CAS OpenIR
N-dependent ozonation efficiency over nitrogen-containing heterocyclic contaminants: A combined density functional theory study on reaction kinetics and degradation pathways
Yao, Yujie1,2; Xie, Yongbing1; Zhao, Binran2; Zhou, Linbi1; Shi, Yanchun1; Wang, Yuxian3; Sheng, Yuxing2; Zhao, He1; Sun, Jiajun1; Cao, Hongbin1
2020-02-15
Source PublicationCHEMICAL ENGINEERING JOURNAL
ISSN1385-8947
Volume382Pages:10
AbstractNitrogen-containing heterocyclic contaminants (NHCs) have aroused intense environmental issues in waterbody because of their high toxicity and strong recalcitrance against natural degradation. In this study, ozonation degradation on four typical NHCs - benzotriazole (BTA), benzimidazole (BMZ), indazole (IDZ), and indole (IDO) was carried out to investigate the effects of N atoms on degradation efficiency. Global softness of the NHCs was calculated by density functional theory (DFT) and correlated with ozonation efficiency. It was discovered that higher global softness of the NHCs resulted in the greater degradation efficiency. Mineralization results together with the quenching tests results suggested that NHCs with ortho-positioned N atoms in heterocyclic ring are easier to be mineralized, while the presence of para-positioned N atoms increased the recalcitrance for destruction. Apart from hydroxyl radicals, superoxide radicals and singlet oxygens were also identified by electron paramagnetic resonance (EPR) spectra. Condensed Fukui index was employed to probe the potential active sites for both direct ozone oxidation and radical-based attack. Single point energies were further calculated among these active sites to seek the initial-stage hydroxylation intermediates. Combined the calculation results with the identified intermediates from time-of-flight mass spectroscopy (TOF-MS), degradation routes of the NHCs were proposed. This study discovered structure-dependent behavior of NHCs on ozonation efficiency and envisaged a more accurate strategy for establishing the degradation pathway.
KeywordNitrogen heterocyclic compounds (NHCs) Ozonation Density functional theory (DFT) Reaction mechanism Degradation pathway
DOI10.1016/j.cej.2019.122708
Language英语
WOS KeywordCATALYTIC OZONATION ; OXIDATION ; BENZOTRIAZOLE ; WATER ; IDENTIFICATION ; OZONE ; DESTRUCTION ; PEROXIDASE ; ACTIVATION ; MECHANISMS
Funding ProjectNational Key Research and Development Program of China[2016YFB0600505] ; Major Science and Technology Program for Water Pollution Control and Treatment[2017ZX07402001] ; National Natural Science Foundation of China[21606253] ; Science Foundation of China University of Petroleum, Beijing[2462016YJRC013]
WOS Research AreaEngineering
WOS SubjectEngineering, Environmental ; Engineering, Chemical
Funding OrganizationNational Key Research and Development Program of China ; Major Science and Technology Program for Water Pollution Control and Treatment ; National Natural Science Foundation of China ; Science Foundation of China University of Petroleum, Beijing
WOS IDWOS:000503381200181
PublisherELSEVIER SCIENCE SA
Citation statistics
Cited Times:4[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/38472
Collection中国科学院过程工程研究所
Corresponding AuthorWang, Yuxian; Cao, Hongbin
Affiliation1.Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing Engn Res Ctr Proc Pollut Control, Beijing 100190, Peoples R China
2.Northwest Univ, Sch Chem Engn, Xian 710069, Shaanxi, Peoples R China
3.China Univ Petr, State Key Lab Heavy Oil Proc, 18 Fuxue Rd, Beijing 102249, Peoples R China
Recommended Citation
GB/T 7714
Yao, Yujie,Xie, Yongbing,Zhao, Binran,et al. N-dependent ozonation efficiency over nitrogen-containing heterocyclic contaminants: A combined density functional theory study on reaction kinetics and degradation pathways[J]. CHEMICAL ENGINEERING JOURNAL,2020,382:10.
APA Yao, Yujie.,Xie, Yongbing.,Zhao, Binran.,Zhou, Linbi.,Shi, Yanchun.,...&Cao, Hongbin.(2020).N-dependent ozonation efficiency over nitrogen-containing heterocyclic contaminants: A combined density functional theory study on reaction kinetics and degradation pathways.CHEMICAL ENGINEERING JOURNAL,382,10.
MLA Yao, Yujie,et al."N-dependent ozonation efficiency over nitrogen-containing heterocyclic contaminants: A combined density functional theory study on reaction kinetics and degradation pathways".CHEMICAL ENGINEERING JOURNAL 382(2020):10.
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