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1.
ACS Nano ; 18(34): 23205-23216, 2024 Aug 27.
Artículo en Inglés | MEDLINE | ID: mdl-39146530

RESUMEN

Achieving selective sensing toward target volatile organic compound gases is of vital importance in the fields of air quality assessment, food freshness evaluation, and diagnosis of patients via exhaled breath. However, chemiresistive sensors that exhibit specificity like biological enzymes in a complex environment are rare. Herein, we developed a strategy of optimizing oxygen vacancy structures in tin oxides to induce specific catalysis, activating 100% selective sensing toward amine gases at room temperature. In situ technologies and theoretical calculations reveal that the "donor-receptor" coordination between nitrogen atoms from amine molecules and bridging oxygen vacancies (OVBri)-induced electron-deficient center is the essence of specific catalysis and provides the bridge from the surface oxidation reaction to electrophysical characteristics evolution, which allows the sensor to exhibit amine-specific sensing behavior, even in gas mixtures. Moreover, OVBri enhances the selectivity by enabling a room-temperature sensing pathway where lattice oxygens participate in catalytic oxidation for amine molecules, resulting in record-high sensing values: 19,938.92 toward 100 ppm of triethylamine, 15,236.78 toward trimethylamine, and 123.41 toward diethylamine. Our findings illustrate the feasibility of designing specific active sites through defect engineering and can contribute to the advancement of highly selective sensors based on catalytic processes.

2.
ACS Appl Mater Interfaces ; 16(31): 41616-41625, 2024 Aug 07.
Artículo en Inglés | MEDLINE | ID: mdl-39052931

RESUMEN

Cu2O, CuO, and mixed phase Cu2O/CuO represent promising candidates for photoelectrochemical H2 evolution due to their strong visible light absorption, earth-abundance, and chemical stability. However, the photoelectrochemical efficiency in these materials remains far below the theoretical limit, largely due to poorly understood surface electron dynamics. These dynamics depend on defect states, such as Cu atom vacancies and phase boundaries, which control electron trapping, charge carrier separation, and recombination. In this work, we study the photoinduced electron and hole dynamics at the surface of various Cu oxides using ultrafast extreme ultraviolet reflection-absorption (XUV-RA) spectroscopy. In Cu2O we find that photoexcitation occurs as electron promotion from primarily Cu 3d valence band to Cu 4s conduction band states compared to O 2p valence band to Cu 4s conduction band states in CuO. In catalysts with a significant concentration of Cu vacancies, we observe fast electron trapping to the Cu 3d defect band occurring in less than 100 fs. In contrast, photoexcited electrons in phase pure CuO do not trap to midgap states; rather these electrons form small polarons within approximately 500 fs. Photoelectrochemical measurements of these catalysts show that Cu vacancy-mediated electron trapping correlates with a significant loss of photocurrent. Together, these results provide a detailed picture of the defect states and associated ultrafast carrier dynamics that govern the photocatalytic efficiency in widely studied Cu2O and CuO photocatalysts.

3.
Environ Res ; 258: 119480, 2024 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-38909948

RESUMEN

In this study, g-C3N4/PANI was prepared by in situ oxidative polymerization. Graphite-phase carbon nitride (g-C3N4) with surface defects was deposited onto the surface of conductive polyaniline (PANI) to form a p-n heterojunction. This construction aimed to create an efficient heterogeneous catalyst, increasing the surface defect level and active sites of the composite, and augmenting its capability to capture and transfer extracellular electrons under anaerobic conditions. This addresses the challenge of low efficiency in direct interspecies electron transfer between bacteria and archaea during anaerobic digestion for methane production. The results showed that the prepared g-C3N4/PANI increased the CH4 yield and CH4 production rate by 82% and 96%, respectively. Notably, the conductivity and XPS test results showed that the ratio of g-C3N4 to PANI was 0.15, and the composite exhibited favorable conductivity, with a uniform distribution of pyrrolic nitrogen, pyridinic nitrogen, and graphitic nitrogen, each accounting for approximately 30%. Furthermore, g-C3N4/PANI effectively enhanced the metabolic efficiency of intermediate products such as acetate and butyrate. Analysis of the microbial community structure revealed that g-C3N4/PANI led to a significant increase in the abundance of hydrogenotrophic methanogen Methanolinea (from 48% to 64%) and enriched Clostridium (a rise of 1%) with direct interspecies electron transfer capability. Microbial community function analysis demonstrated that the addition of g-C3N4/PANI boosted the activities of key enzymes involved in anaerobic digestion, including phosphate transacetylase (PTA), phospho-butyryl transferase (PTB), and NAD-independent lactate dehydrogenase (NNLD), by 47%, 135%, and 153%, respectively. This acceleration in enzymatic activity promoted the metabolism of acetyl-CoA, butyryl-CoA, and pyruvate. Additionally, the function of ABC transporters was enhanced, thereby improving the efficiency of material and energy exchange among microorganisms.


Asunto(s)
Compuestos de Anilina , Metano , Compuestos de Anilina/química , Compuestos de Anilina/metabolismo , Anaerobiosis , Metano/metabolismo , Eliminación de Residuos Líquidos/métodos , Aguas Residuales/química , Grafito/química , Nitrilos/metabolismo , Nitrilos/química
4.
J Imaging ; 10(6)2024 Jun 13.
Artículo en Inglés | MEDLINE | ID: mdl-38921621

RESUMEN

Thanks to the line-scanning camera, the measurement method based on line-scanning stereo vision has high optical accuracy, data transmission efficiency, and a wide field of vision. It is more suitable for continuous operation and high-speed transmission of industrial product detection sites. However, the one-dimensional imaging characteristics of the line-scanning camera cause motion distortion during image data acquisition, which directly affects the accuracy of detection. Effectively reducing the influence of motion distortion is the primary problem to ensure detection accuracy. To obtain the two-dimensional color image and three-dimensional contour data of the heavy rail surface at the same time, a binocular color line-scanning stereo vision system is designed to collect the heavy rail surface data combined with the bright field illumination of the symmetrical linear light source. Aiming at the image motion distortion caused by system installation error and collaborative acquisition frame rate mismatch, this paper uses the checkerboard target and two-step cubature Kalman filter algorithm to solve the nonlinear parameters in the motion distortion model, estimate the real motion, and correct the image information. The experiments show that the accuracy of the data contained in the image is improved by 57.3% after correction.

5.
Small ; 20(34): e2401669, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38573947

RESUMEN

The anti-solvent-free fabrication of high-efficiency perovskite solar cells (PSCs) holds immense significance for the transition from laboratory-scale to large-scale commercial applications. However, the device performance is severely hindered by the increased occurrence of surface defects resulting from the lack of control over nucleation and crystallization of perovskite using anti-solvent methods. In this study, 2-(naphthalen-2-yl)ethylamine hydriodide (NEAI) is employed as the surface passivator for perovskite films without using any anti-solvent. Naphthalene demonstrates strong π-π conjugation, which aids in the efficient extraction of charge carriers. Additionally, the naphthalene-ring moieties form a tight attachment to the perovskite surface. After NEAI treatment, FA and I vacancies are selectively occupied by NEA+ and I- in NEAI respectively, thus effectively passivating the surface defects and isolating the surface from moisture. Ultimately, the optimized NEAI-treated device achieves a promising power conversion efficiency (PCE) of 24.19% (with a certified efficiency of 23.94%), featuring a high fill factor of 83.53%. It stands out as one of the reported high PCEs achieved for PSCs using the spin-coating technique without the need for any anti-solvent so far. Furthermore, the NEAI-treated device can maintain ≈87% of its initial PCE after 2000 h in ambient air with a relative humidity of 30% ± 5%.

6.
Macromol Rapid Commun ; 45(14): e2400049, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38685191

RESUMEN

Hydrogels are usually depicted as a homogenous polymer block with a distinct surface. While defects in the polymer structure are looked into frequently, structural irregularities on the hydrogel surface are often neglected. In this work, thin hydrogel layers of ≈100 nm thickness (nanogels) are synthesized and characterized for their structural irregularities, as they represent the surface of macrogels. The nanogels contain a main-chain responsiveness (thermo responsive) and a responsiveness in the cross-linking points (redox responsive). By combining data from ellipsometry using box-model and two-segment-model analysis, as well as atomic force microscopy, a more defined model of the nanogel surface can be developed. Starting with a more densely cross-linked network at the silica wafer surface, the density of cross-linking gradually decreases toward the hydrogel-solvent interface. Thermo-responsive behavior of the main chain affects the entire network equally as all chain segments change solubility. Cross-linker-based redox-responsiveness, on the other hand, is only governed by the inner, more cross-linked layers of the network. Such dual responsive nanogels hence allow for developing a more detailed model of a hydrogel surface from free radical polymerization. It provides a better understanding of structural defects in hydrogels and how they are affected by responsive functionalities.


Asunto(s)
Nanogeles , Oxidación-Reducción , Propiedades de Superficie , Nanogeles/química , Hidrogeles/química , Temperatura , Polietilenglicoles/química , Tamaño de la Partícula , Polietileneimina/química , Microscopía de Fuerza Atómica
7.
Nano Lett ; 24(12): 3719-3726, 2024 Mar 27.
Artículo en Inglés | MEDLINE | ID: mdl-38484387

RESUMEN

Mixed-halide CsPb(Br/I)3 perovskite quantum dots (QDs) are regarded as one of the most promising candidates for pure-red perovskite light-emitting diodes (PeLEDs) due to their precise spectral tuning property. However, the lead-rich surface of these QDs usually results in halide ion migration and nonradiative recombination loss, which remains a great challenge for high-performance PeLEDs. To solve the above issues, we employ a chelating agent of 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid hydrate (DOTA) to polish the lead-rich surface of the QDs and meanwhile introduce a new ligand of 2,3-dimercaptosuccinic acid (DMSA) to passivate surface defects of the QDs. This synchronous post-treatment strategy results in high-quality CsPb(Br/I)3 QDs with suppressed halide ion migration and an improved photoluminescence quantum yield, which enables us to fabricate spectrally stable pure-red PeLEDs with a peak external quantum efficiency of 23.2%, representing one of the best performance pure-red PeLEDs based on mixed-halide CsPb(Br/I)3 QDs reported to date.

8.
ACS Appl Mater Interfaces ; 16(11): 14263-14274, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38441548

RESUMEN

The dynamic defect tolerance under light soaking is a crucial aspect of halide perovskites. However, the underlying physics of light soaking remains elusive and is subject to debate, exhibiting both positive and negative effects. In this investigation, we demonstrated that surface defects in perovskite films significantly impact the performance and stability of perovskite solar cells, closely correlated with light soaking behaviors. Removing the top surface layer through adhesive tape, the surface defect density noticeably decreases, leading to enhanced photoluminescence (PL) efficiency, prolonged carrier lifetime, and higher conductivity. Consequently, the power conversion efficiency (PCE) of solar cells improves from 17.70% to 20.5%. Furthermore, we confirmed a positive correlation between surface defects and the light soaking effect. Perovskite films with low surface defects surprisingly exhibit a 3-fold increase in PL intensity and an 85% increase in carrier lifetime under 500 s of continuous illumination at an intensity of 100 mW/cm2. Beyond the conventional strategy of suppressing defect trapping, we propose increasing the capability of dynamic defect tolerance as an effective strategy to enhance the optoelectronic properties and performance of perovskite solar cells.

9.
J Colloid Interface Sci ; 663: 541-553, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38428112

RESUMEN

The CO oxidation catalytic activity of catalysts is strongly influenced by the oxygen vacancy defects (OVDs) concentration and the valence state of active metal. Herein, a defect engineering approach was implemented to enhance the oxygen vacancy defects and to modify the valence of metal ions in manganese oxide octahedral molecular sieves (OMS-2) by the introduction of copper (Cu). The characterization and theoretical calculation results reveal that the incorporation of Cu2+ ion into the OMS-2 structure led to a rise in specific surface area and pore volume, weakening of Mn-O bonds, higher proportion of the low-coordinated oxygen species adsorbed in oxygen vacancies (Oads) and an increase in the average oxidation state of manganese. These structural modifications were discovered to considerably reduce the apparent activation energy (Ea), thus ultimately significantly enhancing the CO oxidation activity (T99 at 148 ℃at GHSV = 13,200 h-1) than the original OMS-2 (T99 = 215 ℃ at GHSV = 13,200 h-1). Furthermore, In-situ diffuse reflectance infrared Fourier transform (DRIFT) and In-situ near-ambient pressure X-ray photoelectron spectroscopy (in situ NAP-XPS) results indicate that the bimetallic synergy enhanced by doping strategy accelerates the conversion of oxygen to chemisorbed oxygen species and the reaction rate of CO oxidation through Mn3++Cu2+↔Mn4++Cu+ redox cycle. The findings of this study offer novel perspectives on the design of catalysts with exceptional performance in CO oxidation.

10.
Environ Pollut ; 346: 123591, 2024 Apr 01.
Artículo en Inglés | MEDLINE | ID: mdl-38367696

RESUMEN

This study developed an efficient and stable landfill leachate treatment process, which was based on the combination of biochar catalytic ozonation and activated sludge technology for intensive treatment of landfill leachate, aiming to achieve the standard discharge of leachate. The focus is to investigate the effect of manganese loading on the physicochemical properties of biochar and the mechanism of its catalytic ozonation. It was found that more surface functional groups (CO, Mn-O, etc.) and defects (ID/IG = 1.27) were exposed via the change of original carbon structure by loading Mn, which is conducive to the generation of lattice oxygen. Meanwhile, generating different valence states of Mn metal can improve the redox properties and electron migration rate, and encourage the production of reactive oxygen species (ROS) during the reaction process and enhance the catalytic efficiency. The synergistic action of microorganisms, especially denitrifying bacteria, was found to play a key role in the degradation of nitrogenous pollutants during the activated sludge process. The concentration of NH+4-N was reduced from the initial 1087.03 ± 9.56 mg/L to 9.05 ± 1.91 mg/L, while COD was reduced from 2290 ± 14.14 mg/L to 86.5 ± 2.12 mg/L, with corresponding removal rates of 99.17% and 99.20%, respectively. This method offers high efficiency and stability, achieving discharge standards for leachate (GB16889-2008). The synergy between Mn-loaded biochar and microorganisms in the activated sludge is key to effective treatment. This study offers a new approach to solving the challenge of waste leachate treatment.


Asunto(s)
Carbón Orgánico , Ozono , Contaminantes Químicos del Agua , Ozono/química , Manganeso , Contaminantes Químicos del Agua/química , Aguas del Alcantarillado
11.
ACS Appl Mater Interfaces ; 16(9): 11694-11703, 2024 Mar 06.
Artículo en Inglés | MEDLINE | ID: mdl-38387044

RESUMEN

Recently, photodetectors based on perovskite nanoplatelets (NPLs) have attracted considerable attention in the visible spectral region owing to their large absorption cross-section, high exciton binding energy, excellent charge transfer properties, and appropriate flexibility. However, their stability and performance are still challenging for perovskite NPL photodetectors. Here, a surface engineering strategy to enhance the optical stability of blue-light CsPbBr3 NPLs by acetylenedicarboxylic acid (ATDA) treatment has been developed. ATDA has strong binding capacity and a short chain length, which can effectively passivate defects and significantly improve the photoluminescence quantum efficiency, stability, and carrier mobility of NPLs. As a result, ATDA-treated CsPbBr3 NPLs exhibit improved optical properties in both solutions and films. The NPL solution maintains high PL performance even after being heated at 80 °C for 2 h, and the NPL film remains nondegradable after 4 h of exposure to ultraviolet irradiation. Especially, photodetectors based on the treated CsPbBr3 NPL films demonstrate exceptional performance, especially when the detectivity approaches up to 9.36 × 1012 Jones, which can be comparable to the best CsPbBr3 NPL photodetectors ever reported. More importantly, the assembled devices demonstrated high stability (stored in an air environment for more than 30 days), significantly exceeding that of untreated NPLs.

12.
Small ; 20(24): e2311362, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38192000

RESUMEN

For p-i-n perovskite solar cells (PSCs), nickel oxide (NiOx) hole transport layers (HTLs) are the preferred interfacial layer due to their low cost, high mobility, high transmittance, and stability. However, the redox reaction between the Ni≥3+ and hydroxyl groups in the NiOx and perovskite layer leads to oxidized CH3NH3 + and reacts with PbI in the perovskite, resulting in a large number of non-radiative recombination sites. Among various transition metals, an ultra-thin zinc nitride (Zn3N2) layer on the NiOx surface is chosen to prevent these redox reactions and interfacial issues using a simple solution process at low temperatures. The redox reaction and non-radiative recombination at the interface of the perovskite and NiOx reduce chemically by using interface modifier Zn3N2 to reduce hydroxyl group and defects on the surface of NiOx. A thin layer of Zn3N2 at the NiOx/perovskite interface results in a high Ni3+/Ni2+ ratio and a significant work function (WF), which inhibits the redox reaction and provides a highly aligned energy level with perovskite crystal and rigorous trap-passivation ability. Consequently, Zn3N2-modified NiOx-based PSCs achieve a champion PCE of 21.61%, over the NiOx-based PSCs. After Zn3N2 modification, the PSC can improve stability under several conditions.

13.
ACS Appl Mater Interfaces ; 16(4): 4958-4974, 2024 Jan 31.
Artículo en Inglés | MEDLINE | ID: mdl-38241089

RESUMEN

For years, solution-type electrochromic devices (ECDs) have intrigued researchers' interest and eventually rendered themselves into commercialization. Regrettably, challenges such as electrolyte leakage, high flammability, and complicated edge-encapsulation processes limit their practical utilization, hence necessitating an efficient alternate. In this quest, although the concept of solid/gel-polymer electrolyte (SPE/GPE)-based ECDs settled some issues of solution-type ECDs, an array of problems like high operating voltage, sluggish response time, and poor cycling stability have paralyzed their commercial applicability. Herein, we demonstrate a choreographed-CeO2-nanofiller-doped GPE-based ECD outperforming its solution-type counterpart in all merits. The filler-incorporated polymer electrolyte assembly was meticulously weaved through the electrospinning method, and the resultant host was employed for immobilizing electrochromic viologen species. The filler engineering benefits conceived through the tuned shape of CeO2 nanorod and quantum dots, along with the excellent redox shuttling effect of Ce3+/Ce4+, synchronously yielded an outstanding class of GPE, which upon utilization in ECDs delivered impressive electrochromic properties. A combination of features possessed by a particular device (QD-NR/PVDF-HFP/IL/BzV-Fc ECD) such as exceptionally low driving voltage (0.9 V), high transmittance change (ΔT, ∼69%), fast response time (∼1.8 s), high coloration efficiency (∼339 cm2/C), and remarkable cycling stability (∼90% ΔT-retention after 25,000 cycles) showcased a striking potential in the yet-to-realize market of GPE-based ECDs. This study unveils the untapped potential of choreographed nanofillers that can promisingly drive GPE-based ECDs to the doorstep of commercialization.

14.
J Food Prot ; 87(2): 100213, 2024 02.
Artículo en Inglés | MEDLINE | ID: mdl-38176613

RESUMEN

Food-contact surfaces showing signs of wear pose a substantial risk of Listeria monocytogenes contamination and may serve as persistent sources of cross-contamination in fresh produce packinghouses. This study offers a comprehensive exploration into the influence of surface defects on the efficacies of commonly used sanitizers against L. monocytogenes biofilms on major food-contact surfaces. The 7-day-old L. monocytogenes biofilms were cultivated on food-contact surfaces, including stainless steel, polyvinyl chloride, polyester, low-density polyethylene, and rubber, with and without defects and organic matter. Biofilms on those surfaces were subjected to treatments of 200 ppm chlorine, 400 ppm quaternary ammonium compound (QAC), or 160 ppm peroxyacetic acid (PAA). Results showed that surface defects significantly (P < 0.05) increased the population of L. monocytogenes in biofilms on non-stainless steel surfaces and compromised the efficacies of sanitizers against L. monocytogenes biofilms across various surface types. A 5-min treatment of 200 ppm chlorine caused 1.84-3.39 log10 CFU/coupon reductions of L. monocytogenes on worn surfaces, compared to 2.79-3.93 log10 CFU/coupon reduction observed on new surfaces. Similarly, a 5-min treatment with 400 ppm QAC caused 2.05-2.88 log10 CFU/coupon reductions on worn surfaces, compared to 2.51-3.66 log10 CFU/coupon reductions on new surfaces. Interestingly, PAA sanitization (160 ppm, 1 min) exhibited less susceptibility to surface defects, leading to 3.41-4.35 log10 CFU/coupon reductions on worn surfaces, in contrast to 3.68-4.64 log10 CFU/coupon reductions on new surfaces. Furthermore, apple juice soiling diminished the efficacy of sanitizers against L. monocytogenes biofilms on worn surfaces (P < 0.05). These findings underscore the critical importance of diligent equipment maintenance and thorough cleaning processes to effectively eliminate L. monocytogenes contamination on food-contact surfaces.


Asunto(s)
Listeria monocytogenes , Árboles , Contaminación de Alimentos/prevención & control , Contaminación de Alimentos/análisis , Frutas/química , Cloro , Recuento de Colonia Microbiana , Biopelículas , Ácido Peracético/farmacología , Microbiología de Alimentos , Acero Inoxidable/análisis
15.
Connect Tissue Res ; 65(1): 26-40, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37898909

RESUMEN

PURPOSE/AIM: Cartilage injury and subsequent osteoarthritis (OA) are debilitating conditions affecting millions worldwide. As there are no cures for these ailments, novel therapies are needed to suppress disease pathogenesis. Given that joint injuries are known to produce damage-associated molecular patterns (DAMPs), our central premise is that the Toll-like receptor 4 (TLR4) pathway is a principal driver in the early response to cartilage damage and subsequent pathology. We postulate that TLR4 activation is initiated/perpetuated by DAMPs released following joint damage. Thus, antagonism of the TLR4 pathway immediately after injury may suppress the development of joint surface defects. MATERIALS AND METHODS: Two groups were utilized: (1) 8-week-old, male C57BL6 mice treated systemically with a known TLR4 antagonist and (2) mice injected with vehicle control. A full-depth cartilage lesion on the midline of the patellofemoral groove was created in the right knee of each mouse. The left knee was used as a sham surgery control. Gait changes were evaluated over 4 weeks using a quantitative gait analysis system. At harvest, knee joints were processed for pathologic assessment, Nanostring® transcript expression, and immunohistochemistry (IHC). RESULTS: Short-term treatment with a TLR4 antagonist at 14-days significantly improved relevant gait parameters; improved cartilage metrics and modified Mankin scores were also seen. Additionally, mRNA expression and IHC showed reduced expression of inflammatory mediators in animals treated with the TLR4 antagonist. CONCLUSIONS: Collectively, this work demonstrates that systemic treatment with a TLR4 antagonist is protective to further cartilage damage 14-days post-injury in a murine model of induced disease.


Asunto(s)
Enfermedades de los Cartílagos , Cartílago Articular , Osteoartritis de la Rodilla , Osteoartritis , Ratones , Masculino , Animales , Receptor Toll-Like 4 , Modelos Animales de Enfermedad , Ratones Endogámicos C57BL , Osteoartritis/patología , Cartílago/patología , Enfermedades de los Cartílagos/patología , Cartílago Articular/patología , Osteoartritis de la Rodilla/patología
16.
Discov Nano ; 18(1): 147, 2023 Dec 04.
Artículo en Inglés | MEDLINE | ID: mdl-38047970

RESUMEN

MnOx-based nanomaterials are promising large-scale electrochemical energy storage devices due to their high specific capacity, low toxicity, and low cost. However, their slow diffusion kinetics is still challenging, restricting practical applications. Here, a one-pot and straightforward method was reported to produce Zn-doped MnOx nanowires with abundant defects and tunable small cross-sections, exhibiting an outstanding specific capacitance. More specifically, based on a facile hydrothermal strategy, zinc sites could be uniformly dispersed in the α-MnOx nanowires structure as a function of composition (0.3, 2.1, 4.3, and 7.6 wt.% Zn). Such a process avoided the formation of different crystalline phases during the synthesis. The reproducible method afforded uniform nanowires, in which the size of cross-sections decreased with the increase of Zn composition. Surprisingly, we found a volcano-type relationship between the storage performance and the Zn loading. In this case, we demonstrated that the highest performance material could be achieved by incorporating 2.1 wt.% Zn, exhibiting a remarkable specific capacitance of 1082.2 F.g-1 at a charge/discharge current density of 1.0 A g-1 in a 2.0 mol L-1 KOH electrolyte. The optimized material also afforded improved results for hybrid supercapacitors. Thus, the results presented herein shed new insights into preparing defective and controlled nanomaterials by a simple one-step method for energy storage applications.

17.
ACS Appl Mater Interfaces ; 15(50): 59005-59015, 2023 Dec 20.
Artículo en Inglés | MEDLINE | ID: mdl-38055857

RESUMEN

The fluorination of the aromatic multifunctional Lewis base passivation strategy has been demonstrated recently as an effective approach to markedly enhance the performance of perovskite photovoltaic devices. However, the regulation mechanisms of the passivation efficiency by varying the functional group position of fluorine (F) in the regioisomers have received little attention and inadequate research. Herein, a pair of bifluorine-substituted aminobenzoic acid regioisomers [3-amino-2,6-difluorobenzoic acid (13-FABA) and 4-amino-3,5-difluorobenzoic acid (14-FABA)] were employed to investigate the passivation effects of Lewis bases dependent on behaviors of the ortho/meta-substituted position of fluorine. The density functional theory calculation on electron cloud density, interaction energy, and the basicity of Lewis bases combined with experimental evidence reveal that the ortho-effect induced by fluorine substitution weakens the passivating effect of 13-FABA Lewis base and induces its molecular propensity to form internal salts, accelerating the degradation and deterioration of the device performance. Conversely, 14-FABA with meta-connected fluorine atoms exhibit superior efficacy in suppressing defects and enhancing hydrophobicity. Eventually, the 14-FABA-modified photodetectors (PDs) achieved a high detectivity of 1.69 × 1013 Jones, the comparatively lower dark current density of 2.2 × 10-10 A/cm2 among all-inorganic perovskite PD systems. Our work has not only clarified the fundamental mechanisms of the F-substituted position effects of Lewis base on suppressing defects but also provided a promising passivation strategy for perovskite films via designing the regioisomeric atoms in a multifunctional Lewis base molecule.

18.
Biomimetics (Basel) ; 8(8)2023 Dec 12.
Artículo en Inglés | MEDLINE | ID: mdl-38132537

RESUMEN

The robustness of superhydrophobic objects conflicts with both the inevitable introduction of fragile micro/nanoscale surfaces and three-dimensional (3D) complex structures. The popular metal 3D printing technology can manufacture robust metal 3D complex components, but the hydrophily and mass surface defects restrict its diverse application. Herein, we proposed a strategy that takes the inherent ridges and grooves' surface defects from laser powder bed fusion additive manufacturing (LPBF-AM), a metal 3D printing process, as storage spaces for hydrophobic silica (HS) nanoparticles to obtain superhydrophobic capacity and superior robustness. The HS nanoparticles stored in the grooves among the laser-melted tracks serve as the hydrophobic guests, while the ridges' metal network provides the mechanical strength, leading to robust superhydrophobic objects with desired 3D structures. Moreover, HS nanoparticles coated on the LPBF-AM-printed surface can inhibit corrosion behavior caused by surface defects. It was found that LPBF-AM-printed objects with HS nanoparticles retained superior hydrophobicity after 150 abrasion cycles (~12.5 KPa) or 50 cycles (~37.5 KPa). Furthermore, LPBF-AM-printed ships with superhydrophobic coating maintained great water repellency even after 10,000 cycles of seawater swashing, preventing dynamic corrosion upon surfaces. Our proposed strategy, therefore, provides a low-cost, highly efficient, and robust superhydrophobic coating, which is applicable to metal 3D architectures toward corrosion-resistant requirements.

19.
Chempluschem ; 88(10): e202300367, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37724441

RESUMEN

Solution processed perovskite films usually exhibit numerous defect states on the surfaces of the films. Here in this work, oxalic acid (H2 C2 O4 ), which has two C=O groups, is selected and used to passivate the surface defects of the two-step deposited perovskite films via post-treatment. Strong interaction between H2 C2 O4 molecule and the Pb2+ ions located on the surface of perovskite film has been confirmed via Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy, which can result in an effective suppress of the surface defects. Furthermore, time-resolved PL spectrum indicates that carrier lifetime is prolonged in the H2 C2 O4 passivated perovskite film. After optimizing the H2 C2 O4 concentration, the target perovskite solar cells can demonstrate superior power conversion efficiencies (21.67 % from reverse measurement and 21.54 % from forward measurement) and superior device-stability.

20.
Sensors (Basel) ; 23(16)2023 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-37631650

RESUMEN

The surface defects on a shield subway tunnel can significantly affect the serviceability of the tunnel structure and may compromise operation safety. To effectively detect multiple surface defects, this study uses a tunnel inspection trolley (TIT) based on the mobile laser scanning technique. By conducting an inspection of the shield tunnel on a metro line section, various surface defects are identified with the TIT, including water leakage defects, dislocation, spalling, cross-section deformation, etc. To explore the root causes of the surface defects, association rules between different defects are calculated using an improved Apriori algorithm. The results show that: (i) there are significant differences in different association rules for various surface defects on the shield tunnel; (ii) the average confidence of the association rule "dislocation & spalling → water leakage" is as high as 57.78%, indicating that most of the water leakage defects are caused by dislocation and spalling of the shield tunnel in the sections being inspected; (iii) the weakest rule appears at "water leakage → spalling", with an average confidence of 13%. The association analysis can be used for predicting the critical defects influencing structural reliability and operation safety, such as water leakage, and optimizing the construction and maintenance work for a shield subway tunnel.

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