Wu Shouying, Wu Wei, Fan Jianing, Zhang Linping, Zhong Yi, Xu Hong, Mao Zhiping
Key Laboratory of Science & Technology of Eco-Textile, Ministry of Education, College of Chemistry and Chemical Engineering, Donghua University, No.2999 North Renmin Road, Shanghai, 201620, China.
Key Laboratory of Science & Technology of Eco-Textile, Ministry of Education, College of Chemistry and Chemical Engineering, Donghua University, No.2999 North Renmin Road, Shanghai, 201620, China.
Water Res. 2023 Apr 15;233:119725. doi: 10.1016/j.watres.2023.119725. Epub 2023 Feb 10.
Developing high-performance catalytic systems for eliminating contaminants effectively in water has received a lot of attention. However, the complexity of practical wastewater poses a challenge for degrading organic pollutants. Non-radical active species with strong resistance to interference have shown great advantages in degrading organic pollutants under complex aqueous conditions. Herein, a novel system was constructed by Fe(dpa)Cl (FeL, dpa = N, N'-(4-nitro-1,2-phenylene) dipicolinamide) activating peroxymonosulfate (PMS). The mechanism study verified that the FeL/PMS system had high efficiency in producing high-valent iron-oxo and singlet oxygen (O) to degrade various organic pollutants. In addition, the chemical bonding between PMS and FeL was elucidated by the density functional theory (DFT) calculations. The FeL/PMS system could remove 96% Reactive Red 195 (RR195) in 2 min, which was much higher than other systems involved in this study. More attractively, the FeL/PMS system demonstrated general resistance to interference from common anions (Cl, HCO, NO and SO), humic acid (HA) and pH changes and were thus compatible with various natural waters. This work provides a new approach for producing non-radical active species, which is a promising catalytic system for water treatment.
开发用于有效去除水中污染物的高性能催化系统已受到广泛关注。然而，实际废水的复杂性对有机污染物的降解构成了挑战。对干扰具有强抗性的非自由基活性物种在复杂水相条件下降解有机污染物方面显示出巨大优势。在此，通过Fe(dpa)Cl（FeL，dpa = N，N'-(4-硝基-1,2-亚苯基)二吡啶甲酰胺）活化过一硫酸盐（PMS）构建了一种新型体系。机理研究证实，FeL/PMS体系在产生高价铁氧和单线态氧（O）以降解各种有机污染物方面具有高效性。此外，通过密度泛函理论（DFT）计算阐明了PMS与FeL之间的化学键。FeL/PMS体系在2分钟内可去除96%的活性红195（RR195），远高于本研究中涉及的其他体系。更具吸引力的是，FeL/PMS体系对常见阴离子（Cl、HCO、NO和SO）、腐殖酸（HA）和pH变化的干扰具有普遍抗性，因此与各种天然水兼容。这项工作为产生非自由基活性物种提供了一种新方法，是一种有前景的水处理催化体系。
