Proton transfer triggered in-situ construction of C=N active site to activate PMS for efficient autocatalytic degradation of low-carbon fatty amine

Wang，Lidong1; Wang，Yanan1; Wang，Zhixiang2; Du，Penghui3; Xing，Lei4; Xu，Weichao2; Ni，Jincheng1; Liu，Shuai1; Wang，Yihao1; Yu，Guangfei1; Dai，Qin1

2023-07-15

10.1016/j.watres.2023.120119

Water Research   影响因子和分区

0043-1354

1879-2448

Removal of low-carbon fatty amines (LCFAs) in wastewater treatment poses a significant technical challenge due to their small molecular size, high polarity, high bond dissociation energy, electron deficiency, and poor biodegradability. Moreover, their low Brønsted acidity deteriorates this issue. To address this problem, we have developed a novel base-induced autocatalytic technique for the highly efficient removal of a model pollutant, dimethylamine (DMA), in a homogeneous peroxymonosulfate (PMS) system. A high reaction rate constant of 0.32 min and almost complete removal of DMA within 12 min are achieved. Multi-scaled characterizations and theoretical calculations reveal that the in situ constructed C=N bond as the crucial active site activates PMS to produce abundant O. Subsequently, O oxidizes DMA through multiple H-abstractions, accompanied by the generation of another C=N structure, thus achieving the autocatalytic cycle of pollutant. During this process, base-induced proton transfers of pollutant and oxidant are essential prerequisites for C=N fabrication. A relevant mechanism of autocatalytic degradation is unraveled and further supported by DFT calculations at the molecular level. Various assessments indicate that this self-catalytic technique exhibits a reduced toxicity and volatility process, and a low treatment cost (0.47 $/m). This technology has strong environmental tolerance, especially for the high concentrations of chlorine ion (1775 ppm) and humic acid (50 ppm). Moreover, it not only exhibits excellent degradation performance for different amine organics but also for the coexisting common pollutants including ofloxacin, phenol, and sulforaphane. These results fully demonstrate the superiority of the proposed strategy for practical application in wastewater treatment. Overall, this autocatalysis technology based on the in-situ construction of metal-free active site by regulating proton transfer will provide a brand-new strategy for environmental remediation.

1O2-mediated autocatalysis Base-induced proton transfers C=N active site Dimethylamine (DMA) Peroxymonosulfate activation Wastewater treatment

SCI ; EI

英语

NI论文

其他

National Natural Science Foundation of China[22206070];National Natural Science Foundation of China[52200126];Natural Science Foundation of Hebei Province[E2019502199];Fundamental Research Funds for the Central Universities[XM2112344];

Engineering ; Environmental Sciences & Ecology ; Water Resources

Engineering, Environmental ; Environmental Sciences ; Water Resources

WOS:001008713700001

PERGAMON-ELSEVIER SCIENCE LTD

20232214165977

Amines ; Biodegradability ; Biodegradation ; Bond strength (chemical) ; Carbon ; Environmental technology ; Proton transfer ; Rate constants ; Reclamation

Industrial Wastes Treatment and Disposal:452.4 ; Environmental Engineering:454 ; Biotechnology:461.8 ; Biochemistry:801.2 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; High Energy Physics:932.1

ENVIRONMENT/ECOLOGY

2-s2.0-85160341645

Scopus

1.MOE Key Laboratory of Resources and Environmental Systems Optimization,College of Environmental Science and Engineering,North China Electric Power University,Beijing,102206,China
2.National Key Laboratory of Biochemical Engineering,Beijing Engineering Research Center of Process Pollution Control,Institute of Process Engineering,Chinese Academy of Sciences,Beijing,100190,China
3.School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
4.State Key Joint Laboratory of Environment Simulation and Pollution Control,School of Environment,Tsinghua University,Beijing,100084,China

Wang，Lidong,Wang，Yanan,Wang，Zhixiang,et al. Proton transfer triggered in-situ construction of C=N active site to activate PMS for efficient autocatalytic degradation of low-carbon fatty amine[J]. Water Research,2023,240.

Wang，Lidong.,Wang，Yanan.,Wang，Zhixiang.,Du，Penghui.,Xing，Lei.,...&Dai，Qin.(2023).Proton transfer triggered in-situ construction of C=N active site to activate PMS for efficient autocatalytic degradation of low-carbon fatty amine.Water Research,240.

Wang，Lidong,et al."Proton transfer triggered in-situ construction of C=N active site to activate PMS for efficient autocatalytic degradation of low-carbon fatty amine".Water Research 240(2023).