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1.
Chem Mater ; 36(12): 6027-6037, 2024 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-38947981

RESUMEN

Thermal annealing is the most common postdeposition technique used to crystallize antimony selenide (Sb2Se3) thin films. However, due to slow processing speeds and a high energy cost, it is incompatible with the upscaling and commercialization of Sb2Se3 for future photovoltaics. Herein, for the first time, a fast-annealing technique that uses millisecond light pulses to deliver energy to the sample is adapted to cure thermally evaporated Sb2Se3 films. This study demonstrates how photonic curing (PC) conditions affect the outcome of Sb2Se3 phase conversion from amorphous to crystalline by evaluating the films' crystalline, morphological, and optical properties. We show that Sb2Se3 is readily converted under a variety of different conditions, but the zone where suitable films for optoelectronic applications are obtained is a small region of the parameter space. Sb2Se3 annealing with short pulses (<3 ms) shows significant damage to the sample, while using longer pulses (>5 ms) and a 4-5 J cm-2 radiant energy produces (211)- and (221)-oriented crystalline Sb2Se3 with minimal to no damage to the sample. A proof-of-concept photonically cured Sb2Se3 photovoltaic device is demonstrated. PC is a promising annealing method for large-area, high-throughput annealing of Sb2Se3 with various potential applications in Sb2Se3 photovoltaics.

2.
Chem Commun (Camb) ; 59(7): 944-947, 2023 Jan 19.
Artículo en Inglés | MEDLINE | ID: mdl-36597867

RESUMEN

We report a H2 evolving hybrid photocathode based on Sb2Se3 and a precious metal free molecular catalyst. Through the use of a high surface area TiO2 scaffold, we successfully increased the Ni molecular catalyst loading from 7.08 ± 0.43 to 45.76 ± 0.81 nmol cm-2, achieving photocurrents of 1.3 mA cm-2 at 0 V vs. RHE, which is 81-fold higher than the device without the TiO2 mesoporous layer.

3.
Front Chem ; 10: 954588, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-36226119

RESUMEN

Simple compound antimony selenide (Sb2Se3) is a promising emergent light absorber for photovoltaic applications benefiting from its outstanding photoelectric properties. Antimony selenide thin film solar cells however, are limited by low open circuit voltage due to carrier recombination at the metallic back contact interface. In this work, solar cell capacitance simulator (SCAPS) is used to interpret the effect of hole transport layers (HTL), i.e., transition metal oxides NiO and MoO x thin films on Sb2Se3 device characteristics. This reveals the critical role of NiO and MoO x in altering the energy band alignment and increasing device performance by the introduction of a high energy barrier to electrons at the rear absorber/metal interface. Close-space sublimation (CSS) and thermal evaporation (TE) techniques are applied to deposit Sb2Se3 layers in both substrate and superstrate thin film solar cells with NiO and MoO x HTLs incorporated into the device structure. The effect of the HTLs on Sb2Se3 crystallinity and solar cell performance is comprehensively studied. In superstrate device configuration, CSS-based Sb2Se3 solar cells with NiO HTL showed average improvements in open circuit voltage, short circuit current density and power conversion efficiency of 12%, 41%, and 42%, respectively, over the standard devices. Similarly, using a NiO HTL in TE-based Sb2Se3 devices improved open circuit voltage, short circuit current density and power conversion efficiency by 39%, 68%, and 92%, respectively.

5.
ACS Appl Mater Interfaces ; 12(47): 52595-52602, 2020 Nov 25.
Artículo en Inglés | MEDLINE | ID: mdl-33170631

RESUMEN

The improvement of antimony selenide solar cells by short-term air exposure is explained using complementary cell and material studies. We demonstrate that exposure to air yields a relative efficiency improvement of n-type Sb2Se3 solar cells of ca. 10% by oxidation of the back surface and a reduction in the back contact barrier height (measured by J-V-T) from 320 to 280 meV. X-ray photoelectron spectroscopy (XPS) measurements of the back surface reveal that during 5 days in air, Sb2O3 content at the sample surface increased by 27%, leaving a more Se-rich Sb2Se3 film along with a 4% increase in elemental Se. Conversely, exposure to 5 days of vacuum resulted in a loss of Se from the Sb2Se3 film, which increased the back contact barrier height to 370 meV. Inclusion of a thermally evaporated thin film of Sb2O3 and Se at the back of the Sb2Se3 absorber achieved a peak solar cell efficiency of 5.87%. These results demonstrate the importance of a Se-rich back surface for high-efficiency devices and the positive effects of an ultrathin antimony oxide layer. This study reveals a possible role of back contact etching in exposing a beneficial back surface and provides a route to increasing device efficiency.

6.
Chem Mater ; 32(15): 6676-6684, 2020 Aug 11.
Artículo en Inglés | MEDLINE | ID: mdl-32952296

RESUMEN

Alternatives to lead- and tin-based perovskites for photovoltaics and optoelectronics are sought that do not suffer from the disadvantages of toxicity and low device efficiency of present-day materials. Here we report a study of the double perovskite Cs2TeI6, which we have synthesized in the thin film form for the first time. Exhaustive trials concluded that spin coating CsI and TeI4 using an antisolvent method produced uniform films, confirmed as Cs2TeI6 by XRD with Rietveld analysis. They were stable up to 250 °C and had an optical band gap of ∼1.5 eV, absorption coefficients of ∼6 × 104 cm-1, carrier lifetimes of ∼2.6 ns (unpassivated 200 nm film), a work function of 4.95 eV, and a p-type surface conductivity. Vibrational modes probed by Raman and FTIR spectroscopy showed resonances qualitatively consistent with DFT Phonopy-calculated spectra, offering another route for phase confirmation. It was concluded that the material is a candidate for further study as a potential optoelectronic or photovoltaic material.

7.
ACS Appl Mater Interfaces ; 12(19): 21730-21738, 2020 May 13.
Artículo en Inglés | MEDLINE | ID: mdl-32314567

RESUMEN

The crystal structure of Sb2Se3 gives rise to unique properties that cannot otherwise be achieved with conventional thin-film photovoltaic materials, such as CdTe or Cu(In,Ga)Se2. It has previously been proposed that grain boundaries can be made benign provided only the weak van der Waals forces between the (Sb4Se6)n ribbons are disrupted. Here, it is shown that non-radiative recombination is suppressed even for grain boundaries cutting across the (Sb4Se6)n ribbons. This is due to a remarkable self-healing process, whereby atoms at the grain boundary can relax to remove any electronic defect states within the band gap. Grain boundaries can, however, impede charge transport due to the fact that carriers have a higher mobility along the (Sb4Se6)n ribbons. Because of the ribbon misorientation, certain grain boundaries can effectively block charge collection. Furthermore, it is shown that CdS is not a suitable emitter to partner Sb2Se3 due to Sb and Se interdiffusion. As a result, a highly defective Sb2Se3 interfacial layer is formed that potentially reduces device efficiency through interface recombination.

8.
Nat Commun ; 11(1): 861, 2020 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-32054858

RESUMEN

Determining cost-effective semiconductors exhibiting desirable properties for commercial photoelectrochemical water splitting remains a challenge. Herein, we report a Sb2Se3 semiconductor that satisfies most requirements for an ideal high-performance photoelectrode, including a small band gap and favourable cost, optoelectronic properties, processability, and photocorrosion stability. Strong anisotropy, a major issue for Sb2Se3, is resolved by suppressing growth kinetics via close space sublimation to obtain high-quality compact thin films with favourable crystallographic orientation. The Sb2Se3 photocathode exhibits a high photocurrent density of almost 30 mA cm-2 at 0 V against the reversible hydrogen electrode, the highest value so far. We demonstrate unassisted solar overall water splitting by combining the optimised Sb2Se3 photocathode with a BiVO4 photoanode, achieving a solar-to-hydrogen efficiency of 1.5% with stability over 10 h under simulated 1 sun conditions employing a broad range of solar fluxes. Low-cost Sb2Se3 can thus be an attractive breakthrough material for commercial solar fuel production.

9.
Nanomaterials (Basel) ; 8(5)2018 Apr 25.
Artículo en Inglés | MEDLINE | ID: mdl-29693560

RESUMEN

CdTe wires have been fabricated via a catalyst free method using the industrially scalable physical vapor deposition technique close space sublimation. Wire growth was shown to be highly dependent on surface roughness and deposition pressure, with only low roughness surfaces being capable of producing wires. Growth of wires is highly (111) oriented and is inferred to occur via a vapor-solid-solid growth mechanism, wherein a CdTe seed particle acts to template the growth. Such seed particles are visible as wire caps and have been characterized via energy dispersive X-ray analysis to establish they are single phase CdTe, hence validating the self-catalysation route. Cathodoluminescence analysis demonstrates that CdTe wires exhibited a much lower level of recombination when compared to a planar CdTe film, which is highly beneficial for semiconductor applications.

10.
ACS Appl Mater Interfaces ; 10(4): 3750-3760, 2018 Jan 31.
Artículo en Inglés | MEDLINE | ID: mdl-29345454

RESUMEN

In this manuscript, the inorganic perovskite CsPbI2Br is investigated as a photovoltaic material that offers higher stability than the organic-inorganic hybrid perovskite materials. It is demonstrated that CsPbI2Br does not irreversibly degrade to its component salts as in the case of methylammonium lead iodide but instead is induced (by water vapor) to transform from its metastable brown cubic (1.92 eV band gap) phase to a yellow phase having a higher band gap (2.85 eV). This is easily reversed by heating to 350 °C in a dry environment. Similarly, exposure of unencapsulated photovoltaic devices to water vapor causes current (JSC) loss as the absorber transforms to its more transparent (yellow) form, but this is also reversible by moderate heating, with over 100% recovery of the original device performance. NMR and thermal analysis show that the high band gap yellow phase does not contain detectable levels of water, implying that water induces the transformation but is not incorporated as a major component. Performances of devices with best efficiencies of 9.08% (VOC = 1.05 V, JSC = 12.7 mA cm-2 and FF = 68.4%) using a device structure comprising glass/ITO/c-TiO2/CsPbI2Br/Spiro-OMeTAD/Au are presented, and further results demonstrating the dependence of the performance on the preparation temperature of the solution processed CsPbI2Br films are shown. We conclude that encapsulation of CsPbI2Br to exclude water vapor should be sufficient to stabilize the cubic brown phase, making the material of interest for use in practical PV devices.

11.
Chemphyschem ; 16(6): 1203-9, 2015 Apr 27.
Artículo en Inglés | MEDLINE | ID: mdl-25694349

RESUMEN

The choice of metals suitable as the reflective substrate electrode for top-illuminated organic photovoltaics (OPVs) is extremely limited. Herein, we report a novel substrate electrode for this class of OPV architecture based on an Al | Cu | AlOx triple-layer structure, which offers a reflectivity comparable to that of Al over the wavelength range 400-900 nm, a work function suitable for efficient electron extraction in OPVs and high stability towards oxidation. In addition to demonstrating the advantage of this composite electrode over Al in model top-illuminated OPVs, we also present the results of a photoelectron spectroscopy study, which show that an oxidised 0.8 nm Al layer deposited by thermal evaporation onto an Al | Cu reflective substrate electrode is sufficient to block oxidation of the underlying Cu by air or during deposition of a ZnO1-x electron-transport layer. This is remarkable given that the self-limiting oxide thickness on Al metal is greater than 2 nm.

12.
Adv Mater ; 27(2): 326-31, 2015 Jan 14.
Artículo en Inglés | MEDLINE | ID: mdl-25363479

RESUMEN

A new type of window electrode for organic photovoltaics (OPVs) based on an ultra-thin bilayer of copper and amorphous tungsten suboxide, which derives its remarkable optical and electrical properties from spontaneous diffusion of copper into the oxide layer. As the window electrode in efficient inverted OPVs, this unpatterned electrode is shown to perform as well as indium-tin oxide glass.

13.
Adv Mater ; 25(2): 284-8, 2013 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-23108998

RESUMEN

A low-cost window electrode for organic photovoltaics that simultaneously removes the requirement for conducting oxide and conventional low work function electrodes and functions as a sink for oxygen/water in the heart of the device. Remarkably the functionality of this electrode, which is based on a 7.8 nm nanostructured Cu:Al film, improves upon in situ oxidation as demonstrated in bulk heterojunction organic photovoltaics.


Asunto(s)
Aluminio/química , Cobre/química , Suministros de Energía Eléctrica , Compuestos Orgánicos/química , Energía Solar , Electrodos , Oxidación-Reducción , Oxígeno/química , Semiconductores , Agua/química
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