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1.
Small ; 18(24): e2200184, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35451217

RESUMEN

2D transition-metal dichalcogenides have been reported to possess piezoelectricity due to their lack of inversion symmetry; thus, they are potentially applicable as electromechanical energy harvesters. Herein, the authors propose a lithography-free piezoelectric energy harvester composed of centimeter-scale MoS2 monolayer films with an interdigitated electrode pattern that is enabled only by the large scale of the film. High-quality large-scale synthesis of the monolayer films is conducted by low-pressure chemical vapor deposition with the assistance of an unprecedented Na2 S promoter. The extra sulfur supplied by Na2 S critically passivates the sulfur vacancies. The energy harvester having a large active area of ≈18.3 mm2 demonstrates an unexpectedly high piezoelectric energy harvesting performance of ≈400.4 mV and ≈40.7 nA under a bending strain of 0.57%, with the careful adjustment of side electrodes along the zigzag atomic arrays in the two dominant domain structure. Nanoampere-level harvesting has not yet been reported with any 2D material-based harvester.

2.
Nat Commun ; 15(1): 4129, 2024 May 16.
Artículo en Inglés | MEDLINE | ID: mdl-38755193

RESUMEN

Most reported thin-film piezoelectric energy harvesters have been based on cantilever-type crystalline ferroelectric oxide thin films deposited on rigid substrates, which utilize vibrational input sources. Herein, we introduce flexible amorphous thin-film energy harvesters based on perovskite CaCu3Ti4O12 (CCTO) thin films on a plastic substrate for highly competitive electromechanical energy harvesting. The room-temperature sputtering of CCTO thin films enable the use of plastic substrates to secure reliable flexibility, which has not been available thus far. Surprisingly, the resultant amorphous nature of the films results in an output voltage and power density of ~38.7 V and ~2.8 × 106 µW cm-3, respectively, which break the previously reported record for typical polycrystalline ferroelectric oxide thin-film cantilevers. The origin of this excellent electromechanical energy conversion is systematically explored as being related to the localized permanent dipoles of TiO6 octahedra and lowered dielectric constant in the amorphous state, depending on the stoichiometry and defect states. This is the leading example of a high-performance flexible piezoelectric energy harvester based on perovskite oxides not requiring a complex process for transferring films onto a plastic substrate.

3.
Mater Horiz ; 9(4): 1207-1215, 2022 Apr 04.
Artículo en Inglés | MEDLINE | ID: mdl-35257128

RESUMEN

Strain engineering has been recognized as a critical strategy in modulating the optoelectronic properties of perovskite halide materials. Here, we demonstrate a self-powered, flexible photodetector based on CsPbBr3 thin films with controllable compressive or tensile strain of up to ±0.81%, which was produced in situ via a sequential two-step deposition on bent polymer substrates. The best photoresponsivity of ∼121.5 mA W-1 with a photocurrent of 5.15 µA was achieved at zero bias under a power intensity of 0.47 mW cm-2 for the maximum tensile strain of +0.81%, which corresponds to a ∼100.2% increase relative to that of the unstrained case. The in situ tensile strain adjusted the band alignments, making them favorable for enhanced charge transport and thus a higher photoresponse. The structural origin of this superlative balanced photodetection performance was systematically revealed to be associated with the distortion of coupled PbBr6 octahedra and the atomic displacement within the octahedron.

4.
ACS Appl Mater Interfaces ; 11(28): 25179-25185, 2019 Jul 17.
Artículo en Inglés | MEDLINE | ID: mdl-31260236

RESUMEN

There have been extensive efforts to develop competitive electrocatalysts using carbon black (CB) supports for high-performance proton-exchange membrane fuel cells with less usage of Pt. Herein, we propose a very promising electrocatalyst architecture based on the three-dimensional Pt/indium tin oxide (ITO)/CB support structure which was enabled by a nonconventional deposition process ensuring very uniform impregnation of Pt and ITO nanoparticles into the CB network. The unusual scales of the Pt (∼1.9 nm) and ITO (∼5.6 nm) nanoparticles were directly related to unexpectedly better performance of the electrocatalytic activities. As a highlight, the electrochemical surface area of the electrocatalyst was maintained very well after the 3000 cycle-accelerated durability evaluation by demonstrating an excellent retention of ∼74.9%. Particularly, the CO tolerance exhibited a low value of ∼0.68 V as the absorption current peak, compared to ∼0.79 V for a commercial Pt/CB catalyst containing twice more Pt.

5.
ACS Appl Mater Interfaces ; 11(1): 1004-1012, 2019 Jan 09.
Artículo en Inglés | MEDLINE | ID: mdl-30511826

RESUMEN

We present a planar luminescent layer for glare-free, long-lifespan white light-emitting diodes (LEDs), with attractive light outputs. The novel and facile remote phosphor approach proposed in this work enhances luminescence properties by combining a waveguiding ZnO-based nanostructure with plasmonic Au nanoparticles. The system comprised a microscale yellow phosphor layer that is applied by simple printing onto an Au nanoparticle-dispersed ZnO nanorod array. This architecture resulted in a considerable enhancement in luminous efficacy of approximately 18% because of the combination of waveguide effects from the nanorod structure and plasmonic effects from the Au nanoparticles. Performance was optimized according to the length of the Zn nanorods and the concentration of Au. An optimal efficiency of ∼84.26 lm/W for a silicate phosphor-converted LED was achieved using long ZnO nanorods and an Au concentration of 12.5 ppm. The finite-difference time-domain method was successfully used to verify the luminous efficacy improvements in the Au nanoparticle-intervened nanostructures via the waveguiding and plasmonic effects.

6.
J Phys Chem Lett ; 9(20): 5934-5939, 2018 Oct 18.
Artículo en Inglés | MEDLINE | ID: mdl-30247923

RESUMEN

Experimental verification of optical modulation with external stress has not been easily available in flexible systems. Here, we intentionally induced extra stress in wide band gap ZnO thin films by a unique prestress-driven deposition processing that utilizes a stretching mode. The stretching mode provides homogeneous but biaxial stresses in the hexagonal wurtzite structure, leading to the extension of the c-axis and the contraction of the a-axis. As a result, the reduction of the optical band gap by ∼150 meV was observed for the strain of ∼4.87%. The band gap narrowing was found to occur from the respective downward and upward shifts of the conduction band minimum and valence band maximum under the applied stress. The experimental evidence of optical modulations was supported by the theoretical calculations using density functional theory. The reduced strong interactions between Zn d and O p orbitals were assumed to be responsible for the band gap narrowing.

7.
ACS Appl Mater Interfaces ; 10(18): 16203-16209, 2018 May 09.
Artículo en Inglés | MEDLINE | ID: mdl-29658263

RESUMEN

Colossal dielectric constant CaCu3Ti4O12 has been recognized as one of the rare materials having intrinsic interfacial polarization and thus unusual dielectric characteristics, in which the electrical state of the grain boundary is critical. Here, the direct correlation between the grain boundary potential and relative permittivity is proposed for the CaCu3Ti4O12 thin films doped with Zn, Ga, Mn, and Ag as characterized by Kelvin probe force microscopy. The dopants are intended to provide the examples of variable grain boundary potentials that are driven by chemical states including Cu+, Ti3+, and oxygen vacancy. Grain boundary potential is nearly linearly proportional to the dielectric constant. This effect is attributed to the increased charge accumulation near the grain boundary, depending on the choice of the dopant. As an example, 1 mol % Ag-doped CaCu3Ti4O12 thin films demonstrate the best relative permittivity as associated with a higher grain boundary potential of 120.3 mV compared with 82.6 mV for the reference film. The chemical states across grain boundaries were further verified by using spherical aberration-corrected scanning transmission electron microscopy with the simultaneous electron energy loss spectroscopy.

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