DOI: 10.1016/j.watres.2018.12.010
Scopus记录号: 2-s2.0-85059817030
论文题名: Quantitative structure-activity relationship models for predicting reaction rate constants of organic contaminants with hydrated electrons and their mechanistic pathways
作者: Li C. ; Zheng S. ; Li T. ; Chen J. ; Zhou J. ; Su L. ; Zhang Y.-N. ; Crittenden J.C. ; Zhu S. ; Zhao Y.
刊名: Water Research
ISSN: 431354
出版年: 2019
起始页码: 468
结束页码: 477
语种: 英语
英文关键词: Hydrated electron (e aq − )
; QSAR models
; Quantum chemical calculation
; Second order rate constants
; Single electron transfer
Scopus关键词: Activation energy
; Computational chemistry
; Dyes
; Electron transitions
; Free energy
; Gibbs free energy
; Halogenation
; Hydration
; Molecular graphics
; Molecular orbitals
; Organic pollutants
; Single electron transistors
; Structures (built objects)
; Wastewater treatment
; Water pollution
; Hydrated electron
; QSAR model
; Quantum chemical calculations
; Second-order rate constants
; Single electron transfer
; Rate constants
; aliphatic compound
; halide
; organic compound
; aliphatic hydrocarbon
; electron
; Gibbs free energy
; model
; organic pollutant
; prediction
; quantitative analysis
; quantum mechanics
; reaction kinetics
; reaction rate
; reduction
; wastewater treatment
; Article
; dehalogenation
; dipole
; electric potential
; electron transport
; electrophilicity
; energy
; enthalpy
; multiple linear regression analysis
; polymerization
; priority journal
; quantitative structure activity relation
; quantum chemistry
; reduction (chemistry)
; support vector machine
; thermodynamics
; waste water management
英文摘要: The hydrated electron (e aq − )-based reduction processes are promising for removing organic pollutants in water engineering systems. The reductive kinetics, especially the second order rate constants (k e aq − ) of e aq − with organic compounds, is important for evaluating and modeling the advanced reduction processes. In this study, the k e aq − values for aliphatic compounds and phenyl-based compounds are, for the first time, modeled by the quantitative structure-activity relationship (QSAR) method. The structural features governing the reactivity of two classes of organic compounds toward e aq − were revealed, and the energy of the lowest unoccupied molecular orbital (E LUMO ), one-electron reduction potential (E RED ) and polarizability (α) were found to be the important molecular parameters in both two models. The built QSAR models provide robust predictive tools for estimating the removal of emerging pollutants using e aq − during wastewater treatment processes. Additionally, quantum chemical calculations were employed to probe into the mechanism and feasibility of the single electron transfer (SET) pathway in the e aq − -based reduction process. The thermodynamic investigation suggests that the compounds with electron-withdrawing groups tend to possess higher k e aq − and lower Gibbs free energy (ΔG SET ) and Gibbs free energies of activation (∆ ‡ G SET ∘ ) than the ones with electron-donating groups, indicating the SET process occurs more readily. It is also found that the refractory halogenated compounds can achieve dehalogenation via the SET pathway. © 2018 Elsevier Ltd Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/122031
Appears in Collections: 气候变化事实与影响
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作者单位: State Environmental Protection Key Laboratory of Wetland Ecology and Vegetation Restoration, School of Environment, Northeast Normal University, Changchun, 130117, China; Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, China; Brook Byers Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA 30332, United States
Recommended Citation:
Li C.,Zheng S.,Li T.,et al. Quantitative structure-activity relationship models for predicting reaction rate constants of organic contaminants with hydrated electrons and their mechanistic pathways[J]. Water Research,2019-01-01