Mechanism of catalytic subcritical water oxidation of m-nitroaniline and nitrogen conversion by CuCo2O4 catalyst

Abstract

Catalytic subcritical water oxidation (CSWO) of M−nitroaniline (M−NA) was investigated in a fused quartz tube reactor (FQTR) to determine the effects of reaction parameters on M−NA mineralization rate, total nitrogen (TN) removal rate and nitrogen-containing products distribution. The results indicated that the TN removal rate was only 26.36 % at 200 °C, 200 % excess oxidant and 15 min residence time, while the TN removal rate reached 67.83 % at 360 °C in SWO of M−NA. Compared with SWO of M−NA, the mineralization rate and TN removal rate of CSWO of M−NA increased by about 10 % and 17.83 %, respectively. The main reason is mainly attributed to CuCo2O4 catalyzing the preferential reaction of ·NO2 with ·NH4, hastening N2 generation. Alternatively, the CuCo2O4 catalyst may induce a direct reaction between the nitro and amino groups on M−NA within the benzene ring to form N2. Moreover, degradation pathways and nitrogen migration mechanism of M−NA under SWO/CSWO conditions were proposed. These crucial findings are expected to guide the development of environmentally sustainable catalytic technologies towards addressing significant water pollution challenges.