Surface and catalytic elucidation of Rh/gamma-Al2O3 catalysts during NO reduction by C3H8 in the presence of excess O2, H2O, and SO2.

The present study aims at exploring the surface and catalytic behavior of Rh/gamma-Al(2)O(3) catalysts during the selective reduction of NO by C(3)H(8) in the presence of excess oxygen, H(2)O, and SO(2) with particular emphasis on identifying the elementary steps that describe the reaction mechanism. To this end, detailed activity and stability tests were employed and a precise kinetic analysis was carried out at differential conditions to elucidate the effect of each reactant, including H(2)O and SO(2), on the total reaction rate. At the same time, temperature programmed desorption (TPD) studies in combination with in situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy were carried out under various reaction conditions to correlate the catalytic performance of Rh/gamma-Al(2)O(3) catalyst with its corresponding surface chemistry. The results reveal that in the absence of H(2)O and SO(2), the reaction follows a typical "reduction" type mechanism, where the active intermediates (NO(X), carboxylates, isocyanates) are interacting to yield the final products. In this reaction sequence the formation of carboxylate (C(x)H(y)O(z)) species is considered as the rate determining step. Water affects in a different way the NO and C(3)H(8) conversion performance of Rh/gamma-Al(2)O(3) catalyst; its effect is totally reversible in the case of C(3)H(8) oxidation, while the NO reduction was permanently affected mainly due to the oxidation of Rh active sites. In contrast, SO(2) poisons both reactions irreversibly via the formation of strongly adsorbed sulfate compounds, which hinder the adsorption and consequently the activation of reactants.

NO reduction by propene or CO over alkali-promoted Pd/YSZ catalysts.

The catalytic activity and selectivity of Pd dispersed on 8mol% yttria stabilized zirconia (YSZ) support for the reduction of NO by propene or CO is strongly promoted by alkalis in a wide temperature range 200-500 degrees C. Rate increases by up to one order of magnitude are achievable, accompanied with significant improvement in N(2)-selectivity for the alkali promoted catalysts. The promoting effect of alkalis on both the activity and selectivity can be understood in terms of the effect of alkali promoter on the relative adsorption strengths of reactant species. These achievements could be very useful for the formulation of modern lower cost automotive catalytic converters, capable of controlling automotive emissions more efficiently.

Methane to ethylene with 85 percent yield in a gas recycle electrocatalytic reactor-separator.

Methane was oxidatively coupled to ethylene with an ethylene yield up to 85 percent and a total C(2) hydrocarbon yield up to 88 percent in a gas recycle high-temperature (800 degrees C) electrocatalytic or catalytic reactor where the recycled gas passes continuously through a molecular sieve trap in the recycle loop. Oxygen is supplied either electrocatalytically by means of the solid electrolyte support of the silver-based catalyst or in the gas phase. The C(2) products are obtained by subsequent heating of the molecular sieve trap. The selectivity to ethylene is up to 88 percent for methane conversion up to 97 percent.