Abstract：
:Supercritical water oxidation (SCWO) of 2-, 3- and 4-nitroaniline (NA) was investigated under residence time of 1-6 min, pressure of 18-26 MPa, temperature of 350-500 °C, with initial concentration of 1 mM and 300% excess oxygen. Among these operating conditions, temperature and residence time played a more significant role in decomposing TOC and TN than pressure. Moreover, the products of N-containing species were mainly N2, ammonia and nitrate. When temperature, pressure and retention time enhanced, the yields of NO3- and org-N were reduced, the amount of N2 was increasing, the proportion of NH4+, however, presented a general trend from rise to decline in general. The experiment of aniline/nitrobenzene indicated that TN removal behavior between amino and nitro groups would prefer to happen in the molecule rather than between the molecules, therefore, the smaller interval between the amino and nitro group was the more easily to interreact. This might explain the reason why TN removal efficiency was in an order that 2-NA > 3-NA > 4-NA. The NH4+/NO3- experiment result demonstrated that ammonia and nitrate did convert into N2 during SCWO, however, the formation of N2 was little without auxiliary fuel. Density functional theory (DFT) method was used to calculate the molecular structures of 2-, 3- and 4-NA to further explore reaction mechanism, which verified that amino group was more easily to be attacked than nitro group. Based on these results, the conceivable reaction pathways of 2-, 3- and 4-NA were proposed, which contained three parts, namely denitrification, ring-open and mineralization.
journal_name
Chemospherejournal_title
Chemosphereauthors
Yang B,Cheng Z,Fan M,Jia J,Yuan T,Shen Zdoi
10.1016/j.chemosphere.2018.04.029subject
Has Abstractpub_date
2018-08-01 00:00:00pages
426-432eissn
0045-6535issn
1879-1298pii
S0045-6535(18)30671-4journal_volume
205pub_type
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