Removal of NOx from lean exhaust gas by storage/reduction on H3PW12O40 x 6H2O supported on Ce(x)Zr4-xO8

We have demonstrated the interest of using Zr-Ce mixed oxides as supports for the system H3PW12O40 x 6H2O (HPW) and Pt for the storage (absorption into HPW and adsorption on Zr-Ce support)-reduction of NOx. Zr-Ce oxides adsorb NOx (mainly NO2) as nitrates, which are desorbed thermally as NO2 and NO (12 mg of NOx x g(-1)). On (HPW-Pt)/Zr-Ce system, NO and NO2 are stored equimolarly by substitution of water molecules of the HPW structure. The Zr/Ce support molar ratio has an important influence on the quantity of NOx stored with a maximum for the system Zr/Ce = 0.5. The presence of Pt has no influence on storage capacity but rather on its efficiency, and it is essential when reducing. Pt strongly accelerates both NOx desorption and reduction processes. Reduction of NOx occurs with H2, CO, or an H2/CO mixture. With H2, NO2 is reduced to NO. With CO, it seems reasonable that the mechanism of NO2 reduction concerns its reaction with CO to produce CO2 and NO. Addition of H2 to CO accelerates the reduction process. However, the difference between NOx stored and desorbed implies also the presence of another reduction step. This could be related to an NO interaction with an active site which produces its decomposition with nitrogen as product. The catalytic system proposed is highly selective since no N2O formation was detected.     

Effects of natural water ions and humic acid on catalytic nitrate reduction kinetics using an alumina supported Pd-Cu catalyst

Catalytic nitrate reduction was evaluated for the purpose of drinking water treatment. Common anions present in natural waters and humic acid were evaluated for their effects on NO3(-) hydrogenation over a bimetallic supported catalyst (Pd-Cu/gamma-Al2O3). Groundwater samples, with and without powder activated carbon (PAC) pretreatment, were also evaluated. In the absence of inhibitors the NO3- reduction rate was 2.4 x 10(-01) L/min g cat. However, the addition of constituents (SO4(2-), SO3(2-), HS-, CI-, HCO3-, OH-, and humic acid) on the order of representative concentrations for drinking water decreased the NO3- reduction rate. Sulfite, sulfide, and elevated chloride decreased the NO3- reduction rate by over 2 orders of magnitude. Preferential adsorption of Cl- inhibited NO3- reduction to a greater extent than NO2- reduction. Partial regeneration of catalysts exposed to SO3(2-) was achieved by using a dilute hypochlorite solution, however Cu dissolution occurred. Dissolved constituents in the groundwater sample decreased the NO3- reduction rate to 3.7 x 10(-03) L/min g cat and increased ammonia production. Removal of dissolved organic matter from the groundwater using PAC increased the NO3- reduction rate to 5.06 x 10(-02) L/min g cat and decreased ammonia production. Elemental analyses of catalysts exposed to the natural groundwater suggest that mineral precipitation may also contribute to catalyst fouling.     

Selective photocatalytic oxidation of NH3 to N2 on platinized TiO2 in water

Selective photocatalytic oxidation of NH3 to N2 is proposed as a new treatment method for controlling the levels of ammonia in water. The photocatalytic oxidation of ammonia on naked and metallized TiO2 in water saturated with air, nitrogen, or NO2 gas was investigated. While the slow photocatalytic oxidation of NH3 to NO2-/NO3- is the only pathway for decomposition of NH3 on naked TiO2 and Au/TiO2, a new pathway, that of selective oxidation of ammonia to dinitrogen, opens up on Pt/TiO2. The formation of dinitrogen from the oxidation of 15NH3 was confirmed by mass spectrometric detection of 15N2. The photocatalytic conversion of NH3 to N2 greatly increases when the Pt/TiO2 suspension is saturated with NO2 gas, whereas NO2 itself shows little reactivity with naked TiO2 and Au/TiO2. Over 80% of the total nitrogen available in ammonia (0.1 mM) is converted into N2 within 40 min illumination of the N2O-saturated Pt/TiO2 suspension. The ability of N2O to accept the conduction band electrons of Pt/TiO2 was verified by photoelectrochemical measurements. NO2 reductively decomposes to generate OH radicals on Pt/TiO2; the rate of ammonia degradation in the NO2-saturated Pt/TiO2 suspension significantly decreases in the presence of excess tert-butyl alcohol, an OH radical scavenger. The presence of Pt deposits on the TiO2 particles changes the photocatalytic pathway of ammonia conversion by both enhancing OH radical production from NO2 and stabilizing intermediate NHx (x=0, 1, 2) species to facilitate their recombination into N2.     

DRIFT study of manganese/ titania-based catalysts for low-temperature selective catalytic reduction of NO with NH3

Manganese oxides and iron-manganese oxides supported on TiO2 were prepared by the sol-gel method and used for low-temperature selective catalytic reduction (SCR) of NO with NH3. Base on the previous study, Mn(0.4)/ TiO2 and Fe(0.1)-Mn(0.4)/TiO2 were then selected to carry out the in situ diffuse reflectance infrared transform spectroscopy (DRIFT) investigation for revealing the reaction mechanism. The DRIFT spectroscopy for the adsorption of NH3 indicated the presence of coordinated NH3 and NH4+ on both of the two catalysts. When NO was introduced, the coordinated NH3 on the catalyst surface was consumed rapidly, indicating these species could react with NO effectively. When NH3 was introduced into the sample preadsorbed with NO + O2, SCR reaction would not proceed on Mn(0.4)/TiO2. However, for Fe(0.1)-Mn(0.4)/ TiO2 the bands due to coordinated NH3 on Fe2O3 were formed. Simultaneously, the bidentate nitrates were transformed to monodentate nitrates and NH4+ was detected. And NO2 from the oxidation of NO on catalyst could react with NH4+ leading to the reduction of NO. Therefore, it was suggested that the SCR reaction on Fe(0.1)-Mn(0.4)/TiO2 could also take place in a different way from the reactions on Mn(0.4)/TiO2 proposed by other researchers. Furthermore, the SCR reaction steps for these two kinds of catalysts were proposed.     

Regeneration of sulfur-fouled bimetallic Pd-based catalysts

Pd-based catalysts provide efficient and selective reduction of several drinking water contaminants, but their long-term application requires effective treatments for catalyst regeneration following fouling by constituents in natural waters. This studytested alumina-supported Pd-Cu and Pd-In bimetallic catalysts for nitrate reduction with H2 after sulfide fouling and oxidative regeneration procedures. Both catalysts were severely deactivated after treatment with microM levels of sulfide. Regeneration was attempted with dissolved oxygen, hydrogen peroxide, sodium hypochlorite, and heated air. Only sodium hypochlorite and heated air were effective regenerants, specifically restoring nitrate reduction rates for a Pd-In/gamma-Al2O3 catalyst from 20% to between 39 and 60% of original levels. Results from ICP-MS revealed that sodium hypochlorite caused dissolution of Cu from the Pd-Cu catalyst but that the Pd-In catalyst was chemically stable over a range of sulfide fouling and oxidative regenerative conditions. Analysis byXPS indicated that PdS and In2S3 complexes form during sulfide fouling, where sulfur is present as S2-, and that regeneration with sodium hypochlorite converts a portion of the S2- to S6+, with a corresponding increase in reduction rates. These results indicate that Pd-In catalysts show exceptional promise for being robust under fouling and regeneration conditions that may occur when treating natural waters.     

Photocatalytic activity for degradation of nitrogen oxides over visible light responsive titania-based photocatalysts

This study investigates photocatalytic degradation of nitrogen oxides overtitania-based photocatalysts illuminated by ultraviolet and visible light. The TiO2 photocatalyst was synthesized in a sol-gel process using titanium butoxide as the precursor. After calcination between 150 and 300 degrees C, the synthesized TiO2 responded strongly to visible light photocatalytically degrading NO(x), probably because of the existence of carbonaceous species that act as sensitizers. The optimum calcination temperature was found to be around 200 degrees C. Additionally, platinum ion-doped TiO2 was prepared by impregnation using Pt(NH3)4(NO3)2 as a dopant, which improved the photocatalytic activity that degraded NO(x) in the visible light region. The Pt ion was doped in oxide form at the surface of TiO2 and was expected to be responsible for sensitization. At an optimum calcination temperature of around 200 degrees C, the Pt ion-doped TiO2 exhibited higher activity in the further oxidation of NO2 to NO3- clearly reducing NO2 selectivity. The TiO2 catalysts chemically prepared by either the sol-gel process or impregnation exhibited stronger activity than conventional TiO2 when illuminated under a fluorescent lamp. Rinsing with water was responsible for the restored reactivity of prepared TiO2 catalysts for NO(x) degradation.     

DRIFT study on cerium-tungsten/titania catalyst for selective catalytic reduction of NOx with NH3

CeO(2)/TiO(2) and CeO(2)-WO(3)/TiO(2) catalysts prepared by impregnation method assisted with ultrasonic energy were investigated on the selective catalytic reduction (SCR) of NO(x) (NO and NO(2)) by NH(3). The catalytic activity of 10% CeO(2)/TiO(2) (CeTi) was greatly enhanced by the addition of 6% WO(3) in the broad temperature range of 200-500 °C, the promotion mechanism was proposed on basis of the results of in situ diffuse reflectance infrared transform spectroscopy (DRIFT). When NH(3) was introduced into both catalysts preadsorbed with NO + O(2), SCR would not proceed except for the reaction between NO(2) and ammonia. For CeO(2)/TiO(2) catalysts, coordinated NH(3) linked to Lewis acid sites were the main adsorbed ammonia species. When NO + O(2) was introduced, all the ammonia species consumed rapidly, indicating that these species could react with NO(x) effectively. Two different reaction routes, L-H mechanism at low temperature (<200 °C) and E-R mechanism at high temperatures (>200 °C), were presented for SCR reaction over CeO(2)/TiO(2) catalyst. For CeO(2)-WO(3)/TiO(2) catalysts, the Lewis acid sites on Ce(4+) state could be converted to Br?nsted acid sites due to the unsaturated coordination of Ce(n+) and W(n+) ions. When NO + O(2) was introduced, the reaction proceeded more quickly than that on CeO(2)/TiO(2). The reaction route mainly followed E-R mechanism in the temperature range investigated (150-350 °C) over CeO(2)-WO(3)/TiO(2) catalysts. Tungstation was beneficial for the formation of Ce(3+), which would influence the active sites of the catalyst and further change the mechanisms of SCR reaction. In this way, the cooperation of tungstation and the presence of Ce(3+) state resulted in the better activity of CeO(2)-WO(3)/TiO(2) compared to that of CeO(2)/TiO(2).     

Direct Spectroscopic Evidence of CO Spillover and Subsequent Reaction with Preadsorbed NO(x) on Pd and K Cosupported Mg-Al Mixed Oxides

The CO adsorption and subsequent reaction with preadsorbed NO(x) on Pd and K cosupported Mg-Al mixed oxides (Pd-K/MgAlO, 1/8/100 w/w) were investigated using in situ FTIR spectroscopy. During CO adsorption, a peculiar and well-defined IR band at 2160 cm(-1) was observed. Several elaborately designed experiments such as the competitive adsorption of CO and CO(2) demonstrated that the 2160 cm(-1) band was exclusively assigned to a carbonyl species on K sites due to the CO spillover from Pd to K, which results from a strong Pd-K interaction based on temperature-programmed reduction with H(2) experiments. Importantly, the spillover of CO is found to be involved in the reduction of preadsorbed NO(x) from temperature-programmed surface reactions with CO. Thus, all adsorbed NO(x) can be reduced by CO before desorption. Like the process of "pumping" CO by Pd from the atmosphere to "irrigate the field" of the nitrates/nitrites, the adsorbed NO(x) at not only K sites adjacent to Pd but also at the remote K sites can be reduced into N(2) and N(2)O effectively.     

Electrochemical enhancement of nitric oxide removal from simulated lean-burn engine exhaust via solid oxide fuel cells

A solid oxide fuel cell (SOFC) unit is constructed with Ni-YSZ as the anode, YSZ as the electrolyte, and La(0.6)Sr(0.4)CoO(3)-Ce(0.9)Gd(0.1)O(1.95) as the cathode. The SOFC operation is performed at 600 °C with a cathode gas simulating the lean-burn engine exhaust and at various fixed voltage, at open-circuit voltage, and with an inert gas flowing over the anode side, respectively. Electrochemical enhancement of NO decomposition occurs when an operating voltage is generated; higher O(2) concentration leads to higher enhancement. Smaller NO concentration results in larger NO conversion. Higher operating voltage and higher O(2) concentration can lead to both higher NO conversion and lower fuel consumption. The molar rate of the consumption of the anode fuel can be very much smaller than that of NO to N(2) conversion. This makes the anode fuel consumed in the SOFC-DeNO(x) process to be much less than the equivalent amount of ammonia consumed in the urea-based selective catalytic reduction process. Additionally, the NO conversion increases with the addition of propylene and SO(2) into the cathode gas. These are beneficial for the application of the SOFC-DeNO(x) technology on treating diesel and other lean-burn engine exhausts.     

Alkali metal poisoning of a CeO2-WO3 catalyst used in the selective catalytic reduction of NOx with NH3: an experimental and theoretical study

The alkali metal-induced deactivation of a novel CeO(2)-WO(3) (CeW) catalyst used for selective catalytic reduction (SCR) was investigated. The CeW catalyst could resist greater amounts of alkali metals than V(2)O(5)-WO(3)/TiO(2). At the same molar concentration, the K-poisoned catalyst exhibited a greater loss in activity compared with the Na-poisoned catalyst below 200 °C. A combination of experimental and theoretical methods, including NH(3)-TPD, DRIFTS, H(2)-TPR, and density functional theory (DFT) calculations, were used to elucidate the mechanism of the alkali metal deactivation of the CeW catalyst in SCR reaction. Experiments results indicated that decreases in the reduction activity and the quantity of Br?nsted acid sites rather than the acid strength were responsible for the catalyst deactivation. The DFT calculations revealed that Na and K could easily adsorb on the CeW (110) surface and that the surface oxygen could migrate to cover the active tungsten, and then inhibit the SCR of NO(x) with ammonia. Hot water washing is a convenient and effective method to regenerate alkali metal-poisoned CeW catalysts, and the catalytic activity could be recovered 90% of the fresh catalyst.     

Development of silica/vanadia/titania catalysts for removal of elemental mercury from coal-combustion flue gas

SiO2/V2O5/TiO2 catalysts were synthesized for removing elemental mercury (Hg0) from simulated coal-combustion flue gas. Experiments were carried out in fixed-bed reactors using both pellet and powder catalysts. In contrast to the SiO2-TiO2 composites developed in previous studies, the V2O5 based catalysts do not need ultraviolet light activation and have higher Hg0 oxidation efficiencies. For Hg0 removal by SiO2-V2O5 catalysts, the optimal V2O5 loading was found between 5 and 8%, which may correspond to a maximum coverage of polymeric vanadates on the catalyst surface. Hg0 oxidation follows an Eley-Rideal mechanism where HCI, NO, and NO2 are first adsorbed on the V2O5 active sites and then react with gas-phase Hg0. HCI, NO, and NO2 promote Hg oxidation, while SO2 has an insignificant effect and water vapor inhibits Hgo oxidation. The SiO2-TiO2-V2O5 catalysts exhibit greater Hg0 oxidation efficiencies than SiO2-V2O5, may be because the V-O-Ti bonds are more active than the V-O-Si bonds. This superior oxidation capability is advantageous to power plants equipped with wet-scrubbers where oxidized Hg can be easily captured. The findings in this work revealed the importance of optimizing the composition and microstructures of SCR (selective catalytic reduction) catalysts for Hg0 oxidation in coal-combustion flue gas.     

Atmospheric reactive nitrogen in china: sources, recent trends, and damage costs

Human activities have intensely altered the global nitrogen cycle and produced nitrogenous gases of environmental significance, especially in China where the most serious atmospheric nitrogen pollution worldwide exists. We present a comprehensive assessment of ammonia (NH(3)), nitrogen oxides (NO(x)), and nitrous oxide (N(2)O) emissions in China based on a full cycle analysis. Total reactive nitrogen (Nr) emission more than doubled over the past three decades, during which the trend of increase slowed for NH(3) emissions after 2000, while the trend of increase continued to accelerate for NO(x) and N(2)O emissions. Several hotspots were identified, and their Nr emissions were about 10 times higher than others. Agricultural sources take 95% of total NH(3) emission; fossil fuel combustion accounts for 96% of total NO(x) emission; agricultural (51%) and natural sources (forest and surface water, 39%) both contribute to the N(2)O emission in China. Total atmospheric Nr emissions related health damage in 2008 in China reached US$19-62 billion, accounting for 0.4-1.4% of China's gross domestic product, of which 52-60% were from NH(3) emission and 39-47% were from NO(x) emission. These findings provide policy makers an integrated view of Nr sources and health damage to address the significant challenges associated with the reduction of air pollution.     

Development of nano-niO/Al2O3 catalyst to be used for tar removal in biomass gasification

The objective of this study isto develop a novel supported nano-NiO catalyst for tar removal in biomass gasification/pyrolysis, to significantly enhance the quality of the produced gases. For this purpose, the supported nano-NiO/gamma-Al2O3 catalyst was prepared by deposition-precipitation (DP) method. Different analytical approaches such as XRD, BET, TEM and SEM/EDX were used to characterize the synthesized catalysts. The results showed thatthe prepared nano-NiO/gamma-Al2O3 catalysts had a coated structure with a loading of NiO in catalysts over 12 wt %, and they had also a higher BET surface area over commercial nickel based catalysts. The active components of catalyst were spherical NiO nanoparticles coated on the surface of supports with a size range of 12-18 nm. Furthermore, the activity of the catalysts to remove tar in the process of biomass pyrolysis was also investigated using a bench-scale combined fixed bed reactor. The experiments demonstrated that the tar yield after addition of the catalyst was reduced significantly; the tar removal efficiency reached to 99% for catalytic pyrolysis at 800 degrees C, and the gas yield after addition of the catalyst increased markedly. The compositions of gas products before and after addition of the catalyst in the process also changed significantly. The percentages of CO2 and CH4 in the product gas after addition of the catalysts were obviously reduced, while those of the valuable H2 and CO strongly increased. Therefore, using the prepared NiO/gamma-Al2O3 catalyst in biomass gasification/pyrolysis can significantly improve the quality of the produced gas and meanwhile efficiently eliminate the tar generation.     

Ag/γ-Al2O3催化剂的制备及其对亚甲基蓝的降解性能

以AgNO3和γ-Al2O3为原料,NaBH4和PVP分别作为还原剂和表面活性剂,制备得到Ag/γ-Al2O3复合材料。利用X射线衍射仪、透射电镜和比表面仪表征Ag/γ-Al2O3,结果表明:Ag纳米颗粒在γ-Al2O3表面具有良好的分散性。以亚甲基蓝溶液为模拟印染废水,NaBH4为还原剂,研究了Ag/γ-Al2O3的催化性能,结果表明:Ag/γ-Al2O3具有良好的催化活性,当催化剂用量为1.5 g/L,500 r/min搅拌60 s后,对亚甲基蓝溶液的降解率达到95.7%,催化剂可多次回收使用。     

Significance of RuO2 modified SCR catalyst for elemental mercury oxidation in coal-fired flue gas

Catalytic conversion of elemental mercury (Hg(0)) to its oxidized form has been considered as an effective way to enhance mercury removal from coal-fired power plants. In order to make good use of the existing selective catalytic reduction of NO(x) (SCR) catalysts as a cobenefit of Hg(0) conversion at lower level HCl in flue gas, various catalysts supported on titanium dioxide (TiO(2)) and commercial SCR catalysts were investigated at various cases. Among the tested catalysts, ruthenium oxides (RuO(2)) not only showed rather high catalytic activity on Hg(0) oxidation by itself, but also appeared to be well cooperative with the commercial SCR catalyst for Hg(0) conversion. In addition, the modified SCR catalyst with RuO(2) displayed an excellent tolerance to SO(2) and ammonia without any distinct negative effects on NO(x) reduction and SO(2) conversion. The demanded HCl concentration for Hg(0) oxidation can be reduced dramatically, and Hg(0) oxidation efficiency over RuO(2) doped SCR catalyst was over 90% even at about 5 ppm HCl in the simulated gases. Ru modified SCR catalyst shows a promising prospect for the cobenefit of mercury emission control.     

Plasma-TiO2 catalytic method for high-efficiency remediation of p-nitrophenol contaminated soil in pulsed discharge

Nonthermal discharge plasma and TiO(2) photocatalysis are two techniques capable of organic pollutants removal in soil. In the present study, a pulsed discharge plasma-TiO(2) catalytic (PDPTC) technique by combining the two means, where catalysis of TiO(2) is driven by the pulsed discharge plasma, is proposed to investigate the remediation of p-nitrophenol (PNP) contaminated soil. The experimental results showed that 88.8% of PNP was removed within 10 min of treatment in PDPTC system and enhancing pulse discharge voltage was favorable for PNP degradation. The mineralization of PNP and intermediates generated during PDPTC treatment was followed by UV-vis spectra, denitrification, total organic carbon (TOC), and CO(x) selectivity analyses. Compared with plasma alone system, the enhancement effects on PNP degradation and mineralization were attributed to more amounts of chemically active species (e.g., O(3) and H(2)O(2)) produced in the PDPTC system. The main intermediates were identified as hydroquinone, benzoquinone, catechol, phenol, benzo[d][1, 2, 3]trioxole, acetic acid, formic acid, NO(2)(-), NO(3)(-), and oxalic acid. The evolution of the main intermediates with treatment time suggested the enhancement effect of the PDPTC system. A possible pathway of PNP degradation in soil in such a system was proposed.     

Saturated zone denitrification: potential for natural attenuation of nitrate contamination in shallow groundwater under dairy operations

We present results from field studies at two central California dairies that demonstrate the prevalence of saturated-zone denitrification in shallow groundwater with 3H/ 3He apparent ages of < 35 years. Concentrated animal feeding operations are suspected to be major contributors of nitrate to groundwater, but saturated zone denitrification could mitigate their impact to groundwater quality. Denitrification is identified and quantified using N and O stable isotope compositions of nitrate coupled with measurements of excess N2 and residual NO3(-) concentrations. Nitrate in dairy groundwater from this study has delta15N values (4.3-61 per thousand), and delta18O values (-4.5-24.5 per thousand) that plot with delta18O/delta15N slopes of 0.47-0.66, consistent with denitrification. Noble gas mass spectrometry is used to quantify recharge temperature and excess air content. Dissolved N2 is found at concentrations well above those expected for equilibrium with air or incorporation of excess air, consistent with reduction of nitrate to N2. Fractionation factors for nitrogen and oxygen isotopes in nitrate appear to be highly variable at a dairy site where denitrification is found in a laterally extensive anoxic zone 5 m below the water table, and at a second dairy site where denitrification occurs near the water table and is strongly influenced by localized lagoon seepage.     

NO(x) removal from simulated flue gas by chemical absorption-biological reduction integrated approach in a biofilter

A chemical absorption-biological reduction integrated approach, which combines the advantages of both the chemical and biological technologies, is employed to achieve the removal of nitrogen monoxide (NO) from the simulated flue gas. The biological reduction of NO to nitrogen gas (N2) and regeneration of the absorbent Fe(II)EDTA (EDTA:ethylenediaminetetraacetate) take place under thermophilic conditions (50 +/- 0.5 degrees C). The performance of a laboratory-scale biofilter was investigated for treating NO(x) gas in this study. Shock loading studies were performed to ascertain the response of the biofilter to fluctuations of inlet loading rates (0.48 approximately 28.68 g NO m(-3) h(-1)). A maximum elimination capacity (18.78 g NO m(-3) h(-1)) was achieved at a loading rate of 28.68 g NO m(-3) h(-1) and maintained 5 h operation at the steady state. Additionally, the effect of certain gaseous compounds (e.g., O2 and SO2) on the NO removal was also investigated. A mathematical model was developed to describe the system performance. The model has been able to predict experimental results for different inlet NO concentrations. In summary, both theoretical prediction and experimental investigation confirm that biofilter can achieve high removal rate for NO in high inlet concentrations under both steady and transient states.     

Nitrogen isotopes as indicators of NO(x) source contributions to atmospheric nitrate deposition across the midwestern and northeastern United States

Global inputs of NO(x) are dominated by fossil fuel combustion from both stationary and vehicular sources and far exceed natural NO(x) sources. However, elucidating NO(x) sources to any given location remains a difficult challenge, despite the need for this information to develop sound regulatory and mitigation strategies. We present results from a regional-scale study of nitrogen isotopes (delta15N) in wet nitrate deposition across 33 sites in the midwestern and northeastern U.S. We demonstrate that spatial variations in delta15N are strongly correlated with NO(x) emissions from surrounding stationary sources and additionally that delta15N is more strongly correlated with surrounding stationary source NO(x) emissions than pH, SO4(2-), or NO3- concentrations. Although emission inventories indicate that vehicle emissions are the dominant NO(x) source in the eastern U.S., our results suggest that wet NO3- deposition at sites in this study is strongly associated with NO(x) emissions from stationary sources. This suggests that large areas of the landscape potentially receive atmospheric NO(y) deposition inputs in excess of what one would infer from existing monitoring data alone. Moreover, we determined that spatial patterns in delta15N values are a robust indicator of stationary NO(x) contributions to wet NO3- deposition and hence a valuable complement to existing tools for assessing relationships between NO3- deposition, regional emission inventories, and for evaluating progress toward NO(x) reduction goals.