Diesel fuel desulfurization with hydrogen peroxide promoted by formic acid and catalyzed by activated carbon

摘要

Desulfurization of diesel fuels with hydrogen peroxide was studied using activated carbons as the catalysts. Adsorption and catalytic properties of activated carbons for dibenzothiophene (DBT) were investigated. The higher the adsorption capacity of the carbons is, the better the catalytic performance in the oxidation of DBT is. The effect of aqueous pH on the catalytic activities of the activated carbons was also investigated. Oxidation of DBT is enhanced when the aqueous pH is less than 2, and addition of formic acid can promote the oxidation. The effect of carbon surface chemistry on DBT adsorption and catalytic activity was also investigated. Adsorption of DBT shows a strong dependence on carboxylic group content. The oxidative removal of DBT increases as the surface carbonyl group content increases. Oxidative desulfurization of a commercial diesel fuel (sulfur content, 800 wt. ppm) with hydrogen peroxide was investigated in the presence of activated carbon and formic acid. Much lower residual sulfur content (142 wt. ppm) was found in the oxidized oil after the oxidation by using the hydrogen peroxide-activated carbon formic acid system, compared with a hydrogen peroxide-formic acid system. The resulting oil contained 16 wt. ppm of sulfur after activated carbon adsorption without any negative effects in the fuel quality, and 98 of sulfur could be removed from the diesel oil with 96.5 of oil recovery. Activated carbon has high catalytic activity and can be repeatedly used following simple water washing, with little change in catalytic performance after three regeneration cycles. (C) 2005 Elsevier Ltd. All rights reserved.