Unsaturated ketones are typical oxygenated volatile organic compounds(OVOCs)with high reactivity,and are important precursors in air pollution.The sources of OVOCs are complex and include direct emissions and secondar...Unsaturated ketones are typical oxygenated volatile organic compounds(OVOCs)with high reactivity,and are important precursors in air pollution.The sources of OVOCs are complex and include direct emissions and secondary oxidation formation of VOCs in the atmosphere.2-Cyclohexen-1-one is a widespread substance,and is derived from the industrial catalytic oxidation of cyclohexene.In this paper,we investigated the rate constants of the chemical reactions of 2-cyclohexen-1-one with NO_(3) radicals,which is(7.25±0.29)×10^(-15) cm^(3)·molecule^(-1)·s^(-1) at 298 K and under 1 atm(1 atm=101325Pa).It supplemented the kinetics of NO_(3) radicals database,and revealed its effects in the nighttime atmosphere.In addition,the reaction products of 2-cyclohexen-1-one with NO_(3) radicals were detected by Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS),which revealed a series of nitrate esters in the composition of the secondary organic aerosol(SOA),which may reduce atmospheric visibility.Finally,the possible pathways for the generation of the products were developed.展开更多
Due to altering the budget of important trace gases and changing the composition of atmospheric aerosols,heterogeneous reactions between trace gases and liquid/solid aerosols have become an important subject of atmosp...Due to altering the budget of important trace gases and changing the composition of atmospheric aerosols,heterogeneous reactions between trace gases and liquid/solid aerosols have become an important subject of atmospheric science in recent years.However,the kinetics and mechanism of these reactions have not been well-understood yet.In recent years,we have established an integrated method to study a series of atmospheric heterogeneous reactions under control atmospheric conditions.Using on-line techniques,such as Diffuse Reflectance Infrared Fourier Transform spectroscopy,Raman microspectrometry and Knudsen cell,the heterogeneous reactions of a series of trace gases(NO2,SO2,H2O2,DMS,C2H5 I and Monocarboxylic acids)on mineral oxides and black carbon were investigated.The uptake coefficients and mechanisms at different atmospheric conditions(temperature,relative humidity and reactant concentration)were obtained.In addition,a home-made equipment named rotated wetted-wall reactor was designed for the in situinvestigations of the uptake of volatile organic compounds into the H2SO4 solution and H2SO4/H2O2 mixed solution.In this review,we present the main results obtained in our laboratory studies and propose some challenges that still exist in the heterogeneous reaction studies.展开更多
基金supported by the National Natural Science Foundation of China(Nos.42130606,42022039)the Fund of the Beijing National Laboratory for Molecular Sciences China(No.BNLMS-CXXM-202011)the Project of the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.Y2021013).
文摘Unsaturated ketones are typical oxygenated volatile organic compounds(OVOCs)with high reactivity,and are important precursors in air pollution.The sources of OVOCs are complex and include direct emissions and secondary oxidation formation of VOCs in the atmosphere.2-Cyclohexen-1-one is a widespread substance,and is derived from the industrial catalytic oxidation of cyclohexene.In this paper,we investigated the rate constants of the chemical reactions of 2-cyclohexen-1-one with NO_(3) radicals,which is(7.25±0.29)×10^(-15) cm^(3)·molecule^(-1)·s^(-1) at 298 K and under 1 atm(1 atm=101325Pa).It supplemented the kinetics of NO_(3) radicals database,and revealed its effects in the nighttime atmosphere.In addition,the reaction products of 2-cyclohexen-1-one with NO_(3) radicals were detected by Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS),which revealed a series of nitrate esters in the composition of the secondary organic aerosol(SOA),which may reduce atmospheric visibility.Finally,the possible pathways for the generation of the products were developed.
基金supported by the National Natural Science Foundation of China(Grant Nos.40925016 & 40830101)
文摘Due to altering the budget of important trace gases and changing the composition of atmospheric aerosols,heterogeneous reactions between trace gases and liquid/solid aerosols have become an important subject of atmospheric science in recent years.However,the kinetics and mechanism of these reactions have not been well-understood yet.In recent years,we have established an integrated method to study a series of atmospheric heterogeneous reactions under control atmospheric conditions.Using on-line techniques,such as Diffuse Reflectance Infrared Fourier Transform spectroscopy,Raman microspectrometry and Knudsen cell,the heterogeneous reactions of a series of trace gases(NO2,SO2,H2O2,DMS,C2H5 I and Monocarboxylic acids)on mineral oxides and black carbon were investigated.The uptake coefficients and mechanisms at different atmospheric conditions(temperature,relative humidity and reactant concentration)were obtained.In addition,a home-made equipment named rotated wetted-wall reactor was designed for the in situinvestigations of the uptake of volatile organic compounds into the H2SO4 solution and H2SO4/H2O2 mixed solution.In this review,we present the main results obtained in our laboratory studies and propose some challenges that still exist in the heterogeneous reaction studies.
