Efficient visible light photodegradation of Methylene blue using TiO 2 -graphene based composites has been reported. DFT calculations corroborate the mechanism for Ti-O-C bond formation, leading to an additional band edge and band gap tuning. AbstractHere we report experimental and theoretical study of two TiO 2 -graphene oxide (TG) and TiO 2 -reduced graphene oxide (TR) composites synthesized by a facile and ecological route, for enhanced visible light (~470nm) photocatalyc degradation of Methylene Blue (MB) (99% efficiency), with high rate constant value (1800% over bare TiO 2 ). TG couples TiO 2 nanopowder with Graphene Oxide (GO) while TR couples it with reduced graphene oxide (RGO). The present study, unlike previous reports, discusses never before reported double absorption edges obtained for both TG (3.51 eV and 2.51 eV) and TR (3.42 eV and 2.39 eV) composites, which marks the reason behind feasible visible light (2.56 eV) induced photocatalysis. TiO 2 domains in the composites dominate the higher band edge, while GO/RGO domains explain the lower band edge. Formation of Ti-O-C bond in both TG and TR drives the shifting up of the valence band edge and reduction in band gap. Further, these bonds provide a conductive pathway for charge carriers from TiO 2 nanopowder to the degrading species via the GO/RGO matrix, resulting in decreased charge carrier recombination in TiO 2 and enhanced efficiency.To attest that the developed theory is proof-positive, density function theory (DFT) calculations were performed. DFT obtained energetics and electronic structures support experimental findings by showcasing the play of Ti-O-C bond, resulting in double band edge phenomenon in composites.Finally, the mechanism behind MB degradation is discussed comprehensively and the effect of weight percent of GO/RGO in composite on rate constant and photodegradation efficiency has been studied experimentally and explained by developing analytical equations. 4 promising as it simultaneously possesses excellent absorptivity, transparency, conductivity and reachability, which could assist effective photodegradation of pollutants.There is a pool of reports showing the enhanced photocatalytic activity of TiO 2 nanoparticles with graphene composites for the degradation of organic molecules and photocatalytic splitting of water under UV light. 22, 28-38 Enhanced photocatalytic activity was attributed to the synergetic effect between graphene and TiO 2 nanoparticles, because graphene acts as an excellent electron acceptor and transporter, the Ti-O-C bond open up an easy path for charge transfer which remarkably decreases the recombination of electron−hole pairs. 3 Although claiming good efficiency, many of these reports are based on usage of un-ecological UV light and suffer from low kinetics (k value). [28][29][30] Realizing the importance of efficient visible light photodegradation, there are few reportes which show enhanced photocatalytic activity of TiO 2 -GO/RGO composites under visible light. 39-42 The results and application part is...
Molybdenum nitrides have been employed in a variety of applications. For use in catalysis, the cubic γ phase with the nominal stoichiometry Mo 2 N and the space group Fm3̅ m is typically prepared by high-temperature reaction of MoO 3 with NH 3 . The literature presents conflicting reports of the possible presence of residual oxygen from typical ammonolysis reactions and whether such species influence the crystal structure and morphology. With the aim of resolving these open questions, a comprehensive study of the chemistry, crystal structure, and electronic structure of molybdenum nitride materials prepared by ammonolysis has been undertaken here, with particular focus on the role of reaction temperature. Ammonolysis of MoO 3 was carried out at 973 and 1073 K and yielded single-phase cubic products. Using electron energy loss spectroscopy (EELS), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis, prompt gamma-ray neutron activation analysis, and combustion analysis, significant concentrations of oxygen and, to a lesser extent, hydrogen were found in both materials. The crystal structure of each phase was refined by Rietveld analysis using combined synchrotron X-ray diffraction and neutron diffraction data. The structures were found to be derivatives of the B1 rock salt (halite) structure, as is often reported for "γ-Mo 2 N." However, both materials adopt the space group Pm3̅ m, as opposed to the typically presumed space group of Fm3̅ m, and both have much higher anion content than implied by the stoichiometry Mo 2 N. Ordering of cation vacancies and of anion species is responsible for the loss of the translational symmetry expected for the space group Fm3̅ m. X-ray absorption spectroscopy studies, along with the EELS and XPS results, showed the Mo oxidation state to be diminished with higher temperature synthesis, consistent with the retention of a lower concentration of anions and in particular oxygen. The difficulty in differentiating oxygen and nitrogen and the impossibility of detecting hydrogen by X-ray and electron diffraction methods, especially in the presence of the heavy element Mo, have likely inhibited accurate identification of Mo 1−x (N 1−y O y )H z as the product of MoO 3 ammonolysis. The findings reported here offer a critical assessment for understanding the properties of molybdenum "nitrides" in electronic and catalytic applications.
Atomic layer deposition (ALD) has been used to apply continuous Pt films on powders of the solid acid CsH 2 PO 4 (CDP), in turn, used in the preparation of cathodes in solid acid fuel cells (SAFCs).The film deposition was carried out at 150 °C using trimethyl(methylcyclopentadienyl)platinum (MeCpPtMe 3 ) as the Pt source and ozone as the reactant for ligand removal. Chemical analysis showed a Pt growth rate of 0.09 ± 0.01 wt%/cycle subsequent to an initial nucleation delay of 84 ± 20 cycles. Electron microscopy revealed the contiguous nature of the films prepared using 200 or more cycles. The cathode overpotential (0.48 ± 0.02 V at a current density of 200 mA/cm 2 ) was independent of Pt deposition amount beyond the minimum required to achieve these continuous films. The cell electrochemical characteristics were moreover extremely stable with time, with the cathode overpotentials increasing by no more than 10 mV over a 100 h period of measurement. Thus, ALD holds promise as an effective tool in the preparation of SAFC cathodes with high activity and excellent stability.
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