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

被引：14

作者：

Wang, Lidong ^{[1
]}

Wang, Yanan ^{[1
]}

Wang, Zhixiang ^{[2
]}

Du, Penghui ^{[3
]}

Xing, Lei ^{[4
]}

Xu, Weichao ^{[2
]}

Ni, Jincheng ^{[1
]}

Liu, Shuai ^{[1
]}

Wang, Yihao ^{[1
]}

Yu, Guangfei ^{[1
]}

Dai, Qin ^{[1
]}

机构：

[1] North China Elect Power Univ, Coll Environm Sci & Engn, MOE Key Lab Resources & Environm Syst Optimizat, Beijing 102206, Peoples R China

[2] Chinese Acad Sci, Inst Proc Engn, Beijing Engn Res Ctr Proc Pollut Control, Natl Key Lab Biochem Engn, Beijing 100190, Peoples R China

[3] Southern Univ Sci & Technol, Sch Environm Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China

[4] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Cont, Beijing 100084, Peoples R China

来源：

WATER RESEARCH | 2023年 / 240卷

基金：

中国国家自然科学基金;

关键词：

Base-induced proton transfers; C=N active site; Dimethylamine (DMA); Peroxymonosulfate activation; Wastewater treatment; VOLATILE ORGANIC-COMPOUNDS; SINGLET OXYGEN; PEROXYMONOSULFATE PMS; OXIDATION; KINETICS; DECOMPOSITION; PHASE;

D O I：

10.1016/j.watres.2023.120119

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

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 Bronsted 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-1 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 1O2. Subsequently, 1O2 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 $/m3). 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 insitu construction of metal-free active site by regulating proton transfer will provide a brand-new strategy for environmental remediation.

引用

页数：12