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1.
Phys Chem Chem Phys ; 22(3): 981-984, 2020 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-31912822

RESUMO

Herein, we propose a new approach of molecule occupancy via a vapor treatment to facilitate the conversion of PbI2 to perovskite in sequential deposition. We have shown that the morphology of PbI2 and the subsequent crystallization of perovskite can be effectively tuned, thus leading to the elimination of residual PbI2 and promotion of perovskite growth.

2.
Nanoscale ; 12(3): 1448-1454, 2020 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-31829376

RESUMO

Intercalation has proven to be a powerful strategy for physical and chemical property modulation in two dimensional (2D) van der Waals (vdW) materials. Traditional gaseous and chemical intercalation methods offer the ability for mass production, and the electrochemical method provides reversible fine tuning for in situ material investigation. Spatial control, or even direct patterning, of ions is widely required for practical device fabrication and integration; yet it is not realized. Here we demonstrate a self-driven ion (Co2+, Sn4+, and Cu2+) intercalation approach with patterning ability on vdW α-MoO3. It is proved that the self-driven intercalation was enabled by the formation of a local galvanic cell and could be controlled by the metal electrode potential and the solution concentration. The universality of self-intercalation was confirmed in various types of 2D materials (MoS2, WS2, MoSe2, WSe2 and graphene). Furthermore, the feasibility of building heterostructures by multiple species (Sn & Co) intercalation in a single nanosheet was demonstrated for broadband photodetection. The enhancement of conductivity and photoresponse was found to be due to the synergistic effect of lattice distortion from Sn intercalation and the d orbital from the Co atom. This approach offers a feasible way for direct nano-fabrication in 2D vdW material and functional device integration.

3.
ACS Appl Mater Interfaces ; 11(49): 45979-45990, 2019 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-31722524

RESUMO

The vertical composition distribution of a bulk heterojunction (BHJ) photoactive layer is known to have dramatic effects on photovoltaic performance in polymer solar cells. However, the vertical composition distribution evolution rules of BHJ films are still elusive. In this contribution, three BHJ film systems, composed of polymer donor PBDB-T, and three different classes of acceptor (fullerene acceptor PCBM, small-molecule acceptor ITIC, and polymer acceptor N2200) are systematically investigated using neutron reflectometry to examine how donor-acceptor interaction and solvent additive impact the vertical composition distribution. Our results show that those three BHJ films possess homogeneous vertical composition distributions across the bulk of the film, while very different composition accumulations near the top and bottom surface were observed, which could be attributed to different repulsion, miscibility, and phase separation between the donor and acceptor components as approved by the measurement of the donor-acceptor Flory-Huggins interaction parameter χ. Moreover, the solvent additive 1,8-diiodooctane (DIO) can induce more distinct vertical composition distribution especially in nonfullerene acceptor-based BHJ films. Thus, higher power conversion efficiencies were achieved in inverted solar cells because of facilitated charge transport in the active layer, improved carrier collection at electrodes, and suppressed charge recombination in BHJ solar cells.

4.
Angew Chem Int Ed Engl ; 58(41): 14740-14747, 2019 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-31496040

RESUMO

Metal-organic framework-derived NiCo2.5 S4 microrods wrapped in reduced graphene oxide (NCS@RGO) were synthesized for potassium-ion storage. Upon coordination with organic potassium salts, NCS@RGO exhibits an ultrahigh initial reversible specific capacity (602 mAh g-1 at 50 mA g-1 ) and ultralong cycle life (a reversible specific capacity of 495 mAh g-1 at 200 mA g-1 after 1 900 cycles over 314 days). Furthermore, the battery demonstrates a high initial Coulombic efficiency of 78 %, outperforming most sulfides reported previously. Advanced ex situ characterization techniques, including atomic force microscopy, were used for evaluation and the results indicate that the organic potassium salt-containing electrolyte helps to form thin and robust solid electrolyte interphase layers, which reduce the formation of byproducts during the potassiation-depotassiation process and enhance the mechanical stability of electrodes. The excellent conductivity of the RGO in the composites, and the robust interface between the electrodes and electrolytes, imbue the electrode with useful properties; including, ultrafast potassium-ion storage with a reversible specific capacity of 402 mAh g-1 even at 2 A g-1 .

5.
ACS Appl Mater Interfaces ; 11(17): 15581-15590, 2019 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-30969099

RESUMO

On account of the large radius of K-ions, the electrodes can suffer huge deformation during K-ion insertion and extraction processes. In our work, we unveil the impact of using carboxymethyl cellulose (CMC) instead of poly(vinylidene fluoride) (PVDF) as binders for K-ion storage. Our porous hollow carbon submicrosphere anodes using the CMC binder exhibit a reversible capacity of 208 mA h g-1 after 50 cycles at 50 mA g-1, and even at a high current density of 1 A g-1, they achieve a reversible capacity of 111 mA h g-1 over 3000 cycles with almost no decay, demonstrating remarkably improved reversibility and cycling stability than those using PVDF (18 mA h g-1 after 3000 cycles at 1 A g-1). It is showed that the CMC binder can result in higher adhesion force and better mechanical performance than the PVDF binder, which can restrain the crack during a potassiation/depotassiation process. According to the test of adhesion force, the hollow carbon submicrospheres using the CMC binder show above three times of average adhesion force than that using the PVDF binder. Furthermore, based on the rational design, our hollow carbon submicrospheres also exhibit 62.3% specific capacity contribution below 0.5 V vs K/K+ region, which is helpful to design the full cell with high energy density. We believe that our work will highlight the binder effect to improve the K-ion storage performance.

6.
ACS Appl Mater Interfaces ; 11(17): 15741-15747, 2019 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-30920195

RESUMO

Defects engineering can broaden the absorption band of wide band gap van der Waals (vdW) materials to the visible or near-IR regime at the expense of material stability and photoresponse speed. Herein, we introduce an atomic intercalation method that brings the wide band gap vdW α-MoO3 for vis-MIR broadband optoelectronic conversion. We confirm experimentally that intercalation significantly enhances photoabsorption and electrical conductivity buts effects negligible change to the lattice structure as compared with ion intercalation. Charge transfer from the Sn atom to the lattices induces an optoelectrical change. As a result, the Sn-intercalated α-MoO3 shows room temperature, air stable, broadband photodetection ability from 405 nm to 10 µm, with photoresponsivity better than 9.0 A W-1 in 405-1500 nm, ∼0.4 A W-1 at 3700 nm, and 0.16 A W-1 at 10 µm, response time of ∼0.1 s, and peak D* of 7.3 × 107 cm Hz0.5 W-1 at 520 nm. We further reveal that photothermal effect dominates in our detection range by real-time photothermal-electrical measurement, and the materials show a high temperature coefficient of resistance value of -1.658% K-1 at 300 K. These results provide feasible route for designing broadband absorption materials for photoelectrical, photothermal, or thermal-electrical application.

7.
J Am Chem Soc ; 140(28): 8696-8704, 2018 07 18.
Artigo em Inglês | MEDLINE | ID: mdl-29927248

RESUMO

Plasmon-free surface enhanced Raman scattering (SERS) based on the chemical mechanism (CM) is drawing great attention due to its capability for controllable molecular detection. However, in comparison to the conventional noble-metal-based SERS technique driven by plasmonic electromagnetic mechanism (EM), the low sensitivity in the CM-based SERS is the dominant barrier toward its practical applications. Herein, we demonstrate the 1T' transition metal telluride atomic layers (WTe2 and MoTe2) as ultrasensitive platforms for CM-based SERS. The SERS sensitivities of analyte dyes on 1T'-W(Mo)Te2 reach EM-comparable ones and become even greater when it is integrated with a Bragg reflector. In addition, the dye fluorescence signals are efficiently quenched, making the SERS spectra more distinguishable. As a proof of concept, the SERS signals of analyte Rhodamine 6G (R6G) are detectable even with an ultralow concentration of 40 (400) fM on pristine 1T'-W(Mo)Te2, and the corresponding Raman enhancement factor (EF) reaches 1.8 × 109 (1.6 × 108). The limit concentration of detection and the EF of R6G can be further enhanced into 4 (40) fM and 4.4 × 1010 (6.2 × 109), respectively, when 1T'-W(Mo)Te2 is integrated on the Bragg reflector. The strong interaction between the analyte and 1T'-W(Mo)Te2 and the abundant density of states near the Fermi level of the semimetal 1T'-W(Mo)Te2 in combination gives rise to the promising SERS effects by promoting the charge transfer resonance in the analyte-telluride complex.

8.
Adv Mater ; 30(28): e1801562, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-29797364

RESUMO

The mixed cation lead mixed halide perovskite (MLMP) Csx FA1-x PbIy Br3-y is one of the most promising candidates for both single-junction and tandem solar cells due to its high efficiency and remarkable stability. However, the composition effect on thermal stability and photovoltaic performances has not yet been comprehensively investigated. Therefore, the interplay between composition, crystal structure, morphology, and optoelectronic properties under heat stress, is systematically elucidated here through a series of in situ characterizations. It is revealed for the first time that the FA+ and Br- release synchronously at first even under mild annealing. This leads to a serious FA- and Br-deficiency issue, with only 88.3% of Br and 90.2% of FA retained after annealing at 100 °C, which significantly magnifies the hysteresis, phase segregation, and instability issues. Finally, a trace amount of FA+ and Br- is introduced onto the post-annealed MLMP surface to compensate for the deficiency through vacancy filling. The degradation lifetime to 80% of the initial efficiency (t80 ) is improved from 504 to 1056 h and the hysteresis issue is also well resolved. This work highlights the importance of the synergetic composition effect of the organic cation and halide anion on stability and efficiency optimization for long-term applications.

9.
Materials (Basel) ; 11(5)2018 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-29747404

RESUMO

Solution approaches to NiOx films for electrochromic applications are problematic due to the need of an additional high-temperature annealing treatment step in inert gas. In this study, nanostructured NiOx powder with grain size of about 10.1 nm was synthesized for fabrication of NiOx films for electrochromic application. Non-toxic dispersants of isopropanol and deionized water were used and the whole process was carried out in air. The effects of the number of spin-coating layers, annealing temperature, and the volume ratios of isopropanol to deionized water were systematically investigated. Large transmittance change of 62.3% at 550 nm, high coloration efficiency (42.8 cm²/C), rapid switching time (coloring time is 4 s, bleaching time is 3 s), and good stability were achieved in the optimized NiOx film. The optimized process only required a low processing temperature of 150 °C in air with spin-coating three times and 1:2 volume ratio of isopropanol to deionized water. Finally, good cycle durability of up to 2000 cycles without obvious degradation was demonstrated by cyclic voltammetry tests in a LiClO4/propylene carbonate electrolyte. This study provides a simple and effective approach for fabrication of NiOx films at low temperature in air, which is attractive for further commercialization of electrochromic devices.

10.
Adv Mater ; 30(13): e1705318, 2018 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-29469218

RESUMO

2D van der Waals (vdW) layered polar crystals sustaining phonon polaritons (PhPs) have opened up new avenues for fundamental research and optoelectronic applications in the mid-infrared to terahertz ranges. To date, 2D vdW crystals with PhPs are only experimentally demonstrated in hexagonal boron nitride (hBN) slabs. For optoelectronic and active photonic applications, semiconductors with tunable charges, finite conductivity, and moderate bandgaps are preferred. Here, PhPs are demonstrated with low loss and ultrahigh electromagnetic field confinements in semiconducting vdW α-MoO3 . The α-MoO3 supports strong hyperbolic PhPs in the mid-infrared range, with a damping rate as low as 0.08. The electromagnetic confinements can reach ≈λ0 /120, which can be tailored by altering the thicknesses of the α-MoO3 2D flakes. Furthermore, spatial control over the PhPs is achieved with a metal-ion-intercalation strategy. The results demonstrate α-MoO3 as a new platform for studying hyperbolic PhPs with tunability, which enable switchable mid-infrared nanophotonic devices.

11.
Nanotechnology ; 29(11): 115703, 2018 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-29408804

RESUMO

Here, we report a simple strategy to prepare highly sensitive surface-enhanced Raman spectroscopy (SERS) substrates based on Ag decorated Cu2O nanoparticles by combining two common techniques, viz, thermal oxidation growth of Cu2O nanoparticles and magnetron sputtering fabrication of a Ag nanoparticle film. Methylene blue is used as the Raman analyte for the SERS study, and the substrates fabricated under optimized conditions have very good sensitivity (analytical enhancement factor ∼108), stability, and reproducibility. A linear dependence of the SERS intensities with the concentration was obtained with an R 2 value >0.9. These excellent properties indicate that the substrate has great potential in the detection of biological and chemical substances.

12.
Nanotechnology ; 2018 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-29328059

RESUMO

Here, we report a simple strategy to prepare highly sensitive surface-enhanced Raman spectroscopy (SERS) substrates based on Ag decorated Cu<sub>2</sub>O nanoparticles by combing two commom techniques, viz, thermal oxidation growth of Cu<sub>2</sub>O nanoparticles and magnetron sputtering fabrication of Ag nanopartilce film. Methylene blue was used as raman analyte for the SERS study, and the substrates fabricated under optimized conditions have very good sensitivity (analytical enhancement facor ~10<sup>8</sup>) , stablility and reproducibility. A linear dependence about the SERS intensities with the concentration was obtained with the R<sup>2</sup> value > 0.9. These excellent properties indicate that the substrate have great potential in the detection of biological and chemical substances.

13.
ACS Appl Mater Interfaces ; 9(39): 34085-34092, 2017 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-28884570

RESUMO

Because of the popularity of smart electronics, multifunctional energy storage devices, especially electrochromic supercapacitors (SCs), have attracted tremendous research interest. Herein, a solid-state electrochromic asymmetric SC (ASC) window is designed and fabricated by introducing WO3 and polyaniline as the negative and positive electrodes, respectively. The two complementary materials contribute to the outstanding electrochemical and electrochromic performances of the fabricated device. With an operating voltage window of 1.4 V and an areal capacitance of 28.3 mF cm-2, the electrochromic devices show a high energy density of 7.7 × 10-3 mW h cm-2. Meanwhile, they exhibit an obvious and reversible color transition between light green (uncharged state) and dark blue (charged state), with an optical transmittance change between 55 and 12% at a wavelength of 633 nm. Hence, the energy storage level of the ASC is directly related to its color and can be determined by the naked eye, which means it can be incorporated with other energy cells to visual display their energy status. Particularly, a self-powered and color-indicated system is achieved by combining the smart windows with commercial solar cell panels. We believe that the novel electrochromic ASC windows will have great potential application for both smart electronics and smart buildings.

14.
Nanoscale Res Lett ; 12(1): 506, 2017 Aug 23.
Artigo em Inglês | MEDLINE | ID: mdl-28836136

RESUMO

Efficient Si/organic hybrid solar cells were fabricated with dimethyl sulfoxide (DMSO) and surfactant-doped poly(3,4-ethylenedioxythiophene): polystyrene (PEDOT:PSS). A post-treatment on PEDOT:PSS films with polar solvent was performed to increase the device performance. We found that the performance of hybrid solar cells increase with the polarity of solvent. A high conductivity of 1105 S cm- 1 of PEDOT:PSS was achieved by adopting methanol treatment, and the best efficiency of corresponding hybrid solar cells reaches 12.22%. X-ray photoelectron spectroscopy (XPS) and RAMAN spectroscopy were utilized to conform to component changes of PEDOT:PSS films after solvent treatment. It was found that the removal of the insulator PSS from the film and the conformational changes are the determinants for the device performance enhancement. Electrochemical impedance spectroscopy (EIS) was used to investigate the recombination resistance and capacitance of methanol-treated and untreated hybrid solar cells, indicating that methanol-treated devices had a larger recombination resistance and capacitance. Our findings bring a simple and efficient way for improving the performance of hybrid solar cell.

15.
Adv Mater ; 29(38)2017 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-28833622

RESUMO

The controlled synthesis of MoTe2 and WTe2 is crucial for their fundamental research and potential electronic applications. Here, a simplified ambient-pressure chemical vapor deposition (CVD) strategy is developed to synthesize high-quality and large-scale monolayer and few-layer 1T'-phase MoTe2 (length ≈ 1 mm) and WTe2 (length ≈ 350 µm) crystals by using ordinary salts (KCl or NaCl) as the growth promoter combining with low-cost (NH4 )6 Mo7 O24 ·4H2 O and hydrate (NH4 )10 W12 O41 ·xH2 O as the Mo and W sources, respectively. Atomic force microscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, and transmission electron microscopy confirm the high-quality nature and the atomic structure of the as-grown 1T' MoTe2 and WTe2 flakes. Variable-temperature transport measurements exhibit their semimetal properties. Furthermore, near-field nanooptical imaging studies are performed on the 1T' MoTe2 and WTe2 flakes for the first time. The sub-wavelength effects of 1T'-phase MoTe2 (λp ≈ 140 nm) and WTe2 (λp ≈ 100 nm) are obtained. This approach paves the way for the growth of special transition-metal dichalcogenides materials and boosts the future polaritonic research of 2D telluride compounds.

16.
ACS Appl Mater Interfaces ; 9(6): 5543-5549, 2017 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-28116901

RESUMO

Layered α-MoO3 is a multifunctional material that has significant application in optoelectronic devices. In this study, we show the growth of large-scale, large-size, few-layered (FL) α-MoO3 nanosheet directly on technical substrates (SiO2 and Si) by physical vapor deposition. We suggest that the growth is self-limiting in the [010] direction because of the re-evaporation and high diffusion capacity of MoOx species at high temperature. As-prepared FL α-MoO3 is nonconductive and shows poor response to photoillumination with wavelength of 405 and 630 nm. Its work function is strongly altered by the substrate. Improvement of conductivity and photoresponse is observed after the FL device is annealed in vacuum. Line defects along the [001], [100], and [101] directions belonging to the generation of Os and Oa vacancy states appear, and the interfacial effect is suppressed. Scanning near-field optical microscope shows that the defects are absorption sites. Kelvin probe force microscope reveals decrease of apparent work function under illumination, which confirms that electrons are excited from defects states. Our findings show that intense studies on defect engineering are required to push forward the application of two-dimensional metal oxides.

17.
ACS Appl Mater Interfaces ; 8(47): 32366-32375, 2016 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-27933852

RESUMO

Quantification of intergrain length scale properties of CH3NH3PbI3 (MAPbI3) can provide further understanding of material physics, leading to improved device performance. In this work, we noticed that two typical types of facets appear in sequential deposited perovskite (SDP) films: smooth and steplike morphologies. By mapping the surface potential as well as the photoluminescence (PL) peak position, we revealed the heterogeneity of SDP thin films that smooth facets are almost intrinsic with a PL peak at 775 nm, while the steplike facets are p-type-doped with 5-nm blue-shifted PL peak. Considering the reaction process, we propose that the smooth facets have well-defined crystal lattices that resulted from the interfacial reaction between MAI and PbI2 domains containing low trap states density. The steplike facets are MAI-rich originated from the grain boundaries of PbI2 film and own more trap states. Conversion of steplike facets to smooth facets can be controlled by increasing the reaction time through Ostwald ripening. The improved stability, photoresponsivity up to 0.3 A/W, on/off ratio up to 3900, and decreased photo response time to ∼160 µs show that the trap states can be annihilated effectively to improve the photoelectrical conversion with prolonged reaction time and elimination of steplike facets. Our findings demonstrate the relationship between the facet heterogeneity of SDP films and crystal growth process for the first time, and imply that the systematic control of crystal grain modification will enable amelioration of crystallinity for more-efficient perovskite photoelectrical applications.

18.
ACS Appl Mater Interfaces ; 8(29): 19158-67, 2016 Jul 27.
Artigo em Inglês | MEDLINE | ID: mdl-27391382

RESUMO

UNLABELLED: Organic-inorganic hybrid heterojunctions are poised to push toward novel optoelectronics applications, such as photodetectors, but significant challenges complicating practical use remain. Although all organic based photodetectors have been reported with great success, their potential in high-speed, broadband, self-powered photodetectors have not been fully explored. Herein, a self-powered, broad bandwidth of photodetector based on PEDOT: PSS/Si heterojunction is built by a facial low temperature spin-coating method. By interface engineering of heterojunction with optimal band alignment and heteromicrostructures, enhanced photoresponse performances are obtained. The bandwidth of the hybrid photodetector could be broadened by 10 kHz after interfacial passivation by a methyl group. Further manipulating the geometrical structure of the hybrid heterojunction with silicon nanowire, a broad spectrum response from 300 to 1100 nm, with bandwidth as high as 40.6 kHz, fast response speed of 2.03 µs and high detection of 4.1 × 10(11) Jones under zero bias was achieved. Meanwhile, the close dependence between the photoresponse performance of heterojunctions and Si nanowire length is observed in the top-coverage configuration. Finally, a coverage effects model is proposed based on the competition of Si bulk and surface recombination, which is also confirmed by the designed bottom-coverage experiment. The mechanisms behind the enhanced photoresponse of the hybrid photodetector is attributed to the optimum band alignment, as well as the optimum balance of carrier dissociation and recombination of heterojunction. The scalable and low temperature method would be of great convenience for large-scale fabrication of the PEDOT: PSS/Si hybrid photodetector.

19.
Eur Phys J E Soft Matter ; 39(2): 24, 2016 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-26920527

RESUMO

We investigate crack formation in deposition films from drying colloidal suspension drops, by varying the roughness and texture of the substrate. The experimental results indicate that the crack number or crack spacing presents a general dependence on the substrate roughness, despite the orientation of the substrate textures. Interestingly, the crack spacing decreases with the increase of the roughness. Two possible mechanisms are proposed to understand the dependence of the cracks on roughness. Firstly, the concentration reduction of the drying suspension due to collecting colloidal particles from the substrate textures decreases the crack spacing. Secondly, stress concentration resulting from the defects (the notches in textures) in the dried deposition enhances crack formation. However, a quantitative estimation by the calculation of the stress concentrating factors reveals that the notch of the substrate textures dominates crack variation. The results here bring forth a practical method for controlling the crack orientation and suppression, and a potential application to crack-free coatings, films and paintings during the drying of complex fluids.

20.
Small ; 12(4): 438-45, 2016 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-26663902

RESUMO

The electrical performance of highly crystalline monolayer MoS2 is remarkably enhanced by a self-limited growth strategy on octadecyltrimethoxysilane self-assembled monolayer modified SiO2 /Si substrates. The scattering mechanisms in low-κ dielectric, including the dominant charged impurities, acoustic deformation potentials, optical deformation potentials), Fröhlich interaction, and the remote interface phonon interaction in dielectrics, are quantitatively analyzed.

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