DOI: 10.1016/j.jcou.2016.02.007
Scopus记录号: 2-s2.0-84959270581
论文题名: Photochemistry of carbon dioxide from first principles: Application to photoabsorption of hot CO2
作者: Grebenshchikov S.Yu.
刊名: Journal of CO2 Utilization
ISSN: 22129820
出版年: 2016
卷: 15 语种: 英语
英文关键词: Ab initio
; CO2 reduction
; Photoabsorption
; Photodissociation
Scopus关键词: Absorption spectroscopy
; Calculations
; Chemical reactions
; Electromagnetic wave absorption
; Light absorption
; Photodissociation
; Potential energy
; Quantum chemistry
; Quantum theory
; Radiation
; Temperature distribution
; Ab initio
; Ab initio potential energy surface
; Absorption cross sections
; Excited electronic state
; Photoabsorptions
; Photodissociation dynamics
; Quantum-mechanical calculation
; Transition dipole moments
; Carbon dioxide
英文摘要: Graphical abstract: This paper analyzes the temperature dependence of the absorption spectrum of carbon dioxide in the wavelength range λ≤250nm by means of a first principles model. The model combines the high level ab initio potential energy surfaces of four excited electronic states and their coordinate dependent transition dipole moment vectors with quantum mechanical calculations of the photodissociation dynamics and the absorption spectra corresponding to excitations from many initial rovibrational states of the parent CO2. The calculations demonstrate that photodynamics from first principles can be realized for CO2 with high accuracy: The absorption cross section can be reliably calculated for λ≤250nm and T≤2500K and used for modeling the one-step photolytic reduction of CO2 to CO. An ab initio-based estimate of the contribution of low lying triplet states to the optical absorption of hot CO2 is also given. © 2016 Elsevier Ltd. 资助项目: Deutsche Forschungsgemeinschaft
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/52900
Appears in Collections: 影响、适应和脆弱性