Comprehensive observations of the nocturnal atmospheric oxidation of NO_(3)and N_(2)O_(5)were conducted at a suburban site in Changzhou in the YRD using cavity ring-down spectroscopy(CRDS)from 27 May to 24 June,2019.H...Comprehensive observations of the nocturnal atmospheric oxidation of NO_(3)and N_(2)O_(5)were conducted at a suburban site in Changzhou in the YRD using cavity ring-down spectroscopy(CRDS)from 27 May to 24 June,2019.High concentrations of NO_(3)precursors were observed,and the nocturnal production rate of NO_(3)was determined to be 1.7±1.2 ppbv/hr.However,the nighttime NO_(3)and N_(2)O_(5)concentrations were relatively low,with maximum values of 17.7 and 304.7 pptv,respectively,illustrating the rapid loss ofNO_(3)andN_(2)O_(5).Itwas found that NO_(3)dominated the nighttime atmospheric oxidation,accounting for 50.7%,whileO3 andOH only contributed 34.1%and 15.2%,respectively.For the reactions of NO_(3)with volatile organic compounds(VOCs),styrenewas found to account for 60.3%,highlighting its dominant role in the NO_(3)reactivity.In general,the contributions of the reactions between NO_(3)and VOCs and the N_(2)O_(5)uptake to NO_(3)losswere found to be about 39.5%and 60.5%,respectively,indicating that N_(2)O_(5)uptake also played an important role in the loss of NO_(3)and N_(2)O_(5),especially under the high humidity conditions in China.The formation of nitrate at night mainly originated from N_(2)O_(5)uptake,and the maximum production rate of NO_(3)^(-)reached 6.5 ppbv/hr.The average NOx consumption rate via NO_(3)and N_(2)O_(5)chemistry was found to be 0.4 ppbv/h,accounting for 47.9%of the total NO_(x)removal.The predominant roles of NO_(3)and N_(2)O_(5)in nitrate formation and NO_(x)removal in the YRD region was highlighted in this study.展开更多
NO3 and N2O5 are important participants in nocturnal atmospheric chemical processes,and their concentrations are of great significance in the study of the mechanism of nocturnal atmospheric chemical reactions.A two-ch...NO3 and N2O5 are important participants in nocturnal atmospheric chemical processes,and their concentrations are of great significance in the study of the mechanism of nocturnal atmospheric chemical reactions.A two-channel diode laser based cavity ring-down spectroscopy(CRDS)instrument was developed to monitor the concentrations of NO3 and N2O5 in the atmosphere.The effective absorption length ratio and the total loss coefficient of the instrument were calibrated using laboratory standard samples.The effective absorption cross section of NO3 at 662 nm was derived.A detection sensitivity of 1.1 pptv NO3 in air was obtained at a time resolution of 1 s.N2O5 was converted to NO3 and detected online in the second CRDS channel.The instrument was used to monitor the concentrations of NO3 and N2O5 in the atmosphere of winter in Hefei in real time.By comparing the concentration changes of pollutants such as nitrogen oxides,ozone,PM2:5 in a rapid air cleaning process,the factors affecting the concentrations of NO3 and N2O5 in the atmosphere were discussed.展开更多
基金supported by the National Natural Science Foundation of China(Nos.42030609,91644107,61905003,and U19A2044)the Natural Science Foundation of Anhui Province(No.2008085J20)+1 种基金the National Key Research and Development Program of China(No.2017YFC0209403)the Cultivating Project of Strategic Priority Research Program of Chinese Academy of Sciences(No.XDPB1901)
文摘Comprehensive observations of the nocturnal atmospheric oxidation of NO_(3)and N_(2)O_(5)were conducted at a suburban site in Changzhou in the YRD using cavity ring-down spectroscopy(CRDS)from 27 May to 24 June,2019.High concentrations of NO_(3)precursors were observed,and the nocturnal production rate of NO_(3)was determined to be 1.7±1.2 ppbv/hr.However,the nighttime NO_(3)and N_(2)O_(5)concentrations were relatively low,with maximum values of 17.7 and 304.7 pptv,respectively,illustrating the rapid loss ofNO_(3)andN_(2)O_(5).Itwas found that NO_(3)dominated the nighttime atmospheric oxidation,accounting for 50.7%,whileO3 andOH only contributed 34.1%and 15.2%,respectively.For the reactions of NO_(3)with volatile organic compounds(VOCs),styrenewas found to account for 60.3%,highlighting its dominant role in the NO_(3)reactivity.In general,the contributions of the reactions between NO_(3)and VOCs and the N_(2)O_(5)uptake to NO_(3)losswere found to be about 39.5%and 60.5%,respectively,indicating that N_(2)O_(5)uptake also played an important role in the loss of NO_(3)and N_(2)O_(5),especially under the high humidity conditions in China.The formation of nitrate at night mainly originated from N_(2)O_(5)uptake,and the maximum production rate of NO_(3)^(-)reached 6.5 ppbv/hr.The average NOx consumption rate via NO_(3)and N_(2)O_(5)chemistry was found to be 0.4 ppbv/h,accounting for 47.9%of the total NO_(x)removal.The predominant roles of NO_(3)and N_(2)O_(5)in nitrate formation and NO_(x)removal in the YRD region was highlighted in this study.
基金Hao Wu,Jian Chen,An-wen Liu,and Shui-ming Hu acknowledge the supports from the Ministry of Science and Technology of China(No.2013BAK12B00)the National Natural Science Foundation of China(No.21427804).
文摘NO3 and N2O5 are important participants in nocturnal atmospheric chemical processes,and their concentrations are of great significance in the study of the mechanism of nocturnal atmospheric chemical reactions.A two-channel diode laser based cavity ring-down spectroscopy(CRDS)instrument was developed to monitor the concentrations of NO3 and N2O5 in the atmosphere.The effective absorption length ratio and the total loss coefficient of the instrument were calibrated using laboratory standard samples.The effective absorption cross section of NO3 at 662 nm was derived.A detection sensitivity of 1.1 pptv NO3 in air was obtained at a time resolution of 1 s.N2O5 was converted to NO3 and detected online in the second CRDS channel.The instrument was used to monitor the concentrations of NO3 and N2O5 in the atmosphere of winter in Hefei in real time.By comparing the concentration changes of pollutants such as nitrogen oxides,ozone,PM2:5 in a rapid air cleaning process,the factors affecting the concentrations of NO3 and N2O5 in the atmosphere were discussed.
