Photochemical production of methane in natural waters: implications for its present and past oceanic source

We conducted irradiation experiments with riverine, estuarine, and marine water samples to investigate the possibility of photochemical methane (CH4) formation. CH4 photoproduction was undetectable under oxic conditions or in the absence of methyl radical precursors indicating that its photochemical formation is negligible in the present ocean. Significant photochemical CH4 production was observed in the presence of a methyl radical precursor such as acetone under strictly anoxic conditions. Our results indicate an indirect formation mechanism with coloured dissolved organic matter acting as photosensitizer. We suggest that photochemical CH4 formation might have occurred in the anoxic ocean surface layer of the Archean prior to the onset of O2 accumulation in the atmosphere at around 2300 million years ago. Oceanic CH4 photoproduction via methyl radical (CH3) precursors and its subsequent release to the atmosphere may have contributed to high CH4 mixing ratios in the Archean atmosphere.     

Simulation modeling for nitrogen removal and experimental estimation of mass fractions of microbial groups in single-sludge system

Nitrification-denitrification in a single-sludge nitrogen removal system (SSNRS; with a sufficient carbon source for denitrification) was performed. With an increase in the mixed liquor recycle ratio (R(m)) from 1 to 2, the total nitrogen (TN) removal efficiency at a lower volumetric loading rate (VLR=0.21 NH(4)(+)-N m(-3) d(-1)) increased, but the TN removal efficiency at a higher VLR (0.35 kg NH(4)(+)-N m(-3) d(-1)) decreased. A kinetic model that accounts for the mass fractions of Nitrosomonas, Nitrobacter, nitrate reducer and nitrite reducer (f(n1), f(n2), f(dn1), and f(dn2)) in the SSNRS and an experimental approach for the estimation of the mass fractions of nitrogen-related microbial groups are also proposed. The estimated f(dn1) plus f(dn2) (0.65-0.83) was significantly larger than the f(n1) plus f(n2) (0.28-0.32); the f(n1) (0.21-0.26) was larger than the f(n2) (0.05-0.07); and the f(dn1) (0.32-0.45) varied slightly with the f(dn2) (0.33-0.38). At the lower VLR, the f(dn1) plus f(dn2) increased with increasing R(m); however at the higher VLR, the f(dn1) plus f(dn2) did not increase with increasing R(m). By using the kinetic model, the calculated residual NH(4)(+)-N and NO(2)(-)-N in the anoxic reactor and NO(2)(-)-N and NO(3)(-)-N in the aerobic reactor were in fairly good agreement with the experimental data; the calculated NO(3)(-)-N in the anoxic reactor was over-estimated and the calculated NH(4)(+)-N in the aerobic reactor was under-estimated.     

Catalytic wet oxidation of ammonia: why is N2 formed preferentially against NO3 -?

The role of catalyst and the reason for the preferential formation of N(2) in the catalytic oxidation reaction of ammonia in water over a Ru (3wt.%)/TiO(2) catalyst were elucidated. It was verified that the catalyst in the reaction had no direct relevance to the selective formation of N(2), but was responsible only for the oxidation of aqueous ammonia, NH(3)(aq), finally giving a molecule of nitrous acid. The preferential production of N(2) was experimentally demonstrated due to the homogeneous aqueous phase reaction of the nitrous acid-dissociated NO(2)(-) with NH(4)(+) ions. Even under the highly oxidizing condition, NO(2)(-) was much more likely to react with NH(4)(+) to form N(2) than being oxidized over the catalyst to NO(3)(-) as long as NH(4)(+) was available in solution.     

A cascade of anoxic and oxic fluidized bed biofilm reactors for treatment of synthetic municipal wastewater

In this study, a cascade of anoxic and oxic fluidized bed biofilm reactors system was carried out to treat synthetic municipal wastewater. The parameters of the influent flow rates and C/N ratios were discussed. System performance was acceptable for chemical oxygen demand (COD), ammonia, and total nitrogen removal. A decrease of ammonia and total nitrogen removal efficiencies, however, was observed when the influent flow rates increased to 5.04 and 6.12 1 h(-1). Total nitrogen removal decreased at the influent C/N ratio of 3:1. The measured ratios of COD reduction in the anoxic column to nitrogen removal through nitrification-denitrification were 3.7, 3.5, 3.3, and 3.1 g COD/g(-1) N on average when the influent C/N ratios changed from 6:1 to 3:1. The observed sludge yield (Yobs) was 0.169 g VSS g COD(-1) because of perfect denitrification in the anoxic column and the relatively long solids retention time.     

低COD/N-NH_4比废水的同时硝化反硝化生物处理策略

从生化反应计量学出发 ,提出了对低 COD/ N- NH4比废水可以通过控制营养配比、调控溶解氧浓度和控制生物硝化及生物反硝化 ,经过 NO- 2 途径进行同时硝化反硝化的生物处理策略。对香港低 COD/ N- NH4比的垃圾渗漏水用同时硝化反硝化处理的成功实例进行了讨论     

Quantifying the contribution of nitrification and denitrification to the nitrous oxide flux using 15N tracers

Microbial transformations of nitrification and denitrification are the main sources of nitrous oxide (N2O) from soils. Relative contributions of both processes to N2O emissions were estimated on an agricultural soil using 15N isotope tracers (15NH4+ or 15NO3-), for a 10-day batch experiment. Under unsaturated and saturated conditions, both processes were significantly involved in N2O production. Under unsaturated conditions, 60% of N-N2O came from nitrification, while denitrification contributed around 85-90% under saturated conditions. Estimated nitrification rates were not significantly different whatever the soil moisture content, whereas the proportion of nitrified N emitted as N2O changed from 0.13 to 2.32%. In coherence with previous studies, we interpreted this high value as resulting from the decrease in O2 availability through the increase in soil moisture content. It thus appears that, under limiting aeration conditions, some values for N2O emissions through nitrification could be underestimated.     

Nitrate-consuming processes in a petroleum-contaminated aquifer quantified using push-pull tests combined with 15N isotope and acetylene-inhibition methods

Nitrate consumption in aquifers may result from several biogenic and abiotic processes such as denitrification, assimilatory NO3- reduction, dissimilatory NO3- reduction to ammonium (DNRA), or abiotic NO3- (or NO2-) reduction. The objectives of this study were to investigate the fate of NO3- in a petroleum-contaminated aquifer, and to assess the feasibility of using single-well push-pull tests (PPTs) in combination with 15N isotope and C2H2 inhibition methods for the quantification of processes contributing to NO3- consumption. Three consecutive PPTs were performed in a monitoring well of a heating oil-contaminated aquifer in Erlen, Switzerland. For each test, we injected 500 l of test solution containing 0.5 mM Br- as conservative tracer and either 0.5 mM unlabeled NO3- or approximately 0.3 mM 15N-labeled NO3- as reactant. Test solutions were sparged during preparation and injection with either N2, Ar or 10% C2H2 in Ar. After an initial incubation period of 1.5-3.2 h, we extracted the test solution/groundwater mixtures from the same location and measured concentrations of relevant species including Br-, NO3-, NO2-, N2O, N2, and NH4+. In addition, we determined the 15N contents of N2, N2O, NH4+, and suspended biomass from 15N/14N isotope-ratio measurements. Average total test duration was 50.5 h. First-order rate coefficients (k) were computed from measured NO3- consumption, N2-15N production and N2O-15N production. From measured NO3- consumption we obtained nearly identical estimates of k for all PPTs with small 95% confidence intervals, indicating good reproducibility and accuracy for the tests. Estimates of k from N2-15N production and N2O-15N production indicated that denitrification accounted for only 46-49% of observed NO3- consumption. Production of N2-15N in the presence of C2H2 was observed during one of the tests, which may be an indicator for abiotic NO3- reduction. Moreover, 15N isotope analyses confirmed occurrence of assimilatory NO3- reduction (0.58 at.% 15N in suspended biomass) and to a smaller extent DNRA (up to 4 at.% 15N in NH4+). Our results indicated that the combination of PPTs, 15N-isotope and C2H2 inhibition methods provided improved information on denitrification as well as alternative fates of NO3- in this aquifer.     

Trends in atmospheric ammonium concentrations in relation to atmospheric sulfate and local agriculture

Ammonium (NH(4)(+)) concentrations in air and precipitation at the Institute of Ecosystem Studies (IES) in southeastern New York, USA declined over an 11-year period from 1988 to 1999, but increased from 1999 to 2001. These trends in particulate NH(4)(+) correlated well with trends in particulate SO(4)(2-) over the 1988-2001 period. The NH(4)(+) trends were not as well correlated with local cattle and milk production, which declined continuously throughout the period. This suggests that regional transport of SO(4)(2-) may have a greater impact on concentrations of NH(4)(+) and subsequent deposition than local agricultural emissions of NH(3). Ammonium concentrations in precipitation correlated significantly with precipitation SO(4)(2-) concentrations for the 1984-2001 period although NH(4)(+) in precipitation increased after 1999 and SO(4)(2-) in precipitation continued to decline after 1999. The correlation between NH(4)(+) and SO(4)(2-) was stronger for particulates than for precipitation. Particulate NH(4)(+) concentrations were also correlated with particulate SO(4)(2-) concentrations at 31 of 35 eastern U.S. CASTNet sites that had at least 10 years of data. Air concentrations of NH(4)(+) and SO(4)(2-) were more strongly correlated at the sites that were located within an agricultural landscape than in forested sites. At most of the sites there was either no trend or a decrease in NH(4)(+) dry deposition during the 1988-2001 period. The sites that showed an increasing trend in NH(4)(+) dry deposition were generally located in the southeastern U.S. The results of this study suggest that, in the northeastern U.S., air concentrations of NH(4)(+) and subsequent deposition may be more closely linked to SO(4)(2-) and thus SO(2) emissions than with NH(3) emissions. These results also suggest that reductions in S emissions have reduced NH(4)(+) transport to and NH(4)(+)-N deposition in the Northeast.     

Pilot study on the treatment of low carbon and nitrogen ratio municipal sewage by A1/O2/A3/A4/O5 sludge-membrane coupling process with multi-point inflow

Environmental Science and Pollution Research - A new multi-point inflow pre-anoxic/oxic/anaerobic/anoxic/oxic (A1/O2/A3/A4/O5) sludge-membrane coupling process and pilot plant were developed and...     

Fluxes of N2O, CH4 and CO2 in a meadow ecosystem exposed to elevated ozone and carbon dioxide for three years

Open-top chambers (OTCs) were used to evaluate the effects of moderately elevated O3 (40-50 ppb) and CO2 (+100 ppm) and their combination on N2O, CH4 and CO2 fluxes from ground-planted meadow mesocosms. Bimonthly measurements in 2002-2004 showed that the daily fluxes of N2O, CH4 and CO2 reacted mainly to elevated O3, while the fluxes of CO2 also responded to elevated CO2. However, the fluxes did not show any marked response when elevated O3 and CO2 were combined. N2O and CO2 emissions were best explained by soil water content and air and soil temperatures, and they were not clearly associated with potential nitrification and denitrification. Our results suggest that the increasing O3 and/or CO2 concentrations may affect the N2O, CH4 and CO2 fluxes from the soil, but longer study periods are needed to verify the actual consequences of climate change for greenhouse gas emissions.     

水解酸化-A2O污泥减量工艺的运行性能研究

生物处理单元采用水解酸化、多级串联接触曝气、连续流的除磷脱氮A2／O工艺，并辅以外排厌氧富磷污水侧流除磷，开发了一个新型的具有强化除磷脱氮功能的污泥减量HA—A／A—MCO工艺。用该工艺处理校园生活污水发现，在SRT60d、进水COD316～407mg／L、NH4＋-N30～40mg／L、TN35～53mg／L、TP8—12mg／L的条件下，出水COD≤18mg／L、NH4＋-N≤2．1mg／L、TN≤10．3mg／L、TP≤0．44mg／L。研究还发现，水解酸化池处理产生的VFA能有效促进生物除磷脱氮，导致厌氧释磷量达57mg／L，进入化学除磷池的侧流液量仅相当于进水量的13％；系统最主要的脱氮形式是SND和缺氧反硝化，SND脱氮占脱氮总量的50％，缺氧反硝化占26％；HA-A／A—MCO系统有效实现了生物相分离，并利用生物捕食作用获得较低的污泥产率，0．1gMLSS／gCOD。     

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.     

分段进水SBR短程生物脱氮过程中N_2O产生及控制

利用SBR,控制曝气量为60 L/h,利用在线pH曲线控制曝气时间,成功实现了短程生物脱氮过程,并考察了不同进水方式下SBR运行性能及N2O产量。结果表明,分段进水能够有效降低短程生物脱氮过程中外加碳源投加量。在原水进水碳氮比较低时,采用递增进水量的进水方式,能够有效降低生物脱氮过程中NO-2积累量,从而降低系统N2O产量。1次进水、2次等量进水和2次递增进水方式下,生物脱氮过程中N2O产量分别为11.1、8.86和5.04 mg/L。硝化过程中NO-2-N的积累是导致系统N2O产生的主要原因。部分氨氧化菌（AOB）在限氧条件下以NH＋4-N作为电子供体,NO-2-N作为电子受体进行反硝化,最终产物是N2O。     

A/O膜生物反应器处理高浓度氨氮废水试验研究

对A/O膜生物反应器处理高浓度氨氮废水进行了研究,着重考察硝化液回流比和C/N对系统脱氮效能的影响.研究表明,当硝化液回流比为2、C/N为6时.系统对COD、氨氮、TN的平均去除率分别达96.17%、97.76%、76.29%;A/O膜生物反应器稳定运行期间,氨氮容积负荷去除量与进水氨氮容积负荷呈现良好的线性关系;当A/O膜生物反应器内MLSS稳定在9～13 g/L时,上清液COD较低,膜压差增长缓慢.     

Microbial kinetic analysis of three different types of EBNR process

The disadvantages of developed biological nutrient removal (BNR) processes (additional energy for liquid circulation and addition of external carbon substrate for denitrification in anoxic zones) were improved by reconfiguring the process into (1) an anaerobic zone followed by multiple stages of aerobic-anoxic zones (TNCU3 process) or (2) anaerobic, oxic, anoxic, oxic zones in sequence (TNCU2 process). These two pilot plants were operated at a recycling sludge ratio of 0.5 without internal recycle of nitrified supernatant. The sludge retention time was maintained at 10 d. The main objective of this study is to analyze the kinetics of different microorganisms in these two processes and A2O process by using the Activated Sludge Model No. 2d. The effective removal efficiency of carbon, total phosphorus and total nitrogen at 87-98%, 92-100% and 63-80%, respectively, were achieved in the testing runs. According to model simulations, the microbial kinetics in the TNCU3 and TNCU2 processes would be affected by different operations. When the step feeding strategy was adopted, the HRT was longer due to the less influent flowrate in the front stages and the microbes would grow in quantities by about 6% in the aerobic reactors. In the followed anoxic reactors, the microbes would decrease in quantities by about 12% due to the dilution effect. The dilution effects in TNCU3 and TNCU2 processes did not take place in A2O process because the recycling mixed liquid from the aerobic reactor to the anoxic reactor still contained particulate components. The XH, XPAO, and XAUT concentrations in the effluent of the last tank were lower when the step-feeding mode was adopted. The TNCU3 and TNCU2 processes could be operated efficiently without nitrified liquid circulation and addition of external carbon substrate for denitrification.     

Dry deposition of nitrogen and sulfur to Ponderosa and Jeffrey pine in the San Bernardino national forest in Southern California

Little is known about the concentrations, deposition rates, and effects of nitrogenous and sulfurous compounds in photochemical smog in the San Bernardino National Forest (SBNF) in southern California. Dry deposition of NO(3)(-) and NH(4)(+) to foliage of ponderosa pine (Pinus ponderosa Laws.) and Jeffrey pine (Pinus jeffreyi Grev. & Balf.) was correlated (R = 0.83-0.88) with historical average hourly O(3) concentations at 10 sites across an O(3) gradient in the SBNF. Mean deposition fluxes of NO(3)(-) to ponderosa and Jeffrey pine branches were 0.82 nmol M(-2)s(-1) at Camp Paivika (CP), a high-pollution site, and 0.19 nmol m(-2) s(-1) at Camp Osceola (CAO), a low-pollution site. Deposition fluxes of NH(4)(+) were 0.32 nmol m(-2) s(-1) at CP and 0.17 nmol m(-2) s(-1) at CAO, while mean values for SO(4)(2-) were 0.03 at CP and 0.02 nmol m(-2) s(-1) at CAO. Deposition fluxes to paper and nylon filters were higher in most cases than fluxes to pine branches at the same site. The results of this study suggest that an atmospheric concentration and deposition gradient of N and S compounds occurs along with the west-east O(3) gradient in the SBNF. Annual stand-level dry deposition rates for S and N at CP and CAO were estimated. Further studies are needed to determine if high N deposition loads in the SBNF significantly affect plant/soil nutrient relations, tree health, and the response of ponderosa pine to ozone.     

Dynamics of nitrogen in a PAHs contaminated soil amended with biosolid or vermicompost in the presence of earthworms

Nitrogen mineralization in PAHs contaminated soil in presence of Eisenia fetida amended with biosolid or vermicompost was investigated. Sterilized and unsterilized soil was contaminated with PAHs, added with E. fetida and biosolid or vermicompost and incubated aerobically for 70 days, while dynamics of inorganic N were monitored. Addition of E. fetida to sterilized soil increased concentration of NH(4)(+) 100> mg N kg(-1), while concentrations in unsterilized remained <60 mg N kg(-1) except for soil amended with biosolid plus PAHs where it increased to >80 mg kg(-1). Addition of PAHs had no significant effect on concentration of NH(4)(+) compared to the unamended soil, except in the soil added with biosolid. Addition of E. fetida to sterilized soil increased concentration of NO(2)(-) 15> mg N kg(-1) while concentrations in unsterilized soil remained <7.5 mg N kg(-1) except for soil amended with biosolid where it increased to >20 mg kg(-1). Addition of PAHs had no significant effect on concentration of NO(2)(-) compared to the unamended soil. Addition of biosolid and vermicompost increased concentration of NO(3)(-), while addition of E. fetida decreased concentration of NO(3)(-) in biosolid amended soil. It was found that NH(4)(+) and NO(2)(-) oxidizers were present in the gut of E. fetida, but their activity was not sufficient enough to inhibit a temporarily increase in concentrations of NH(4)(+) and NO(2)(-). Contamination with PAHs induced immobilization of N in biosolid or vermicompost amended soil, as did feeding of E. fetida on biosolid or vermicompost.     

A modified UCT method for biological nutrient removal: configuration and performance

A pilot-scale prototype activated sludge system is presented, which combines both, the idea of University of Cape Town (UCT) concept and the step denitrification cascade for removal of carbon, nitrogen and phosphorus. The experimental set-up consists of an anaerobic selector and stepwise feeding in subsequent three identical pairs of anoxic and oxic tanks. Raw wastewater with influent flow rates ranging between 48 and 168 l d(-1) was fed to the unit at hydraulic residence times (HRTs) of 5-18 h and was distributed at percentages of 60/25/15%, 40/30/30% and 25/40/35% to the anaerobic selector, 2nd and 3rd anoxic tanks, respectively (influent flow distribution before the anaerobic selector). The results for the entire experimental period showed high removal efficiencies of organic matter of 89% as total chemical oxygen demand removal and 95% removal for biochemical oxygen demand, 90% removal of total Kjeldahl nitrogen and total nitrogen removal through denitrification of 73%, mean phosphorus removal of 67%, as well as excellent settleability. The highest removal efficiency and the optimum performance were recorded at an HRT of about 9h and influent flow rate of 96 l d(-1), in which 60% is distributed to the anaerobic selector, 25% to the second anoxic tank and 15% to the last anoxic tank. Consequently, the plant configuration enhanced removal efficiency, optimized performance, saved energy, formed good settling sludge and provided operational assurance.     

Full-scale biofilter reduction efficiencies assessed using portable 24-hour sampling units

Portable 24-hr sampling units were used to collect air samples from eight biofilters on four animal feeding operations. The biofilters were located on a dairy, a swine nursery, and two swine finishing farms. Biofilter media characteristics (age, porosity, density, particle size, water absorption capacity, pressure drop) and ammonia (NH3), hydrogen sulfide (H2S), sulfur dioxide (SO2), methane (CH4), and nitrous oxide (N2O) reduction efficiencies of the biofilters were assessed. The deep bed biofilters at the dairy farm, which were in use for a few months, had the most porous media and lowest unit pressure drops. The average media porosity and density were 75% and 180 kg/m3, respectively. Reduction efficiencies of H2S and NH3 (biofilter 1: 64% NH3, 76% H2S; biofilter 2: 53% NH3, 85% H2S) were close to those reported for pilot-scale biofilters. No N2O production was measured at the dairy farm. The highest H2S, SO2, NH3, and CH4 reduction efficiencies were measured from a flat-bed biofilter at the swine nursery farm. However, the highest N2O generation (29.2%) was also measured from this biofilter. This flat-bed biofilter media was dense and had the lowest porosity. A garden sprinkler was used to add water to this biofilter, which may have filled media pores and caused N2O production under anaerobic conditions. Concentrations of H2S and NH3 were determined using the portable 24-hr sampling units and compared to ones measured with a semicontinuous gas sampling system at one farm. Flat-bed biofilters at the swine finishing farms also produced low amounts of N2O. The N2O production rate of the newer media (2 years old) with higher porosity was lower than that of older media (3 years old) (P = 0.042).     

Do tubificid worms influence the fate of organic matter and pollutants in stormwater sediments?

In urban area, management of stormwater leads to the accumulation of polluted sediments at the water-sediment interface of various aquatic ecosystems. In many cases, these sediments are colonised by dense populations of tubificid worms. However, the influence of tubificid worms on the fate of stormwater sediments has never been tackled. The aim of this study was to measure in sediment columns the influence of tubificid worms on sediment reworking, organic matter processing (O(2) uptake and release of NH(4)(+), NO(3)(-), PO(4)(3-), and dissolved organic carbon), release of hydrocarbons and heavy metals, and microbial characteristics. Results showed that tubificid worms increased the release of NH(4)(+), PO(4)(3-), and dissolved organic carbon by 2-, 4-, and 3-fold, respectively. O(2) uptake also increased by more than 35% due to tubificid activity. The increase in the percentages of active bacteria and hydrolytic activity in the presence of worms indicated that the higher sediment respiration was caused by the stimulation of microbial communities. A reduction of the number of sulphate-reducing bacteria in the uppermost layers of the sediment was attributed to the penetration of O(2) due to worm activity. These significant effects of tubificid worms were probably linked to the dense network of burrows, which enhanced the exchange surface between the water column and the sediment. No release of heavy metals and hydrocarbons to the water phase was detected in the sediment columns. Understanding the fate and effect of organic stormwater sediments in the natural environment requires the integration of the role of bioturbation in urban pollution studies.