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Hydrodehalogenation of chlorobenzene on activated carbon and activated carbon supported catalysts
Danilo Santoro1, Vincent de Jong, Robert Louw
1Center for Chemistry and the Environment, Leiden Institute of Chemistry, Gorlaeus Labs, Leiden University, 2300 RA Leiden, The Netherlands.
Abstract:
Chlorinated aromatic compounds in (waste) gases can be removed and/or dehalogenated by passing over a bed of activated carbon (AC) in a hydrogen containing atmosphere. Dehalogenation of the model compound chlorobenzene (PhCl) to HCl is complete at 490 degrees C--rather than the approximately 900 degrees C needed for the mere gas-phase reaction--but part of the benzene moieties is retained on the AC, resulting in its rather rapid deactivation, apparently due to a large decrease in surface area. Therefore, <1 mmol PhCl per gram of 'catalyst' could be processed. At 600 degrees C chlorobenzene yields 100% of both HCl and benzene, but still the AC lost most of its activity in time. Performances are compared of three different commercial ACs. As a HCl-washed AC is just as active, metals are not involved. This acid-washed AC was used as a support for 10 wt% Ni or Fe catalysts. While Fe did not show appreciable activity, results with Ni are promising. The yields of HCl and benzene from PhCl are approximately 100% already at T<400 degrees C, and T(50%) congruent with 260 degrees C, over 200 degrees C lower than with AC alone. There is no appreciable decrease of activity after having injected >20 mmol PhCl per gram of catalyst at partial conversion.