Abstract. Black carbon (BC) is known to have major impacts on both human health and climate. The populated megacity represents the most complex anthropogenic BC emissions where the sources and related impacts are very uncertain. This study provides source attribution and characterization of BC in the Beijing urban environment during the joint UK–China APHH (Air Pollution and Human Health) project, in both winter (November–December 2016) and summer (May–June 2017). The size-resolved mixing state of BC-containing particles was characterized by a single-particle soot photometer (SP2) and their mass spectra was measured by a soot particle aerosol mass spectrometer (SP-AMS). The refractory BC (rBC) mass loading was around a factor of 2 higher in winter relative to summer, and more variable coatings were present, likely as a result of additional surface emissions from the residential sector and favourable condensation in the cold season. The characteristics of the BC were relatively independent of air mass direction in summer, whereas in winter air masses from the Northern Plateau were considerably cleaner and contained less-coated and smaller BC, but the BC from the Southern Plateau had the largest core size and coatings. We compare two online source apportionment methods using simultaneous measurements made by the SP2, which measures physical properties of BC, and the chemical approach using the positive matrix factorization (PMF) of mass spectra from the SP-AMS for the first time. A method is proposed to isolate the BC from the transportation sector using a mode of small BC particles (core diameter Dc<0.18 µm and coating thickness ct < 50 nm). This mode of BC highly correlated with NOx concentration in both seasons (∼14 ng m−3 BC ppb−1 NOx) and corresponded with the morning traffic rush hour, contributing about 30 % and 40 % of the total rBC mass (35 % and 55 % in number) in winter and summer respectively. The BC from coal burning or biomass burning was characterized by moderate coatings (ct = 50–200 nm) contributing ∼20 %–25 % of rBC mass. Large uncoated BC particles (Dc>0.18 µm and ct < 50 nm) were more likely to be contributed by coal combustion, as these particles were not present in urban London. This mode was present in Beijing in both winter (∼30 %–40 % rBC mass) and summer (∼40 % rBC mass) but may be dominated by the residential and industrial sector respectively. The contribution of BC thickly coated with secondary species (ct > 200 nm) to the total rBC mass increased with pollution level in winter but was minor in summer. These large BC particles importantly enhanced the absorption efficiency at high pollution levels – in winter when PM1 > 100 µg m−3 or BC > 2 µg m−3, the absorption efficiency of BC increased by 25 %–70 %. The reduction of emissions of these large BC particles and the precursors of the associated secondary coating will be an effective way of mitigating the heating effect of BC in urban environments.
Abstract. Measurements of OH, HO2, complex RO2 (alkene- and aromatic-related RO2) and total RO2 radicals taken during the integrated Study of AIR Pollution PROcesses in Beijing (AIRPRO) campaign in central Beijing in the summer of 2017, alongside observations of OH reactivity, are presented. The concentrations of radicals were elevated, with OH reaching up to 2.8×107moleculecm-3, HO2 peaking at 1×109moleculecm-3 and the total RO2 concentration reaching 5.5×109moleculecm-3. OH reactivity (k(OH)) peaked at 89 s−1 during the night, with a minimum during the afternoon of ≈22s-1 on average. An experimental budget analysis, in which the rates of production and destruction of the radicals are compared, highlighted that although the sources and sinks of OH were balanced under high NO concentrations, the OH sinks exceeded the known sources (by 15 ppbv h−1) under the very low NO conditions (<0.5 ppbv) experienced in the afternoons, demonstrating a missing OH source consistent with previous studies under high volatile organic compound (VOC) emissions and low NO loadings. Under the highest NO mixing ratios (104 ppbv), the HO2 production rate exceeded the rate of destruction by ≈50ppbvh-1, whilst the rate of destruction of total RO2 exceeded the production by the same rate, indicating that the net propagation rate of RO2 to HO2 may be substantially slower than assumed. If just 10 % of the RO2 radicals propagate to HO2 upon reaction with NO, the HO2 and RO2 budgets could be closed at high NO, but at low NO this lower RO2 to HO2 propagation rate revealed a missing RO2 sink that was similar in magnitude to the missing OH source. A detailed box model that incorporated the latest Master Chemical Mechanism (MCM3.3.1) reproduced the observed OH concentrations well but over-predicted the observed HO2 under low concentrations of NO (<1 ppbv) and under-predicted RO2 (both the complex RO2 fraction and other RO2 types which we classify as simple RO2) most significantly at the highest NO concentrations. The model also under-predicted the observed k(OH) consistently by ≈10s-1 across all NOx levels, highlighting that the good agreement for OH was fortuitous due to a cancellation of missing OH source and sink terms in its budget. Including heterogeneous loss of HO2 to aerosol surfaces did reduce the modelled HO2 concentrations in line with the observations but only at NO mixing ratios <0.3 ppbv. The inclusion of Cl atoms, formed from the photolysis of nitryl chloride, enhanced the modelled RO2 concentration on several mornings when the Cl atom concentration was calculated to exceed 1×104atomscm-3 and could reconcile the modelled and measured RO2 concentrations at these times. However, on other mornings, when the Cl atom concentration was lower, large under-predictions in total RO2 remained. Furthermore, the inclusion of Cl atom chemistry did not enhance the modelled RO2 beyond the first few hours after sunrise and so was unable to resolve the modelled under-prediction in RO2 observed at other times of the day. Model scenarios, in which missing VOC reactivity was included as an additional reaction that converted OH to RO2, highlighted that the modelled OH, HO2 and RO2 concentrations were sensitive to the choice of RO2 product. The level of modelled to measured agreement for HO2 and RO2 (both complex and simple) could be improved if the missing OH reactivity formed a larger RO2 species that was able to undergo reaction with NO, followed by isomerisation reactions reforming other RO2 species, before eventually generating HO2. In this work an α-pinene-derived RO2 species was used as an example. In this simulation, consistent with the experimental budget analysis, the model underestimated the observed OH, indicating a missing OH source. The model uncertainty, with regards to the types of RO2 species present and the radicals they form upon reaction with NO (HO2 directly or another RO2 species), leads to over an order of magnitude less O3 production calculated from the predicted peroxy radicals than calculated from the observed peroxy radicals at the highest NO concentrations. This demonstrates the rate at which the larger RO2 species propagate to HO2, to another RO2 or indeed to OH needs to be understood to accurately simulate the rate of ozone production in environments such as Beijing, where large multifunctional VOCs are likely present.
Integrated Urban hydrometeorological, climate and environmental Services (IUS) is a WMO initiative to aid development of science-based services to support safe, healthy, resilient and climate friendly cities. Guidance for Integrated Urban Hydrometeorological, Climate and Environmental Services (Volume I) has been developed with the intent to provide an overview of the concept, methods and good practices for producing and providing these services to respond to the hazards across a range of time scales (weather to climate). This involves combining (dense) heterogeneous observation networks, high-resolution forecasts, multi-hazard early warning systems and climate services to assist cities in setting and implementing mitigation and adaptation strategies for the management and building of resilient and sustainable cities. IUS include research, evaluation and delivery with a wide participation from city governments, national hydrometeorological services, international organizations, universities, research institutions and private sector stakeholders. An overview of the IUS concept with key messages, examples of good practice and recommendations are provided. The research community will play an important role to: identify critical research challenges; provide impact forecasts and warnings; develop and deliver IUS internationally, and; support national and local communities in the implementation of IUS thereby contributing to the United Nations' Sustainable Development Goals at all scales. 2015-2030 (UNDRR, 2015) aims to substantially reduce impacts of disaster in terms of mortality, economic loss and damages, and disruption of basic services, while contributing to the mitigation of technological and security risks, through the provision of impact-based services (WMO, 2016). These services consider hazards, vulnerability and exposure. Governments, businesses and the public need to understand how the hydrometeorological hazard may affect their lives, livelihoods, property and economic activity in order to take appropriate actions. As weather, air quality, climate and the water cycle know no national boundaries, international cooperation at a global scale is essential to develop commensurate services and to reap the benefits from their application. The WMO, a United Nations Specialized Agency, provides the framework for such international cooperation. This intergovernmental organization's 193 member states and territories (called Members) are mainly concerned with issues at a national, regional and international J o u r n a l P r e -p r o o f Journal Pre-proof the Guidance (Vol. 1) for the broader scientific community and stakeholders. Following a background discussion (section 2), the IUS concepts are outlined (section 3). Results from surveys of urban experts and WMO members (section 4) are used to articulate the science and knowledge gaps (section 5) and to illustrate the lessons learnt and recommendations (section 6). This is followed by concluding remarks (section 7).J o u r n a l P r e -p r o o f Journal Pre-proof ...
The formation of isoprene nitrates (IsN) can lead to significant secondary organic aerosol (SOA) production and they can act as reservoirs of atmospheric nitrogen oxides. In this work, we estimate the rate of production of IsN from the reactions of isoprene with OH and NO3 radicals during the summertime in Beijing. While OH dominates the loss of isoprene during the day, NO3 plays an increasingly important role in the production of IsN from the early afternoon onwards. Unusually low NO concentrations during the afternoon resulted in NO3 mixing ratios of ca. 2 pptv at approximately 15:00, which we estimate to account for around a third of the total IsN production in the gas phase.Heterogeneous uptake of IsN produces nitrooxyorganosulfates (NOS). Two mononitrated NOS were correlated with particulate sulfate concentrations and appear to be formed from sequential NO3 and OH oxidation. Di-and trinitrated isoprene-related NOS, formed from multiple NO3 oxidation steps, peaked during the night. This work highlights that NO3 chemistry can play a key role in driving biogenic− anthropogenic interactive chemistry in Beijing with respect to the formation of IsN during both the day and night.
di saBatino, JunXia dou, daniel r. dreW, John M. edWards, JoaChiM fallMann, krzysztof fortuniak, JeMMa gornall, toBias groneMeier, Christos h. halios, denise hertWig, kohin hirano, alBert a. M. holtslag, zhiWen luo, gerald Mills, Makoto nakayoshi, kathy Pain, k. heinke sChlünzen, stefan sMith, lionel soulhaC, gert-Jan steeneveld, ting sun, natalie e theeuWes, david thoMson, JaMes a. voogt, helen C. Ward, zheng-tong Xie, and Jian zhong W ith the majority of people experiencing weather in urban areas, it is critical to understand cities, weather, and climate impacts. Increasing climate extremes (e.g., heat stress, air pollution, flash flooding) combined with the density of people means it is essential that city infrastructure and operations can withstand high-impact weather. Thus, there is a huge opportunity to mitigate climate change effects and provide healthier environments through design and planning to reduce the background climate and urban effects. However, our understanding of the underlying urban atmospheric processes are primarily derived from studies of separate aspects, rather than the complete, human-environment system. Air quality modeling has not been widely integrated with aerosol feedbacks on local climate, while few city-greening scenarios have tested the impacts on boundary layer pollutant dispersion or the carbon cycle. Building design guidelines have been developed without incorporating the impact of waste heat on local temperatures, which, in turn, determines building performance. Integration of such feedbacks is imperative as they define, rather than just modify, urban climate.There is an urgent need to link processes that people experience at street level (human scale) to processes at neighborhood, city, and regional scales. As these scales have traditionally been the focus for specialists in different fields, few observation and model systems cross these scales. However, understanding the interactions between these scales is critical for the design of future parametrizations ES261OCTOBER 2017 AMERICAN METEOROLOGICAL SOCIETY | and observation networks. Although models and observational methods are emerging that permit research into scale interactions [e.g., high-resolution numerical weather prediction (NWP), large-domain computational fluid dynamic (CFD) models, remote sensing, extensive sensor networks, vertical remote sensing], an integrated approach across methodologies is currently lacking.To tackle these scale interactions requires diverse skills from a wide range of research communities. This is a daunting challenge. However, improved understanding of urban atmospheric processes such as clouds and precipitation, heat transfer, and convection would enable improvements in urban system models to provide seamless hazard prediction at all time scales. Hence, an initial focus on the meteorological aspects of the research challenge may be a more manageable problem, even though the scope is still large. As such, it was identified that within the United Kingdom there is an urgent need to devel...
Abstract. We examine the street-scale variation of NOx, NO2, O3 and PM2.5 concentrations in Beijing during the Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-China) winter measurement campaign in November–December 2016. Simulations are performed using the urban air pollution dispersion and chemistry model ADMS-Urban and an explicit network of road source emissions. Two versions of the gridded Multi-resolution Emission Inventory for China (MEIC v1.3) are used: the standard MEIC v1.3 emissions and an optimised version, both at 3 km resolution. We construct a new traffic emissions inventory by apportioning the transport sector onto a detailed spatial road map. Agreement between mean simulated and measured pollutant concentrations from Beijing's air quality monitoring network and the Institute of Atmospheric Physics (IAP) field site is improved when using the optimised emissions inventory. The inclusion of fast NOx–O3 chemistry and explicit traffic emissions enables the sharp concentration gradients adjacent to major roads to be resolved with the model. However, NO2 concentrations are overestimated close to roads, likely due to the assumption of uniform traffic activity across the study domain. Differences between measured and simulated diurnal NO2 cycles suggest that an additional evening NOx emission source, likely related to heavy-duty diesel trucks, is not fully accounted for in the emissions inventory. Overestimates in simulated early evening NO2 are reduced by delaying the formation of stable boundary layer conditions in the model to replicate Beijing's urban heat island. The simulated campaign period mean PM2.5 concentration range across the monitoring network (∼15 µg m−3) is much lower than the measured range (∼40 µg m−3). This is likely a consequence of insufficient PM2.5 emissions and spatial variability, neglect of explicit point sources, and assumption of a homogeneous background PM2.5 level. Sensitivity studies highlight that the use of explicit road source emissions, modified diurnal emission profiles, and inclusion of urban heat island effects permit closer agreement between simulated and measured NO2 concentrations. This work lays the foundations for future studies of human exposure to ambient air pollution across complex urban areas, with the APHH-China campaign measurements providing a valuable means of evaluating the impact of key processes on street-scale air quality.
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