ABTS 作为激活剂和电子穿梭来激活过硫酸盐以进行双氯芬酸降解：ABTS•+、SO4•– 和•OH 的形成和贡献,Environmental Science & Technology

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ABTS 作为激活剂和电子穿梭来激活过硫酸盐以进行双氯芬酸降解：ABTS•+、SO4•– 和•OH 的形成和贡献
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2022-10-19 , DOI: 10.1021/acs.est.2c04318
Yixin Huang ₁ , Jing Zou ₁ , Jinbin Lin ₁ , Haoyu Yang ₁ , Mengyun Wang _{1,

2} , Jiawen Li ₁ , Wei Cao ₁ , Baoling Yuan _{1,

3} , Jun Ma ₂

Affiliation

有机化合物对过二硫酸盐（PDS）的活化引起了越来越多的关注。然而，有机化合物活化PDS存在一些固有的缺点，包括活化剂分解快、抗干扰能力差等，限制了其应用。有趣的是，我们发现 2,2'-azino-bis (3-乙基苯并噻唑啉-6-磺酸盐) (ABTS) 可以充当 PDS 活化的活化剂和电子穿梭机，从而在 2.0–pH 范围内增强双氯芬酸 (DCF) 的降解。 11.0。PDS/ABTS 系统中产生了ABTS ^•+、^• OH 和SO ₄^•–等多种活性物质，而只有ABTS ^•+和^• OH 直接导致DCF 降解。ABTS ^{•+是通过ABTS 与PDS、SO}₄^•–和^• OH反应生成的，是DCF 降解的主要反应物种。在 PDS/ABTS 系统中没有观察到 ABTS 的显着分解，并且 ABTS 既充当激活剂又充当电子穿梭。提出了DCF的四种可能的降解途径，并且经过PDS/ABTS系统处理后DCF的毒性降低。PDS/ABTS系统对常见天然水成分具有良好的抗干扰能力。此外，将ABTS封装到纤维素中得到ABTS@Ce珠，PDS/ABTS@Ce系统具有优异的DCF降解性能。这项研究提出了一个新的视角来重新考虑有机化合物激活 PDS 的机制，并强调了有机自由基对污染物去除的巨大贡献。

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ABTS as Both Activator and Electron Shuttle to Activate Persulfate for Diclofenac Degradation: Formation and Contributions of ABTS•+, SO4•–, and •OH

The activation of peroxydisulfate (PDS) by organic compounds has attracted increasing attention. However, some inherent drawbacks including quick activator decomposition and poor anti-interference capacity limited the application of organic compound-activated PDS. It was interestingly found that 2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonate) (ABTS) could act as both activator and electron shuttle for PDS activation to enhance diclofenac (DCF) degradation over a pH range of 2.0–11.0. Multiple reactive species of ABTS^•+, ^•OH, and SO₄^•– were generated in the PDS/ABTS system, while only ABTS^•+ and ^•OH directly contributed to DCF degradation. ABTS^•+, generated via the reactions of ABTS with PDS, SO₄^•–, and ^•OH, was the dominant reactive species of DCF degradation. No significant decomposition of ABTS was observed in the PDS/ABTS system, and ABTS acted as both activator and electron shuttle. Four possible degradation pathways of DCF were proposed, and the toxicity of DCF decreased after treatment with the PDS/ABTS system. The PDS/ABTS system had good anti-interference capacity to common natural water constituents. Additionally, ABTS was encapsulated into cellulose to obtain ABTS@Ce beads, and the PDS/ABTS@Ce system possessed excellent performance on DCF degradation. This study proposes a new perspective to reconsider the mechanism of activating PDS with organic compounds and highlights the considerable contribution of organic radicals on contaminant removal.

更新日期：2022-10-19

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