UV/H2O2对化工废水中2 6-二氯吡啶的降解研究
2021-03-24谷振超邬东陈莉荣
谷振超 邬东 陈莉荣



摘 要:含氮杂环化合物随着化工行业的发展不断进入环境中,增加了对生态环境的威胁.考察了UV/H2O2对化工废水中含氮杂环化合物2,6-二氯吡啶(2,6-DCLPY)的降解特征,降解过程中的2,6-DCLPY浓度通过紫外分光光度法测定;并对2,6-DCLPY降解反应的影响因素包括初始2,6-DCLPY浓度、H2O2浓度、pH和共存阴离子等进行了研究. 结果表明:2,6-DCLPY 在UV/H2O2体系下的降解符合准一级反应动力学,该体系中羟基自由基(·OH)是降解2,6-DCLPY的主要活性物质,UV起协同作用;随着H2O2用量的提高,2,6-DCLPY的降解效率也逐渐提高,当H2O2和2,6-DCLPY的投加摩尔比为37 ∶ 1,pH为7.2时达到最高降解率77.3%. 共存阴离子HCO-3和NO-3因能与·OH直接发生反应,对降解反应有显著的抑制作用.吡啶环上存在氨基等给电子基团有利于吡啶类污染物的降解,而氯等吸电子基团会抑制吡啶类污染物的降解.
关键词:光催化;UV/H2O2;2,6-二氯吡啶;含氮杂环化合物;羟基自由基
Abstract:With the development of the chemical industry, nitrogen-containing heterocyclic compounds constantly enters the environment, which increases the threat to the ecological environment. The degradation characteristics of the nitrogen-containing heterocyclic compounds 2,6-dichloropyridine(2,6-DCLPY) in chemical wastewater by UV/H2O2 were investigated, and the concentration of 2,6-DCLPY in the degradation process was determined by ultraviolet spectrophotometry. The influencing factors of 2,6-DCLPY degradation reaction including initial 2,6-DCLPY concentration,H2O2 concentration, pH and coexisting anions were studied. The results showed that the degradation of 2,6-DCLPY under UV/H2O2 system accorded with quasi-first-order reaction kinetics. Hydroxyl radical(·OH) was the main active substance for degradation of 2,6-DCLPY, while UV played a synergistic effect. The degradation efficiency of 2,6-DCLPY gradually increased with the increasing H2O2 dosage, and the highest degradation rate could reach 77.3% when the molar ratio of H2O2 and 2,6-DCLPY was 37 ∶ 1 and the pH was 7.2. The coexisting anions HCO3- and NO3- can directly react with ·OH, which leaded to significant inhibitory effect on the degradation reaction. The presence of electron-donating groups such as amino groups on the pyridine ring is conducive to the degradation of pyridine pollutants,while electron-withdrawing groups such as chlorine inhibits the degradation of pyridine pollutants.
Key words:photocatalysis;UV/H2O2;2,6-dichloropyridinr;nitrogen-containing heterocyclic compound;hydroxyl radicals
2,6-二氯吡啶(2,6-DCLPY)是一種应用广泛的含氮杂环化合物,不仅是许多杀菌剂、香料和特定农医药物的基本原料[1],还经常作为染料、树脂和部分精细化学品生产过程中的溶剂使用[2]. 因此,它普遍存在于焦化废水、医药废水和精细化工等工业废水中[3-7]. 这些化工废水中的2,6-DCLPY因结构中含有难降解的吡啶环结构并具有较强的生物毒性,难以被一般物化处理工艺或生化手段去除[8-9]. 此外,它具有较强的水溶性和生物活性,可以在土壤、水体和沉积物中迁移和富集,对生态安全构成直接威胁[10]. 已经从包括北海(0.07 ng/L)、英国沿海(0.13 ng/L)、易北河(8.76 ng/L)等……
