Comparison and development of dynamic flux chambers to determine odorous compound emission rates from area sources

Two dynamic flux chambers for direct measurement of odorous compound emissions from quiescent liquid surfaces were investigated under simulated conditions in the laboratory. Initially, a flux chamber built according to the model recommended by French standard NF X 43-104 was studied. This chamber was used in two different ways. The first led to a lack of precision concerning emissions rates from the sampled liquid surface, whereas the second led to an overestimation of the measurements. The second part of the study was devoted to an improved dynamic flux chamber, built according to the feedback from the results obtained using the normalised sampling system. Laboratory tests showed good accuracy and precision. This work underlines the importance of the aerodynamic performances of a dynamic sampling system.     

Abatement of ammonia and hydrogen sulfide emissions from a swine lagoon using a polymer biocover

The purpose of this research was to determine the efficiency of a polymer biocover for the abatement of H2S and NH3 emissions from an east-central Missouri swine lagoon with a total surface area of 7800 m2. The flux rate of NH3, H2S, and CH4 was monitored continuously from two adjacent, circular (d = 66 m) control and treatment plots using a nonintrusive, micrometeorological method during three independent sampling periods that ranged between 52 and 149 hr. Abatement rates were observed to undergo a temporal acclimation event in which NH3 abatement efficiency improved from 17 to 54% (p = < 0.0001 to 0.0005) and H2S abatement efficiency improved from 23 to 58% (p < 0.0001) over a 3-month period. The increase in abatement efficiency for NH3 and H2S over the sampling period was correlated with the development of a stable anaerobic floc layer on the bottom surface of the biocover that reduced mass transfer of NH3 and H2S across the surface. Analysis of methanogenesis activity showed that the biocover enhanced the rate of anaerobic digestion by 25% when compared with the control. The biocover-enhanced anaerobic digestion process was shown to represent an effective mechanism to counteract the accumulation of methanogenic substrates in the biocovered lagoon.     

Comparison of seasonal phenol and p-cresol emissions from ground-level area sources in a dairy operation in central Texas

Although there are more than 200 odor-causing volatile organic compounds (VOCs), phenol and p-cresol are two prominent odor-causing VOCs found downwind from concentrated animal feeding operations (CAFOs). The VOC emissions from cattle and dairy production are difficult to quantify accurately because of their low concentrations, spatial variability, and limitations of available instruments. To quantify VOCs, a protocol following US. Environmental Protection Agency (EPA) Method TO-14A has been established based on the isolation flux chamber method and a portable gas chromatograph (GC) coupled with a purge-and-trap system. The general objective of this research was to quantify phenol and p-cresol emission rates (ERs) from different ground-level area sources (GLASs) in a free-stall dairy during summer and winter seasons using this protocol. Two-week-long sampling campaigns were conducted in a dairy operation in central Texas. Twenty-nine air samples were collected during winter and 37 samples were collected during summer from six specifically delineated GLASs (barn, loafing pen, lagoon, settling basin, silage pile, and walkway) at the free-stall dairy. Thirteen VOCs were identified during the sampling period and the GC was calibrated for phenol and p-cresol, the primary odorous VOCs identified. The overall calculated ERs for phenol and p-cresol were 2656 +/- 728 and 763 +/- 212 mg hd(-1) day(-1), respectively, during winter. Overall phenol and p-cresol ERs were calculated to be 1183 +/- 361 and 551 +/- 214 mg hd(-1) day(-1), respectively, during summer. In general, overall phenol and p-cresol ERs during winter were about 2.3 and 1.4 times, respectively, higher than those during summer.     

Sustainable oil and grease removal from synthetic stormwater runoff using bench-scale bioretention studies.

One of the principal components of the contaminant load in urban stormwater runoff is oil and grease (O&G) pollution, resulting from vehicle emissions. A mulch layer was used as a contaminant trap to remove O&G (dissolved and particulate-associated naphthalene, dissolved toluene, and dissolved motor oil hydrocarbons) from a synthetic runoff during a bench-scale infiltration study. Approximately 80 to 95% removal of all contaminants from synthetic runoff was found via sorption and filtration. Subsequently, approximately 90% of the sorbed naphthalene, toluene, oil, and particulate-associated naphthalene was biodegraded within approximately 3, 4, 8, and 2 days after the event, respectively, based on decreases in contaminant concentrations coupled with increases of microbial populations. These results indicate the effectiveness and sustainability of placing a thin layer of mulch on the surface of a bioretention facility for reducing O&G pollution from urban stormwater runoff.     

酸性洗涤塔-生物滤塔-生物曝气池组合工艺处理恶臭气体NH3和H2S

采用酸性洗涤塔、生物滤塔和生物曝气池的组合工艺处理NH3、H2S恶臭混合气体,研究表明,该组合工艺对NH3和H2S有很好的去除效果,在进气流量为35 L/min,喷淋量45 L/h时,NH3进气浓度50.15~525.4 mg/m3,H2S进气浓度10.23~110.36 mg/m3时,NH3单一进气去除率稳定在99%以上,H2S单一进气去除率90%以上。混合进气后,NH3去除率几乎为100%,H2S的去除率提高至98%以上。在一定的浓度范围内,NH3和H2S之间的相互作用对两者的去除效果没有明显的影响,而且起到了相互促进降解的作用。同时,进气流量和填料层高度都会影响NH3、H2S的去除率。系统对进气容积负荷变化的缓冲能力强,在偶尔超负荷条件下运行并不能使系统崩溃,并且微生物对高负荷逐渐表现出适应性。大部分溶于水的氨由生物曝气池去除,去除率达到96.9%。     

Precipitation of Zn(II), Cu(II) and Pb(II) at bench-scale using biogenic hydrogen sulfide from the utilization of volatile fatty acids

Biological production of hydrogen sulfide (H(2)S) using sulfate-reducing bacteria (SRB) has important potential within environmental biotechnology. The aim of this work was to study the possibility of using SRB for the treatment of an acid mine drainage (AMD) at bench-scale. This process involved three stages: the optimization of H(2)S production through the utilization of total volatile fatty acids (TVFAs) by SRB, the establishment of a biofilm reactor for sulfide production, and the precipitation of metals by using the biologically produced H(2)S. The substrates used for TVFAs production consisted of papaya, apple and banana. The H(2)S produced from the degradation of TVFAs was utilized for the precipitation of a metal-contaminated effluent collected from Bolivar mine (Oruro, Bolivia). The maximum concentration of H(2)S obtained was approximately 16mM. Removal efficiencies of ca. 100% for copper, above 94% for zinc, and above 92% for lead were achieved.     

Biological treatment process of air loaded with an ammonia and hydrogen sulfide mixture

The physico-chemical characteristics of granulated sludge lead us to develop its use as a packing material in air biofiltration. Then, the aim of this study is to investigate the potential of unit systems packed with this support in terms of ammonia and hydrogen sulfide emissions treatment. Two laboratory scale pilot biofilters were used. A volumetric load of 680 g H2S m(-3) empty bed day(-1) and 85 g NH3 m(-3) empty bed day(-1) was applied for eight weeks to a unit called BGSn (column packed with granulated sludge and mainly supplied with hydrogen sulfide); a volumetric load of 170 g H2S m(-3) empty bed day(-1) and 340 g NH3 m(-3) empty bed day(-1) was applied for eight weeks to the other called BGNs (column packed with granulated sludge and mainly supplied with ammonia). Ammonia and hydrogen sulfide elimination occur in the biofilters simultaneously. The hydrogen sulphide and ammonia removal efficiencies reached are very high: 100% and 80% for BGSn; 100% and 80% for BGNs respectively. Hydrogen sulfide is oxidized into sulphate and sulfur. The ammonia oxidation products are nitrite and nitrate. The nitrogen error mass balance is high for BGSn (60%) and BGNs (36%). This result could be explained by the denitrification process which would have occurred in anaerobic zones. High percentages of ammonia or hydrogen sulfide are oxidized on the first half of the column. The oxidation of high amounts of hydrogen sulfide would involve some environmental stress on nitrifying bacterial growth and activity.     

pH对生物滤池处理含H2S和NH3混合恶臭气体的影响

研究了pH对生物滤池处理含H2S和NH3混合恶臭气体的影响,以及不同pH下的物质转化情况和去除机制。结果表明,不同pH下,生物滤池对H2S和NH3的去除率是不同的。在强酸性(pH为2左右)和中性(pH为7左右)条件下,H2S均有较好的去除效果,这分别归于嗜酸性硫细菌和非嗜酸性硫细菌的生物降解作用。低pH下,NH3的去除归于化学中和作用;中性(pH为7左右)条件下,NH3有较高的去除率,主要依靠生物硝化作用。通过考察pH对生物滤池处理效果的影响,确定了生物滤池处理含H2S和NH3混合恶臭气体的pH控制条件和去除机制,为恶臭气体生物处理工艺的选择提供依据。     

复合生物滤池处理H2S和NH3的挂膜与工艺条件

采用复合生物滤池(生物滴滤池 生物过滤池)处理H2S和NH3组成的混合恶臭气体,填料分别为经表面改性的天然斜发沸石和木屑.实验研究了该工艺的驯化挂膜情况和主要工艺条件,结果表明,天然斜发沸石和木屑改性后,驯化挂膜周期为10～14 d,比文献中颗粒活性炭挂膜缩短14～18 d.复合生物滤池的最佳工艺条件为:高度120 cm,循环液流量4.56 L/h.同时,生物滴滤池处理水溶性好的NH3气体效果较生物过滤池好,而生物过滤池处理水溶性差的H2S气体较生物滴滤池好.因此,复合生物滤池可用于处理不同水溶性的混合恶臭气体.     

Crystal seed-enhanced ammonia nitrogen and phosphate recovery from landfill leachate using struvite precipitation technique

Environmental Science and Pollution Research - Nitrogen and phosphorous are limiting and crucial elements for all living organisms. The recovery of nitrogen and phosphorous as struvite gained...     

Emissions of ammonia, hydrogen sulfide, and odor before, during, and after slurry removal from a deep-pit swine finisher

It is a common practice in the midwestern United States to raise swine in buildings with under-floor slurry storage systems designed to store manure for up to one year. These so-called "deep-pit" systems are a concentrated source for the emissions of ammonia (NH3), hydrogen sulfide (H2S), and odors. As part of a larger six-state research effort (U.S. Department of Agriculture-Initiative for Future Agriculture and Food Systems Project, "Aerial Pollutant Emissions from Confined Animal Buildings"), realtime NH3 and H2S with incremental odor emission data were collected for two annual slurry removal events. For this study, two 1000-head deep-pit swine finishing facilities in central Iowa were monitored with one-year storage of slurry maintained in a 2.4 m-deep concrete pit (or holding tank) below the animal-occupied zone. Results show that the H2S emission, measured during four independent slurry removal events over two years, increased by an average of 61.9 times relative to the before-removal H2S emission levels. This increase persisted during the agitation process of the slurry that on average occurred over an 8-hr time period. At the conclusion of slurry agitation, the H2S emission decreased by an average of 10.4 times the before-removal emission level. NH3 emission during agitation increased by an average of 4.6 times the before-removal emission level and increased by an average of 1.5 times the before-removal emission level after slurry removal was completed. Odor emission increased by a factor of 3.4 times the before-removal odor emission level and decreased after the slurry-removal event by a factor of 5.6 times the before-removal emission level. The results indicate that maintaining an adequate barn ventilation rate regardless of animal comfort demand is essential to keeping gas levels inside the barn below hazardous levels.     

Determination of ammonia and hydrogen sulfide emissions from a commercial dairy farm with an exercise yard and the health-related impact for residents

Environmental Science and Pollution Research - Airborne emissions from concentrated animal feeding operations (CAFOs) have the potential to pose a risk to human health and the environment. Here, we...     

高强紫外球形灯光解氧化硫化氢气体

提出了采用可产臭氧的高强球形紫外灯光解氧化硫化氢气体。考察了硫化氢初始浓度、湿度、含氧量、停留时间对硫化氢去除效率的影响。实验结果表明,硫化氢浓度在低浓度范围内,对硫化氢的去除效率可以达到99％以上。反应体系内气体湿度比含氧量对硫化氢的去除效率的影响更明显。气体湿度控制在45％～60％和反应停留时间控制在6～10s范围内为最佳。高强紫外球形灯处理硫化氢过程分别存在直接光解和臭氧氧化作用及两者的协同作用。     

Adaptation of a speciation sampling cartridge for measuring ammonia flux from cattle feedlots using relaxed eddy accumulation

Improved measurements of ammonia losses from cattle feedlots are needed to quantify the national NH₃ emissions inventory and evaluate management techniques for reducing emissions. Speciation cartridges composed of glass honeycomb denuders and filter packs were adapted to measure gaseous NH₃ and aerosol NH₄⁺ fluxes using relaxed eddy accumulation (REA). Laboratory testing showed that a cartridge equipped with four honeycomb denuders had a total capture capacity of 1800 μg of NH₃. In the field, a pair of cartridges was deployed adjacent to a sonic anemometer and an open-path gas analyzer on a mobile tower. High-speed valves were attached to the inlets of the cartridges and controlled by a datalogger so that up- and down-moving eddies were independently sampled based on direction of the vertical wind speed and a user-defined deadband. Air flowed continuously through the cartridges even when not sampling by means of a recirculating air handling system. Eddy covariance measurement of CO₂ and H₂O, as measured by the sonic and open-path gas analyzer, were used to determine the relaxation factor needed to compute REA-based fluxes. The REA system was field tested at the Beef Research Unit at Kansas State University in the summer and fall of 2007. Daytime NH₃ emissions ranged between 68 and 127 μg m^?2 s^?1; fluxes tended to follow a diurnal pattern correlated with latent heat flux. Daily fluxes of NH₃ were between 2.5 and 4.7 g m^?2 d^?1 and on average represented 38% of fed nitrogen. Aerosol NH₄⁺ fluxes were negligible compared with NH₃ emissions. An REA system designed around the high-capacity speciation cartridges can be used to measure NH₃ fluxes from cattle feedlots and other strong sources. The system could be adapted to measure fluxes of other gases and aerosols.     

多级串联腐殖土固定床处理氨气硫化氢恶臭气体的机理

设计了腐殖土固定床串联缺氧SBR多级反应器对填埋场臭气与渗滤液进行协同处理,以气体表面负荷、水力负荷、污染物负荷为影响因素进行正交实验,探究腐殖土固定床对氨气与硫化氢的处理效能与去除机理,并运用物料衡算的方法对腐殖土固定床去除氨气的机理进行分析。结果表明：腐殖土固定床对氨气与硫化氢的平均去除率分别为95%与98%,各因素对氨气去除率的影响大小的依次顺序为气体表面负荷>污染物负荷>水力负荷,各因素对硫化氢去除率的影响大小的依次顺序为污染物负荷>气体表面负荷=水力负荷,最佳实验条件为气体表面负荷为7 m·h⁻¹,水力负荷为0.12 m·d⁻¹,氨气负荷为10 mg·(m³·h)⁻¹,硫化氢负荷为2 mg·(m³·h)⁻¹。机理分析的结果表明多级串联腐殖土固定床对氨气去除主要是靠气相与液相的分压差 (浓度差) ,传质受进口氨气浓度、即氨气气相分压影响,此过程中气膜阻力远大于液膜阻力,近似于气膜控制过程,且各级液相氨氮等效形成的分压差距较小、气相与液相的分压差 (浓度差) 与气液有效传质面积逐级减。本研究结果可为现有的填埋场臭气处理技术上发展腐殖土固定床协同处理臭气渗滤液工艺提供参考。     

Industrial sources influence air concentrations of hydrogen sulfide and sulfur dioxide in rural areas of western Canada

A survey of monthly average concentrations of sulfur dioxide (SO2) and hydrogen sulfide (H2S) at rural locations in western Canada (provinces of Alberta, British Columbia, and Saskatchewan) was conducted in 2001-2002, as part of an epidemiological study of the effects of oil and gas industry emissions on the health of cattle. Repeated measurements were obtained at some months and locations. We aimed to develop statistical models of the effect of oil and gas infrastructure on air concentrations. The regulatory authorities supplied the information on location of the different oil and gas facilities during the study period and, for Alberta, provided data on H2S content of wells and flaring volumes. Linear mixed effects models were used to relate observed concentrations to proximity and type of oil and gas infrastructure. Low concentrations were recorded; the monthly geometric mean was 0.1-0.2 ppb for H2S, and 0.3-1.3 ppb for SO2. Substantial variability between repeated measurements was observed. The precision of the measurement method was 0.005 ppb for both contaminants. There were seasonal trends in the concentrations, but the spatial variability was greater. This was explained, in part, by proximity to oil/gas/bitumen wells and (for SO2) gas plants. Wells within 2 km of monitoring stations had the greatest impact on measured concentrations. For H2S, 8% of between-location variability was explained by proximity to industrial sources of emissions; for SO2 this proportion was 18%. In Alberta, proximity to sour gas wells and flares was associated with elevated H2S concentrations; however, the estimate of the effect of sour gas wells in the immediate vicinity of monitoring stations was unstable. Our study was unable to control for all possible sources of the contaminants. However, the results suggest that oil and gas extraction activities contribute to air pollution in rural areas of western Canada.     

The sorption of hydrogen sulfide from hot syngas by metal oxides over supports

Six 5 wt.% metal sorbents including Mn, Fe, Cu, Co, Ce and Zn supported on gamma-Al2O3, prepared by the incipient wetness impregnation method with calcination at 700 degrees C for 2 h, have been investigated for sorption of hydrogen sulfide in the temperature range of 500-700 degrees C. The sorption experiments were conducted in a fixed-bed reactor in terms of breakthrough curves and characterized by X-ray powder diffraction. The results reveal that the copper and manganese sorbents exhibit the best performance because they provide nearly 100% utilization, but the copper sorbent has a lower sulfur sorption capacity compared with the manganese sorbent. The zinc and cerium sorbents are not good candidates attributed to the vaporization of zinc and unexpected product for cerium. Effects of support materials on 5 wt.% manganese were also investigated by using gamma-Al2O3, SiO2 and TiO2 in this study. Five weight percent Mn/gamma-Al2O3 shows the best performance among support candidates. On the basis of XRPD and BET surface area analysis, TiO2 appears a huge loss in BET surface area associated with a significant formation of rutile form.     

Oxidation of gas mixtures containing dimethyl sulfide, hydrogen sulfide, and methanethiol using a two-stage biotrickling filter

A biofiltration technique was developed for removing a mixture of hydrogen sulfide (H2S), methanethiol (MeSH), and dimethyl sulfide (Me2S) from waste gases. Since H2S, especially at high concentrations, disturbs the removal of Me2S, two biotrickling filters with different microbes and operating pH levels were connected in series to create a two-stage system. Different loads of these gases were studied in order to determine their impact on the removal capacity of the system. The microbial consortia for these filters were enriched from the sludge of a Finnish refinery with bubbling H2S or Me2S. Acclimation for Me2S took 2 weeks, though no acclimation time was needed for the other gases. The first filter, at a pH of 2, removed most of the H2S and some of the MeSH and Me2S. The second filter, at a pH of approximately 6.5, removed the rest of the MeSH and most of the Me2S. The total maximum loads of the whole two-stage biotrickling filter were 1150 g/m3/day for H2S-S (suffix S indicates the results are counted as sulfur amounts), 879 g/m3/day for Me2S-S, and 66 g/m3/day for MeSH-S treated in a gas mixture. The average removal efficiencies for all gases tested were 99% or higher.     

Removal of hydrogen sulfide gas and landfill leachate treatment using coal bottom ash.

Coal bottom ashes produced from three thermal power plants were used in column and batch experiments to investigate the adsorption capacity of the coal ash. Hydrogen sulfide and leachates collected from three sanitary landfill sites were used as adsorbate gas and solutions, respectively. Experimental results showed that coal bottom ash could remove H2S from waste gas or reduce the concentrations of various pollutants in the leachate. Each gram of bottom ash could remove up to 10.5 mg of H2S. In treating the landfill leachate, increasing ash dosage increased the removal efficiency but decreased the adsorption amount per unit mass of ash. For these tested ashes, the removal efficiencies of chemical oxygen demand (COD), NH3-N, total Kjeldhal nitrogen (TKN), P, Fe3+, Mn2+, and Zn2+ were 36.4-50, 24.2-39.4, 27.0-31.1, 82.2-92.9, 93.8-96.5, 93.7-95.4, and 80.5-82.2%, respectively; the highest adsorption capacities for those parameters were 3.5-5.6, 0.22-0.63, 0.36-0.45, 0.027-0.034, 0.050-0.053, 0.029-0.032, and 0.006 mg/g of bottom ash, respectively. The adsorption of pollutants in the leachate conformed to Freundlich's adsorption model.     

Design and performance characterization strategy using modeling for biofiltration control of odorous hydrogen sulfide

Biofilter, dynamic modeling software characterizing contaminant removal via biofiltration, was used in the preliminary design of a biofilter to treat odorous hydrogen sulfide (H2S). Steady-state model simulations were run to generate performance plots for various influent concentrations, loadings, residence times, media sizes, and temperatures. Although elimination capacity and removal efficiency frequently are used to characterize biofilter performance, effluent concentration can be used to characterize performance when treating to a target effluent concentration. Model simulations illustrate that, at a given temperature, a biofilter cannot reduce H2S emissions below a minimum value, no matter how large the biofilter or how long the residence time. However, a higher biofilter temperature results in lower effluent H2S concentrations. Because dynamic model simulations show that shock loading can significantly increase the effluent concentration above values predicted by the steady-state model simulations, it is recommended that, to consistently meet treatment objectives, dynamic feed conditions should be considered. This study illustrates that modeling can serve as a valuable tool in the design and performance optimization of biofilters.