Nitrous oxide generation in full-scale biological nutrient removal wastewater treatment plants

International guidance for estimating emissions of the greenhouse gas, nitrous oxide (N₂O), from biological nutrient removal (BNR) wastewater systems is presently inadequate. This study has adopted a rigorous mass balance approach to provide comprehensive N₂O emission and formation results from seven full-scale BNR wastewater treatment plants (WWTP). N₂O formation was shown to be always positive, yet highly variable across the seven plants. The calculated range of N₂O generation was 0.006-0.253 kgN₂O-N per kgN denitrified (average: 0.035 ± 0.027). This paper investigated the possible mechanisms of N₂O formation, rather than the locality of emissions. Higher N₂O generation was shown to generally correspond with higher nitrite concentrations, but with many competing and parallel nitrogen transformation reactions occurring, it was very difficult to clearly identify the predominant mechanism of N₂O production. The WWTPs designed and operated for low effluent TN (i.e. <10 mgN L⁻¹) had lower and less variable N₂O generation factors than plants that only achieved partial denitrification.     

Summer fluxes of atmospheric greenhouse gases N2O, CH4 and CO2 from mangrove soil in South China

The atmospheric fluxes of N₂O, CH₄ and CO₂ from the soil in four mangrove swamps in Shenzhen and Hong Kong, South China were investigated in the summer of 2008. The fluxes ranged from 0.14 to 23.83 μmol m⁻² h⁻¹, 11.9 to 5168.6 μmol m⁻² h⁻¹ and 0.69 to 20.56 mmol m⁻² h⁻¹ for N₂O, CH₄ and CO₂, respectively. Futian mangrove swamp in Shenzhen had the highest greenhouse gas fluxes, followed by Mai Po mangrove in Hong Kong. Sha Kong Tsuen and Yung Shue O mangroves in Hong Kong had similar, low fluxes. The differences in both N₂O and CH₄ fluxes among different tidal positions, the landward, seaward and bare mudflat, in each swamp were insignificant. The N₂O and CO₂ fluxes were positively correlated with the soil organic carbon, total nitrogen, total phosphate, total iron and NH₄⁺-N contents, as well as the soil porosity. However, only soil NH₄⁺-N concentration had significant effects on CH₄ fluxes.     

The effect of pH on N2O production under aerobic conditions in a partial nitritation system

Ammonia-oxidising bacteria (AOB) are a major contributor to nitrous oxide (N₂O) emissions during nitrogen transformation. N₂O production was observed under both anoxic and aerobic conditions in a lab-scale partial nitritation system operated as a sequencing batch reactor (SBR). The system achieved 55 ± 5% conversion of the 1 g NH₄⁺-N/L contained in a synthetic anaerobic digester liquor to nitrite. The N₂O emission factor was 1.0 ± 0.1% of the ammonium converted. pH was shown to have a major impact on the N₂O production rate of the AOB enriched culture. In the investigated pH range of 6.0-8.5, the specific N₂O production was the lowest between pH 6.0 and 7.0 at a rate of 0.15 ± 0.01 mg N₂O-N/h/g VSS, but increased with pH to a maximum of 0.53 ± 0.04 mg N₂O-N/h/g VSS at pH 8.0. The same trend was also observed for the specific ammonium oxidation rate (AOR) with the maximum AOR reached at pH 8.0. A linear relationship between the N₂O production rate and AOR was observed suggesting that increased ammonium oxidation activity may have promoted N₂O production. The N₂O production rate was constant across free ammonia (FA) and free nitrous acid (FNA) concentrations of 5-78 mg NH₃-N/L and 0.15-4.6 mg HNO₂-N/L, respectively, indicating that the observed pH effect was not due to changes in FA or FNA concentrations.     

Nitrous oxide emissions for early warning of biological nitrification failure in activated sludge

Experiments were carried out to establish whether nitrous oxide (N₂O) could be used as a non-invasive early warning indicator for nitrification failure. Eight experiments were undertaken; duplicate shocks DO depletion, influent ammonia increases, allylthiourea (ATU) shocks and sodium azide (NaN₃) shocks were conducted on a pilot-scale activated sludge plant which consisted of a 315 L completely mixed aeration tank and 100 L clarifier. The process performed well during pre-shock stable operation; ammonia removals were up to 97.8% and N₂O emissions were of low variability (<0.5 ppm). However, toxic shock loads produced an N₂O response of a rise in off-gas concentrations ranging from 16.5 to 186.3 ppm, followed by a lag-time ranging from 3 to 5 h ((0.43-0.71) × HRT) of increased NH₃-N and/or NO₂⁻ in the effluent ranging from 3.4 to 41.2 mg L⁻¹. It is this lag-time that provides the early warning for process failure, thus mitigating action can be taken to avoid nitrogen contamination of receiving waters.     

Quantification of greenhouse gas emissions from sludge treatment wetlands

Constructed wetlands are nowadays successfully employed as an alternative technology for wastewater and sewage sludge treatment. In these systems organic matter and nutrients are transformed and removed by a variety of microbial reaction and gaseous compounds such as methane (CH₄) and nitrous oxide (N₂O) may be released to the atmosphere. The aim of this work is to introduce a method to determine greenhouse gas emissions from sludge treatment wetlands (STW) and use the method in a full-scale system. Sampling and analysing techniques used to determine greenhouse gas emissions from croplands and natural wetlands were successfully adapted to the quantification of CH₄ and N₂O emissions from an STW. Gas emissions were measured using the static chamber technique in 9 points of the STW during 13 days. The spatial variation in the emission along the wetland did not follow some specific pattern found for the temporal variation in the fluxes. Emissions ranged from 10 to 5400 mgCH₄/m² d and from 20 to 950 mgN₂O/m² d, depending on the feeding events. The comparison between the CH₄ and N₂O emissions of different sludge management options shows that STW have the lowest atmospheric impact in terms of CO₂ equivalent emissions (Global warming potential with time horizon of 100 years): 17 kgCO₂eq/PE y for STW, 36 kgCO₂eq/PE y for centrifuge and 162 kgCO₂eq/PE y for untreated sludge transport, PE means Population Equivalent.     

Interaction between temperature and ammonia in mesophilic digesters for animal waste treatment

Four anaerobic sequencing batch reactors (ASBRs) were operated during a period of 988 days to evaluate the effect of temperature, ammonia, and their interconnectivity on the methane yield of anaerobic processes for animal waste treatment. During period 1 (day 0-378), the methane yield was 0.31 L CH₄/g volatile solids (VS) for all digesters (with no statistical differences among them) at a temperature and total ammonium-N levels of 25 °C and ∼1200 mg NH₄⁺-N/L, respectively. During period 2 (day 379-745), the methane yield at 25 °C decreased by 45% when total ammonium-N and ammonia-N were increased in two of the four ASBRs to levels >4000 mg NH₄⁺-N/L and >80 mg NH₃-N/L, respectively. During period 3 (day 746-988), this relative inhibition was reduced from 45% to 13% compared to the low-ammonia control reactors when the operating temperature was increased from 25 °C to 35 °C (while the free ammonia levels increased from ∼100 to ∼250 mg NH₃-N/L). The 10 °C increase in temperature doubled the rate constant for methanogenesis, which overwhelmed the elevated toxicity effects caused by the increasing concentration of free ammonia. Thus, the farmer/operator may alleviate ammonia toxicity by increasing the operating temperature within the mesophilic range. We extrapolated our data to correlate temperature, ammonia, and methane yield and to hypothesize that the difference between high- and low-ammonia reactors is negligible at the optimum mesophilic temperature of 38 °C.     

Nitrogen transformations and greenhouse gas emissions from a riparian wetland soil: an undisturbed soil column study

Riparian wetlands bordering intensively managed agricultural fields can act as biological filters that retain and transform agrochemicals such as nitrate and pesticides. Nitrate removal in wetlands has usually been attributed to denitrification processes which in turn imply the production of greenhouse gases (CO₂ and N₂O). Denitrification processes were studied in the Salburua wetland (northern Spain) by using undisturbed soil columns which were subsequently divided into three sections corresponding to A-, Bg- and B2g-soil horizons. Soil horizons were subjected to leaching with a 200 mg NO₃⁻ L^− 1 solution (rate: 90 mL day^− 1) for 125 days at two different temperatures (10 and 20 °C), using a new experimental design for leaching assays which enabled not only to evaluate leachate composition but also to measure gas emissions during the leaching process. Column leachate samples were analyzed for NO₃⁻ concentration, NH₄⁺ concentration, and dissolved organic carbon. Emissions of greenhouse gases (CO₂ and N₂O) were determined in the undisturbed soil columns. The A horizon at 20 °C showed the highest rates of NO₃⁻ removal (1.56 mg N-NO₃⁻ kg⁻¹ DW soil day^− 1) and CO₂ and N₂O production (5.89 mg CO₂ kg⁻¹ DW soil day^− 1 and 55.71 μg N-N₂O kg⁻¹ DW soil day^− 1). For the Salburua wetland riparian soil, we estimated a potential nitrate removal capacity of 1012 kg N-NO₃⁻ ha^− 1 year^− 1, and potential greenhouse gas emissions of 5620 kg CO₂ ha^− 1 year^− 1 and 240 kg N-N₂O ha^− 1 year^− 1.     

Effects of wood ash fertilization on forest floor greenhouse gas emissions and tree growth in nutrient poor drained peatland forests

Wood ash (3.1, 3.3 or 6.6 tonnes dry weight ha^− 1) was used to fertilize two drained and forested peatland sites in southern Sweden. The sites were chosen to represent the Swedish peatlands that are most suitable for ash fertilization, with respect to stand growth response. The fluxes of carbon dioxide (CO₂), methane (CH₄) and nitrous oxide (N₂O) from the forest floor, measured using opaque static chambers, were monitored at both sites during 2004 and 2005 and at one of the sites during the period 1 October 2007-1 October 2008. No significant (p > 0.05) changes in forest floor greenhouse gas exchange were detected. The annual emissions of CO₂ from the sites varied between 6.4 and 15.4 tonnes ha^− 1, while the CH₄ fluxes varied between 1.9 and 12.5 kg ha^− 1. The emissions of N₂O were negligible. Ash fertilization increased soil pH at a depth of 0-0.05 m by up to 0.9 units (p < 0.01) at one site, 5 years after application, and by 0.4 units (p < 0.05) at the other site, 4 years after application. Over the first 5 years after fertilization, the mean annual tree stand basal area increment was significantly larger (p < 0.05) at the highest ash dose plots compared with control plots (0.64 m² ha^− 1 year^− 1 and 0.52 m² ha^− 1 year^− 1, respectively). The stand biomass, which was calculated using tree biomass functions, was not significantly affected by the ash treatment. The groundwater levels during the 2008 growing season were lower in the high ash dose plots than in the corresponding control plots (p < 0.05), indicating increased evapotranspiration as a result of increased tree growth. The larger basal area increment and the lowered groundwater levels in the high ash dose plots suggest that fertilization promoted tree growth, while not affecting greenhouse gas emissions.     

Long-term ammonia removal in a coconut fiber-packed biofilter: Analysis of N fractionation and reactor performance under steady-state and transient conditions

A comprehensive study of long-term ammonia removal in a biofilter packed with coconut fiber is presented under both steady-state and transient conditions. Low and high ammonia loads were applied to the reactor by varying the inlet ammonia concentration from 90 to 260 ppm_v and gas contact times ranging from 20 to 36 s. Gas samples and leachate measurements were periodically analyzed and used for characterizing biofilter performance in terms of removal efficiency (RE) and elimination capacity (EC). Also, N fractions in the leachate were quantified to both identify the experimental rates of nitritation and nitratation and to determine the N leachate distribution. Results showed stratification in the biofilter activity and, thus, most of the NH₃ removal was performed in the lower part of the reactor. An average EC of 0.5 kg N-NH₃ m⁻³ d⁻¹ was obtained for the whole reactor with a maximum local average EC of 1.7 kg N-NH₃ m⁻³ d⁻¹. Leachate analyses showed that a ratio of 1:1 of ammonium and nitrate ions in the leachate was obtained throughout steady-state operation at low ammonia loads with similar values for nitritation and nitratation rates. Low nitratation rates during high ammonia load periods occurred because large amounts of ammonium and nitrite accumulated in the packed bed, thus causing inhibition episodes on nitrite-oxidizing bacteria due to free ammonia accumulation. Mass balances showed that 50% of the ammonia fed to the reactor was oxidized to either nitrite or nitrate and the rest was recovered as ammonium indicating that sorption processes play a fundamental role in the treatment of ammonia by biofiltration.     

Investigating the potential role of ammonia in ion chemistry of fine particulate matter formation for an urban environment

To investigate the potential role of ammonia in ion chemistry of PM_2.5 aerosol, measurements of PM_2.5 (particulate matter having aerodynamic diameter < 2.5 µm) along with its ionic speciation and gaseous pollutants (sulfur dioxide (SO₂), nitrogen oxides (NO_x), ammonia (NH₃) and nitric acid (HNO₃)) were undertaken in two seasons (summer and winter) of 2007-2008 at four sampling sites in Kanpur, an urban-industrial city in the Ganga basin, India. Mean concentrations of water-soluble ions were observed in the following order (i) summer: SO₄²⁻ (26.3 µg m^− 3) > NO₃⁻ (16.8) > NH₄⁺ (15.1) > Ca²⁺ (4.1) > Na⁺ (2.4) > K⁺ (2.1 µg m^− 3) and (ii) winter: SO₄²⁻ (28.9 µg m^− 3) > NO₃⁻ (23.0) > NH₄⁺ (16.4) > Ca²⁺(3.4) > K⁺(3.3) > Na⁺ (3.2 µg m^− 3). The mean molar ratio of NH₄⁺ to SO₄²⁻ was 2.8 ± 0.6 (mostly >2), indicated abundance of NH₃ to neutralize H₂SO₄. The excess of NH₄⁺ was inferred to be associated with NO₃⁻ and Cl⁻. Higher sulfur conversion ratio (F_s: 58%) than nitrogen conversion ratio (F_n: 39%) indicated that SO₄²⁻ was the preferred secondary species to NO₃⁻. The charge balance for the ion chemistry of PM_2.5 revealed that compounds formed from ammonia as precursor are (NH₄)₂SO₄, NH₄NO₃ and NH₄Cl. This study conclusively established that while there are higher contributions of NH₄⁺, SO₄²⁻ to PM_2.5 in summer but for nitrates (in particulate phase), it is the winter season, which is critical because of low temperatures that drives the reaction between ammonia and HNO₃ in forward direction for enhanced nitrate formation. In summary, inorganic secondary aerosol formation accounted for 30% mass of PM_2.5 and any particulate control strategy should include optimal control of primary precursor gases including ammonia.     

Effects of water regime during rice-growing season on annual direct N2O emission in a paddy rice-winter wheat rotation system in southeast China

Annual paddy rice-winter wheat rotation constitutes one of the typical cropping systems in southeast China, in which various water regimes are currently practiced during the rice-growing season, including continuous flooding (F), flooding-midseason drainage-reflooding (F-D-F), and flooding-midseason drainage-reflooding and moisture but without waterlogging (F-D-F-M). We conducted a field experiment in a rice-winter wheat rotation system to gain an insight into the water regime-specific emission factors and background emissions of nitrous oxide (N₂O) over the whole annual cycle. While flooding led to an unpronounced N₂O emission during the rice-growing season, it incurred substantial N₂O emission during the following non-rice season. During the non-rice season, N₂O fluxes were, on average, 2.61 and 2.48 mg N₂O-N m⁻² day^− 1 for the 250 kg N ha^− 1 applied plots preceded by the F and F-D-F water regimes, which are 56% and 49% higher than those by the F-D-F-M water regime, respectively. For the annual rotation system experienced by continuous flooding during the rice-growing season, the relationship between N₂O emission and nitrogen input predicted the emission factor and background emission of N₂O to be 0.87% and 1.77 kg N₂O-N ha^− 1, respectively. For the plots experienced by the water regimes of F-D-F and F-D-F-M, the emission factors of N₂O averaged 0.97% and 0.85%, with background N₂O emissions of 2.00 kg N₂O-N ha^− 1 and 1.61 kg N₂O-N ha^− 1 for the annual rotation system, respectively. Annual direct N₂O-N emission was estimated to be 98.1 Gg yr^− 1 in Chinese rice-based cropping systems in the 1990s, consisting of 32.3 Gg during the rice-growing season and 65.8 Gg during the non-rice season, which accounts for 25-35% of the annual total emission from croplands in China.     

Heat balance and tracer gas technique for airflow rates measurement and gaseous emissions quantification in naturally ventilated livestock buildings

Experiments were performed to study the airflow rates (AFRs) in a naturally ventilated building through four summer seasons and three winter seasons. The AFRs were determined using heat balance (HB), tracer gas technique (TGT) and CO₂-balance as averages of the values of all experiments carried out through the different seasons. The statistical analyses were correlation analysis, regression model and t-test. Continuous measurements of gaseous concentrations (NH₃, CH₄, CO₂ and N₂O) and temperatures inside and outside the building were performed. The HB showed slightly acceptable results through summer seasons and unsatisfactory results through winter seasons. The CO₂-balance showed unexpected high differences to the other methods in some cases. The TGT showed reliable results compared to HB and CO₂-balance. The AFRs, subject to TGT, were 0.12 m³ s⁻¹ m⁻², 1.15 m³ s⁻¹ cow⁻¹, 0.88 m³ s⁻¹ LU⁻¹, 56 h⁻¹, 395 m³ s⁻¹ and 470 kg s⁻¹ through summer seasons, and 0.08 m³ s⁻¹ m⁻², 0.83 m³ s⁻¹ cow⁻¹, 0.64 m³ s⁻¹ LU⁻¹ 39 h⁻¹, 275 m³ s⁻¹ and 328 kg s⁻¹ through winter seasons. The AFRs are not independent values, rather they were estimated for specific reference values, which are: area, cow and LU as well as rates. The emission rates through summer seasons, subject to TGT, were 9.4, 40, 3538 and 2.3 g h⁻¹ cow⁻¹; and through winter seasons were 4.8, 19, 2332 and 2.6 g h⁻¹ cow⁻¹, for NH₃, CH₄, CO₂ and N₂O, respectively.     

Emission of CO2 and N2O from soil cultivated with common bean (Phaseolus vulgaris L.) fertilized with different N sources

Addition of different forms of nitrogen fertilizer to cultivated soil is known to affect carbon dioxide (CO₂) and nitrous oxide (N₂O) emissions. In this study, the effect of urea, wastewater sludge and vermicompost on emissions of CO₂ and N₂O in soil cultivated with bean was investigated. Beans were cultivated in the greenhouse in three consecutive experiments, fertilized with or without wastewater sludge at two application rates (33 and 55 Mg fresh wastewater sludge ha^− 1, i.e. 48 and 80 kg N ha^− 1 considering a N mineralization rate of 40%), vermicompost derived from the wastewater sludge (212 Mg ha^− 1, i.e. 80 kg N ha^− 1) or urea (170 kg ha^− 1, i.e. 80 kg N ha^− 1), while pH, electrolytic conductivity (EC), inorganic nitrogen and CO₂ and N₂O emissions were monitored. Vermicompost added to soil increased EC at onset of the experiment, but thereafter values were similar to the other treatments. Most of the NO₃⁻ was taken up by the plants, although some was leached from the upper to the lower soil layer. CO₂ emission was 375 C kg ha^− 1 y^− 1 in the unamended soil, 340 kg C ha^− 1 y^− 1 in the urea-amended soil and 839 kg ha^− 1 y^− 1 in the vermicompost-amended soil. N₂O emission was 2.92 kg N ha^− 1 y^− 1 in soil amended with 55 Mg wastewater sludge ha^− 1, but only 0.03 kg N ha^− 1 y^− 1 in the unamended soil. The emission of CO₂ was affected by the phenological stage of the plant while organic fertilizer increased the CO₂ and N₂O emission, and the yield per plant. Environmental and economic implications must to be considered to decide how many, how often and what kind of organic fertilizer could be used to increase yields, while limiting soil deterioration and greenhouse gas emissions.     

Application of high rate nitrifying trickling filters for potable water treatment

The interference of ammonia with chlorination is a prevalent problem encountered by water treatment plants located throughout South East Asia. The efficacy of high rate, plastic-packed trickling filters as a pre-treatment process to remove low concentrations of ammonia from polluted surface water was investigated. This paper presents the findings from a series of pilot experiments, which were designed to investigate the effect of specific conditions—namely low ammonia feed concentrations (0.5-5.0 mg NH₄-N L⁻¹), variations in hydraulic surface load (72.5-145 m³ m⁻² d⁻¹) and high suspended solid loads (51 ± 25 mg L⁻¹)—on filter nitrifying capacity. The distribution of nitrification activity throughout a trickling filter bed was also characterised. Results confirmed that high hydraulic rate trickling filters were able to operate successfully, under ammonia-N concentrations some 10- to 50-fold lower and at hydraulic loading rates 30-100 times greater than those of conventional wastewater applications. Mass transport limitations posed by low ammonia-N concentrations on overall filter performance were insignificant, where apparent nitrification rates (0.4-1.6 g NH₄-N m⁻² d⁻¹), equivalent to that of wastewater filters were recorded. High inert suspended solid loadings had no adverse effect on nitrification. Results imply that implementation of high rate trickling filters at the front-end of a water treatment train would reduce the ammonia-related chlorine demand, thereby offering significant cost savings.     

Treating landfill leachate using passive aeration trickling filters; effects of leachate characteristics and temperature on rates and process dynamics

Biological ammoniacal-nitrogen (NH₄⁺-N) and organic carbon (TOC) treatment was investigated in replicated mesoscale attached microbial film trickling filters, treating strong and weak strength landfill leachates in batch mode at temperatures of 3, 10, 15 and 30 °C. Comparing leachates, rates of NH₄⁺-N reduction (0.126-0.159 g m^− 2 d^− 1) were predominantly unaffected by leachate characteristics; there were significant differences in TOC rates (0.072-0.194 g m^− 2 d^− 1) but no trend relating to leachate strength. Rates of total oxidised nitrogen (TON) accumulation (0.012-0.144 g m^− 2 d^− 1) were slower for strong leachates. Comparing temperatures, treatment rates varied between 0.029-0.319 g NH₄⁺-N m^− 2 d^− 1 and 0.033-0.251 g C m^− 2 d^− 1 generally increasing with rising temperatures; rates at 3 °C were 9 and 13% of those at 30 °C for NH₄⁺-N and TOC respectively. For the weak leachates (NH₄⁺-N < 140 mg l^− 1) complete oxidation of NH₄⁺-N was achieved. For the strong leachates (NH₄⁺-N 883-1150 mg l^− 1) a biphasic treatment response resulted in NH₄⁺-N removal efficiencies of between 68 and 88% and for one leachate no direct transformation of NH₄⁺-N to TON in bulk leachate. The temporal decoupling of NH₄⁺-N oxidation and TON accumulation in this leachate could not be fully explained by denitrification, volatilisation or anammox, suggesting temporary storage of N within the treatment system. This study demonstrates that passive aeration trickling filters can treat well-buffered high NH₄⁺-N strength landfill leachates under a range of temperatures and that leachate strength has no effect on initial NH₄⁺-N treatment rates. Whether this approach is a practicable option depends on a range of site specific factors.     

Effect of some parameters on the formation of chloroform during chloramination of aqueous solutions of resorcinol

The effects of various factors (N/Cl ratio used to prepare monochloramine, monochloramine doses, pH and contact time) on the monochloramine demand and on the chloroform yield during chloramination of resorcinol have been investigated. Chloramination experiments were carried out at 24 ± 1 °C, at pH values ranging from 6.5 to 12 using a bicarbonate/carbonate buffer and preformed monochloramine solutions prepared at pH 8.5 with N/Cl ratios ([NH₄Cl]₀/[Total free Cl₂]₀ ranging from 1.0 to 150 mol/mol). Kinetic experiments ([Resorcinol]₀ = 5 or 100 μM, [NH₂Cl]₀/[Resorcinol]₀ = 20 mol/mol, pH = 8.5 ± 0.1) showed a slow increase of the monochloramine consumption with reaction time. The monochloramine demands after reaction times of 7 days ([Resorcinol]₀ = 100 μM) and 14 days ([Resorcinol]₀ = 5 μM) were equal to 8.5 mol of NH₂Cl/mole of resorcinol and were higher than the chlorine demands (≈7.3 mol/mol). Chloroform yields from monochloramination of resorcinol were lower than 8% (<80 mmol of CHCl₃/mole of resorcinol) and were less than the yields obtained by chlorination (0.9-0.95 mol/mol). Chloroform productions increased with increasing monochloramine dose and reaction time and decreased with increasing pH values within the pH range 6.5-10. Chloroform formation markedly decreased when the N/Cl ratio increased from 1 to 1.5 mol/mol and was suppressed at N/Cl > 100 mol/mol. The data obtained in the present work suggest that free chlorine released from monochloramine hydrolysis plays a significant role on the formation of chloroform during chloramination of resorcinol at N/Cl ratios close to unity (1.0 < N/Cl < 1.5).     

Bacterial, viral and turbidity removal by intermittent slow sand filtration for household use in developing countries: experimental investigation and modeling

A two-factor three-block experimental design was developed to permit rigorous evaluation and modeling of the main effects and interactions of sand size (d₁₀ of 0.17 and 0.52 mm) and hydraulic head (10, 20, and 30 cm) on removal of fecal coliform (FC) bacteria, MS2 bacteriophage virus, and turbidity, under two batch operating modes (‘long’ and ‘short’) in intermittent slow sand filters (ISSFs). Long operation involved an overnight pause time between feeding of two successive 20 L batches (16 h average batch residence time (RT)). Short operation involved no pause between two 20 L batch feeds (5 h average batch RT). Conditions tested were representative of those encountered in developing country field settings. Over a ten week period, the 18 experimental filters were fed river water augmented with wastewater (influent turbidity of 5.4-58.6 NTU) and maintained with the wet harrowing method. Linear mixed modeling allowed systematic estimates of the independent marginal effects of each independent variable on each performance outcome of interest while controlling for the effects of variations in a batch’s actual residence time, days since maintenance, and influent turbidity. This is the first study in which simultaneous measurement of bacteria, viruses and turbidity removal at the batch level over an extended duration has been undertaken with a large number of replicate units to permit rigorous modeling of ISSF performance variability within and across a range of likely filter design configurations and operating conditions.On average, the experimental filters removed 1.40 log fecal coliform CFU (SD 0.40 log, N = 249), 0.54 log MS2 PFU (SD 0.42 log, N = 245) and 89.0 percent turbidity (SD 6.9 percent, N = 263). Effluent turbidity averaged 1.24 NTU (SD 0.53 NTU, N = 263) and always remained below 3 NTU. Under the best performing design configuration and operating mode (fine sand, 10 cm head, long operation, initial HLR of 0.01-0.03 m/h), mean 1.82 log removal of bacteria (98.5%) and mean 0.94 log removal of MS2 viruses (88.5%) were achieved.Results point to new recommendations regarding filter design, manufacture, and operation for implementing ISSFs in local settings in developing countries. Sand size emerged as a critical design factor on performance. A single layer of river sand used in this investigation demonstrated removals comparable to those reported for 2 layers of crushed sand. Pause time and increased residence time each emerged as highly beneficial for improving removal performance on all four outcomes. A relatively large and significant negative effect of influent turbidity on MS2 viral removal in the ISSF was measured in parallel with a much smaller weaker positive effect of influent turbidity on FC bacterial removal. Disturbance of the schmutzdecke by wet harrowing showed no effect on virus removal and a modest reductive effect on the bacterial and turbidity removal as measured 7 days or more after the disturbance. For existing coarse sand ISSFs, this research indicates that a reduction in batch feed volume, effectively reducing the operating head and increasing the pore:batch volume ratio, could improve their removal performance by increasing batch residence time.     

Source identification of nitrous oxide on autotrophic partial nitrification in a granular sludge reactor

Emission of nitrous oxide (N₂O) during biological wastewater treatment is of growing concern since N₂O is a major stratospheric ozone-depleting substance and an important greenhouse gas. The emission of N₂O from a lab-scale granular sequencing batch reactor (SBR) for partial nitrification (PN) treating synthetic wastewater without organic carbon was therefore determined in this study, because PN process is known to produce more N₂O than conventional nitrification processes. The average N₂O emission rate from the SBR was 0.32 ± 0.17 mg-N L⁻¹ h⁻¹, corresponding to the average emission of N₂O of 0.8 ± 0.4% of the incoming nitrogen load (1.5 ± 0.8% of the converted NH₄⁺). Analysis of dynamic concentration profiles during one cycle of the SBR operation demonstrated that N₂O concentration in off-gas was the highest just after starting aeration whereas N₂O concentration in effluent was gradually increased in the initial 40 min of the aeration period and was decreased thereafter. Isotopomer analysis was conducted to identify the main N₂O production pathway in the reactor during one cycle. The hydroxylamine (NH₂OH) oxidation pathway accounted for 65% of the total N₂O production in the initial phase during one cycle, whereas contribution of the NO₂⁻ reduction pathway to N₂O production was comparable with that of the NH₂OH oxidation pathway in the latter phase. In addition, spatial distributions of bacteria and their activities in single microbial granules taken from the reactor were determined with microsensors and by in situ hybridization. Partial nitrification occurred mainly in the oxic surface layer of the granules and ammonia-oxidizing bacteria were abundant in this layer. N₂O production was also found mainly in the oxic surface layer. Based on these results, although N₂O was produced mainly via NH₂OH oxidation pathway in the autotrophic partial nitrification reactor, N₂O production mechanisms were complex and could involve multiple N₂O production pathways.     

N2O emission from a partial nitrification-anammox process and identification of a key biological process of N2O emission from anammox granules

Emission of nitrous oxide (N₂O) during biological wastewater treatment is of growing concern. The emission of N₂O from a lab-scale two-reactor partial nitrification (PN)-anammox reactor was therefore determined in this study. The average emission of N₂O from the PN and anammox process was 4.0 ± 1.5% (9.6 ± 3.2% of the removed nitrogen) and 0.1 ± 0.07% (0.14 ± 0.09% of the removed nitrogen) of the incoming nitrogen load, respectively. Thus, a larger part (97.5%) of N₂O was emitted from the PN reactor. The total amount of N₂O emission from the PN reactor was correlated to nitrite (NO₂⁻) concentration in the PN effluent rather than DO concentration. In addition, further studies were performed to indentify a key biological process that is responsible for N₂O emission from the anammox process (i.e., granules). In order to characterize N₂O emission from the anammox granules, the in situ N₂O production rate was determined by using microelectrodes for the first time, which was related to the spatial organization of microbial community of the granule as determined by fluorescence in situ hybridization (FISH). Microelectrode measurement revealed that the active N₂O production zone was located in the inner part of the anammox granule, whereas the active ammonium consumption zone was located above the N₂O production zone. Anammox bacteria were present throughout the granule, whereas ammonium-oxidizing bacteria (AOB) were restricted to only the granule surface. In addition, addition of penicillin G that inhibits most of the heterotrophic denitrifiers and AOB completely inhibited N₂O production in batch experiments. Based on these results obtained, denitrification by putative heterotrophic denitrifiers present in the inner part of the granule was considered the most probable cause of N₂O emission from the anammox reactor (i.e., granules).     

Oxone/Co oxidation as an advanced oxidation process: Comparison with traditional Fenton oxidation for treatment of landfill leachate

In this paper, the application of Fenton and Oxone/Co²⁺ oxidation processes for landfill leachate treatment was investigated. The removal of the chemical oxygen demand (COD), suspended substances (SS) and the color of the landfill leachate by Fenton oxidation to that by Oxone/Co²⁺ oxidation were compared under optimal operational conditions. For Fenton oxidation process, the optimal conditions were determined as: [H₂O₂] = 80 mmol L⁻¹, [H₂O₂]/[Fe²⁺] = 2.0, initial pH = 2.5, reaction temperature = 37.5 ± 1 °C, reaction time = 160 min, number of stepwise addition = 3. Under the given conditions, 56.9% of the COD removal efficiency was achieved, but the SS and the color of the treated landfill leachate increased due to the generation of a large quantity of ferric hydroxide sludge. In reference to Oxone/Co²⁺ oxidation process, the optimal conditions were determined as: [Oxone] = 4.5 mmol L⁻¹, [Oxone]/[Co²⁺] = 10⁴, pH = 6.5, reaction temperature = 30 ± 1 °C, reaction time = 300 min, number of stepwise addition = 7, the COD, SS and the color removal efficiencies were 57.5, 53.3 and 83.3%, respectively. From this work, it can be concluded that Oxone/Co²⁺ oxidation process demonstrated higher degradation efficiencies of the COD, SS and color for landfill leachate treatment than that by Fenton oxidation process. It also suggested that Oxone/Co²⁺ oxidation process could be considered as one of the most promising technologies for practical applicability to treat landfill leachate in large scale. For further improving the efficiency of Oxone/Co²⁺ oxidation process, we proposed that combination of it with other technologies in future such as ultraviolet, ultrasound and biological methods.