Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.5194/acp-20-6671-2020 |
Atmospheric chemical loss processes of isocyanic acid (HNCO): a combined theoretical kinetic and global modelling study | |
Rosanka, Simon1; Vu, Giang H. T.2,3; Nguyen, Hue M. T.2,3; Pham, Tien, V4; Javed, Umar1; Taraborrelli, Domenico1; Vereecken, Luc1 | |
2020-06-08 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2020 |
卷号 | 20期号:11页码:6671-6686 |
文章类型 | Article |
语种 | 英语 |
国家 | Germany; Vietnam |
英文摘要 | Isocyanic acid (HNCO) is a chemical constituent suspected to be harmful to humans if ambient concentrations exceed similar to 1 ppbv. HNCO is mainly emitted by combustion processes but is also inadvertently released by NOx mitigation measures in flue gas treatments. With increasing biomass burning and more widespread usage of catalytic converters in car engines, good prediction of HNCO atmospheric levels with global models is desirable. Little is known directly about the chemical loss processes of HNCO, which limits the implementation in global Earth system models. This study aims to close this knowledge gap by combining a theoretical kinetic study on the major oxidants reacting with HNCO with a global modelling study. The potential energy surfaces of the reactions of HNCO with OH and NO3 radicals, Cl atoms, and ozone were studied using high-level CCSD(T)/CBS(DTQ)//M06-2X/aug-cc-pVTZ quantum chemical methodologies, followed by transition state theory (TST) theoretical kinetic predictions of the rate coefficients at temperatures of 200-3000 K. It was found that the reactions are all slow in atmospheric conditions, with k (300 K) <= 7 x 10(-16) cm(3) molecule(-)(1)s(-1), and that product formation occurs predominantly by H abstraction; the predictions are in good agreement with earlier experimental work, where available. The reverse reactions of NCO radicals with H2O, HNO3, and HCl, of importance mostly in combustion, were also examined briefly. The findings are implemented into the atmospheric model EMAC (ECHAM/MESSy Atmospheric Chemistry) to estimate the importance of each chemical loss process on a global scale. The EMAC predictions confirm that the gas-phase chemical loss of HNCO is a negligible process, contributing less than 1 % and leaving heterogeneous losses as the major sinks The removal of HNCO by clouds and precipitation contributes about 10 % of the total loss, while globally dry deposition is the main sink, accounting for similar to 90 %. The global simulation also shows that due to its long chemical lifetime in the free troposphere, HNCO can be efficiently transported into the UTLS by deep convection events. Daily-average mixing ratios of ground-level HNCO are found to regularly exceed 1 ppbv in regions dominated by biomass burning events, but rarely exceed levels above 10 ppt in other areas of the troposphere, though locally instantaneous toxic levels are expected. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000538775000001 |
WOS关键词 | OH RADICALS KINETICS ; GAS-PHASE OXIDATION ; TECHNICAL NOTE ; HYDROGEN-CYANIDE ; STATE DISTRIBUTIONS ; PULSE-RADIOLYSIS ; EMISSION FACTORS ; SHOCK-TUBE ; CHEMISTRY ; SUBMODEL |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/274351 |
专题 | 地球科学 |
作者单位 | 1.Forschungszentrum Julich, Inst Energy & Climate Res, Julich, Germany; 2.Hanoi Natl Univ Educ, Fac Chem, Hanoi, Vietnam; 3.Hanoi Natl Univ Educ, Ctr Computat Sci, Hanoi, Vietnam; 4.Hanoi Univ Sci & Technol, Sch Chem Engn, Hanoi, Vietnam |
推荐引用方式 GB/T 7714 | Rosanka, Simon,Vu, Giang H. T.,Nguyen, Hue M. T.,et al. Atmospheric chemical loss processes of isocyanic acid (HNCO): a combined theoretical kinetic and global modelling study[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2020,20(11):6671-6686. |
APA | Rosanka, Simon.,Vu, Giang H. T..,Nguyen, Hue M. T..,Pham, Tien, V.,Javed, Umar.,...&Vereecken, Luc.(2020).Atmospheric chemical loss processes of isocyanic acid (HNCO): a combined theoretical kinetic and global modelling study.ATMOSPHERIC CHEMISTRY AND PHYSICS,20(11),6671-6686. |
MLA | Rosanka, Simon,et al."Atmospheric chemical loss processes of isocyanic acid (HNCO): a combined theoretical kinetic and global modelling study".ATMOSPHERIC CHEMISTRY AND PHYSICS 20.11(2020):6671-6686. |
条目包含的文件 | 条目无相关文件。 |
除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。
修改评论