Enhanced Efficiency of Dye-Sensitized Solar Cells Based on Polymer-Assisted Dispersion of Platinum Nanoparticles/Carbon Nanotubes Nanohybrid Films as FTO-Free Counter Electrodes.

In this study, polymer-assisted dispersants are used to stabilize the nanohybrids of platinum nanoparticles (PtNPs)/carbon nanotubes (CNTs) through non-covalent bond forces. These dispersants aim to replace the florine-doped tin oxide (FTO) glass in traditional dye-sensitized solar cells (DSSCs) as counter electrodes. The large specific surface area, high conductivity, and redox potential of PtNPs/CNT nanohybrids are used as the basis to utilize them as the counter electrode material to fabricate a dye-sensitized solar cell. The conductivity results indicate that the resistance of the PtNP/CNT nanohybrid film can be reduced to 7.25 Ω/sq. When carbon nanotubes are mixed with platinum nanoparticles at a weight ratio of 5/1, the photoelectric conversion efficiency of DSSCs can reach 6.28%. When using the FTO-containing substrate as the counter electrode, its conversion efficiency indicates that the micro-/nano-hybrid material formed by PtNPs/CNTs also exhibits an excellent photoelectric conversion efficiency (8.45%) on the traditional FTO substrate. Further, a large-area dye-sensitive cell is fabricated, showing that an 8 cm × 8 cm cell has a conversion efficiency of 7.95%. Therefore, the traditional Pt counter electrode can be replaced with a PtNP/CNT nanohybrid film, which both provides dye-sensitive cells with a high photoelectric conversion efficiency and reduces costs.

Improving the Lifetime of CsPbBr3 Perovskite in Water Using Self-Healing and Transparent Elastic Polymer Matrix.

This study developed a simple and efficient strategy to stabilize inorganic halide perovskite CsPbX3 at high relative humidity by embedding it into the matrix with elastic and self-healing features. The polymer matrix has a naturally hydrophobic characteristic of n-butyl acrylate segment (n-BA) and cross-linkable and healable moiety from N-(hydroxymethyl) acrylamide segment (NMA). It was chosen due to the provisions of both a surrounding protective layer for inorganic perovskite and elastic, as well as healing ability to the whole organic-inorganic composite. This fabricated CsPbBr3/PBA-co-PNMA composite was demonstrated to stably persist against the suffering from hydrolysis of perovskites when exposed to a high moisture environment. The PL intensity of the composite after crosslinking was found to be relatively stable after 30 days of exposure to air. Upon water immersion, the PL intensity of composite only showed a decrease of 32% after the first 6 h, then remained stable for 6 h afterward. Furthermore, this fabricated composite was not only flexible and relatively transparent but also exhibited excellent self-healing capability in ambient conditions (T = 25°C), in which the self-healing efficiency after 24 h was above 40%. The tensile strength and stretching ability of 5 wt% perovskite content in the random copolymer were observed to be 3.8 MPa and 553.5% respectively. Overall, flexible and self-healing properties combining with high luminescence characteristics are very promising materials for next-generation soft optical devices.

Charge generation dynamics in hematite photoanodes decorated with gold nanostructures under near infrared excitation.

Photochemical water splitting offers a useful solution for efficient energy conversion into hydrogen gas. Hematite has been focused on this purpose as the photoanode due to the advantages of low-cost, chemical stability, and suitable bandgap. The photocatalytic ability, however, is limited by the short-lived carriers and lack of photoresponse in the near infrared (NIR) region. As a solution, combining hematite with a noble metal can enhance the photocatalytic performance toward longer wavelength. Gold nanoparticles indicate characteristic absorption in the visible and NIR regions and photo-induced injection of electrons into the semiconductor. In this study, a hybrid material of hematite photoanodes with gold nanostructures was fabricated and the carrier dynamics under NIR excitation was elucidated by femtosecond transient absorption spectroscopy. The observed strong positive absorption under NIR excitation of Au nanorods (NRs) on the hematite anode indicated an increased electron density in hematite due to electron transfer from AuNRs, demonstrating efficient charge carrier generation in hematite by the decorated gold nanostructure.

Dual Functional Polymer Interlayer for Facilitating Ion Transport and Reducing Charge Recombination in Dye-Sensitized Solar Cells.

Dye-sensitized solar cells (DSSCs) present low-cost alternatives to conventional wafer-based inorganic solar cells and have remarkable power conversion efficiency. To further enhance performance, we propose a new DSSC architecture with a novel dual-functional polymer interlayer that prevents charge recombination and facilitates ionic conduction, as well as maintaining dye loading and regeneration. Poly(vinylidene fluoride-trifluoroethylene) (p(VDF-TrFE)) was coated on the outside of a dye-sensitized TiO2 photoanode by a simple solution process that did not sacrifice the amount of adsorbed dye molecules in the DSSC device. Light-intensity-modulated photocurrent and photovoltage spectroscopy revealed that the proposed p(VDF-TrFE)-coated anode yielded longer electron lifetime and improved the injection of photogenerated electrons into TiO2, thereby reducing the electron transport time. Comparative cyclic voltammetry and UV-visible absorption spectroscopy based on a ferrocene-ferrocenium external standard material demonstrated that p(VDF-TrFE) enhanced the power conversion efficiency from 7.67% to 9.11%. This dual functional p(VDF-TrFE) interlayer is a promising candidate for improving the performance of DSSCs and can also be employed in other electrochemical devices.

Triggering comprehensive enhancement in oxygen evolution reaction by using newly created solvent.

Theoretical calculations indicate that the properties of confined liquid water, or liquid water at surfaces, are dramatically different from those of liquid bulk water. Here we present an experimentally innovative strategy on comprehensively efficient oxygen evolution reaction (OER) utilizing plasmon-induced activated water, creating from hot electron decay at resonantly illuminated Au nanoparticles (NPs). Compared to conventional deionized (DI) water, the created water owns intrinsically reduced hydrogen-bonded structure and a higher chemical potential. The created water takes an advantage in OER because the corresponding activation energy can be effectively reduced by itself. Compared to DI water-based solutions, the OER efficiencies at Pt electrodes increased by 69.3%, 21.1% and 14.5% in created water-based acidic, neutral and alkaline electrolyte solutions, respectively. The created water was also effective for OERs in photoelectrochemically catalytic and in inert systems. In addition, the efficiency of OER increased by 47.5% in created water-based alkaline electrolyte solution prepared in situ on a roughened Au electrode. These results suggest that the created water has emerged as an innovative activator in comprehensively effective OERs.

Efficient surface enhanced Raman scattering on confeito-like gold nanoparticle-adsorbed self-assembled monolayers.

Confeito-like gold nanoparticles (AuNPs; average diameter = 80 nm) exhibiting a plasmon absorption band at 590 nm were adsorbed through immersion-adsorption on two self-assembled monolayers (SAMs) of 3-aminopropyltriethoxysilane (APTES-SAM) and polystyrene spheres coated with amine-terminated poly(amido amine) dendrimers (DEN/PS-SAM). The surface enhanced Raman scattering (SERS) effect on the SAM substrates was examined using the molecules of a probe dye, rhodamine 6G (R6G). The Raman scattering was strongly intensified on both substrates, but the enhancement factor (>10,000) of the AuNP/DEN/PS-SAM hierarchy substrate was 5-10 times higher than that of the AuNP/APTES-SAM substrate. This strong enhancement is attributed to the large surface area of the substrate and the presence of hot spots. Furthermore, analyzing the R6G concentration dependence of SERS suggested that the enhancement mechanism effectively excited the R6G molecules in the first layer on the hot spots and invoked the strong SERS effect. These results indicate that the SERS activity of confeito-like AuNPs on SAM substrates has high potential in molecular electronic devices and ultrasensitive analyses.

Quantitative evaluation on activated property-tunable bulk liquid water with reduced hydrogen bonds using deconvoluted Raman spectroscopy.

Interesting properties of water with distinguishable hydrogen-bonding structure on interfacial phase or in confined environment have drawn wide attentions. However, these unique properties of water are only found within the interfacial phase and confined environment, thus, their applications are limited. In addition, quantitative evaluation on these unique properties associating with the enhancement of water's physical and chemical activities represents a notable challenge. Here we report a practicable production of free-standing liquid water at room temperature with weak hydrogen-bonded structure naming Au nanoparticles (NPs)-treated (AuNT) water via treating by plasmon-induced hot electron transfer occurred on resonantly illuminated gold NPs (AuNPs). Compared to well-known untreated bulk water (deionized water), the prepared AuNT water exhibits many distinct activities in generally physical and chemical reactions, such as high solubilities to NaCl and O2. Also, reducing interaction energy within water molecules provides lower overpotential and higher efficiency in electrolytic hydrogen production. In addition, these enhanced catalytic activities of AuNT water are tunable by mixing with deionized water. Also, most of these tunable activities are linearly proportional to its degree of nonhydrogen-bonded structure (DNHBS), which is derived from the O-H stretching in deconvoluted Raman spectrum.

Uniform GaN thin films grown on (100) silicon by remote plasma atomic layer deposition.

The growth of uniform gallium nitride (GaN) thin films was reported on (100) Si substrate by remote plasma atomic layer deposition (RP-ALD) using triethylgallium (TEG) and NH3 as the precursors. The self-limiting growth of GaN was manifested by the saturation of the deposition rate with the doses of TEG and NH3. The increase in the growth temperature leads to the rise of nitrogen content and improved crystallinity of GaN thin films, from amorphous at a low deposition temperature of 200 °C to polycrystalline hexagonal structures at a high growth temperature of 500 °C. No melting-back etching was observed at the GaN/Si interface. The excellent uniformity and almost atomic flat surface of the GaN thin films also infer the surface control mode of the GaN thin films grown by the RP-ALD technique. The GaN thin films grown by RP-ALD will be further applied in the light-emitting diodes and high electron mobility transistors on (100) Si substrate.

Innovative fabrication of a Au nanoparticle-decorated SiO2 mask and its activity on surface-enhanced Raman scattering.

Surface-enhanced Raman scattering (SERS) utilizing the well-defined localized surface plasmon resonance (LSPR) of Ag and Au nanoparticles (NPs) under resonant irradiation has emerged as a promising spectroscopy technique for providing vibrational information on trace molecules. The Raman scattering intensity from molecules close to the surface of these finely divided metals can be significantly enhanced by a factor of more than 10(6). In addition to the high sensitivity, the reproducibility of the SERS signal is also an important parameter for its reliable application. In this work, we report on the innovative and facile fabrication of a Au NP-decorated SiO2 mask coated on indium tin oxide (ITO) glass as a SERS array substrate. First, a highly ordered porous SiO2 mask with pore sizes of 350 nm in diameter and wall thickness of 60 nm was deposited on ITO glass by using spin coating. Then, Au NPs were controllably decorated into the pores of the conductive ITO glass-bottomed SiO2 mask by using sonoelectrochemical deposition-dissolution cycling (SEDDC). Experimental results indicate that the SERS effect of Rhodamine 6G (R6G) observed on this developed substrate increases with an increase in the deposition time of Au NPs in SEDDC. The corresponding optimal enhancement factor (EF) that is obtained is ca. 6.5 × 10(7). Significantly, this system achieves an optimal reproducibility under a medium-length deposition time of Au NPs in SEDDC with a relative standard deviation (RSD) of 12% for measurements of five spots on different areas. The low RSD of the SERS signal and the large EF suggest that the developed array system can serve as an excellent spectroscopy platform for practical applications in analytical chemistry.

Hierarchically assembled ZnO nanoparticles on high diffusion coefficient ZnO nanowire arrays for high efficiency dye-sensitized solar cells.

In this study, ZnO nanoparticles (ZnO NPs) were conformally covered on the surfaces of ZnO nanowires (ZnO NWs) with high diffusion coefficient (1.2 × 10(-2) cm(2) s(-1)) to make a composite photoanode. By using N719 to sensitize the composite photoanode, the conversion efficiency can reach 7.14%.

Controlled synthesis of CdSe quantum dots by a microwave-enhanced process: a green approach for mass production.

A method that does not employ hot-injection techniques has been developed for the size-tunable synthesis of high-quality CdSe quantum dots (QDs) with zinc blende structure. In this environmentally benign synthetic route, which uses less toxic precursors, solvents, and capping ligands, CdSe QDs that absorb visible light are obtained. The size of the as-prepared CdSe QDs and thus their optical properties can be manipulated by changing the microwave reaction conditions. The QDs were characterized by XRD, TEM, UV/Vis, FTIR, time-resolved fluorescence spectroscopy, and fluorescence spectrophotometry. In this approach, the reaction is conducted in open air and at a much lower temperature than in hot-injection techniques. The use of microwaves in this process allows for a highly reproducible and effective synthesis protocol that is fully adaptable for mass production and can be easily employed to synthesize a variety of semiconductor QDs with the desired properties. Possible applications of the CdSe QDs were assessed by deposition on TiO(2) films.

Synthesis CdSe(x)S(1-x) core/shell type quantum dots via one injection method.

The photoluminescence quantum yield (PL-QY) of ternary colloidal CdSe(x)S(1-x) quantum dots (QDs), which were prepared by a one-injection method, enhances with increasing S content. The possible enhancement mechanism was explored by structural analysis via X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS). Both found that the enhancement of PL-QY of ternary CdSe(x)S(1-x) QDs strongly correlated with self-formed core/shell conformation in the non-coordination solution.

Adsorption and binding of capping molecules for highly luminescent CdSe nanocrystals--DFT simulation studies.

During CdSe nanocrystal growth, loss of surface capping molecules occurs leading to a decrease of photoluminescence (PL) quantum yield. In general, aliphatic capping molecules are applied to passivate the surface of CdSe nanocrystals to modulate the optical properties of the CdSe. In this work, two kinds of alkylamine (n-butylamine (n-BA) and n-hexylamine (n-HA)) and oleic acid (OA) were used to modify the surfaces of the CdSe nanocrystals. From the PL spectra and quantum yield analyses, we observed that the PL emission peak positions of the modified CdSe nanocrystals have blue shifted for all three capping molecules. However, the PL quantum yield of the CdSe nanocrystals increased after introduction of the alkylamine molecules, but decreased with oleic acid. The detailed mechanism was not clear until now. In this study, a density function theory (DFT) simulation was employed to demonstrate binding energy and charge analyses of CdSe with n-BA, n-HA and OA. By comparing the binding energy of the bare CdSe nanocrystals to that of the CdSe with the capping molecules, it was shown that n-BA and n-HA as capping molecules help to increase the charge on Se and decrease it on cadmium of the CdSe.

Outperformed electrochromic behavior of poly(ethylene glycol)-template nanostructured tungsten oxide films with enhanced charge transfer/transport characteristics.

Porous tungsten oxide films of nanocrystalline tungsten oxide embedded in an amorphous tungsten oxide matrix have been synthesized via poly(ethylene glycol) (PEG)-template sol-gel technique with peroxopolytungstic acid precursor. The effects of PEG addition on the microstructure and electrochromic performance of the tungsten oxide films are investigated. Charge transfer/transport properties in the tungsten oxide films are studied by electrochemical impedance spectroscopy (EIS) as well. Triclinic tungsten oxide film is formed in the absence of PEG. The PEG-template tungsten oxide film demonstrates an electrochromic performance superior to that of the crystalline tungsten oxide film, including larger transmittance modulation and coloration/bleaching efficiency as well as faster response times. EIS measurements indicate that faster charge-transfer rates at the tungsten oxide/electrolyte interface and larger Li(+) diffusion coefficients in tungsten oxide are achieved in the PEG-template film. We suggest that the PEG-template tungsten oxide film with a porous crystalline/amorphous nanostructure provides an effective means for charge transfer/transport to encourage its superior electrochromic performance.