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1.
Artigo em Inglês | MEDLINE | ID: mdl-32134239

RESUMO

Control of forward and inverse reactions between perovskites and precursor materials is key to attaining high-quality perovskite materials. Many techniques focus on synthesizing nanostructured CsPbX3 materials (e.g., nanowires) via a forward reaction (CsX + PbX2 → CsPbX3). However, low solubility of inorganic perovskites and complex phase transition make it difficult to realize the precise control of composition and length of nanowires using the conventional forward approach. Herein, we report the self-assembly inverse growth of CsPbBr3 micronanowires (MWs) (CsPb2Br5 → CsPbBr3 + PbBr2↑) by controlling phase transition from CsPb2Br5 to CsPbBr3. The two-dimensional (2D) structure of CsPb2Br5 serves as nucleation sites to induce initial CsPbBr3 MW growth. Also, phase transition allows crystal rearrangement and slows down crystal growth, which facilitates the MW growth of CsPbBr3 crystals along the 2D planes of CsPb2Br5. A CsPbBr3 MW photodetector constructed based on the inverse growth shows a high responsivity of 6.44 A W-1 and detectivity of ∼1012 Jones. Large grain size, high crystallinity, and large thickness can effectively alleviate decomposition/degradation of perovskites, which leads to storage stability for over 60 days in humid environment (relative humidity = 45%) and operational stability for over 3000 min under illumination (wavelength = 400 nm, light intensity = 20.06 mW cm-2).

2.
J Am Chem Soc ; 141(8): 3515-3523, 2019 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-30646682

RESUMO

Increasing the stability of perovskites is essential for their integration in commercial photovoltaic devices. Halide mixing is suggested as a powerful strategy toward stable perovskite materials. However, the stabilizing effect of the halides critically depends on their distribution in the mixed compound, a topic that is currently under intense debate. Here we successfully determine the exact location of the I and Cl anions in the  CH3NH3PbBr3- yI y and CH3NH3PbBr3- zCl z mixed halide perovskite lattices and correlate it with the enhanced stability we find for the latter. By combining scanning tunneling microscopy and density functional theory, we predict that, for low ratios, iodine and chlorine incorporation have different effects on the electronic properties and stability of the CH3NH3PbBr3 perovskite material. In addition, we determine the optimal Cl incorporation ratio for stability increase without detrimental band gap modification, providing an important direction for the fabrication of stable perovskite devices. The increased material stability induced by chlorine incorporation is verified by performing photoelectron spectroscopy on a half-cell device architecture. Our findings provide an answer to the current debate on halide incorporation and demonstrate their direct influence on device stability.

3.
Adv Mater ; 31(11): e1804284, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30680833

RESUMO

Perovskite solar cells (PSCs) have attracted great attention in the past few years due to their rapid increase in efficiency and low-cost fabrication. However, instability against thermal stress and humidity is a big issue hindering their commercialization and practical applications. Here, by combining thermally stable formamidinium-cesium-based perovskite and a moisture-resistant carbon electrode, successful fabrication of stable PSCs is reported, which maintain on average 77% of the initial value after being aged for 192 h under conditions of 85 °C and 85% relative humidity (the "double 85" aging condition) without encapsulation. However, the mismatch of energy levels at the interface between the perovskite and the carbon electrode limits charge collection and leads to poor device performance. To address this issue, a thin-layer of poly(ethylene oxide) (PEO) is introduced to achieve improved interfacial energy level alignment, which is verified by ultraviolet photoemission spectroscopy measurements. Indeed as a result, power conversion efficiency increases from 12.2% to 14.9% after suitable energy level modification by intentionally introducing a thin layer of PEO at the perovskite/carbon interface.

4.
Nat Commun ; 9(1): 3880, 2018 09 24.
Artigo em Inglês | MEDLINE | ID: mdl-30250031

RESUMO

Besides high efficiency, the stability and reproducibility of perovskite solar cells (PSCs) are also key for their commercialization. Herein, we report a simple perovskite formation method to fabricate perovskite films with thickness over 1 µm in ambient condition on the basis of the fast gas-solid reaction of chlorine-incorporated hydrogen lead triiodide and methylamine gas. The resultant thick and smooth chlorine-incorporated perovskite films exhibit full coverage, improved crystallinity, low surface roughness and low thickness variation. The resultant PSCs achieve an average power conversion efficiency of 19.1 ± 0.4% with good reproducibility. Meanwhile, this method enables an active area efficiency of 15.3% for 5 cm × 5 cm solar modules. The un-encapsulated PSCs exhibit an excellent T80 lifetime exceeding 1600 h under continuous operation conditions in dry nitrogen environment.

5.
ACS Appl Mater Interfaces ; 10(26): 22513-22519, 2018 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-29879837

RESUMO

Organic field-effect transistors (OFETs) are the most fundamental device units in organic electronics. Interface engineering at the semiconductor/dielectric interface is an effective approach for improving device performance, particularly for enhancing charge transport in conducting channels. Here, we report flat-lying molecular monolayers that exhibit good uniformity and high crystallinity at the semiconductor/dielectric interface, deposited through slow thermal evaporation. Transistor devices achieve high carrier mobility up to 2.80 cm2 V-1 s-1, which represents a remarkably improvement in device performance compared with devices that are completely based on fast-evaporated films. Interfacial flat-lying monolayers benefit charge transport by suppressing the polarization of dipoles and narrowing the broadening of trap density of states. Our work provides a promising strategy for enhancing the performance of OFETs by using interfacial flat-lying molecular monolayers.

6.
J Phys Chem Lett ; 9(6): 1318-1323, 2018 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-29493240

RESUMO

In organic field-effect transistors, the first few molecular layers at the semiconductor/dielectric interface are regarded as the active channel for charge transport; thus, great efforts have been devoted to the modification and optimization of molecular packing at such interfaces. Here, we report organic monolayers with large-area uniformity and high crystallinity deposited by an antisolvent-assisted spin-coating method acting as the templating layers between the dielectric and thermally evaporated semiconducting layers. The predeposited crystalline monolayers significantly enhance the film crystallinity of upper layers and the overall performance of transistors using these hybrid-deposited semiconducting films, showing a high carrier mobility up to 11.3 cm2 V-1 s-1. Additionally, patterned transistor arrays composed of the templating monolayers are fabricated, yielding an average mobility of 7.7 cm2 V-1 s-1. This work demonstrates a promising method for fabricating low-cost, high-performance, and large-area organic electronics.

7.
Adv Mater ; 30(18): e1707635, 2018 May.
Artigo em Inglês | MEDLINE | ID: mdl-29578268

RESUMO

The ability to release, as electrical energy, potential energy stored at the water:carbon interface is attractive, since water is abundant and available. However, many previous reports of such energy converters rely on either flowing water or specially designed ionic aqueous solutions. These requirements restrict practical application, particularly in environments with quiescent water. Here, a carbon-based chemical-to-electricity device that transfers the chemical energy to electrical form when coming into contact with quiescent deionized water is reported. The device is built using carbon nanotube yarns, oxygen content of which is modulated using oxygen plasma-treatment. When immersed in water, the device discharges electricity with a power density that exceeds 700 mW m-2 , one order of magnitude higher than the best previously published result. X-ray absorption and density functional theory studies support a mechanism of operation that relies on the polarization of sp2 hybridized carbon atoms. The devices are incorporated into a flexible fabric for powering personal electronic devices.

8.
J Phys Chem B ; 122(2): 511-520, 2018 01 18.
Artigo em Inglês | MEDLINE | ID: mdl-28514169

RESUMO

The rapid rise of power conversion efficiency (PCE) of low cost organometal halide perovskite solar cells suggests that these cells are a promising alternative to conventional photovoltaic technology. However, anomalous hysteresis and unsatisfactory stability hinder the industrialization of perovskite solar cells. Interface engineering is of importance for the fabrication of highly stable and hysteresis free perovskite solar cells. Here we report that a surface modification of the widely used TiO2 compact layer can give insight into interface interaction in perovskite solar cells. A highest PCE of 18.5% is obtained using anatase TiO2, but the device is not stable and degrades rapidly. With an amorphous TiO2 compact layer, the devices show a prolonged lifetime but a lower PCE and more pronounced hysteresis. To achieve a high PCE and long lifetime simultaneously, an insulating polymer interface layer is deposited on top of TiO2. Three polymers, each with a different functional group (hydroxyl, amino, or aromatic group), are investigated to further understand the relation of interface structure and device PCE as well as stability. We show that it is necessary to consider not only the band alignment at the interface, but also interface chemical interactions between the thin interface layer and the perovskite film. The hydroxyl and amino groups interact with CH3NH3PbI3 leading to poor PCEs. In contrast, deposition of a thin layer of polymer consisting of an aromatic group to prevent the direct contact of TiO2 and CH3NH3PbI3 can significantly enhance the device stability, while the same time maintaining a high PCE. The fact that a polymer interface layer on top of TiO2 can enhance device stability, strongly suggests that the interface interaction between TiO2 and CH3NH3PbI3 plays a crucial role. Our work highlights the importance of interface structure and paves the way for further optimization of PCEs and stability of perovskite solar cells.

9.
ACS Nano ; 11(8): 8464-8470, 2017 08 22.
Artigo em Inglês | MEDLINE | ID: mdl-28767215

RESUMO

The determination of structural evolution at the atomic level is essential to understanding the intrinsic physics and chemistries of nanomaterials. Mechanochemistry represents a promising method to trace structural evolution, but conventional mechanical tension generates random breaking points, which makes it unavailable for effective analysis. It remains difficult to find an appropriate model to study shear deformations. Here, we synthesize high-modulus carbon nanotubes that can be cut precisely, and the structural evolution is efficiently investigated through a combination of geometry phase analysis and first-principles calculations. The lattice fluctuation depends on the anisotropy, chirality, curvature, and slicing rate. The strain distribution further reveals a plastic breaking mechanism for the conjugated carbon atoms under cutting. The resulting sliced carbon nanotubes with controllable sizes and open ends are promising for various applications, for example, as an anode material for lithium-ion batteries.

10.
J Phys Chem Lett ; 8(14): 3193-3198, 2017 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-28649837

RESUMO

Organo-lead-halide perovskites are promising materials for optoelectronic applications. Perovskite solar cells have reached power conversion efficiencies of over 22%, and perovskite light-emitting diodes have recently achieved over 11% external quantum efficiency. To date, most research on perovskite light-emitting diodes has focused on solution-processed films. There are many advantages of a vapor-based growth process to prepare perovskites, including ease of patterning, ability to batch process, and material compatibility. We investigated an all-vapor perovskite growth process by chemical vapor deposition and demonstrated luminance up to 560 cd/m2.

11.
Small ; 12(18): 2419-24, 2016 05.
Artigo em Inglês | MEDLINE | ID: mdl-27002590

RESUMO

A perovskite solar cell fiber is created with a high power conversion efficiency of 7.1% through a controllable deposition method. A combination of aligned TiO2 nanotubes, a uniform perovskite layer, and transparent aligned carbon nanotube sheet contributes to the high photovoltaic performance. It is flexible and stable, and can be woven into smart clothes for wearable applications.


Assuntos
Compostos de Cálcio , Óxidos , Energia Solar , Titânio , Vestuário , Microscopia Eletrônica de Varredura
12.
Angew Chem Int Ed Engl ; 54(49): 14880-4, 2015 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-26460095

RESUMO

A new family of hierarchically helical carbon-nanotube fibers with many nano- and micro-scale channels has been synthesized. They demonstrate remarkable mechanical actuations in response to water and moisture. The water or moisture is first rapidly transported through the trunk micron-scale channels and then efficiently infiltrates into the interconnected capillary nanoscale channels, similar to the blood flow in our body. Therefore, rapid and large contraction and rotation of the fiber occurs with a high reversibility. These mechanically actuating fibers are promising for various applications, and smart windows and louvers have been investigated as two demonstrations.

14.
Small ; 11(9-10): 1150-5, 2015 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-24889384

RESUMO

A novel carbon nanomaterial with aligned carbon nanotubes (CNTs) chemically bonded to a single-layered, large area graphene sheet is designed and fabricated, showing remarkable electronic and electrocatalytic properties. When the carbon nanomaterial is used as a counter electrode, the resulting dye-sensitized solar cell exhibits ≈11% enhancement of energy conversion efficiency than aligned CNT array.

15.
Adv Mater ; 27(6): 1042-7, 2015 Feb 11.
Artigo em Inglês | MEDLINE | ID: mdl-25446835

RESUMO

A hierarchically helical organization of carbon nanotubes into macroscopic fibers enables sophistication while controlling three-dimensional electromechanical actuations, e.g., an artificial swing and tail. The actuation generates a stress of more than 260 times that of a typical natural skeletal muscle and an accelerated velocity of more than 10 times that of a cheetah at low electric currents with high reversibility, good stability, and availability to various media.


Assuntos
Materiais Biomiméticos/síntese química , Voo Animal/fisiologia , Fibras Musculares Esqueléticas/fisiologia , Nanofibras/química , Nanotubos de Carbono/química , Asas de Animais/fisiologia , Animais , Condutividade Elétrica , Campos Eletromagnéticos , Teste de Materiais , Movimento (Física) , Nanofibras/efeitos da radiação , Nanofibras/ultraestrutura , Nanotubos de Carbono/efeitos da radiação , Nanotubos de Carbono/ultraestrutura
16.
Adv Mater ; 26(48): 8120-5, 2014 Dec 23.
Artigo em Inglês | MEDLINE | ID: mdl-25338951

RESUMO

Aligned carbon-nanotube (CNT) sheets are used as building blocks to prepare light-weight, frequency-tunable and high-performance microwave absorbers, and the absorption frequency can be accurately controlled by stacking them with different intersectional angles. A remarkable reflection loss of -47.66 dB is achieved by stacking four aligned CNT sheets with an intersectional angle of 90° between two neighboring ones. The incorporation of a second phase such as a metal and a conducting polymer greatly enhances the microwave-absorption capability.

17.
Angew Chem Int Ed Engl ; 53(39): 10425-8, 2014 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-25047870

RESUMO

Perovskite solar cells have triggered a rapid development of new photovoltaic devices because of high energy conversion efficiencies and their all-solid-state structures. To this end, they are particularly useful for various wearable and portable electronic devices. Perovskite solar cells with a flexible fiber structure were now prepared for the first time by continuously winding an aligned multiwalled carbon nanotube sheet electrode onto a fiber electrode; photoactive perovskite materials were incorporated in between them through a solution process. The fiber-shaped perovskite solar cell exhibits an energy conversion efficiency of 3.3%, which remained stable on bending. The perovskite solar cell fibers may be woven into electronic textiles for large-scale application by well-developed textile technologies.

18.
Adv Mater ; 26(3): 466-70, 2014 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-24174379

RESUMO

An all-solid-state, coaxial and self-powered "energy fiber" is demonstrated that simultaneously converts solar energy to electric energy and further stores it. The "energy fiber" is flexible and can be scaled up for the practical application by the well-developed textile technology, and may open a new avenue to future photoelectronics and electronics.

19.
Adv Mater ; 26(8): 1217-22, 2014 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-24282151

RESUMO

Twisted, aligned carbon nanotube/silicon composite fibers with remarkable mechanical and electronic properties are designed to develop novel flexible lithium-ion batteries with a high cyclic stability. The core-sheath architecture and the aligned structure of the composite nanotube offer excellent combined properties.

20.
Adv Mater ; 26(11): 1694-8, 2014 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-24347052

RESUMO

A novel core-sheath carbon nanostructured fiber is created with high tensile strength, electrical conductivity, and electrocatalytic activity. In particular, the designed ribbon-like nanostructure on the outer surface favors the attachment and impregnation of a second functional phase that is critical for electronic devices. As a demonstration, novel wire-shaped dye-sensitized solar cells are produced with high energy conversion efficiencies up to 6.83%.

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