School of Civil and Transportation Engineering, Guangdong University of Technology, Guangzhou 510006, Guangdong, China.
School of Civil and Transportation Engineering, Guangdong University of Technology, Guangzhou 510006, Guangdong, China.
J Hazard Mater. 2023 Jun 15;452:131374. doi: 10.1016/j.jhazmat.2023.131374. Epub 2023 Apr 6.
N-nitrosodimethylamine (NDMA) is formed during ozonation of model compounds with dimethylhydrazine groups, such as daminozide (DMZ) and 2-furaldehyde 2,2-dimethylhydrazone (2-F-DMH) at pH 7 with yields of 100 % and 87 %, respectively. In this study, ozone/hydrogen peroxide (O/HO) and ozone/peroxymonosulfate (O/PMS) were investigated to control NDMA formation, and O/PMS (50-65 %) was more effective than O/HO (10-25 %) with a ratio of HO or PMS to O of 8:1. The reaction of PMS or HO to decompose ozone could not compete with the ozonation of model compound because of the high second-order rate constants of the ozonation of DMZ (5 ×10 M s) or 2-F-DMH (1.6 ×10 M s). The R value of the sulfate radical (SO) showed a linear relationship with NDMA formation, indicating that SO significantly contributed to its control. NDMA formation could be further controlled by injecting small quantities of ozone numerous times to minimize the dissolved ozone concentration. The effects of tannic acid, bromide and bicarbonate on NDMA formation were also investigated during ozonation, O/HO, and O/PMS processes. Bromate formation was more pronounced in the O/PMS process than in the O/HO process. Therefore, in practical applications of O/HO or O/PMS processes, the generation of NDMA and bromate should be detected.
N-亚硝基二甲胺(NDMA)是在 pH 值为 7 时,用臭氧氧化具有二甲肼基团的模型化合物,如二甲肼(DMZ)和 2-糠醛 2,2-二甲基腙(2-F-DMH)时形成的,产率分别为 100%和 87%。在本研究中,考察了臭氧/过氧化氢(O/HO)和臭氧过一硫酸盐(O/PMS)对控制 NDMA 形成的效果,O/PMS(50-65%)比 O/HO(10-25%)更有效,HO 或 PMS 与 O 的比例为 8:1。由于 DMZ(5×10M s)或 2-F-DMH(1.6×10M s)的臭氧氧化的二级速率常数较高,PMS 或 HO 分解臭氧的反应无法与模型化合物的臭氧氧化竞争。硫酸根自由基(SO)的 R 值与 NDMA 形成呈线性关系,表明 SO 对其控制作用显著。通过多次注入少量臭氧来最小化溶解臭氧浓度,可进一步控制 NDMA 的形成。还在臭氧氧化、O/HO 和 O/PMS 过程中考察了没食子酸、溴化物和碳酸氢盐对 NDMA 形成的影响。在 O/PMS 过程中,溴酸盐的形成比在 O/HO 过程中更为明显。因此,在实际应用中,应检测 O/HO 或 O/PMS 过程中 NDMA 和溴酸盐的生成。