Pub Date : 2018-01-01DOI: 10.1080/16000889.2018.1468704
G. Messori, Dave van Wees, F. Pausata, J. A. Acosta Navarro, A. Hannachi, F. Dentener
Abstract Air quality management is strongly driven by legislative aspects related to the exceedance of air quality limit values. Here, we use the Norwegian Climate Centre’s Earth System Model to assess the impact of a future scenario of maximum feasible aerosol emission abatement and increasing greenhouse gases (RCP4.5) on urban PM2.5 concentrations in Europe. Daily PM2.5 concentrations are assessed using a novel downscaling method which allows us to compute exceedances of current and planned air quality thresholds. For the latter, we assume that future ambitious emission reductions are likely to be accompanied by stricter air quality thresholds. The changes in PM2.5 concentrations are discussed in the context of the large-scale atmospheric changes observed relative to the present-day climate. Our results show a more positive North Atlantic Oscillation mean state in the future, combined with a large eastward shift of both North Atlantic sea-level pressure centres of action. This is associated with more frequent mid-latitude blocking and a northward shift of the jet stream. These changes favour higher than expected anthropogenic urban PM2.5 concentrations in Southern Europe, while they have the opposite effect on the northern half of the continent. In the future scenario, PM concentrations in substantial parts of Southern Europe are found to exceed the World Health Organisation Air Quality Guideline daily limit of 25 μg/m3 on 25 to over 50 days per year, and annual guidelines of 10 µg/m3 on more than 80% of the 30 years analysed in our study. We conclude that alterations in atmospheric circulation in the future, induced by stringent maximum feasible air pollution mitigation as well as GHG emissions, will negatively influence the effectiveness of these emission abatements over large parts of Europe. This has important implications for future air quality policies.
{"title":"The impact of future atmospheric circulation changes over the Euro-Atlantic sector on urban PM2.5 concentrations","authors":"G. Messori, Dave van Wees, F. Pausata, J. A. Acosta Navarro, A. Hannachi, F. Dentener","doi":"10.1080/16000889.2018.1468704","DOIUrl":"https://doi.org/10.1080/16000889.2018.1468704","url":null,"abstract":"Abstract Air quality management is strongly driven by legislative aspects related to the exceedance of air quality limit values. Here, we use the Norwegian Climate Centre’s Earth System Model to assess the impact of a future scenario of maximum feasible aerosol emission abatement and increasing greenhouse gases (RCP4.5) on urban PM2.5 concentrations in Europe. Daily PM2.5 concentrations are assessed using a novel downscaling method which allows us to compute exceedances of current and planned air quality thresholds. For the latter, we assume that future ambitious emission reductions are likely to be accompanied by stricter air quality thresholds. The changes in PM2.5 concentrations are discussed in the context of the large-scale atmospheric changes observed relative to the present-day climate. Our results show a more positive North Atlantic Oscillation mean state in the future, combined with a large eastward shift of both North Atlantic sea-level pressure centres of action. This is associated with more frequent mid-latitude blocking and a northward shift of the jet stream. These changes favour higher than expected anthropogenic urban PM2.5 concentrations in Southern Europe, while they have the opposite effect on the northern half of the continent. In the future scenario, PM concentrations in substantial parts of Southern Europe are found to exceed the World Health Organisation Air Quality Guideline daily limit of 25 μg/m3 on 25 to over 50 days per year, and annual guidelines of 10 µg/m3 on more than 80% of the 30 years analysed in our study. We conclude that alterations in atmospheric circulation in the future, induced by stringent maximum feasible air pollution mitigation as well as GHG emissions, will negatively influence the effectiveness of these emission abatements over large parts of Europe. This has important implications for future air quality policies.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"70 1","pages":"1 - 22"},"PeriodicalIF":0.0,"publicationDate":"2018-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"87112309","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2018-01-01DOI: 10.1080/16000889.2018.1468705
H. Niu, Shi-chang Kang, Xixi Lu, Xiaofei Shi
Abstract Water-soluble organic carbon (WSOC) widely stored in glaciers from local and distant sources, and then released it to downstream environments under a warming climate. Climatic driven changes to glacial run-off are larger and represent an important flux of organic carbon. However, very few WSOC data are currently available to fully characterize WSOC variation in the temperate glacierized regions of the Tibetan Plateau (TP). This study first systematically evaluated the concentration characteristics and light absorbing property of WSOC, and insoluble particulate carbon (IPC) in snow and ice of a typical temperate glacier on Mt. Yulong. Average concentrations of WSOC were 0.61 ± 0.21 mg L−1 in Baishui glacier on Mt. Yulong. WSOC concentrations in surface aged snow were dramatically decreased with the time extension during the entire monsoon season due to extensive glacial melting and scavenging effects by meltwater. The MAC values of WSOC calculated at 365 nm was 6.31 ± 0.34 m2 g−1 on Mt. Yulong, and there exists distinct spectral dependence of MACwsoc within the wavelength range (260 – 700 nm). The low AAE330–400 values suggest the light absorption of WSOC is more spectrally neutral. The flux of WSOC in Baishui glacier was 0.99 gC m−2 yr−1, while the IPC flux was 4.77 gC m−2 yr−1. Total WSOC storage in the Baishui glacier was estimated to be 1.5 tone C and total IPC storage was 7.25 tone C (1 tone = 106 g). Moreover, glacial melting was reinforced by the soluble and insoluble light absorbing impurities (ILAIs) in glaciers, Baishui glacier can be considered as a fraction of carbon source under the scenario of a warming climate, more importantly, WSOC in snow and ice needs to be taken into account in calculating the radiative forcing of ILAIs and accelerating glacial melting.
在气候变暖的背景下,水溶性有机碳(WSOC)广泛储存在冰川中,并向下游环境释放。气候驱动的冰川径流变化更大,代表了有机碳的重要通量。然而,目前能够全面表征青藏高原温带冰川区WSOC变化特征的WSOC数据很少。本研究首次系统评价了玉龙山典型温带冰川冰雪中WSOC和不溶性颗粒碳(IPC)的浓度特征和吸光特性。玉龙山白水冰川WSOC平均浓度为0.61±0.21 mg L−1。在整个季风季节,由于广泛的冰川融化和融水的清除作用,地表陈年雪中WSOC浓度随着时间的延长而显著降低。在365 nm处,玉龙山WSOC的MAC值为6.31±0.34 m2 g−1,在260 ~ 700 nm波长范围内,MACwsoc存在明显的光谱依赖性。较低的AAE330-400值表明WSOC的光吸收光谱更为中性。白水冰川WSOC通量为0.99 gC m−2 yr−1,IPC通量为4.77 gC m−2 yr−1。白水冰川WSOC总储存量为1.5 tone C, IPC总储存量为7.25 tone C (1 tone = 106 g)。此外,冰川中可溶性和不溶性光吸收杂质(ILAIs)加强了冰川融化,白水冰川可以作为气候变暖情景下的一部分碳源,更重要的是,在计算ILAIs的辐射强迫和加速冰川融化时,需要考虑冰雪中的WSOC。
{"title":"Distributions and light absorption property of water soluble organic carbon in a typical temperate glacier, southeastern Tibetan Plateau","authors":"H. Niu, Shi-chang Kang, Xixi Lu, Xiaofei Shi","doi":"10.1080/16000889.2018.1468705","DOIUrl":"https://doi.org/10.1080/16000889.2018.1468705","url":null,"abstract":"Abstract Water-soluble organic carbon (WSOC) widely stored in glaciers from local and distant sources, and then released it to downstream environments under a warming climate. Climatic driven changes to glacial run-off are larger and represent an important flux of organic carbon. However, very few WSOC data are currently available to fully characterize WSOC variation in the temperate glacierized regions of the Tibetan Plateau (TP). This study first systematically evaluated the concentration characteristics and light absorbing property of WSOC, and insoluble particulate carbon (IPC) in snow and ice of a typical temperate glacier on Mt. Yulong. Average concentrations of WSOC were 0.61 ± 0.21 mg L−1 in Baishui glacier on Mt. Yulong. WSOC concentrations in surface aged snow were dramatically decreased with the time extension during the entire monsoon season due to extensive glacial melting and scavenging effects by meltwater. The MAC values of WSOC calculated at 365 nm was 6.31 ± 0.34 m2 g−1 on Mt. Yulong, and there exists distinct spectral dependence of MACwsoc within the wavelength range (260 – 700 nm). The low AAE330–400 values suggest the light absorption of WSOC is more spectrally neutral. The flux of WSOC in Baishui glacier was 0.99 gC m−2 yr−1, while the IPC flux was 4.77 gC m−2 yr−1. Total WSOC storage in the Baishui glacier was estimated to be 1.5 tone C and total IPC storage was 7.25 tone C (1 tone = 106 g). Moreover, glacial melting was reinforced by the soluble and insoluble light absorbing impurities (ILAIs) in glaciers, Baishui glacier can be considered as a fraction of carbon source under the scenario of a warming climate, more importantly, WSOC in snow and ice needs to be taken into account in calculating the radiative forcing of ILAIs and accelerating glacial melting.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"60 1","pages":"1 - 15"},"PeriodicalIF":0.0,"publicationDate":"2018-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"74943110","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2017-01-01DOI: 10.1080/16000889.2017.1347484
Zhouxiang Zhang, Xiaoye Zhang, Yangmei Zhang, Yaqiang Wang, Huai-gang Zhou, X. Shen, H. Che, Junying Sun, Luyuan Zhang
Abstract Heavy aerosol pollution episodes (HPEs) usually start from late autumn and become more serious in winter in Beijing and its vicinity (BIV). In this study, we examine the reasons for the formation and change of HPEs in the areas of northern BIV. The size-resolved chemical components of PM1 and meteorological conditions were investigated during HPEs in autumn and winter of 2015. Stable regional atmosphere and higher atmospheric condensation processes associated with southerly and lower speed wind led to the formation of HPEs. After the start of these HPEs, the concentration of fine particles increased more than twice in several hours. ~80% of the ‘explosive’ growth in PM mass can be considered as a positive feedback of meteorological factors that come from even more stable atmosphere and larger condensation rate of water vapour, which was derived from the interaction between formed aerosol pollution and the meteorological factors within boundary layer. Nitrate was the largest fraction of PM1 in autumn, and the most significantly increased component during HPEs relative to clean period during both of autumn and winter. The proportion of organic aerosol (OA) was similar to that of nitrate in autumn, but its rise in HPE was much smaller, mainly because of the high concentration of OA existed during clean periods. Compared with the largest increase of nitrate, the similar uplift was found for ammonium production, showing that a large amount of ammonium was mainly formed by the combination of in HPEs, rather than . In addition to the lower southerly wind carrying pollutants from southern part of BIV, westerly wind from central Inner Mongolia and north Shanxi can also bring air pollutants originating from coal combustion, contributing to the heavy pollution in the northern BIV area in winter, and resulting in higher sulphate, nitrate and OA masses.
{"title":"Characteristics of chemical composition and role of meteorological factors during heavy aerosol pollution episodes in northern Beijing area in autumn and winter of 2015","authors":"Zhouxiang Zhang, Xiaoye Zhang, Yangmei Zhang, Yaqiang Wang, Huai-gang Zhou, X. Shen, H. Che, Junying Sun, Luyuan Zhang","doi":"10.1080/16000889.2017.1347484","DOIUrl":"https://doi.org/10.1080/16000889.2017.1347484","url":null,"abstract":"Abstract Heavy aerosol pollution episodes (HPEs) usually start from late autumn and become more serious in winter in Beijing and its vicinity (BIV). In this study, we examine the reasons for the formation and change of HPEs in the areas of northern BIV. The size-resolved chemical components of PM1 and meteorological conditions were investigated during HPEs in autumn and winter of 2015. Stable regional atmosphere and higher atmospheric condensation processes associated with southerly and lower speed wind led to the formation of HPEs. After the start of these HPEs, the concentration of fine particles increased more than twice in several hours. ~80% of the ‘explosive’ growth in PM mass can be considered as a positive feedback of meteorological factors that come from even more stable atmosphere and larger condensation rate of water vapour, which was derived from the interaction between formed aerosol pollution and the meteorological factors within boundary layer. Nitrate was the largest fraction of PM1 in autumn, and the most significantly increased component during HPEs relative to clean period during both of autumn and winter. The proportion of organic aerosol (OA) was similar to that of nitrate in autumn, but its rise in HPE was much smaller, mainly because of the high concentration of OA existed during clean periods. Compared with the largest increase of nitrate, the similar uplift was found for ammonium production, showing that a large amount of ammonium was mainly formed by the combination of in HPEs, rather than . In addition to the lower southerly wind carrying pollutants from southern part of BIV, westerly wind from central Inner Mongolia and north Shanxi can also bring air pollutants originating from coal combustion, contributing to the heavy pollution in the northern BIV area in winter, and resulting in higher sulphate, nitrate and OA masses.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"44 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"74061237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2017-01-01DOI: 10.1080/16000889.2017.1299672
Yan-Li Wang, Xue‐Yan Liu, Wei Song, Wen Yang, B. Han, Xiaoyan Dou, Xu-Dong Zhao, Zhaoliang Song, Cong‐Qiang Liu, Z. Bai
Abstract Nitrogen isotope (δ15N) has been employed to differentiate major sources of atmospheric N. However, it remains a challenge to quantify contributions of multiple sources based on δ15N values of the N mixture in atmospheric samples. This study measured δ15N of bulk N in PM2.5 at an urban site of Beijing during a severe haze episode of 22–30 January 2013 and a background site of Qinghai, north-western China from 6 September to 15 October 2013, then applied a Bayesian isotope mixing model (SIAR, Stable Isotope Analysis in R) to analyse the N sources. At Beijing site, δ15N values of PM2.5 (−4.1‰ to +13.5‰, +2.8 ± 6.4‰) were distributed within the range of major anthropogenic sources (including NH3 and NO2 from coal combustion, vehicle exhausts and domestic wastes/sewage). At Menyuan site, δ15N values of PM2.5 (+8.0‰ to +27.9‰, +18.5 ± 5.8‰) were significantly higher than that of potential sources (including NH3 and NO2 from biomass burning, animal wastes, soil N cycle, fertilizer application and dust N). High molar ratios of to and/or in PM2.5 at the background site suggested that the equilibrium of NH3 ↔ caused apparent 15N enrichments in ammonium. Results of the SIAR model showed that 39 and 32% of bulk N in PM2.5 of Beijing site were contributed from N emissions of coal combustion and vehicle exhausts, respectively, whereas N in PM2.5 at Menyuan site was derived mainly from N emissions of biomass burning (46%) and NH3 volatilization (34%). These results revealed that the stoichiometry between NH3 and acidic gases plays an important role in controlling the bulk δ15N signatures of PM2.5 and emissions of reactive N from coal combustion and urban transportation should be strictly controlled to advert the risk of haze episodes in Beijing.
氮同位素(δ15N)已被用于区分大气氮的主要来源,然而,基于大气样品中氮混合物的δ15N值来量化多种来源的贡献仍然是一个挑战。本研究测量了2013年1月22日至30日北京城市站点和2013年9月6日至10月15日中国西北青海省背景站点PM2.5中体氮的δ15N,然后应用贝叶斯同位素混合模型(SIAR, Stable isotope Analysis in R)分析了N源。北京站点PM2.5的δ15N值(−4.1‰~ +13.5‰,+2.8±6.4‰)分布在主要人为源(燃煤NH3和NO2、机动车尾气和生活垃圾/污水)范围内。在门源站点,PM2.5的δ15N值(+8.0‰~ +27.9‰,+18.5±5.8‰)显著高于潜在源(包括生物质燃烧产生的NH3和NO2、动物粪便、土壤N循环、施肥和粉尘N)。背景站点PM2.5中to和/或的高摩尔比表明NH3的平衡导致铵态氮明显富集。SIAR模型结果显示,北京站点PM2.5中散氮的39%和32%分别来自燃煤和机动车尾气的N排放,而门源站点PM2.5中的N主要来自生物质燃烧的N排放(46%)和NH3挥发(34%)。结果表明,NH3与酸性气体之间的化学计量在控制PM2.5的体δ15N特征中起重要作用,应严格控制燃煤和城市交通中活性N的排放,以降低北京雾霾的发生风险。
{"title":"Source appointment of nitrogen in PM2.5 based on bulk δ15N signatures and a Bayesian isotope mixing model","authors":"Yan-Li Wang, Xue‐Yan Liu, Wei Song, Wen Yang, B. Han, Xiaoyan Dou, Xu-Dong Zhao, Zhaoliang Song, Cong‐Qiang Liu, Z. Bai","doi":"10.1080/16000889.2017.1299672","DOIUrl":"https://doi.org/10.1080/16000889.2017.1299672","url":null,"abstract":"Abstract Nitrogen isotope (δ15N) has been employed to differentiate major sources of atmospheric N. However, it remains a challenge to quantify contributions of multiple sources based on δ15N values of the N mixture in atmospheric samples. This study measured δ15N of bulk N in PM2.5 at an urban site of Beijing during a severe haze episode of 22–30 January 2013 and a background site of Qinghai, north-western China from 6 September to 15 October 2013, then applied a Bayesian isotope mixing model (SIAR, Stable Isotope Analysis in R) to analyse the N sources. At Beijing site, δ15N values of PM2.5 (−4.1‰ to +13.5‰, +2.8 ± 6.4‰) were distributed within the range of major anthropogenic sources (including NH3 and NO2 from coal combustion, vehicle exhausts and domestic wastes/sewage). At Menyuan site, δ15N values of PM2.5 (+8.0‰ to +27.9‰, +18.5 ± 5.8‰) were significantly higher than that of potential sources (including NH3 and NO2 from biomass burning, animal wastes, soil N cycle, fertilizer application and dust N). High molar ratios of to and/or in PM2.5 at the background site suggested that the equilibrium of NH3 ↔ caused apparent 15N enrichments in ammonium. Results of the SIAR model showed that 39 and 32% of bulk N in PM2.5 of Beijing site were contributed from N emissions of coal combustion and vehicle exhausts, respectively, whereas N in PM2.5 at Menyuan site was derived mainly from N emissions of biomass burning (46%) and NH3 volatilization (34%). These results revealed that the stoichiometry between NH3 and acidic gases plays an important role in controlling the bulk δ15N signatures of PM2.5 and emissions of reactive N from coal combustion and urban transportation should be strictly controlled to advert the risk of haze episodes in Beijing.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"27 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"80428373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2017-01-01DOI: 10.1080/16000889.2017.1325723
Yilong Wang, G. Broquet, P. Ciais, F. Chevallier, F. Vogel, N. Kadygrov, Lin Wu, Yi Yin, Rong Wang, S. Tao
Abstract National annual inventories of CO2 emitted during fossil fuel consumption (FFCO2) bear 5–10% uncertainties for developed countries, and are likely higher at intra annual scales or for developing countries. Given the current international efforts of mitigating actions, there is a need for independent verifications of these inventories. Atmospheric inversion assimilating atmospheric gradients of CO2 and radiocarbon measurements could provide an independent way of monitoring FFCO2 emissions. A strategy would be to deploy such measurements over continental scale networks and to conduct continental to global scale atmospheric inversions targeting the national and one-month scale budgets of the emissions. Uncertainties in the high-resolution distribution of the emissions could limit the skill for such a large-scale inversion framework. This study assesses the impact of such uncertainties on the potential for monitoring the emissions at large scale. In practice, it is more specifically dedicated to the derivation, typical quantification and analysis of critical sources of errors that affect the inversion of FFCO2 emissions when solving for them at a relatively coarse resolution with a coarse grid transport model. These errors include those due to the mismatch between the resolution of the transport model and the spatial variability of the actual fluxes and concentrations (i.e. the representation errors) and those due to the uncertainties in the spatial and temporal distribution of emissions at the transport model resolution when solving for the emissions at large scale (i.e. the aggregation errors). We show that the aggregation errors characterize the impact of the corresponding uncertainties on the potential for monitoring the emissions at large scale, even if solving for them at the transport model resolution. We propose a practical method to quantify these sources of errors, and compare them with the precision of FFCO2 measurements (i.e. the measurement errors) and the errors in the modelling of atmospheric transport (i.e. the transport errors). The results show that both the representation and measurement errors can be much larger than the aggregation errors. The magnitude of representation and aggregation errors is sensitive to sampling heights and temporal sampling integration time. The combination of these errors can reach up to about 50% of the typical signals, i.e. the atmospheric large-scale mean afternoon FFCO2 gradients between sites being assimilated by the inversion system. These errors have large temporal auto-correlation scales, but short spatial correlation scales. This indicates the need for accounting for these temporal auto-correlations in the atmospheric inversions and the need for dense networks to limit the impact of these errors on the inversion of FFCO2 emissions at large scale. More generally, comparisons of the representation and aggregation errors to the errors in simulated FFCO2 gradients due to uncertainties in cur
{"title":"Estimation of observation errors for large-scale atmospheric inversion of CO2 emissions from fossil fuel combustion","authors":"Yilong Wang, G. Broquet, P. Ciais, F. Chevallier, F. Vogel, N. Kadygrov, Lin Wu, Yi Yin, Rong Wang, S. Tao","doi":"10.1080/16000889.2017.1325723","DOIUrl":"https://doi.org/10.1080/16000889.2017.1325723","url":null,"abstract":"Abstract National annual inventories of CO2 emitted during fossil fuel consumption (FFCO2) bear 5–10% uncertainties for developed countries, and are likely higher at intra annual scales or for developing countries. Given the current international efforts of mitigating actions, there is a need for independent verifications of these inventories. Atmospheric inversion assimilating atmospheric gradients of CO2 and radiocarbon measurements could provide an independent way of monitoring FFCO2 emissions. A strategy would be to deploy such measurements over continental scale networks and to conduct continental to global scale atmospheric inversions targeting the national and one-month scale budgets of the emissions. Uncertainties in the high-resolution distribution of the emissions could limit the skill for such a large-scale inversion framework. This study assesses the impact of such uncertainties on the potential for monitoring the emissions at large scale. In practice, it is more specifically dedicated to the derivation, typical quantification and analysis of critical sources of errors that affect the inversion of FFCO2 emissions when solving for them at a relatively coarse resolution with a coarse grid transport model. These errors include those due to the mismatch between the resolution of the transport model and the spatial variability of the actual fluxes and concentrations (i.e. the representation errors) and those due to the uncertainties in the spatial and temporal distribution of emissions at the transport model resolution when solving for the emissions at large scale (i.e. the aggregation errors). We show that the aggregation errors characterize the impact of the corresponding uncertainties on the potential for monitoring the emissions at large scale, even if solving for them at the transport model resolution. We propose a practical method to quantify these sources of errors, and compare them with the precision of FFCO2 measurements (i.e. the measurement errors) and the errors in the modelling of atmospheric transport (i.e. the transport errors). The results show that both the representation and measurement errors can be much larger than the aggregation errors. The magnitude of representation and aggregation errors is sensitive to sampling heights and temporal sampling integration time. The combination of these errors can reach up to about 50% of the typical signals, i.e. the atmospheric large-scale mean afternoon FFCO2 gradients between sites being assimilated by the inversion system. These errors have large temporal auto-correlation scales, but short spatial correlation scales. This indicates the need for accounting for these temporal auto-correlations in the atmospheric inversions and the need for dense networks to limit the impact of these errors on the inversion of FFCO2 emissions at large scale. More generally, comparisons of the representation and aggregation errors to the errors in simulated FFCO2 gradients due to uncertainties in cur","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"63 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"86078563","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2017-01-01DOI: 10.1080/16000889.2017.1303228
Zirui Liu, B. Hu, Junke Zhang, J. Xin, Fang-kun Wu, Wenkang Gao, Mingxing Wang, Yuesi Wang
Abstract To study the impacts of emission controls on aerosol physical and chemical properties, real-time measurements of size-resolved aerosol number concentration and chemical composition were conducted in urban Beijing during the 2014 Asia-Pacific Economic Cooperation (APEC) summit, in a period that a series of measures, for example shutting down or halting production from factories and power plants, and restricting the number of vehicles on the roads were implemented in Beijing and surrounding regions. Significantly, reductions in particle mass concentration (55% for PM2.5 and 48% for PM10) were observed during the APEC summit. A clear decrease in secondary inorganic aerosols (SIA), such as sulphate, nitrate and ammonium, was found during APEC, with the reduction ranged from 65.7 to 72.2% for PM1, in which sulphate showed the largest decrease compared with periods before APEC. As a comparison, organics showed a much smaller decrease of 44.3% for PM1 during APEC. These changes were mainly caused by large reductions in accumulation mode particles, which decreased by 36% compared with 19% for Aitken mode particles. The results from the positive matrix factorization (PMF) of particle number concentration indicate that regionally transported aerosols showed significant decreases (70%), similar to those of SIA during APEC, whereas primary factors from traffic and local combustion sources presented much smaller decreases, with the reduction ranged from 4 to 40%. The elevated contributions of these sources indicated the presence of strong local source emissions. The changes in particle chemical composition, size distribution and sources during the evolution of pollution episodes with and without emission controls are further illustrated. Our results highlight the importance of regional atmospheric transport in the formation of severe pollution episodes in Beijing, indicating that reducing the precursors of secondary aerosol over regional scales represent the key steps to reduce the urban particulate pollution. However, stricter emission controls on local source emissions are needed to further mitigate air pollution in Beijing.
{"title":"Characterization of fine particles during the 2014 Asia-Pacific economic cooperation summit: Number concentration, size distribution and sources","authors":"Zirui Liu, B. Hu, Junke Zhang, J. Xin, Fang-kun Wu, Wenkang Gao, Mingxing Wang, Yuesi Wang","doi":"10.1080/16000889.2017.1303228","DOIUrl":"https://doi.org/10.1080/16000889.2017.1303228","url":null,"abstract":"Abstract To study the impacts of emission controls on aerosol physical and chemical properties, real-time measurements of size-resolved aerosol number concentration and chemical composition were conducted in urban Beijing during the 2014 Asia-Pacific Economic Cooperation (APEC) summit, in a period that a series of measures, for example shutting down or halting production from factories and power plants, and restricting the number of vehicles on the roads were implemented in Beijing and surrounding regions. Significantly, reductions in particle mass concentration (55% for PM2.5 and 48% for PM10) were observed during the APEC summit. A clear decrease in secondary inorganic aerosols (SIA), such as sulphate, nitrate and ammonium, was found during APEC, with the reduction ranged from 65.7 to 72.2% for PM1, in which sulphate showed the largest decrease compared with periods before APEC. As a comparison, organics showed a much smaller decrease of 44.3% for PM1 during APEC. These changes were mainly caused by large reductions in accumulation mode particles, which decreased by 36% compared with 19% for Aitken mode particles. The results from the positive matrix factorization (PMF) of particle number concentration indicate that regionally transported aerosols showed significant decreases (70%), similar to those of SIA during APEC, whereas primary factors from traffic and local combustion sources presented much smaller decreases, with the reduction ranged from 4 to 40%. The elevated contributions of these sources indicated the presence of strong local source emissions. The changes in particle chemical composition, size distribution and sources during the evolution of pollution episodes with and without emission controls are further illustrated. Our results highlight the importance of regional atmospheric transport in the formation of severe pollution episodes in Beijing, indicating that reducing the precursors of secondary aerosol over regional scales represent the key steps to reduce the urban particulate pollution. However, stricter emission controls on local source emissions are needed to further mitigate air pollution in Beijing.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"48 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"73552145","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2017-01-01DOI: 10.1080/16000889.2017.1339548
Mengmeng Li, Tijian Wang, M. Xie, B. Zhuang, Shu Li, Yong Han, Pu-long Chen
Abstract Severe haze events and their radiation feedbacks exert a profound impact on the weather and tropospheric chemistry. Using the on-line-coupled Weather Research and Forecasting with Chemistry (WRF-Chem) model, this study investigates the impacts of direct aerosol-radiation feedbacks on local air quality (i.e. particulate matter and ozone photochemistry) during a severe autumn haze episode in Nanjing megacity, eastern China. Pronounced radiation feedbacks are found for the predictions of meteorological and chemical variables. In response to the negative radiative forcing of scattering-dominant anthropogenic haze aerosols, the instantaneous irradiance and temperature at the surface lower by 130 W m−2 and 1.1–1.4 °C, respectively, leading to a reduction of boundary layer height by 103.2–232.6 m (11–38%) and vertical wind speed by 0.1–0.8 mm s−1 (2–30% at mid-day) during this haze event. Such a stable atmosphere favours the accumulation of fine particles (30.5 μg m−3, 28.7%) and NO2 (6.0 ppb, 23.7%) in the urban pollution plume. The weaker turbulent mixing and photochemical activity associated with the enhanced titration loss, and reduced downward radiation and photolysis rate result in a 0.1−5.0 ppb (12.0%) reduction of near-surface ozone. The simulations highlight that the aerosol-radiation feedbacks play an important role in the atmospheric transport and chemistry of large urban pollution plumes.
{"title":"Impacts of aerosol-radiation feedback on local air quality during a severe haze episode in Nanjing megacity, eastern China","authors":"Mengmeng Li, Tijian Wang, M. Xie, B. Zhuang, Shu Li, Yong Han, Pu-long Chen","doi":"10.1080/16000889.2017.1339548","DOIUrl":"https://doi.org/10.1080/16000889.2017.1339548","url":null,"abstract":"Abstract Severe haze events and their radiation feedbacks exert a profound impact on the weather and tropospheric chemistry. Using the on-line-coupled Weather Research and Forecasting with Chemistry (WRF-Chem) model, this study investigates the impacts of direct aerosol-radiation feedbacks on local air quality (i.e. particulate matter and ozone photochemistry) during a severe autumn haze episode in Nanjing megacity, eastern China. Pronounced radiation feedbacks are found for the predictions of meteorological and chemical variables. In response to the negative radiative forcing of scattering-dominant anthropogenic haze aerosols, the instantaneous irradiance and temperature at the surface lower by 130 W m−2 and 1.1–1.4 °C, respectively, leading to a reduction of boundary layer height by 103.2–232.6 m (11–38%) and vertical wind speed by 0.1–0.8 mm s−1 (2–30% at mid-day) during this haze event. Such a stable atmosphere favours the accumulation of fine particles (30.5 μg m−3, 28.7%) and NO2 (6.0 ppb, 23.7%) in the urban pollution plume. The weaker turbulent mixing and photochemical activity associated with the enhanced titration loss, and reduced downward radiation and photolysis rate result in a 0.1−5.0 ppb (12.0%) reduction of near-surface ozone. The simulations highlight that the aerosol-radiation feedbacks play an important role in the atmospheric transport and chemistry of large urban pollution plumes.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"43 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"83590327","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2017-01-01DOI: 10.1080/16000889.2017.1331102
J. Engström, C. Leck
Abstract Filter-based optical measurements of black carbon in air, a constituent of soot, have been determined with a 528 nm light source during the period from 1 June 2005 to 31 May 2009 on samples taken at Godavari in Nepal, Sinhagad in India and Hanimaadhoo in the Maldives. In order to reduce systematic errors due to the light scattering of non-absorbing particles co-deposited on the filter, such as inorganic salts and mineral dust, an additional sensor recording backscattered light was implemented. Two protocols of corrections (optical and chemical) were applied to the samples collected at the observatories. The Indian monsoon circulation with its two annual phases in combination with the location of the combustion sources and their contribution relative to other non-anthropogenic sources dominated the observed patterns of black carbon at two of the observatories: in India and the Maldives. The observatory in Nepal was however mainly influenced by combustion sources all year around concealing possible variability related to the monsoon circulation. At the receptor observatory in the Maldives, peak values in the black carbon absorption coefficient occurred during the winter season (December to April) when air was transported from the polluted Indian subcontinent out over the Indian Ocean. A close to two orders of magnitude lower values were recorded in air that had spent more than 10-days over the Indian Ocean during the monsoon season (July to September), suggested to be dominated by particulate matter from remote marine biogenic sources and not by combustion sources.
{"title":"Seasonal variability in atmospheric black carbon at three stations in South-Asia","authors":"J. Engström, C. Leck","doi":"10.1080/16000889.2017.1331102","DOIUrl":"https://doi.org/10.1080/16000889.2017.1331102","url":null,"abstract":"Abstract Filter-based optical measurements of black carbon in air, a constituent of soot, have been determined with a 528 nm light source during the period from 1 June 2005 to 31 May 2009 on samples taken at Godavari in Nepal, Sinhagad in India and Hanimaadhoo in the Maldives. In order to reduce systematic errors due to the light scattering of non-absorbing particles co-deposited on the filter, such as inorganic salts and mineral dust, an additional sensor recording backscattered light was implemented. Two protocols of corrections (optical and chemical) were applied to the samples collected at the observatories. The Indian monsoon circulation with its two annual phases in combination with the location of the combustion sources and their contribution relative to other non-anthropogenic sources dominated the observed patterns of black carbon at two of the observatories: in India and the Maldives. The observatory in Nepal was however mainly influenced by combustion sources all year around concealing possible variability related to the monsoon circulation. At the receptor observatory in the Maldives, peak values in the black carbon absorption coefficient occurred during the winter season (December to April) when air was transported from the polluted Indian subcontinent out over the Indian Ocean. A close to two orders of magnitude lower values were recorded in air that had spent more than 10-days over the Indian Ocean during the monsoon season (July to September), suggested to be dominated by particulate matter from remote marine biogenic sources and not by combustion sources.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"32 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89465374","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2017-01-01DOI: 10.1080/16000889.2017.1361757
M. Mohr, T. Laemmel, M. Maier, D. Schindler
Abstract Small air pressure fluctuations in the atmosphere are responsible for the pressure pumping effect, which leads to an enhancement of soil gas transport. To investigate the spatial variability of these air pressure fluctuations, several high-precision differential pressure sensors were installed at the floor of a Scots pine forest. The alignment of the pressure sensors allowed for the determination of the propagation direction and speed of the observed air pressure fluctuations. Below-canopy and above-canopy airflow characteristics were monitored to find possible links between the air pressure fluctuations and the airflow. Results show that the propagation direction of the air pressure fluctuations observed at the forest floor correspond to the above-canopy and not to the below-canopy wind direction. Moreover, propagation speed of the air pressure fluctuations is higher than the below-canopy wind speed and corresponds to above-canopy wind speed. These findings indicate a connection between below-canopy air pressure fluctuations and above-canopy airflow. The air pressure fluctuations were found to be well correlated up to a distance of 15 m. With increasing distance, the correlation strongly decreases. However, the calculated pressure pumping coefficient, which quantifies the strength of the pressure pumping effect, yields similar values up to a distance of 90 m. This allowed specifying the range of influence of the air pressure fluctuations.
{"title":"Spatial variability of wind-induced air pressure fluctuations responsible for pressure pumping","authors":"M. Mohr, T. Laemmel, M. Maier, D. Schindler","doi":"10.1080/16000889.2017.1361757","DOIUrl":"https://doi.org/10.1080/16000889.2017.1361757","url":null,"abstract":"Abstract Small air pressure fluctuations in the atmosphere are responsible for the pressure pumping effect, which leads to an enhancement of soil gas transport. To investigate the spatial variability of these air pressure fluctuations, several high-precision differential pressure sensors were installed at the floor of a Scots pine forest. The alignment of the pressure sensors allowed for the determination of the propagation direction and speed of the observed air pressure fluctuations. Below-canopy and above-canopy airflow characteristics were monitored to find possible links between the air pressure fluctuations and the airflow. Results show that the propagation direction of the air pressure fluctuations observed at the forest floor correspond to the above-canopy and not to the below-canopy wind direction. Moreover, propagation speed of the air pressure fluctuations is higher than the below-canopy wind speed and corresponds to above-canopy wind speed. These findings indicate a connection between below-canopy air pressure fluctuations and above-canopy airflow. The air pressure fluctuations were found to be well correlated up to a distance of 15 m. With increasing distance, the correlation strongly decreases. However, the calculated pressure pumping coefficient, which quantifies the strength of the pressure pumping effect, yields similar values up to a distance of 90 m. This allowed specifying the range of influence of the air pressure fluctuations.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"30 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89964062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2017-01-01DOI: 10.1080/16000889.2017.1391663
Chenxi Xu, X. Shao, W. An, T. Nakatsuka, Yong Zhang, M. Sano, Zhengtang Guo
Abstract Tree ring cellulose oxygen isotopes (δ18O) were measured on 21 trees of Qilian juniper from the Animaqing Mountains, Tibetan Plateau, to investigate intra- and inter-tree variability, potential juvenile and elevation effects and climatic implications. There are no significant differences in mean and standard deviation of tree ring δ18O values at different heights in individual trees. Tree ring δ18O values from different directions show a high degree of coherence. The mean and standard deviation for vertical and circumferential δ18O time series are very similar, and δ18O data from different heights and directions are highly correlated (r > 0.88). The δ18O values of young trees are lower than those of old trees in the first 10 years of tree growth. Tree ring δ18O data from five different altitudes are highly correlated (r > 0.88) and share similar climatic signals. As such, an altitude effect on tree ring δ18O is not observed. Our results indicate that samples from one site, regardless of sampling height, direction or altitude, can be used to reconstruct a long-term δ18O record. Tree ring δ18O data from the Animaqing Mountains show a significant negative correlation (r = −0.67; p < 0.001) with May–July regional precipitation and appear to be a promising proxy for precipitation reconstruction.
{"title":"Negligible local-factor influences on tree ring cellulose δ18O of Qilian juniper in the Animaqing Mountains of the eastern Tibetan Plateau","authors":"Chenxi Xu, X. Shao, W. An, T. Nakatsuka, Yong Zhang, M. Sano, Zhengtang Guo","doi":"10.1080/16000889.2017.1391663","DOIUrl":"https://doi.org/10.1080/16000889.2017.1391663","url":null,"abstract":"Abstract Tree ring cellulose oxygen isotopes (δ18O) were measured on 21 trees of Qilian juniper from the Animaqing Mountains, Tibetan Plateau, to investigate intra- and inter-tree variability, potential juvenile and elevation effects and climatic implications. There are no significant differences in mean and standard deviation of tree ring δ18O values at different heights in individual trees. Tree ring δ18O values from different directions show a high degree of coherence. The mean and standard deviation for vertical and circumferential δ18O time series are very similar, and δ18O data from different heights and directions are highly correlated (r > 0.88). The δ18O values of young trees are lower than those of old trees in the first 10 years of tree growth. Tree ring δ18O data from five different altitudes are highly correlated (r > 0.88) and share similar climatic signals. As such, an altitude effect on tree ring δ18O is not observed. Our results indicate that samples from one site, regardless of sampling height, direction or altitude, can be used to reconstruct a long-term δ18O record. Tree ring δ18O data from the Animaqing Mountains show a significant negative correlation (r = −0.67; p < 0.001) with May–July regional precipitation and appear to be a promising proxy for precipitation reconstruction.","PeriodicalId":22320,"journal":{"name":"Tellus B: Chemical and Physical Meteorology","volume":"111 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2017-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91350696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}