We introduce a simple and inexpensive procedure for epitaxial lift-off of wafer-size flexible and transparent foils of single-crystal gold using silicon as a template. Lateral electrochemical undergrowth of a sacrificial SiO layer was achieved by photoelectrochemically oxidizing silicon under light irradiation. A 28-nanometer-thick gold foil with a sheet resistance of 7 ohms per square showed only a 4% increase in resistance after 4000 bending cycles. A flexible organic light-emitting diode based on tris(bipyridyl)ruthenium(II) that was spin-coated on a foil exploited the transmittance and flexibility of the gold foil. Cuprous oxide as an inorganic semiconductor that was epitaxially electrodeposited onto the gold foils exhibited a diode quality factor of 1.6 (where = 1.0 for an ideal diode), compared with a value of 3.1 for a polycrystalline deposit. Zinc oxide nanowires electrodeposited epitaxially on a gold foil also showed flexibility, with the nanowires intact up to 500 bending cycles.
Epitaxial films through spin coating A simple way to coat a surface with a uniform film is by spin coating. The substrate is spun at high speed, and a droplet of solution containing the coating is added at the center, spreads out, and evaporates. This method is used to make polycrystalline inorganic coatings and amorphous films, such as polymers used in lithography. Kelso et al. performed spin coating with single-crystal substrates, carefully controlling the thickness of the spreading solution on the basis of its viscosity and the rotation rate. In this way, they achieved epitaxial growth—in which the crystallites are oriented by the substrate—for perovskites, zinc oxide, and sodium chloride. Science , this issue p. 166
Designing high-efficiency electrocatalysts for water oxidation has become an increasingly important concept in the catalysis community due to its implications in clean energy generation and storage. In this respect transition-metal-doped mixed-metal selenides incorporating earth-abundant elements such as Ni and Fe have attracted attention due to their unexpectedly high electrocatalytic activity toward the oxygen evolution reaction (OER) with low overpotential in alkaline medium. In this article, quaternary mixed-metal selenide compositions incorporating Ni-Fe-Co were investigated through combinatorial electrodeposition by exploring the ternary phase diagram of Ni-Fe-Co systems. The OER electrocatalytic activity of the resultant quaternary and ternary mixed-metal selenide compositions was measured in order to systematically investigate the trend of catalytic activity as a function of catalyst composition. Accordingly, the composition(s) exhibiting the best catalytic efficiency for the quaternary Fe-Co-Ni mixed-metal selenide was identified. It was observed that the quaternary selenide outperformed the binary as well as the ternary metal selenides in this Ni-Fe-Co phase space. The elemental composition and relative abundance of the elements in the catalyst film was ascertained from energy dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS). Mapping of the OER catalytic activity as a function of catalyst composition indicated that catalytic efficiency was more pronounced in the Fe-rich region with moderate amounts of Ni and trace amounts of Co doping, and the best performance was exhibited by (Ni0.25Fe0.68Co0.07)3Se4, which showed an overpotential of 230 mV (vs RHE) at 10 mA cm–2 with stability exceeding 8 h for continuous oxygen generation. It was also observed that typically the quaternary metal selenide composition was close to AB2Se4, which shows a spinel structure type. Electrochemical measurements along with density functional theory (DFT) calculations were performed to correlate the enhancement of catalytic activity toward the Fe-rich region with composition. First-principles DFT calculations were used to estimate the hydroxyl adsorption energy (E ads) on the surface of the mixed-metal selenides with varying compositions. This adsorption energy could be directly correlated to the onset of OER activity, and the results matched very well with the experimentally observed trend with respect to onset overpotential. The knowledge of the trend of catalytic activity as a function of composition will be very important for catalyst design through targeted material synthesis. This work represents an example of a systematic phase exploration for quaternary metal selenides and provides a strong foundation which can be expanded to study other mixed-metal selenide combinations.
Surfaces of achiral materials exhibit two-dimensional chirality if they lack mirror symmetry. An example is the (643) surface of face-centered-cubic metals such as Au. The (643) and (6̅4̅3̅) surfaces are non-superimposable mirror images of each other. Chiral surfaces offer the possibility of serving as heterogeneous catalysts for chiral synthesis or providing a platform for chiral separation or crystallization. Here, we show the symmetry requirements for surface chirality, and we demonstrate that chiral surfaces can be produced by electrochemically depositing epitaxial films of Au onto commercially available Si(643) wafers. Au(643) is deposited onto one side of the wafer, and its enantiomer Au(6̅4̅3̅) is deposited on the other side of the wafer. In addition to the (643) orientation, the (8 14 17) orientation of Au is produced on the Si(643) wafers. The (8 14 17) orientation has a similar kinked surface to the (643) surface, but it has staggered kinks. Other metal films including Pt, Ni, Cu, and Ag that are electrodeposited onto the Au films exhibit strong in-plane and out-of-plane order. Hence, the method provides a pathway for producing chiral surfaces of a wide range of materials, and it obviates the need to work with expensive single crystals. The Ag/Au/Si(643) surface showed a preference for the electrochemical oxidation of d-glucose, whereas the Ag/Au/Si(6̅4̅3̅) surface showed preference for the oxidation of l-glucose.
An eco-friendly method was developed for the synthesis of 2-benzimidazoles over an Fe3O4@SiO2@(NH4)6Mo7O24 magnetic core–shell nanocomposite using hydrogen peroxide.
An ultrathin, epitaxial Au layer was electrochemically deposited on n-Si(111) to form a Schottky junction that was used as the photoanode in a regenerative photoelectrochemical cell. Au serves as a semitransparent contact that both stabilizes n-Si against photopassivation and catalyzes the oxidation of Fe to Fe. In this cell, Fe was oxidized at the n-Si(111)/Au(111) photoanode and Fe was reduced at the Au cathode, leading to the conversion of solar energy into electrical energy with no net chemical reaction. The photocurrent was limited to 11.9 mA·cm because of the absorption of light by the Fe redox couple. When a transparent solution of sulfite ion was oxidized at the photoanode, photocurrent densities as high as 28.5 mA·cm were observed with AM 1.5 light of 100 mW·cm intensity. One goal of the work was to determine the effect of the Au layer on the interfacial energetics as a function of the Au coverage. There was a decrease in the barrier height from 0.81 to 0.73 eV as the gold coverage was increased from island growth with 10% coverage to a dense Au film with a thickness of 11 nm. In all cases, the band-bending in n-Si was induced by the n-Si/Au Schottky junction instead of the energetic mismatch between the Fermi level of n-Si and the redox couple. The dense Au film gave the greatest stability. Although the photocurrent of the n-Si/Au photoanode with 10.2% island coverage dropped nearly to zero within 2 h, the photocurrent of the photoanode with a dense 11 nm thick Au film only decreased to 92% of its initial value after irradiation at open circuit with AM 1.5 light for 16 h. A 2.1 nm thick layer of SiO formed between the Au film and n-Si. With further irradiation, the fill factor decreased because of the increase of series resistance as the SiO layer thickness exceeded tunneling dimensions.
Protein kinase B (Akt) and protein kinase Ca (PKCa) play important roles in the regulation of cell apoptosis. The aim of this study was to investigate the expression of Akt and PKCa in chondrocytes of human knee osteoarthritic (OA) cartilage, further evaluating their role in chondrocyte apoptosis during OA progression. Human knee OA cartilages were obtained from 38 patients undergoing knee arthroplasty, which is the medium-late stage of OA. Healthy knee cartilages were obtained from 11 amputees. The samples taken from the condyle of femur were collected routinely for morphological, immunohistochemical and Western blot detection, respectively. Light microscopy and laser-scanning confocal microscopy were used for morphological observation. The optical density with computer image analysis evaluated the intensity of immunohistochemical reaction of Akt and PKCa in OA cartilage. Western blot detected the protein expression levels. The results indicated that Akt and PKCa were involved in OA progression, along with the increase of cell apoptosis. In OA cartilage, Akt decreased (p < 0.05) and PKCa increased (p < 0.05). There was a negative correlation and interaction between Akt and PKCa (r = -0.8). These results demonstrated that both Akt and PKCa are related to increased chondrocyte apoptosis in human OA cartilage. The correlation between human OA progression, the role of Akt and PKCa, and chondrocyte apoptosis allows for new therapeutic strategies to be considered.
Lu and Tang claim that the spin-coated films in our study are not epitaxial. They assume that all of the background intensity in the x-ray pole figures of the spin-coated materials is due to randomly oriented grains. There is no evidence for randomly oriented grains in the 2θ x-ray patterns. The background intensity in the pole figures is also comparable to the background from the single-crystal substrates, which is inconsistent with their assumption.
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