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通过添加高碘酸盐,在 InO/Vis-LED 工艺中增强羟基自由基生成以降解微量污染物。

Enhanced hydroxyl radical generation for micropollutant degradation in the InO/Vis-LED process through the addition of periodate.

机构信息

School of Biotechnology and Health Science, Wuyi University, Jiangmen, Guangdong Province 529020, China.

School of Biotechnology and Health Science, Wuyi University, Jiangmen, Guangdong Province 529020, China.

出版信息

Water Res. 2023 Sep 1;243:120401. doi: 10.1016/j.watres.2023.120401. Epub 2023 Jul 23.

DOI:10.1016/j.watres.2023.120401
PMID:37536249
Abstract

Periodate (PI) as an oxidant has been extensively studied for organic foulants removal in advanced oxidation processes. Here PI was introduced into InO/Vis-LED process to enhance the formation of ·OH for promoting the degradation of organic foulants. Results showed that the addition of PI would significantly promote the removal of sulfamethoxazole (SMX) in the InO/Vis-LED process (from 9.26% to 100%), and ·OH was proved to be the dominant species in the system. Besides, the process exhibited non-selectivity in the removal of different organic foulants. Comparatively, various oxidants (e.g., peroxymonosulfate, peroxydisulfate, and hydrogen peroxide) did not markedly promote the removal of SMX in the InO/Vis-LED process. Electrochemical analyses demonstrated that PI could effectively receive photoelectrons, thus inhibiting the recombination of photogenerated electron-hole (e/h) pairs. The holes then oxidized the adsorbed HO to generate ·OH, and the PI converted to iodate at the same time. Additionally, the removal rate of SMX reduced from 100% to 17.2% as Vis-LED wavelengths increased from 440 to 560 nm, because of the low energy of photons produced at longer wavelengths. Notably, the species of PI do not affect its ability to accept electrons, resulting in the degradation efficiency of SMX irrespective of pH (4.0-10.0). The coexistence of inorganic cations and anions (such as Cl, CO/HCO, SO, Ca, and Mg) also had an insignificant effect on SMX degradation. Furthermore, the process also showed excellent degradation potential in real water. The proposed strategy provides a new insight for visible light-catalyzed activation of PI and guidance to explore green catalytic processes for high-efficiency removal of various organic foulants.

摘要

过碘酸盐(PI)作为一种氧化剂,已在高级氧化工艺中被广泛研究用于去除有机污染物。本研究将 PI 引入 InO/Vis-LED 工艺中,以增强·OH 的生成,促进有机污染物的降解。结果表明,PI 的加入可显著促进 InO/Vis-LED 工艺中磺胺甲恶唑(SMX)的去除(从 9.26%提高至 100%),且·OH 被证明是该体系中的主要活性物种。此外,该工艺对不同有机污染物的去除表现出非选择性。相比之下,各种氧化剂(如过一硫酸盐、过二硫酸盐和过氧化氢)并未显著促进 InO/Vis-LED 工艺中 SMX 的去除。电化学分析表明,PI 可有效接收光生电子,从而抑制光生电子-空穴(e/h)对的复合。生成的空穴将吸附的 HO 氧化为·OH,同时 PI 转化为碘酸盐。此外,随着 Vis-LED 波长从 440nm 增加到 560nm,SMX 的去除率从 100%降低至 17.2%,这是由于长波长下产生的光子能量较低。值得注意的是,PI 的形态并不影响其接受电子的能力,因此 SMX 的降解效率不受 pH 值(4.0-10.0)的影响。无机阳离子和阴离子(如 Cl、CO/HCO、SO、Ca 和 Mg)的共存对 SMX 降解也没有显著影响。此外,该工艺在实际水样中也表现出优异的降解潜力。该策略为可见光催化 PI 活化提供了新的思路,并为探索高效去除各种有机污染物的绿色催化工艺提供了指导。

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