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1.
Eur J Ophthalmol ; : 11206721241252476, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38693770

RESUMO

PURPOSES: To investigate the features of the anterior segment structures in neovascular glaucoma (NVG) and analyze its differences from primary angle-closure glaucoma (PACG). METHODS: This study included patients who were first diagnosed with monocular NVG and PACG at the Affiliated Eye Hospital of Nanchang University during August 2019 to June 2022. Ultrasound biomicroscopy (UBM) was used to measure the anterior segment parameters of those eyes, including anterior chamber depth (ACD), anterior chamber width (ACW), anterior chamber area (ACA), iris area (IA), maximum iris thickness (ITMAX), middle iris thickness (ITMID), iris curvature (IC), lens vault (LV), angle opening distance (AOD500), trabecular iris angle (TIA500), trabecular-iris space area (TISA500) and peripheral anterior synechia (PAS) length. RESULTS: In this study, paired samples t-test showed that IA [1.170(0.324) mm2], ITMAX [0.368(0.079) mm], ITMID [0.280(0.062) mm] and IC [0.147(0.037) mm] of NVG were smaller than F-NVG [2.058(0.195) mm2, 0.611(0.045) mm, 0.415(0.049) mm and 0.272(0.077) mm], the AOD500, TIA500, and TISA500 of NVG were also smaller than F-NVG. Independent samples t-test showed that ACD [2.349(0.350) mm] and ACA [16.326(3.547) mm2] of NVG were larger than PACG [1.971(0.240) mm, 12.030(1.860) mm2], but the IA [1.170(0.324) mm2], ITMAX [0.368(0.079) mm], ITMID [0.280(0.062) mm], IC [0.147(0.037) mm] and LV [0.436(0.172 mm)] were smaller than PACG [1.740(0.294) mm2, 0.548(0.084) mm, 0.404(0.065) mm, 0.283(0.060) mm and 0.737(0.196) mm]. Among the 16 patients with 360° angle-closure NVG, the PAS length was 0.834 (0.326) mm, which exceeded the Schwalbe line. CONCLUSION: In NVG, the iris is atrophied, thinned, and straight, while the ACD is normal or slightly shallow. In 360° angle-closure NVG, the PAS length exceeds the Schwalbe line, presenting a pseudo angle phenomenon and a hockey stick sign. Notably, the anterior segment structure morphology of NVG exhibit differences from those of PACG.

2.
Artigo em Inglês | MEDLINE | ID: mdl-38682823

RESUMO

In the selective oxidation of H2S, the catalytic activity over N-doped carbon-based catalysts is significantly influenced by the accessibility of active sites and the mass transfer rates of reactant molecules (e.g., H2S and O2) as well as generated sulfur monomers. Therefore, it is crucial for enhancing the initial performance via the controlled synthesis of carbon-based catalysts with highly exposed active sites and unique porous structures. Herein, we reported on an efficient strategy to synthesize nanosized N-doped carbon particles with hierarchical porous structures by directly pyrolyzing an oversaturated NaCl-encapsulated ZIF-8 precursor mixture. The introduction of NaCl not only serves as a pollution-free template to promote the formation of graphitic carbon layers but also acts as an intercalating agent to guide the derivation of hierarchical porous structures, as well as enhances the amount of active nitrogen species in the catalysts. As a result, the as-prepared H-NC800 catalyst shows excellent H2S selective oxidation performance (sulfur formation rate is 794 gsulfur·kgcat-1·h-1), good stability (>80 h), and antiwater vapor properties. The characterization results and DFT calculations indicate the crucial role of pyridinic N in the adsorbing and activating reactant molecules (H2S, O2). Furthermore, nanoscale N-doped carbon particles accelerated the rapid transport of generated sulfur monomers under a hierarchical porous structure. This investigation introduces a distinctive strategy for synthesizing ZIF-8-derived N-doped carbon nanosized with a hierarchical porous structure, while its efficient and stable H2S selective oxidation performance highlights significant potential for practical implementation in the industrial desulfurization process.

3.
ACS Appl Mater Interfaces ; 16(10): 12446-12454, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38427847

RESUMO

Recently, perovskite solar cells (PSCs) based on quasi-two-dimensional (quasi-2D) perovskites have drawn more attention due to their excellent stability, although their efficiencies are still lower than those of 3D ones. Here we applied post-treatment of 2D perovskite GAMA5Pb5I16 (GA = guanidinium, MA = methylammonium) films with acetaminophen (AMP) to improve their performance. The efficiency of the solar cells with 2 mg/mL AMP post-treatment increased to 18.01% from 16.72% for those without post-treatment. The efficiency improvement results from the enlarged grain size, reduced trap state density, and better energy level matching after AMP post-treatment. In addition, the stability of the solar cells is improved. The solar cells with AMP post-treatment maintain 91% of the original power conversion efficiency value after aging for 30 days in the atmosphere. This work opens a new approach for the efficiency and stability enhancement of quasi-2D PSCs.

4.
Front Oncol ; 13: 1247682, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-38074651

RESUMO

Purpose: This bi-institutional study aimed to establish a robust model for predicting clinically significant prostate cancer (csPCa) (pathological grade group ≥ 2) in PI-RADS 3 lesions in the transition zone by comparing the performance of combination models. Materials and methods: This study included 243 consecutive men who underwent 3-Tesla magnetic resonance imaging (MRI) and ultrasound-guided transrectal biopsy from January 2020 and April 2022 which is divided into a training cohort of 170 patients and a separate testing cohort of 73 patients. T2WI and DWI images were manually segmented for PI-RADS 3 lesions for the mean ADC and radiomic analysis. Predictive clinical factors were identified using both univariate and multivariate logistic models. The least absolute shrinkage and selection operator (LASSO) regression models were deployed for feature selection and for constructing radiomic signatures. We developed nine models utilizing clinical factors, radiological features, and radiomics, leveraging logistic and XGboost methods. The performances of these models was subsequently compared using Receiver Operating Characteristic (ROC) analysis and the Delong test. Results: Out of the 243 participants with a median age of 70 years, 30 were diagnosed with csPCa, leaving 213 without a csPCa diagnosis. Prostate-specific antigen density (PSAD) stood out as the only significant clinical factor (odds ratio [OR], 1.068; 95% confidence interval [CI], 1.029-1.115), discovered through the univariate and multivariate logistic models. Seven radiomic features correlated with csPCa prediction. Notably, the XGboost model outperformed eight other models (AUC of the training cohort: 0.949, and validation cohort: 0.913). However, it did not surpass the PSAD+MADC model (P > 0.05) in the training and testing cohorts (AUC, 0.949 vs. 0.888 and 0.913 vs. 0.854, respectively). Conclusion: The machine learning XGboost model presented the best performance in predicting csPCa in PI-RADS 3 lesions within the transitional zone. However, the addition of radiomic classifiers did not display any significant enhancement over the compound model of clinical and radiological findings. The most exemplary and generalized option for quantitative prostate evaluation was Mean ADC+PSAD.

5.
Nano Lett ; 23(24): 11999-12005, 2023 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-38100577

RESUMO

Redispersion is an effective method for regeneration of sintered metal-supported catalysts. However, the ambiguous mechanistic understanding hinders the delicate controlling of active metals at the atomic level. Herein, the redispersion mechanism of atomically dispersed Pt on CeO2 is revealed and manipulated by in situ techniques combining well-designed model catalysts. Pt nanoparticles (NPs) sintered on CeO2 nano-octahedra under reduction and oxidation conditions, while redispersed on CeO2 nanocubes above ∼500 °C in an oxidizing atmosphere. The dynamic shrinkage and disappearance of Pt NPs on CeO2 (100) facets was directly visualized by in situ TEM. The generated atomically dispersed Pt with the square-planar [PtO4]2+ structure on CeO2 (100) facets was also confirmed by combining Cs-corrected STEM and spectroscopy techniques. The redispersion and atomic control were ascribed to the high mobility of PtO2 at high temperatures and its strong binding with square-planar O4 sites over CeO2 (100). These understandings are important for the regulation of atomically dispersed platinum catalysts.

6.
Eur J Ophthalmol ; : 11206721231208244, 2023 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-37872653

RESUMO

BACKGROUND: Emerging evidence suggested a significant association between optic atrophy 1 (OPA1) polymorphisms and primary open angle glaucoma (POAG) risk. However, the current data are inconsistent or even contradictory. Given these, we conducted a meta-analysis to examine the precise association between OPA1 polymorphisms and POAG risk. MATERIALS AND METHODS: Online databases were retrieved, and the related studies were reviewed from inception to December 1, 2022. Odds ratios (ORs) and corresponding 95% confidence intervals (CIs) were calculated to examine the statistical power of each genetic model. In addition, heterogeneity, sensitivity, cumulative analysis, and publication bias were analyzed to guarantee statistical power. RESULT: Overall, 14 studies within 11 publications (involving 2,413 POAG patients and 1,904 controls) were included and some significant association between OPA1 rs166850 C/T (T vs. C: OR = 1.24, 95%CI = 1.06-1.45, P = 0.01, I2 = 39.0%; CT vs. CC: OR = 1.37, 95%CI = 1.05-1.79, P = 0.02, I2 = 41.6%; CT + TT vs. CC: 1.37, 95%CI = 1.06-1.77, P = 0.02, I2 = 41.6%), rs10451941T/C (TC + CC vs. TT: OR = 1.79, 95%CI = 1.41-2.28, P < 0.01, I2 = 71.9%) polymorphisms and POAG susceptibility. In addition, further significant associations were also observed in the stratified analysis, especially in normal tension glaucoma groups and Caucasian descendants. CONCLUSION: The observed evidences suggest that OPA1 polymorphisms may be associate with POAG susceptibility significantly.

7.
BMC Cancer ; 23(1): 1005, 2023 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-37858067

RESUMO

BACKGROUND: SH2 domain containing 1A (SH2D1A) expression has been linked to cancer progression. However, the functions of SH2D1A in hepatocellular carcinoma (HCC) have not been reported. METHODS: The effects of SH2D1A on the proliferation, migration, and invasion of HCC cells and the related pathways were re-explored in cell models with SH2D1A overexpression using the CCK-8, migration and invasion assays and western blotting. The functions and mechanisms of genes co-expressed with SH2D1A were analyzed using gene ontology (GO) and Kyoto Encyclopedia of Genes and Genomes (KEGG) analysis. The relationship between SH2D1A expression and immune microenvironment features in HCC was explored. RESULTS: Elevated SH2D1A expression promoted cell proliferation, migration, and invasion, which was related to the overexpression of p-Nf-κB and BCL2A1 protein levels in HCC. SH2D1A expression was related to the immune, stromal, and ESTIMATE scores, and the abundance of immune cells, such as B cells, CD8+ T cells, and T cells. SH2D1A expression was significantly related to the expression of immune cell markers, such as PDCD1, CD8A, and CTLA4 in HCC. CONCLUSION: SH2D1A overexpression was found to promote cell growth and metastasis via the Nf-κB signaling pathway and may be related to the immune microenvironment in HCC. The findings indicate that SH2D1A can function as a biomarker in HCC.


Assuntos
Carcinoma Hepatocelular , Neoplasias Hepáticas , Proteína Associada à Molécula de Sinalização da Ativação Linfocitária , Humanos , Biomarcadores Tumorais/genética , Biomarcadores Tumorais/imunologia , Carcinoma Hepatocelular/genética , Carcinoma Hepatocelular/imunologia , Carcinoma Hepatocelular/patologia , Linfócitos T CD8-Positivos , Biologia Computacional , Neoplasias Hepáticas/genética , Neoplasias Hepáticas/imunologia , Neoplasias Hepáticas/patologia , Processos Neoplásicos , NF-kappa B , Proteína Associada à Molécula de Sinalização da Ativação Linfocitária/genética , Proteína Associada à Molécula de Sinalização da Ativação Linfocitária/imunologia , Microambiente Tumoral/genética , Microambiente Tumoral/imunologia
8.
ACS Appl Mater Interfaces ; 15(24): 29178-29185, 2023 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-37279435

RESUMO

Poor stability retards the industrialization of perovskite solar cells (PSCs). One of the effective ways to solve this issue is to modify the perovskite surface to improve the efficiency and stability of the PSCs. Herein, we synthesized CuFeS2 nanocrystals and applied them to modify the perovskite surface. The efficiency of the PSCs with CuFeS2 modification is improved to 20.17% from 18.64% for the control devices. Some investigations demonstrate that the CuFeS2 modification passivates the perovskite surface defects and induces better energy band arrangement. Furthermore, the stability of the PSCs with CuFeS2 modification is improved compared with the devices without CuFeS2 modification. The efficiency of the PSCs with CuFeS2 modification maintains 93% of its initial value, whereas that of the devices without CuFeS2 modification decreases to 61% of the initial value. This work demonstrates that CuFeS2 is a novel material used as a modification layer to enhance the efficiency and stability of the PSCs.

9.
Opt Lett ; 48(11): 2841-2844, 2023 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-37262224

RESUMO

The formation mechanism of laser-induced periodic surface structures (LIPSS) has been a key to high-resolution sub-diffraction lithography or high-efficiency large-area nanotexturing. We show the evolution of LIPSS formation from a nanohole seed structure to high-spatial-frequency LIPSS by using a tightly focused and rectangular-shaped laser beam with different shape-polarization orientations. Formation of LIPSS based on light intensity distribution without invoking any long-range electromagnetic modes achieved quantitative match between modeling and experiment. Our results clearly show the entire step-like and deterministic process of LIPSS evolution based on experimental data and numerical simulations, revealing the dominant structural near-field enhancement on the ripple formation. A rectangular-shaped beam with an aspect ratio of 7:3 was used to break the symmetry of a circularly shaped focus. By azimuthally rotating the orientation of the focal spot and the polarization, it is possible to visualize the far-field effect for the initial seed structure formation and the competition between the far and near fields in the subsequent structure evolution.

10.
Nano Lett ; 23(13): 6116-6123, 2023 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-37387619

RESUMO

2D/3D perovskite heterostructures show great potential to boost efficiency and stability of perovskite solar cells (PSCs). Here, a solvent-free transfer-imprinting-assisted growth (TIAG) method is employed to in situ grow 2D/3D perovskite heterojunctions. The solid-state transfer of spacer cation by the TIAG process enables a spatially confined growth of the 2D perovskite interlayer with uniform morphology between the 3D perovskites and charge transport layer. Meanwhile, the pressure associated with the TIAG process promotes the crystalline orientation, which is beneficial to carrier transport. As a result, the inverted PSC achieved a PCE of 23.09% (with certified 22.93%) and maintained 90% of their initial PCE after aging at 85 °C for 1200 h or operating for 1100 h under continuous AM 1.5 illumination. Flexible inverted PSCs achieved a PCE of 21.14% with mechanical robustness by maintaining above 80% of their initial PCE after 10000 bending cycles under a 3 mm bending radius.

11.
Chem Soc Rev ; 52(11): 3627-3662, 2023 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-37158259

RESUMO

The selective methanation of CO2 is an important research area to meet the net-zero emission targets. Furthermore, it is crucial to develop solutions to achieve carbon neutrality, hydrogen utilization, carbon circularity, and chemical-energy storage. This conversion can be realized via the thermocatalytic multistep power-to-X route or by direct electro- (or photoelectro)-catalytic technologies. Herein, we discuss the need to accelerate direct technologies. Improving these technologies requires a better understanding of the catalytic chemistry and the complexity of the aspects to consider in bridging catalytic and electrocatalytic CO2 methanation. In this tutorial review, initially we analyze the fundamental question of the competitive adsorption of key reactants and regulation strategies to promote the overall reaction. Then, this approach is used to guide the reader in understanding the differences between thermocatalysis and electrocatalysis. Finally, the complexity of the aspects necessary to include in modelling and designing next-generation electrocatalysts for CO2 methanation is analyzed.

12.
Chemistry ; 29(42): e202301036, 2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37150751

RESUMO

Hydrogen peroxide (H2 O2 ) electrosynthesis via the 2e- Oxygen Reduction Reaction (ORR) represents a highly challenging, environmentally friendly and cost-effective alternative to the current anthraquinone-based technology. Various lightweight element hetero-doped carbon nanostructures are promising and cheap metal-free electrocatalysts for H2 O2 synthesis, particularly those containing O-functionalities. The exact role of O-containing functional groups as electroactive sites for the process remains debated if not highly controversial. Herein, we have reported on the covalent exohedral functionalization of the outer surface of extra-pure multi-walled carbon nanotubes (MWCNTs) with discrete O-functional groups as a unique approach to prepare selective electrocatalysts for the process. This kind of decoration has added fundamental tiles to the puzzling structure/reactivity relationship of O-containing carbon-based catalysts for ORR, clearing doubts on the controversial role of hydroxyl/phenol groups as key functionalities for the design of more performing 2e- ORR electrocatalysts.

13.
Opt Express ; 31(9): 14796-14807, 2023 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-37157336

RESUMO

Femtosecond laser-induced deep-subwavelength structures have attracted much attention as a nanoscale surface texturization technique. A better understanding of the formation conditions and period control is required. Herein, we report a method of non-reciprocal writing via a tailored optical far-field exposure, where the period of ripples varies along different scanning directions, and achieve a continuous manipulation of the period from 47 to 112 nm (±4 nm) for a 100-nm-thick indium tin oxide (ITO) on glass. A full electromagnetic model was developed to demonstrate the redistributed localized near-field at different stages of ablation with nanoscale precision. It explains the formation of ripples and the asymmetry of the focal spot determines the non-reciprocity of ripple writing. Combined with beam shaping techniques, we achieved non-reciprocal writing (regarding scanning direction) using an aperture-shaped beam. The non-reciprocal writing is expected to open new paths for precise and controllable nanoscale surface texturing.

14.
J Colloid Interface Sci ; 646: 922-931, 2023 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-37235937

RESUMO

Recently, quasi two-dimensional (Q-2D) perovskites with alternating cations in the interlayer space (ACI) have attracted more attentions owing to their elevated stability compared with three-dimensional (3D) analogs. While the efficiency of the devices derived from Q-2D perovskites is much smaller than that based on 3D perovskites. Here, we utilized urea and methoxyamine hydrochloride (MOAH) dual additives to acquire high quality Q-2D ACI perovskite GA(MA)5Pb5I16 (GA = guanidinium, MA = methylammonium) films. The efficiency of the perovskite solar cells (PSCs) derived from the Q-2D perovskite films induced by the synergistic effect of urea and MOAH dual additives increases to 20.32% from 17.21% for the devices without additive. This efficiency enhancement could be attributed to the enlarged grain size, improved crystallinity, optimized quantum well thickness distribution, and reduced trap states of the perovskite films. Moreover, the solar cells with dual additives present improved stability. The efficiency of devices with dual additives holds 95% of the original value after storage for 1600 h in ambient air. These results prove that the synergistic effect of urea and MOAH is an effective method to achieve highly efficient and stable Q-2D PSCs.

15.
Nano Lett ; 23(9): 3769-3774, 2023 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-37129232

RESUMO

High-resolution patterning of perovskite quantum dots (PQDs) is of significant importance for satisfying various practical applications, including high-resolution displays and image sensing. However, due to the limitation of the instability of PQDs, the existing patterning strategy always involves chemical reagent treatment or mask contact that is not suitable for PQDs. Therefore, it is still a challenge to fabricate high-resolution full-color PQD arrays. Here, we present a femtosecond laser-induced forward transfer (FsLIFT) technology, which enables the programmable fabrication of high-resolution full-color PQD arrays and arbitrary micropatterns. The FsLIFT process integrates transfer, deposition, patterning, and alignment in one step without involving a mask and chemical reagent treatment, guaranteeing the preservation of the photophysical properties of PQDs. A full-color PQD array with a high resolution of 2 µm has been successfully achieved. We anticipate that our facile and flexible FsLIFT technology can facilitate the development of diverse practical applications based on patterned PQDs.

16.
Nanoscale ; 15(11): 5494-5498, 2023 Mar 16.
Artigo em Inglês | MEDLINE | ID: mdl-36853238

RESUMO

Patterned quantum dots (QDs) and perovskites have attracted a great deal of attention in the fabrication of optoelectronic device arrays for transistors, image sensors and displays. However, the resolution of current patterning technologies is insufficient for nanopatterned QDs and perovskites to be integrated in advanced optoelectronic and photonic applications. Herein, we demonstrate a femtosecond laser regulatory focus ablation (FsLRFA) patterning technique of a fluorescent film involving both semiconductor core-shell QDs and perovskite up to 1/10th of the scale of the diffraction limit. Annular lines with a 200 nm-width are obtained after the irradiation of the femtosecond laser. Moreover, the combination of ablated different geometries enables the laser focal spot as brushes for FsLRFA patterning technology to fabricate delicate and programmable patterns on the fluorescent film. This technology with nanoscale resolution and patterning capability paves the road toward highly integrated applications based on QDs and perovskites.

17.
Chemphyschem ; 24(9): e202200860, 2023 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-36782095

RESUMO

Halide perovskites are emerging emitters with excellent optoelectronic properties. Contrary to the large grain fabrication goal in perovskite solar cells, perovskite light-emitting diodes (PeLEDs) based on small grain enable efficient radiative recombination because of relatively higher charge carrier densities due to spatial confinement. However, achieving small-sized grain growth with superior crystal quality and film morphology remains a challenge. In this work, we demonstrated a nanostructured stamp thermal imprinting strategy to boost the surface coverage and improve the crystalline quality of CsPbBr3 film, particularly confine the grain size, leading to the improvement of luminance and efficiency of PeLEDs. We improved the thermal imprinting process utilizing the nanostructured stamp to selectively manipulate the nucleation and growth in the nanoscale region and acquire small-sized grain accompanied by improved crystal quality and surface morphology of the film. By optimizing the imprinting pressure and the period of the nanostructures, appropriate grain size, high surface coverage, small surface roughness and improved crystallization could be achieved synchronously. Finally, the maximum luminance and efficiency of PeLEDs achieved by nanostructured stamp imprinting with a period of 320 nm are 67600 cd/m2 and 16.36 cd/A, respectively. This corresponds to improvements of 123 % in luminance and 100 % in efficiency, compared to that of PeLEDs without the imprinting.

18.
ACS Appl Mater Interfaces ; 15(8): 10986-10993, 2023 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-36692254

RESUMO

Femtosecond laser ablation (FsLA) technology has been demonstrated to achieve programmable ablation and removal of diverse materials with high precision. Owing to the cross-scale and digital processing characteristics, the FsLA technology has attracted increasing interest. However, the moderate repeatability of FsLA limits its application in the fabrication of advanced micro-/nanostructures due to the nonidentity of each laser pulse and fluctuation of environment. Fortunately, moderate repeatability combined with programmable ablation and high precision perfectly matches with the technical requirements of a physical unclonable fluorescent anticounterfeiting label. Herein, we applied FsLA to quantum dot (QD) films to fabricate a physical unclonable multilevel fluorescent anticounterfeiting label. Visual Jilin University logos, quick response (QR) codes, microlines, and microholes have been achieved for the multilevel anticounterfeiting functions. Of particular significance, the microholes with a macroidentical and microidentifiable geometry guarantee the physical unclonable functions (PUFs). Moreover, the fluorescent anticounterfeiting label is compatible with deep learning algorithms that facilitate authentication to be convenient and accurate. This work shows a fantastic future potential to be a core anticounterfeiting technique for commercial products and drugs.

19.
Small ; 19(6): e2205758, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36461724

RESUMO

To develop a non-precious highly efficient cocatalyst to replace Pt on graphitic carbon nitride (g-C3 N4 ) for solar H2 production is great significant, but still remains a huge challenge. The emerging single-atom catalyst presents a promising strategy for developing highly efficient non-precious cocatalyst owing to its unique adjustability of local coordination environment and electronic structure. Herein, this work presents a facile approach to achieve single Ni sites (Ni1 -N2 S) with unique local coordination structure featuring one Ni atom coordinated with two nitrogen atoms and one sulfur atom, confirmed by high-angle annular dark-field scanning transmission electron microscopy, X-ray absorption spectroscopy, and density functional theory calculation. Thanks to the unique electron structure of Ni1 -N2 S sites, the 1095 µmol g-1 h-1 of high H2 evolution rate with 4.1% of apparent quantum yield at 420 nm are achieved. This work paves a pathway for designing a highly efficient non-precious transition metal cocatalyst for photocatalytic H2 evolution.

20.
Opt Lett ; 47(24): 6440-6443, 2022 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-36538457

RESUMO

Harvesting light by metallic structures with sharp corners, or the so-called photonic singularities, has exhibit their potential in nanophotonics, sensing, and bio-medical applications. The high-quality light confinement of the light energy mainly relies on the precise preparation of nanoscale photonic singularities. However, the realization of massive photonic singularities still meets the challenges on integration and low-cost mask multiplexing. Here, we show an angle-dependent elevated nanosphere lithography to achieve massive photonic singularities for spatially modulated light harvesting at the near-infrared regime. The photonic geometrical singularity is constructed by the gold crescent array of plasmonic materials. The numerical simulation shows that the light can be localized at the spatially distributed singularities. This phenomenon is verified experimentally through the infrared spectral measurement. Our work provides the possibility to produce integrated light-harvesting devices for numerous optical applications in illumination, display, and enhanced nonlinear excitation.


Assuntos
Ouro , Fótons , Ouro/química , Óptica e Fotônica
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