites, which suppresses defect formation. This results in compact, smooth and uniform RDP thin films with narrowband emission and high photoluminescence quantum yield. This enables LEDs with an EQE of 25.6% with an average of 22.1 ±1.2% over 40 devices, and an operating half-life of two hours at an initial luminance of 7,200 candela per metre squared, indicating tenfold-enhanced operating stability relative to the best-known perovskite LEDs with an EQE exceeding 20%1,4-6.

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