NH2OH与NO2−对anammox体系中N2O排放的影响

厌氧氨氧化(anammox)为新型生物脱氮工艺,面临N₂O温室气体排放问题。羟胺(NH₂OH)与亚硝酸盐 (NO₂⁻) 是影响anammox体系N₂O排放的重要环境因子。基于批次实验,考察了不同质量浓度NH₂OH和NO₂⁻对anammox体系中N₂O释放的影响。结果表明,在[NO₂⁻]为100~300mg·L⁻¹条件下,N₂O排放量随NH₂OH质量浓度递增;而当[NO₂⁻]增至300~500 mg·L⁻¹,投加高质量浓度NH₂OH(30、50 mg·L⁻¹)能抑制N₂O的产生。微生物群落多样性分析表明,低[NO₂⁻]的环境中,NH₂OH会增加体系中异养菌的相对丰度,并抑制anammox菌的生长;而在高[NO₂⁻]的环境中,高质量浓度的NH₂OH可促进anammox菌与共存异养细菌的生长。功能基因分析表明,N₂O的排放量受到硝化、反硝化及硝酸盐异化还原产铵(DNRA)代谢途径调控,并与norB、nrfA基因丰度呈显著正相关(P<0.05 ) 。因此,anammox体系N₂O产量受到NO₂⁻与NH₂OH综合作用的影响,当进水[NO₂⁻]较高时可通过投加适量NH₂OH降低N₂O排放量,而当进水NO₂⁻不足时可通过抑制NH₂OH的累积量以减少N₂O的生成。该研究结果可为anammox工艺的低碳运行提供参考。     

Determining seasonal greenhouse gas emissions from ground-level area sources in a dairy operation in central Texas

Greenhouse gas (GHG) emissions from agricultural production operations are recognized as an important air quality issue. A new technique following the U.S. Environmental Protection Agency Method TO-14A was used to measure GHG emissions from ground-level area sources (GLAS) in a free-stall dairy operation in central Texas. The objective of this study was to quantify and report GHG emission rates (ERs) from the dairy during the summer and winter using this protocol. A weeklong sampling was performed during each season. A total of 75 and 66 chromatograms of air samples were acquired from six delineated GLAS (loafing pen, walkway, barn, silage pile, settling basin, and lagoon) of the same dairy during summer and winter, respectively. Three primary GHGs--methane (CH4), carbon dioxide (CO2), and nitrous oxide (N2O)--were identified from the dairy operation during the sampling periods. The estimated overall ERs for CH4, CO2, and N2O during the summer for this dairy were 274, 6005, and 7.96 g head(-1)day(-1), respectively. During the winter, the estimated overall CH4, CO2, and N2O ERs were 52, 7471, and 3.59 g head(-1)day(-1), respectively. The overall CH4 and N2O ERs during the summer were approximately 5.3 and 2.2 times higher than those in the winter for the free-stall dairy. These seasonal variations were likely due to fluctuations in ambient temperature, dairy manure loading rates, and manure microbial activity of GLAS. The annualized ERs for CH4, CO2, and N2O for this dairy were estimated to be 181, 6612, and 6.13 g head(-1)day(-1), respectively. Total GHG emissions calculated for this dairy with 500 cows were 2250 t of carbon dioxide equivalent (CO2e) per year.     

Determination of the nitrous oxide emission potential of deammonification under anoxic conditions

Various studies have been performed to determine nitrous oxide (N2O) emissions from conventional biological nitrogen removal processes in wastewater treatment like nitrification and denitrification in the main stream. However, with respect to the overall emissions of a wastewater treatment plant, part-stream treatment for high-strength wastewater (e.g., sludge liquor) is also expected to hold a significant emission potential because of high concentrations and extreme boundary conditions. This paper presents results from a laboratory-scale study on nitrous oxide production by biomass from a deammonification process (nitritation + anammox) under anoxic conditions. It was discovered that N2O formation results from incomplete endogenous denitrification rather than anammox and is dependent on substrate availability. Based on direct measurements of the dissolved N2O concentrations in a sequencing batch reactor, the dynamic behavior of N2O production is characterized in more detail. The results show that, during anoxic conditions, the N2O emission potential of deammonification is significantly lower than from conventional denitrification.     

SBBR工艺硝化过程中DO对N2O产生量的影响

利用生物膜序批式反应器(SBBR),考察不同溶解氧(DO)条件下硝化过程中N2O产生及释放过程。研究结果表明:DO浓度增大有利于控制系统中N2O的产生;DO浓度分别为(1.92±0.14)mg/L、(2.34±0.11)mg/L和(2.70±0.11)mg/L时,硝化过程中N2O释放因子(N2O总产量与NH4+-N转化量的比值)分别为5.47%、5.36%和4.77%。分析其原因主要是DO浓度的减小使DO对生物膜的穿透力降低,氧传递能力减弱后生物膜系统内易发生以N2O为产物的氨氧化细菌(AOB)反硝化反应。同时,在研究的3种不同的DO条件下,低DO运行条件更有利于SBBR实现亚硝酸盐型同步硝化反硝化。     

鱼菜共生系统氮素迁移转化的研究与优化

中国是世界上最大的水产养殖国,但是含有大量氮元素化合物的养殖废水对周围环境的污染已经成为影响该行业可持续发展的关键因素。鱼菜共生系统被认为是解决这一问题的有效途径。作为一种新兴的生态系统,目前对鱼菜共生系统中氮元素迁移转化规律的研究较少。通过对实验室规模的鱼菜共生系统进行研究,揭示系统内氮的迁移转化规律,掌握N2O的释放规律,同时尝试采用填料级配分层、添加硝化细菌等方式对系统进行优化。研究结果表明,投入系统的饵料中氮素以氨氮的形式被排出鱼体外后,在微生物作用下转化为亚硝酸盐氮及硝酸盐氮,进一步被植物吸收利用,提高了氮的利用效率。鱼菜共生系统以N2O形式释放的氮素约占氮素总输入的1.54%,与普通水产养殖相比,其N2O转化率没有明显增加。另外,采用填料级配分层以及添加硝化细菌等方法对系统进行优化,可促进系统内硝酸盐的积累,减少N2O释放,提高系统的经济效益和环境效益。     

A comparative analysis of using trip-based versus link-based traffic data for regional mobile source emissions estimation

The current method used for calculating vehicle emissions integrates travel data and associated vehicle emission factors. Travel data from traditional travel demand models are normally link-based (e.g., volumes on roadway segments), while California emission factors are trip-based (i.e., average emission factors over an entire trip), creating a mismatch in the modeling interface. Using dynamic simulation for trip assignment, we present a new modeling framework that consistently provides both trip-based and link-based VMT-speed distributions. Using the Sacramento Metropolitan Area and Kern County in California, we demonstrate the feasibility of this new method and quantify the effects of using trip-based versus link-based travel data on regional peak period emission inventories. The comparison results indicate that for the base scenario in both studied regions, the link-based method generally results in higher emissions than the trip-based method. The sensitivities of the link and trip-based methods to road network variations also appear dissimilar. The link-based emissions are more sensitive to facility-related changes, while the trip-based emissions are more sensitive to demand-related changes. This suggests that greater care may need to be taken to specify the effects of this modeling interface issue within the transportation conformity process and subsequent mobile emissions analysis.     

Real-time ozone mapping using a regression-interpolation hybrid approach, applied to Tucson, Arizona

Real-time ozone (O3) maps, intended for public access and mass media, are generated from spatially interpolating (i.e., kriging) sparse monitoring data and are typically characterized by over-smoothed surfaces that inadequately represent local-scale spatial patterns (e.g., averaged over 1 km2). In this paper, a hybrid regression-interpolation methodology is developed to enhance the representation of local-scale spatiotemporal patterns with an application to Tucson, Arizona. The mapping of local patterns is enhanced with pre-interpolation regression modeling of local-scale deviation-from-mean variability, preserving variation in the monitor data that is ubiquitous across the modeling domain (i.e., the areal mean). The model is trained on several years of deviation-from-mean hourly O3 data, and predictor variables are developed using theoretically and empirically derived proxy regression variables. The regression model explains a significant proportion of the variation in the data (r2 = 0.54), with an average error of 7.1 ppb. When augmented with the areal mean, the r2 of the pre-interpolation model increases to 0.847. Model residuals are then spatially interpolated to the extents of the modeling domain. Final concentration estimate maps are the summation of areal mean, regression, and spatially interpolated surfaces, preserving absolute values at monitor locations.     

Quantification of hourly variability in NO(x) emissions for baseload coal-fired power plants

The objectives of this paper are to (1) quantify variability in hourly utility oxides of nitrogen (NO(x)) emission factors, activity factors, and total emissions; (2) investigate the autocorrelation structure and evaluate cyclic effects at short and long scales of the time series of total hourly emissions; (3) compare emissions for the ozone (O3) season versus the entire year to identify seasonal differences, if any; and (4) evaluate interannual variability. Continuous emissions monitoring data were analyzed for 1995 and 1998 for 32 units from nine baseload power plants in the Charlotte, NC, airshed. Unit emissions have a strong 24-hr cycle attributable primarily to the capacity factor. Typical ranges of the coefficient of variation for emissions at a given hour of the day were from 0.2 to 0.45. Little difference was found when comparing weekend emissions with the entire week or when comparing the O3 season with the entire year. There were substantial differences in the mean and standard deviation of emissions when comparing 1995 and 1998 data, indicative of the effect of retrofits of control technology during the intervening time. The wide range of variability and its autocorrelation should be accounted for when developing probabilistic utility emission inventories for analysis of near-term future episodes.     

Toxic emissions from mobile sources: a total fuel-cycle analysis for conventional and alternative fuel vehicles

Mobile sources are among the largest contributors of four hazardous air pollutants--benzene, 1,3-butadiene, acetaldehyde, and formaldehyde--in urban areas. At the same time, federal and state governments are promoting the use of alternative fuel vehicles as a means to curb local air pollution. As yet, the impact of this movement toward alternative fuels with respect to toxic emissions has not been well studied. The purpose of this paper is to compare toxic emissions from vehicles operating on a variety of fuels, including reformulated gasoline (RFG), natural gas, ethanol, methanol, liquid petroleum gas (LPG), and electricity. This study uses a version of Argonne National Laboratory's Greenhouse Gas, Regulated Emissions, and Energy Use in Transportation (GREET) model, appropriately modified to estimate toxic emissions. The GREET model conducts a total fuel-cycle analysis that calculates emissions from both downstream (e.g., operation of the vehicle) and upstream (e.g., fuel production and distribution) stages of the fuel cycle. We find that almost all of the fuels studied reduce 1,3-butadiene emissions compared with conventional gasoline (CG). However, the use of ethanol in E85 (fuel made with 85% ethanol) or RFG leads to increased acetaldehyde emissions, and the use of methanol, ethanol, and compressed natural gas (CNG) may result in increased formaldehyde emissions. When the modeling results for the four air toxics are considered together with their cancer risk factors, all the fuels and vehicle technologies show air toxic emission reduction benefits.     

Toxic Emissions from Mobile Sources: A Total Fuel-Cycle Analysis for Conventional and Alternative Fuel Vehicles

ABSTRACT

Mobile sources are among the largest contributors of four hazardous air pollutants—benzene, 1,3-butadiene, acetal-dehyde, and formaldehyde—in urban areas. At the same time, federal and state governments are promoting the use of alternative fuel vehicles as a means to curb local air pollution. As yet, the impact of this movement toward alternative fuels with respect to toxic emissions has not been well studied. The purpose of this paper is to compare toxic emissions from vehicles operating on a variety of fuels, including reformulated gasoline (RFG), natural gas, ethanol, methanol, liquid petroleum gas (LPG), and electricity. This study uses a version of Argonne National Laboratory's Greenhouse Gas, Regulated Emissions, and Energy Use in Transportation (GREET) model, appropriately modified to estimate toxic emissions. The GREET model conducts a total fuel-cycle analysis that calculates emissions from both downstream (e.g., operation of the vehicle) and upstream (e.g., fuel production and distribution) stages of the fuel cycle. We find that almost all of the fuels studied reduce 1,3-buta-diene emissions compared with conventional gasoline (CG). However, the use of ethanol in E85 (fuel made with 85% ethanol) or RFG leads to increased acetaldehyde emissions, and the use of methanol, ethanol, and compressed natural gas (CNG) may result in increased formaldehyde emissions. When the modeling results for the four air toxics are considered together with their cancer risk factors, all the fuels and vehicle technologies show air toxic emission reduction benefits.     

On-road remote sensing of liquefied petroleum gas (LPG) vehicle emissions measurement and emission factors estimation

In the present study, the real-world on-road liquefied petroleum gas (LPG) vehicle/taxi emissions of carbon monoxide (CO), hydrocarbon (HC) and nitric oxide (NO) were investigated. A regression analysis approach based on the measured LPG vehicle emission data was also used to estimate the on-road LPG vehicle emission factors of CO, HC and NO with respect to the effects of instantaneous vehicle speed and acceleration/deceleration profiles for local urban driving patterns. The results show that the LPG vehicle model years and driving patterns have a strong correlation to their emission factors. A unique correlation of LPG vehicle emission factors (i.e., g km⁻¹ and g l⁻¹) on different model years for urban driving patterns has been established. Finally, a comparison was made between the average LPG, and petrol [Chan, T.L., Ning, Z., Leung, C.W., Cheung, C.S., Hung, W.T., Dong, G., 2004. On-road remote sensing of petrol vehicle emissions measurement and emission factors estimation in Hong Kong. Atmospheric Environment 38, 2055–2066 and 3541] and diesel [Chan, T.L., Ning, Z., 2005. On-road remote sensing of diesel vehicle emissions measurement and emission factors estimation in Hong Kong. Atmospheric Environment 39, 6843–6856] vehicle emission factors. It has shown that the introduction of the replacement of diesel taxis to LPG taxis has alleviated effectively the urban street air pollution. However, it has demonstrated that proper maintenance on the aged LPG taxis should also be taken into consideration.     

Seasonal effect on N2O formation in nitrification in constructed wetlands

Constructed wetlands are considered to be important sources of nitrous oxide (N(2)O). In order to investigate the contribution of nitrification in N(2)O formation, some environmental factors, plant species and ammonia-oxidizing bacteria (AOB) in active layers have been compared. Vegetation cells indicated remarkable effect of seasons and different plant species on N(2)O emission and AOB amount. Nitrous oxide data showed large temporal and spatial fluctuations ranging 0-52.8 mg N(2)O m(-2)d(-1). Higher AOB amount and N(2)O flux rate were observed in the Zizania latifolia cell, reflecting high potential of global warming. Roles of plants as ecosystem engineers are summarized with rhizosphere oxygen release and organic matter transportation to affect nitrogen transformation. The Phragmites australis cell contributed to keeping high T-N removal performance and lower N(2)O emission. The distribution of AOB also supported this result. Statistical analysis showed several environmental parameters affecting the strength of observed greenhouse gases emission, such as water temperature, water level, TOC, plant species and plant cover.     

Agricultural opportunities to mitigate greenhouse gas emissions

Agriculture is a source for three primary greenhouse gases (GHGs): CO(2), CH(4), and N(2)O. It can also be a sink for CO(2) through C sequestration into biomass products and soil organic matter. We summarized the literature on GHG emissions and C sequestration, providing a perspective on how agriculture can reduce its GHG burden and how it can help to mitigate GHG emissions through conservation measures. Impacts of agricultural practices and systems on GHG emission are reviewed and potential trade-offs among potential mitigation options are discussed. Conservation practices that help prevent soil erosion, may also sequester soil C and enhance CH(4) consumption. Managing N to match crop needs can reduce N(2)O emission and avoid adverse impacts on water quality. Manipulating animal diet and manure management can reduce CH(4) and N(2)O emission from animal agriculture. All segments of agriculture have management options that can reduce agriculture's environmental footprint.     

Factors controlling natural VOC emissions in a southeastern US pine forest

A one-year field study was conducted to investigate the control factors of the monoterpene emissions from slash and loblolly pine saplings at the Austin Cary Forest site in Florida. The α-pinene, camphene, β-pinene, myrcene, d-limonene, and β-phellandrene were identified in the emission samples collected from native pine trees. The α-pinene was the principal (>60%) monoterpene emitted by both slash and loblolly pine saplings. Terpene emission rates in spring were the highest and most volatile for slash pine trees, possibly due to the influences of bud formation and elongation. Loblolly pine emissions, under a similar environmental temperature range, revealed different seasonal patterns of emissions when compared to those for slash pines. Emission rates of monoterpenes from slash and loblolly pine trees were found to depend on temperature, season's change (e.g., bud emissions), tree age, needle surface wetness, and rough handling. It is suggested that the emission control factors besides the environmental temperature should also be taken into account in assessing regional biogenic emissions for compling a worldwide hydrocarbon emission inventory. It is also found that monoterpene emission rates could easily change over a long period of time (e.g., years), and so it is desirable to analyze the emission data based on the short term (e.g., season, month) for reasonable temperature-emission algorithm.     

Methane and nitrous oxide emissions from an irrigated rice of North India

Upland rice was grown in the kharif season (June-September) under irrigated condition in New Delhi, India (28 degree 40'N and 77 degree 12'E) to monitor CH4 and N2O emission, as influenced by fertilizer urea, ammonium sulphate and potassium nitrate alone (at 120 kg ha-1) and mixed with dicyandiamide (DCD), added at 10% of applied N. The experimental soil was a typic ustochrept (Inceptisol), clay loam, in which rice (Oryza sativa L., var. Pusa-169, duration: 120-125 days) was grown and CH4 and N2O was monitored for 105 days by closed chamber method, starting from the 5 days and 1 day after transplanting, respectively. Methane fluxes had a considerable temporal variation (CV=52-77%) and ranged from 0.05 (ammonium sulphate) to 3.77 mg m-2 h-1 (urea). There was a significant increase in the CH4 emission on the application of fertilizers while addition of DCD with fertilizers reduced emissions. Total CH4 emission (105 days) ranged from 24.5 to 37.2 kg ha-1. Nitrous oxide fluxes were much lower than CH4 fluxes and had ranged from 0.18 to 100.5 g m-2 h-1 with very high temporal variation (CV=69-143%). Total seasonal N2O emission from different treatments ranged from 0.037 to 0.186 kg ha-1 which was a N loss of 0.10-0.12% of applied N. All the fertilizers significantly increased seasonal N2O emission while application of DCD reduced N2O emissions significantly in the range of 10-53%.     

CH4 and N2O emissions from Spartina alterniflora and Phragmites australis in experimental mesocosms

Spartina alterniflora, a perennial grass with C(4)-photosynthesis, shows great invading potential in the coastal ecosystems in the east of China. We compared trace gas emissions from S. alterniflora with those from a native C(3) plant, Phragmites australis, by establishing brackish marsh mesocosms to experimentally assess the effects of plant species (S. alterniflora vs. P. australis), flooding status (submerged vs. non-submerged), and clipping (plants clipped or not) on trace gas emissions. The results show that trace gas emission rates were higher in S. alterniflora than P. australis mesocosms due to the higher biomass and density of the former, which could fix more available substrates to the soil and potentially emit more trace gases. Meanwhile, trace gas emission rates were higher in non-submerged than submerged soils, suggesting that water might act as a diffusion barrier in the brackish marsh mesocosms. Interestingly, methane (CH(4)) emission rates were lower in clipped non-submerged mesocosms than in non-clipped submerged mesocosms, but nitrous oxide (N(2)O) emissions were enhanced. CH(4) emissions were significantly correlated with the plant biomass and stem density (R(2)>0.48, P<0.05) for both species, suggesting that both the two species might play important roles in CH(4) production and transport and also act as suppliers of easily available substrates for the methanogenic bacteria in wetland ecosystems. N(2)O emissions, however, were not significantly correlated with plant biomass and density (P>0.05).     

Mercury volatilisation and phytoextraction from base-metal mine tailings

Experiments were carried out in plant growth chambers and in the field to investigate plant-mercury accumulation and volatilisation in the presence of thiosulphate (S2O3)-containing solutions. Brassica juncea (Indian mustard) plants grown in Hg-contaminated Tui mine tailings (New Zealand) were enclosed in gastight volatilisation chambers to investigate the effect of ammonium thiosulphate ([NH4]2 S2O3) on the plant-Hg volatilisation process. Application of (NH4)2 S2O3 to substrates increased up to 6 times the Hg concentration in shoots and roots of B. juncea relative to controls. Volatilisation rates were significantly higher in plants irrigated only with water (control) when compared to plants treated with (NH4)2 S2O3. Volatilisation from barren pots (without plants) indicated that Hg in tailings is subject to biological and photochemical reactions. Addition of sodium thiosulphate (Na2S2O3) at 5 g/kg of substrate to B. juncea plants grown at the Tui mine site confirmed the plant growth chambers studies showing the effectiveness of thio-solutions at enhancing shoot Hg concentrations. Mercury extraction from the field plots yielded a maximum value of 25 g/ha. Mass balance studies revealed that volatilisation is a dominant pathway for Hg removal from the Tui mine site. A preliminary assessment of the risks of volatilisation indicated that enhanced Hg emissions by plants would not harm the local population and the regional environment.     

The effect of the limited availability of H2O2 in the competitive deposition of sulfur and oxidized nitrogen

To understand the influence of the reduction of SO2 emissions from a single source in the S and N deposition around its local environment, the application of the Sulphur Transport Eulerian Model 2 (STEM-II) was introduced in this paper. Observed local deposition patterns were analysed and explained in terms of the main processes involved in the pollutants deposition. It was necessary to take into account the limited availability of H2O2 because of its influence on both S(IV) and oxidized nitrogen deposition. In order to estimate the quantitative relationship between the SO2 emissions reduction and the observed S and N deposition patterns, these processes were simulated for different meteorological conditions. Simulation results were in agreement with both observed deposition patterns and limited availability of H2O2, specially if significant changes in the S deposition patterns were considered. Both observed and estimated S deposition patterns changed their top value location from the Southwest (1990) to the Northwest (1997) of the domain, because of the reduction of dry deposition. The global reduction of total S depositions, estimated and observed, were in good agreement too. Model simulations could explain the higher S dry deposition reduction, considering the emissions reduction strategy applied.     

Interlaborafory Comparison of Formaldehyde Emissions from Particleboard Underlayment in Small-Scale Environmental Chambers

Formaldehyde (CH₂O) emissions from particleboard underlayment have been measured in 0.17 and 0.2 m³ chambers at separate laboratories to test the comparability of small scale environmental chamber measurements under different ventilation and product loading conditions. Absolute CH₂O calibration was established through intermethod comparison of different monitoring techniques against a CH₂O generation apparatus. Interlaboratory precision was enhanced via co-calibration of each laboratory’s CH₂O colorimetric analyzer against the same blank and bi-level generation source at the beginning and end of the study. The results show excellent intermethod and interlaboratory agreement in both the CH₂O calibration and particleboard emissions testing. The CH₂O emission rates of the test specimens demonstrate a Fick’s Law dependence on CH₂O vapor concentration. Measured CH₂O concentrations are described by a single-compartment, single emitter model, and are inversely proportional to the ratio [N/L (m/h)] of the air exchange rate [N(h^-1)] and product loading [L(m^-1)]. Comparison tests at varying N and L, but uniform N/L were performed; similar CH2O concentrations were measured for N and L levels selected from an indoor compartment model, and for fivefold larger N and L values, which are more convenient for small-scale chamber testing.     

北京市生活垃圾焚烧发电厂温室气体排放及影响因素

以北京高安屯垃圾焚烧发电厂为例,利用《温室气体排放核算指南生活垃圾焚烧企业》（DB 11/T 1416-2017）,核算固定设施排放源的直接排放、间接排放和避免排放,并分析影响排放的主要因素。结果表明,2015年高安屯垃圾焚烧发电厂吨垃圾净CO2排放量为0.165 t,其中生活垃圾中矿物碳焚烧贡献量为0.375 t;燃烧产生的N2O贡献量为0.015 t;化石燃料燃烧贡献量为0.002 t;发电上网减排量为0.227 t。降低塑料类在入炉生活垃圾中的比例是减少垃圾焚烧发电厂温室气体排放的关键途径之一。