Atmospheric deposition of particulate organic nitrogen (ONp) is a significant process in the global nitrogen cycle and may be pivotally important for N-limited ecosystems. However, past models largely overlooked the spatial and chemical inhomogeneity of atmospheric ONp and were thus deficient in assessing global ONp impacts. We constructed a comprehensive global model of atmospheric gaseous and particulate organic nitrogen (ON), including the latest knowledge on emissions and secondary formations. Using this model, we simulated global atmospheric ONp abundances consistent with observations. Our estimated global atmospheric ON deposition was 26 Tg N yr-1, predominantly in the form of ONp (23 Tg N yr-1) and mostly from wildfires (37%), oceans (22%) and aqueous productions (17%). Globally, ONp contributed as much as 40% to 80% of the total N deposition downwind of biomass-burning regions. Atmospheric ONp deposition thus constituted the dominant external N supply to the N-limited boreal forests, tundras and the Arctic Ocean, and its importance may be amplified in a future warming climate.

Nitrogen is a significant element that constitutes ambient organic aerosol. Individual N-containing organic molecules are known to have both natural and anthropogenic sources and implicated in a wide-ranging health and environmental effects. Yet, unlike carbon (C), the total quantity of aerosol organic nitrogen (ON) remains largely unquantified, hindering a quantitative understanding of their major sources and impacts. Here, aerosol ON is quantitatively surveyed in hundreds of aerosol filter samples collected from sites of varying urban influence in China using our recently developed method that permits simple, and yet sensitive, simultaneous detection of inorganic and organic nitrogen. Annual average ON concentration was in the range of 0.4–1.4 μg N m −3 , representing 17–31% of aerosol total nitrogen. Monte Carlo simulations constrained by paired ON and OC measurements suggest N-containing organic molecules contributed typically 37–50%, with a 95% confidence interval of [12%, 94%], to ambient organic aerosols. Source apportionment analysis reveals that biomass burning and secondary formation are dominant ON sources, accounting for 21–24% and ~ 30% of ON, respectively. Primary biological aerosol is also a significant source of ON (7–18%), with its contribution more prominent in non-urban atmospheres. The results provide the quantitative data for the extent of presence of organic nitrogenous aerosol and the origin of their major sources. Such data, we anticipate, would bring forth a breakthrough in our ability to describe and model organic aerosols and to assess their environmental impacts, such as atmospheric nitrogen nutrient inputs to ecosystems.

The evaporative emissions of anthropogenic volatile organic compounds (AVOCs) are sensitive to ambient temperature. This sensitivity forms an air pollution-meteorology connection that has not been assessed on a regional scale. We parametrized the temperature dependence of evaporative AVOC fluxes in a regional air quality model and evaluated the impacts on surface ozone in the Beijing-Tianjin-Hebei (BTH) area of China during the summer of 2017. The temperature dependency of AVOC emissions drove an enhanced simulated ozone-temperature sensitivity of 1.0 to 1.8 μg m-3 K-1, comparable to the simulated ozone-temperature sensitivity driven by the temperature dependency of biogenic VOC emissions (1.7 to 2.4 μg m-3 K-1). Ozone enhancements driven by temperature-induced AVOC increases were localized to their point of emission and were relatively more important in urban areas than in rural regions. The inclusion of the temperature-dependent AVOC emissions in our model improved the simulated ozone-temperature sensitivities on days of ozone exceedance. Our results demonstrated the importance of temperature-dependent AVOC emissions on surface ozone pollution and its heretofore unrepresented role in air pollution-meteorology interactions.

露天生物质燃烧是温室气体(CO2、CH4、N2O)的重要排放源之一,这些排放可影响本地、区域和全球的大气化学和气候变化,并带来一系列生态环境问题,进而对人类及其他生物的生存环境产生影响.本研究采用卫星火点排放清单(FINN),对2010-2019年中国露天生物质燃烧温室气体排放进行研究,并分析秸秆禁燃政策对温室气体排放的影响,对后续秸秆禁燃政策的制定具有重要参考价值.结果表明,我国2010-2019年平均年温室气体排放量为1.53×108t(将CH4和N2O的温室效应换算为同等效应的CO2当量单位),总体呈波动性下降趋势.温室气体排放量最大的植被类型是森林(7.43×107t)和农作物(3.19×107t),分别占总排放量的48.7％和20.9％.从月分布来看,露天生物质燃烧排放的温室气体集中在2-6月,3月是高峰值.从空间分布上看,排放主要集中在华南、西南和华东地区,占总排放量的72.9％.从2013年以来,秸秆禁燃政策的加强在一定程度上降低了露天农作物秸秆燃烧排放的温室气体和PM2.5.从变化量看,28个省份实现了秸秆燃烧排放的温室气体与PM2.5同步下降.

Inorganic nitrogen (IN) and organic nitrogen ( ON) molecules constitute a significant part of atmospheric aerosol. Unlike IN, the total ON quantity remains largely unquantified due to a lack of a simple and direct measurement method. This analytical deficiency hinders the quantitative assessment of the various environmental and health effect impacts by aerosol ON. In this work, we developed an analyzer system that utilizes programmed thermal evolution of carbonaceous and nitrogenous aerosols and chemiluminescence detection coupled with the multivariate curve resolution data treatment to achieve simultaneous quantification of IN and ON. The system is capable of detecting IN and ON as low as 96 ng N per sample on a small filter aliquot (1 cm(2)) without any pretreatment. This method breakthrough opens the door to quantifying an important pool of aerosol N that was analytically inaccessible in the past and holds the promise to quantifying IN and ON in other environmental samples. As a demonstration, quantification of aerosol ON at an urban site in Hong Kong, China, in samples spanning over a year reveals ON constituting a significant fraction (9-52%) of the total aerosol nitrogen and having major source origins in both secondary formation and primary emissions.

The outbreak of coronavirus (COVID-19) has forced China to lockdown many cities and restrict transportation, industrial, and social activities. This provides a great opportunity to look at the impacts of pandemic quarantine on air quality and premature death due to exposure to air pollution. In this study, we applied the difference-in-differences (DID) model to quantify the casual impacts of COVID-19 lockdown on air quality at 278 cities across China. A widely used exposure-response function was further utilized to estimate the short-term health impacts associated with changes in PM2.5 due to lockdown. Results show that lockdown has caused drastic reduction in air pollution level in terms of all criteria pollutants except ozone. On average, concentrations of PM2.5, PM10, NO2, SO2 and CO are estimated to drop by 14.3 μg/m3, 22.2 μg/m3, 17.7 μg/m3, 2.9 μg/m3, and 0.18 mg/m3 as the result of lockdown. Cities with more confirmed cases of COVID-19 are related to stronger responses in air quality, despite that similar lockdown measures were implemented by the local governments. The improvement of air quality caused by COVID-19 lockdown in northern cities is found to be smaller than that of southern cities. Avoided premature death associated with PM2.5 exposures over the 278 cities was estimated to be 50.8 thousand. Our results re-emphasize the effectiveness of emission controls on air quality and associated health impacts. The high cost of lockdown, still high level of air pollution during lockdown and smaller effects in northern cities implies that source-specific mitigation policies are needed for continuous and sustainable reduction of air pollution.

Levoglucosan has been widely used to quantitatively assess biomass burning's contribution to ambient aerosols, but previous such assessments have not accounted for levoglucosan's degradation in the atmosphere. We develop the first global simulation of atmospheric levoglucosan, explicitly accounting for its chemical degradation, to evaluate the impacts on levoglucosan's use in quantitative aerosol source apportionment. Levoglucosan is emitted into the atmosphere from the burning of plant matter in open fires (1.7 Tg yr-1) and as biofuels (2.1 Tg yr-1). Sinks of atmospheric levoglucosan include aqueous-phase oxidation (2.9 Tg yr-1), heterogeneous oxidation (0.16 Tg yr-1), gas-phase oxidation (1.4 × 10-4 Tg yr-1), and dry and wet deposition (0.27 and 0.43 Tg yr -1). The global atmospheric burden of levoglucosan is 19 Gg with a lifetime of 1.8 days. Observations show a sharp decline in levoglucosan's concentrations and its relative abundance to organic carbon aerosol (OC) and particulate K+ from near-source to remote sites. We show that such features can only be reproduced when levoglucosan's chemical degradation is included in the model. Using model results, we develop statistical parametrizations to account for the atmospheric degradation in levoglucosan measurements, improving their use for quantitative aerosol source apportionment.

The outbreak of COVID-19 in China has led to massive lockdowns in order to reduce the spread of the epidemic and control human-to-human transmission. Subsequent reductions in various anthropogenic activities have led to improved air quality during the lockdown. In this study, we apply a widely used exposure-response function to estimate the short-term health impacts associated with PM2.5 changes over the Yangtze River Delta (YRD) region due to COVID-19 lockdown. Concentrations of PM2.5 during lockdown period reduced by 22.9% to 54.0% compared to pre-lockdown level. Estimated PM2.5-related daily premature mortality during lockdown period is 895 (95% confidential interval: 637-1,081), which is 43.3% lower than pre-lockdown period and 46.5% lower compared with averages of 2017-2019. According to our calculation, total number of avoided premature death aassociated with PM2.5 reduction during the lockdown is estimated to be 42.4 thousand over the YRD region, with Shanghai, Wenzhou, Suzhou (Jiangsu province), Nanjing, and Nantong being the top five cities with largest health benefits. Avoided premature mortality is mostly contributed by reduced death associated with stroke (16.9 thousand, accounting for 40.0%), ischemic heart disease (14.0 thousand, 33.2%), and chronic obstructive pulmonary disease (7.6 thousand, 18.0%). Our calculations do not support or advocate any idea that pandemics produce a positive note to community health. We simply present health benefits from air pollution improvement due to large emission reductions from lowered human and industrial activities. Our results show that continuous efforts to improve air quality are essential to protect public health, especially over city-clusters with dense population.