摘要
The heterogeneous hydrolysis of dinitrogen pentoxide(N2O5)plays an important role in regulating NOx.The N2O5 uptake coefficient,γ(N2O5),was determined using an iterative box model that was constrained to observational data obtained in suburban Beijing from February to March 2016.The box model determined 2289 individualγ(N2O5)values that varied from<0.001 to 0.02 with an average value of 0.0046±0.0039(and a median value of 0.0032).We found the derived winterγ(N2O5)values in Beijing were relatively low as compared to values reported in previous field studies conducted during winter in Hong Kong(average value of 0.014)and the eastern U.S.coast(median value of 0.0143).In our study,field evidence of the suppression ofγ(N2O5)values due to pNO3-content,organics and the enhancement by aerosol liquid water content(ALWC)is in line with previous laboratory study results.Low ALWC,high pNO3-content,and particle morphology(inorganic core with an organic shell)accounted for the lowγ(N2O5)values in the North China Plain(NCP)during wintertime.The field-derivedγ(N2O5)values are well reproduced by a revised parameterization method,which includes the aerosol size distribution,ALWC,nitrate and organic coating,suggesting the feasibility of comprehensive parameterization in the NCP during wintertime.
通过迭代盒子模型定量了北京冬季污染过程的N2O5摄取系数γ(N2O5),发现其均值远低于其他地区冬季.颗粒物中硝酸盐强烈抑制N2O5非均相摄取,有机物也存在一定的抑制作用,但是颗粒物含水量是促进摄取的重要因素.华北冬季颗粒物中硝酸盐浓度高,含水量低是γ(N2O5)较低的关键因素.经典的γ(N2O5)参数化方案存在系统性高估,在改进的参数化方案中综合考虑了颗粒物粒径分布差异、含水量、硝酸盐和有机物镀膜的影响之后,参数化方案的预测能力得到有效提高.
作者
Haichao Wang
Xiaorui Chen
Keding Lu
Zhaofeng Tan
Xuefei Ma
Zhijun Wu
Xin Li
Yuhan Liu
Dongjie Shang
Yusheng Wu
Limin Zeng
Min Hu
Sebastian Schmitt
Astrid Kiendler-Scharr
Andreas Wahner
Yuanhang Zhang
王海潮;陈肖睿;陆克定;谭照峰;马雪飞;吴志军;李歆;刘禹含;尚冬杰;吴宇声;曾立民;胡敏;Sebastian Schmitt;Astrid Kiendler-Scharr;Andreas Wahner;张远航(State Key Joint Laboratory of Environmental Simulation and Pollution Control,College of Environmental Sciences and Engineering,Peking University,Beijing 100871,China;Institute of Energy and Climate Research,IEK-8:Troposphere,Forschungszentrum Jülich GmbH,Jülich 52428,Germany;Center for Excellence in Regional Atmospheric Environment,Chinese Academy of Sciences,Xiamen 361021,China;Institute of Energy and Climate Research,IEK-8:Troposphere,Forschungszentrum Julich GmbH,Julich 52428,Germany;Now at TSI GmbH,Aachen 52068,Germany)
基金
supported by the National Natural Science Foundation of China(21976006,41907185,91844301,91544225)
Beijing Natural Science Foundation,China(JQ19031)
China Postdoctoral Science Foundation(2018M641095,2019T120023)。