M-Au/TiO2 (M = Ag, Pd, Pt) composites were prepared through a facile one-pot photodeposition synthesis and evaluated for solar water splitting (SWS) with and without a sacrificial agent. The M-Au combination exhibits a dominant role in augmenting the H2 generation activity by forming a bi-metallic system. Degussa P25 was used as a TiO2 substrate to photodeposit Au followed by Au + M (M = Ag/Pd/Pt). The SWS activity of the M-Au/TiO2 was determined through photocatalytic H2 production in the presence of methanol as a sacrificial agent under one sun conditions with an AM1.5 filter. The highest H2 yield was observed for Pt0.5-Au1/TiO2 and was around 1.3 ± 0.07 mmol h(-1) g(-1), with an apparent quantum yield (AQY) of 6.4%. Pt0.5-Au1/TiO2 also demonstrated the same activity for 25 cycles of five hours each for 125 h. Critically, the same Pt0.5-Au1/TiO2 catalyst was active in overall SWS (OSWS) without any sacrificial agent, with an AQY = 0.8%. The amount of Au and/or Pt was varied to obtain the optimum composition and it was found that the Pt0.5-Au1/TiO2 composition exhibits the best activity. Detailed characterization by physico-chemical, spectral and microscopy measurements was carried out to obtain an in-depth understanding of the origin of the photocatalytic activity of Pt0.5-Au1/TiO2. These in-depth studies show that gold interacts predominantly with oxygen vacancies present on titania surfaces, and Pt preferentially interacts with gold for an effective electron-hole pair separation at Pt-Au interfaces and electron storage in metal particles. The Pt in Pt0.5-Au1/TiO2 is electronically and catalytically different from the Pt in Pt/TiO2 and it is predicted that the former suppresses the oxygen reduction reaction.
The γ-radiolysis derived chemical grafting of graphite nanosheets with poly(ethylene-glycol) results in a remarkable decrease in the friction coefficient and significantly enhanced antiwear characteristics of steel–steel sliding interfaces.
Nanotube and nanosheet morphologies have been celebrated for their electron transport properties. Present work has been explored to exploit the same by combining 1D TiO2 nanotube (1D‐TN) with 2D reduced graphene oxide (rGO) along with nano gold for visible light sensitization for photocatalytic H2 generation under one sun condition and visible light (λ≥ 400 nm). Vertical and horizontal electron transport in 1D‐TN and rGO, respectively, is combined with the visible light absorption capability of Au nanoparticle. H2 yield (HY) varies between 100 and 655 µmol/g.h with an apparent quantum yield between 0.45 and 3.2 %, respectively, depending on Au/rGO/1D‐TN preparation method and reaction conditions. It has been demonstrated that interfacial contact between rGO/1D‐TN and Au is crucial for high photocatalytic HY. Preparation method influences charge utilization, and hence HY, to a large extent. Nonetheless, the maximum HY reported in the present work is just comparable to HY reported in literature with the most commonly found spherical morphology, and this leads to a question of, is there any real influence of 1D and/or 2D materials, particularly, towards light harvesting applications?
Electrocatalytic oxidation of methanol on silica hollow spheres, loaded with platinum nanoparticles (Pt-SiO2-HS), is reported. The functionalized hollow silica spheres were prepared by the surfactant (lauryl ester of tyrosine) template-assisted synthesis. These spheres were loaded with platinum nanoparticles by γ-radiolysis. Energy-dispersive X-ray analysis (EDAX) and X-ray photoelectron spectroscopy (XPS) analyses confirmed presence of Si and Pt in the composite. High-resolution transmission electron microscopy showed the formation of uniformly deposited Pt nanoparticles over the hollow spheres with a predominant Pt(111) lattice plane on the surface. In spite of the poor conducting nature of the silica support, the oxidation potential and current density per unit mass for methanol oxidation were noted to be ca. 0.72 V vs NHE and 270 mA mg(-1), respectively, which are among the best values reported in its class. The composite did not show any sign of a degradation even after repeated use. In fact, the anodic current was found to increase under constant polarization, which is attributed to a facile reaction between adsorbed CO with a surface hydroxyl group present on the silica support. These results are in favor of Pt-SiO2-HS as a promising electrocatalyst material in the direct methanol fuel cell (DMFC) applications.
High-quality reduced graphene oxide (rGO) nanosheets (NSs) were synthesized by the oxidation of graphite followed by hydrazine treatment for the reduction of the oxygen functionalities. γ-Radiolysis was then used for the functionalization of the rGO-NSs with poly(ethylene glycol) 200 (PEG200). The functionalization resulted in the intercalation of PEG200 molecules in rGO through hydrogen bonding between the hydroxyl groups of rGO and the oxygen atoms of PEG200 molecules. This resulted in an increase in the d spacing of the graphene sheets and a decrease in the defect density of the carbon network in the rGO. The friction coefficient and wear of sliding steel surfaces were reduced by 38% and 55%, respectively, when 0.03 mg mL −1 PEG200-functionalized rGO dispersed in PEG200 was used. The lubrication properties can be described by bipolar interactions between PEG200 and rGO, leading to effective dispersion. Chemical analysis of wear particles showed decomposition of rGO into nanosized graphite domains, as exhibited by mechanical energy produced in tribo-contact. Moreover, these domains formed effective and stable tribofilms on the steel wear tracks that easily sheared under the action of contact stress. This significantly enhanced the antifriction and antiwear properties, resulting in improved oxidation resistance of PEG200 under the tribo-contact. It was found that, at high rGO concentrations, the lubrication efficiency decreased as a result of graphene− graphene intersheet collisions, producing mechanical energy and chemical defects at contact interfaces.
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