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磺胺嘧啶在实验室规模反应器中的光催化氧化和光过硫酸盐氧化:催化剂载体、氧化剂用量、去除率和降解途径分析。

Photocatalytic-oxidation and photo-persulfate-oxidation of sulfadiazine in a laboratory-scale reactor: Analysis of catalyst support, oxidant dosage, removal-rate and degradation pathway.

机构信息

Department of Civil Engineering, National Institute of Technology, Calicut, Kerala, 673601, India.

Department of Civil Engineering, Indian Institute of Technology Madras, Chennai, Tamilnadu, 600036, India.

出版信息

J Environ Manage. 2018 Sep 15;222:164-173. doi: 10.1016/j.jenvman.2018.05.052. Epub 2018 May 26.

Abstract

The extent of sulfadiazine (SDZ) removal via photo-degradation (UV-C), photocatalysis with TiO (UV-C/TiO) and photo-persulfate-oxidation (UV-C/PS) was investigated in a batch reactor under different UV-C power levels (i.e. 14, 28, 42 and 56 W). Moreover, effects of suspended/immobilized catalyst, i.e. TiO slurry/TiO supported on granular activated carbon (GAC-TiO), on SDZ removal and corresponding SDZ degradation kinetics under different catalyst loading (1-6 g/L) were explored. Around 41.7% SDZ removal was observed after 120 min in UV-C system at the highest power level, i.e. 56 W. On the other hand, photocatalysis with TiO and GAC-TiO has shown better SDZ removal than photo-degradation. In UV-C/TiO (4 g/L and 28 W) and UV-C/GAC-TiO (5 g/L and 28 W) systems, SDZ removals were 91.8% after 120 min and 100% after 60 min, respectively; however, TOC analysis has revealed that 45.4% and 60.8% SDZ was mineralized in these systems, respectively. In UV-C/PS system, near complete degradation of SDZ (99.8%) was observed within 10 min under 50 mg/L of PS and 28 W UV illumination. On the other hand, complete SDZ removal was observed in PS alone system at a dosage of 1000 mg/L but the formation of SO was found to be a drawback. In photolysis and photocatalysis systems, SDZ removal followed pseudo-first-order kinetics whereas the kinetics followed pseudo-second-order in UV-C/PS system. The comparison of electrical energy consumed (E) in different systems revealed that UV-C/GAC-TiO and UV-C/PS system were energy efficient compared with other systems. The LC-MS analysis has confirmed the cleavage of C-N bonds in the pyrimidine ring followed by S-N bonds in the sulfonyl group, which was found to be the major degradation pathway of SDZ.

摘要

磺胺嘧啶(SDZ)通过光降解(UV-C)、TiO 光催化(UV-C/TiO)和过硫酸盐氧化(UV-C/PS)去除的程度在不同 UV-C 功率水平(即 14、28、42 和 56 W)的间歇式反应器中进行了研究。此外,还研究了悬浮/固定催化剂(即 TiO 浆料/TiO 负载在颗粒状活性炭(GAC-TiO)上)对磺胺嘧啶去除的影响以及在不同催化剂负载(1-6 g/L)下的相应磺胺嘧啶降解动力学。在最高功率水平(即 56 W)下,UV-C 系统中 120 分钟后观察到磺胺嘧啶去除率约为 41.7%。另一方面,TiO 和 GAC-TiO 的光催化作用比光降解作用更能有效地去除磺胺嘧啶。在 UV-C/TiO(4 g/L 和 28 W)和 UV-C/GAC-TiO(5 g/L 和 28 W)系统中,磺胺嘧啶在 120 分钟后分别去除了 91.8%和 100%,但 TOC 分析表明,这两个系统中磺胺嘧啶分别矿化了 45.4%和 60.8%。在 UV-C/PS 系统中,在 50 mg/L PS 和 28 W UV 照射下,磺胺嘧啶在 10 分钟内几乎完全降解(99.8%)。另一方面,在 1000 mg/L 的 PS 单独系统中观察到完全去除磺胺嘧啶,但发现 SO 的形成是一个缺点。在光解和光催化系统中,磺胺嘧啶的去除遵循假一级动力学,而在 UV-C/PS 系统中遵循假二级动力学。不同系统中消耗的电能(E)的比较表明,与其他系统相比,UV-C/GAC-TiO 和 UV-C/PS 系统更节能。LC-MS 分析证实了嘧啶环中的 C-N 键断裂,随后是磺酰基中的 S-N 键断裂,这被认为是磺胺嘧啶的主要降解途径。

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