The ozonation kinetics of oxalic acid in water in the presence of an activated carbon has been
investigated at acid pH. The presence of the activated carbon significantly enhances the
degradation rate of oxalic acid if compared to single ozonation and single adsorption. According
to total organic carbon measurements, nearly complete mineralization of oxalic acid can be
achieved depending on the experimental conditions. The presence of tert-butyl alcohol, which
scarcely adsorbs on the carbon surface at the conditions investigated, led to a significant reduction
of the oxalic acid removal rate. Consequently, experimental results suggest that the reaction
proceeds in the water phase between oxalic acid and oxidant species, likely hydroxyl radicals,
coming from the ozone decomposition on the carbon surface. The proposed mechanism yielded
a first-order kinetics with respect to ozone, close to the 0.8 order experimentally observed. Also,
the energy of activation was found to be approximately 15 kcal mol-1.
Landfill leachates of the city of Badajoz (in the southwest of Spain) have been treated by wet air oxidation at high temperature (180-270 °C) and pressure (40-70 atm). Typical operating variables such as temperature and oxygen partial pressure have been investigated with no effect of any being found and moderate to low chemical oxygen demand conversions (20-30% depending on initial COD concentration). Initial pH shows a positive influence when acidic conditions are used. Addition of hydrogen peroxide (0.01 M) as a hydroxyl radical promoter is able to provide an additional 15% increase in the final COD removal achieved. If a sulfate radical promoter is used (i.e., Oxone) the process is significantly improved, with COD conversions in the range 60-80%, also depending on the initial COD of the leachates. A first attempt to comprehend the chemistry of this oxidizing system suggests an instantaneous decomposition of Oxone that initiates the radical chain also involving hydroxyl and organic radicals.
This paper deals with the modifications of the chemical surface functionalities and the textural changes
of a glassy carbon produced by three oxidizing agents: ozone, hydrogen peroxide, and oxygen plasma. The
chemical surface changes are evaluated by using Fourier transform infrared spectroscopy, temperature-programmed desorption−mass spectrometry, and chemical titrations of the surface functionalities by
using the Boehm method. The textural modifications are studied by mercury porosimetry and by N2 and
CO2 adsorption at 77 and 273 K, respectively. Ozone is a more effective oxidizing agent than H2O2 and
oxygen plasma. It is able to introduce much larger amounts of oxygen functionalities on the surface than
the other oxidizing agents. Moreover, the textural characteristics of the original sample remain almost
unchanged after the treatments with oxygen peroxide and with oxygen plasma, while ozone produces
modifications in surface area and mesoporosity. Nevertheless, ozone modifications of surface area seem
to be partially produced by the fixation of the oxygen functionalities at the entrance of the micropores
which partially hinder the access of the adsorbates.
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