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Abbreviation (ISO4): Prog Chem      Editor in chief: Jincai ZHAO

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Progress in Chemistry >

2024 , Vol. 36 >Issue 8: 1145 - 1156

DOI: https://doi.org/10.7536/PC240111

Review

Atmospheric Chemistry and Measurement Research on Organic Nitrates

  • Dou Shao 1, 2 ,
  • Min Qin , 1, * ,
  • Wu Fang 1 ,
  • Baobin Han 1, 2 ,
  • Jianye Xie 1, 2 ,
  • Xiadan Zhao 1, 2 ,
  • Zhitang Liao 1, 2 ,
  • Jiaqi Hu 1, 2 ,
  • Enbo Ren 1, 2
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  • 1 Key Laboratory of Environmental Optics and Technology, Anhui Institute of Optics and Fine Mechanics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China
  • 2 University of Science and Technology of China, Hefei 230026, China
*e-mail:

Received date: 2024-01-11

  Revised date: 2024-03-23

  Online published: 2024-07-01

Supported by

National Natural Science Foundation of China(42175151)

National Natural Science Foundation of China(U21A2028)

National Key Research & Development Program of China(2022YFC3701100)

Plan for Anhui Major Provincial Science & Technology Project(202203a07020003)

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Abstract

Organic nitrates(ONs)are an important nitrogen-containing organic compounds in the atmosphere.Atmospheric ONs are primarily produced by secondary photochemical reactions between atmospheric oxidants and volatile organic compounds in the presence of nitrogen oxides.Their generation and removal processes are closely related to the atmospheric nitrogen cycle,ozone,and the formation of secondary organic aerosols.Additionally,partial gas-phase ONs can enter the particle phase through gas-particle distribution or multiple oxidations,forming particle-phase ONs,which will promote the generation of PM2.5and further damage to human health.Currently,various chemical and spectroscopic measurement techniques have been successfully applied to measure the concentrations of single species and total ONs,and comprehensive field observations of various atmospheric components have been carried out in different regions to explore the mechanism of ONs generation involving nitrogen oxides,the impact of ONs on regional nitrogen chemistry,and the contribution of particulate ONs to secondary organic aerosols.This article discusses the important role of ONs in atmospheric chemistry by elucidating their mechanisms of generation and removal.It summarizes the measurement methods for ONs and highlights the characteristics and applications of different methods.The focus is placed on indoor smoke chamber researches related to ONs and field observation results in different regions.The observed data combined with atmospheric chemical models,further explain the atmospheric chemical effects of ONs.Additionally,it identifies some shortcomings in current researches,that need to be improved in subsequent researches 。

Contents

1 Introduction

2 Sources and sinks of atmospheric organic nitrates

3 Quantification methods of atmospheric organic nitrates

4 Researches on indoor smog chamber of organic nitrates

5 Field observations of organic nitrates

5.1 International field observations

5.2 Domestic field observations

6 Conclusion and outlook

Key words： organic nitrates; atmospheric chemistry; measurement technology; field observations

Cite this article

Dou Shao , Min Qin , Wu Fang , Baobin Han , Jianye Xie , Xiadan Zhao , Zhitang Liao , Jiaqi Hu , Enbo Ren . Atmospheric Chemistry and Measurement Research on Organic Nitrates[J]. Progress in Chemistry, 2024 , 36(8) : 1145 -1156 . DOI: 10.7536/PC240111

1 Introduction

Organic nitrates(ONs)generally refer to a class of Organic compounds containing nitrate functional group（—ONO2）,which is an important reactive nitrogen oxide（NOy=NO+NO2+NO3+ΣONs+HNO3+HONO+2N2O5+…）.According to the structure of other groups in ONs,they can be divided into peroxynitrates（RO2NO2,PNs)and alkyl nitrates（RONO2,ANs).PNs(PANs)containing acyl groups have relatively high thermal stability and are relatively abundant in the atmosphere,while those without acyl groups are susceptible to thermal decomposition and are less abundant in the atmosphere[1]。 According to the length of carbon chain,ANs can be divided into short-chain ANs(C≤2),medium-long-chain ANs(3≤C≤5)and long-chain ANs(C>5)[2]。 ONs in the atmosphere mainly come from the interaction process of volatile organic compounds(VOCs)and atmospheric oxidants,and the ONs generated by the reaction of$\mathrm{RO}\bullet$/$\mathrm{RO}\bullet_{2}$and NO2can be used as a reservoir of nitrogen oxides（NOx）,which can be transported to remote areas through the atmosphere and decomposed again to release NOx,which plays an important role in the regional nitrogen cycle,and then affects the subsequent generation of ozone（O3）[3,4]。 In addition,gas-phase ONs with different volatilities can also enter the particle phase through gas-particle partitioning or multiple oxidation to form particle-phase ONs,which has an important impact on the formation of secondary organic aerosols(SOA)in areas with high NOxlevels.Observed data show that particulate ONs account for 9%to 25%of organic aerosols(OA)in urban areas and 5%to 12%of OA in rural areas in the southeastern United States[5]; In the forest area of Bakersfield,monoterpene oxidation dominates the production of ONs at night,contributing about 27%to 40%to the growth of OA[6]; In addition,particle-phase ONs from secondary transformation are also widespread in OA fractions in urban and rural areas of Europe,accounting for an average of 42%of the organic fraction in PM1[7]; Airborne observations over the Korean Peninsula show that 25%of ONs are in the particulate phase,which is expected to account for 15%of OA[8]; in Beijing,China,particulate ONs in OA in winter can reach 25%[9]。 Particle-phase ONs in atmospheric particulate matter can further affect The atmospheric environment and endanger human health.the source,sink and atmospheric chemistry of ONs have attracted more and more attention。
in the actual atmospheric environment,there are many kinds of VOCs precursors of ONs,and the physical and chemical processes affecting their formation vary with the atmospheric environment,so the ONs generated are also varied,and various measurement techniques are used to quantify the single species of ONs and the total amount of ONs.field observations have been carried out in many regions around the world,but due to the lack of standards,it is difficult to quantify ONs with different structures and properties.At present,atmospheric chemistry studies are mostly carried out by combining Field observation data with atmospheric chemistry models,or by carrying out smog box studies for ONs generation in the laboratory[10⇓⇓⇓⇓⇓⇓⇓~18]。 in this paper,the generation and dissipation mechanism,measurement methods,indoor smoke chamber research and field observation of ONs are summarized In detail,the latest research progress of ONs is clarified,and the future development direction is summarized。

2 Sources and sinks of atmospheric organic nitrates

ONs in the atmosphere are mainly divided into natural sources and anthropogenic sources.As the most abundant species in PNs,peroxyacetyl nitrate(PAN)was first discovered in the Los Angeles smog event[19]。 There is no natural source of PAN in the atmosphere,and it can only be generated secondarily through subsequent photochemical reactions,which has been used as one of the important indicators of photochemical pollution[20,21]。 Unlike PAN,ANs can be either directly emitted by nature or produced by humans.Primary emissions from the ocean and biomass burning are the main natural sources[22,23][24⇓~26]。 The volatilization of saturated short-chain ANs in tropical waters is the main natural source of short-chain ANs.For example,methyl nitrate（MeONO2）is the most affected by marine emissions,and the direct emission of ANs from the ocean gradually decreases with the increase of carbon chain[27,28]; In temperate waters,ANs are In equilibrium and are not volatile.In addition to natural emission sources,ANs can be secondarily generated through photochemical reactions.The three main pathways of secondary photochemical reaction to ONs include:[29,30]
(1)Hydrocarbon oxidation initiated by OH radicals
Hydrocarbon oxidation initiated by OH radicals is the main pathway for the formation of ONs during daytime.Under the oxidation of OH radicals,saturated hydrocarbons undergo dehydrogenation or unsaturated hydrocarbons undergo addition reaction to form$\mathrm{R}\bullet$(formula 1),followed by rapid reaction of$\mathrm{R}\bullet$with O2to form$\mathrm{RO}_{2\bullet}$(formula 2 )。
$\mathrm{RH} / \mathrm{R}_{1}=\mathrm{R}_{2}+\mathrm{OH} \rightarrow \mathrm{R} \bullet+\mathrm{H}_{2} \mathrm{O}$
$\mathrm{R} \bullet+\mathrm{O}_{2} \rightarrow \mathrm{RO}_{2} \bullet$
In the presence of NOx,the branching reaction of$\mathrm{RO}_{2\bullet}$and NO generates$\mathrm{RO}\bullet$and NO2(Equation 3),which continue to participate in the NOxcycle,and the branching reaction(Equation 4)generates ANs,in which(Equation 3)plays a dominant role,and the branching ratio of the reaction isα.$\mathrm{RO}_{2\bullet}$also reacts with NO2to generate PNs(Equation 5).In general,the yield of ONs from the reaction of unsaturated hydrocarbon compounds with OH radicals is higher than that of saturated hydrocarbon compounds,and both isoprene andα-pinene react with OH radicals to form ONs through addition[9,31]。
$\alpha \mathrm{RO}_{2} \bullet+\mathrm{NO} \rightarrow \mathrm{RO} \bullet+\mathrm{NO}_{2}$
$(1-\alpha) \mathrm{RO}_{2} \bullet+\mathrm{NO} \rightarrow \mathrm{RONO}_{2}$
$\mathrm{RO}_{2} \bullet+\mathrm{NO}_{2} \rightarrow \mathrm{RO}_{2} \mathrm{NO}_{2}$
Olefin Oxidation Initiated by（2）NO3Radical
Olefin oxidation initiated by NO3radicals is the main pathway for the formation of ONs at night.The NO3radical reacts with the carbon-carbon double bond to form$\mathrm{R}\bullet$(Equation 6),and similar to(Equation 2),$\mathrm{R}\bullet$rapidly reacts with O2to form$\mathrm{RO}_{2\bullet}$(Equation 7).$\mathrm{RO}_{2\bullet}$reacts with HO2,RO2,or NO3to form a stable aldehyde,alcohol,or nitrate product 。
$\mathrm{R}_{1}=\mathrm{R}_{2}+\mathrm{NO}_{3} \rightarrow \mathrm{R}_{1}\left(\mathrm{ONO}_{2}\right) \mathrm{R}_{2} \bullet$
$\mathrm{R}_{1}\left(\mathrm{ONO}_{2}\right) \mathrm{R}_{2} \bullet+\mathrm{O}_{2} \rightarrow \mathrm{R}_{1}\left(\mathrm{ONO}_{2}\right) \mathrm{R}_{2} \mathrm{O}_{2}$
Biogenic Volatile Organic Compounds Oxidation Induced by（3）O3 ;
O3reacts with carbon-carbon double bonds to form primary ozone compounds(POZ)(Equation 8),POZ rapidly decomposes via a Kjeldahl intermediate to form OH and$\mathrm{RO}_{2}$（in the presence of O2),and in the presence of NO,RO2generates ONs via a series of oxidation reactions(Equation 9).In addition,O3can also produce OH radicals by photolysis or react with NO2to produce NO3radicals,which can be further oxidized with VOCs to produce ONs 。
$\mathrm{R}_{1}=\mathrm{R}_{2}+\mathrm{O}_{3} \rightarrow \mathrm{POZ}$
$\mathrm{POZ}+\mathrm{O}_{2} \rightarrow \mathrm{OH}+\mathrm{RO}_{2} \rightarrow \mathrm{ONs}$
In the first generation of ONs produced by the above process,the ONs with lower volatility directly enter the particle phase through gas-particle partitioning,while the ONs with higher volatility are oxidized many times to produce multifunctional ONs with more stability and lower saturated vapor pressure,and then enter the particle phase through gas-particle partitioning[29]。 the gas-particle partition of ONs follows the adsorption partition theory,and the fraction of a substance in equilibrium in the stationary phase can be expressed by formula(1):[32]
$K_{\mathrm{p}}=\frac{C_{\mathrm{i}, \mathrm{p}}}{C_{\mathrm{i}}}=\frac{C_{\mathrm{OA}} / C_{\mathrm{i}}^{*}(T)}{1+C_{\mathrm{OA}} / C_{\mathrm{i}}^{*}(T)}$
Where$C_{i,p}$and$C_{i}$represent the concentration of species I in the particulate phase and the total concentration in the atmosphere(including gas phase and particulate phase),respectively,$C_{\mathrm{i}}^{*}(T)$represents the temperature(T)-dependent saturation concentration of species I,and C{OA}represents the concentration of OA.According to equation(1),the air-particle partition balance is related to T as well as OA concentration[33]。 However,due to the complexity of the atmospheric environment and the diversity of ONs,the process of multiple oxidation of different kinds of gas-phase ONs to particle-phase ONs is still worth exploring,which is of great significance for the atmospheric chemical estimation and environmental impact assessment of secondary organic matter。
The generated ONs are removed by photolysis,hydrolysis,thermal decomposition,and sedimentation[34][35][36]。 For example,in the stratosphere above 7 km,photolysis is the most important removal pathway of PAN,and the main loss pathway of PAN in the troposphere is thermal decomposition[37]; For ANs,reaction with OH(Formula 10),photolysis(Formula 11)and hydrolysis are important loss pathways,which compete with each other.the number of alkyl substituents,functional groups and carbon skeleton are three important factors controlling The hydrolysis rate of ANs[38,39][39⇓~41][35]。
$\mathrm{RONO}_{2}+\mathrm{OH} \rightarrow \mathrm{ROH}+\mathrm{NO}_{3}$
$\mathrm{RONO}_{2}+\mathrm{h} \nu \rightarrow \mathrm{RO}+\mathrm{NO}_{2}$
the generation and elimination mechanisms of the above different types of ONs cannot be generalized.Precursor VOCs,oxidants and atmospheric environment all have effects on the generation of ONs,and the research on the removal methods of ONs such as photolysis and hydrolysis is relatively limited.understanding the sources and sinks of different ONs as deeply as possible will help to improve the atmospheric model and make a deeper Understanding of the atmospheric nitrogen cycle。

3 Quantification of atmospheric organic nitrates

There are many kinds of ONs and their concentrations in The atmosphere are relatively low,so it is very difficult to quantify different kinds of ONs.at present,most of them are aimed At specific kinds of ON or the total amount of ON.the common quantitative methods include Gas chromatography/Liquid chromatography mass spectrum(GC/LC-MS),Gas chromatography-electron capture detector(GC-ECD),and Chemical ionization mass spectrometry(CIMS[42⇓⇓⇓~46][47⇓~49][50⇓~52][53⇓~55][56,57][58⇓⇓⇓⇓⇓⇓⇓⇓~67]。 A variety of quantitative methods provide options for outfield observations of ONs.Table 1 summarizes the characteristics and applications of different quantitative methods.Several measurement methods are described in detail below。
表1 Different quantitative methods for ONs[42⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓~67]

Table 1 The different quantitative methods for organic nitrates[42⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓~67]

Method Characteristic Application Ref
GC/LC-MS Low resolution, long offline analysis time Quantitative specific ONs 42⇓⇓⇓~46
GC-ECD Low detection limit and high sensitivity Quantitative specific ONs 47⇓~49
CIMS Soft ionization, fast response, high sensitivity, and strong selectivity Quantitative specific ONs 50⇓~52
AMS High resolution; uncertainty exists in the ratio method Quantitative ∑ONs 53⇓~55
FTIR Mature and simple, no pre-processing required; low resolution, high detection limit Quantitative ∑ONs 56,57
TD High resolution, sensitivity, requiring interference correction Quantitative ∑ONs 58⇓⇓⇓⇓⇓⇓⇓⇓~67
GC-MS was one of the early methods used to quantify specific ONs[29]。 In this method,the collected membrane samples were separated by gas chromatography,and then the fragments were separated by mass spectrometry according to the different mass-to-charge ratios of ions,so as to realize the quantitative analysis of specific ONs.GC-MS is suitable for the separation and determination of semi-volatile ONs;LC-MS is suitable for the quantitative analysis of thermally unstable and polar ONs.The two methods can provide a strong basis for the identification of complex ONs.GC-ECD is a commonly used quantitative analysis method.The difference between this method and GC-MS is that the detector is different.ECD detector is a kind of radioactive ionization detector,which usesβ-particles with a certain energy emitted in the decay process of radioactive isotopes as the ionization source.When the carrier gas separated by gas chromatography contains a small amount of electronegative components into the ion chamber,the base flow changes significantly,so as to obtain the concentration information of specific ONs.At present,GC-ECD is mostly used for quantitative analysis of PAN.FIGAERO-CIMS uses reactive ions to adduct to nitrate molecules for mass spectrometry,which has soft ionization,fast response and high sensitivity,and can realize real-time measurement of a variety of ONs.AMS uses a hard ionization source to obtain the NO+/NO2+information of mass spectrometry fragments,and uses the difference of the ratio in organic and inorganic nitrates to distinguish and quantifyΣONs(ratio method),but the NO+/NO2+ratio of different ONs is also different,so there is uncertainty.AMS combined with the orthogonal factor matrix receptor model(PMF)can analytically judge the relative contribution of organic and inorganic nitrate,which can compensate for the error caused by the uncertainty of the ratio method to a certain extent 。
Distinguishing from the above chemical methods,FTIR is one of the early spectroscopic methods used to quantifyΣONs[57]。 The method uses the specific absorption(860,1280,1630~1640 cm-1）)of the nitrate functional group in the infrared spectrum to quantify the total amount,and the measurement process does not require pretreatment,which is simple and convenient,but has low resolution and high detection limit.TD method was first proposed by Day et al.,which is one of the commonly used methods to quantifyΣONs[58]。 The method takes advantage of the thermal decomposition characteristics of ONs,which is heated to different temperatures to decompose into NO2and other free radicals(RO or RO2）),and the laser-induced fluorescence detector(LIF)is used to measure the NO2produced by decomposition,thus realizing the measurement ofΣPNs andΣANs.In 2009,Paul et al.Combined TD and cavity ring-down spectroscopy(CRDS)to measure atmospheric NO2,ΣPNs andΣANs simultaneously[59]。 Rollins et al.Combined with a gas stripper to quantify particulate phase ONs[62]。 In 2021,Li et al.Combined with Broadband Cavity Enhanced Absorption Spectroscopy(BBCEAS)also realized the classification measurement ofΣONs[64]。
as mentioned above,a variety of measurement methods have been successfully applied to laboratory studies and field observations under different conditions.for the measurement of specific ONs,it is mostly dependent on the standard,and the instrument needs to be calibrated regularly(such as GC/LC-MS and GC-ECD).in addition,when comparing the observed data with the model processing results,the measurement bias may be caused by the lack of understanding of the unknown ONs generated in a specific atmospheric environment.In order to meet the requirements of long-term,rapid and accurate measurement,the TD method is often Used for the field observation ofΣONs,but this method has a variety of interference factors,which need to be considered in the instrument design method,such as the deduction of known interference factors or quantitative calibration,and the requirements for instrument design and laboratory calibration are high.In addition,the TD method can also be Used to study the gas-particle distribution of ONs.Aruffo et al.used the TD-LIF technology to study the gas-particle distribution of ONs formed by photooxidation ofα-pinene.Rollins et al.used the observation data of TD-LIF in Bakersfield,USA,and showed that 21%ofΣANs were in the particle phase[68][32]。

4 Indoor smog chamber study of organic nitrates

in order to further clarify the formation mechanism of ONs and its impact on atmospheric chemistry,many research groups have conducted smoke chamber simulations in the laboratory,reacting different VOCs precursors with atmospheric oxidants,and measuring the ONs generated in different reaction systems.VOCs commonly used in smog chamber simulation include biogenic VOCs(BVOCs)and anthropogenic VOCs(AVOCs)。
At present,isoprene and monoterpenes(α-pinene,β-pinene,limonene,etc.)Are the main BVOCs related to the smoke chamber experiment of ONs.All kinds of BVOCs will react rapidly to produce SOA and ONs in the presence of NOx,but the yield of ONs is different due to the different kinds of BVOCs.The yield of ONs in the+NO3”of isoprene is 65%~90%,and the high yield ONs can be used as the sink of NOxat night[69⇓⇓~72]。 Studies on the+NO3”ofα-pinene show that,due to different experimental conditions(source of（NO3,concentration of precursor and choice of seed particle),The reaction pathway（“RO2+RO2”,“RO2+NO3”and“RO2+HO2”）of RO2are different,resulting in a large difference in the yield of SOA(0~>21%),so the yield of ONs is controversial[73⇓⇓⇓~77]。 In most studies,the"α-pinene+OH"reaction was mainly used to obtain high yields of SOA and ONs.For example,Rindelaub et al.Reported the photochemical reaction of"α-pinene+OH"under high NOxconditions with an ONs yield of 26%±7%[78]。 In addition,the gas-particle partition of ONs obtained from the reaction of"α-pinene+OH"was correlated with OA concentration,temperature,and NOxlevel[68,79]。 Highly oxygenated ONs(HOM-ONs)were observed in the"α-pinene&β-pinene+OH"and"β-pinene+NO3”"reactions,and their formation could be explained by unimolecular or bimolecular reactions of RO2radicals[80,81]。 Experiments have shown that the yield of"limonene+NO3”"is equivalent to that of"limonene+OH"(~30%),but the reaction between"liminene+NO3”"and OH shows that there is an unclear reaction pathway in the RO2,which still needs further exploration[82,83][83]。 Some studies have also carried out smoke chamber simulation on the removal methods of ONs in different systems,such as photolysis and hydrolysis.The photolysis rate of gas-phase ONs(MT-ONs)produced by the reaction of"monoterpene+OH"is less than that of C1-C6ANs,which may be due to the larger absorption cross-section of MT-ONs[39]。 Relative humidity and PH have a great influence on the hydrolysis rate of ONs[78,79,84⇓ ~86]。 NOxcan be effectively removed by photolysis and hydrolysis of ONs.In general,the smog chamber study of different BVOCs oxidation systems is of great significance for atmospheric chemical analysis in areas with large emissions such as forests(such as the southeastern United States),and provides necessary theoretical support for complex field observations.However,the formation of related ONs is still highly uncertain due to different experimental conditions(BVOCs species and concentrations,oxidant sources and concentrations,NOxlevels,relative humidity,etc.)And unclear reaction mechanism(dominant reaction of（RO2loss).The research on the removal methods such as hydrolysis and photolysis of ONs is also limited,and the laboratory simulation under controllable conditions of ONs will be further improved and further analyzed with the observation data in the future 。
Smog box simulations of the oxidation of AVOCs to ONs are relatively rare.Photooxidation of aromatic hydrocarbons such as toluene is a potential source of urban SOA[87]。 The oxidation of aromatic hydrocarbons such as benzene and OH radicals generally proceeds by addition to form benzene-OH adducts,which react with O2to give RO2radicals,followed by a series of reactions or termination products,including PNs[88⇓~90]。 In addition,several studies have revealed that the formation of SOA by aromatic oxidation depends on the level of NOx,which may be related to the formation of ONs[87,88,91,92]。 However,the understanding of ONs generated by oxidation of AVOCs is still very limited,and further research is needed。

5 Outfield observation of organic nitrates

5.1 International field observation

the field observation of ONs was first carried out in Europe and The United States.PAN was first found as photochemical smog pollution.The concentration of PAN varies significantly with different pollution levels and different atmospheric environments.in clean areas,the concentration of PAN can be as low as pptv,while in heavily polluted urban areas,it can reach tens of ppbv[19]。 in 1988,Atlas reported the observation of C≥3 ANs in the troposphere of the North Pacific Ocean,and its concentration level was in the order of pptv,which directly verified the existence and transport of ANs in the troposphere[93]。 since the 21st century,with the continuous development of measurement technology,field observation activities related to ONs have been carried out one after another.Table 2 summarizes the field observations related to ONs in foreign regions Since 2010,mainly including observations over Europe(Finland,the United Kingdom,and Germany),North America(the United States,Canada,and Mexico),Asia(South Korea and Japan),and some oceans[30,94][95][16][6,32,50,96⇓⇓⇓⇓⇓⇓ ~103][24,25][43][13,104][105][106]。 the main measurement methods were TD and GC-ECD.It can be seen from Table 2 that the overall concentration of ONs is low.with the different types of observation stations,the concentration of ONs varies within the range of<0.1~1.87 ppbv.the concentration in remote areas is low,while the concentration in urban areas With large traffic volume and greatly affected by human activities is relatively high;the concentration of ONs is mainly affected by the local photochemical reaction and the transmission of polluted air masses in other areas[30,96,104]; In the area not affected by the external aging air mass,the formation mechanism of ONs is clear,and has obvious diurnal and seasonal variation trends;Multiple outfield observations show that the formation of ONs in the daytime and nighttime is dominated by OH radicals and NO3radicals,respectively,and the generated ONs can be used as a temporary reservoir of NOx.Sobanski et al.Observed that the ONs generated by photochemical reactions can be used as a reservoir of up to 75%of the local NOxat the mountaintop forest city site in southwestern Germany,and observed that ONs account for 30%-45%of the NOyin SOAS outfield observations[16,30,96,97,101][16][96]; In addition,some measurement results show that ONs are related to the formation of SOA and O3.For example,Rollins et al.estimated through observation and calculation that ANs in particulate phase account for 17%~23%of OA in Sheffield,California.In KORUS-AQ airborne observation,1/4 of ONs are in particulate phase,contributing about 15%to OA.Lindaas et al.observed that the formation of high concentration of O3is related to PANs in Colorado[32][8][107]; The occurrence of some pollution events may lead to a significant increase in the concentration of ONs.In the 2010 Gulf of Mexico oil spill and two airborne measurements of the London plume,high NOxemissions and some volatile alkanes reacted quickly.Since the generation of ANs and O3compete with each other,the generation of O3is inhibited when ANs are generated rapidly,and the atmospheric chemical processes in these pollution events can be well explained by the existing NOx-VOCs-ONs oxidation mechanism[43][95]。
表2 Field Observation of Organic Nitrate Esters Abroad in the Past 2010[6,8,13,16,24,25,30,32,43,50,94⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓ ~113]

Table 2 Field observations on organic nitrates in foreign regions since 2010[6,8,13,16,24,25,30,32,43,50,94⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓ ~113]

At present,the oxidation of ONs has been verified in areas with high BVOCs emissions,and their correlation with local SOA,NOxand O3has been extensively studied[6,50,94,95,98,100]; However,some observations and model analysis results over cities and oceans show that there are still some unexplained ONs sources,which may be related to the oxidation mechanism of AVOCs-NOx,and need to be further explored in combination with the laboratory experiments mentioned above[8]。

5.2 Domestic and foreign field observation

With the development of modern industry,air pollution in China is becoming more and more serious.Urban areas with developed industry and dense population have been suffering from air pollution such as haze and photochemical smog for a long time.In view of the complex atmospheric environment with high NOxand high pollution in some areas of China,the field observation of ONs has gradually increased in recent years,mainly in the North China Plain,the Yellow River Delta,the Pearl River Delta and Hong Kong,and the field observation data are still relatively scarce[17,114⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓ ~128][129⇓~131][132⇓~134][27,135⇓⇓⇓ ~139]。
In the spring and summer of 1990,the research team of Peking University used GC-ECD to measure PAN in Zhongguancun,Beijing,and the results showed that the concentration of PAN was related to the levels of O3and NOx,and the concentration in summer was significantly higher than that in spring.In addition,the laboratory simulation also proved that ethane（C3H6）was an important precursor of PAN in the atmosphere[140]。 Since the 20th century,the field observation of PAN has gradually increased,and the measurement sites are mostly concentrated in the suburban areas of key cities and some remote areas(Qinghai-Tibet Plateau).From August to September 2022,the observation results of Zhang et al.At a typical urban sampling site in Beijing showed that the average and maximum concentrations of PAN were(1.00±0.97)ppbv and 4.84 ppbv,respectively[141]; The average concentration during the severe photochemical pollution period was about 3.1 times higher than that during the cleaning period.In addition,there was a good positive correlation between O3and PAN.The analysis results also showed that acetaldehyde（CH3CHO）and methylglyoxal（CH3COCHO）were the largest precursors for the formation of PNs,and their contributions to the total PA radicals were about 67%-83%and 17%-30%,respectively.In November 2008,Li et al.Carried out a four-month observation campaign in the rural area of Wangdu,Hebei Province,and the maximum and average values of PAN were 4.38 ppbv and(0.93±0.67)ppbv,respectively.The diurnal variation and formation rate of PAN were related to the concentration of PM2.5.The double-peak interlacing phenomenon of PAN and PM2.5provided a basis for its possible aggravation of haze through the formation of SOA[142]。 Xu et al.Conducted two measurements in the Nam Co Plateau region from August 17 to 24,2011 and from May 15 to July 13,2012,respectively,and the average concentrations were 0.36 ppbv and 0.44 ppbv,respectively,which were significantly lower than those in urban areas.The evolution of the boundary layer affected the diurnal patterns of PAN and O3,and pointed out that regional transport had an important impact on tropospheric photochemistry in the high altitude region of the Qinghai-Tibet Plateau[143]。 Table 3 summarizes the field observation results of PAN in some representative regions in China.It can be seen that in urban areas(Beijing,Jinan,etc.),the concentration is relatively high,and the maximum concentration can reach more than ten ppbv,while in remote areas such as the Qinghai-Tibet Plateau,the maximum concentration of PAN is only 0.99 ppbv.different regions show Different concentration levels and trends due to factors such as photochemical reactions and regional transport[143]。
表3 PAN observation in typical areas of China[117,121,128,133,143]

Table 3 PAN observations in some typical regions of China[117,121,128,133,143]

site type Time Average concentration
(ppbv)		 Maximum concentration
(ppbv)		 Ref
Beijing Rural 2015.8~2019.2 0.94 2.41 121
Urban 2016.11~2017.1 1.2 7.1 117
The Pearl River Delta Rural 2006.7~2006.7 1.3 3.9 133
Jinan, Shandong Urban 2016.4~2016.7 2.54 13.47 128
Nam Co, Tibet Plateau Remote 2012.5~2012.7 0.44 0.99 143
In 2001,Simpson et al.Measured seven C1-C5ANs in Tai O,Hong Kong,China[132]。 At present,there are more and more field observations of ANs in China,which mainly focus on the measurement of C1-C5ANs,the use of models for source apportionment and the exploration of the interaction between ANs and O3.As shown in Fig.1,the concentration of 2-BuONO2was the highest among the different AN concentrations in the pptv order,followed by 2-PrONO2in the C1-C5ANs.Wang et al.Measured C1-C4ANs concentrations in urban areas of China,and the results showed that 2-BuONO2was the most abundant ANs species,which was consistent with the observation in Hong Kong,and its concentration ranged from 48 to 88 pptv[144]。 In the past two years,Zeng et al.'s Long-term observation of ANs in Hong Kong,China showed that the average concentration of 2-BuONO2was always the highest,while the other C1-C4ANs showed an upward trend.Using PMF to analyze the sources,it was found that the formation of photochemical secondary reactions and the emission of biomass burning might be the reasons for the increase of ANs concentration in the atmospheric environment of Hong Kong[139]。 In 2017,Zhang et al conducted C1-C5ANs observations in a rural coastal area and an open-pit oil field in the Yellow River Delta region of northern China,and the concentration in summer was higher than that in winter and spring.However,its precursor VOCs showed an opposite seasonal variation pattern,which demonstrated the significant effects of oilfield emissions and biomass burning on the formation of VOCs and ANs,and provided scientific support for the development of photochemical air pollution control strategies in the Yellow River Delta region[130]。
图1 我国典型地区C1-C5ANs浓度水平[26,27,132,136,137,139,144,145]

Fig. 1 Concentration levels of C1-C5ANs in typical regions of China[26,27,132,136,137,139,144,145]

Particle-phase ONs were measured by AMS for part of the field observations.For example,Zhu et al.Observed particle-phase ONs in rural areas of the North China Plain,with a mass concentration of 1.48~3.39μg/m3,and the high correlation between particle-phase ONs and biomass burning emissions revealed that the formation of particle-phase ON may be closely related to primary emissions in rural areas of North China[115]。 In addition to the above observations of specific ONs,Li et al.Also reported the measurement results ofΣPNs andΣANs in Chengdu in the summer of 2019,and the average concentrations ofΣPNs andΣANs in the daytime were(1.3±1.1)ppbv and(0.5±0.3)ppbv,respectively.The peak values were 7.7 ppbv and 1.9 ppbv,respectively,revealing that OH oxidation of aldehydes and ketones is an important source of PNs precursors,quantifying the inhibition of O3production by PNs chemistry through modeling,and emphasizing the importance of aromatics control to mitigate photochemical pollution in Chengdu,which deepens the understanding of photochemical pollution in western cities of China[18]。

6 Conclusion and prospect

In this paper,the atmospheric chemistry,formation and disappearance mechanism,measurement method,indoor smoke chamber study and field observation of ONs are summarized in detail.As an indispensable part of regional atmospheric chemistry in the context of high NOxenvironment,its formation and removal have an important impact on atmospheric composition and atmospheric oxidation.A variety of measurement techniques provide options for ONs field observations with different requirements.Although researchers have a certain understanding of the atmospheric chemistry of ONs,there are still some unknowns that need to be further explored:
(1)Due to the variety of precursor VOCs and the different composition of ONs,there are still some limitations in the understanding of the physical and chemical characteristics of different ONs.In addition,the formation mechanism of ONs focuses on the atmospheric oxidation of BVOCs.Daytime and nighttime are dominated by OH radical and NO3radical oxidation,respectively,while AVOCs are important components in urban regional chemistry,and there are relatively few studies on their participation in the formation of ONs,which need further exploration 。
(2)The ONs measurement technique is mainly aimed at the measurement of specific ONs(such as PANs,C1-C5ANs,etc.)AndΣONs(ΣANs andΣPNs).GC-ECD is a common method to measure specific ONs,which requires regular calibration.TD method is often used to quantifyΣONs,which also has some errors due to various interference factors and depends on the interference calibration of the laboratory.Therefore,for the future measurement of ONs,it is necessary to improve the measurement technology to achieve fast and accurate online measurement of ONs to meet the measurement needs under different observation conditions 。
(3)The smog chamber study of ONs showed that the yield of ONs from different precursor VOCs varied with different conditions(oxidant concentration,precursor concentration,RH,RO2reaction pathway,NOxlevel,etc.);There are many kinds of ONs,and the removal methods of photolysis and hydrolysis of different ONs can not be generalized,so there is still a high degree of uncertainty about the laboratory research of ONs 。
(4)There is a lack of systematic analysis of gas-particle partitioning of ONs in different atmospheric environments.The gas-particle partitioning of ONs with low volatility is related to temperature,OA concentration and NOxlevel,while the structure of ONs with high volatility is different.The distribution process of ONs into the particle phase after multiple oxidations is extremely complex,and there are relatively few studies on the gas-particle distribution analysis of ONs in the actual atmosphere combined with observational data,and there is a lack of more detailed grasp and understanding of the formation of SOA by ONs in the gas phase into the particle phase 。
(5)Most of the field observations in China focus on the measurement of specific ONs,and there are fewΣONs and airborne observation data,and there is also a lack of real-time measurement of ONs in some sudden pollution events.the above observation data are combined with the model to analyze the data,reveal the special source of ONs in specific cases and the important role in atmospheric chemical processes,and further improve the atmospheric chemical mechanism of ONs。
Future research related to ONs should focus on the above deficiencies,combine and improve theoretical models,explore various aspects of ONs under different atmospheric conditions from multiple dimensions and levels,and gradually improve the comprehensive understanding of ONs,an important substance。

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