Global variability in atmospheric new particle formation mechanisms.

A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric aerosol particles are initially formed1,2. Although new particle formation (NPF) mechanisms have been described at specific sites3-6, in most regions, such mechanisms remain uncertain to a large extent because of the limited ability of atmospheric models to simulate critical NPF processes1,7. Here we synthesize molecular-level experiments to develop comprehensive representations of 11 NPF mechanisms and the complex chemical transformation of precursor gases in a fully coupled global climate model. Combined simulations and observations show that the dominant NPF mechanisms are distinct worldwide and vary with region and altitude. Previously neglected or underrepresented mechanisms involving organics, amines, iodine oxoacids and HNO3 probably dominate NPF in most regions with high concentrations of aerosols or large aerosol radiative forcing; such regions include oceanic and human-polluted continental boundary layers, as well as the upper troposphere over rainforests and Asian monsoon regions. These underrepresented mechanisms also play notable roles in other areas, such as the upper troposphere of the Pacific and Atlantic oceans. Accordingly, NPF accounts for different fractions (10-80%) of the nuclei on which cloud forms at 0.5% supersaturation over various regions in the lower troposphere. The comprehensive simulation of global NPF mechanisms can help improve estimation and source attribution of the climate effects of aerosols.

Anthropogenic short-lived halogens increase human exposure to mercury contamination due to enhanced mercury oxidation over continents.

Mercury (Hg) is a contaminant of global concern, and an accurate understanding of its atmospheric fate is needed to assess its risks to humans and ecosystem health. Atmospheric oxidation of Hg is key to the deposition of this toxic metal to the Earth's surface. Short-lived halogens (SLHs) can provide halogen radicals to directly oxidize Hg and perturb the budget of other Hg oxidants (e.g., OH and O3). In addition to known ocean emissions of halogens, recent observational evidence has revealed abundant anthropogenic emissions of SLHs over continental areas. However, the impacts of anthropogenic SLHs emissions on the atmospheric fate of Hg and human exposure to Hg contamination remain unknown. Here, we show that the inclusion of anthropogenic SLHs substantially increased local Hg oxidation and, consequently, deposition in/near Hg continental source regions by up to 20%, thereby decreasing Hg export from source regions to clean environments. Our modeling results indicated that the inclusion of anthropogenic SLHs can lead to higher Hg exposure in/near Hg source regions than estimated in previous assessments, e.g., with increases of 8.7% and 7.5% in China and India, respectively, consequently leading to higher Hg-related human health risks. These results highlight the urgent need for policymakers to reduce local Hg and SLHs emissions. We conclude that the substantial impacts of anthropogenic SLHs emissions should be included in model assessments of the Hg budget and associated health risks at local and global scales.

Spatially and Temporally Differentiated NOx and VOCs Emission Abatement Could Effectively Gain O3-Related Health Benefits.

The increasing level of O3 pollution in China significantly exacerbates the long-term O3 health damage, and an optimized health-oriented strategy for NOx and VOCs emission abatement is needed. Here, we developed an integrated evaluation and optimization system for the O3 control strategy by merging a response surface model for the O3-related mortality and an optimization module. Applying this system to the Yangtze River Delta (YRD), we evaluated driving factors for mortality changes from 2013 to 2017, quantified spatial and temporal O3-related mortality responses to precursor emission abatement, and optimized a health-oriented control strategy. Results indicate that insufficient NOx emission abatement combined with deficient VOCs control from 2013 to 2017 aggravated O3-related mortality, particularly during spring and autumn. Northern YRD should promote VOCs control due to higher VOC-limited characteristics, whereas fastening NOx emission abatement is more favorable in southern YRD. Moreover, promotion of NOx mitigation in late spring and summer and facilitating VOCs control in spring and autumn could further reduce O3-related mortality by nearly 10% compared to the control strategy without seasonal differences. These findings highlight that a spatially and temporally differentiated NOx and VOCs emission control strategy could gain more O3-related health benefits, offering valuable insights to regions with severe ozone pollution all over the world.

Rapid hydrolysis of NO2 at High Ionic Strengths of Deliquesced Aerosol Particles.

Nitrogen dioxide (NO2) hydrolysis in deliquesced aerosol particles forms nitrous acid and nitrate and thus impacts air quality, climate, and the nitrogen cycle. Traditionally, it is considered to proceed far too slowly in the atmosphere. However, the significance of this process is highly uncertain because kinetic studies have only been made in dilute aqueous solutions but not under high ionic strength conditions of the aerosol particles. Here, we use laboratory experiments, air quality models, and field measurements to examine the effect of the ionic strength on the reaction kinetics of NO2 hydrolysis. We find that high ionic strengths (I) enhance the reaction rate constants (kI) by more than an order of magnitude compared to that at infinite dilution (kI=0), yielding log10(kI/kI=0) = 0.04I or rate enhancement factor = 100.04I. A state-of-the-art air quality model shows that the enhanced NO2 hydrolysis reduces the negative bias in the simulated concentrations of nitrous acid by 28% on average when compared to field observations over the North China Plain. Rapid NO2 hydrolysis also enhances the levels of nitrous acid in other polluted regions such as North India and further promotes atmospheric oxidation capacity. This study highlights the need to evaluate various reaction kinetics of atmospheric aerosols with high ionic strengths.

Fostering a Holistic Understanding of the Full Volatility Spectrum of Organic Compounds from Benzene Series Precursors through Mechanistic Modeling.

A comprehensive understanding of the full volatility spectrum of organic oxidation products from the benzene series precursors is important to quantify the air quality and climate effects of secondary organic aerosol (SOA) and new particle formation (NPF). However, current models fail to capture the full volatility spectrum due to the absence of important reaction pathways. Here, we develop a novel unified model framework, the integrated two-dimensional volatility basis set (I2D-VBS), to simulate the full volatility spectrum of products from benzene series precursors by simultaneously representing first-generational oxidation, multigenerational aging, autoxidation, dimerization, nitrate formation, etc. The model successfully reproduces the volatility and O/C distributions of oxygenated organic molecules (OOMs) as well as the concentrations and the O/C of SOA over wide-ranging experimental conditions. In typical urban environments, autoxidation and multigenerational oxidation are the two main pathways for the formation of OOMs and SOA with similar contributions, but autoxidation contributes more to low-volatility products. NOx can reduce about two-thirds of OOMs and SOA, and most of the extremely low-volatility products compared to clean conditions, by suppressing dimerization and autoxidation. The I2D-VBS facilitates a holistic understanding of full volatility product formation, which helps fill the large gap in the predictions of organic NPF, particle growth, and SOA formation.

Modeling the Formation of Organic Compounds across Full Volatility Ranges and Their Contribution to Nanoparticle Growth in a Polluted Atmosphere.

Nanoparticle growth influences atmospheric particles' climatic effects, and it is largely driven by low-volatility organic vapors. However, the magnitude and mechanism of organics' contribution to nanoparticle growth in polluted environments remain unclear because current observations and models cannot capture organics across full volatility ranges or track their formation chemistry. Here, we develop a mechanistic model that characterizes the full volatility spectrum of organic vapors and their contributions to nanoparticle growth by coupling advanced organic oxidation modeling and kinetic gas-particle partitioning. The model is applied to Nanjing, a typical polluted city, and it effectively captures the volatility distribution of low-volatility organics (with saturation vapor concentrations <0.3 µg/m3), thus accurately reproducing growth rates (GRs), with a 4.91% normalized mean bias. Simulations indicate that as particles grow from 4 to 40 nm, the relative fractions of GRs attributable to organics increase from 59 to 86%, with the remaining contribution from H2SO4 and its clusters. Aromatics contribute much to condensable organic vapors (∼37%), especially low-volatility vapors (∼61%), thus contributing the most to GRs (32-46%) as 4-40 nm particles grow. Alkanes also contribute 19-35% of GRs, while biogenic volatile organic compounds contribute minimally (<13%). Our model helps assess the climatic impacts of particles and predict future changes.

High-uniformity and high-performance waveguide Ge photodetectors for the O and C bands.

This paper presents the test results for high-performance and high-uniformity waveguide silicon-based germanium (Ge) photodetectors (PDs) for the O band and C band. Both wafer-scale and chip-scale test results are provided. The fabricated lateral p-i-n (LPIN) PDs exhibit a responsivity of 0.97 A/W at a bias of -2V, a bandwidth of 60 GHz, and a no-return-to-zero (NRZ) eye diagram rate of 53.125 Gb/s. Additionally, an average dark current of 22.4 nA was obtained in the vertical p-i-n (VPIN) PDs at -2V by optimizing the doping process. The device can reach an average responsivity of 0.9 A/W in the O band. The standard deviation in a wafer with a dark current and responsivity is as low as 7.77 nA and 0.03 A/W at -2V, respectively.

Combined solar power and storage as cost-competitive and grid-compatible supply for China's future carbon-neutral electricity system.

As the world's largest CO2 emitter, China's ability to decarbonize its energy system strongly affects the prospect of achieving the 1.5 °C limit in global, average surface-temperature rise. Understanding technically feasible, cost-competitive, and grid-compatible solar photovoltaic (PV) power potentials spatiotemporally is critical for China's future energy pathway. This study develops an integrated model to evaluate the spatiotemporal evolution of the technology-economic-grid PV potentials in China during 2020 to 2060 under the assumption of continued cost degression in line with the trends of the past decade. The model considers the spatialized technical constraints, up-to-date economic parameters, and dynamic hourly interactions with the power grid. In contrast to the PV production of 0.26 PWh in 2020, results suggest that China's technical potential will increase from 99.2 PWh in 2020 to 146.1 PWh in 2060 along with technical advances, and the national average power price could decrease from 4.9 to 0.4 US cents/kWh during the same period. About 78.6% (79.7 PWh) of China's technical potential will realize price parity to coal-fired power in 2021, with price parity achieved nationwide by 2023. The cost advantage of solar PV allows for coupling with storage to generate cost-competitive and grid-compatible electricity. The combined systems potentially could supply 7.2 PWh of grid-compatible electricity in 2060 to meet 43.2% of the country's electricity demand at a price below 2.5 US cents/kWh. The findings highlight a crucial energy transition point, not only for China but for other countries, at which combined solar power and storage systems become a cheaper alternative to coal-fired electricity and a more grid-compatible option.

Chemical characteristics of long-term acid rain and its impact on lake water chemistry: A case study in Southwest China.

The chemical composition of acid rain and its impact on lake water chemistry in Chongqing, China, from 2000 to 2020 were studied in this study. The regional acid rain intensity is affected jointly by the acid gas emissions and the neutralization of alkaline substances. The pH of precipitation experienced three stages of fluctuating decline, continuous improvement, and a slight correction. Precipitation pH showed inflection points in 2010, mainly due to the total control actions of SO2 and NOx implemented in 2011. The total ion concentrations in rural areas and urban areas were 489.08 µeq/L and 618.57 µeq/L, respectively. The top four ions were SO42-, Ca2+, NH4+ and NO3-, which accounted for more than 90% of the total ion concentration, indicating the anthropogenic effects. Before 2010, SO42- fluctuated greatly while NO3- continued to rise; however, after 2010, both SO42- and NO3- began to decline rapidly, with the rates of -12.03 µeq/(L·year) and -4.11 µeq/(L·year). Because the decline rate of SO42- was 2.91 times that of NO3-, the regional acid rain has changed from sulfuric acid rain to mixed sulfuric and nitric acid rain. The lake water is weakly acidic, with an average pH of 5.86, and the acidification frequency is 30.00%. Acidification of lake water is jointly affected by acid deposition and acid neutralization capacity of lake water. Acid deposition has a profound impact on water acidification, and nitrogen (N) deposition, especially reduced N deposition, should be the focus of future research.

PIC-integrable high-responsivity germanium waveguide photodetector in the C + L band.

We report the demonstration of a germanium waveguide p-i-n photodetector (PD) for the C + L band light detection. Tensile strain is transferred into the germanium layer using a SiN stressor on top surface of the germanium. The simulation and experimental results show that the trenches must be formed around the device, so that the strain can be transferred effectively. The device exhibits an almost flat responsivity with respect to the wavelength range from 1510 nm to 1630 nm, and high responsivity of over 1.1 A/W is achieved at 1625 nm. The frequency response measurement reveals that a high 3 dB bandwidth (f3dB) of over 50 GHz can be obtained. The realization of the photonic-integrated circuits (PIC)-integrable waveguide Ge PDs paves the way for future telecom applications in the C + L band.

Tracking Carbon Flows from Coal Mines to Electricity Users in China Using an Ensemble Model.

Accurately tracking carbon flows is crucial for preventing carbon leakage and allocating responsibility for reducing CO2eq emissions. In this study, we developed an ensemble model to effectively track carbon flows within China's power system. Our approach integrates coal quality tests, individual power plant datasets, a dynamic material-energy flow analysis model, and an extended version of an interconnected power grid model that incorporates transmission and distribution (T&D) losses. Our results not only provide accurate quantification of unit-based CO2eq emissions based on coal quality data but also enable the assessment of emissions attributed to T&D losses and emission shifts resulting from interprovincial coal and electricity trade. Remarkably, for CO2eq emissions from coal-fired units, the disparity between the guideline and our study can be as high as [-95%, 287%]. We identify Guangdong, Hebei, Jiangsu, and Zhejiang provinces as the major importers of both coal and electricity, responsible for transferring nearly half of their user-based emissions to coal and power bases. Significantly, T&D losses, often overlooked, contribute to 15-20% of provincial emissions at the user side. Our findings emphasize the necessity of up-to-date life cycle emissions and spatial carbon shifts in effectively allocating emission reduction responsibilities from the national level to provinces.

Mortality Burden of Cardiovascular Disease Attributable to Ozone in China: 2019 vs 2050.

Due to a combination of lifestyle risk factors, the burden of cardiovascular disease (CVD) has been increasing in China, affecting an estimated 330 million people. Environmental risk factors can exacerbate these risks or independently contribute to CVD. Ozone is an overlooked and invisible risk factor, and it plays a significant role in the development of CVD. Our study provides a novel quantification of the ozone-attributable CVD mortality burden based on daily maximum 8-h average ozone concentration during May to October (6mDMA8) in Chinese adults in 2050, projected under Shared Socioeconomic Pathways 585 and 126, and using the updated WHO air quality guideline level. The study also considers the contributions made by changes in ozone exposure, population aging, population size, and baseline death rates of CVD between 2019 and 2050. While adopting a sustainable and green pathway (SSP 126) can reduce the projected magnitude of premature CVD deaths to 359,200 in 2050, it may not be sufficient to reduce the CVD mortality burden significantly. Therefore, it is crucial to implement strategies for stricter ozone control and reducing the baseline death rate of CVD to mitigate the impacts of ozone on Chinese adults.

Extreme Emission Reduction Requirements for China to Achieve World Health Organization Global Air Quality Guidelines.

A big gap exists between current air quality in China and the World Health Organization (WHO) global air quality guidelines (AQG) released in 2021. Previous studies on air pollution control have focused on emission reduction demand in China but ignored the influence of transboundary pollution, which has been proven to have a significant impact on air quality in China. Here, we develop an emission-concentration response surface model coupled with transboundary pollution to quantify the emission reduction demand for China to achieve WHO AQG. China cannot achieve WHO AQG by its own emission reduction for high transboundary pollution of both PM2.5 and O3. Reducing transboundary pollution will loosen the reduction demand for NH3 and VOCs emissions in China. However, to meet 10 µg·m-3 for PM2.5 and 60 µg·m-3 for peak season O3, China still needs to reduce its emissions of SO2, NOx, NH3, VOCs, and primary PM2.5 by more than 95, 95, 76, 62, and 96% respectively, on the basis of 2015. We highlight that both extreme emission reduction in China and great efforts in addressing transboundary air pollution are crucial to reach WHO AQG.

Identification and Parametrization of Key Factors Affecting Levoglucosan Emission During Solid Fuel Burning.

Levoglucosan (LG) is a pyrolysis product of cellulose and hemicellulose at low combustion temperatures. However, LG release cannot be determined only by considering the contents of cellulose and hemicellulose exclusively due to the complexity of combustion processes and the physical-chemical properties of the fuel. This study detected the emission factors (EFs) of LG from 22 different solid fuel samples (including coal and biomass) by considering 18 different fuel properties and five combustion parameters. The average LGEFs during solid fuel burning varied in a range of 0.03-136 mg kg-1, with a magnitude difference of 1-4 orders. While the variations in cellulose (59.5-368 mg g-1) and hemicellulose (73.5-165 mg g-1) contents of fuel samples were only one- to 6-fold. A short combustion duration (<150 min) and a medium combustion temperature (200-400 °C) influenced by volatile and ash contents are crucial for the generation and accumulation of LG. A random forest coupled with the Akaike information criterion stepwise regression model successfully explained 96% of the total LG emission variation using three variables (ash content, cellulose content, and modified combustion efficiency). The ash content promoted coke formation and LG chain cracking by increasing the pyrolysis temperature and is considered the most important factor. The alkali metal in ash can reduce the energy barrier of intramolecular ring contraction reactions and inhibit the dehydration reactions, which led to additional heat being utilized by the competitive pathways of LG formation. This study provided a method to address the parametrization and release mechanisms of combustion source emissions.

Global Anthropogenic Emissions of Full-Volatility Organic Compounds.

Traditional global emission inventories classify primary organic emissions into nonvolatile organic carbon and volatile organic compounds (VOCs), excluding intermediate-volatility and semivolatile organic compounds (IVOCs and SVOCs, respectively), which are important precursors of secondary organic aerosols. This study establishes the first global anthropogenic full-volatility organic emission inventory with chemically speciated or volatility-binned emission factors. The emissions of extremely low/low-volatility organic compounds (xLVOCs), SVOCs, IVOCs, and VOCs in 2015 were 13.2, 10.1, 23.3, and 120.5 Mt, respectively. The full-volatility framework fills a gap of 18.5 Mt I/S/xLVOCs compared with the traditional framework. Volatile chemical products (VCPs), domestic combustion, and on-road transportation sources were dominant contributors to full-volatility emissions, accounting for 30, 30, and 12%, respectively. The VCP and on-road transportation sectors were the main contributors to IVOCs and VOCs. The key emitting regions included Africa, India, Southeast Asia, China, Europe, and the United States, among which China, Europe, and the United States emitted higher proportions of IVOCs and VOCs owing to the use of cleaner fuel in domestic combustion and more intense emissions from VCPs and on-road transportation activities. The findings contribute to a better understanding of the impact of organic emissions on global air pollution and climate change.

Facility-Level Emissions and Synergistic Control of Energy-Related Air Pollutants and Carbon Dioxide in China.

Boilers involve ∼60% of primary energy consumption in China and emit more air pollutants and CO2 than any other infrastructures. Here, we established a nationwide, facility-level emission data set considering over 185,000 active boilers in China by fusing multiple data sources and jointly using various technical means. The emission uncertainties and spatial allocations were significantly improved. We found that coal-fired power plant boilers were not the most emission-intensive boilers with regard to SO2, NOx, PM, and mercury but emitted the highest CO2. However, biomass- and municipal waste-fired combustion, regarded as zero-carbon technologies, emitted a large fraction of SO2, NOx, and PM. Future biomass or municipal waste mixing in coal-fired power plant boilers can make full use of the advantages of zero-carbon fuel and the pollution control devices of coal-fired power plants. We identified small-size boilers, medium-size boilers using circulating fluidized bed boilers, and large-size boilers located in China's coal mine bases as the main high emitters. Future focuses on high-emitter control can substantially mitigate the emissions of SO2 by 66%, NOx by 49%, PM by 90%, mercury by 51%, and CO2 by 46% at the most. Our study sheds light on other countries wishing to reduce their energy-related emissions and thus the related impacts on humans, ecosystems, and climates.

Ecological Study on Global Health Effects due to Source-Specific Ambient Fine Particulate Matter Exposure.

Ambient air pollution of fine particulate matter with diameters less than 2.5 µm (PM2.5) is associated with millions of premature deaths per year, recognized as a leading global health concern. The dose-response relation between ambient PM2.5 exposure and mortality risk is the most fundamental information for assessments of the health effects of PM2.5. The existing dose-response relations were generally developed based on the assumption of equal contribution to toxicity from various sources. However, the sources of PM2.5 may significantly influence health effects. In this study, we conducted an ecological study to investigate the global long-term correlation between source-specific PM2.5 exposure and cause-specific mortality risk (SPECM) based on the regional aggregate data of the publically available official health databases from 528 regions worldwide with a total registered population of 3.2 billion. The results provided preliminary epidemiological evidence for differing chronic health effects across various sources. The relative mortality risks of lung cancer and circulatory diseases were closely correlated with the primary emissions from industrial and residential combustion sources. Chronic lower respiratory diseases were mostly associated with the mass concentration of particulate matter.

Isotopic Fractionation Characteristics of Speciated Mercury from Local Biomass Combustion in the Tibetan Plateau.

As the Third Pole of the world, the Tibetan Plateau (TP) is sensitive to anthropogenic influences. Biomass combustion is one of the most important anthropogenic sources of mercury (Hg) emissions in the TP. However, due to the lack of knowledge about Hg emission characteristics and activity levels in the plateau, atmospheric Hg emissions from biomass combustion in the TP are under large uncertainties. Here, based on pilot-scale experiments, we found that particle-bound mercury (PBM; mean of 83.1-87.7 ng/m3) occupied 17.93-49.31% of the total emitted Hg and the PBM δ202Hg values (average -1.65‰ to -0.77‰) were significantly higher than those of the corresponding feeding biomass. The Δ200Hg values of total gaseous mercury and PBM were more negative (-0.08‰ to -0.05‰) than other anthropogenic emissions, providing unique isotopic fingerprints for this sector. Together with the investigated local activity levels, Hg emissions from biomass combustion reached 402 ± 74 kg/a, which were dozens of times higher than previous estimates. The emissions were characterized by conspicuous spatial heterogeneity, concentrated in the northern and central TP. Specialized Hg emissions and the Hg isotope fingerprint of local biomass combustion can aid in evaluating the influence of this sector on the fragile ecosystems of the TP.

Vehicular Ammonia Emissions Significantly Contribute to Urban PM2.5 Pollution in Two Chinese Megacities.

Ammonia (NH3) plays a vital role in the formation of fine particulate matter (PM2.5). Prior studies have primarily focused on the control of agricultural NH3 emissions, the dominant source of anthropogenic NH3 emissions. The air quality impact from vehicular NH3 emissions, which could be particularly important in urban areas, has not been adequately evaluated. We developed high-resolution vehicular NH3 emission inventories for Beijing and Shanghai based on detailed link-level traffic profiles and conducted atmospheric simulations of ambient PM2.5 concentrations contributed by vehicular NH3 emissions. We found that vehicular NH3 emissions shared high proportions among total anthropogenic NH3 emissions in the urban areas of Beijing (86%) and Shanghai (45%), where vehicular NH3 was primarily emitted by gasoline vehicles. Local vehicular NH3 emissions could be responsible for approximately 3% of urban PM2.5 concentrations during wintertime, and the contributions could be much higher during polluted periods (∼3 µg m-3). We also showed that controlling vehicular NH3 emissions will be effective and feasible to alleviate urban PM2.5 pollution for megacities in the near future.

Present Knowledge and Future Perspectives of Atmospheric Emission Inventories of Toxic Trace Elements: A Critical Review.

Toxic trace elements (TEs) can pose serious risks to ecosystems and human health. However, a comprehensive understanding of atmospheric emission inventories for several concerning TEs has not yet been developed. In this study, we systematically reviewed the status and progress of existing research in developing atmospheric emission inventories of TEs focusing on global, regional, and sectoral scales. Multiple studies have strengthened our understanding of the global emission of TEs, despite attention being mainly focused on Hg and source classification in different studies showing large discrepancies. In contrast to those of developed countries and regions, the officially published emission inventory is still lacking in developing countries, despite the fact that studies on evaluating the emissions of TEs on a national scale or one specific source category have been numerous in recent years. Additionally, emissions of TEs emitted from waste incineration and traffic-related sources have produced growing concern with worldwide rapid urbanization. Although several studies attempt to estimate the emissions of TEs based on PM emissions and its source-specific chemical profiles, the emission factor approach is still the universal method. We call for more extensive and in-depth studies to establish a precise localization national emission inventory of TEs based on adequate field measurements and comprehensive investigation to reduce uncertainty.