Effect of oxygenated liquid additives on the urea based SNCR process

An experimental investigation was performed to study the effect of oxygenated liquid additives, H₂O₂, C₂H₅OH, C₂H₄(OH)₂ and C₃H₅(OH)₃ on NO_x removal from flue gases by the selective non-catalytic reduction (SNCR) process using urea as a reducing agent. Experiments were performed with a 150 kW pilot scale reactor in which a simulated flue gas was generated by the combustion of methane operating with 6% excess oxygen in flue gases. The desired levels of initial NO_x (500 ppm) were achieved by doping the fuel gas with ammonia. Experiments were performed throughout the temperature range of interest, i.e. from 800 to 1200 °C for the investigation of the effects of the process additives on the performance of aqueous urea DeNO_x. With H₂O₂ addition a downward shift of 150 °C in the peak reduction temperature from 1130 to 980 °C was observed during the experimentation, however, the peak reduction efficiency was reduced from 81 to 63% when no additive was used. The gradual addition of C₂H₅OH up to a molar ratio of 2.0 further impairs the peak NO_x reduction efficiency by reducing it to 50% but this is accompanied by a downward shift of 180 °C in the peak reduction temperature. Further exploration using C₂H₄(OH)₂ suggested that a 50% reduction could be attained for all the temperatures higher than 940 °C. The use of C₃H₅(OH)₃ as a secondary additive has a significant effect on the peak reduction efficiency that decreased to 40% the reductions were achievable at a much lower temperature of 800 °C showing a downward shift of 330 °C.     

Size distributions of fine and ultrafine particles in the city of Strasbourg: correlation between number of particles and concentrations of NO(x) and SO(2) gases and some soluble ions concentration determination

An Electrical Low Pressure Impactor (ELPI) was used during spring and autumn 2003 in the centre of Strasbourg for the measurement of atmospheric aerosols size distribution. The concentration of NO(x) and SO(2) in air was simultaneously measured with specific analysers. Samples were collected in the range 0.007-10 microm in equivalent aerodynamic diameter size. Number distributions are representative of a pollution originating from urban traffic with a particle size distribution exhibiting a nucleation mode below 29 nm and an accumulation mode around 80 nm in size. A mean particle density equal to 39000+/-35000 total particles per cm(3) with a size ranging from 7 to 10 microm was obtained after a sampling period of 2 weeks in spring. About 86.9% of the number of particles have an aerodynamic diameter below 0.1 microm and 13.1% between 0.1 and 1 microm. Correlation coefficients between the number of particles impacted on each ELPI plate and gas concentrations (SO(2) and NO(x)) showed that the numbers of particles with diameter between 0.10 and 0.62 microm are highly related to the NO(x) concentration. This result indicates that particles are traffic induced since NO(x) is mainly emitted by cars as shown by measurements on various sites. Particles are less clearly correlated to the SO(2) concentration. Particle analysis on different ELPI plates for a sampling period of 2 weeks in autumn showed high level of soluble NO(3)(-), SO(4)(2-) and NH(4)(+) ions. Indeed, up to 90% b.w. of these three species were found in the particle range 0.1-1 microm. The formation of particulate NH(4)NO(3) is favoured by high NO(x) concentration, which induces the formation of gaseous HNO(3).     

Photo-oxidation of NO using an exterior paint--screening of various commercial titania in powder pressed and paint films

The present work aims to evaluate the photocatalytic activity of photo-TiO(2) from various producers (Evonik, Kemira, Kronos, Millennium, Sachtleben and Tayca), in the form of powder pressed films and upon incorporation in a water-based paint, for outdoor NO abatement. The photocatalytic activity of the different samples was evaluated in terms of NO conversion and selectivity towards nitrite and nitrate ions following approximately the ISO 22197-1:2007(E) standard. The highest yields obtained for powder pressed films were achieved with VLP7000 (0.70), followed by VLP7101 (0.55) and UVLP7500 (0.55), all from Kronos. On the other hand, when incorporated in paint films, the highest yields were obtained with PC500 and PC105 from Millennium and UV100 from Sachtleben (ca. 0.15). The paint matrix plays an important role on the photocatalytic activity. In particular, the time for steady state is one or two orders of magnitude higher when the photocatalysts are incorporated in paint films in relation to the powder pressed films. The paint films were activated following the procedure recommended by the above-mentioned standard. However, the photocatalytic activity of films incorporating P25 (Evonik) was displayed only when higher power radiation and higher humidity conditions were used. This allowed for similar levels of photocatalytic activity as the other paint films.     

氮氧化物控制技术现状与进展

介绍了几种最新的氮氧化物(NOx)控制技术,对主要的两种脱硝技术-选择性非催化还原(SCNR)和选择性催化还原(SCR)技术进行较为详细的讨论,并介绍了低温SCR、双氧水氧化、臭氧氧化脱硝技术的最新研究进展。     

火电厂脱硝的尿素制氨技术概述

选择性催化还原法（简称SCR）脱硝用还原剂氨气的制备原料主要有液氨、氨水及尿素三种。由于液氨工艺系统简单,运输、投资、运行成本较低,在目前的工程中已广泛应用,但存在的缺点是对系统的安全性要求较高。根据《危险化学品重大危险源辨识标准》（GB18218—2009）,液氨储量超过10吨视为重大危险源,因此,某些特殊地区（如北京、广州等地）要求还原剂制备系统采用安全性要求较低的尿素工艺。尿素工艺又分为热解法和水解法制氨,本文分别说明了两种工艺的技术原理、工艺流程。     

Effects of fuel reactivity and injection timing on diesel engine combustion and emissions

Recent strategies for simultaneously reducing NOx and soot emissions have focused on achieving nearly premixed, low-temperature combustion (LTC) in diesel engines. A promising approach in this regard is to vary fuel reactivity in order to control the ignition delay and optimize the level of premixing and reduce emissions. The present study examines such a strategy by performing 3-D simulations in a single-cylinder of a diesel engine. Simulations employ the state-of-the-art two-phase models and a validated semi-detailed reaction mechanism. The fuel reactivity is varied by using a blend of n-heptane and iso-octane, which represent surrogates for gasoline and diesel fuels, respectively. Results indicate that the fuel reactivity strongly influences ignition delay and combustion phasing, whereas the start of injection (SOI) affects combustion phasing. As fuel reactivity is reduced, the ignition delay is increased and the combustion phasing is retarded. The longer ignition delay provides additional time for mixing, and reduces equivalence ratio stratification. Consequently, the premixed combustion is enhanced relative to diffusion combustion, and thus the soot emission is reduced. NO_x emission is also reduced due to reduced diffusion combustion and lower peak temperatures caused by delayed combustion phasing. An operability range is observed in terms of fuel reactivity and SOI, beyond which the mixture may not be sufficiently well mixed, or compression ignited. The study demonstrates the possibility of finding an optimum range of fuel reactivity, SOI, and EGR for significantly reducing engine out emissions for a given load and speed.     

Experimental measurement and modeling of the rate of absorption of carbon dioxide by aqueous ammonia

In this work, the rate of absorption of carbon dioxide by aqueous ammonia solvent has been studied by applying a newly built wetted wall column. The absorption rate in aqueous ammonia was measured at temperatures from 279 to 304 K for 1 to 10 wt% aqueous ammonia with loadings varying from 0 to 0.8 mol CO₂/mol NH₃. The absorption rate in 30 wt% aqueous mono-ethanolamine (MEA) was measured at 294 and 314 K with loadings varying from 0 to 0.4 as comparison.It was found that at 304 K, the rate of absorption of carbon dioxide by 10 wt% NH₃ solvent was comparable to the rates for 30 wt% MEA at 294 and 314 K (a typical absorption temperature for this process). The absorption rate using ammonia was however significantly lower at temperatures of 294 K and lower as applied in the Chilled Ammonia Process. However, at these low temperatures, the rate of absorption in ammonia has only a small temperature dependency.The rate of absorption decreases strongly with decreasing ammonia concentrations and increasing CO₂ loadings.The rate of absorption of carbon dioxide by aqueous ammonia solvent was modeled using the measurements of the unloaded solutions and the zwitter-ion mechanism. The model could successfully predict the experimental measurements of the absorption rate of CO₂ in loaded ammonia solutions.     

Evaluation of the temporal variations of air quality in Taipei City, Taiwan, from 1994 to 2003

Data collected from the five air-quality monitoring stations established by the Taiwan Environmental Protection Administration in Taipei City from 1994 to 2003 are analyzed to assess the temporal variations of air quality. Principal component analysis (PCA) is adopted to convert the original measuring pollutants into fewer independent components through linear combinations while still retaining the majority of the variance of the original data set. Two principal components (PCs) are retained together explaining 82.73% of the total variance. PC1, which represents primary pollutants such as CO, NO(x), and SO(2), shows an obvious decrease over the last 10 years. PC2, which represents secondary pollutants such as ozone, displays a yearly increase over the time period when a reduction of primary pollutants is obvious. In order to track down the control measures put forth by the authorities, 47 days of high PM(10) concentrations caused by transboundary transport have been eliminated in analyzing the long-term trend of PM(10) in Taipei City. The temporal variations over the past 10 years show that the moderate peak in O(3) demonstrates a significant upward trend even when the local primary pollutants have been well under control. Monthly variations of PC scores demonstrate that primary pollution is significant from January to April, while ozone increases from April to August. The results of the yearly variations of PC scores show that PM(10) has gradually shifted from a strong correlation with PC1 during the early years to become more related to PC2 in recent years. This implies that after a reduction of primary pollutants, the proportion of secondary aerosols in PM(10) may increase. Thus, reducing the precursor concentrations of secondary aerosols will be an effective way to lower PM(10) concentrations.     

Anaerobic digestion of dairy manure with enhanced ammonia removal

Poor ammonia-nitrogen removal in methanogenic anaerobic reactors digesting animal manure has been reported as an important disadvantage of anaerobic digestion (AD) in several studies. Development of anaerobic processes that are capable of producing reduced ammonia-nitrogen levels in their effluent is one of the areas where further research must be pursued if AD technology is to be made more effective and economically advantageous. One approach to removing ammonia from anaerobically digested effluents is the forced precipitation of magnesium ammonium phosphate hexahydrate (MgNH4PO4 x 6H2O), commonly called struvite. Struvite is a valuable plant nutrient source for nitrogen and phosphorus since it releases them slowly and has non-burning features because of its low solubility in water. This study investigated coupling AD and controlled struvite precipitation in the same reactor to minimize the nitrogen removal costs and possibly increase the performance of the AD by reducing the ammonia concentration which has an adverse effect on anaerobic bacteria. The results indicated that up to 19% extra COD and almost 11% extra NH3 removals were achieved relative to a control by adding 1750 mg/L of MgCl2 x 6H2O to the anaerobic reactor.     

Estimates of health benefits due to reductions in ambient NO2 levels

A method is presented here by which the actual numbers of individuals in the U.S. population who would be expected to suffer respiratory illness as a result of exposure to ambient nitrogen dioxide (NO₂) concentrations in excess of the Federally-designated ambient air quality standard can be estimated. At the same time we have attempted to quantify how these adverse health effects would be alleviated by various degrees of reductions in current ambient concentrations. In addition, the health benefit expected to be derived by various NO_x emission control strategies will be examined utilizing the health benefit estimation method presented.It is estimated that there were approximately 33.2×10⁶ excess cases of respiratory illnesses in the U.S. in 1973 associated with ambient NO₂ concentrations in excess of the national ambient standard. A reduction of approximately 50 to 60 percent below 1973 NO₂ levels is needed to essentially eliminate excess respiratory illness associated with ambient NO₂ concentration.     

Advanced oxidation treatment of pulp mill effluent for TOC and toxicity removals

Pulp mill effluent was treated by different advanced oxidation processes (AOPs) consisting of UV, UV/H2O2, TiO2-assisted photo-catalysis (UV/TiO2) and UV/H2O2/TiO2 in lab-scale reactors for total organic carbon (TOC) and toxicity removals. Effects of some operating parameters such as the initial pH, oxidant and catalyst concentrations on TOC and toxicity removals were investigated. Almost every method resulted in some degree of TOC and toxicity removal from the pulp mill effluent. However, the TiO2-assisted photo-catalysis (UV/TiO2) resulted in the highest TOC and toxicity removals under alkaline conditions when compared with the other AOPs tested. Approximately, 79.6% TOC and 94% toxicity removals were obtained by the TiO2-assisted photo-catalysis (UV/TiO2) with a titanium dioxide concentration of 0.75gl(-1) at pH 11 within 60min.     

Removal of mercury from aqueous solutions using activated carbon prepared from agricultural by-product/waste

Removal of mercury from aqueous solutions using activated carbon prepared from Ceiba pentandra hulls, Phaseolus aureus hulls and Cicer arietinum waste was investigated. The influence of various parameters such as effect of pH, contact time, initial metal ion concentration and adsorbent dose for the removal of mercury was studied using a batch process. The experiments demonstrated that the adsorption process corresponds to the pseudo-second-order-kinetic models and the equilibrium adsorption data fit the Freundlich isotherm model well. The prepared adsorbents ACCPH, ACPAH and ACCAW had removal capacities of 25.88 mg/g, 23.66 mg/g and 22.88 mg/g, respectively, at an initial Hg(II) concentration of 40 mg/L. The order of Hg(II) removal capacities of these three adsorbents was ACCPH > ACPAH > ACCAW. The adsorption behavior of the activated carbon is explained on the basis of its chemical nature. The feasibility of regeneration of spent activated carbon adsorbents for recovery of Hg(II) and reuse of the adsorbent was determined using HCl solution.     

Analysis of the nitrifying bacterial community in BioCube sponge media using fluorescent in situ hybridization (FISH) and microelectrodes

There is growing interest in the development of more cost-effective and retrofit technologies for the upgrade and expansion of existing wastewater treatment plants with extreme space constraints. A free-floating sponge media (BioCube) process, using a 24L lab scale reactor, was operated to study the nitrification profiles and microbial community. The COD removal efficiencies were maintained, at an average of 95%, with the mixed liquor suspended solids (MLSS) inside the BioCube sponge media maintained at 12,688mg/L. The nitrification removal efficiencies were between 92% and 100%, with an average value of 99%. From the results of microelectrode measurements, the ammonium ion concentration was found to rapidly decrease from the surface of the BioCube sponge media to a depth of 2mm due to chemical reactions carried out by ammonia oxidizing bacteria (AOB) species. Multi-fluorescence in situ hybridization (FISH) has been used to investigate the spatial distributions of various microbial activities within reactors. Microbial communities were targeted using different oligonucleotide probes specific to AOB and nitrite oxidizing bacteria (NOB). There were a large number of AOB populations, but these were not uniformly distributed in the biofilm compared to the NOB populations.     

Usability of food industry waste oils as fuel for diesel engines

Two cogeneration units were each fitted with a prechamber (IDI) diesel engine in order to test the feasibility of using waste oils from the food industry as a fuel source, and additionally to test emissions generated by the combustion of these fuels. Esterified waste oils and animal fats as well as mustard oil were tested and compared to the more or less "common" fuels: diesel, rapeseed oil and rapeseed methyl ester. The results show that, in principle, each of these fuels is suitable for use in a prechamber diesel engine. Engine performance can be maintained at a constant level. Without catalytic conversion, the nitrogen oxides emissions were comparable. A significant reduction in NO(x) was achieved through the injection of urea. Combining a urea injection with the SCR catalytic converter reduced NO(x) emissions between 53% and 67%. The carbon monoxide emissions from waste oils are not significantly different from those of "common" fuels and can be reduced the same way as of hydrocarbon emissions, through utilization of a catalytic converter. The rate of carbon monoxide reduction by catalytic conversion was 84-86%. A lower hydrocarbon concentration was associated with fuels of agricultural origin. With the catalytic converter a reduction of 29-42% achieved. Each prechamber diesel engine exhibited its own characteristic exhaust, which was independent of fuel type. The selective catalytic reduction of the exhaust emissions can be realized without restriction using fuels of agricultural origin.     

Broadcast urea reduces N2O but increases NO emissions compared with conventional and shallow-applied anhydrous ammonia in a coarse-textured soil

Despite the importance of anhydrous ammonia (AA) and urea as nitrogen (N) fertilizer sources in the United States, there have been few direct comparisons of their effects on soil nitrous oxide (NO) and nitric oxide (NO) emissions. We compared N oxide emissions, yields, and N fertilizer recovery efficiency (NFRE) in a corn ( L.) production system that used three different fertilizer practices: urea that was broadcast and incorporated (BU) and AA that was injected at a conventional depth (0.20 m) (AAc) and at a shallower depth (0.10 m) (AAs). Averaged over 2 yr in an irrigated loamy sand in Minnesota, growing season NO emissions increased in the order BU < AAc < AAs. In contrast, NO emissions were greater with BU than with AAc or AAs. Emissions of NO ranged from 0.5 to 1.4 kg N ha (50-140 g N Mg grain), while NO emissions ranged from 0.2 to 0.7 kg N ha (20-70 g N Mg grain). Emissions of total N oxides (NO + NO) increased in the order AAc < BU < AAs. Despite having the greatest emissions of NO and total N oxides, the AAs treatment had greater NFRE compared with the AAc treatment. These results provide additional evidence that AA emits more NO, but less NO, than broadcast urea and show that practices to reduce NO emissions do not always improve N use efficiency.     

我国大气细颗粒物污染防治目标和控制措施研究

我国面临着严重的细颗粒物(PM2.5)污染问题,PM2.5对人体健康、能见度、气候变化、生态系统等均产生了不良影响。本文旨在提出我国PM2.5污染防治目标和控制措施,为从根本上改善空气质量提供科学依据。首先,本文提出了2020年和2030年我国PM2.5污染防治目标。其次,采用能源和污染排放技术模型,分情景预测了我国未来一次大气污染物排放量的变化趋势。基于情景预测结果和此前研究建立的一次污染物排放与PM2.5浓度间的非线性关系,确定了2020年—2030年与PM2.5浓度改善相适应的全国和重点区域大气污染物减排目标。最后,利用能源和污染排放技术模型,提出了实现大气污染物减排的技术措施和对策建议。研究表明,2030年全国二氧化硫、氮氧化物、一次PM2.5和挥发性有机物的排放量应分别比2012年至少削减51%、64%、53%和36%,氨排放量也要略有下降。对于污染严重的重点区域,必须采取更严格的控制力度。要实现上述减排,应加快能源结构调整,推进煤炭清洁高效集中可持续利用,建立"车-油-路"一体的移动源控制体系,并强化多源多污染物的末端控制。     

Removal of faecal bacteria from septage by treating it in a full-scale duckweed-covered pond system

Performance of a full-scale duckweed-covered treatment system in removing faecal bacteria is presented. The system consisted of three ponds in series and received septage from holding tanks. Inflow averaged between 36 m³ d⁻¹ in the cold season and 60 m³ d⁻¹ in the warm season, resulting in a total hydraulic retention time of 88 and 58 days, respectively. Duckweed (Lemna minor) colonized the ponds in the summer and continued to grow in the cold season. Due to the difficult harvesting process of the duckweed biomass, the investigation of the treatment efficiency was carried out without plant harvesting. The system was monitored for temperature, pH, oxygen, chlorophyll-a, Escherichia coli and Enterococci. Duckweed growth resulted in chlorophyll-a concentration reduction from 924 to 13 μg L⁻¹, causing neutral and anoxic conditions in the pond water. A temperature effect was noticed on the E. coli decay coefficient with a decreasing trend along the treatment system. Enterococci always decayed less than E. coli. Differences on decay coefficients and removal efficiencies were not observed between the three ponds for both bacterial types. Effluent quality in terms of E. coli was 489 and 1377 cfu/100 mL, in the warm and the cold seasons, respectively, with average removals of 99.65 ± 1.46% and 99.33 ± 3.03%. Total Enterococci removal was 88.91 ± 23.1% in the warm season and 94.43 ± 24.45% in the cold season, resulting in mean effluent values of 1058 and 1404 cfu/100 mL, respectively. The seasonal differences in total removal efficiencies were insignificant for both bacterial types.     

Oil windfalls in Brazil and their long-run social impacts

In 1997, Brazil changed the regulatory framework of its oil and gas sector. After this change, a restrict subset of localities started to receive large amounts of oil rents. The goal of this paper is to evaluate whether such rents distributed under this law contributed to improving some social indicators relative to the national average in the eligible municipalities. We used a “difference-in-differences” measurement to compare changes in selected social indicators within affected Municipalities in the last two decades, taking the unaffected districts as control group. The Municipal data on social indicators were collected from three National Censuses, conducted in 1991, 2000 and 2010. Results show that royalties had a positive and statistically significant impact on household’s access to electric wiring, piped water and waste collection, as well as in the decrease of illiteracy rate. This means the eligible districts were able to improve some of their social indicators in the long-run.     

One way to reduce the NOX Emission of biodiesels: The increase of cetane number

Compared to conventional diesel fuels, biodiesels normally have lower smoke and particulate matter, while higher nitrogen oxides (NO_X) emissions. In our study, an attempt was made to reduce the NO_X emissions of biodiesels by increasing the cetane numbers (CNs). Three kinds of biodiesels with extremely high CNs (70.1, 76.9, 80.9, respectively) were developed. Their main physical and chemical properties were tested. With a two-cylinder direct injection diesel engine, their emission performances were experimentally investigated. The results indicate that, CN, freezing point, as well as viscosity of biodiesels are linearly increased with the increase of carbon number. The NO_X emission for biodiesels with high CNs is lower than that of conventional diesel fuels. High CN promotes smoke formation as well while lower smoke emissions are still obtained for biodiesels when certain oxygen contents are present. That is, the smoke/NO_X tradeoff is broken. Besides, as fuel CN is elevated, NO_X for biodiesels decreases but smoke and carbon monoxide emissions are increased.     

The influence of the precursor and synthesis method on the CO2 capture capacity of carpet waste-based sorbents

Adsorption is one of the most promising technologies for reducing CO₂ emissions and at present several different types of sorbents are being investigated. The use of sorbents obtained from low-cost and abundant precursors (i.e. solid wastes) appears an attractive strategy to adopt because it will contribute to a reduction not only in operational costs but also in the amount of waste that is dumped and burned in landfills every year. Following on from previous studies by the authors, in this work several carbon-based adsorbents were developed from different carpet wastes (pre-consumer and post-consumer wastes) by chemical activation with KOH at various activation temperatures (600–900 °C) and KOH:char impregnation ratios (0.5:1 to 4:1). The prepared materials were characterised by chemical analysis and gas adsorption (N₂, −196 °C; CO₂, 0 °C), and tested for CO₂ adsorption at temperatures of 25 and 100 °C. It was found that both the type of precursor and the conditions of activation (i.e. impregnation ratios, and activation temperatures), had a huge influence on the microporosity of the resultant samples and their CO₂ capture capacities. The carbon-based adsorbent that presented the maximum CO₂ capture capacities at 25 and 100 °C (13.8 wt.% and 3.1 wt.%, respectively), was prepared from a pre-consumer carpet waste and was activated at 700 °C using a KOH:char impregnation ratio of 1:1. This sample showed the highest narrow microporosity volume (0.47 cm³ g⁻¹), thus confirming that only pores of less than 1 nm are effective for CO₂ adsorption at atmospheric pressure.