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Quinones stimulate reactive oxygen species production from zero-valent iron over centimeter distances
Water Research ( IF 11.4 ) Pub Date : 2025-01-16 , DOI: 10.1016/j.watres.2025.123141
Junye Ma, Wanchao Yu, Xuan Li, Shuxuan Chen, Binbin Wu, Jingyi Wang, Baoliang Chen, Chiheng Chu

Zero-valent iron (ZVI) has demonstrated high potential for in-situ remediation of contaminated groundwater and soils. Upon exposure to oxygen, ZVI generates reactive oxygen species (ROS). In parallel with the electron transfer mediated-reductive path, ROS plays a critical role in the oxidative degradation of organic pollutants during ZVI remediation of groundwater and soil. Yet, the efficiency is often constrained by the confined ROS production localized to the surface or immediate vicinity of ZVI particles. Here, we demonstrate that quinones significantly enhance ROS production from ZVI over centimeter-scale distances. H₂O₂ and OH were detected over 1 cm from ZVI particles after 24 h of incubation, with production increasing alongside quinone concentration and incubation time, reaching 318.3 ± 50.0 µM and 1263.2 ± 143.5 nM at 2 mm, respectively. The broad applicability of quinone in promoting remote ROS generation was demonstrated for various ZVI materials. This remote ROS production is driven by sequential electron transfer from ZVI to quinone, long-distance electron transfer via quinone, and subsequent electron transfer from reduced quinone to oxygen. The resulting increase in ROS production amount and extended range improved ZVI remediation efficiency by 5- to 15-fold for organic pollutant degradation. These findings provide a promising strategy for enhancing ROS-mediated ZVI remediation in heterogeneous environments.

中文翻译:


醌刺激零价铁在厘米距离内产生活性氧



零价铁 (ZVI) 已被证明具有对受污染的地下水和土壤进行原位修复的巨大潜力。暴露于氧气后,ZVI 会产生活性氧 (ROS)。与电子转移介导的还原路径并行,ROS 在地下水和土壤 ZVI 修复过程中有机污染物的氧化降解中起着关键作用。然而,效率通常受到局限于 ZVI 颗粒表面或附近受限的 ROS 产生的限制。在这里,我们证明醌在厘米级距离上显着提高了 ZVI 的 ROS 产生。孵育 24 小时后,在 ZVI 颗粒中超过 1 cm 处检测到 H₂O₂ 和 •OH,随着醌浓度和孵育时间的增加,产量增加,在 2 mm 处分别达到 318.3 ± 50.0 μM 和 1263.2 ± 143.5 nM。醌在促进远程 ROS 生成方面的广泛适用性已在各种 ZVI 材料中得到证明。这种远程 ROS 生产是由从 ZVI 到醌的顺序电子转移、通过醌的长距离电子转移以及随后从还原醌到氧的电子转移驱动的。由此产生的 ROS 产量增加和范围扩大,将零价铁的有机污染物降解修复效率提高了 5 到 15 倍。这些发现为在异构环境中增强 ROS 介导的 ZVI 修复提供了一种有前途的策略。
更新日期:2025-01-16
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