The mechanism and structure requirements of selective and total oxidation of methane in a chemical looping process are both experimentally and theoretically examined on La 1−x Sr x FeO 3−δ (x = 0, 0.2, and 0.5) and La 0.5 Sr 0.5 Fe 1−x Co x O 3−δ (x = 0.5 and 1) perovskites. The oxygen mobility in the perovskites described by the formation energy of oxygen vacancy is found to have a pronounced effect on the catalytic activity and selectivity. In particular, the selectivity is controlled largely by the surface oxygen concentration or the oxygen vacancy concentration on perovskites, which depends strongly on the bulk oxygen concentration and the relative rate of the lattice oxygen diffusion with respect to the surface reaction. The substitution of Sr for La at the A site and the substitution of Co for Fe at the B site of the ABO 3 perovskites dramatically increase the oxygen mobility. A higher oxygen diffusion rate, and hence enrichment of oxygen on the surface, would improve the catalyst selectivity toward total oxidation.
We describe a rapid environmentally friendly wet-chemical approach to synthesize extremely stable non-toxic, biocompatible, water-soluble monodispersed gold nanoparticles (AuNPs) in one step at room temperature. The particles have been successfully achieved in just a few minutes by merely adding sodium hydroxide (NaOH) acting as an initiator for the reduction of HAuCl(4) in aqueous solution in the presence of polyvinylpyrrolidone (PVP) without the use of any reducing agent. It is also proved to be highly efficient for the preparation of AuNPs with controllable sizes. The AuNPs show remarkable stability in water media with high concentrations of salt, various buffer solutions and physiological conditions in biotechnology and biomedicine. Moreover, the AuNPs are also non-toxic at high concentration (100 microM). Therefore, it provides great opportunities to use these AuNPs for biotechnology and biomedicine. This new approach also involved several green chemistry concepts, such as the selection of environmentally benign reagents and solvents, without energy consumption, and less reaction time.
It was found that the Pt loading obtained by immobilization of colloidal Pt oxide particles on carbon nanofibers (CNFs) at a pH of 9−10 varied from 1.4 to 19.6 wt % (nominal loading 19.4 wt %). The amount of Pt deposited depended significantly on the CNF properties. The study targeted the identification of the determining carbon support properties for the successful preparation of Pt catalysts. CNFs, multiwall carbon nanotubes (MWNTs), and Vulcan XC-72R were utilized as supports. Platelet and fishbone CNFs with different surface areas, graphene layer stacking angles, and amount of surface oxygen groups were obtained by catalytic chemical vapor deposition. The carbon supports were thoroughly characterized by transmission electron microscopy (TEM), N2-adsorption measurements, X-ray diffraction (XRD), temperature-programmed oxidation (TPO), ζ-potential measurements, and X-ray photoelectron spectroscopy (XPS). Characterization of the deposited Pt particles by TEM revealed similar sizes but differences with respect to particle location. Based on TEM, BET, XRD, and XPS, a clear indication of the importance of surface defects and edge sites for successful immobilization of Pt oxide colloid particles was found for all carbon supports. From XPS a linear relationship was found between the fraction of species originating at a binding energy of 285.1 eV and the final Pt loading. These species can be sp3-hybridized carbon, defects, and/or dangling bonds (edge structure). The surface oxygen groups were found to have a decisive effect on the immobilization of Pt. Negative linear trends were found between the Pt loading obtained on CNFs and the O 1s/C 1s ratio and number of carboxylic groups determined from XPS. It is based on the results believed that the oxygen-free defect and edge structure can play a vital and important role in the preparation of more effective CNF-supported catalysts.
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