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Abstract: Unsupported catalysts show great promise for the production of nanocarbon material. This study aims to investigate the formation of carbon nanofibres from the pyrolysis of acetylene using a non-porous mesh as a catalyst. Our results showed that temperature and total gas flow rate have significant effects on the formation of carbon nanofibres on the non-porous Ni mesh catalyst. Opposite effects of gas flow rate on the yield of carbon on Ni mesh surface were observed for the pyrolysis of acetylene at low (620°C) and high (750°C) temperature. Analysis of carbon nanofibres using scanning electron microscopy, FT-Raman spectroscopy and thermogravimetric analysis showed that the structural ordering in the produced carbon changed with the yield of carbon. [Copyright &y& Elsevier]

Abstract: In a typical industrial catalyst, a small amount of catalytically active species is finely dispersed inside a large amount of porous support material. The reactor volume is mainly occupied by the catalyst support, not by the catalytic species itself. The use of fluidised nanoparticles as catalyst without the need of a support may result in drastic reduction in catalytic reactor volume for major savings in capital and operating costs. Here we report for the first time the use of fluidised NiO nanoparticles to catalyse ethane–oxygen reaction at temperatures of 240–420°C. Our data indicate that the fluidised NiO nanoparticles exhibit very different characteristics from the traditional porous catalyst. The lack of a rigid porous structure in the fluidised NiO nanoparticle catalyst allows ethyl radicals to desorb from the catalyst surface into the gas phase to initiate further gas-phase radical chain reactions. Therefore, the ethane–oxygen reaction catalysed by the fluidised NiO nanoparticles shows some typical behaviour of gas-phase reactions. In contrast, the rigid porous structure in the NiO/SiO2 catalyst does not allow the radicals to desorb from catalyst surface into the bulk gas phase. [Copyright &y& Elsevier]

Abstract: The catalytic reactions between O2 and hydrocarbons are an important class of reactions in energy and chemical industries. This study aims to investigate the complicated reactions involving reactive radicals on the catalyst surface and in the gas phase during the partial oxidation/combustion of light alkanes. In order to avoid intra-particle transport constraints associated with the traditional porous catalysts, a non-porous nickel mesh catalyst has been used in this study for the partial oxidation of ethane with O2 at 625°C at atmospheric pressure. The catalytic effects of the nickel mesh strongly depended on the flow rate of gas reactants passing through the mesh. At a low gas flow rate, the nickel mesh catalyst showed negative effects for the oxidation of ethane. At a high gas flow rate, the same catalyst showed positive catalytic effects. Our results can be explained by considering the selective/preferential adsorption and desorption of different radicals onto and from the catalyst surface. It is believed that the desorption of some surface generated radicals (e.g. OH radicals) may be greatly affected by the thickness of the mass transfer gas film around the mesh wires, which in turn is affected by the gas flow rate passing through the mesh. [Copyright &y& Elsevier]

Highlights • Effect of pre-reforming by Fe/bio-char catalyst on bio-oil reforming was studied. • Fe/bio-char pre-reforming increases the H 2 and CO yields from bio-oil reforming. • Fe/bio-char catalyst promotes the transformation of aromatics into light compounds. • Less coke was formed on Ni-based catalyst due to Fe/bio-char catalyst at 550–600 °C. • Pre-reforming promotes the formation of NiO and NiAl 2 O 4 on Ni-based catalyst. Abstract Ni-based catalyst is prone to the deactivation by coke deposition during the catalytic steam reforming of bio-oil. In order to optimize catalytic activity of the Ni-based catalyst, a two-stage catalytic reforming scheme was proposed whereby a low-temperature (350–600 °C) pre-reforming process with a less expensive catalyst was introduced prior to the Ni-based catalyst. To study this scheme, the reforming experiments with different combinations of Fe/bio-char (in the first stage) and Ni-Ca/γ-Al 2 O 3 (in the second stage) were conducted. In addition to the quantification of product yields, the tar and gas were characterized with an ultraviolet (UV) fluorescence spectroscopy, a gas chromatography/mass spectrometer (GC/MS) and a gas chromatography (GC). The results indicate that significant proportions of naphthalenes and polycyclic aromatics in the intermediate volatiles turned into furans, phenols and non-aromatics, which are easier to be reformed on Ni-based catalysts, via the Fe/bio-char pre-reforming, resulting in the increase of the final H 2 and CO yields of the overall process. At high pre-reforming temperatures (550–600 °C), the coke formation on Ni-based catalyst was significantly inhibited due to the Fe/bio-char pre-reforming. In addition, the results indicate that the spent Ni-based catalyst had more free NiO and NiAl 2 O 4 spinel than the fresh one, suggesting that the increase in the catalytic activity of Ni-based catalyst during the reforming process was promoted by Fe/bio-char pre-reforming. [ABSTRACT FROM AUTHOR]

This study investigated the interaction of nickel species with alumina versus calcination temperature and nickel loading. A total of 22 Ni/Al 2 O 3 catalysts, calcined at the temperature from 500 to 1000 °C at a 50 °C increment, were employed for the study. High calcination temperature led to the formation of nickel–alumina spinel via the solid phase reaction, which shifted the reduction temperature to higher ranges. The catalyst, however, still achieved good activity after full reduction of the nickel–alumina spinel. Nevertheless, the high calcination temperature led to the collapse of the small pores and the formation of the big one, resulting in the significant decrease of specific surface area. At higher nickel loadings, more nickel species weakly interacted with alumina formed as the reactive center of alumina was saturated. With the increase of nickel loading, the catalytic activities were not varied much but the catalytic stability and the resistivity towards coking enhanced. The coke produced over the catalyst at low nickel loading tended to be amorphous, while the coke produced at the high nickel loading was more fibrous. Furthermore, the coke produced at the low loading contained more small aromatic rings and more oxygen-containing functional groups. The higher nickel loading possibly promoted the catalytic cracking reactions to form more catalytic coke while the low nickel loading probably favored the polymerization reactions to form the polymeric coke. In addition, the calcination at the higher temperature could enhance the stability of the catalysts, which might be related to the enlarged pore sizes. [ABSTRACT FROM AUTHOR]

Ni-based catalysts are prone to be deactivated by carbon deposition. This study aims to investigate the influence mechanism of different types of carbon deposition on the activity of Ni/α-Al 2 O 3 catalyst at various steam-to-carbon (S/C) ratios during steam reforming of toluene for hydrogen production. At a low S/C ratio of 1, the catalytic activity of Ni/α-Al 2 O 3 was inhibited due to the covering and blocking of Ni active sites by the formation of amorphous carbon on the Ni surface. While at a high S/C ratio of 3, more than 80 wt% of carbon deposition was found to be self-growth carbon nanotubes (CNTs) with an average diameter of around 15 nm. The activity of Ni/α-Al 2 O 3 in steam reforming of toluene was unusually promoted, which can be attributed to the tip-growth mechanism of CNTs, whereby the Ni particles migrated to the tip or the surface of CNTs, resulting in the improved active site dispersion. [ABSTRACT FROM AUTHOR]