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一种用于微污染物降解的新型铁(II)/柠檬酸盐/紫外线/过氧单硫酸盐工艺:响应面法优化及水基质的影响

A novel Fe(II)/citrate/UV/peroxymonosulfate process for micropollutant degradation: Optimization by response surface methodology and effects of water matrices.

作者信息

Ling Li, Zhang Dapeng, Fang Jingyun, Fan Chihhao, Shang Chii

机构信息

Department of Civil and Environmental Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong.

SYSU-HKUST Research Center for Innovative Environmental Technology (SHRCIET), School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou 510275, PR China; Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Guangzhou 510275, China.

出版信息

Chemosphere. 2017 Oct;184:417-428. doi: 10.1016/j.chemosphere.2017.06.004. Epub 2017 Jun 4.

Abstract

This paper applied the response surface methodology (RSM) to optimizing a novel Fe(II)/citrate/UV/PMS process in the degradation of a model micropollutant, carbamazepine (CBZ), a persistent emerging contaminant frequently detected in surface water and groundwater. The experimental conditions in terms of two responses, CBZ removal efficiency (Y1) and cost per unit CBZ removal (Y2), were optimized by the central composite design (CCD) in RSM. Modeling data exhibited that the optimum condition resulting in the lowest Y2 while achieving >70% of Y1 was at a UV dose of 265.5 mJ/cm and Fe(II), PMS and citrate concentrations of 12.2 μM, 100 μM and 26.4 μM, respectively. Increasing Fe(II) concentration led to the decrease in CBZ degradation and cost-effectiveness of the process. On the other hand, increasing the UV dose, PMS concentration and citrate/Fe(II) ratio over 265.5 mJ/cm, 100 μM and 2.16:1, respectively, slightly increased the CBZ degradation, but significantly increased the cost. Under the optimized condition, the experimentally obtained values for Y1 and Y2 were 70.44% and 0.0104 H K$/%/m, respectively. The predicted Y1 and Y2 were 71.07% and 0.0098 H K$/%/m, respectively, suggesting that RSM can be readily used to determine the optimum condition of the Fe(II)/citrate/UV/PMS process for CBZ degradation. Other aqueous constituents which impacted the CBZ removal in the Fe(II)/citrate/UV/PMS process are in the following order: NOM > alkalinity > bromide > ammonia ≈ chloride (both negligible).

摘要

本文应用响应面法(RSM)优化了一种新型的Fe(II)/柠檬酸盐/UV/PMS工艺,用于降解模型微污染物卡马西平(CBZ),这是一种在地表水和地下水中经常检测到的持久性新兴污染物。通过RSM中的中心复合设计(CCD),对以CBZ去除效率(Y1)和单位CBZ去除成本(Y2)这两个响应为指标的实验条件进行了优化。建模数据表明,在UV剂量为265.5 mJ/cm²、Fe(II)、PMS和柠檬酸盐浓度分别为12.2 μM、100 μM和26.4 μM时,可实现Y2最低且Y1>70%的最佳条件。Fe(II)浓度的增加导致CBZ降解率降低以及该工艺的成本效益降低。另一方面,分别将UV剂量、PMS浓度和柠檬酸盐/Fe(II)比例提高到超过265.5 mJ/cm²、100 μM和2.16:1时,CBZ降解率略有增加,但成本显著增加。在优化条件下,实验得到的Y1和Y2值分别为70.44%和0.0104 HK$/(%/m)。预测的Y1和Y2分别为71.07%和0.0098 HK$/(%/m),这表明RSM可很容易地用于确定Fe(II)/柠檬酸盐/UV/PMS工艺降解CBZ的最佳条件。在Fe(II)/柠檬酸盐/UV/PMS工艺中影响CBZ去除的其他水性成分的影响顺序如下:天然有机物>碱度>溴化物>氨≈氯化物(两者均可忽略不计)。

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