PM2.5 and water-soluble inorganic ion concentrations decreased faster in urban than rural areas in China.

We investigated variations of PM2.5 and water-soluble inorganic ions chemical characteristics at nine urban and rural sites in China using ground-based observations. From 2015 to 2019, mean PM2.5 concentration across all sites decreased by 41.9 µg/m3 with a decline of 46% at urban sites and 28% at rural sites, where secondary inorganic aerosol (SIAs) contributed to 21% (urban sites) and 17% (rural sites) of the decreased PM2.5. SIAs concentrations underwent a decline at urban locations, while sulfate (SO42-), nitrate (NO3-), and ammonium (NH4+) decreased by 49.5%, 31.3% and 31.6%, respectively. However, only SO42- decreased at rural sites, NO3- increased by 21% and NH4+ decreased slightly. Those changes contributed to an overall SIAs increase in 2019. Higher molar ratios of NO3- to SO42- and NH4+ to SO42- were observed at urban sites than rural sites, being highest in the heavily polluted days. Mean molar ratios of NH3/NHx were higher in 2019 than 2015 at both urban and rural sites, implying increasing NHx remained as free NH3. Our observations indicated a slower transition from sulfate-driven to nitrate-driven aerosol pollution and less efficient control of NOx than SO2 related aerosol formation in rural regions than urban regions. Moreover, the common factor at urban and rural sites appears to be a combination of lower SO42- levels and an increasing fraction of NO3- to PM2.5 under NH4+-rich conditions. Our findings imply that synchronous reduction in NOx and NH3 emissions especially rural areas would be effective to mitigate NO3--driven aerosol pollution.

Ammonia Dry Deposition in an Alpine Ecosystem Traced to Agricultural Emission Hotpots.

Elevated reactive nitrogen (Nr) deposition is a concern for alpine ecosystems, and dry NH3 deposition is a key contributor. Understanding how emission hotspots impact downwind ecosystems through dry NH3 deposition provides opportunities for effective mitigation. However, direct NH3 flux measurements with sufficient temporal resolution to quantify such events are rare. Here, we measured NH3 fluxes at Rocky Mountain National Park (RMNP) during two summers and analyzed transport events from upwind agricultural and urban sources in northeastern Colorado. We deployed open-path NH3 sensors on a mobile laboratory and an eddy covariance tower to measure NH3 concentrations and fluxes. Our spatial sampling illustrated an upslope event that transported NH3 emissions from the hotspot to RMNP. Observed NH3 deposition was significantly higher when backtrajectories passed through only the agricultural region (7.9 ng m-2 s-1) versus only the urban area (1.0 ng m-2 s-1) and both urban and agricultural areas (2.7 ng m-2 s-1). Cumulative NH3 fluxes were calculated using observed, bidirectional modeled, and gap-filled fluxes. More than 40% of the total dry NH3 deposition occurred when air masses were traced back to agricultural source regions. More generally, we identified that 10 (25) more national parks in the U.S. are within 100 (200) km of an NH3 hotspot, and more observations are needed to quantify the impacts of these hotspots on dry NH3 deposition in these regions.

Assessing Contributions of Agricultural and Nonagricultural Emissions to Atmospheric Ammonia in a Chinese Megacity.

Ammonia (NH3) is the predominant alkaline gas in the atmosphere contributing to formation of fine particles-a leading environmental cause of increased morbidity and mortality worldwide. Prior findings suggest that NH3 in the urban atmosphere derives from a complex mixture of agricultural (mainly livestock production and fertilizer application) and nonagricultural (e.g., urban waste, fossil fuel-related emissions) sources; however, a citywide holistic assessment is hitherto lacking. Here we show that NH3 from nonagricultural sources rivals agricultural NH3 source contributions in the Shanghai urban atmosphere. We base our conclusion on four independent approaches: (i) a full-year operation of a passive NH3 monitoring network at 14 locations covering urban, suburban, and rural landscapes; (ii) model-measurement comparison of hourly NH3 concentrations at a pair of urban and rural supersites; (iii) source-specific NH3 measurements from emission sources; and (iv) localized isotopic signatures of NH3 sources integrated in a Bayesian isotope mixing model to make isotope-based source apportionment estimates of ambient NH3. Results indicate that nonagricultural sources and agricultural sources are both important contributors to NH3 in the urban atmosphere. These findings highlight opportunities to limit NH3 emissions from nonagricultural sources to help curb PM2.5 pollution in urban China.

Increasing importance of deposition of reduced nitrogen in the United States.

Rapid development of agriculture and fossil fuel combustion greatly increased US reactive nitrogen emissions to the atmosphere in the second half of the 20th century, resulting in excess nitrogen deposition to natural ecosystems. Recent efforts to lower nitrogen oxides emissions have substantially decreased nitrate wet deposition. Levels of wet ammonium deposition, by contrast, have increased in many regions. Together these changes have altered the balance between oxidized and reduced nitrogen deposition. Across most of the United States, wet deposition has transitioned from being nitrate-dominated in the 1980s to ammonium-dominated in recent years. Ammonia has historically not been routinely measured because there are no specific regulatory requirements for its measurement. Recent expansion in ammonia observations, however, along with ongoing measurements of nitric acid and fine particle ammonium and nitrate, permit new insight into the balance of oxidized and reduced nitrogen in the total (wet + dry) US nitrogen deposition budget. Observations from 37 sites reveal that reduced nitrogen contributes, on average, ∼65% of the total inorganic nitrogen deposition budget. Dry deposition of ammonia plays an especially key role in nitrogen deposition, contributing from 19% to 65% in different regions. Future progress toward reducing US nitrogen deposition will be increasingly difficult without a reduction in ammonia emissions.

Reducing Wet Ammonium Deposition in Rocky Mountain National Park: the Development and Evaluation of A Pilot Early Warning System for Agricultural Operations in Eastern Colorado.

Agricultural emissions are the primary source of ammonia (NH3) deposition in Rocky Mountain National Park (RMNP), a Class I area, that is granted special air quality protections under the Clean Air Act. Between 2014 and 2016, the pilot phase of the Colorado agricultural nitrogen early warning system (CANEWS) was developed for agricultural producers to voluntarily and temporarily minimize emissions of NH3 during periods of upslope winds. The CANEWS was created using trajectory analyses driven by outputs from an ensemble of numerical weather forecasts together with the climatological expertize of human forecasters. Here, we discuss the methods for the CANEWS and offer preliminary analyses of 33 months of the CANEWS based on atmospheric deposition data from two sites in RMNP as well as responses from agricultural producers after warnings were issued. Results showed that the CANEWS accurately predicted 6 of 9 high N deposition weeks at a lower-elevation observation site, but only 4 of 11 high N deposition weeks at a higher-elevation site. Sixty agricultural producers from 39 of Colorado's agricultural operations volunteered for the CANEWS, and a two-way line of communication between agricultural producers and scientists was formed. For each warning issued, an average of 23 producers responded to a postwarning survey. Over 75% of responding CANEWS participants altered their practices after an alert. While the current effort was insufficient to reduce atmospheric deposition, we were encouraged by the collaborative spirit between agricultural, scientific, and resource management communities. Solving a broad and complex social-ecological problem requires both a technological approach, such as the CANEWS, and collaboration and trust from all participants, including agricultural producers, land managers, university researchers, and environmental agencies.

Residential Coal Combustion as a Source of Levoglucosan in China.

Levoglucosan (LG) has been widely identified as a specific marker for biomass burning (BB) sources and frequently utilized in estimating the BB contribution to atmospheric fine particles all over the world. However, this study provides direct evidence to show that coal combustion (CC) is also a source of LG, especially in the wintertime in Northern China, based on both source testing and ambient measurement. Our results show that low-temperature residential CC could emit LG with emission factors (EF) ranging from 0.3 to 15.9 mg kg-1. Ratios of LG to its isomers, mannosan and galactosan, differ between CC and BB emissions, and the wintertime ratios in Beijing ambient PM2.5 and source-specific tracers including carbon isotopic signatures all indicated a significant contribution from CC to ambient levoglucosan in winter in Beijing. The results suggest that LG cannot be used as a distinct source marker for biomass burning in special cases such as some cities in the northern China, where coal is still widely used in the residential and industrial sectors. Biomass burning sources could be overestimated, although such an over-estimation could vary spatially and temporally.

Aerosol liquid water driven by anthropogenic nitrate: implications for lifetimes of water-soluble organic gases and potential for secondary organic aerosol formation.

Aerosol liquid water (ALW) influences aerosol radiative properties and the partitioning of gas-phase water-soluble organic compounds (WSOCg) to the condensed phase. A recent modeling study drew attention to the anthropogenic nature of ALW in the southeastern United States, where predicted ALW is driven by regional sulfate. Herein, we demonstrate that ALW in the Po Valley, Italy, is also anthropogenic but is driven by locally formed nitrate, illustrating regional differences in the aerosol components responsible for ALW. We present field evidence for the influence of controllable ALW on the lifetimes and atmospheric budgets of reactive organic gases and note the role of ALW in the formation of secondary organic aerosol (SOA). Nitrate is expected to increase in importance due to increased emissions of nitrate precursors, as well as policies aimed at reducing sulfur emissions. We argue that the impacts of increased particulate nitrate in future climate and air quality scenarios may be under predicted because they do not account for the increased potential for SOA formation in nitrate-derived ALW, nor do they account for the impacts of this ALW on reactive gas budgets and gas-phase photochemistry.

Regime shift in secondary inorganic aerosol formation and nitrogen deposition in the rural United States.

Secondary inorganic aerosols play an important role in air pollution and climate change, and their formation modulates the atmospheric deposition of reactive nitrogen (including oxidized and reduced nitrogen), thus impacting the nitrogen cycle. Large-scale and long-term analyses of secondary inorganic aerosol formation based on model simulations have substantial uncertainties. Here we improve constraints on secondary inorganic aerosol formation using decade-long in situ observations of aerosol composition and gaseous precursors from multiple monitoring networks across the United States. We reveal a shift in the secondary inorganic aerosol formation regime in the rural United States between 2011 and 2020, making rural areas less sensitive to changes in ammonia concentrations and shortening the effective atmospheric lifetime of reduced forms of reactive nitrogen. This leads to potential increases in reactive nitrogen deposition near ammonia emission hotspots, with ecosystem impacts warranting further investigation. Ammonia (NH3), a critical but not directly regulated precursor of fine particulate matter in the United States, has been increasingly scrutinized to improve air quality. Our findings, however, show that controlling NH3 became significantly less effective for mitigating fine particulate matter in the rural United States. We highlight the need for more collocated aerosol and precursor observations for better characterization of secondary inorganic aerosols formation in urban areas.

Microscopic evaluation of trace metals in cloud droplets in an acid precipitation region.

Mass concentrations of soluble trace metals and size, number, and mixing properties of nanometal particles in clouds determine their toxicity to ecosystems. Cloud water was found to be acidic, with a pH of 3.52, at Mt. Lu (elevation 1,165 m) in an acid precipitation region in South China. A combination of Inductively Coupled Plasma Mass Spectrometry (ICPMS) and Transmission Electron Microscopy (TEM) for the first time demonstrates that the soluble metal concentrations and solid metal particle number are surprisingly high in acid clouds at Mt. Lu, where daily concentrations of SO2, NO2, and PM10 are 18 µg m(-3), 7 µg m(-3), and 22 µg m(-3). The soluble metals in cloudwater with the highest concentrations were zinc (Zn, 200 µg L(-1)), iron (Fe, 88 µg L(-1)), and lead (Pb, 77 µg L(-1)). TEM reveals that 76% of cloud residues include metal particles that range from 50 nm to 1 µm diameter with a median diameter of 250 nm. Four major metal-associated particle types are Pb-rich (35%), fly ash (27%), Fe-rich (23%), and Zn-rich (15%). Elemental mapping shows that minor soluble metals are distributed within sulfates of cloud residues. Emissions of fine metal particles from large, nonferrous industries and coal-fired power plants with tall stacks were transported upward to this high elevation. Our results suggest that the abundant trace metals in clouds aggravate the impacts of acid clouds or associated precipitation on the ecosystem and human health.

Variations in the OM/OC ratio of urban organic aerosol next to a major roadway.

Understanding the organic matter/organic carbon (OM/OC) ratio in ambient particulate matter (PM) is critical to achieve mass closure in routine PM measurements, to assess the sources of and the degree of chemical processing organic aerosol particles have undergone, and to relate ambient pollutant concentrations to health effects. Of particular interest is how the OM/OC ratio varies in the urban environment, where strong spatial and temporal gradients in source emissions are common. We provide results of near-roadway high-time-resolution PM1 OM concentration and OM/OC ratio observations during January 2008 at Fyfe Elementary School in Las Vegas, NV, 18 m from the U.S. 95 freeway soundwall, measured with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The average OM/OC ratio was 1.54 (+/- 0.20 standard deviation), typical of environments with a low amount of secondary aerosol formation. The 2-min average OM/OC ratios varied between 1.17 and 2.67, and daily average OM/OC ratios varied between 1.44 and 1.73. The ratios were highest during periods of low OM concentrations and generally low during periods of high OM concentrations. OM/OC ratios were low (1.52 +/- 0.14, on average) during the morning rush hour (average OM = 2.4 microg/m3), when vehicular emissions dominate this near-road measurement site. The ratios were slightly lower (1.46 +/- 0.10) in the evening (average OM = 6.3 microg/m3), when a combination of vehicular and fresh residential biomass burning emissions was typically present during times with temperature inversions. The hourly averaged OM/OC ratio peaked at 1.66 at midday. OM concentrations were similar regardless of whether the monitoring site was downwind or upwind of the adjacent freeway throughout the day, though they were higher during stagnant conditions (wind speed < 0.5 m/sec). The OM/OC ratio generally varied more with time of day than with wind direction and speed.

Aerosol species concentrations and source apportionment of ammonia at Rocky Mountain National Park.

Changes in ecosystem function at Rocky Mountain National Park (RMNP) are occurring because of emissions of nitrogen and sulfate species along the Front Range of the Colorado Rocky Mountains, as well as sources farther east and west. The nitrogen compounds include both oxidized and reduced nitrogen. A year-long monitoring program of various oxidized and reduced nitrogen species was initiated to better understand their origins as well as the complex chemistry occurring during transport from source to receptor. Specifically the goals of the study were to characterize the atmospheric concentrations of nitrogen species in gaseous, particulate, and aqueous phases (precipitation and clouds) along the east and west sides of the Continental Divide; identify the relative contributions to atmospheric nitrogen species in RMNP from within and outside of the state of Colorado; identify the relative contributions to atmospheric nitrogen species in RMNP from emission sources along the Colorado Front Range versus other areas within Colorado; and identify the relative contributions to atmospheric nitrogen species from mobile sources, agricultural activities, and large and small point sources within the state of Colorado. Measured ammonia concentrations are combined with modeled releases of conservative tracers from ammonia source regions around the United States to apportion ammonia to its respective sources, using receptor modeling tools.

On-road mobile mapping of spatial variations and source contributions of ammonia in Beijing, China.

Ammonia (NH3) measurements were performed with a mobile platform deploying a cavity ring-down spectroscopy NH3 analyzer in Beijing. The transect and loop sampling strategy revealed that the Beijing urban area is more strongly affected by NH3 emissions than surrounding areas. Although average enhancements of on-road NH3 were small compared to background levels, traffic emissions clearly dominated city enhancements of NH3, carbon dioxide (CO2), acetaldehyde and acetone. Increments of on-road NH3 ranged between 5.1 ppb and 11.4 ppb in urban areas, representing an enhancement of 20.6 % to 47.9 % over the urban background. The vehicle NH3:CO2 emission ratio was 0.26 ppb/ppm, about a factor of 1.5 higher than the value derived from the available emission inventory. The obtained NH3 emission factor was approximately 306.9 mg/kg. If the annual gasoline consumption in Beijing is accurate, annual NH3 emissions from vehicles are estimated at 1.5 Gg. The influx and outflux of NH3 in Beijing during monitoring periods fluctuated due to variations of wind direction (WD), wind speed (WS), and planetary boundary layer height (PBLH). Net fluxes at the 4th Ring Road were larger than zero, suggesting that local emissions were important in urban Beijing. Negative net fluxes at the 6th Ring Road reveal a large amount of NH3 transported from agricultural regions south of Beijing lost during transport across the city, for example by deposition or particle formation in the city. Our analyses have important implications for regional NH3 emission estimates and for improving vehicular NH3 emission inventory allocations.

Observations of ozone, acyl peroxy nitrates, and their precursors during summer 2019 at Carlsbad Caverns National Park, New Mexico.

Carlsbad Caverns National Park (CAVE) is located in southeastern New Mexico and is adjacent to the Permian Basin, one of the most productive oil and natural gas (O&G) production regions in the United States. Since 2018, ozone (O3) at CAVE has frequently exceeded the 70 ppbv 8-hour National Ambient Air Quality Standard. We examine the influence of regional emissions on O3 formation using observations of O3, nitrogen oxides (NOx = NO + NO2), a suite of volatile organic compounds (VOCs), peroxyacetyl nitrate (PAN), and peroxypropionyl nitrate (PPN). Elevated O3 and its precursors are observed when the wind is from the southeast, the direction of the Permian Basin. We identify 13 days during the July 25 to September 5, 2019 study period when the maximum daily 8-hour average (MDA8) O3 exceeded 65 ppbv; MDA8 O3 exceeded 70 ppbv on 5 of these days. The results of a positive matrix factorization (PMF) analysis are used to identify and attribute source contributions of VOCs and NOx. On days when the winds are from the southeast, there are larger contributions from factors associated with primary O&G emissions; and, on high O3 days, there is more contribution from factors associated with secondary photochemical processing of O&G emissions. The observed ratio of VOCs to NOx is consistently high throughout the study period, consistent with NOx-limited O3 production. Finally, all high O3 days coincide with elevated acyl peroxy nitrate abundances with PPN to PAN ratios > 0.15 ppbv ppbv-1 indicating that anthropogenic VOC precursors, and often alkanes specifically, dominate the photochemistry.Implications: The results above strongly indicate NOx-sensitive photochemistry at Carlsbad Caverns National Park indicating that reductions in NOx emissions should drive reductions in O3. However, the NOx-sensitivity is largely driven by emissions of NOx into a VOC-rich environment, and a high PPN:PAN ratio and its relationship to O3 indicate substantial influence from alkanes in the regional photochemistry. Thus, simultaneous reductions in emissions of NOx and non-methane VOCs from the oil and gas sector should be considered for reducing O3 at Carlsbad Caverns National Park. Reductions in non-methane VOCs will have the added benefit of reducing formation of other secondary pollutants and air toxics.

Source characterization of volatile organic compounds at Carlsbad Caverns National Park.

Carlsbad Caverns National Park (CAVE), located in southeastern New Mexico, experiences elevated ground-level ozone (O3) exceeding the National Ambient Air Quality Standard (NAAQS) of 70 ppbv. It is situated adjacent to the Permian Basin, one of the largest oil and gas (O&G) producing regions in the US. In 2019, the Carlsbad Caverns Air Quality Study (CarCavAQS) was conducted to examine impacts of different sources on ozone precursors, including nitrogen oxides (NOx) and volatile organic compounds (VOCs). Here, we use positive matrix factorization (PMF) analysis of speciated VOCs to characterize VOC sources at CAVE during the study. Seven factors were identified. Three factors composed largely of alkanes and aromatics with different lifetimes were attributed to O&G development and production activities. VOCs in these factors were typical of those emitted by O&G operations. Associated residence time analyses (RTA) indicated their contributions increased in the park during periods of transport from the Permian Basin. These O&G factors were the largest contributor to VOC reactivity with hydroxyl radicals (62%). Two PMF factors were rich in photochemically generated secondary VOCs; one factor contained species with shorter atmospheric lifetimes and one with species with longer lifetimes. RTA of the secondary factors suggested impacts of O&G emissions from regions farther upwind, such as Eagle Ford Shale and Barnett Shale formations. The last two factors were attributed to alkenes likely emitted from vehicles or other combustion sources in the Permian Basin and regional background VOCs, respectively.Implications: Carlsbad Caverns National Park experiences ground-level ozone exceeding the National Ambient Air Quality Standard. Volatile organic compounds are critical precursors to ozone formation. Measurements in the Park identify oil and gas production and development activities as the major contributors to volatile organic compounds. Emissions from the adjacent Permian Basin contributed to increases in primary species that enhanced local ozone formation. Observations of photochemically generated compounds indicate that ozone was also transported from shale formations and basins farther upwind. Therefore, emission reductions of volatile organic compounds from oil and gas activities are important for mitigating elevated O3 in the region.

Abundant nitrogenous secondary organic aerosol formation accelerated by cloud processing.

Nitrogenous organic (CHON), crucial for secondary organic aerosol (SOA), forms through poorly studied mechanisms in clouds. Our study explores CHON transformation during cloud processes (CPs). These processes play a vital role in enhancing the variety of CHONs, leading to the formation of CHONs with oxygen atom counts ranging from 1 to 10 and double bond equivalent (DBE) values spanning from 2 to 10. We proposed that the CHONs formed during CPs are formed through aqueous phase reactions with CHO compound precursors via nucleophilic attacks by NH3. This scheme can be account for roughly three-quarters of the CHONs by number in cloud water, and near two-thirds of all CHONs are formed through reactions between NH3 and carbonyl-containing biogenic volatile organic compound (BVOC) ozonolysis intermediates. This study provides the first insights into the evolution of CHONs during CPs and reveals the significant roles of CPs in the formation of CHONs.

Microfluidic electrochemical sensor for on-line monitoring of aerosol oxidative activity.

Particulate matter (PM) air pollution has a significant impact on human morbidity and mortality; however, the mechanisms of PM-induced toxicity are poorly defined. A leading hypothesis states that airborne PM induces harm by generating reactive oxygen species in and around human tissues, leading to oxidative stress. We report here a system employing a microfluidic electrochemical sensor coupled directly to a particle-into-liquid sampler (PILS) system to measure aerosol oxidative activity in an on-line format. The oxidative activity measurement is based on the dithiothreitol (DTT) assay, where, after being oxidized by PM, the remaining reduced DTT is analyzed by the microfluidic sensor. The sensor consists of an array of working, reference, and auxiliary electrodes fabricated in a poly(dimethylsiloxane)-based microfluidic device. Cobalt(II) phthalocyanine-modified carbon paste was used as the working electrode material, allowing selective detection of reduced DTT. The electrochemical sensor was validated off-line against the traditional DTT assay using filter samples taken from urban environments and biomass burning events. After off-line characterization, the sensor was coupled to a PILS to enable on-line sampling/analysis of aerosol oxidative activity. Urban dust and industrial incinerator ash samples were aerosolized in an aerosol chamber and analyzed for their oxidative activity. The on-line sensor reported DTT consumption rates (oxidative activity) in good correlation with aerosol concentration (R(2) from 0.86 to 0.97) with a time resolution of approximately 3 min.

Fragmentation analysis of water-soluble atmospheric organic matter using ultrahigh-resolution FT-ICR mass spectrometry.

Isolated water-soluble atmospheric organic matter (AOM) analytes extracted from radiation fogwater samples were analyzed using collision induced dissociation with ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Tandem mass analysis was performed on several mass ranges between 100 and 400 Da to characterize the functional groups of AOM species. Compounds containing nitrogen and/or sulfur were targeted because of the high number of oxygen atoms contained in their molecular formulas. Due to the large number of isobaric ions in the precursor isolation ranges, large numbers of product ions resulted from collision induced dissociation. Common neutral losses were assigned by matching the molecular formulas of the expected product ions with the detected product ions within the appropriate mass spectra. Since polar functional groups are expected to affect the hygroscopic properties of aerosols, the losses of H(2)O, CO(2), CH(3)OH, HNO(3), CH(3)NO(3), SO(3), SO(4) and combinations of these were specifically targeted. Among the 421 compounds studied, the most frequently observed neutral losses were CO(2) (54%), H(2)O (43%) and CH(3)OH (40%). HNO(3) losses were observed for 63% of the studied nitrogen containing compounds and 33% of the studied compounds containing both nitrogen and sulfur. SO(3) losses were observed for 85% of the studied sulfur containing compounds and 42% of studied compounds containing both nitrogen and sulfur. A number of molecular formulas matching those of monoterpene ozonolysis SOA were observed; they include organonitrates, organosulfates, and nitroxy-organosulfates. Overall, the results of fragmentation analysis of 400+ individual molecular precursors elucidate the complexity and multifunctional nature of the isolated water-soluble AOM.

Spatiotemporal variations of nitrogen and phosphorus deposition across China.

Atmospheric deposition is an important pathway for the input of anthropogenic and natural nutrients to terrestrial and aquatic ecosystems. However, previous measurements focused mainly on hotspot locations, ignoring the fact that the deposition magnitudes of various nutrient species (e.g., nitrogen (N), phosphorus (P)) at a national scale should be investigated jointly. To better characterize national scale bulk deposition, precipitation samples were collected at 41 sites across China from September 2015 to August 2016 and September 2017 to August 2018. The bulk deposition fluxes of total nitrogen (TN) and total phosphorus (TP) over the network were 27.5 kg N ha-1 yr-1 and 0.92 kg P ha-1 yr-1, respectively. Contributions of NH4+, NO3-, and dissolved organic nitrogen (DON) to TN averaged 32%, 32%, and 36%, respectively. Significant spatial and seasonal variations in concentrations and deposition fluxes of all nutrient species were observed reflecting effects of local reactive nitrogen (Nr) and P emissions and rainfall amount. Major sources were energy resource consumption for NO3-, agricultural activities for NH4+, and a mixed contribution of both anthropogenic and natural sources for DON and TP. Atmospheric N and P deposition represent important external nutrient inputs to ecosystems and a high ratio of TN to TP (29.9) may induce relative P-limitation and further increase the risk of eutrophication. This work reveals a new map of atmospheric N and P deposition and identifies regions where emissions should be controlled to mitigate long-term impacts of atmospheric deposition over China.