0000000000704040
AUTHOR
E. A. Popov
From a fixed bed Ag–alumina catalyst to a modified reactor design: how to enhance the crucial heterogeneous–homogeneous reactions in HC-SCR
Abstract A highly active Ag/alumina catalyst for continuous reduction of NO to nitrogen with n-octane under lean conditions was prepared. It was observed in the reactor set-up experiments for optimization of the converter, that surface generated gas phase species are crucial for obtaining high conversion. EPR and matrix isolated FTIR studies at low temperature (10–18 K) were performed for identification of the radicals. Experimental data, observed at steady state conditions in the temperature range 300–550 °C, was used to produce an artificial neural network model of the catalytic converter with four catalyst beds.
Rotation of methyl radicals in molecular solids.
Electron spin resonance (ESR) measurements were carried out to study the rotation of methyl radicals (CH(3)) in solid carbon monoxide, carbon dioxide, and nitrogen matrices. The radicals were produced by dissociating methane by plasma bursts generated by a focused 193 nm ArF excimer laser radiation during the gas condensation on the substrate. The ESR spectra exhibit anisotropic features that persist over the temperature range examined, and in most cases this indicates a restriction of rotation about the C(2) symmetry axis. A nonrotating CH(3) was also observed in a CO(2) matrix. The intensity ratio between the symmetric (A) and antisymmetric (E) nuclear spin states was recorded as a functi…
Rotation of methyl radicals in a solid krypton matrix
Electron spin resonance (ESR) measurements were carried out to study the rotation of methyl radicals (CH(3)) in a solid krypton matrix at 17-31 K temperature range. The radicals were produced by dissociating methane by plasma bursts generated by a focused 193 nm excimer laser radiation during the krypton gas condensation on the substrate. The ESR spectrum exhibits only isotropic features at the temperature range examined, and the intensity ratio between the symmetric (A) and antisymmetric (E) spin state lines exhibits weaker temperature dependence than in a solid argon matrix. However, the general appearance of the methyl radical spectrum depends strongly on temperature due to the pronounce…
HC-SCR of NOx over Ag/alumina: a combination of heterogeneous and homogeneous radical reactions?
Matrix isolation combined with EPR and FT-IR technique at low temperature has been used to study the gas phase species involved in HC-SCR over a highly active Ag/alumina catalyst. A combination of heterogeneous and homogeneous (radical) reactions is proposed to take place over a Ag/alumina catalyst during HC-SCR. Radicals of low molecular weight were trapped in a growing argon matrix behind the Ag/alumina catalyst. In the same matrix, cyanogen isocyanate was detected and is suggested to be a key intermediate for the formation of amines and ammonia via the hydrolysis of isocyanate species.