研究报告
王敏,田秉汝,潘晓雪,李玉成,王遵尧.高铁酸盐对丁基羟基茴香醚的去除效果和机理研究[J].环境科学学报,2022,42(4):131-140
高铁酸盐对丁基羟基茴香醚的去除效果和机理研究
- The removal performance and mechanisms of aqueous butylated hydroxyanisole (BHA) by Fe(VI)
- 基金项目:国家自然科学基金青年项目(No.22106001);水源涵养和生态保育清洁小流域技术综合集成应用推广(No.2017ZX07603002)
- 王敏
- 安徽大学资源与环境工程学院,合肥 230601;安徽大学湿地保护与生态恢复重点实验室,合肥 230601
- 田秉汝
- 南京大学环境学院污染控制与资源化国家重点实验室,南京 210023
- 潘晓雪
- 安徽大学资源与环境工程学院,合肥 230601;安徽大学湿地保护与生态恢复重点实验室,合肥 230601
- 李玉成
- 安徽大学资源与环境工程学院,合肥 230601;安徽大学湿地保护与生态恢复重点实验室,合肥 230601
- 王遵尧
- 南京大学环境学院污染控制与资源化国家重点实验室,南京 210023
- 摘要:通过研究高铁酸盐(Fe(VI))对丁基羟基茴香醚(BHA)的去除效果和机理,阐明这种广泛使用的抗氧化剂在水处理中的转化归趋.详细考察了溶液pH值、氧化剂量、BHA初始浓度、常见阴阳离子、腐殖酸(HA)和实际水质对其去除效果的影响.结果表明Fe(VI)可高效去除水中BHA,升高pH值、增加氧化剂投加量及分批投加Fe(VI),对BHA去除率更高.当pH= 9.0时,分别于0和30 s分两次投加100 μmol·L-1的Fe(VI)可将50 μmol·L-1 BHA在60 s内完全去除.体系中离子Cl-、HSO3-、NO2-、Ca2+、Cu2+、Fe3+和腐殖酸(HA)的存在则会抑制底物的降解,且Cl-、HSO3-和Ca2+的抑制效果随着添加浓度的升高而增强;而NO3-和HCO3-则无明显影响.特别的是,Mg2+(0.5 mmol·L-1)和NH4+(0.5和5 mmol·L-1)对BHA的去除起到一定的促进作用.此外,BHA在实际水质如自来水、河水、二沉池出水和合成废水中相对高的去除率(55% ~ 70%)进一步展示出Fe(VI)的实际应用能力.LC-MS和理论计算结果指出Fe(VI)氧化BHA的机理包括氧转移和抽氢反应,而大量聚合物的生成使溶液矿化度仅约20%.本研究可为水和废水中BHA类抗氧化剂的去除和环境归趋提供一定理论依据.
- Abstract:In this work, the removal performance and mechanism of butylated hydroxyanisole (BHA) by Fe(VI) were investigated to clarify the trend and final fate of this widely used antioxidant in water treatment processes. The effects of various environmental factors (i.e., solution pH, oxidant dose, initial concentration of BHA, common anions and cations, humic acid, and different water matrices) on the removal of BHA were systematically investigated. Results showed the high removal efficiency of BHA by Fe(VI), which could be improved with the increase in solution pH, oxidant dosage, and multiple additions of Fe(VI). After the additions of 100 μmol·L-1 Fe(VI) at 0 and 30 s, 50 μmol·L-1 of BHA could be completely removed within 60 s at pH 9.0. However, typical ions (Cl-, HSO3-, NO2-, Ca2+, Cu2+, Fe3+) and HA in the degradation system could inhibit the removal of BHA; and these inhibitory effects could be enhanced as the concentrations of Cl-, HSO3-, and Ca2+ were elevated. While other ions, i.e., NO3- and HCO3- exerted no significant influence on the removal of BHA. Specifically, both Mg2+ (0.5 mmol·L-1) and NH4+ (0.5 and 5 mmol·L-1) played positive roles in the elimination of the substrate to some extent. In addition, the relatively high removal efficiencies of BHA (55%~70%) in real water samples such as tap water, river water, secondary clarifier effluent and synthetic wastewater further demonstrated the ability of Fe(VI) in practical applications. The results of LC-MS data and theoretical calculation demonstrated that Fe(VI) mainly oxidized BHA by H abstraction reaction and oxygen transfer. Due to the generation of large amounts of BHA polymers, there were only ~20% mineralization degree of reaction solution. Our findings can provide some theoretical foundation for the treatment, trend and fate of BHA-like antioxidants in water and wastewater.