Abstract
Nitrogen transformation processes have an important impact on human life. In this work, the synergistic denitrification mechanism in the process of supercritical water oxidation (SCWO) was studied. N-containing organic compounds had better denitrification effects than the inorganics because they could produce more active radicals. Nitroaniline had higher total nitrogen (TN) removal rates than those of compounds containing only amino or nitro group due to the intramolecular synergistic denitrification. Meanwhile, intermolecular synergistic denitrification was found between nitro and amino/N-heterocyclic compounds, but its denitrification efficiency was not as good as intramolecular synergistic denitrification. The reaction mechanism of synergistic denitrification was proposed, which was similar to anaerobic ammonia oxidation. In addition, the overall equilibrium process of intermolecular synergistic denitrification was established. It included the rapid reduction of org-N at the early stage of SCWO process, as well as the limiting step of slow denitrification rate of NH4+ and NO3− in the late stage. The relationship between TN removal rate of mixture (kMIX-TN) and monomer compound (kNO2-TN or kNH2-TN) could be expressed by an equation, that was kMIX-TN = 3.3698 kNO2-TN·kNH2-TN + 0.0901, with R2 of 0.7788, which demonstrated that kMIX-TN was linearly related to kNO2-TN·kNH2-TN. All these works provided theoretical basis for nitrogen removal in water by SCWO technology.
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