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Enhanced oxidation of carbamazepine by UV-LED/persulfate and UV-LED/H2O2 processes in the presence of trace copper ions
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-09-24 , DOI: 10.1016/j.cej.2020.127119
Anhong Cai , Jing Deng , Tianxin Zhu , Cheng Ye , Jun Li , Shiqing Zhou , Qingsong Li , Xueyan Li

In this study, the degradation of carbamazepine (CBZ) was comparatively investigated by UV-LED/persulfate (PS) and UV-LED/H2O2 processes in the presence of trace Cu2+ at neutral pH. Results showed that the introduction of trace Cu2+ accelerated CBZ degradation and more favorable performance was achieved in UV-LED/PS process. As oxidants dosage raised from 0.2 to 1.0 mM, the pseudo-first-order rate constant (kobs) value of CBZ both linearly increased in UV-LED/PS/Cu2+ and UV-LED/H2O2/Cu2+ processes. The promotion effect of Cu2+ at low level was more significant than that at high level in both processes at neutral pH. With reducing solution pH from 7.2 to 3.1, the kobs value dramatically increased from 0.136 to 0.399 min-1 in UV-LED/PS/Cu2+ process, while its value exhibited the imperceptible change in UV-LED/H2O2/Cu2+ process. ·OH functioned as the major contributor to CBZ degradation in two processes in pH range of 3.1-7.2. The addition of humic acid (HA), HCO3- and Cl- impeded CBZ degradation in UV-LED/H2O2/Cu2+ process. As for UV-LED/PS/Cu2+ process, the kobs value significantly increased in the presence of Cl-, while the introduction of HA and HCO3- restrained the removal. Total eleven degradation intermediates of CBZ were identified and a reasonable degradation pathway was proposed based on HPLC-MS/MS analysis and the calculation of Gaussian program. The acute toxicities of reacted solution enhanced in both processes within 15 min, especially in UV-LED/PS/Cu2+ process. In terms of electrical energy per order value, UV-LED/PS/Cu2+ process was found to be more cost-effective than UV-LED/H2O2/Cu2+ process. It was also noticed that UV-LED/PS process was more effective for CBZ removal in natural water in the presence of trace Cu2+.



中文翻译:

在痕量铜离子存在下,通过UV-LED /过硫酸盐和UV-LED / H 2 O 2工艺增强卡马西平的氧化

在这项研究中,在中性pH值存在微量Cu 2+的情况下,通过UV-LED /过硫酸盐(PS)和UV-LED / H 2 O 2工艺比较了卡马西平(CBZ)的降解。结果表明,在UV-LED / PS工艺中,微量Cu 2+的引入促进了CBZ的降解,并获得了更好的性能。随着氧化剂剂量从0.2 mM增加到1.0 mM,在UV-LED / PS / Cu 2+和UV-LED / H 2 O 2 / Cu 2中,CBZ的假一级速率常数(k obs)值均线性增加。+流程。Cu 2+的促进作用在中性pH值下,两个过程中的低浓度值都比高浓度值更显着。与还原溶液的pH值从7.2至3.1,所述ķ OBS值急剧从0.136增加至0.399分钟-1在UV-LED / PS /铜2+过程,同时它的值显示在UV-LED /了细微的变化ħ 2 ö 2 / Cu 2+工艺。·OH在3.1-7.2的pH范围内的两个过程中是CBZ降解的主要起因。腐殖酸(HA),HCO的加入3 -和Cl -阻碍CBZ降解在UV-LED / H 2 ö 2 /铜2+过程。至于UV-LED / PS / Cu2+过程中,ķ OBS值显著在氯的存在增加- ,同时引入HA和HCO的3 -抑制了去除。基于HPLC-MS / MS分析和高斯程序的计算,确定了总共11种CBZ降解中间体,并提出了合理的降解途径。在15分钟内两个过程中,特别是在UV-LED / PS / Cu 2+过程中,反应溶液的急性毒性均得到增强。就每订单价值的电能而言,发现UV-LED / PS / Cu 2+工艺比UV-LED / H 2 O 2 / Cu 2+具有更高的成本效益。处理。还注意到在存在痕量Cu 2+的情况下,UV-LED / PS工艺对于天然水中CBZ的去除更有效。

更新日期:2020-09-25
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