Atmospheric oxidation capacity is the basis for converting freshly emitted substances into secondary products and is dominated by reactions involving hydroxyl radicals (OH) during daytime. In this study, we present in situ measurements of ROx radical (hydroxy OH, hydroperoxy HO2, and organic peroxy RO2) precursors and products; the measurements are carried out in four Chinese megacities (Beijing, Shanghai, Guangzhou, and Chongqing) during photochemically polluted seasons. The atmospheric oxidation capacity is evaluated using an observation-based model and radical chemistry precursor measurements as input. The radical budget analysis illustrates the importance of HONO and HCHO photolysis, which account for ∼50 % of the total primary radical sources. The radical propagation is efficient due to abundant NO in urban environments. Hence, the production rate of secondary pollutants, that is, ozone (and fine-particle precursors (H2SO4, HNO3, and extremely low volatility organic compounds, ELVOCs) is rapid, resulting in secondary air pollution. The ozone budget demonstrates its high production in urban areas; also, its rapid transport to downwind areas results in rapid increase in local ozone concentrations. The O3–NOx–VOC (volatile organic compound) sensitivity tests show that ozone production is VOC-limited and that alkenes and aromatics should be mitigated first for ozone pollution control in the four studied megacities. In contrast, NOx emission control (that is, a decrease in NOx) leads to more severe ozone pollution. With respect to fine-particle pollution, the role of the HNO3–NO3 partitioning system is investigated using a thermal dynamic model (ISORROPIA 2). Under high relative humidity (RH) and ammonia-rich conditions, nitric acid converts into nitrates. This study highlights the efficient radical chemistry that maintains the atmospheric oxidation capacity in Chinese megacities and results in secondary pollution characterized by ozone and fine particles.
Background: The ongoing outbreak of COVID-19 has spread rapidly and sparked global concern. While the transmission of SARS-CoV-2 through human respiratory droplets and contact with infected persons is clear, the aerosol transmission of SARS-CoV-2 has been little studied. Methods: Thirty-five aerosol samples of three different types (total suspended particle, size segregated and deposition aerosol) were collected in Patient Areas (PAA) and Medical Staff Areas (MSA) of Renmin Hospital of Wuhan University (Renmin) and Wuchang Fangcang Field Hospital (Fangcang), and Public Areas (PUA) in Wuhan, China during COVID-19 outbreak. A robust droplet digital polymerase chain reaction (ddPCR) method was employed to quantitate the viral SARS-CoV-2 RNA genome and determine aerosol RNA concentration. Results: The ICU, CCU and general patient rooms inside Renmin, patient hall inside Fangcang had undetectable or low airborne SARS-CoV-2 concentration but deposition samples inside ICU and air sample in Fangcang patient toilet tested positive. The airborne SARS-CoV-2 in Fangcang MSA had bimodal distribution with higher concentration than those in Renmin during the outbreak but turned negative after patients number reduced and rigorous sanitization implemented. PUA had undetectable airborne SARS-CoV-2 concentration but obviously increased with accumulating crowd flow. Conclusions: Room ventilation, open space, proper use and disinfection of toilet can effectively limit aerosol transmission of SARS-CoV-2. Gathering of crowds with asymptomatic carriers is a potential source of airborne SARS-CoV-2. The virus aerosol deposition on protective apparel or floor surface and their subsequent resuspension is a potential transmission pathway and effective sanitization is critical in minimizing aerosol transmission of SARS-CoV-2.
Growing shipping activities in port areas have generated negative impacts on climate, air quality and human health. To better evaluate the environmental impact of ship emissions, an experimental characterization of air pollution from ships was conducted in Shanghai Port in the summer of 2016. The ambient concentrations of gaseous NO, NO2, SO2 and O3 in addition to fine particulate matter concentrations (PM2.5), particle size distributions and the chemical composition of individual particles from ship emission were continuously monitored for 3 months. Ship emission plumes were visible at the port site in terms of clear peaks in the gaseous species and particulate matter concentrations. The SO2 and vanadium particle numbers were found to correlate best with ship emissions in Shanghai Port. Single-particle data showed that ship emission particles at the port site mainly concentrated in a smaller size range (<0.4 µm), where their number contributions were more important than their mass contributions to ambient particulate matter. The composition of ship emission particles at the port site suggested that they were mostly freshly emitted particles: their mass spectra were dominated by peaks of sulfate, elemental carbon (EC), and trace metals such as V, Ni, Fe and Ca, in addition to displaying very low nitrate signals. The gaseous NOx composition in some cases of plumes showed evidence of atmospheric transformation by ambient O3, which subsequently resulted in O3 depletion in the area. Quantitative estimations in this study showed that ship emissions contributed 36.4 % to SO2, 0.7 % to NO, 5.1 % to NO2, −0.9 % to O3, 5.9 % to PM2.5 and 49.5 % to vanadium particles in the port region if land-based emissions were included, and 57.2 % to SO2, 71.9 % to NO, 30.4 % to NO2, −16.6 % to O3, 27.6 % to PM2.5 and 77.0 % to vanadium particles if land-based emissions were excluded.
The Yangtze River Delta (YRD) and the megacity of Shanghai are host to one of the busiest port clusters in the world; the region also suffers from high levels of air pollution. The goal of this study was to estimate the contributions of shipping to regional emissions, air quality, and population exposure and to characterize the importance of the geographic spatiality of shipping lanes and different types of ship-related sources for the baseline year of 2015, which was prior to the implementation of China's Domestic Emission Control Areas (DECAs) in 2016. The WRF-CMAQ model, which combines the Weather Research and Forecasting model (WRF) and the Community Multi-scale Air Quality (CMAQ) model, was used to simulate the influence of coastal and inland-water shipping, port emissions and ship-related cargo transport on air quality and on the population-weighted concentrations (which is a measure of human exposure). Our results showed that the impact of shipping on air quality in the YRD was primarily attributable to shipping emissions within 12 NM (nautical miles) of shore, but emissions coming from the coastal area between 24 and 96 NM still contributed substantially to ship-related PM2.5 concentrations in the YRD. The overall contribution of ships to the PM2.5 concentration in the YRD could reach 4.62 µg m−3 in summer when monsoon winds transport shipping emissions onshore. In Shanghai city, inland-water going ships were major contributors (40 %–80 %) to the shipping impact on urban air quality. Given the proximity of inland-water ships to the urban populations of Shanghai, the emissions of inland-water ships contributed more to population-weighted concentrations. These research results provide scientific evidence to inform policies for controlling future shipping emissions; in particular, in the YRD region, expanding the boundary of 12 NM from shore in China's current DECA policy to around 100 NM from shore would include most of shipping emissions affecting air pollutant exposure, and stricter fuel standards could be considered for the ships on inland rivers and other waterways close to residential regions.
Nitrate aerosol plays an increasingly important role in wintertime haze pollution in China. Despite intensive research on wintertime nitrate chemistry in recent years, quantitative constraints on the formation mechanisms of nitrate aerosol in the Yangtze River Delta (YRD), one of the most developed and densely populated regions in eastern China, remain inadequate. In this study, we identify the major nitrate formation pathways and their key controlling factors during the winter haze pollution period in the eastern YRD using 2-year (2018–2019) field observations and detailed observation-constrained model simulations. We find that the high atmospheric oxidation capacity, coupled with high aerosol liquid water content (ALWC), made both the heterogeneous hydrolysis of dinitrogen pentoxide (N2O5) and the gas-phase OH oxidation of nitrogen dioxide (NO2) important pathways for wintertime nitrate formation in this region, with contribution percentages of 69 % and 29 % in urban areas and 63 % and 35 % in suburban areas during the haze pollution episodes, respectively. We further find that the gas-to-particle partitioning of nitric acid (HNO3) was very efficient so that the rate-determining step in the overall formation process of nitrate aerosol was the oxidation of NOx to HNO3 through both heterogeneous and gas-phase processes. The atmospheric oxidation capacity (i.e., the availability of O3 and OH radicals) was the key factor controlling the production rate of HNO3 from both processes. During the COVID-19 lockdown (January–February 2020), the enhanced atmospheric oxidation capacity greatly promoted the oxidation of NOx to nitrate and hence weakened the response of nitrate aerosol to the emission reductions in urban areas. Our study sheds light on the detailed formation mechanisms of wintertime nitrate aerosol in the eastern YRD and highlights the demand for the synergetic regulation of atmospheric oxidation capacity and NOx emissions to mitigate wintertime nitrate and haze pollution in eastern China.