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1.
Micron ; 187: 103719, 2024 Sep 16.
Artículo en Inglés | MEDLINE | ID: mdl-39293141

RESUMEN

Scanning Tunneling Microscopy (STM) is widely used for observing atomic structures due to its ultra-high spatial resolution. As the core units of STM, the coarse stepper motor and imaging unit, have conflicting size requirements for piezo tubes. Longer piezo tubes yield greater output force and easier movement for the motor, while shorter tubes enhance imaging precision and stability for the scanner. Traditional STMs typically employ a large piezo tube for coarse stepping and a smaller one for independent imaging to address this issue. Here, we present the new design of a piezo tube stacked STM, in which two independent piezo tubes act together during tip-sample approach process and only one shorter tube works during scanning imaging. Both tubes are fixed to the framework, ensuring high rigidity and compactness. The new design enables us to achieve both coarse stepping and imaging functions with a total length of only 25 mm for the two tubes, effectively reducing the length of whole STM, facilitating its integration into narrow low-temperature spaces for imaging applications. Using this device, we obtained high-quality atomic images of graphite sample surfaces at room temperature. Continuous scanning imaging of the same area on Au film at 300 K demonstrates the STM's high stability in both X-Y and Z directions. Atomic images, I-V spectra, and di/dv spectra obtained at 2 K on graphite surface illustrate the excellent application potential of this device in low-temperature environments. Finally, atomic images obtained of graphite in sweeping the magnetic fields from 0 T to 11 T in a huge vibrational dry magnet prove the new STM's excellent performance in extreme conditions.

2.
Small ; : e2405400, 2024 Sep 05.
Artículo en Inglés | MEDLINE | ID: mdl-39235363

RESUMEN

The development of alternative conductive polymers for the well-known poly (3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is of great significance for improving the stability in long-term using and high-temperature environments. Herein, an innovative PEDOT:S-ANF aqueous dispersion is successfully prepared by using sulfamic acid (SA) to modified aramid nanofibers (S-ANF) as an alternative dispersant for PSS and the subsequent in situ polymerization of PEDOT. Thanks to the excellent film forming ability and surface negative groups of S-ANF, the PEDOT:S-ANF films show comparable tensile strength and elongation to unmodified PEDOT:ANF. Meanwhile, PEDOT:S-ANF has a high conductivity of 27.87 S cm-1, which is more than 20 times higher than that of PEDOT:PSS. The film exhibits excellent electromagnetic interference (EMI) shielding and thermoelectric performance, with a shielding effectiveness (SE) of 31.14 dB and a power factor (PF) of 0.43 µW m-1K-2. As a substitute for PSS, S-ANF exhibits significant structural and physicochemical properties, resulting in excellent chemical and thermal stability. Even under harsh conditions such as immersing to 0.1 M HCl, 0.1 M NaOH, and 3.5% NaCl solution, or high temperature conditions, the PEDOT:S-ANF films still maintain exceptional EMI shielding performance. Therefore, this multifunctional conductive polymer exhibits enormous potential and even proves its reliability in extreme situations.

3.
Nano Lett ; 2024 Sep 13.
Artículo en Inglés | MEDLINE | ID: mdl-39269918

RESUMEN

Solution-processable electrodes are promising for next-generation electronics due to their simplicity, cost-effectiveness, and potential for large-area fabrication. However, current solution-processable electrodes based on conductive polymers, carbon-based compounds, and metal nanowires face challenges related to stability, patterning, and production scalability. Here we introduce a novel approach using 3D tin halide perovskites (THPs) combined with a photolithography-free solution patterning technique to fabricate solution-processed electrodes. We demonstrate the preparation of highly conductive CsSnI3 films (234.9 S cm-1) and the fabrication of patterned 35 × 35 perovskite electrode arrays on a 4-in. silicon wafer. These electrodes, used as source/drain electrodes in organic transistors, resulted in devices showing high uniformity and stability. This electrode fabrication strategy is also applicable to other 3D THPs like FASnI3 and MASnI3, showcasing versatility for diverse applications. The results highlight the feasibility and advantages of using 3D THPs as solution-processable electrodes, providing a new material system for the advancement of solution-processed electronics.

4.
ACS Appl Mater Interfaces ; 16(34): 45189-45196, 2024 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-39137356

RESUMEN

Near-infrared (NIR) light, valuable for its biological penetration and invisibility to the human eye, is a crucial tool in biomedicine, environmental monitoring, anticounterfeiting, and information encryption, yet traditional NIR luminescent materials are often unstable in humid conditions. Here, a highly stable MgGeO3:Mn2+ glass ceramic (GC) with NIR luminescence was successfully synthesized. As-obtained GC700 boasts exceptional luminescent capabilities and possesses abundant trap structures, enabling data inscription with a 405 nm laser and retrieval via laser/thermal excitation. Moreover, the emission peak of Mn2+ can be manipulated from 630 to 691 nm by increasing the annealing treatment temperature. With the harnessing of the effective NIR emission, stable carrier characteristics, and numerous trap structures, there is potential for application in information encryption. Accordingly, we explored the application of MgGeO3:Mn2+ GC (GC700 and GC800) samples in precious three-dimensional (3D) information storage and NIR mechanoluminescence (ML) for biological tissue imaging. These applications demonstrate the potential and versatility of electron-capturing NIR luminescent materials in a range of cutting-edge fields.

5.
Micromachines (Basel) ; 15(8)2024 Jul 30.
Artículo en Inglés | MEDLINE | ID: mdl-39203632

RESUMEN

In this article, a miniaturized and highly stable frequency-selective rasorber (FSR) incorporating an embedded transmission window is designed. This FSR consists of a lossy layer loaded with resistors, an air layer, and a bandpass layer. The lossy layer is provided with a rectangular, square ring structure loaded with four 180 Ω resistors and four quadrilateral metal plates. The four metal plates are connected to the four corners of the inner ring around the square ring and are radially distributed along the diagonal. The bandpass layer is a square metal patch that a cross-ring slot structure is loaded inside of, and the cross points lie in the direction along the diagonal of the unit. The inner boundary of the cross-ring is composed of two mutually perpendicular and long rectangular elements. This FSR shows an embedded transmission window from 3.63 GHz to 3.80 GHz and has a transmission rate of 93% at 3.72 GHz. Moreover, both sides of the transmission band, namely, 1.86-3.35 GHz and 3.99-8.28 GHz, have an absorption rate of more than 80% and bilateral relative bandwidth of more than 50%. In addition, this structure exhibits excellent miniaturization performance, polarization insensitivity, and angular stability. Finally, a prototype of the designed FSR is processed and measured. The measured results are basically consistent with the simulation results.

6.
J Colloid Interface Sci ; 676: 139-148, 2024 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-39024814

RESUMEN

A promising method of producing hydrogen peroxide (H2O2) is the electrochemical two-electron water oxidation reaction (2e- WOR). In this process, it is important to design electrocatalysts that are both earth abundant and environmentally friendly, as well as offering high stability and production rates. The research of WOR catalysts, such as the extensively used transition metal oxides, is mainly focused on the modification of transition metal elements. Few studies pay attention to the protective heterostructure of metal oxides. Here, we demonstrate for the first time an organometallic skeleton protection strategy to develop highly stable WOR catalysts for H2O2 generation. Unlike the pure ZnO and zeolite imidazole framework-8 (ZIF-8) catalysts, ZnO@ZIF-8 enabled the production of hydrogen peroxide at high voltages. The experimental results demonstrate that the ZnO@ZIF-8 catalyst stably generates H2O2 even under a high voltage of 3.0 V vs. RHE, with a yield reaching 2845.819 µmolmin-1 g-1. ZnO@ZIF-8 shows a relatively low overpotential, with a current density of 10 mA cm-2 and an overpotential of 110 mV. The ZnO@ZIF-8 catalyst's maximal FE value was 4.72 %. Moreover, the ZnO@ZIF-8 catalyst exhibits remarkable durability even after an extended 60-hour stability test. Operando Raman and theoretic calculation analyses reveal that the metal-organic skeleton being encapsulated on the metal oxide surface synergizes with each other, not only expanding the electrochemical surface area, but also adjusting the catalyst metal sites' adsorption capacity. A novel approach to the modification of 2e- WOR metal oxide catalyst is presented in this work.

7.
J Colloid Interface Sci ; 675: 815-824, 2024 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-39002232

RESUMEN

Oxygen vacancy engineering in transition metal oxides is an effective strategy for improving catalytic performance. Herein, defect-enriched Mn2O3 catalysts were constructed by controlling the calcination temperature. The high content of oxygen vacancies and accompanying Mn4+ ions were generated in Mn2O3 catalysts calcined at low temperature, which could greatly improve the low-temperature reducibility and migration of surface oxygen species. DFT theoretical calculations further confirmed that molecular oxygen and toluene were easily adsorbed over defective α-Mn2O3 (222) facets with an energy of -0.29 and -0.48 eV, respectively, and corresponding OO bond length is stretched to 1.43 Å, resulting in the highly reactive oxygen species. Mn2O3-300 catalyst with abundant oxygen vacancies exhibited the highest specific reaction rate and lowest activation energy. Furthermore, the optimized catalyst possessed the outstanding stability, water tolerance and CO2 yield. In comparison with the fresh Mn2O3-300 catalyst, the physical structure and surface property of the used catalyst remained almost unchanged regardless of whether undergoing the stability test at consecutive catalytic runs as well as high temperature, and water resistance test. In situ DRIFTS spectra further elucidated that introducing the water vapor had little effect on the reaction intermediates, indicating the excellent durability of the defect-enriched catalyst.

8.
Angew Chem Int Ed Engl ; : e202412289, 2024 Jul 22.
Artículo en Inglés | MEDLINE | ID: mdl-39037065

RESUMEN

Extending covalent organic frameworks (COFs) into crystalline carbon-free covalent backbones is an important strategy to endow these materials with more exotic functions. Integrating metal-free inorganic and organic components into one covalent framework is an effective way to address the issue of poor thermal/solvent stability in the field of nonlinear optics (NLO). However, constructing such structures is very challenging. Here, we linked 3-connected nods (BO3) and 2-connected organic building blocks (Te(Ph)2) together to produce colorless single crystals (size up to 400 µm) of a three-dimensional (3D) chiral covalent framework (CityU-22). The single-crystal X-ray diffraction (SCXRD) analysis reveals that CityU-22 has a non-carbon Te-O-B-O bond-based network with the srs topology. The chiral CityU-22 displays good stability under the treatment of different common solvents or heat (the decomposition temperature above 300 °C). Due to its non-π-conjugated backbone (-Te-O-B-O-), CityU-22 shows an ultraviolet NLO behavior with a second-harmonic generation (SHG) response similar to KH2PO4 (KDP).

9.
Adv Sci (Weinh) ; 11(31): e2403352, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38874020

RESUMEN

Lead-free halide perovskites possess excellent photoelectric properties, making them widely used in the photoelectric fields. Herein, lead-free double perovskite crystals (PCs) doped with manganese (Cs2NaInCl6:Mn2+) are successfully prepared by the more energy-efficient crystallization method. The crystals emit bright orange-red light under the ultraviolet (UV) lamp, showing unique optical properties. They have the highest photoluminescence quantum yield of 42.91%. The white light-emitting diodes (LEDs) are fabricated using these perovskite crystals, which show a color rendering index of 92 and external quantum efficiency (EQE) as high as 16.3%. Furtherly, perovskite-modified fiber paper made of aramid chopped fibers (ACFs) and polyphenylene sulfide (PPS) exhibited fluorescent properties under different conditions. This paper combines fiber composite technology with PPS fiber filter bags, which are widely used in environmental protection, for the first time and demonstrates functional fiber filter bags with fluorescent characteristics. This filter bag provides an idea for the automatic detection of industrial filtration. Meanwhile, after being exposed to industrial waste gas for 60 h, the filter bag can maintain superior fluorescence performance. In this study, lead-free double perovskites are synthesized using an efficient method for preparing high-performance LEDs and high-stability fluorescent fibers. Concurrently, the application of perovskites in environmental protection is expanded.

10.
Adv Sci (Weinh) ; 11(31): e2401350, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38884251

RESUMEN

A supercritical carbon dioxide (SCCO2) fluid, characterized by gas-like diffusivity, near-zero surface tension, and excellent mass transfer properties, is used as a precursor to produce silicon oxycarbide (SiOC) coating. SCCO2 disperses and reacts with Si particles to form an interfacial layer consisting of Si, O, and C. After an 850 °C annealing process, a conformal SiOC coating layer forms, resulting in core-shell Si@SiOC particles. High-resolution transmission electron microscopy and its X-ray line-scan spectroscopy, X-ray photoelectron spectroscopy, Fourier-transform infrared spectroscopy, and Raman spectroscopy, are used to examine the SiOC formation mechanism. Effects of SCCO2 interaction time on the SiOC properties are investigated. The SiOC layer connects the Si@SiOC particles, improving electron and Li+ transport. Cyclic voltammetry, galvanostatic intermittent titration technique, and electrochemical impedance spectroscopy are employed to examine the role of SiOC during charging/discharging. Operando X-ray diffraction data reveal that the SiOC coating reduces crystal size of the formed Li15Si4 and increases its formation/elimination reversibility during cycling. The Si@SiOC electrode shows a capacitiy of 2250 mAh g-1 at 0.2 A g-1. After 500 cycles, the capacity retention is 72% with Coulombic efficiency above 99.8%. A full cell consisting of Si@SiOC anode and LiNi0.8Co0.1Mn0.1O2 cathode is constructed, and its performance is evaluated.

11.
ACS Appl Mater Interfaces ; 16(27): 34632-34640, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38916478

RESUMEN

Point-of-care testing (POCT) technologies facilitate onsite detection of pathogens in minutes to hours. Among various POCT approaches, pressure-based sensors that utilize gas-generating reactions, particularly those catalyzed by nanozymes (e.g., platinum nanoparticles, PtNPs, or platinum-coated gold nanoparticles, and Au@PtNPs) have been shown to provide rapid and sensitive detection capabilities. The current study introduces Au-Pt alloy-coated gold nanoparticles (Au@AuPtNPs), an innovative nanozyme with enhanced catalytic activity and relatively high stability. For pathogen detection, Au@AuPtNPs are modified with H1 or H2 hairpin DNAs that can be triggered to undergo a hybridization chain reaction (HCR) that leads to their aggregation upon recognition by an initiator strand (Ini) with H1-/H2-complementary aptamers tethered to magnetic beads (MBs). Pathogen binding to the aptamer exposes Ini, which then binds Au@AuPtNPs and initiates a HCR, resulting in Au@AuPtNP aggregation on MBs. These Au@AuPtNP aggregates exhibit strong catalysis of O2 from the H2O2 substrate, which is measured by a pressure meter, enabling detection of Escherichia coli (E. coli) O157:H7 at concentrations as low as 3 CFU/mL with high specificity. Additionally, E. coli O157:H7 could also be detected in simulated water and tea samples. This method eliminates the need for costly, labor- and training-intensive instruments, supporting its further testing and validation for deployment as a rapid-response POCT application in the detection of bacterial contaminants.


Asunto(s)
Escherichia coli O157 , Oro , Nanopartículas del Metal , Platino (Metal) , Escherichia coli O157/aislamiento & purificación , Nanopartículas del Metal/química , Oro/química , Platino (Metal)/química , Catálisis , Técnicas Biosensibles/métodos , Sistemas de Atención de Punto , Peróxido de Hidrógeno/química , Peróxido de Hidrógeno/análisis , Aptámeros de Nucleótidos/química
12.
ACS Appl Mater Interfaces ; 16(27): 35053-35062, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38941512

RESUMEN

The practical applications of bifunctional ruthenium-based electrocatalysts with two active sites of Ru nanoparticles covered with RuO2 skins are limited. One reason is the presence of multiple equally distributed facets, some of which are inactive. In contrast, ruthenium nanorods with a high aspect ratio have multiple unequally distributed facets containing the dominance of active faces for efficient electrocatalysis. However, the synthesis of ruthenium nanorods has not been achieved due to difficulties in controlling the growth. Additionally, it is known that the adsorption capacity of intermediates can be impacted by the surface of the catalyst. Inspired by these backgrounds, the surface-modified (SM) ruthenium nanorods having a dominant active facet of hcp (100) through chemisorbed oxygen and OH groups (SMRu-NRs@NF) are rationally synthesized through the surfactant coordination method. SMRu-NRs@NF exhibits excellent hydrogen evolution in acid and alkaline solutions with an ultralow overpotential of 215 and 185 mV reaching 1000 mA cm-2, respectively. Moreover, it has also shown brilliant oxygen evolution electrocatalysis in alkaline solution with a low potential of 1.58 V to reach 1000 mA cm-2. It also exhibits high durability over 143 h for the evolution of oxygen and hydrogen at 1000 mA cm-2. Density functional theory studies confirmed that surface modification of a ruthenium nanorod with chemisorbed oxygen and OH groups can optimize the reaction energy barriers of hydrogen and oxygen intermediates. The surface-modified ruthenium nanorod strategy paves a path to develop the practical water splitting electrocatalyst.

13.
Nano Lett ; 2024 Jun 04.
Artículo en Inglés | MEDLINE | ID: mdl-38832838

RESUMEN

Theoretically, tandem quantum-dot light-emitting diodes (QLEDs) hold great promise for achieving both high efficiency and high stability in display applications. However, in practice, their operational stability remains considerably inferior to that of state-of-the-art devices. In this study, we developed a new tandem structure with optimal electrical and optical performance to simultaneously improve the efficiency and stability of tandem QLEDs. Electrically, upon development of a barrier-free interconnecting layer enabled by an indium-zinc oxide bridging layer and a conductive ZnMgO layer, the driving voltage of the tandem QLEDs is remarkably reduced. Optically, upon development of a top-emitting structure and optimization of the cavity length guided by a theoretical simulation, a maximum light extraction efficiency is achieved. As a result, the red tandem QLEDs exhibit a maximum external quantum efficiency of 49.01% and a T95 lifetime at 1000 cd/m2 of >50 000 h, making them one of the most efficient and stable QLEDs ever reported.

14.
ACS Appl Mater Interfaces ; 16(24): 31067-31075, 2024 Jun 19.
Artículo en Inglés | MEDLINE | ID: mdl-38859577

RESUMEN

Although organic-inorganic hybrid one-dimensional (1D) lead halide postperovskites (LHPPs) have been reported to show white luminescence and tunable photoluminescence quantum yield (PLQY), their structure-property relationships are not fully understood. Here, we used Mn2+ to test the doping effect on the luminescence of two 1D-LHPPs compounds, namely, {TETA[Pb2Br6]}n 1 and {TETA[Pb2Cl6]}n 2, where TETA = triethylenetetrammonium. We found the pristine compounds show yellowish (551 nm) and bluish (447 nm) emission for 1 and 2, respectively, nanosecond excitation lifetimes (4.17 ns for 1 and 2.29 ns for 2) and low PLQYs (4.65 and 3.57% for 1 and 2, respectively). By fine-doping the Mn2+ ions to ca. 8% the PLQYs for 1 and 2 are maximized to 24 and 25% for 1 and 2, respectively. Upon the increasing Mn2+ dopant, the emission wavelengths can also vary gradually from 551 to 615 nm and from 447 to 660 nm for 1 and 2, respectively, covering almost the whole visible-light range, and the excitation lifetimes are enhanced to microseconds (0.77 µs for 1 and 0.39 µs for 2), owing to the more spin-forbidden d-d transition (4T1-6A1) component from the Mn2+ ions present in the photoluminescence spectra. Moreover, these Mn2+-doped 1D-LHPPs demonstrate high structural and optical stability in humid and high-temperature environments. Hence, such doped materials can be fabricated into a UV-pumped white light-emitting diode, rendering the potential application for solid-state lighting and display systems.

15.
Anal Chim Acta ; 1306: 342613, 2024 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-38692794

RESUMEN

Glucose detection is of significant importance in providing information to the human health management. However, conventional enzymatic glucose sensors suffer from a limited long-term stability due to the losing activity of the enzymes. In this work, the AuNi bimetallic aerogel with a well-defined nanowire network is synthesized and applied as the sensing nanomaterial in the non-enzymatic glucose detection. The three-dimensional (3D) hierarchical porous structure of the AuNi bimetallic aerogel ensures the high sensitivity of the sensor (40.34 µA mM-1 cm-2). Theoretical investigation unveiled the mechanism of the boosting electrocatalytic activity of the AuNi bimetallic aerogel toward glucose. A better adhesion between the sensing nanomaterial and the screen-printing electrodes (SPEs) is obtained after the introduction of Ni. On the basis of a wide linearity in the range of 0.1-5 mM, an excellent selectivity, an outstanding long-term stability (90 days) as well as the help of the signal processing circuit and an M5stack development board, the as-prepared glucose sensor successfully realizes remote monitoring of the glucose concentration. We speculate that this work is favorable to motivating the technological innovations of the non-enzymatic glucose sensors and intelligent sensing devices.


Asunto(s)
Técnicas Biosensibles , Técnicas Electroquímicas , Geles , Glucosa , Oro , Níquel , Técnicas Biosensibles/métodos , Níquel/química , Geles/química , Oro/química , Glucosa/análisis , Electrodos , Nanocables/química , Humanos , Límite de Detección
16.
Small Methods ; : e2400172, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38807542

RESUMEN

Delicately manipulating nanomorphology is recognized as a vital and effective approach to enhancing the performance and stability of organic solar cells (OSCs). However, the complete removal of solvent additives with high boiling points is typically necessary to maintain the operational stability of the device. In this study, two commercially available organic intermediates, namely thieno[3,2-b]thiophene (TT) and 3,6-dibromothieno[3,2-b]thiophene (TTB) are introduced, as solid additives in OSCs. The theoretical simulations and experimental results indicate that TT and TTB may exhibit stronger intermolecular interactions with the acceptor Y6 and donor PM6, respectively. This suggests that the solid additives (SAs) can selectively intercalate between Y6 and PM6 molecules, thereby improving the packing order and crystallinity. As a result, the TT-treated PM6:Y6 system exhibits a favorable morphology, improved charge carrier mobility, and minimal charge recombination loss. These characteristics contribute to an impressive efficiency of 17.75%. Furthermore, the system demonstrates exceptional thermal stability (T80 > 2800 h at 65 °C) and outstanding photostability. The universal applicability of TT treatment is confirmed in OSCs employing D18:L8-BO, achieving a significantly higher PCE of 18.3%. These findings underscore the importance of using appropriate solid additives to optimize the blend morphology of OSCs, thereby improving photovoltaic performance and thermal stability.

17.
J Agric Food Chem ; 72(20): 11706-11715, 2024 May 22.
Artículo en Inglés | MEDLINE | ID: mdl-38728528

RESUMEN

In this study, we devised a photothermally stable phytochemical dye by leveraging alizarin in conjunction with the metal-organic framework ZIF-8 (AL@ZIF-8). The approach involved grafting alizarin into the microporous structure of ZIF-8 through physical adsorption and hydrogen-bonding interactions. AL@ZIF-8 significantly enhanced the photostability and thermostability of alizarin. The nanoparticles demonstrate substantial color changes in various pH environments, showcasing their potential for meat freshness monitoring. Furthermore, we introduced an intelligent film utilizing poly(vinyl alcohol)-sodium alginate-AL@ZIF-8 (PA-SA-ZA) for detecting beef freshness. The sensor exhibited a superior water contact angle (52.34°) compared to the alizarin indicator. The color stability of the film was significantly enhanced under visible and UV light (ΔE < 5). During beef storage, the film displayed significant color fluctuations correlating with TVB-N (R2=0.9067), providing precise early warning signals for assessing beef freshness.


Asunto(s)
Alginatos , Colorimetría , Alcohol Polivinílico , Alginatos/química , Animales , Alcohol Polivinílico/química , Bovinos , Colorimetría/métodos , Antraquinonas/química , Embalaje de Alimentos/instrumentación , Fitoquímicos/química , Carne Roja/análisis , Estructuras Metalorgánicas/química
18.
ACS Appl Mater Interfaces ; 16(22): 28709-28718, 2024 Jun 05.
Artículo en Inglés | MEDLINE | ID: mdl-38780517

RESUMEN

MXenes, represented by Ti3C2Tx, have been widely studied in the electrochemical energy storage fields, including lithium-ion batteries, for their unique two-dimensional structure, tunable surface chemistry, and excellent electrical conductivity. Recently, Nb2CTx, as a new type of MXene, has attracted more and more attention due to its high theoretical specific capacity of 542 mAh g-1. However, the preparation of few-layer Nb2CTx nanosheets with high-quality remains a challenge, which limits their research and application. In this work, high-quality few-layer Nb2CTx nanosheets with a large lateral size and a high conductivity of up to 500 S cm-1 were prepared by a simple HCl-LiF hydrothermal etching method, which is 2 orders of magnitude higher than that of previously reported Nb2CTx. Furthermore, from its aqueous ink, the viscosity-tunable organic few-layer Nb2CTx ink was prepared by HCl-induced flocculation and N-methyl-2-pyrrolidone treatment. When using the organic few-layer Nb2CTx ink as an additive-free anode of lithium-ion batteries, it showed excellent cycling performance with a reversible specific capacity of 524.0 mAh g-1 after 500 cycles at 0.5 A g-1 and 444.0 mAh g-1 after 5000 cycles at 1 A g-1. For rate performance, a specific capacity of 159.8 mAh g-1 was obtained at a high current density of 5 A g-1, and an excellent capacity retention rate of about 95.65% was achieved when the current density returned to 0.5 A g-1. This work presents a simple and scalable process for the preparation of high-quality Nb2CTx and its aqueous/organic ink, which demonstrates important application potential as electrodes for electrochemical energy storage devices.

19.
J Colloid Interface Sci ; 671: 434-440, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-38815378

RESUMEN

Photoelectrochemical (PEC) water splitting is an effective and sustainable method for solar energy harvesting. However, the technology is still far away from practical application because of the high cost and low efficiency. Here, we report a low-cost, stable and high-performing industrial-Si-based photoanode (n-Indus-Si/Co-2mA-xs) that is fabricated by simple electrodeposition. Systematic characterizations such as scanning electron microscopy, X-ray photoelectron spectroscopy have been employed to characterize and understand the working mechanisms of this photoanode. The uniform and adherent dispersion of co-catalyst particles result in high built-in electric field, reduced charge transfer resistance, and abundant active sites. The core-shell structure of co-catalyst particles is formed after the activation process. The reconstructed morphology and modified chemical states of the surface co-catalyst particles improve the separation and transfer of charges, and the reaction kinetics for water oxidation greatly. Our work demonstrates that large-scale PEC water splitting can be achieved by engineering the industrial-Si-based photoelectrode, which shall guide the development of solar energy conversion in the industry.

20.
ACS Appl Mater Interfaces ; 16(15): 18824-18832, 2024 Apr 17.
Artículo en Inglés | MEDLINE | ID: mdl-38566471

RESUMEN

Aqueous ammonium ion hybrid supercapacitor (A-HSC) is an efficient energy storage device based on nonmetallic ion carriers (NH4+), which combines advantages such as low cost, safety, and sustainability. However, unstable electrode structures are prone to structural collapse in aqueous electrolytes, leading to fast capacitance decay, especially in host materials represented by vanadium-based oxidation. Here, the Co2+ preintercalation strategy is used to stabilize the VO2 tunnel structure and improve the electrochemical stability of the fast NH4+ storage process. In addition, the understanding of the NH4+ storage mechanism has been deepened through ex situ structural characterization and electrochemical analysis. The results indicate that Co2+ preintercalation effectively enhances the conductivity and structural stability of VO2, and inhibits the dissolution of V in aqueous electrolytes. In addition, the charge storage mechanisms of NH4+ intercalation/deintercalation and the reversible formation/fracture of hydrogen bonds were revealed.

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