The overlooked role of Cr(VI) in micropollutant degradation under solar light irradiation

化学 六价铬 光解 降级(电信) 光化学 吸光度 辐照 电子顺磁共振 腐植酸 核化学 碳酸氢盐 无机化学 有机化学 电信 色谱法 肥料 物理 核磁共振 计算机科学 核物理学
作者
Tao Yang,Cui Huang,Linqian An,Ge Zeng,Juan Li,Changyu Liu,Xiaolong Xu,Jianbo Jia,Jun Ma
出处
期刊:Water Research [Elsevier BV]
卷期号:242: 120309-120309 被引量:9
标识
DOI:10.1016/j.watres.2023.120309
摘要

Hexavalent chromium (Cr(VI)) is ubiquitous in natural environments, whereas its role in the transformation of coexisting contaminants may have been overlooked. In this work, it was reported for the first time that the irradiation of Cr(VI) by solar light (solar light/Cr(VI) system) could effectively degrade various micropollutants with different structures. The removal efficiency of selected micropollutants was increased by 13.3-64.8% by the solar light/Cr(VI) system compared to that by direct solar photolysis. Meanwhile, the oxidation rates were enhanced by 2.2-21.5 folds, while they were negligible by Cr(VI) oxidation alone. Experiments by specific scavengers, probe compounds, fluorescence absorbance, and electron spin resonance analysis demonstrated that hydroxyl radical (•OH) was the major reactive species in the solar light/Cr(VI) system. Further experiments showed that the generation of •OH was closely related to the intermediate Cr(V) generated from Cr(VI) reduction, and Cr(V) could be re-oxidized back to Cr(VI). Increasing solution pH negatively affected model micropollutant (carbamazepine (CBZ)) degradation by the solar light/Cr(VI) system, mainly due to the decreased quantum yield of •OH at higher pH. Coexisting sulfate ions showed negligible effect on CBZ degradation in the solar light/Cr(VI) system, while the presence of bicarbonate, chloride, and humic acid inhibited CBZ degradation to varying degrees, owing to their diverse scavenging effects on •OH. Furthermore, moderate CBZ degradation was also achieved by natural solar light photolysis of Cr(VI). This study demonstrated the pivotal role of Cr(VI) in the transformation of micropollutants under solar irradiation, which advances the understanding of the fate of micropollutants in natural environments.
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