A mitochondrial STAT3-methionine metabolism axis promotes ILC2-driven allergic lung inflammation.

BACKGROUND: Group 2 innate lymphoid cells (ILC2s), the innate counterpart of TH2 cells, play a critical role in type 2 immune responses. However, the molecular regulatory mechanisms of ILC2s are still unclear. OBJECTIVE: The aim of this study was to explore the importance of signal transducer and activator of transcription 3 (STAT3) to ILC2 function in allergic lung inflammation. METHODS: Acute and chronic asthma models were established by intranasal administration of the protease allergen papain in VavicreStat3fl/fl, Il5tdtomato-creStat3fl/fl, and RorccreStat3fl/fl mice to verify the necessity of functional STAT3 for ILC2 allergic response. The intrinsic role of STAT3 in regulating ILC2 function was examined by generation of bone marrow chimera mice. The underlying mechanism was studied through confocal imaging, metabolomics analysis, and chromatin immunoprecipitation quantitative PCR. RESULTS: STAT3 is essential for ILC2 effector function and promotes ILC2-driven allergic inflammation in the lung. Mechanistically, the alarmin cytokine IL-33 induces a noncanonical STAT3 phosphorylation at serine 727 in ILC2s, leading to translocation of STAT3 into the mitochondria. Mitochondrial STAT3 further facilitates adenosine triphosphate synthesis to fuel the methionine cycle and generation of S-adenosylmethionine, which supports the epigenetic reprogramming of type 2 cytokines in ILC2s. STAT3 deficiency, inhibition of STAT3 mitochondrial translocation, or blockade of methionine metabolism markedly dampened the ILC2 allergic response and ameliorated allergic lung inflammation. CONCLUSION: The mitochondrial STAT3-methionine metabolism pathway is a key regulator that shapes ILC2 effector function through epigenetic regulation, and the related proteins or metabolites represent potential therapeutic targets for allergic lung inflammation.

Cyclophilin A associates with enterovirus-71 virus capsid and plays an essential role in viral infection as an uncoating regulator.

Viruses utilize host factors for their efficient proliferation. By evaluating the inhibitory effects of compounds in our library, we identified inhibitors of cyclophilin A (CypA), a known immunosuppressor with peptidyl-prolyl cis-trans isomerase activity, can significantly attenuate EV71 proliferation. We demonstrated that CypA played an essential role in EV71 entry and that the RNA interference-mediated reduction of endogenous CypA expression led to decreased EV71 multiplication. We further revealed that CypA directly interacted with and modified the conformation of H-I loop of the VP1 protein in EV71 capsid, and thus regulated the uncoating process of EV71 entry step in a pH-dependent manner. Our results aid in the understanding of how host factors influence EV71 life cycle and provide new potential targets for developing antiviral agents against EV71 infection.

Evidence for Different Reactive Hg Sources and Chemical Compounds at Adjacent Valley and High Elevation Locations.

The spatial distribution of chemical compounds and concentration of reactive mercury (RM), defined as the sum of gaseous oxidized mercury (GOM) and <3 µm particulate bound mercury (PBM), are poorly characterized. The objective of this study was to understand the chemistry, concentration, and spatial and temporal distribution of GOM at adjacent locations (12 km apart) with a difference in elevation of ∼1000 m. Atmospheric GOM measurements were made with passive and active samplers using membranes, and at one location, a Tekran mercury measurement system was used. The chemistry of GOM varied across time and location. On the basis of data collected, chemistry at the low elevation site adjacent to a highway was primarily influenced by pollutants generated by mobile sources (GOM = nitrogen and sulfur-based compounds), and the high elevation site (GOM = halogen-based compounds) was affected by long-range transport in the free troposphere over the marine boundary layer into Nevada. Data collected at these two locations demonstrate that different GOM compounds exist depending on the oxidants present in the air. Measurements of GOM made by the KCl denuder in the Tekran instrument located at the low elevation site were lower than that measured using membranes by 1.7-13 times. Accurate measurements of atmospheric concentrations and chemistry of RM are necessary for proper assessment of environmental impacts, and field measurements are essential for atmospheric models, which in turn influence policy decisions.

Use of passive sampling methods and models to understand sources of mercury deposition to high elevation sites in the Western United States.

To understand gaseous oxidized mercury (GOM) sources to the Western US, data were collected with passive samplers for ambient GOM concentrations and dry deposition at 10 sites from the coast of the Pacific Ocean to Great Basin National Park. Tests were done to better understand the samplers and the materials used. Measured dry deposition of GOM was significantly higher at sites >2000 m elevation relative to those below due to high GOM concentrations and atmospheric turbulence. At these high elevation sites, GOM dry deposition was higher in spring due to long-range transport from Asia (air parcels from the free troposphere) and some high GOM dry deposition events were related to regional emissions. Dry deposition of GOM at two sites was calculated using the passive sampler data and a multiple-resistance model. A previously developed relationship between the sampling rate of the passive sampler and GOM concentrations was used to estimate dry deposition and a scaling factor of 3 was used to adjust GOM concentrations, due to underestimation by KCl-coated denuder measurements. With the scaling factor of 3, modeled deposition was in the range of results estimated from two different models settings. However, dry deposition did not correlate consistently with either model. The disagreement could be due to uncertainties associated with measurements and/or modeling, or different GOM compounds existing in the atmosphere. If the atmospheric GOM compounds are known, dry deposition velocities could be estimated more accurately. Lastly, we investigated the potential for use of a new sampling material for GOM and checked the efficiency of the passive sampler.

Uncertainties of Gaseous Oxidized Mercury Measurements Using KCl-Coated Denuders, Cation-Exchange Membranes, and Nylon Membranes: Humidity Influences.

Quantifying the concentration of gaseous oxidized mercury (GOM) and identifying the chemical compounds in the atmosphere are important for developing accurate local, regional, and global biogeochemical cycles. The major hypothesis driving this work was that relative humidity affects collection of GOM on KCl-coated denuders and nylon membranes, both currently being applied to measure GOM. Using a laboratory manifold system and ambient air, GOM capture efficiency on 3 different collection surfaces, including KCl-coated denuders, nylon membranes, and cation-exchange membranes, was investigated at relative humidity ranging from 25 to 75%. Recovery of permeated HgBr2 on KCl-coated denuders declined by 4-60% during spikes of relative humidity (25 to 75%). When spikes were turned off GOM recoveries returned to 60 ± 19% of permeated levels. In some cases, KCl-coated denuders were gradually passivated over time after additional humidity was applied. In this study, GOM recovery on nylon membranes decreased with high humidity and ozone concentrations. However, additional humidity enhanced GOM recovery on cation-exchange membranes. In addition, reduction and oxidation of elemental mercury during experiments was observed. The findings in this study can help to explain field observations in previous studies.

Construction and antibacterial activities of walnut green husk polysaccharide based silver nanoparticles (AgNPs).

In this paper, the size-controllable nano­silver particles (AgNPs) were synthesized from walnut green husk polysaccharide, and its cytotoxicity and antibacterial activity were evaluated. Firstly, acidic polysaccharide WGHP2 was extracted from walnut green husk, and then the silver ion in AgNO3 was reduced in WGHP2 aqueous solution using NaBH4, so as to synthesize the nano­silver composite. The nano­silver composite was characterized by transmission electron microscope, Fourier infrared spectroscopy, ultraviolet-visible spectrometer, scanning electron microscope, inductively coupled plasma mass spectrometry and X-ray photoelectron spectroscopy. The results show that AgNPs stabilized by WGHP2 are mainly regular spheres with an average particle size distribution of 15.04-19.23 nm. The particle size distribution and morphology of AgNPs changed with the concentration of silver precursor, which is related to the dispersion of silver precursor in polysaccharide aqueous solution and the formation of AgO coordination bond between silver precursor and polysaccharide molecules. These coordination bonds changed the ability of nanoparticles to produce and release Ag+, and thus regulated their antibacterial activity and cytotoxicity, as evidenced by the experimental result of the cytotoxicity of the nano­silver particle against PC12 cells and the bacteriostatic effect on E.coli and S.aureus. Conclusively, WGHP2-Ag has good stability, antibacterial activity and low cytotoxicity.

Comparison of the toxic effects of polystyrene and sulfonated polystyrene on wheat under cadmium stress.

With advances in plastic resource utilization technologies, polystyrene (PS) and sulfonated polystyrene (SPS) microplastics continue to be produced and retained in environmental media, potentially posing greater environmental risks. These plastics, due to their different physicochemical properties, may have different environmental impacts when compounded with other pollutants. The objective of this study was to investigate the combined toxic effects of PS and SPS on wheat using cadmium (Cd) as a background contaminant. The results demonstrated that Cd significantly impeded the normal growth of wheat by disrupting root development. Both PS and SPS exhibited hormesis at low concentrations and promoted wheat growth. Under combined toxicity, PS reduced oxidative stress and promoted the uptake of essential metal elements in wheat. Additionally, KEGG pathway analysis revealed that PS facilitated the repair of Cd-induced blockage of the TCA cycle and glutathione metabolism. However, high concentrations of SPS in combined toxicity not only enhanced oxidative stress and interfered with the uptake of essential metal elements, but also exacerbated the blocked TCA cycle and interfered with pyrimidine metabolism. These differences are related to the different stability (Zeta potential, Hydrodynamic particle size) of the two microplastics in the aquatic environment and their ability to carry heavy metal ions, especially Cd. The results of this study provide important insights into understanding the effects of microplastics on crops in the context of Cd contamination and their environmental and food safety implications.

Intraepithelial lymphocytes promote intestinal regeneration through CD160/HVEM signaling.

Chemotherapy and radiotherapy frequently lead to intestinal damage. The mechanisms governing the repair or regeneration of intestinal damage are still not fully elucidated. Intraepithelial lymphocytes (IELs) are the primary immune cells residing in the intestinal epithelial layer. However, whether IELs are involved in intestinal epithelial injury repair remains unclear. Here, we found that IELs rapidly infiltrated the intestinal crypt region and are crucial for the recovery of the intestinal epithelium post-chemotherapy. Interestingly, IELs predominantly promoted intestinal regeneration by modulating the proliferation of transit-amplifying (TA) cells. Mechanistically, the expression of CD160 on IELs allows for interaction with herpes virus entry mediator (HVEM) on the intestinal epithelium, thereby activating downstream nuclear factor kappa (NF-κB) signaling and further promoting intestinal regeneration. Deficiency in either CD160 or HVEM resulted in reduced proliferation of intestinal progenitor cells, impaired intestinal damage repair, and increased mortality following chemotherapy. Remarkably, the adoptive transfer of CD160-sufficient IELs rescued the Rag1 deficient mice from chemotherapy-induced intestinal inflammation. Overall, our study underscores the critical role of IELs in intestinal regeneration and highlights the potential applications of targeting the CD160-HVEM axis for managing intestinal adverse events post-chemotherapy and radiotherapy.

Comparison of gaseous oxidized Hg measured by KCl-coated denuders, and nylon and cation exchange membranes.

The chemical compounds that make up gaseous oxidized mercury (GOM) in the atmosphere, and the reactions responsible for their formation, are not well understood. The limitations and uncertainties associated with the current method applied to measure these compounds, the KCl-coated denuder, are not known due to lack of calibration and testing. This study systematically compared the uptake of specific GOM compounds by KCl-coated denuders with that collected using nylon and cation exchange membranes in the laboratory and field. In addition, a new method for identifying different GOM compounds using thermal desorption is presented. Different GOM compounds (HgCl2, HgBr2, and HgO) were found to have different affinities for the denuder surface and the denuder underestimated each of these compounds. Membranes measured 1.3 to 3.7 times higher GOM than denuders in laboratory and field experiments. Cation exchange membranes had the highest collection efficiency. Thermodesorption profiles for the release of GOM compounds from the nylon membrane were different for HgO versus HgBr2 and HgCl2. Application of the new field method for collection and identification of GOM compounds demonstrated these vary as a function of location and time of year. Understanding the chemistry of GOM across space and time has important implications for those developing policy regarding this environmental contaminant.

Fast time resolution oxidized mercury measurements during the Reno Atmospheric Mercury Intercomparison Experiment (RAMIX).

The Reno Atmospheric Mercury Intercomparison Experiment (RAMIX) was carried out from 22 August to 16 September, 2011 in Reno, NV to evaluate the performance of new and existing methods to measure atmospheric mercury (Hg). Measurements were made using a common sampling manifold to which controlled concentrations of Hg species, including gaseous elemental mercury (GEM) and HgBr2 (a surrogate gaseous oxidized mercury (GOM) compound), and potential interferents were added. We present an analysis of Hg measurements made using the University of Washington's Detector for Oxidized Hg Species (DOHGS), focusing on tests of GEM and HgBr2 spike recovery, the potential for interference from ozone (O3) and water vapor (WV), and temporal variability of ambient reactive mercury (RM). The mean GEM and HgBr2 spike recoveries measured with the DOHGS were 95% and 66%, respectively. The DOHGS responded linearly to HgBr2. We found no evidence that elevated O3 interfered in the DOHGS RM measurements. A reduction in RM collection and retention efficiencies at very high ambient WV mixing ratios is possible. Comparisons between the DOHGS and participating Hg instruments demonstrate good agreement for GEM and large discrepancies for RM. The results suggest that existing GOM measurements are biased low.

Do we understand what the mercury speciation instruments are actually measuring? Results of RAMIX.

From August 22 to September 16, 2012, atmospheric mercury (Hg) was measured from a common manifold in the field during the Reno Atmospheric Mercury Intercomparison eXperiment. Data were collected using Tekran systems, laser induced fluorescence, and evolving new methods. The latter included the University of Washington-Detector for Oxidized Mercury, the University of Houston Mercury instrument, and a filter-based system under development by the University of Nevada-Reno. Good transmission of total Hg was found for the manifold. However, despite application of standard protocols and rigorous quality control, systematic differences in operationally defined forms of Hg were measured by the sampling systems. Concentrations of reactive Hg (RM) measured with new methods were at times 2-to-3-fold higher than that measured by Tekran system. The low RM recovery by the latter can be attributed to lack of collection as the system is currently configured. Concentrations measured by all instruments were influenced by their sampling location in-the-manifold and the instrument analytical configuration. On the basis of collective assessment of the data, we hypothesize that reactions forming RM were occurring in the manifold. Results provide a new framework for improved understanding of the atmospheric chemistry of Hg.

Terpenoids as anti-inflammatory substances inhibiting COX-2 isolated from the fibrous roots of Alangium chinense (Lour.) Harms.

A new sesquiterpene, 1-carbonyl-2,8-dihydroxy-11-oxabicyclo [4,4,1] germacra- 2(3),4(5),6(7),8(9)-tetraene (1) and four known compounds (3E, 23E)-3-caffeoyl-23-coumaroylhederagenin (2), (3E, 23E)-dicoumaroylhederagenin (3), morettinone (4), 24-ehylcholesta-3,6-dione (5) were isolated from the ethyl acetate layer of the fibrous root of Alangium chinense (Lour.) Harms. The structure of compound 1 was characterized by its 1H-NMR, 13C-NMR, DEPT, HMBC, HSQC spectrums, and the structures of the known compounds were determined by comparison of their spectroscopic data with those reported by the literatures. The obtained compounds were evaluated for their anti-inflammatory against cyclooxygenase (COX-2). Compound 1 has a good inhibitory effect against COX-2 with IC50 20.43 ± 4.72 µM. The compounds 2-5 have inhibitory effect against COX-2 with IC50 49.19 ± 0.76, 23.29 ± 0.99, 47.78 ± 1.33, and 44.44 ± 0.12 µM, respectively.

Bioactive substances inhibiting COX-2 and cancer cells isolated from the fibrous roots of Alangium chinense (Lour.) Harms.

Alangium chinense has been used as a traditional folk medicine for centuries to treat rheumatism, skin diseases, and diabetes by the people of Southeast Asia. However, the bioactive constituents inhibiting COX-2 and cancer cells (HepG2, Caco-2, HeLa) remain unclear. In this study one new (14) along with twenty-four known compounds (1-13, 15-25) were isolated from the fibrous roots of Alangium chinense by chromatographic methods, and identified by NMR, and Gaussian and CD calculation. Compounds 1, 2, 13, 16, 17, 19, 20, 23, and 24 were isolated from this plant for the first time. Their inhibition effects on COX-2 enzyme and cancer cells were evaluated by MTT assay. Compounds 1-4, 13-14, and 16-18 can be used as good inhibitors against COX-2 enzyme, and compounds 1, 13, 14, and 17 were stronger than the positive control (celecoxib). In addition, molecular docking suggested that compounds 13, 17, and 18 belong to ellagic acids and have good inhibition against COX-2 enzyme. While compounds 1, 5, 13 and 21 showed cytotoxicity against HepG2 cells, compounds 2 and 21 showed cytotoxicity against Caco-2 cells, and compound 20 showed cytotoxicity against HeLa cells.

Empirical nitrogen and sulfur critical loads of U.S. tree species and their uncertainties with machine learning.

Critical loads (CLs) of atmospheric deposition for nitrogen (N) and sulfur (S) are used to support decision making related to air regulation and land management. Frequently, CLs are calculated using empirical methods, and the certainty of the results depends on accurate representation of underlying ecological processes. Machine learning (ML) models perform well in empirical modeling of processes with non-linear characteristics and significant variable interactions. We used bootstrap ensemble ML methods to develop CL estimates and assess uncertainties of CLs for the growth and survival of 108 tree species in the conterminous United States. We trained ML models to predict tree growth and survival and characterize the relationship between deposition and tree species response. Using four statistical methods, we quantified the uncertainty of CLs in 95 % confidence intervals (CI). At the lower bound of the CL uncertainty estimate, 80 % or more of tree species have been impacted by nitrogen deposition exceeding a CL for tree survival over >50 % of the species range, while at the upper bound the percentage is much lower (<20 % of tree species impacted across >60 % of the species range). Our analysis shows that bootstrap ensemble ML can be effectively used to quantify critical loads and their uncertainties. The range of the uncertainty we calculated is sufficiently large to warrant consideration in management and regulatory decision making with respect to atmospheric deposition.

Evidence for a free troposphere source of mercury in wet deposition in the Western United States.

Mercury (Hg) in wet deposition in the United States is measured as part of the National Atmospheric Deposition Program--Hg Deposition Network (MDN). This study focused on compiling and assessing data collected since 2003 at two sites in Nevada, and at one in Nevada and three in Idaho where data were collected over shorter time intervals. At all locations the highest volume weighted concentrations and deposition were observed in the summer, a time of low precipitation, but high gaseous oxidized Hg (GOM) concentrations. Detailed assessment of high Hg wet deposition events showed variability across the region and higher deposition at the higher elevation sites. Potential Source Contribution Function analyses showed no specific point sources associated with the high Hg wet deposition events, but air masses derived predominantly from the southwest. Although this region has potential local and regional sources of GOM, detailed back trajectory analyses, the environmental setting of Nevada, results from other studies in Nevada, and GEOS-Chem modeling results point toward a free troposphere contribution to mercury in wet deposition input to this area of the western United States.

An application of passive samplers to understand atmospheric mercury concentration and dry deposition spatial distributions.

Two modified passive samplers were evaluated at multiple field locations. The sampling rate (SR) of the modified polyurethane foam (PUF)-disk passive sampler for total gaseous mercury (TGM) using gold-coated quartz fiber filters (GcQFF) and gaseous oxidized mercury (GOM) using ion-exchange membranes (IEM) were 6.4 ± 1.4 and 15.3 ± 0.3 m(3) day(-1), respectively. The relative percent difference between TGM and GOM concentrations measured by a Tekran system and the passive samplers averaged 19 ± 14 and 13 ± 12% and ranged between 4-44 and 1.5-41%, respectively. The GcQFF and IEM substrates were also evaluated as collection media for surrogate surface dry deposition measurements. Mercury (Hg) concentration and dry deposition gradients were observed using these samplers at an urban/industrial site and compared to a rural/remote site. The Hg dry deposition rates measured by the surrogate surfaces were always higher than those calculated by a widely used inferential modeling method (1.3-50 fold). The Hg dry deposition measured at urban and suburban sites were comparable to those calculated from model. However, they were very different at a rural site, probably due to the low concentrations. Both methods are relatively low cost and will aid in understanding spatial distributions of Hg ambient air concentrations and dry deposition.

Air quality and health-related impacts of traditional and alternate jet fuels from airport aircraft operations in the U.S.

Aviation emissions from landing and takeoff operations (LTO) can degrade local and regional air quality leading to adverse health outcomes in populations near airports and downwind. In this study we aim to quantify the air quality and health-related impacts from commercial LTO emissions in the continental U.S. for two recent years' inventories, 2011 and 2016. We quantify the LTO-attributable PM2.5, O3, and NO2 concentrations and health outcomes for mortality and multiple morbidity health endpoints. We also quantify the impacts from two scenarios representing a nation-wide implementation of 5% or 50% blends of sustainable alternative jet fuels. We estimate 80 (68-93) and 88 (75-100) PM2.5-attributable and 610 (310-920) and 1,100 (570-1,700) NO2-attributable premature mortalities in 2011 and 2016, respectively. We estimate a net decrease of 28 (14-56) and 54 (27-110) in O3-attributable premature mortalities across the U.S. in 2011 and 2016, respectively due to the large O3 titration effects near the airports. We also find that the asthma exacerbations due to NO2 exposures from LTO emissions increase from 100,000 (2,500-200,000) in 2011 to 170,000 (4,400-340,000) in 2016. Implementing a 5% or 50% blend of sustainable alternative jet fuel in 2016 results in a 1% or 18% reduction, respectively in PM2.5-attributable premature mortalities. Monetizing the value of avoided total premature mortalities, we find that a 50%-blended sustainable alternative jet fuel results in a 19% decrease in PM2.5 damages per ton of fuel burned and a 2% decrease in total damages per ton of fuel burned as compared to damages from traditional jet fuel. We also quantify health impacts by state and find California to be the most impacted by LTO emissions. We find that LTO-attributable PM2.5 and NO2 premature mortalities increase by 10% and 80%, respectively from 2011 to 2016 and that NO2-attributable premature mortalities are responsible for 91% of total LTO-attributable premature mortalities in both 2011 and 2016. And since we find LTO-attributable NO2 to be unaffected by the implementation of sustainable alternative jet fuels, additional approaches focused on NOX reductions in the combustor are needed to mitigate the air quality-related health impacts from LTO emissions.

Group 3 Innate Lymphoid Cells Protect the Host from the Uropathogenic Escherichia coli Infection in the Bladder.

Innate lymphoid cells (ILCs) are crucial in orchestrating immunity and maintaining tissue homeostasis in various barrier tissues, but whether ILCs influence immune responses in the urinary tract remains poorly understood. Here, bladder-resident ILCs are comprehensively explored and identified their unique phenotypic and developmental characteristics. Notably, bladder-resident ILCs rapidly respond to uropathogenic Escherichia coli (UPEC) infection. It is found that ILC3 is necessary for early protection against UPEC infection in the bladder. Mechanistically, UPEC infection leads to interleukin (IL)-1ß production in the bladder via a MyD88-dependent pathway, which promotes ILC3 activation. ILC3-expressed IL-17A further recruits neutrophils and controls UPEC infection in the bladder. Together, these results demonstrate a critical role for bladder ILCs in the host defense against UPEC infection.

Gut microbial metabolites facilitate anticancer therapy efficacy by modulating cytotoxic CD8+ T cell immunity.

Recent studies in both mice and humans have suggested that gut microbiota could modulate tumor responsiveness to chemo- or immunotherapies. However, the underlying mechanism is not clear yet. Here, we found that gut microbial metabolites, especially butyrate, could promote the efficacy of oxaliplatin by modulating CD8+ T cell function in the tumor microenvironment. Butyrate treatment directly boosted the antitumor cytotoxic CD8+ T cell responses both in vitro and in vivo in an ID2-dependent manner by promoting the IL-12 signaling pathway. In humans, the oxaliplatin responder cancer patients exhibited a higher amount of serum butyrate than did non-responders, which could also increase ID2 expression and function of human CD8+ T cells. Together, our findings suggest that the gut microbial metabolite butyrate could promote antitumor therapeutic efficacy through the ID2-dependent regulation of CD8+ T cell immunity, indicating that gut microbial metabolites could be effective as a part of cancer therapy.

Impacts of the Canadian forest fires on atmospheric mercury and carbonaceous particles in Northern New York.

The impact of Canadian forest fires in Quebec on May 31, 2010 on PM(2.5), carbonaceous species, and atmospheric mercury species was observed at three rural sites in northern New York. The results were compared with previous studies during a 2002 Quebec forest fire episode. MODIS satellite images showed transport of forest fire smoke from southern Quebec, Canada to northern New York on May 31, 2010. Back-trajectories were consistent with this regional transport. During the forest fire event, as much as an 18-fold increase in PM(2.5) concentration was observed. The concentrations of episode-related OC, EC, BC, UVBC, and their difference (Delta-C), reactive gaseous mercury (RGM), and particle-bound mercury (PBM) were also significantly higher than those under normal conditions, suggesting a high impact of Canadian forest fire emissions on air quality in northern New York. PBM, RGM, and Delta-C are all emitted from forest fires. The correlation coefficient between Delta-C and other carbonaceous species may serve as an indicator of forest fire smoke. Given the marked changes in PBM, it may serve as a more useful tracer of forest fires over distances of several hundred kilometers relative to GEM. However, the Delta-C concentration changes are more readily measured.