Comparison of acetaminophen degradation in UV-LED-based advance oxidation processes: Reaction kinetics, radicals contribution, degradation pathways and acute toxicity assessment
Comparison of acetaminophen degradation in UV-LED-based advance oxidation processes: Reaction kinetics, radicals contribution, degradation pathways and acute toxicity assessment
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基于 UV-LED 的高级氧化过程中对乙酰氨基酚降解的比较：反应动力学、自由基贡献、降解途径和急性毒性评估
DOI：
10.1016/j.scitotenv.2020.137993
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发表时间：
2020-06-25
影响因子：
9.8
通讯作者：
Wang, Jiping
中科院分区：
文献类型：
--
作者：
Li, Boqiang;Ma, Xiaoyan;Wang, Jiping
采用UV-LED/氯胺（UV-LED/NH2Cl）、UV-LED/过氧化氢（UV-LED/H2O2）和UV-LED/过硫酸盐（UV-LED/PS）等紫外发光二极管（UV-LED）高级氧化工艺（AOPs）去除对乙酰氨基酚（AAP）。结果表明，与单独使用紫外照射和氧化剂相比，复合处理能有效地降解AAP。3种基于UV-LED的AOPs对AAP的降解顺序为UV-LED/PS N UV-LED/H2O2 N UV-LED/NH2Cl，并遵循准一级动力学。降解速率常数（k(obs)）随氧化剂用量的增加而增加，而过量则降低了AAP的降解。HO中心点、SO4中心点-和Cl中心点在AAP作用下的二阶速率常数分别为5.15 × 10(9)、7.66 × 10(9)和1.08 × 10(10) M-1 s（-1）。在中性条件下，在UV-LED/NH2Cl体系中，UV-LED、HO中心点和Cl中心点对AAP降解的贡献分别为4.21%、60.15%和35.64%，而在UV-LED/PS体系中，UV-LED、HO中心点和SO中心点-对AAP降解的贡献分别为2.09%、22.84%和75.07%。同时，发现所涉及的反应物质的相应贡献是ph依赖性的。天然有机材料（NOM）抑制了AAP的降解，Cl-、HCO3-和NO3-的存在对3种混合过程中AAP的降解有不同的影响。三种基于uv - led的AOPs在实际水中对AAP的降解均受到显著抑制。此外，还鉴定了三种uv - led基AOPs的中间产物，并提出了可能的降解途径。采用费氏弧菌进行急性毒性生物测定，结果表明UV-LED/PS工艺比UV-LED/H2O2和UV-LED/NH2Cl工艺更能降低反应后AAP溶液的急性毒性。在3种基于UV-LED的AOPs中，UV-LED/PS是降解AAP最有效的工艺。(c) 2020 Elsevier B.V.版权所有
Ultraviolet light emitting diode (UV-LED)-based advanced oxidation processes (AOPs) including UV-LED/chloramine (UV-LED/NH2Cl), UV-LED/hydrogen peroxide (UV-LED/H2O2) and UV-LED/persulfate (UV-LED/PS), were adopted for acetaminophen (AAP) removal. Results showed that AAP could be effectively degraded by the hybrid processes compared to solely using with UV irradiation and oxidants. The AAP degradation in the three UV-LED-based AOPs were in the order of UV-LED/PS N UV-LED/H2O2 N UV-LED/NH2Cl and followed a pseudo-first-order kinetics. The degradation rate constant (k(obs)) increased with increasing oxidant dosage, whereas overdosing lowered the AAP degradation. The second-order rate constants of HO center dot, SO4 center dot-, and Cl center dot with AAP were calculated as 5.15 x 10(9), 7.66 x 10(9) and 1.08 x 10(10) M-1 s(-1), respectively. Under neutral conditions, the contributions of UV-LED, HO center dot, and Cl center dot to AAP degradation were 4.21%, 60.15% and 35.64% in the UV-LED/NH2Cl system, whereas the respective contributions of UV-LED, HO center dot and SO center dot- to AAP degradation were 2.09%, 22.84% and 75.07% in UV-LED/PS system, respectively. Meanwhile, the corresponding contributions of the involved reactive species were found to be pH-dependence. The natural organic materials (NOM) inhibited the AAP degradation, and the presence of Cl-, HCO3-, and NO3- had different effects on AAP degradation in the three hybrid processes. The AAP degradation was significantly inhibited in the three UV-LED-based AOPs in real water. In addition, the intermediate products were also identified, and possible degradation pathways were proposed in the three UV-LED-based AOPs. The acute toxicity bioassay using bacterium Vibrio fischeri suggested that the UV-LED/PS process was more effective than the UV-LED/H2O2 and UV-LED/NH2Cl processes in reducing the acute toxicity of the reacted AAP solution. Among the three UV-LED-based AOPs, the UV-LED/PS was found to be the most efficient process for AAP degradation. (c) 2020 Elsevier B.V. All rights reserved.