The real-time detection of the mixing states of polycyclic aromatic hydrocarbons(PAHs)and nitro-PAHs in ambient particles is of great significance for analyzing the source,aging process,and health effects of PAHs and ...The real-time detection of the mixing states of polycyclic aromatic hydrocarbons(PAHs)and nitro-PAHs in ambient particles is of great significance for analyzing the source,aging process,and health effects of PAHs and nitro-PAHs;yet there is still few effective technology to achieve this type of detection.In this study,11 types of PAH and nitro-PAH standard sampleswere analyzed using a high performance-single particle aerosolmass spectrometer(HP-SPAMS)in lab studies.The identification principles‘parent ions’and‘mass-to-charge(m/z)=77’of each compound were obtained in this study.It was found that different laser energies did not affect the identification of the parent ions.The comparative experiments of ambient atmospheric particles,cooking and biomass burning emitted particles with and without the addition of PAHs were conducted and ruled out the interferences from primary and secondary organics on the identification of PAHs.Besides,the reliability of the characteristic ions extraction method was evaluated through the comparative study of similarity algorithm and deep learning algorithm.In addition,the real PAH-containing particles from vehicle exhaust emissions and ambient particles were also analyzed.This study improves the ability of single particle mass spectrometry technology to detect PAHs and nitro-PAHs,and HP-SPAMS was superior to SPAMS for detecting single particles containing PAHs and nitro-PAHs.This study provides support for subsequent ambient observations to identify the characteristic spectrum of single particles containing PAHs and nitro-PAHs.展开更多
An experiment facility has been set up for the study of metal cluster compounds in our laboratory, which consists of a nano-electrospray ionization source, an ion transmission and focus system, and a reflectron time-o...An experiment facility has been set up for the study of metal cluster compounds in our laboratory, which consists of a nano-electrospray ionization source, an ion transmission and focus system, and a reflectron time-of-fight mass spectrometer. Taking advantage of the nano-electrospray ionization source, polyvalent ions are usually produced in the ＂ionization＂ process and the obtained mass resolution of the equipment is over 8000. The molecular ion peaks of metal cluster compounds [Au20（PPhpy2）10Cl2]（SbF6）4, where PPhpy2=bis（2- pyridyl）phenylphosphine, and [AuaAg2（C）L6]（BF4）4, where L=2-（diphenylphosphino）-5- methylpyridine, are distinguished in the respective mass spectrum, accompanied by some fragment ion peaks. In addition, the mass-to-charge ratios of the parent ions are determi- nated. Preliminary results suggest that the device is a powerful tool for the study of metal cluster compounds. It turns out that the information obtained by the instrumentation serves as an essential supplement to single crystal X-ray diffraction for structure characterization of metal cluster compounds.展开更多
ATSI Model 3800 aerosol time-of-flight mass spectrometer(ATOFMS)was deployed for single-particle analysis in Shanghai during theWorld Exposition(EXPO),2010.Measurements on two extreme cases:polluted day(1st May)and cl...ATSI Model 3800 aerosol time-of-flight mass spectrometer(ATOFMS)was deployed for single-particle analysis in Shanghai during theWorld Exposition(EXPO),2010.Measurements on two extreme cases:polluted day(1st May)and clean day(25th September)were compared to show how meteorological conditions affected the concentration and composition of ambient aerosols.Mass spectra of 90496 and 50407 particles were analyzed respectively during the two sampling periods.The ART-2a neural network algorithm was applied to sort the collected particles.Seven major classes of particles were obtained:dust,sea salt,industrial,biomass burning,organic carbon(OC),elementary carbon(EC),and NH4-rich particles.Number concentration of ambient aerosols showed a strong anti-correlation with the boundary layer height variation.The external mixing states of aerosols were quite different during two sampling periods because of different air parcel trajectories.Number fraction of biomass burning particles(43.3%)during polluted episode was much higher than that(21.6%)of clean time.Air parcels from the East China Sea on clean day diluted local pollutant concentration and increased the portion of sea salt particle dramatically(13.3%).The large contribution of biomass burning particles in both cases might be an indication of a constant regional background of biomass burning emission.Mass spectrum analysis showed that chemical compositions and internal mixing states of almost all the particle types were more complicate during polluted episode compared with those observed in clean time.Strong nitrate signals in the mass spectra suggested that most of the particles collected on polluted day had gone through some aging processes before reaching the sampling site.展开更多
It is difficult to rapidly and on-line detect trace volatile organic compounds for miniature massspectrometry due to its limited sampling volume at slow pumping speed. In this paper, we developed anew radiofrequency f...It is difficult to rapidly and on-line detect trace volatile organic compounds for miniature massspectrometry due to its limited sampling volume at slow pumping speed. In this paper, we developed anew radiofrequency field enhanced chemical ionization source （RF-ECI） with vacuum ultraviolet （VUV）lamp by coupling radiofrequency electric field and direct-current field together. The experiment resultsshowed that the sensitivity of benzene, toluene, hydrogen sulfide and other compounds increased by 2-3orders of magnitude under the introduction of RF-ECI comparing to traditional single photon ionization（SPI）. At the same time, the reagent ion of O2＋ realized the charge transfer reaction chemical ionization,and the RF-ECI effectively expanded the detection range of the VUV lamp based SPI. The VUV lamp hasinherent advantages in the on-site analytical instrument for its small size and low power consumption,and the VUV lamp based RF-ECI miniature time-of-flight mass spectrometer （TOFMS） has a limit-of-detection for H2S as low as 0.0571 mg/m3, and it is expected to be used widely in the field of on-site rapidanalvsis.展开更多
To investigate the effect of covID-19 control measures on aerosol chemistry,the chemical compositions,mixing states,and formation mechanisms of carbonaceous particles in the urban atmosphere of Liao-cheng in the North...To investigate the effect of covID-19 control measures on aerosol chemistry,the chemical compositions,mixing states,and formation mechanisms of carbonaceous particles in the urban atmosphere of Liao-cheng in the North China Plain(NCP)were compared before and during the pandemic using a single particle aerosol mass spectrometry(SPAMS).The results showed that the concentrations of five air pollutants including PM2.5,PM1o,SO2,NO2,and cO decreased by 41.2%-71.5%during the pandemic compared to those before the pandemic,whereas O3 increased by 1.3 times during the pandemic because of the depressed titration of O3 and more favorable meteorological conditions.The count and percentage contribution of carbonaceous particles in the total detected particles were lower during the pandemic than those before the pandemic.The carbonaceous particles were dominated by elemental and organic carbon(ECOC,35.9%),followed by elemental carbon-aged(EC-aged,19.6%)and organic carbon-fresh(OC-fresh,13.5%)before the pandemic,while EC-aged(25.3%),ECOC(17.9%),and secondary ions-rich(SEC,17.8%)became the predominant species during the pandemic.The carbonaceous particle sizes during the pandemic showed a broader distribution than that before the pandemic,due to the condensation and coagulation of carbonaceous particles in the aging processes.The relative aerosol acidity(Rra)was smaller before the pandemic than that during the pandemic,indicating the more acidic particle aerosol during the pandemic closely related to the secondary species and relative humidity(RH).More than 95.0%and 86.0%of carbonaceous particles in the whole period were internally mixed with nitrate and sulfate,implying that most of the carbonaceous particles were associated with secondary oxidation during their formation processes.The diurnal variations of oxalate particles and correlation analyses suggested that oxalate particles before the pandemic were derived from aqueous oxidation driven by RH and liquid water content(LwC),while oxalate particles during the pandemic were originated from O3-dominatedphotochemical oxidation.展开更多
大气气溶胶因其对气候和公众健康的影响而成为当今环境研究领域的中心课题.单颗粒分析是目前国际上大气气溶胶研究的一个前沿领域,该方法具有高的时间和空间分辨率,能够提供全颗粒物分析所无法提供的大量信息.利用自主研制的单颗粒气溶...大气气溶胶因其对气候和公众健康的影响而成为当今环境研究领域的中心课题.单颗粒分析是目前国际上大气气溶胶研究的一个前沿领域,该方法具有高的时间和空间分辨率,能够提供全颗粒物分析所无法提供的大量信息.利用自主研制的单颗粒气溶胶质谱仪(single particle aerosol mass spectrometer,SPAMS),对广东鹤山地区气溶胶进行在线分析.重点分析含金属颗粒的相关性、数浓度和可能的来源,并简单介绍该仪器的产业化情况.展开更多
基金financially supported by the Key-Area Research and Development Program of Guangdong Province (No. 2020B1111360001)the National Natural Science Foundation of China (NSFC) (No. 41805093, 41827804)+3 种基金the NSFC of Guangdong Province (No. 2021A1515011206)the National Key Research and Development Program of China (No. 2016YFC0200105)Guangdong Special Support Program (No. 2019BT02Z546, 2019TQ05L169)the Guangdong Enterprise Science and Technology Commissioner Project (No. GDKTP2020035200)
文摘The real-time detection of the mixing states of polycyclic aromatic hydrocarbons(PAHs)and nitro-PAHs in ambient particles is of great significance for analyzing the source,aging process,and health effects of PAHs and nitro-PAHs;yet there is still few effective technology to achieve this type of detection.In this study,11 types of PAH and nitro-PAH standard sampleswere analyzed using a high performance-single particle aerosolmass spectrometer(HP-SPAMS)in lab studies.The identification principles‘parent ions’and‘mass-to-charge(m/z)=77’of each compound were obtained in this study.It was found that different laser energies did not affect the identification of the parent ions.The comparative experiments of ambient atmospheric particles,cooking and biomass burning emitted particles with and without the addition of PAHs were conducted and ruled out the interferences from primary and secondary organics on the identification of PAHs.Besides,the reliability of the characteristic ions extraction method was evaluated through the comparative study of similarity algorithm and deep learning algorithm.In addition,the real PAH-containing particles from vehicle exhaust emissions and ambient particles were also analyzed.This study improves the ability of single particle mass spectrometry technology to detect PAHs and nitro-PAHs,and HP-SPAMS was superior to SPAMS for detecting single particles containing PAHs and nitro-PAHs.This study provides support for subsequent ambient observations to identify the characteristic spectrum of single particles containing PAHs and nitro-PAHs.
文摘An experiment facility has been set up for the study of metal cluster compounds in our laboratory, which consists of a nano-electrospray ionization source, an ion transmission and focus system, and a reflectron time-of-fight mass spectrometer. Taking advantage of the nano-electrospray ionization source, polyvalent ions are usually produced in the ＂ionization＂ process and the obtained mass resolution of the equipment is over 8000. The molecular ion peaks of metal cluster compounds [Au20（PPhpy2）10Cl2]（SbF6）4, where PPhpy2=bis（2- pyridyl）phenylphosphine, and [AuaAg2（C）L6]（BF4）4, where L=2-（diphenylphosphino）-5- methylpyridine, are distinguished in the respective mass spectrum, accompanied by some fragment ion peaks. In addition, the mass-to-charge ratios of the parent ions are determi- nated. Preliminary results suggest that the device is a powerful tool for the study of metal cluster compounds. It turns out that the information obtained by the instrumentation serves as an essential supplement to single crystal X-ray diffraction for structure characterization of metal cluster compounds.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.20937001 and 40875074)Science&Technology Commission of Shanghai Municipality(10JC1402000).
文摘ATSI Model 3800 aerosol time-of-flight mass spectrometer(ATOFMS)was deployed for single-particle analysis in Shanghai during theWorld Exposition(EXPO),2010.Measurements on two extreme cases:polluted day(1st May)and clean day(25th September)were compared to show how meteorological conditions affected the concentration and composition of ambient aerosols.Mass spectra of 90496 and 50407 particles were analyzed respectively during the two sampling periods.The ART-2a neural network algorithm was applied to sort the collected particles.Seven major classes of particles were obtained:dust,sea salt,industrial,biomass burning,organic carbon(OC),elementary carbon(EC),and NH4-rich particles.Number concentration of ambient aerosols showed a strong anti-correlation with the boundary layer height variation.The external mixing states of aerosols were quite different during two sampling periods because of different air parcel trajectories.Number fraction of biomass burning particles(43.3%)during polluted episode was much higher than that(21.6%)of clean time.Air parcels from the East China Sea on clean day diluted local pollutant concentration and increased the portion of sea salt particle dramatically(13.3%).The large contribution of biomass burning particles in both cases might be an indication of a constant regional background of biomass burning emission.Mass spectrum analysis showed that chemical compositions and internal mixing states of almost all the particle types were more complicate during polluted episode compared with those observed in clean time.Strong nitrate signals in the mass spectra suggested that most of the particles collected on polluted day had gone through some aging processes before reaching the sampling site.
基金financially supported by the National Natural Science Foundation of China(Nos.21375129 and 21675155)
文摘It is difficult to rapidly and on-line detect trace volatile organic compounds for miniature massspectrometry due to its limited sampling volume at slow pumping speed. In this paper, we developed anew radiofrequency field enhanced chemical ionization source （RF-ECI） with vacuum ultraviolet （VUV）lamp by coupling radiofrequency electric field and direct-current field together. The experiment resultsshowed that the sensitivity of benzene, toluene, hydrogen sulfide and other compounds increased by 2-3orders of magnitude under the introduction of RF-ECI comparing to traditional single photon ionization（SPI）. At the same time, the reagent ion of O2＋ realized the charge transfer reaction chemical ionization,and the RF-ECI effectively expanded the detection range of the VUV lamp based SPI. The VUV lamp hasinherent advantages in the on-site analytical instrument for its small size and low power consumption,and the VUV lamp based RF-ECI miniature time-of-flight mass spectrometer （TOFMS） has a limit-of-detection for H2S as low as 0.0571 mg/m3, and it is expected to be used widely in the field of on-site rapidanalvsis.
基金supported by the National Natural Science Fund of China(grant number 42177083)Natural Science Foundation of Shandong Province(grant number ZR2020MD113)and Open Funds of State Key Laboratory of Loess and Quaternary Geology,Institute of Earth Environment,Chinese Academy of Sciences(grant number SKLLOG2020).
文摘To investigate the effect of covID-19 control measures on aerosol chemistry,the chemical compositions,mixing states,and formation mechanisms of carbonaceous particles in the urban atmosphere of Liao-cheng in the North China Plain(NCP)were compared before and during the pandemic using a single particle aerosol mass spectrometry(SPAMS).The results showed that the concentrations of five air pollutants including PM2.5,PM1o,SO2,NO2,and cO decreased by 41.2%-71.5%during the pandemic compared to those before the pandemic,whereas O3 increased by 1.3 times during the pandemic because of the depressed titration of O3 and more favorable meteorological conditions.The count and percentage contribution of carbonaceous particles in the total detected particles were lower during the pandemic than those before the pandemic.The carbonaceous particles were dominated by elemental and organic carbon(ECOC,35.9%),followed by elemental carbon-aged(EC-aged,19.6%)and organic carbon-fresh(OC-fresh,13.5%)before the pandemic,while EC-aged(25.3%),ECOC(17.9%),and secondary ions-rich(SEC,17.8%)became the predominant species during the pandemic.The carbonaceous particle sizes during the pandemic showed a broader distribution than that before the pandemic,due to the condensation and coagulation of carbonaceous particles in the aging processes.The relative aerosol acidity(Rra)was smaller before the pandemic than that during the pandemic,indicating the more acidic particle aerosol during the pandemic closely related to the secondary species and relative humidity(RH).More than 95.0%and 86.0%of carbonaceous particles in the whole period were internally mixed with nitrate and sulfate,implying that most of the carbonaceous particles were associated with secondary oxidation during their formation processes.The diurnal variations of oxalate particles and correlation analyses suggested that oxalate particles before the pandemic were derived from aqueous oxidation driven by RH and liquid water content(LwC),while oxalate particles during the pandemic were originated from O3-dominatedphotochemical oxidation.
文摘大气气溶胶因其对气候和公众健康的影响而成为当今环境研究领域的中心课题.单颗粒分析是目前国际上大气气溶胶研究的一个前沿领域,该方法具有高的时间和空间分辨率,能够提供全颗粒物分析所无法提供的大量信息.利用自主研制的单颗粒气溶胶质谱仪(single particle aerosol mass spectrometer,SPAMS),对广东鹤山地区气溶胶进行在线分析.重点分析含金属颗粒的相关性、数浓度和可能的来源,并简单介绍该仪器的产业化情况.
