模型模拟结合便携测量预测紫外高级氧化工艺对水中微污染物的去除

黄妍妍, 李梦凯, 孙喆, 李文涛, James R. Bolton, 强志民

工程（英文） ›› 2024, Vol. 37 ›› Issue (6) : 97-105.

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工程（英文） ›› 2024, Vol. 37 ›› Issue (6) : 97-105. DOI: 10.1016/j.eng.2023.10.009
研究论文
Article

模型模拟结合便携测量预测紫外高级氧化工艺对水中微污染物的去除

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Facilitated Prediction of Micropollutant Degradation via UV-AOPs in Various Waters by Combining Model Simulation and Portable Measurement

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Highlight

• Water matrix scavenging capacities for $ \mathrm{HO}^{·}$, $ \mathrm{SO}_{4}^{·-}$ and $ \mathrm{Cl}^{·}$ were measured portably.

• Model simulation consisted of photochemical, QSAR, and SSA models.

• k′p,MP values in UV-AOPs were predicted in real waters and verified experimentally.

• The developed method facilitates the selection and optimization of UV-AOPs.

摘要

紫外高级氧化工艺（UV-AOPs）对水中微污染物的降解效果受水基质强烈干扰。UV-AOPs产生的各种活性自由基（RR）与水基质和目标微污染物具有不同的反应活性，因此，对UV-AOPs进行工艺选择和优化具有重要意义。本研究通过结合模型模拟与便携测量，开发了UV-AOPs对微污染物的光子剂量基降解速率常数（k′p,MP）预测方法。便携测量通过细管流光反应系统测定水基质对UV-AOPs中主要RR（即HO•、SO4•−和Cl•）的捕获容量（RRSC）。模型模拟由光化学模型、定量构效关系模型和自由基浓度稳态近似模型组成。本研究测定了八种水体的RRSC值，水基质越复杂，其RRSC值越大。然后，以磺胺二甲基嘧啶、咖啡因和卡马西平为模型微污染物，预测了这八种水体中UV-AOPs对其降解的k′p,MP值并进行了实验验证。研究发现由于对RR更强烈的竞争，具有更高RRSC值的水基质将导致更低的k′p,MP值，例如，在一饮用水厂的原水（RRSC = 9.47 × 104 s−1）和砂滤池出水（RRSC = 2.87 × 104 s−1）中，UV/H2O2降解卡马西平的k′p,MP值分别为130.9和332.5 m2·einstein-1。本研究开发的方法有助于UV-AOPs的工艺选择和优化，对提升水处理效率和节约成本具有重要意义。

Abstract

The degradation of micropollutants in water via ultraviolet (UV)-based advanced oxidation processes (AOPs) is strongly dependent on the water matrix. Various reactive radicals (RRs) formed in UV-AOPs have different reaction selectivities toward water matrices and degradation efficiencies for target micropollutants. Hence, process selection and optimization are crucial. This study developed a facilitated prediction method for the photon fluence-based rate constant for micropollutant degradation (k′p,MP) in various UV-AOPs by combining model simulation with portable measurement. Portable methods for measuring the scavenging capacities of the principal RRs (RRSCs) involved in UV-AOPs (i.e., $ \mathrm{HO}^{·}$, $ \mathrm{SO}_{4}^{·-}$, and $ \mathrm{Cl}^{·}$) using a mini-fluidic photoreaction system were proposed. The simulation models consisted of photochemical, quantitative structure–activity relationship, and radical concentration steady-state approximation models. The RRSCs were determined in eight test waters, and a higher RRSC was found to be associated with a more complex water matrix. Then, by taking sulfamethazine, caffeine, and carbamazepine as model micropollutants, the k′p,MP values in various UV-AOPs were predicted and further verified experimentally. A lower k′p,MP was found to be associated with a higher RRSC for a stronger RR competition; for example, k′p,MP values of 130.9 and 332.5 m2·einstein–1, respectively, were obtained for carbamazepine degradation by UV/H2O2 in the raw water (RRSC = 9.47 × 104 s−1) and sand-filtered effluent (RRSC = 2.87 × 104 s−1) of a drinking water treatment plant. The developed method facilitates process selection and optimization for UV-AOPs, which is essential for increasing the efficiency and cost-effectiveness of water treatment.

关键词

紫外高级氧化工艺 / 微污染物降解 / 活性自由基 / 水基质 / 模型模拟

Keywords

UV-AOPs / Micropollutant degradation / Reactive radicals / Water matrix / Model simulation

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黄妍妍, 李梦凯, 孙喆. 模型模拟结合便携测量预测紫外高级氧化工艺对水中微污染物的去除. Engineering. 2024, 37(6): 97-105 https://doi.org/10.1016/j.eng.2023.10.009

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