当前位置: X-MOL 学术Sep. Purif. Technol. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Degradation of Congo red by UV photolysis of nitrate: Kinetics and degradation mechanism
Separation and Purification Technology ( IF 8.6 ) Pub Date : 2021-01-12 , DOI: 10.1016/j.seppur.2020.118276
Shishun Wang , Congwei Luo , Fengxun Tan , Xiaoxiang Cheng , Qiao Ma , Daoji Wu , Peijie Li , Fumiao Zhang , Jun Ma

The efficiency of Congo red (CR) removal by low-pressure ultraviolet photolysis of nitrate (UV/NO3) process was investigated in this study. Results showed that CR degradation through direct UV (254 nm) photolysis could be ignored, but CR was obviously removed in UV/NO3 process. Moreover, the contributions of UV, radical dotNO2 and radical dotOH to the degradation of CR were explored to be roughly 0.63%, 17.46% and 81.90%, respectively. In addition, the observed pseudo-first-order rate constants for the degradation of CR (kobs) were assessed by the effects of different water matrices and operation conditions, including NO3 dosage, CR concentration, solution pH, chloride ion (Cl), natural organic matter (NOM) and carbonate/bicarbonate (CO32−/HCO3). The kobs was increased by nearly 12.9 times with the addition of NO3 dosage from 1 mM to 200 mM due to the generation of more active components (e.g., radical dotOH and radical dotNO2). Higher doses of CR reduced the kobs, which could be attributed to the filter effects of CR on UV irradiation. Although the photolysis of NO3 could be expedited under acidic conditions, the kobs was decelerated because of the protonation of CR (pKa = 4.1, 25 °C). While in alkaline conditions, the kobs was also reduced as the decrease in redox potential of radical dotOH. The presence of Cl (0–7 mM) exhibited no scavenging effect on the kobs, which suggested the secondary radicals (i.e., chlorine radicals (e.g., Clradical dot, Cl2radical dot)) could oxidize CR effectively. NOM restricted the degradation of CR significantly, resulting from the filter effects of NOM (ε = 0.11 Lradical dotmgC−1radical dotcm−1) on UV and the effects of radical scavenging. The kobs was improved obviously with the participation of CO32−/HCO3 (0–7 mM), ascribing to the oxidation of carbonate radical (CO3radical dot) and the increased steady state concentration of radical dotNO2. The degradation of CR in UV/NO3 process has the potential for practical applications in real water. Furthermore, eight intermediates were proposed by Liquid chromatography-tandem mass spectrometry (LC-MS/MS). Hydroxylation, nitrification and other aromatic products in the reaction of CR with radical dotOH and/or radical dotNO2 were readily produced by H-abstraction, addition reaction and electron transfer.



中文翻译:

硝酸盐的紫外光解降解刚果红:动力学和降解机理

刚果红效率通过低压(CR)去除硝酸盐的紫外光解(UV / NO 3 - )处理在本研究中调查。结果表明,通过直接UV CR降解(254纳米)光解可以忽略不计,但在CR UV / NO明显除去3 -过程。此外,UV,激进点NO 2激进点OH对CR降解的贡献分别约为0.63%,17.46%和81.90%。此外,通过不同水基质和操作条件(包括NO 3-)的影响,评估了观察到的CR降解的拟一级反应速率常数(k obs剂量,CR浓度,溶液的pH值,氯离子(CL - ),天然有机物质(NOM)和碳酸盐/碳酸氢盐(CO 3 2- / HCO 3 - )。所述ķ OBS通过加入NO的增加近12.9倍3 -剂量从1 mM到200mM的由于多种活性成分(例如,产生激进点OH和激进点NO 2)。较高剂量的CR可降低k obs,这可能归因于CR对紫外线辐射的滤光效果。虽然NO的光解3 -可以酸性条件下,下加快ķ OBS由于CR的质子传递而使d减速(pKa = 4.1,25°C)。在碱性条件下,随着OH氧化还原电位的降低,k obs也降低激进点。氯的存在-(0-7毫米)显示出在没有清除作用ķ OBS,这表明辅助基团(即,氯自由基(例如Cl 激进点,氯2 激进点- ))可有效地氧化CR。NOM显着限制了CR的降解,这归因于NOM对UV的过滤作用(ε  = 0.11 L 激进点mgC -1激进点 cm -1)和自由基清除的作用。该ķ OBS用CO的参与明显提高3 2- / HCO 3 -(0-7毫米),归咎于到的碳酸根(CO氧化3 激进点- )和增加的稳态浓度激进点NO 2。CR的在UV / NO的降解3 -过程具有用于实时水实际应用中的潜力。此外,通过液相色谱-串联质谱法(LC-MS / MS)提出了八种中间体。CR与激进点OH和/或激进点NO 2的反应中的羟基化,硝化和其他芳族产物很容易通过氢吸收,加成反应和电子转移而产生。

更新日期:2021-01-20
down
wechat
bug