Newly discovered two-dimensional (2D) atomic crystals (nanosheet) of platinum diselenide (PtSe2) have progressively attracted attention due to their expected high performance in catalysis, sensing, electronics, and optoelectronics applications. Further extraordinary physicochemical properties are expected if these nanosheets of platinum diselenide can possess mesoporosity as this may enable a high range of molecular adsorption, enhancing their functionalities in catalysis, batteries, supercapacitors, and sensing. Here, we present for the first time a straightforward, aqueous-phase synthetic strategy for the preparation of scalable nanosheets of platinum diselenide with mesoporous structure via a surfactant-templated self-assembly followed by a thermal annealing phase-transformation process. We used hexamethylenetetramine as a hexagonal honeycomb (sp2-sp3 orbital) scaffold for assembling the Pt and Se organic complexes to form the nanosheet structure, which is stable, preserving the 2D structure and mesoporosity during a thermal annealing at 500 °C. Density functional theory analysis then indicated that the mesoporous nanosheets of platinum diselenide exhibit a high free-energy and large density of π electrons crossing the Fermi level, inferring a high-catalytic performance. This effortless strategy is currently being extended to the synthesis of other transition metal dichalcogenides, including the preparation of multi-metal atomic dichalcogenide nanosheets, for a wide variety of scientific and technological applications.
Silver nanoparticles deposited on quartz substrates are widely used as SERS substrates. The nanoparticles can be deposited directly from colloidal solution by dipping technique. However, the adhesion of the particles on the quartz surface is very poor. Normally the substrate is pre-treated with hydroxylation or silanisation process. In this paper, we have demonstrated that the application of the sequence pre-treatment hydroxylation and silanisation have improved the density of silver nanoplates desposited on the quartz surface. •Sequence hydroxylation and silanisation pre-treatment assists the deposition of the nanoplate on the surface.•Various immersion times of the quartz surface into the colloidal nanoplates determined size distributions and density surface of the nanoplates on the surface.
Localized surface plasmon resonance (LSPR) properties of metallic nanostructures, such as gold, are very sensitive to the dielectric environment of the material, which can simply be adjusted by changing its shape and size through modification of the synthesizing process. Thus, these unique properties are very promising, particularly for the detection of various types of chemicals, for example boric acid which is a non-permitted preservative employed in food preparations. For the sensing material, gold (Au) nanoplates with a variety of shapes, i.e., triangular, hexagonal, truncated pentagon and flat rod, were prepared using a seed-mediated growth method. The yield of Au nanoplates was estimated to be ca. 63% over all areas of the sensing material. The nanoplates produced two absorption bands, i.e., the transverse surface plasmon resonance (t-SPR) and the longitudinal surface plasmon resonance (l-SPR) at 545 nm and 710 nm, respectively. In the sensing study, these two bands were used to examine the response of gold nanoplates to the presence of boric acid in an aqueous environment. In a typical process, when the sample is immersed into an aqueous solution containing boric acid, these two bands may change their intensity and peak centers as a result of the interaction between the boric acid and the gold nanoplates. The changes in the intensities and peak positions of t-SPR and l-SPR linearly correlated with the change in the boric acid concentration in the solution.
Highly efficient and remarkable selective acetone conversion to isopropanol has been achieved via a heterogeneous catalytic hydrogenation of acetone by NaBH4 in the presence of semihollow palladium nanoparticles (PdNPs) grown on ITO substrate. PdNPs with high surface defect grown on an indium tin oxide (ITO) surface were prepared via a simple immersion of the substrate into a solution containing K2PdCl6, sodium dodecyl sulphate (SDS), and formic acid for 2 h at room temperature. The sample showed remarkably high heterogeneous catalytic efficiency by producing 99.8% of isopropanol within 6 min using only 0.28 μg of PdNPs on the ITO surface. The present system exhibits heterogenenous catalytic hydrogenation efficiency 1 × 10(6) time higher than using the conventional Raney Ni system.
A simple method for the synthesis of ZnO nanofilms composed of vertical array of quasi-1D ZnO nanostructures (quasi-NRs) on the surface was demonstrated via a 1D crystal growth of the attached nanoseeds under a rapid hydrolysis process of zinc salts in the presence of ammonia at room temperature. In a typical procedure, by simply controlling the concentration of zinc acetate and ammonia in the reaction, a high density of vertically oriented nanorod-like morphology could be successfully obtained in a relatively short growth period (approximately 4 to 5 min) and at a room-temperature process. The average diameter and the length of the nanostructures are approximately 30 and 110 nm, respectively. The as-prepared quasi-NRs products were pure ZnO phase in nature without the presence of any zinc complexes as confirmed by the XRD characterisation. Room-temperature optical absorption spectroscopy exhibits the presence of two separate excitonic characters inferring that the as-prepared ZnO quasi-NRs are high-crystallinity properties in nature. The mechanism of growth for the ZnO quasi-NRs will be proposed. Due to their simplicity, the method should become a potential alternative for a rapid and cost-effective preparation of high-quality ZnO quasi-NRs nanofilms for use in photovoltaic or photocatalytics applications.PACS: 81.07.Bc; 81.16.-c; 81.07.Gf.
A combinative effect of two or more individual material properties, such as lattice parameters and chemical properties, has been well-known to generate novel nanomaterials with special crystal growth behavior and physico-chemical performance. This paper reports unusually high catalytic performance of AgPt nanoferns in the hydrogenation reaction of acetone conversion to isopropanol, which is several orders higher compared to the performance shown by pristine Pt nanocatalysts or other metals and metal-metal oxide hybrid catalyst systems. It has been demonstrated that the combinative effect during the bimetallisation of Ag and Pt produced nanostructures with a highly anisotropic morphology, i.e., hierarchical nanofern structures, which provide high-density active sites on the catalyst surface for an efficient catalytic reaction. The extent of the effect of structural growth on the catalytic performance of hierarchical AgPt nanoferns is discussed.
This Research Article reports an unusually high efficiency heterogeneous photodegradation of methyl orange (MO) in the presence of Ag nanoparticle-loaded ZnO quasi-nanotube or nanoreactor (A-ZNRs) nanocatalyst grown on FTO substrate. In typical process, photodegradation efficiency of as high as 21.6% per μg per Watts of used catalyst and UV power can be normally obtained within only a 60-min reaction time from this system, which is 10(3) order higher than the reported results. This is equivalent to the turnover frequency of 360 mol mol(-1) h(-1). High-density hexagonal A-ZNRs catalysts were grown directly on FTO substrate via a seed-mediated microwave-assisted hydrolysis growth process utilizing Ag nanoparticle of approximately 3 nm in size as nanoseed and mixture aqueous solution of Zn(NO3)·6H2O, hexamethylenetetramine (HMT), and AgNO3 as the growth solution. A-ZNRs adopts hexagonal cross-section morphology with the inner surface of the reactor characterized by a rough and rugged structure. Transmission electron microscopy imaging shows the Ag nanoparticle grows interstitially in the ZnO nanoreactor structure. The high photocatalytic property of the A-ZNRs is associated with the highly active of inner side's surface of A-ZNRs and the oxidizing effect of Ag nanoparticle. The growth mechanism as well as the mechanism of the enhanced-photocatalytic performance of the A-ZNRs will be discussed.
This paper reports a facile, solution-phase approach to synthesizing a one-dimensional amorphous face-centered-cubic (fcc) platinum (a-Pt) nanostructure (nanofibers) directly on an indium-tin oxide (ITO) substrate. The electron microscopy analysis result shows that the a-Pt nanofiber has a diameter and length of approximately 50 nm and 1 μm, respectively, and is grown in high density on the entire surface of the ITO substrate. The X-ray photoelectron spectroscopy analysis result further reveals that the a-Pt nanofibers feature metallic properties with highly reactive surface chemistry, promising novel performance in electrochemistry, catalysis, and sensors. A synergetic interplay between the formic acid reducing agent and the hexamethylenetetramine surfactant in the reduction of Pt ions is assumed as the driving force for the formation of the amorphous phase in the Pt nanostructure. The catalytic properties of a-Pt were examined in the acetone hydrogenation reaction under microwave irradiation. a-Pt shows excellent heterogeneous catalytic properties for converting acetone to isopropyl alcohol with turnover number and frequency as high as 400 and 140 min(-1), respectively. The preparation and formation mechanism of the a-Pt nanofibers will be discussed in detail in this paper.
This paper reports the synthesis of two-dimensional, hierarchical, porous, and (001)-faceted metal (Ag, Zn, and Al)-doped TiO2 nanostructures (TNSs) and the study of their photocatalytic activity. Two-dimensional metal-doped TNSs were synthesized using the hydrolysis of ammonium hexafluorotitanate in the presence of hexamethylenetetramine and metal precursors. Typical morphology of metal-doped TNSs is a hierarchical nanosheet that is composed of randomly stacked nanocubes (dimensions of up to 5 μm and 200 nm in edge length and thickness, respectively) and has dominant (001) facets exposed. Raman analysis and X-ray photoelectron spectroscopy results indicated that the Ag doping, compared to Zn and Al, much improves the crystallinity degree and at the same time dramatically lowers the valence state binding energy of the TNS and provides an additional dopant oxidation state into the system for an enhanced electron-transfer process and surface reaction. These are assumed to enhance the photocatalytic of the TNS. In a model of photocatalytic reaction, that is, rhodamine B degradation, the AgTNS demonstrates a high photocatalytic activity by converting approximately 91% of rhodamine B within only 120 min, equivalent to a rate constant of 0.018 m-1 and ToN and ToF of 94 and 1.57 min-1, respectively, or 91.1 mmol mg-1 W-1 degradation when normalized to used light source intensity, which is approximately 2 times higher than the pristine TNS and several order higher when compared to Zn- and Al-doped TNSs. Improvement of the crystallinity degree, decrease in the defect density and the photogenerated electron and hole recombination, and increase of the oxygen vacancy in the AgTNS are found to be the key factors for the enhancement of the photocatalytic properties. This work provides a straightforward strategy for the preparation of high-energy (001) faceted, two-dimensional, hierarchical, and porous Ag-doped TNSs for potential use in photocatalysis and photoelectrochemical application.
Perovskite solar cells have emerged as a potential energy alternative due to their low cost of fabrication and high power conversion efficiency. Unfortunately, their poor ambient stability has critically limited their industrialization and application in real environmental conditions. Here, we show that by introducing hexamine molecules into the perovskite lattice, we can enhance the photoactive phase stability, enabling high-performance and air-processable perovskite solar cells. The unencapsulated and freshly prepared perovskite solar cells produce a power conversion efficiency of 16.83% under a 100 mW cm-2 1.5G solar light simulator and demonstrate high stability properties when being stored for more than 1500 h in humid air with relative humidity ranging from 65 to 90%. We envisage that our findings may revolutionize perovskite solar cell research, pushing the performance and stability to the limit and bringing the perovskite solar cells toward industrialization.
A deficiency in the photoelectrical dynamics at the interface due to the surface traps of the TiO2 electron transport layer (ETL) has been the critical factor for the inferiority of the power conversion efficiency (PCE) in the perovskite solar cells. Despite its excellent energy level alignment with most perovskite materials, its large density of surface defect as a result of sub lattice vacancies has been the critical hurdle for an efficient photovoltaic process in the device. Here, we report that atoms thick 2D TiS2 layer grown on the surface of a (001) faceted and single-crystalline TiO2 nanograss (NG) ETL have effectively passivated the defects, boosting the charge extractability, carrier mobility, external quantum efficiency, and the device stability. These properties allow the perovskite solar cells (PSCs) to produce a PCE as high as 18.73% with short-circuit current density (Jsc), open-circuit voltage (Voc), and fill-factor (FF) values as high as 22.04 mA/cm2, 1.13 V, and 0.752, respectively, a 3.3% improvement from the pristine TiO2-NG-based PSCs. The present approach should find an extensive application for controlling the photoelectrical dynamic deficiency in perovskite solar cells.
The crystallinity properties of perovskite influence their optoelectrical performance in solar cell applications. We optimized the grain shape and crystallinity of perovskite film by annealing treatment from 130 to 170 °C under high humidity (relative humidity of 70%). We found that the grain size, grain interface, and grain morphology of the perovskite are optimized when the sample was annealed at 150 °C for 1 h in the air. At this condition, the perovskite film is composed of 250 nm crystalline shape grain and compact inter-grain structure with an invincible grain interface. Perovskite solar cells device analysis indicated that the device fabricated using the samples annealed at 150 °C produced the highest power conversion efficiency, namely 17.77%. The open circuit voltage (Voc), short-circuit current density (Jsc), and fill factor (FF) of the device are as high as 1.05 V, 22.27 mA/cm2, and 0.76, respectively. Optoelectrical dynamic analysis using transient photoluminescence and electrochemical impedance spectroscopies reveals that (i) carrier lifetime in the champion device can be up to 25 ns, which is almost double the carrier lifetime of the sample annealed at 130 °C. (ii) The interfacial charge transfer resistance is low in the champion device, i.e., ~20 Ω, which has a crystalline grain morphology, enabling active photocurrent extraction. Perovskite's behavior under annealing treatment in high humidity conditions can be a guide for the industrialization of perovskite solar cells.