Articles | Volume 19, issue 18
Research article 20 Sep 2019
Research article | 20 Sep 2019
Evolution of anthropogenic air pollutant emissions in Guangdong Province, China, from 2006 to 2015
Yahui Bian et al.
No articles found.
Wenjie Wang, David D. Parrish, Xin Li, Min Shao, Ying Liu, Ziwei Mo, Sihua Lu, Min Hu, Xin Fang, Yusheng Wu, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15617–15633,Short summary
During the past decade, China has devoted very substantial resources to improving the environment. These efforts have improved atmospheric particulate matter loading, but ambient ozone levels have continued to increase. In this paper we investigate the causes of the increasing ozone concentrations through analysis of a data set that is, to our knowledge, unique: a 12-year data set including ground-level O3, NOx, and VOC precursors collected at an urban site in Beijing.
Luolin Wu, Jian Hang, Xuemei Wang, Min Shao, and Cheng Gong
Geosci. Model Dev. Discuss.,
Preprint under review for GMDShort summary
In order to improve the resolution and numerical accuracy of urban air quality simulation, this study has developed the APFoam-1.0 to examine the micro-scale reactive pollutant formation and dispersion in the urban area. The model has been validated and shows the good agreement with wind tunnel experimental data. Model sensitivity cases reveal that the vehicle emissions, background concentrations and wind conditions are the key factors affecting the photochemical reaction process.
Caihong Wu, Chaomin Wang, Sihang Wang, Wenjie Wang, Bin Yuan, Jipeng Qi, Baolin Wang, Hongli Wang, Chen Wang, Wei Song, Xinming Wang, Weiwei Hu, Shengrong Lou, Chenshuo Ye, Yuwen Peng, Zelong Wang, Yibo Huangfu, Yan Xie, Manni Zhu, Junyu Zheng, Xuemei Wang, Bin Jiang, Zhanyi Zhang, and Min Shao
Atmos. Chem. Phys., 20, 14769–14785,Short summary
Based on measurements from an online mass spectrometer, we quantify volatile organic compound (VOC) concentrations from numerous ions of the mass spectrometer, using information from laboratory-obtained calibration results. We find that most VOC concentrations are from oxygenated VOCs (OVOCs). We further show that these OVOCs also contribute significantly to OH reactivity. Our results suggest the important role of OVOCs in VOC emissions and chemistry in urban air.
Sarah E. Benish, Hao He, Xinrong Ren, Sandra J. Roberts, Ross J. Salawitch, Zhanqing Li, Fei Wang, Yuying Wang, Fang Zhang, Min Shao, Sihua Lu, and Russell R. Dickerson
Atmos. Chem. Phys., 20, 14523–14545,Short summary
Airborne observations of ozone and related pollutants show smog was pervasive in spring 2016 over Hebei Province, China. We find high amounts of ozone precursors throughout and even above the PBL, continuing to generate ozone at high rates to be potentially transported downwind. Concentrations even in the rural areas of this highly industrialized province promote widespread ozone production, and we show that to improve air quality over Hebei both NOx and VOCs should be targeted.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Chaomin Wang, Bin Yuan, Caihong Wu, Sihang Wang, Jipeng Qi, Baolin Wang, Zelong Wang, Weiwei Hu, Wei Chen, Chenshuo Ye, Wenjie Wang, Yele Sun, Chen Wang, Shan Huang, Wei Song, Xinming Wang, Suxia Yang, Shenyang Zhang, Wanyun Xu, Nan Ma, Zhanyi Zhang, Bin Jiang, Hang Su, Yafang Cheng, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 20, 14123–14138,Short summary
We utilized a novel online mass spectrometry method to measure the total concentration of higher alkanes at each carbon number at two different sites in China, allowing us to take into account SOA contributions from all isomers for higher alkanes. We found that higher alkanes account for significant fractions of SOA formation at the two sites. The contributions are comparable to or even higher than single-ring aromatics, the most-recognized SOA precursors in urban air.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions are predictable and explained by key emissions. These results are used to estimate the premature mortality associated to SOA in urban regions.
Wenjie Wang, Jipeng Qi, Jun Zhou, Bin Yuan, Yuwen Peng, Sihang Wang, Jonathan Williams, Vinayak Sinha, and Min Shao
Atmos. Meas. Tech. Discuss.,
Revised manuscript accepted for AMTShort summary
We designed a new reactor for measurements of OH reactivity (i.e. OH radicals loss freqency) based on the comparative reactivity method work under the conditions with high NOx conditions, such as in cities. We performed a series laboratory tests to evaluate the new reactor to prove this. The new reactor was used in the field and performed well to measure OH reactivity in air influenced by upwind cities.
Zhenhao Ling, Qianqian Xie, Min Shao, Zhe Wang, Tao Wang, Hai Guo, and Xuemei Wang
Atmos. Chem. Phys., 20, 11451–11467,Short summary
The observation data from a receptor site in the Pearl River Delta region were analyzed by a photochemical box model with near-explicit chemical mechanisms (i.e., the Master Chemical Mechanism, MCM), improvements with reversible and irreversible heterogeneous processes of glyoxal and methylglyoxal, and the gas-particle partitioning of oxidation products in the present study.
Mingfu Cai, Baoling Liang, Qibin Sun, Shengzhen Zhou, Xiaoyang Chen, Bin Yuan, Min Shao, Haobo Tan, and Jun Zhao
Atmos. Chem. Phys., 20, 9153–9167,Short summary
Cloud condensation nuclei activity in marine atmosphere affects cloud formation and the solar radiation balance over ocean. We employed advanced instruments to measure aerosol hygroscopicity and chemical composition in the northern South China Sea. Our results show that marine aerosols can be affected by local emissions or pollutants from long-range transport. Our study highlights dynamical variations in particle properties and the impact of long-range transport on this region during summertime.
Luolin Wu, Ming Chang, Xuemei Wang, Jian Hang, Jinpu Zhang, Liqing Wu, and Min Shao
Geosci. Model Dev., 13, 23–40,Short summary
We developed the Real-time On-road Emission (ROE v1.0) model to obtain the street-scale on-road hot emissions by using real-time big data for traffic provided by the Gaode Map navigation application. The results are close to other emission inventories. Meanwhile, we applied our results to a street-level air quality model for studying the impact of the national holiday traffic volume change on air quality. The model can be further extended to more districts in China or other countries.
Leifeng Yang, Huihong Luo, Zibing Yuan, Junyu Zheng, Zhijiong Huang, Cheng Li, Xiaohua Lin, Peter K. K. Louie, Duohong Chen, and Yahui Bian
Atmos. Chem. Phys., 19, 12901–12916,Short summary
Ozone (O3) pollution is increasing in China and the underlying reason for this is unknown, making effective control unrealistic. Using an innovative approach, we quantitatively identified the impact of meteorology and precursor emission changes, both local and nonlocal, on the long-term O3 trend in the PRD. Meteorology can contribute to up to 15 % of long-term O3 variations. The undesirable NOx/VOC control ratio over the past few years is most likely responsible for the O3 increase in the PRD.
Wenjie Wang, Xin Li, Min Shao, Min Hu, Limin Zeng, Yusheng Wu, and Tianyi Tan
Atmos. Chem. Phys., 19, 9413–9429,Short summary
We quantitatively evaluated the relationship between photolysis frequencies and AOD based on 4 years of observational data in Beijing. This study concludes that the influence of aerosol on photolysis frequencies and thus on the rate of oxidation of VOCs and NOx to ozone is important for determining the atmospheric effects of controlling the precursor emissions of these two important air pollutants (aerosols and ozone).
Zhuoran He, Xuemei Wang, Zhenhao Ling, Jun Zhao, Hai Guo, Min Shao, and Zhe Wang
Atmos. Chem. Phys., 19, 8801–8816,Short summary
In this study, source apportionment of volatile organic compounds (VOCs) and their contributions to photochemical O3 formation were analyzed by the positive matrix factorization model and an observation-based model using data collected at a receptor site in the Pearl River Delta (PRD) region. Furthermore, the policies for controlling VOCs are briefly reviewed. The findings could provide quantitative information for devising appropriate measures against VOCs, NOx and O3 pollution in the PRD.
Liqing Wu, Xuemei Wang, Sihua Lu, Min Shao, and Zhenhao Ling
Atmos. Chem. Phys., 19, 8141–8161,Short summary
Semi-volatile and intermediate-volatility organic compounds (S–IVOCs) are considered critical precursors of secondary organic aerosol (SOA), which is an important component of fine particulate matter (PM2.5). In this study, an emission inventory of S–IVOCs in the Pearl River Delta (PRD) region was developed for the first time for the year 2010, while the contributions of S–IVOCs to SOA formation was evaluated by the WRF-Chem model.
Zhaofeng Tan, Keding Lu, Andreas Hofzumahaus, Hendrik Fuchs, Birger Bohn, Frank Holland, Yuhan Liu, Franz Rohrer, Min Shao, Kang Sun, Yusheng Wu, Limin Zeng, Yinsong Zhang, Qi Zou, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 19, 7129–7150,Short summary
Atmospheric OH, HO2, and RO2 radicals; OH reactivity; and trace gases measured in the Pearl River Delta in autumn 2014 are used for radical budget analyses. The RO2 budget suggests that unexplained OH reactivity is due to unmeasured volatile organic compounds. The OH budget points to a missing OH source and that of RO2 to a missing RO2 sink at low NO. This could indicate a common, unknown process that converts RO2 to OH without the involvement of NO, which would reduce ozone production by 30 %.
Guo Li, Yafang Cheng, Uwe Kuhn, Rongjuan Xu, Yudong Yang, Hannah Meusel, Zhibin Wang, Nan Ma, Yusheng Wu, Meng Li, Jonathan Williams, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Hang Su
Atmos. Chem. Phys., 19, 2209–2232,Short summary
VOCs play a key role in atmospheric chemistry. Emission and deposition on soil have been suggested as important sources and sinks of atmospheric trace gases. The exchange characteristics and heterogeneous chemistry of VOCs on soil, however, are not well understood. We used a newly designed differential coated-wall flow tube system to investigate the long-term variability of bidirectional air–soil exchange of 13 VOCs at ambient air conditions of an urban background site in Beijing.
Hansen Cao, Tzung-May Fu, Lin Zhang, Daven K. Henze, Christopher Chan Miller, Christophe Lerot, Gonzalo González Abad, Isabelle De Smedt, Qiang Zhang, Michel van Roozendael, François Hendrick, Kelly Chance, Jie Li, Junyu Zheng, and Yuanhong Zhao
Atmos. Chem. Phys., 18, 15017–15046,Short summary
Our top-down estimates for annual total Chinese NMVOC emissions was 30.7 to 49.5 Tg y−1, including 16.4 to 23.6 Tg y−1 from anthropogenic sources, 12.2 to 22.8 Tg y−1 from biogenic sources, and 2.08 to 3.13 Tg y−1 from biomass burning. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. The glyoxal and formaldehyde constraints helped distinguish the NMVOC species from different sources.
Daocheng Gong, Hao Wang, Shenyang Zhang, Yu Wang, Shaw Chen Liu, Hai Guo, Min Shao, Congrong He, Duohong Chen, Lingyan He, Lei Zhou, Lidia Morawska, Yuanhang Zhang, and Boguang Wang
Atmos. Chem. Phys., 18, 14417–14432,Short summary
The complex air pollution in the air-polluted Pearl River Delta (PRD) region in southern China has significantly elevated the background atmospheric oxidative capacity of the adjacent forests and subsequently lowered the levels of important biogenic volatile organic compounds, such as isoprene, which probably affect the regional air quality and ecological environment in the long term.
Weiqiang Yang, Yanli Zhang, Xinming Wang, Sheng Li, Ming Zhu, Qingqing Yu, Guanghui Li, Zhonghui Huang, Huina Zhang, Zhenfeng Wu, Wei Song, Jihua Tan, and Min Shao
Atmos. Chem. Phys., 18, 12663–12682,Short summary
We present observation-based evaluations of the reduction of ambient VOCs under intervention control measures during APEC China 2014 in Beijing and the contributions of emissions from domestic solid fuel burning to ambient VOCs during winter heating. Controlling vehicle exhaust and solvent use was found to be effective in reducing ambient VOCs in non-heating periods, and controlling emissions from residential burning of solid fuels became much more important during winter heating.
Zhaofeng Tan, Franz Rohrer, Keding Lu, Xuefei Ma, Birger Bohn, Sebastian Broch, Huabin Dong, Hendrik Fuchs, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Yuhan Liu, Anna Novelli, Min Shao, Haichao Wang, Yusheng Wu, Limin Zeng, Min Hu, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 18, 12391–12411,Short summary
We present the first wintertime OH, HO2, and RO2 measurements in Beijing, China. OH concentrations are nearly 2-fold larger than those observed in foreign cities during wintertime. The high OH and large OH reactivities indicate photochemical processes can be effective even during wintertime. A box model largely underestimated HO2 and RO2 concentrations during pollution episodes correlated with high NOx, indicating a deficit current chemistry in the high NOx regime.
Zhuofei Du, Min Hu, Jianfei Peng, Wenbin Zhang, Jing Zheng, Fangting Gu, Yanhong Qin, Yudong Yang, Mengren Li, Yusheng Wu, Min Shao, and Shijin Shuai
Atmos. Chem. Phys., 18, 9011–9023,Short summary
By combining approaches involving chassis dynamometer measurements and environmental chamber simulations, we find that gasoline direct injection (GDI) vehicles contribute more primary aerosol and secondary organic aerosol than port fuel injection (PFI) vehicles. Our results highlight the considerable potential contribution of GDI vehicles to urban air pollution, since the market share of GDI vehicles will dominate over that of PFI vehicles in the future.
Cheng Li, Jens Borken-Kleefeld, Junyu Zheng, Zibing Yuan, Jiamin Ou, Yue Li, Yanlong Wang, and Yuanqian Xu
Atmos. Chem. Phys., 18, 6075–6093,Short summary
We developed an integrated approach based on the Automatic Identification System (AIS) to promote the estimation of sectoral ship emissions in China. Based upon this approach, the sector-based contributions, decadal evolution from 2004 to 2013, emission projection to 2040, and impact of different sizes of Emission Control Areas (ECAs) on emission reductions were investigated, aiming to provide solid scientific support for ship emissions control policy making in China.
Guo Li, Hang Su, Uwe Kuhn, Hannah Meusel, Markus Ammann, Min Shao, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 18, 2669–2686,Short summary
Coated-wall flow tube reactors are frequently used to investigate gas uptake and heterogeneous or multiphase reaction kinetics under laminar flow conditions. In previous applications, the effects of coating surface roughness on flow conditions were not well quantified. In this study, a criterion is proposed to eliminate/minimize the potential effects of coating surface roughness on laminar flow in coated-wall flow tube experiments and validate the applications of diffusion correction methods.
Jianfei Peng, Min Hu, Song Guo, Zhuofei Du, Dongjie Shang, Jing Zheng, Jun Zheng, Limin Zeng, Min Shao, Yusheng Wu, Don Collins, and Renyi Zhang
Atmos. Chem. Phys., 17, 10333–10348,Short summary
Rapid growth of BC particles was observed in Beijing using a new outdoor chamber, with an average growth rate of 26 ± 11 nm h−1. Secondary organic aerosol (SOA) accounted for more than 90 % of the coating mass. The hygroscopic growth factor of BC particles increased to 1.06–1.08 upon ageing. The κ (kappa) values for BC particles were calculated as only 0.035, indicating that initial photochemical ageing of BC particles does not appreciably alter the particle hygroscopicity in Beijing.
Yudong Yang, Min Shao, Stephan Keßel, Yue Li, Keding Lu, Sihua Lu, Jonathan Williams, Yuanhang Zhang, Liming Zeng, Anke C. Nölscher, Yusheng Wu, Xuemei Wang, and Junyu Zheng
Atmos. Chem. Phys., 17, 7127–7142,Short summary
Total OH reactivity is an important parameter to evaluate understanding of atmospheric chemistry, especially the VOC contribution to air pollution. Measured by comparative reactivity methods, total OH reactivity in Beijing and Heshan revealed significant differences between measured and calculated results, such as missing reactivity, which were related to unmeasured primary or secondary species. This missing reactivity would introduce a 21–30 % underestimation for ozone production efficiency.
Zhaofeng Tan, Hendrik Fuchs, Keding Lu, Andreas Hofzumahaus, Birger Bohn, Sebastian Broch, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinsong Zhang, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 17, 663–690,Short summary
In this study, we performed accurate OH measurements as well as selective HO2 and RO2 measurements at a rural site in North China Plain with state-of-the-art instruments newly developed. We confirmed the previous discovery on the enhancement of the OH in low NOx with which little O3 production was associated, and we found a missing RO2 source in high NOx which promoted higher O3 production. Our results are of vital importance for ozone abatement strategies currently under discussion for China.
Hendrik Fuchs, Zhaofeng Tan, Keding Lu, Birger Bohn, Sebastian Broch, Steven S. Brown, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Kyung-Eun Min, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinson Zhang, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 17, 645–661,Short summary
OH reactivity was measured during a 1-month long campaign at a rural site in the North China Plain in 2014. OH reactivity measurements are compared to calculations using OH reactant measurements. Good agreement is found indicating that all important OH reactants were measured. In addition, the chemical OH budget is analyzed. In contrast to previous campaigns in China in 2006, no significant imbalance between OH production and destruction is found.
Yee Jun Tham, Zhe Wang, Qinyi Li, Hui Yun, Weihao Wang, Xinfeng Wang, Likun Xue, Keding Lu, Nan Ma, Birger Bohn, Xin Li, Simonas Kecorius, Johannes Größ, Min Shao, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 16, 14959–14977,Short summary
This work addresses the unclear global significance of chlorine activation processes in the troposphere. The first high-quality measurement data set of ClNO2 in northern China revealed strong ClNO2 production in the residual layers, and demonstrated its significant effects on radical budget and ozone production. Our findings imply the widespread effects of ClNO2 over the polluted regions of northern China, which may increase photochemical and haze pollution.
Qinyi Li, Li Zhang, Tao Wang, Yee Jun Tham, Ravan Ahmadov, Likun Xue, Qiang Zhang, and Junyu Zheng
Atmos. Chem. Phys., 16, 14875–14890,Short summary
The regional distributions and impacts of N2O5 and ClNO2 remain poorly understood. To address the problem, we developed a chemical transport model further and conducted the first high-resolution simulation of the distributions of the two species. Our research demonstrated the significant impacts of the two gases on the lifetime of nitrogen oxides, secondary nitrate production and ozone formation in southern China and highlighted the necessity of considering this chemistry in air quality models.
Wei Hu, Min Hu, Wei-Wei Hu, Hongya Niu, Jing Zheng, Yusheng Wu, Wentai Chen, Chen Chen, Lingyu Li, Min Shao, Shaodong Xie, and Yuanhang Zhang
Atmos. Chem. Phys., 16, 13213–13230,Short summary
An Aerodyne high-resolution time-of-flight AMS was deployed at a suburban site in the Sichuan Basin, southwestern China, under high emission intensity, and unique geographical and adverse meteorological conditions. OA was the most abundant component (36 %) in PM1, characterized by a relatively high oxidation state. The contributions of BBOA and BC to PM1 were high in primary emission episodes, highlighting the critical influence of biomass burning.
Guo Li, Hang Su, Xin Li, Uwe Kuhn, Hannah Meusel, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Yafang Cheng
Atmos. Chem. Phys., 16, 10299–10311,Short summary
Indoor and outdoor formaldehyde (HCHO) are both of considerable concern because of its health effects and its role in atmospheric chemistry. The heterogeneous reactions between gaseous HCHO with soils can pose important impact on both HCHO budget and soil ecosystem. Our results confirms that HCHO uptake by soil is a complex process involving both adsorption/desorption and chemical reactions. Soil and soil-derived airborne particles can either act as a source or a sink for HCHO.
Mingmin Zou, Xiaozhen Xiong, Naoko Saitoh, Juying Warner, Ying Zhang, Liangfu Chen, Fuzhong Weng, and Meng Fan
Atmos. Meas. Tech., 9, 3567–3576,Short summary
Both AIRS and GOSAT TANSO-FTS TIR have been used to retrieve atmosphere CH4. The purpose of an intercomparison is to provide useful information to users on the characteristics of these two different products when they investigate the spatial and temporal variation of CH4. On the other hand, AIRS V6 CH4 data were already validated by comparing with aircraft data. This intercomparison is also a kind of indirect validation to GOSAT data.
Xuekun Fang, Min Shao, Andreas Stohl, Qiang Zhang, Junyu Zheng, Hai Guo, Chen Wang, Ming Wang, Jiamin Ou, Rona L. Thompson, and Ronald G. Prinn
Atmos. Chem. Phys., 16, 3369–3382,Short summary
This is the first study reporting top-down estimates of benzene and toluene emissions in southern China using atmospheric measurement data from a rural site in the area, an atmospheric transport model and an inverse modeling method. This study shows in detail the temporal and spatial differences between the inversion estimate and four different bottom-up emission inventories (RCP, REAS, MEIC; Yin et al., 2015). We propose that more observations are urgently needed in future.
Yaning Kang, Mingxu Liu, Yu Song, Xin Huang, Huan Yao, Xuhui Cai, Hongsheng Zhang, Ling Kang, Xuejun Liu, Xiaoyuan Yan, Hong He, Qiang Zhang, Min Shao, and Tong Zhu
Atmos. Chem. Phys., 16, 2043–2058,Short summary
The multi-year (1980–2012) comprehensive ammonia emissions inventories were compiled for China on 1 km × 1 km grid. Various realistic parameters (ambient temperature, wind speed, soil acidity, synthetic fertilizer types, etc.) were considered in these inventories to synthetically refine the emission factors of ammonia volatilization according to local agricultural practice. This paper shows the interannual trend and spatial distribution of ammonia emissions in details over recent decades.
N. Li, T.-M. Fu, J. J. Cao, J. Y. Zheng, Q. Y. He, X. Long, Z. Z. Zhao, N. Y. Cao, J. S. Fu, and Y. F. Lam
Atmos. Chem. Phys. Discuss.,
Revised manuscript not accepted
Y. Liu, B. Yuan, X. Li, M. Shao, S. Lu, Y. Li, C.-C. Chang, Z. Wang, W. Hu, X. Huang, L. He, L. Zeng, M. Hu, and T. Zhu
Atmos. Chem. Phys., 15, 3045–3062,
M. Wang, M. Shao, W. Chen, S. Lu, Y. Liu, B. Yuan, Q. Zhang, Q. Zhang, C.-C. Chang, B. Wang, L. Zeng, M. Hu, Y. Yang, and Y. Li
Atmos. Chem. Phys., 15, 1489–1502,
X. Li, F. Rohrer, T. Brauers, A. Hofzumahaus, K. Lu, M. Shao, Y. H. Zhang, and A. Wahner
Atmos. Chem. Phys., 14, 12291–12305,
Q. Zhang, B. Yuan, M. Shao, X. Wang, S. Lu, K. Lu, M. Wang, L. Chen, C.-C. Chang, and S. C. Liu
Atmos. Chem. Phys., 14, 6089–6101,
M. Wang, M. Shao, W. Chen, B. Yuan, S. Lu, Q. Zhang, L. Zeng, and Q. Wang
Atmos. Chem. Phys., 14, 5871–5891,
M. Li, Q. Zhang, D. G. Streets, K. B. He, Y. F. Cheng, L. K. Emmons, H. Huo, S. C. Kang, Z. Lu, M. Shao, H. Su, X. Yu, and Y. Zhang
Atmos. Chem. Phys., 14, 5617–5638,
K. D. Lu, F. Rohrer, F. Holland, H. Fuchs, T. Brauers, A. Oebel, R. Dlugi, M. Hu, X. Li, S. R. Lou, M. Shao, T. Zhu, A. Wahner, Y. H. Zhang, and A. Hofzumahaus
Atmos. Chem. Phys., 14, 4979–4999,
W. T. Chen, M. Shao, S. H. Lu, M. Wang, L. M. Zeng, B. Yuan, and Y. Liu
Atmos. Chem. Phys., 14, 3047–3062,
Z. B. Wang, M. Hu, D. Mogensen, D. L. Yue, J. Zheng, R. Y. Zhang, Y. Liu, B. Yuan, X. Li, M. Shao, L. Zhou, Z. J. Wu, A. Wiedensohler, and M. Boy
Atmos. Chem. Phys., 13, 11157–11167,
W. W. Hu, M. Hu, B. Yuan, J. L. Jimenez, Q. Tang, J. F. Peng, W. Hu, M. Shao, M. Wang, L. M. Zeng, Y. S. Wu, Z. H. Gong, X. F. Huang, and L. Y. He
Atmos. Chem. Phys., 13, 10095–10112,
C.-C. Chang, M. Shao, C. C. K. Chou, S.-C. Liu, J.-L. Wang, K.-Z. Lee, C.-H. Lai, T. Zhu, and P.-H. Lin
Atmos. Chem. Phys. Discuss.,
Revised manuscript not accepted
B. Yuan, W. W. Hu, M. Shao, M. Wang, W. T. Chen, S. H. Lu, L. M. Zeng, and M. Hu
Atmos. Chem. Phys., 13, 8815–8832,
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meteorological influences on daily variability in summertime surface ozone in eastern ChinaVariability in a four-network composite of atmospheric CO2 differences between three primary baseline sitesQuantifying the impact of synoptic circulation patterns on ozone variability in northern China from April to October 2013–2017Multivariate statistical air mass classification for the high-alpine observatory at the Zugspitze Mountain, GermanySpeciated atmospheric mercury and sea–air exchange of gaseous mercury in the South China SeaMethane emissions from oil and gas platforms in the North SeaAssessing London CO2, CH4 and CO emissions using aircraft measurements and dispersion modelling2005–2017 ozone trends and potential benefits of local measures as deduced from air quality measurements in the north of the Barcelona metropolitan areaCountry-scale greenhouse gas budgets using shipborne measurements: a case study for the UK and IrelandIntercomparison of midlatitude tropospheric and lower-stratospheric water vapor measurements and comparison to ECMWF humidity dataEddy flux measurements of sulfur dioxide deposition to the sea surfaceQuantifying uncertainties from mobile-laboratory-derived emissions of well pads using inverse Gaussian methodsObserving local CO2 sources using low-cost, near-surface urban monitorsSpatiotemporal variability of NO2 and PM2.5 over Eastern China: observational and model analyses with a novel statistical methodSpatial–temporal patterns of inorganic nitrogen air concentrations and deposition in eastern ChinaPhenomenology of summer ozone episodes over the Madrid Metropolitan Area, central SpainShip-based MAX-DOAS measurements of tropospheric NO2, SO2, and HCHO distribution along the Yangtze RiverGradient flux measurements of sea–air DMS transfer during the Surface Ocean Aerosol Production (SOAP) experimentMeasurements of atmospheric ethene by solar absorption FTIR spectrometryOzone pollution around a coastal region of South China Sea: interaction between marine and continental airAbundance and sources of atmospheric halocarbons in the Eastern MediterraneanDiurnal, synoptic and seasonal variability of atmospheric CO2 in the Paris megacity areaAtmospheric carbonyl sulfide (OCS) measured remotely by FTIR solar absorption spectrometryTemporal variation of VOC fluxes measured with PTR-TOF above a boreal forestLong-term trends of surface ozone and its influencing factors at the Mt Waliguan GAW station, China – Part 2: The roles of anthropogenic emissions and climate variabilityGaseous elemental mercury (GEM) fluxes over canopy of two typical subtropical forests in south ChinaObservations of ozone depletion events in a Finnish boreal forestMobile measurement of methane emissions from natural gas developments in northeastern British Columbia, CanadaImpacts of large-scale circulation on urban ambient concentrations of gaseous elemental mercury in New York, USASurface ozone at Nam Co in the inland Tibetan Plateau: variation, synthesis comparison and regional representativenessTrends and annual cycles in soundings of Arctic tropospheric ozoneEstimation of bubble-mediated air–sea gas exchange from concurrent DMS and CO2 transfer velocities at intermediate–high wind speedsEstimating the size of a methane emission point source at different scales: from local to landscapeGenesis of diamond dust, ice fog and thick cloud episodes observed and modelled above Dome C, AntarcticaImpact of typhoons on the composition of the upper troposphere within the Asian summer monsoon anticyclone: the SWOP campaign in Lhasa 2013An investigation on the origin of regional springtime ozone episodes in the western Mediterranean
Yuming Jin, Ralph F. Keeling, Eric J. Morgan, Eric Ray, Nicholas C. Parazoo, and Britton B. Stephens
Atmos. Chem. Phys., 21, 217–238,Short summary
We propose a new atmospheric coordinate (Mθe) based on equivalent potential temperature (θe) but with mass as the unit. This coordinate is useful in studying the spatial and temporal distribution of long-lived chemical tracers (CO2, CH4, O2 / N2, etc.) from sparse data, like airborne observation. Using this coordinate and sparse airborne observation (HIPPO and ATom), we resolve the Northern Hemisphere mass-weighted average CO2 seasonal cycle with high accuracy.
Hossein Maazallahi, Julianne M. Fernandez, Malika Menoud, Daniel Zavala-Araiza, Zachary D. Weller, Stefan Schwietzke, Joseph C. von Fischer, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 14717–14740,Short summary
Methane accounts for ∼ 25 % of current climate warming. The current lack of methane measurements is a barrier for tracking major sources, which are key for near-term climate mitigation. We use mobile measurements to identify and quantify methane emission sources in Utrecht (NL) and Hamburg (DE) with a focus on natural gas pipeline leaks. The measurements resulted in fixing the major leaks by the local utility, but coordinated efforts are needed at national levels for further emission reductions.
Chenchao Zhan, Min Xie, Chongwu Huang, Jane Liu, Tijian Wang, Meng Xu, Chaoqun Ma, Jianwei Yu, Yumeng Jiao, Mengmeng Li, Shu Li, Bingliang Zhuang, Ming Zhao, and Dongyang Nie
Atmos. Chem. Phys., 20, 13781–13799,Short summary
The Yangtze River Delta (YRD) region has been suffering from severe ozone (O3) pollution in recent years. Synoptic systems, like typhoons, can have a significant effect on O3 episodes. However, research on landfall typhoons affecting O3 in the YRD is limited. This work aims to reveal the main processes of landfall typhoons affecting surface O3 and estimate health impacts of O3 during the study period in the YRD, which can be useful for taking reasonable pollution control measures in this area.
José M. Esbrí, Pablo L. Higueras, Alba Martínez-Coronado, and Rocío Naharro
Atmos. Chem. Phys., 20, 12995–13010,Short summary
The aim of this work was to identify criteria to obtain the minimum amount of data with the maximum meaning and representativeness in order to delimit risk areas, both in a spatial and temporal respect. We have constructed a model of vertical mercury movements which could be used to predict the location and timing of mercury inhalation risk. Also, we have designed a monitoring strategy to identify the relevant criteria, which involved the measurement of gaseous mercury in a vertical section.
Alina Fiehn, Julian Kostinek, Maximilian Eckl, Theresa Klausner, Michał Gałkowski, Jinxuan Chen, Christoph Gerbig, Thomas Röckmann, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Pawel Jagoda, Norman Wildmann, Christian Mallaun, Rostyslav Bun, Anna-Leah Nickl, Patrick Jöckel, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 20, 12675–12695,Short summary
A severe reduction of greenhouse gas emissions is necessary to fulfill the Paris Agreement. We use aircraft- and ground-based in situ observations of trace gases and wind speed from two flights over the Upper Silesian Coal Basin, Poland, for independent emission estimation. The derived methane emission estimates are within the range of emission inventories, carbon dioxide estimates are in the lower range and carbon monoxide emission estimates are slightly higher than emission inventory values.
Flora Kluge, Tilman Hüneke, Matthias Knecht, Michael Lichtenstern, Meike Rotermund, Hans Schlager, Benjamin Schreiner, and Klaus Pfeilsticker
Atmos. Chem. Phys., 20, 12363–12389,Short summary
The presented study reports on airborne measurements of formaldehyde, glyoxal, methylglyoxal, and CO over the Amazon basin and lays a special focus on the influence of biomass burning emissions on the atmospheric profiles of these carbonyl compounds within the planetary boundary layer as well as in the free and upper troposphere.
Alkuin Maximilian Koenig, Olivier Magand, Paolo Laj, Marcos Andrade, Isabel Moreno, Fernando Velarde, Grover Salvatierra, René Gutierrez, Luis Blacutt, Diego Aliaga, Thomas Reichler, Karine Sellegri, Olivier Laurent, Michel Ramonet, and Aurélien Dommergue
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
The environmental cycling of atmospheric mercury, a harmful global contaminant, is still not sufficiently constrained, partly due to missing data in remote regions. Here, we address this issue by presenting 20 months of atmospheric mercury measurements, sampled in the Bolivian Andes. We observe a significant seasonal pattern, whose key features we explore. Moreover, we deduce ratios to constrain South American biomass burning mercury emissions and the mercury uptake by the Amazon rainforest.
Wei Wang, Laurens Ganzeveld, Samuel Rossabi, Jacques Hueber, and Detlev Helmig
Atmos. Chem. Phys., 20, 11287–11304,Short summary
Trees exchange with the atmosphere nitrogen oxides and ozone, affecting the tropospheric composition and consequently air quality and ecosystem health. We examined the leaf-level gas exchanges for four typical tree species (pine, maple, oak, aspen) found in northern Michigan, US. The leaves largely absorb the gases, showing little evidence of emission. We measured the uptake rates that can be used to improve model studies of the source and sink processes controlling these gases in forests.
Ingeborg Levin, Ute Karstens, Markus Eritt, Fabian Maier, Sabrina Arnold, Daniel Rzesanke, Samuel Hammer, Michel Ramonet, Gabriela Vítková, Sebastien Conil, Michal Heliasz, Dagmar Kubistin, and Matthias Lindauer
Atmos. Chem. Phys., 20, 11161–11180,Short summary
Based on observations and Stochastic Time-Inverted Lagrangian Transport (STILT) footprint modelling, a sampling strategy has been developed for tall tower stations of the Integrated Carbon Observation System (ICOS) research infrastructure atmospheric station network. This strategy allows independent quality control of in situ measurements, provides representative coverage of the influence area of the sites, and is capable of automated targeted sampling of fossil fuel CO2 emission hotspots.
Peter G. Simmonds, Matthew Rigby, Alistair J. Manning, Sunyoung Park, Kieran M. Stanley, Archie McCulloch, Stephan Henne, Francesco Graziosi, Michela Maione, Jgor Arduini, Stefan Reimann, Martin K. Vollmer, Jens Mühle, Simon O'Doherty, Dickon Young, Paul B. Krummel, Paul J. Fraser, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Mi-Kyung Park, Hyeri Park, Tim Arnold, Chris Rennick, L. Paul Steele, Blagoj Mitrevski, Ray H. J. Wang, and Ronald G. Prinn
Atmos. Chem. Phys., 20, 7271–7290,Short summary
Sulfur hexafluoride (SF6) is a potent greenhouse gas which is regulated under the Kyoto Protocol. From a 40-year record of measurements, collected at five global monitoring sites and archived air samples, we show that its concentration in the atmosphere has steadily increased. Using modelling techniques, we estimate that global emissions have increased by about 24 % over the past decade. We find that this increase is driven by the demand for SF6-insulated switchgear in developing countries.
Santiago Botía, Christoph Gerbig, Julia Marshall, Jost V. Lavric, David Walter, Christopher Pöhlker, Bruna Holanda, Gilberto Fisch, Alessandro Carioca de Araújo, Marta O. Sá, Paulo R. Teixeira, Angélica F. Resende, Cleo Q. Dias-Junior, Hella van Asperen, Pablo S. Oliveira, Michel Stefanello, and Otávio C. Acevedo
Atmos. Chem. Phys., 20, 6583–6606,Short summary
A long record of atmospheric methane concentrations in central Amazonia was analyzed. We describe events in which concentrations at 79 m are higher than at 4 m. These events are more frequent during the nighttime of dry season, but we found no association with fire signals. Instead, we suggest that a combination of nighttime transport and a nearby source could explain such events. Our research gives insights into how methane is transported in the complex nocturnal atmosphere in Amazonia.
Nikolay V. Balashov, Kenneth J. Davis, Natasha L. Miles, Thomas Lauvaux, Scott J. Richardson, Zachary R. Barkley, and Timothy A. Bonin
Atmos. Chem. Phys., 20, 4545–4559,Short summary
An accurate independent verification methodology to estimate methane (a powerful greenhouse gas) emissions is essential for the effective implementation of policies that aim to reduce the impacts of climate change. In this paper, four uncertainties that complicate the independent estimation of urban methane emissions are identified: the definition of urban domain, background heterogeneity, emissions temporal variability, and missing sources. Ways to improve emission estimates are suggested.
Jia Chen, Florian Dietrich, Hossein Maazallahi, Andreas Forstmaier, Dominik Winkler, Magdalena E. G. Hofmann, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 3683–3696,Short summary
We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Pavlos Kalabokas, Niels Roland Jensen, Mauro Roveri, Jens Hjorth, Maxim Eremenko, Juan Cuesta, Gaëlle Dufour, Gilles Foret, and Matthias Beekmann
Atmos. Chem. Phys., 20, 1861–1885,Short summary
The influence of tropospheric ozone on the surface measurements at a regional air pollution station in the pre-Alpine area of northern Italy is investigated. During such episodes the local air pollution parameters show generally very low values, while the ozone levels reach high values, occasionally exceeding the ozone air quality standards. Better understanding of ozone variability over the examined region will help in the formulation of more effective policies for the environment and climate.
Han Han, Jane Liu, Lei Shu, Tijian Wang, and Huiling Yuan
Atmos. Chem. Phys., 20, 203–222,Short summary
We statistically assessed the impacts of local and synoptic meteorology on daily surface ozone in eastern China in summer during 2013–2018. The results show that the meteorology described by a multiple linear regression model explains 43 % of variations in surface ozone. The most important local meteorological factors vary with location in eastern China. The maximum impact of the predominant synoptic pattern on surface ozone can reach ± 8 µg m-3 or ± 16 % of the daily mean over some regions.
Roger J. Francey, Jorgen S. Frederiksen, L. Paul Steele, and Ray L. Langenfelds
Atmos. Chem. Phys., 19, 14741–14754,Short summary
25-year composites of interhemispheric baseline CO2 differences demonstrate close agreement between 4 monitoring networks. Variability from monthly to multiyear time frames mostly reflects variability in upper troposphere dynamical indices chosen to represent eddy and mean transport interhemispheric exchange. Monthly interhemispheric atmospheric fluxes are much larger than air–surface terrestrial exchanges. The composite differences offer unusual constraints on transport in global carbon models.
Jingda Liu, Lili Wang, Mingge Li, Zhiheng Liao, Yang Sun, Tao Song, Wenkang Gao, Yonghong Wang, Yan Li, Dongsheng Ji, Bo Hu, Veli-Matti Kerminen, Yuesi Wang, and Markku Kulmala
Atmos. Chem. Phys., 19, 14477–14492,Short summary
We analyzed the surface ozone variation characteristics and quantified the impact of synoptic and local meteorological factors on northern China during the warm season based on multi-city, in situ ozone and meteorological data, as well as meteorological reanalysis. The results of quantitative exploration on synoptic and local meteorological factors influencing both interannual and day-to-day ozone variations will provide the scientific basis for evaluating emission reduction measures.
Armin Sigmund, Korbinian Freier, Till Rehm, Ludwig Ries, Christian Schunk, Anette Menzel, and Christoph K. Thomas
Atmos. Chem. Phys., 19, 12477–12494,Short summary
Air masses at the Schneefernerhaus mountain site at Zugspitze Mountain, Germany, were classified with respect to the atmospheric layer from which they originated and their degree of pollution. Measurements of several gases, particulate matter, and standard meteorological quantities indicated that polluted air was lifted to the site in 31 % of cases and clean air descended to the site in approximately 14 % cases while most of the remaining cases were ambiguous.
Chunjie Wang, Zhangwei Wang, Fan Hui, and Xiaoshan Zhang
Atmos. Chem. Phys., 19, 10111–10127,Short summary
A low GEM level indicated that the SCS suffered less anthropogenic influence. There was no significant difference in GEM and HgP2.5 values between day and night, but the RGM level was higher in daytime than in nighttime. The size distribution of HgP in PM10 was observed to be bi-modal, but the coarse modal was the dominant size. The annual emission flux of Hg0 from the SCS was estimated to be 159 ton yr-1. The dry deposition was an important pathway for the input of atmospheric Hg to the SCS.
Stuart N. Riddick, Denise L. Mauzerall, Michael Celia, Neil R. P. Harris, Grant Allen, Joseph Pitt, John Staunton-Sykes, Grant L. Forster, Mary Kang, David Lowry, Euan G. Nisbet, and Alistair J. Manning
Atmos. Chem. Phys., 19, 9787–9796,Short summary
Currently, bottom-up methods estimate that 0.13 % of methane produced by UK North Sea oil and gas installations is lost. Here we measure emissions from eight platforms in the North Sea and, when considered collectively, the methane loss is estimated at 0.19 % of gas production. As this ambient loss is not explicitly accounted for in the bottom-up approach, these measured emissions represent significant additional emissions above previous estimates.
Joseph R. Pitt, Grant Allen, Stéphane J.-B. Bauguitte, Martin W. Gallagher, James D. Lee, Will Drysdale, Beth Nelson, Alistair J. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 8931–8945,Short summary
This paper presents a new method to assess inventory estimates of greenhouse gas and air pollutant emissions for large cities and their surrounding regions. A case study using data sampled by a research aircraft around London was used to test the method. We found that the UK national inventory agrees with our observations for CO but needed lower emissions for CH4 to agree with the measured data. Repeated studies could help determine how these emissions vary on different timescales.
Jordi Massagué, Cristina Carnerero, Miguel Escudero, José María Baldasano, Andrés Alastuey, and Xavier Querol
Atmos. Chem. Phys., 19, 7445–7465,
Carole Helfter, Neil Mullinger, Massimo Vieno, Simon O'Doherty, Michel Ramonet, Paul I. Palmer, and Eiko Nemitz
Atmos. Chem. Phys., 19, 3043–3063,Short summary
We present a novel approach to estimate the annual budgets of carbon dioxide (881.0 ± 128.5 Tg) and methane (2.55 ± 0.48 Tg) of the British Isles from shipborne measurements taken over a 3-year period (2015–2017). This study brings independent verification of the emission budgets estimated using alternative products and investigates the seasonality of these emissions, which is usually not possible.
Stefan Kaufmann, Christiane Voigt, Romy Heller, Tina Jurkat-Witschas, Martina Krämer, Christian Rolf, Martin Zöger, Andreas Giez, Bernhard Buchholz, Volker Ebert, Troy Thornberry, and Ulrich Schumann
Atmos. Chem. Phys., 18, 16729–16745,Short summary
We present an intercomparison of the airborne water vapor measurements during the ML-CIRRUS mission. Although the agreement of the hygrometers significantly improved compared to studies from recent decades, systematic differences remain under specific meteorological conditions. We compare the measurements to model data, where we observe a model wet bias in the lower stratosphere close to the tropopause, likely caused by a blurred humidity gradient in the model tropopause.
Jack G. Porter, Warren De Bruyn, and Eric S. Saltzman
Atmos. Chem. Phys., 18, 15291–15305,Short summary
Deposition to the sea surface is a major loss pathway for highly soluble atmospheric trace gases. These fluxes are important to biogeochemical cycles, climate, and air quality. Here we report measurements of air–sea fluxes of sulfur dioxide, sensible heat, and momentum to coastal waters. Transfer velocities derived from the data show a dependence on molecular diffusivity, demonstrating the importance of diffusion in the interfacial layer on the atmospheric side of the air–sea interface.
Dana R. Caulton, Qi Li, Elie Bou-Zeid, Jeffrey P. Fitts, Levi M. Golston, Da Pan, Jessica Lu, Haley M. Lane, Bernhard Buchholz, Xuehui Guo, James McSpiritt, Lars Wendt, and Mark A. Zondlo
Atmos. Chem. Phys., 18, 15145–15168,Short summary
Mobile laboratory measurements have been widely used to quantify methane emissions from point sources such as oil and gas wells, but the emission uncertainties are poorly constrained. We designed a hierarchical measurement strategy to sample natural gas emissions in the Marcellus Shale play based upon high-resolution modeling of select sites. Our study quantifies the largest sources of error with this approach and provides guidance on how to best implement mobile laboratory sampling protocols.
Alexis A. Shusterman, Jinsol Kim, Kaitlyn J. Lieschke, Catherine Newman, Paul J. Wooldridge, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 13773–13785,Short summary
We describe the diversity and heterogeneity of urban CO2 levels observed using the BErkeley Atmospheric CO2 Observation Network, a distributed instrument of > 50 CO2 sensors stationed every ~ 2 km across the San Francisco Bay Area. We demonstrate that relatively simple mathematical techniques, applied to these observations, can be used to detect the small changes in highway CO2 emissions expected to result from upcoming fuel economy regulations, affirming the policy relevance of low-cost sensors.
Mengyao Liu, Jintai Lin, Yuchen Wang, Yang Sun, Bo Zheng, Jingyuan Shao, Lulu Chen, Yixuan Zheng, Jinxuan Chen, Tzung-May Fu, Yingying Yan, Qiang Zhang, and Zhaohua Wu
Atmos. Chem. Phys., 18, 12933–12952,Short summary
Eastern China is heavily polluted by NO2, PM2.5, and other air pollutants. Our study uses EOF–EEMD to analyze the spatiotemporal variability of ground-level NO2, PM2.5, and their associations with meteorological processes. Their regular diurnal cycles are mainly affected by human activities, while irregular day-to-day variations are dominated by weather processes representing synchronous variation or north–south opposing changes over Eastern China.
Wen Xu, Lei Liu, Miaomiao Cheng, Yuanhong Zhao, Lin Zhang, Yuepeng Pan, Xiuming Zhang, Baojing Gu, Yi Li, Xiuying Zhang, Jianlin Shen, Li Lu, Xiaosheng Luo, Yu Zhao, Zhaozhong Feng, Jeffrey L. Collett Jr., Fusuo Zhang, and Xuejun Liu
Atmos. Chem. Phys., 18, 10931–10954,Short summary
Our main results demonstrate that atmospheric Nr pollution in eastern China is more serious in the northern region than in the southern region. Any effects of current emission controls are not yet apparent in Nr pollution. NH3 emissions from fertilizer use were the largest contributor (36 %) to total inorganic Nr deposition. Our results provide useful information for policy-makers that mitigation of NH3 emissions should be a priority to tackle serious N deposition.
Xavier Querol, Andrés Alastuey, Gotzon Gangoiti, Noemí Perez, Hong K. Lee, Heeram R. Eun, Yonghee Park, Enrique Mantilla, Miguel Escudero, Gloria Titos, Lucio Alonso, Brice Temime-Roussel, Nicolas Marchand, Juan R. Moreta, M. Arantxa Revuelta, Pedro Salvador, Begoña Artíñano, Saúl García dos Santos, Mónica Anguas, Alberto Notario, Alfonso Saiz-Lopez, Roy M. Harrison, Millán Millán, and Kang-Ho Ahn
Atmos. Chem. Phys., 18, 6511–6533,Short summary
We show the main drivers of high O3 episodes in and around Madrid. High levels of ultrafine particles (UFPs) are evidenced, but we demonstrate that most O3 arises from the fumigation of high atmospheric layers, whereas UFPs are generated inside the PBL. O3 contributions from the fumigation of the vertical recirculation of regional air masses, hemispheric transport, and horizontally from direct urban plume transport are shown. Complexity arises from the need to quantify them to abate surface O3.
Qianqian Hong, Cheng Liu, Ka Lok Chan, Qihou Hu, Zhouqing Xie, Haoran Liu, Fuqi Si, and Jianguo Liu
Atmos. Chem. Phys., 18, 5931–5951,Short summary
We presented ship-based MAX-DOAS measurements of tropospheric trace gases' distribution along the eastern part of the Yangtze River during winter 2015. Tropospheric VCDs of NO2, SO2, and HCHO were retrieved from MAX-DOAS measurement spectra. Enhanced tropospheric NO2 and SO2 VCDs were detected over downwind areas of industrial zones over the Yangtze River. Our results indicate that different pollution control strategies should be applied in different provinces.
Murray J. Smith, Carolyn F. Walker, Thomas G. Bell, Mike J. Harvey, Eric S. Saltzman, and Cliff S. Law
Atmos. Chem. Phys., 18, 5861–5877,Short summary
The transfer of gases across the air–sea interface has a significant influence on climate. During a research voyage in the South Pacific we measured the transfer rate of the biogenic gas dimethyl sulfide (DMS) from the ocean using two independent methods. The agreement between the techniques provides confidence in their use in compilations of global gas transfer. We also identified physical conditions under which the observations are not well predicted by a standard gas transfer model.
Geoffrey C. Toon, Jean-Francois L. Blavier, and Keeyoon Sung
Atmos. Chem. Phys., 18, 5075–5088,Short summary
Remote sensing measurements of ethene have been made from the ground and from balloons. Ethene can be measured at low altitudes in polluted regions, such as the Los Angeles basin. Here ethene amounts have decreased by a factor of 3 over the past 25 years due to increasingly strict emission control regulations (e.g., on vehicle exhaust).
Hao Wang, Xiaopu Lyu, Hai Guo, Yu Wang, Shichun Zou, Zhenhao Ling, Xinming Wang, Fei Jiang, Yangzong Zeren, Wenzhuo Pan, Xiaobo Huang, and Jin Shen
Atmos. Chem. Phys., 18, 4277–4295,Short summary
While oceanic air is generally thought to be clean, the air pollution over waters in proximity to the coasts is not well recognized. This research indicated that ozone was higher over South China Sea (SCS) than that in the adjacent continental area, while continental anticyclone, tropical cyclone and land breeze favored O3 formation over SCS. In addition, weaker NO titration and stronger atmospheric oxidative capacity led to higher O3 production efficiency over SCS.
Fabian Schoenenberger, Stephan Henne, Matthias Hill, Martin K. Vollmer, Giorgos Kouvarakis, Nikolaos Mihalopoulos, Simon O'Doherty, Michela Maione, Lukas Emmenegger, Thomas Peter, and Stefan Reimann
Atmos. Chem. Phys., 18, 4069–4092,Short summary
Anthropogenic halocarbon emissions contribute to stratospheric ozone depletion and global warming. We measured atmospheric halocarbons for 6 months on Crete to extend the coverage of the existing observation network to the Eastern Mediterranean. The derived emission estimates showed a contribution of 16.8 % (13.6–23.3 %) and 53.2 % (38.1–84.2 %) of this region to the total HFC and HCFC emissions of the analyzed European domain and a reduction of the underlying uncertainties by 40–80 %.
Irène Xueref-Remy, Elsa Dieudonné, Cyrille Vuillemin, Morgan Lopez, Christine Lac, Martina Schmidt, Marc Delmotte, Frédéric Chevallier, François Ravetta, Olivier Perrussel, Philippe Ciais, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, T. Gerard Spain, and Christophe Ampe
Atmos. Chem. Phys., 18, 3335–3362,Short summary
Urbanized and industrialized areas are the largest source of fossil CO2. This work analyses the atmospheric CO2 variability observed from the first in situ network deployed in the Paris megacity area. Gradients of several ppm are found between the rural, peri-urban and urban sites at the diurnal to the seasonal scales. Wind direction and speed as well as boundary layer dynamics, correlated to highly variable urban emissions, are shown to be key regulator factors of the observed CO2 records.
Geoffrey C. Toon, Jean-Francois L. Blavier, and Keeyoon Sung
Atmos. Chem. Phys., 18, 1923–1944,Short summary
OCS is the main form of atmospheric sulfur. It is produced near the earth's surface and destroyed primarily in the stratosphere, where it is converted to stratospheric sulfate aerosol (SSA). SSA plays an important role in atmospheric chemistry and transport and so it is important to better understand the factors that regulate OCS and hence SSA. Ground-based and balloon-borne infrared spectra observed over the past 30 years are analyzed to provide an improved OCS dataset.
Simon Schallhart, Pekka Rantala, Maija K. Kajos, Juho Aalto, Ivan Mammarella, Taina M. Ruuskanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 815–832,Short summary
Emissions of volatile organic compounds (VOCs) have impact to air quality, human health and climate. We investigated the development of VOC exchange in a boreal forest between April and June 2013. VOC exchange and diversity increased towards summer, but over 75 % of the biogenic net exchange was driven by methanol, monoterpenes and acetone only. The boreal forest emitted less than 0.2 % carbon in form of VOCs in relation to the carbon uptake.
Wanyun Xu, Xiaobin Xu, Meiyun Lin, Weili Lin, David Tarasick, Jie Tang, Jianzhong Ma, and Xiangdong Zheng
Atmos. Chem. Phys., 18, 773–798,Short summary
The impact of anthropogenic emissions and climate variability on the long-term trends and periodicity of surface ozone measured at Mt Waliguan (WLG) for the period of 1994–2013 is studied. STT ozone and rising emissions in eastern China contribute to spring and autumnal increasing trends, respectively. The 2–3-, 3–7-, and 11-year periodicities in the ozone data are linked to the QBO, EASMI, and sunspot cycle, respectively. An empirical model is obtained for normalised monthly ozone at WLG.
Qian Yu, Yao Luo, Shuxiao Wang, Zhiqi Wang, Jiming Hao, and Lei Duan
Atmos. Chem. Phys., 18, 495–509,Short summary
This study provides high-quality direct observation data of a clean and a contaminated site in subtropical south China and quantifies the natural forest Hg emission. We find that clean and contaminated forests present a net GEM source with annual average values of 6.67 and 0.30 ng m-2 h-1, respectively; daily variations of GEM fluxes showed a source in the daytime with a peak at 13:00, and as a sink or balance at night; and higher atmospheric GEM concentration restricted the forest GEM emission.
Xuemeng Chen, Lauriane L. J. Quéléver, Pak L. Fung, Jutta Kesti, Matti P. Rissanen, Jaana Bäck, Petri Keronen, Heikki Junninen, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 49–63,Short summary
We analysed a 20-year-long dataset collected in a Finnish boreal forest at SMEAR II station to investigate the frequency and strength of ozone depletion events. We could identify a number of ozone depletion events that lasted for more than 3 h, mainly in the autumn and winter months. Their occurrence was likely related to the formation of a low mixing layer under the conditions of low temperatures, low wind speeds, high relative humidities and limited intensity of solar radiation.
Emmaline Atherton, David Risk, Chelsea Fougère, Martin Lavoie, Alex Marshall, John Werring, James P. Williams, and Christina Minions
Atmos. Chem. Phys., 17, 12405–12420,Short summary
Methane is a potent greenhouse gas, and leaks from natural gas infrastructure are thought to be a significant emission source. We used a mobile survey method to measure GHGs near Canadian infrastructure. Our results show that ~ 47 % of active wells were emitting. Abandoned and aging wells were also associated with emissions. We estimate methane emissions from this development are just over 111 Mt year−1, which is more than previous government estimates, but less than similar studies in the US.
Huiting Mao, Dolly Hall, Zhuyun Ye, Ying Zhou, Dirk Felton, and Leiming Zhang
Atmos. Chem. Phys., 17, 11655–11671,Short summary
Mercury (Hg) is a global pollutant hazardous to human and ecosystem health, and its emission control is imperative. Anthropogenic mercury emissions have been reduced by 78 % in the United States from 1990 to 2014. However, no clearly defined trend was observed in Hg concentrations at urban locations such as the one in this study. This indicates that other factors may have dominated over anthropogenic emission control. The implications of this study could hence be highly policy relevant.
Xiufeng Yin, Shichang Kang, Benjamin de Foy, Zhiyuan Cong, Jiali Luo, Lang Zhang, Yaoming Ma, Guoshuai Zhang, Dipesh Rupakheti, and Qianggong Zhang
Atmos. Chem. Phys., 17, 11293–11311,Short summary
We presented 5-year surface ozone measurements at Nam Co in the inland Tibetan Plateau and made a synthesis comparison of diurnal and seasonal patterns on regional and hemispheric scales. Surface ozone at Nam Co is mainly dominated by natural processes and is less influenced by stratospheric intrusions and human activities than on the rim of the Tibetan Plateau. Ozone at Nam Co is representative of background that is valuable for studying ozone-related effects on large scales.
Bo Christiansen, Nis Jepsen, Rigel Kivi, Georg Hansen, Niels Larsen, and Ulrik Smith Korsholm
Atmos. Chem. Phys., 17, 9347–9364,Short summary
Ozone soundings in the troposphere from nine Arctic stations covering the period 1984–2014 have been analyzed. Stations with the best data coverage show a consistent and significant temporal variation with a maximum near 2005 followed by a decrease. Some significant changes are found in the annual cycle in agreement with the notion that the ozone summer maximum is appearing earlier in the year. Such changes in Arctic ozone in the free troposphere have not been reported before.
Thomas G. Bell, Sebastian Landwehr, Scott D. Miller, Warren J. de Bruyn, Adrian H. Callaghan, Brian Scanlon, Brian Ward, Mingxi Yang, and Eric S. Saltzman
Atmos. Chem. Phys., 17, 9019–9033,Short summary
The mechanisms that determine the air–sea exchange of gases such as carbon dioxide are not well understood. During a research cruise in the North Atlantic, we simultaneously measured the air–sea transfer of two gases with contrasting solubility over a range in wind and wave conditions. We compare the transfer of these gases to improve understanding of how bubbles from breaking waves may mediate air–sea gas fluxes.
Stuart N. Riddick, Sarah Connors, Andrew D. Robinson, Alistair J. Manning, Pippa S. D. Jones, David Lowry, Euan Nisbet, Robert L. Skelton, Grant Allen, Joseph Pitt, and Neil R. P. Harris
Atmos. Chem. Phys., 17, 7839–7851,Short summary
High methane mixing ratios occurred at our long-term measurement site. Isotopic measurements show the source is a landfill 7 km away; the emissions were estimated using three different approaches. The emission estimates made by near-source and middle-distance methods agree well for a period of intense observation. The estimate of the inverse modelling is similar to the labour-intensive middle-distance approach, which shows it can be used to identify point sources within an emission landscape.
Philippe Ricaud, Eric Bazile, Massimo del Guasta, Christian Lanconelli, Paolo Grigioni, and Achraf Mahjoub
Atmos. Chem. Phys., 17, 5221–5237,Short summary
The novelty of the paper is to combine a large set of measurements and meteorological models to study the genesis of thick cloud and diamond dust/ice fog (ice crystals) episodes above Dome C, Antarctica. The originality of the work is to attribute the presence of thick cloud and diamond dust/ice fog to advection and microphysical processes with oceanic and continental origin of air masses, respectively. Thick cloud episodes are reproduced by the models but not diamond dust/ice fog episode.
Dan Li, Bärbel Vogel, Jianchun Bian, Rolf Müller, Laura L. Pan, Gebhard Günther, Zhixuan Bai, Qian Li, Jinqiang Zhang, Qiujun Fan, and Holger Vömel
Atmos. Chem. Phys., 17, 4657–4672,Short summary
High-resolution ozone and water vapour profiles over Lhasa, China, were measured in August 2013. The correlations between ozone and water vapour profiles show a strong variability in the upper troposphere. These relationships were investigated using CLaMS trajectory calculations. The model results demonstrate that three tropical cyclones (Jebi, Utor, and Trami), occurring over the western Pacific, had a strong impact on the vertical structure of ozone and water vapour profiles.
Pavlos Kalabokas, Jens Hjorth, Gilles Foret, Gaëlle Dufour, Maxim Eremenko, Guillaume Siour, Juan Cuesta, and Matthias Beekmann
Atmos. Chem. Phys., 17, 3905–3928,Short summary
The main atmospheric mechanisms linked with spring surface ozone episodes over the western Mediterranean are examined. It comes out that high surface midday ozone values are usually linked with regional ozone episodes, which are strongly influenced by some specific meteorological conditions. The better understanding of the ozone variability in the lower troposphere and the boundary layer over the examined regions will help in the formulation of more effective policies in environment and climate.
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During 2006–2015, emissions of SO2, NOx, PM2.5 and PM10 saw an obvious downtrend. However, most emissions still have large reduction potential. On-road mobile sources and solvent use are the two key sources that should receive more effective control measures in GD. Also, controls measures on VOC and NH3 should be weighted since they still increased in 2006–2015. Since most control measures focused on PRD rather than non-PRD in GD, emissions in non-PRD were increasingly important.
During 2006–2015, emissions of SO2, NOx, PM2.5 and PM10 saw an obvious downtrend. However, most...