Novel insights into the control of N-nitrosodimethylamine (NDMA) and bromate formation during heterogeneous catalytic ozonation
Novel insights into the control of N-nitrosodimethylamine (NDMA) and bromate formation during heterogeneous catalytic ozonation
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DOI：
10.1016/j.cej.2023.145913
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发表时间：
2023-09
影响因子：
15.1
通讯作者：
Yang Song;Jianshan Peng;Ziquan Zhao;Wen Qin;Jin Jiang;Jun Ma
中科院分区：
文献类型：
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作者：
Yang Song;Jianshan Peng;Ziquan Zhao;Wen Qin;Jin Jiang;Jun Ma
n -亚硝基二甲胺（NDMA）和溴酸盐（BrO3-）是臭氧氧化过程中存在的消毒副产物，亟待解决。本研究以O3/Al2O3、O3/MnOx/Al2O3和O3/β-FeOOH/Al2O3为研究对象，研究了臭氧氧化daminozide （DMZ）和Br-对NDMA和bro3生成的控制作用。在不添加丁醇（TBA）的情况下，随着臭氧剂量（20 ~ 100 μM）的增加，NDMA生成量从0.66 μM下降到0.37 μM。在O3/ al2o3过程中（0.55 ~ 0.21 μM） NDMA的生成控制效率更高，这是由于羟基自由基（•OH）产率高，而在O3/MnOx/ al2o3和O3/β-FeOOH/ al2o3过程中NDMA的生成变化几乎可以忽略（分别为~ 0.63 μM和~ 0.65 μM）。不同浓度的Br-、HCO3 -、单宁酸和腐植酸均影响NDMA的形成，这与臭氧或•OH的竞争有关。在臭氧化过程中，催化剂的加入可以有效控制HOBr分解生成的bro3以及催化剂对bro3的吸附或还原作用。臭氧氧化对bro3生成的控制效率依次为O3/β-FeOOH/Al2O3> O3/MnOx/Al2O3> O3/Al2O3>。在不含Br-的实际水样中，在催化剂的存在下观察到NDMA的显著控制。在含Br-的实际水样中，催化剂的存在和不存在都降低了NDMA的生成，并且在O3/Al2O3、O3/MnOx/Al2O3和O3/β-FeOOH/Al2O3过程中对bro3的生成有很大的控制能力。因此，可以利用催化剂的添加来控制臭氧化过程中的消毒副产物。
N-nitrosodimethylamine (NDMA) and bromate (BrO3-) have been found to be disinfection by-products during ozonation, which need to be solved urgently. In this study, O3/Al2O3, O3/MnOx/Al2O3and O3/β-FeOOH/Al2O3were used to investigate the control of NDMA and BrO3-formation during the ozonation of daminozide (DMZ) and Br-. During ozonation alone, NDMA formation decreased from 0.66 to 0.37 μM with increasing ozone dosages (20–100 μM) withouttert-butanol (TBA). Greater control efficiency for NDMA formation was observed during the O3/Al2O3process (0.55–0.21 μM), which was attributed to the high hydroxyl radical (•OH) yield, and NDMA formation during the O3/MnOx/Al2O3and O3/β-FeOOH/Al2O3processes changed negligibly (∼0.63 and ∼ 0.65 μM, respectively). The formation of NDMA was affected by different concentrations of Br-, HCO3–, tannic acid, and humic acid, which was attributed to the competition for ozone or •OH. During ozonation process, the addition of catalysts could effectively control BrO3-formation due to the decomposition of HOBr and the adsorption or reduction of BrO3-by catalysts. The control efficiencies of BrO3-formation were in the order of O3/β-FeOOH/Al2O3> O3/MnOx/Al2O3> O3/Al2O3> ozonation alone. In a real water sample without Br-, significant control of NDMA was observed in the presence of the catalysts. In a real water sample containing Br-, NDMA formation decreased in the presence and absence of catalysts, and a great control capacity for BrO3-formation was exhibited during the O3/Al2O3, O3/MnOx/Al2O3and O3/β-FeOOH/Al2O3processes. Therefore, the addition of catalysts can be utilized to control disinfection by-products during ozonation.