Due to the non-linearity in ozone(O_(3))formation,reducing the emission of nitrogen oxides(NO_(x))may increase O_(3) concentration.Given the counteractive O_(3) response to NO_(x) reduction,overall impact of air pollu...Due to the non-linearity in ozone(O_(3))formation,reducing the emission of nitrogen oxides(NO_(x))may increase O_(3) concentration.Given the counteractive O_(3) response to NO_(x) reduction,overall impact of air pollution controls can be ambiguous when the assessments focus on the changes in pollutant concentrations.In this study,a risk-based method was used to gauge the net effect of air pollution controls on mortality risk in the Beijing–Tianjin–Hebei(BTH)region during the 2022 Winter Olympics and Paralympics(WOP).This mega-event presents a unique opportunity to investigate the efficacy of deep cuts in pollutant emissions.Results show that O_(3) concentrations greatly increased as nitrogen dioxide(NO_(2))concentrations decreased in the BTH.Due to the active photochemical formations,O_(3) became the dominant pollutant that affected human health during the WOP.Despite the substantial O_(3) increases,the health benefits of NO_(2) reductions overwhelmed the adverse health effects of O_(3) increases in most regions of the BTH(at 81 out of 112 stations).After considering the impacts of particulate matter,the integrated health risk of air pollution mixtures declined almost everywhere in the BTH.Our results underscore the great necessity of changing the assessment paradigm of pollution control from using concentration-based methods to using risk-based methods.Together with the carbon neutrality policy,stringent control of NO_(x)emission from combustion sources is a promising way to achieve synergistic control solutions for air pollution and climate change.展开更多
Considerable efforts have been devoted to characterising the chemical components of vehicle exhaust.However,these components may not accurately reflect the contribution of vehicle exhaust to atmospheric reactivity bec...Considerable efforts have been devoted to characterising the chemical components of vehicle exhaust.However,these components may not accurately reflect the contribution of vehicle exhaust to atmospheric reactivity because of the presence of species not accounted for(“missing species”)given the limitations of analytical instruments.In this study,we improved the laser photolysis–laser-induced fluorescence(LP-LIF)technique and applied it to directly measure the total OH reactivity(TOR)in exhaust gas from light-duty gasoline vehicles in China.The TOR for China Ⅰ to Ⅵ-a vehicles was 15.6,16.3,8.4,2.6,1.5,and 1.6×10^(4) sec^(-1),respectively,reflecting a notable drop as emission standards were upgraded.The TOR was comparable between cold and warm starts.The missing OH reactivity(MOR)values for China Ⅰ to Ⅳ vehicles were close to zero with a cold start but were much higher with a warm start.The variations in oxygenated volatile organic compounds(OVOCs)under different emission standards and for the two start conditions were similar to those of the MOR,indicating that OVOCs and the missing species may have similar production processes.Online measurement revealed that the duration of the stable driving stage was the primary factor leading to the production of OVOCs and missing species.Our findings underscore the importance of direct measurement of TOR from vehicle exhaust and highlight the necessity of adding OVOCs and other organic reactive gases in future upgrades of emission standards,such that the vehicular contribution to atmospheric reactivity can be more effectively controlled.展开更多
Speciated characterization of Volatile Organic Compounds (VOCs),including oxygenated VOCs (OVOCs),from construction machinery and river ships in China is currently lacking.In this regard,we conducted field measurement...Speciated characterization of Volatile Organic Compounds (VOCs),including oxygenated VOCs (OVOCs),from construction machinery and river ships in China is currently lacking.In this regard,we conducted field measurement on speciated VOC (including OVOC) emissions from six construction machinery and five river ships in the Pearl River Delta (PRD) region to identify VOC emission characteristics.We noticed that OVOC emissions from construction machinery and ships accounted for more than 50%of the total VOC emissions,followed by alkenes,aromatics and alkanes.Formaldehyde and acetaldehyde were the most emission species,accounting for 61.8%-83.2%of OVOCs.For construction machinery,the fuel-based emission factors of roller,grader and pile driver were 3.12,3.12 and 7.36 g/kg,respectively.With the rigorous restraint by the national emission standards,VOC emissions of construction machinery had decreased considerably,especially during stageⅢ.Ozone formation potential was also significantly reduced due to the significant decrease in emissions of OVOCs and alkenes with higher reactivity.For river ships,the fuel-based emission factors of cargo ships and speedboat were 1.46 and 0.44 g/kg,respectively.VOC emissions from construction machinery and river ships in Guangdong Province in 2017 were 8851.0 and 4361.0 ton,respectively.This study filled the knowledge gaps of reactive gas emissions from different kinds of non-road mobile sources over the PRD,and more importantly,highlighted the necessity in adding OVOC measurement to give a complete and accurate depiction of reactive gas emissions from non-road mobile sources.展开更多
In the past decade,ozone(O_(3))pollution has been continuously worsening in most developing countries.The accurate identification of the nonlinear relationship between O_(3) and its precursors is a prerequisite for fo...In the past decade,ozone(O_(3))pollution has been continuously worsening in most developing countries.The accurate identification of the nonlinear relationship between O_(3) and its precursors is a prerequisite for formulating effective O_(3) control measures.At present,precursor-based O_(3) isopleth diagrams are widely used to infer O_(3) control strategy at a particular location.However,there is frequently a large gap between the O_(3)-precursor nonlinearity delineated by the O_(3) isopleths and the emission source control measures to reduce O_(3) levels.Consequently,we developed an emission source-based O_(3) isopleth diagram that directly illustrates the O_(3) level changes in response to synergistic control on two types of emission sources using a validated numerical modeling system and the latest regional emission inventory.Isopleths can be further upgraded to isosurfaces when co-control on three types of emission sources is investigated.Using Guangzhou and Foshan as examples,we demonstrate that similar precursor-based O_(3) isopleths can be associated with significantly different emission source co-control strategies.In Guangzhou,controlling solvent use emissions was the most effective approach to reduce peak O_(3) levels.In Foshan,co-control of on-road mobile,solvent use,and fixed combustion sources with a ratio of 3:1:2 or 3:1:3 was best to effectively reduce the peak O_(3) levels below 145 ppbv.This study underscores the importance of using emission source-based O_(3) isopleths and isosurface diagrams to guide a precursor emission control strategy that can effectively reduce the peak O_(3) levels in a particular area.展开更多
Understanding ozone(O_(3))formation regime is a prerequisite in formulating an effective O_(3)pollution control strategy.Photochemical indicator is a simple and direct method in identifying O_(3)formation regimes.Most...Understanding ozone(O_(3))formation regime is a prerequisite in formulating an effective O_(3)pollution control strategy.Photochemical indicator is a simple and direct method in identifying O_(3)formation regimes.Most used indicators are derived from observations,whereas the role of atmospheric oxidation is not in consideration,which is the core driver of O_(3)formation.Thus,it may impact accuracy in signaling O_(3)formation regimes.In this study,an advanced three-dimensional numerical modeling system was used to investigate the relationship between atmospheric oxidation and O_(3)formation regimes during a long-lasting O_(3)exceedance event in September 2017 over the Pearl River Delta(PRD)of China.We discovered a clear relationship between atmospheric oxidative capacity and O_(3)formation regime.Over eastern PRD,O_(3)formation was mainly in a NO x-limited regime when HO_(2)/OH ratio was higher than 11,while in a VOC-limited regime when the ratio was lower than 9.5.Over central and western PRD,an HO_(2)/OH ratio higher than 5 and lower than 2 was indicative of NO x-limited and VOC-limited regime,respectively.Physical contribution,including horizontal transport and vertical transport,may pose uncertainties on the indication of O_(3)formation regime by HO_(2)/OH ratio.In comparison with other commonly used photochemical indicators,HO_(2)/OH ratio had the best performance in differentiating O_(3)formation regimes.This study highlighted the necessities in using an atmospheric oxidative capacity-based indicator to infer O_(3)formation regime,and underscored the importance of characterizing behaviors of radicals to gain insight in atmospheric processes leading to O_(3)pollution over a photochemically active region.展开更多
基金supported by the NSFC/RGC Joint Research Project (Nos.42161160329 and N_HKUST609/21)the Research Grants Council of Hong Kong (Nos.GRF 16202120 and T24/504/17)the Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province (No.2019B121205004)。
文摘Due to the non-linearity in ozone(O_(3))formation,reducing the emission of nitrogen oxides(NO_(x))may increase O_(3) concentration.Given the counteractive O_(3) response to NO_(x) reduction,overall impact of air pollution controls can be ambiguous when the assessments focus on the changes in pollutant concentrations.In this study,a risk-based method was used to gauge the net effect of air pollution controls on mortality risk in the Beijing–Tianjin–Hebei(BTH)region during the 2022 Winter Olympics and Paralympics(WOP).This mega-event presents a unique opportunity to investigate the efficacy of deep cuts in pollutant emissions.Results show that O_(3) concentrations greatly increased as nitrogen dioxide(NO_(2))concentrations decreased in the BTH.Due to the active photochemical formations,O_(3) became the dominant pollutant that affected human health during the WOP.Despite the substantial O_(3) increases,the health benefits of NO_(2) reductions overwhelmed the adverse health effects of O_(3) increases in most regions of the BTH(at 81 out of 112 stations).After considering the impacts of particulate matter,the integrated health risk of air pollution mixtures declined almost everywhere in the BTH.Our results underscore the great necessity of changing the assessment paradigm of pollution control from using concentration-based methods to using risk-based methods.Together with the carbon neutrality policy,stringent control of NO_(x)emission from combustion sources is a promising way to achieve synergistic control solutions for air pollution and climate change.
基金supported by the National Natural Science Foundation of China(Nos.91644221 and 41627809)the National Key Research and Development Program of China(Nos.2016YFC0202201 and 2018YFC0213904)the Key-Area Research and Development Program of Guangdong Province(No.2019B110206001).
文摘Considerable efforts have been devoted to characterising the chemical components of vehicle exhaust.However,these components may not accurately reflect the contribution of vehicle exhaust to atmospheric reactivity because of the presence of species not accounted for(“missing species”)given the limitations of analytical instruments.In this study,we improved the laser photolysis–laser-induced fluorescence(LP-LIF)technique and applied it to directly measure the total OH reactivity(TOR)in exhaust gas from light-duty gasoline vehicles in China.The TOR for China Ⅰ to Ⅵ-a vehicles was 15.6,16.3,8.4,2.6,1.5,and 1.6×10^(4) sec^(-1),respectively,reflecting a notable drop as emission standards were upgraded.The TOR was comparable between cold and warm starts.The missing OH reactivity(MOR)values for China Ⅰ to Ⅳ vehicles were close to zero with a cold start but were much higher with a warm start.The variations in oxygenated volatile organic compounds(OVOCs)under different emission standards and for the two start conditions were similar to those of the MOR,indicating that OVOCs and the missing species may have similar production processes.Online measurement revealed that the duration of the stable driving stage was the primary factor leading to the production of OVOCs and missing species.Our findings underscore the importance of direct measurement of TOR from vehicle exhaust and highlight the necessity of adding OVOCs and other organic reactive gases in future upgrades of emission standards,such that the vehicular contribution to atmospheric reactivity can be more effectively controlled.
基金supported by the National Key Research and Development Program of China (No.2016YFC0202201)the National Natural Science Foundation of China (No.91644221)。
文摘Speciated characterization of Volatile Organic Compounds (VOCs),including oxygenated VOCs (OVOCs),from construction machinery and river ships in China is currently lacking.In this regard,we conducted field measurement on speciated VOC (including OVOC) emissions from six construction machinery and five river ships in the Pearl River Delta (PRD) region to identify VOC emission characteristics.We noticed that OVOC emissions from construction machinery and ships accounted for more than 50%of the total VOC emissions,followed by alkenes,aromatics and alkanes.Formaldehyde and acetaldehyde were the most emission species,accounting for 61.8%-83.2%of OVOCs.For construction machinery,the fuel-based emission factors of roller,grader and pile driver were 3.12,3.12 and 7.36 g/kg,respectively.With the rigorous restraint by the national emission standards,VOC emissions of construction machinery had decreased considerably,especially during stageⅢ.Ozone formation potential was also significantly reduced due to the significant decrease in emissions of OVOCs and alkenes with higher reactivity.For river ships,the fuel-based emission factors of cargo ships and speedboat were 1.46 and 0.44 g/kg,respectively.VOC emissions from construction machinery and river ships in Guangdong Province in 2017 were 8851.0 and 4361.0 ton,respectively.This study filled the knowledge gaps of reactive gas emissions from different kinds of non-road mobile sources over the PRD,and more importantly,highlighted the necessity in adding OVOC measurement to give a complete and accurate depiction of reactive gas emissions from non-road mobile sources.
基金supported by the National Natural Science Foundation of China(No.91644221)the National Key Re-search and Development Program(2016YFC0202201).
文摘In the past decade,ozone(O_(3))pollution has been continuously worsening in most developing countries.The accurate identification of the nonlinear relationship between O_(3) and its precursors is a prerequisite for formulating effective O_(3) control measures.At present,precursor-based O_(3) isopleth diagrams are widely used to infer O_(3) control strategy at a particular location.However,there is frequently a large gap between the O_(3)-precursor nonlinearity delineated by the O_(3) isopleths and the emission source control measures to reduce O_(3) levels.Consequently,we developed an emission source-based O_(3) isopleth diagram that directly illustrates the O_(3) level changes in response to synergistic control on two types of emission sources using a validated numerical modeling system and the latest regional emission inventory.Isopleths can be further upgraded to isosurfaces when co-control on three types of emission sources is investigated.Using Guangzhou and Foshan as examples,we demonstrate that similar precursor-based O_(3) isopleths can be associated with significantly different emission source co-control strategies.In Guangzhou,controlling solvent use emissions was the most effective approach to reduce peak O_(3) levels.In Foshan,co-control of on-road mobile,solvent use,and fixed combustion sources with a ratio of 3:1:2 or 3:1:3 was best to effectively reduce the peak O_(3) levels below 145 ppbv.This study underscores the importance of using emission source-based O_(3) isopleths and isosurface diagrams to guide a precursor emission control strategy that can effectively reduce the peak O_(3) levels in a particular area.
基金sponsored by the National Natural Science Foundation of China(Nos.91644221,41575009)。
文摘Understanding ozone(O_(3))formation regime is a prerequisite in formulating an effective O_(3)pollution control strategy.Photochemical indicator is a simple and direct method in identifying O_(3)formation regimes.Most used indicators are derived from observations,whereas the role of atmospheric oxidation is not in consideration,which is the core driver of O_(3)formation.Thus,it may impact accuracy in signaling O_(3)formation regimes.In this study,an advanced three-dimensional numerical modeling system was used to investigate the relationship between atmospheric oxidation and O_(3)formation regimes during a long-lasting O_(3)exceedance event in September 2017 over the Pearl River Delta(PRD)of China.We discovered a clear relationship between atmospheric oxidative capacity and O_(3)formation regime.Over eastern PRD,O_(3)formation was mainly in a NO x-limited regime when HO_(2)/OH ratio was higher than 11,while in a VOC-limited regime when the ratio was lower than 9.5.Over central and western PRD,an HO_(2)/OH ratio higher than 5 and lower than 2 was indicative of NO x-limited and VOC-limited regime,respectively.Physical contribution,including horizontal transport and vertical transport,may pose uncertainties on the indication of O_(3)formation regime by HO_(2)/OH ratio.In comparison with other commonly used photochemical indicators,HO_(2)/OH ratio had the best performance in differentiating O_(3)formation regimes.This study highlighted the necessities in using an atmospheric oxidative capacity-based indicator to infer O_(3)formation regime,and underscored the importance of characterizing behaviors of radicals to gain insight in atmospheric processes leading to O_(3)pollution over a photochemically active region.