Abstract: Catalytic oxidation of benzene assisted by ozone, on alumina, silica, and boehmite-supported Ni/Pd catalysts was investigated at 353 K to assess the influence of the support on the reaction. Three bimetallic Ni/Pd nanosized samples with loading 4.7% of Ni and 0.17% of Pd supported on SiO2, AlOOH and Al2O3 were synthesized by the extractive-pyrolytic method. The phase composition was characterized by means of XRD and the surface area and pore size were estimated using Brunauer–Emmett–Teller (BET) and Barrett–Joyner–Halenda (BJH) methods. At the beginning of the reaction, catalysts were significantly deactivated due to the accumulation of intermediates on the catalyst surface and after 60 minutes it turned stable. Ni/Pd/AlOOH catalyst showed the highest steady-state activity in comparison with the Ni/Pd/SiO2 and Ni/Pd/Al2O3 catalysts. Their activity depends on the ozone decomposition potential of the catalysts because of generating oxidizing active species. The sample with the highest ozone decomposition ability which correlated to the surface area of the support oxidizes benzene to the highest extent.
Abstract: Single-walled carbon nanotubes (SWCNTs) are generally synthesized by chemical vapor deposition (CVD) using Fe, Co, and Ni as catalysts. However, due to the Ostwald ripening of metal catalysts, the diameter distribution of the grown SWCNTs is considerably wide (>2 nm), which is not suitable for electronics applications. In addition, reduction in the growth temperature is desirable for fabricating SWCNT devices compatible with the LSI process. Herein, we performed SWCNT growth by alcohol catalytic CVD using platinum-group metal catalysts (Pt, Rh, and Pd) because these metals have high melting points, and the reduction in the Ostwald ripening of catalyst particles is expected. Our results revealed that web-like SWCNTs were obtained from Pt and Rh catalysts at growth temperature between 500 °C and 600 °C by optimizing the ethanol pressure. The SWCNT yield from Pd catalysts was considerably low. By decreasing the growth temperature, the diameter and chirality distribution of SWCNTs from Pt and Rh catalysts became small and narrow. In particular, the diameters of most SWCNTs grown using Pt catalysts were below 1 nm and their diameter distribution was considerably narrow. On the contrary, SWCNTs can grow from Rh catalysts even at 300 °C by optimizing the growth condition, which is the lowest temperature recorded for SWCNT growth. Our results demonstrated that platinum-group metals are useful for the growth of small-diameter SWCNTs and facilitate low-temperature growth.
Abstract: This study investigates the in-situ regeneration of deactivated Pt-Pd catalyst in a laboratory-scale catalysis reactor. Different regeneration conditions are tested and the activity and characteristics of regenerated catalysts are analyzed. Experimental results show that the conversion efficiencies of C3H6 by different regenerated Pt-Pd catalysts were significantly improved from 77%, 55% and 41% to 86%, 98% and 99%, respectively. The best regeneration conditions was 52ppm ozone, 500oC, and 10min. Regeneration temperature has more influences than ozone concentration and regeneration time. With the comparisons of characteristics of deactivated catalyst and regenerated catalyst, the major poison species (carbon, metals, chloride, and sulfate) on the spent catalysts can be effectively removed by ozone regeneration.
Abstract: The supported Pd catalysts were analyzed by X-ray
diffraction and X-ray absorption spectroscopy in order to determine
their global and local structure. The average particle size of the
supported Pd catalysts was determined by X-ray diffraction method.
One of the main purposes of the present contribution is to focus on
understanding the specific role of the Pd particle size determined by
X-ray diffraction and that of the support oxide. Based on X-ray
absorption fine structure spectroscopy analysis we consider that the
whole local structure of the investigated samples are distorted
concerning the atomic number but the distances between atoms are
almost the same as for standard Pd sample. Due to the strong
modifications of the Pd cluster local structure, the metal-support
interface may influence the electronic properties of metal clusters
and thus their reactivity for absorption of the reactant molecules.
Abstract: Palladium-catalyzed hydrodechlorination is a
promising alternative for the treatment of environmentally relevant
water bodies, such as groundwater, contaminated with chlorinated
organic compounds (COCs). In the aqueous phase
hydrodechlorination of COCs, Pd-based catalysts were found to have
a very high catalytic activity. However, the full utilization of the
catalyst-s potential is impeded by the sensitivity of the catalyst to
poisoning and deactivation induced by reduced sulfur compounds
(e.g. sulfides). Several regenerants have been tested before to recover
the performance of sulfide-fouled Pd catalyst. But these only
delivered partial success with respect to re-establishment of the
catalyst activity. In this study, the deactivation behaviour of
Pd/Al2O3 in the presence of sulfide was investigated. Subsequent to
total deactivation the catalyst was regenerated in the aqueous phase
using potassium permanganate. Under neutral pH condition,
oxidative regeneration with permanganate delivered a slow recovery
of catalyst activity. However, changing the pH of the bulk solution to
acidic resulted in the complete recovery of catalyst activity within a
regeneration time of about half an hour. These findings suggest the
superiority of permanganate as regenerant in re-activating Pd/Al2O3
by oxidizing Pd-bound sulfide.