Electro-stimulated anaerobic oxidation of methane with synergistic denitrification by adding AQS: Electron transfer mode and mechanism.

Denitrifying anaerobic methane-oxidizing (DAMO) processes, which link anaerobic methane oxidation (AMO) and denitrification, have a promising prospect in anaerobic wastewater treatment. In bioelectrochemical systems (BES), DAMO consortium presented potent metabolic activity. However, the extracellular electron transfer (EET) in BES was poorly understood. This study investigated the EET mechanisms and modes of electron transport in BES dominated by anaerobic methanotrophic bacteria. In the bioreactors with the auxiliary voltage of 0.5 and 1.1 V, named EMN-0.5 and EMN-1.1, respectively, biological voltages of 0.198 and 0.329 V were generated with power densities of 0.6 and 1.20 mW/m2, after removing the voltage. High throughput and metagenome analyses demonstrated that main methanotrophs were DAMO bacteria and Methylocystis sp. The electroactive bacteria detected were Pseudomonas sp., Hypomicrobium sp., Thiobacillus sp, and Rhodococcus sp. The pil, cytochrome c, hdr, and he/fp genes related to EET were present on the electrode surfaces. Carbon 13 isotope tracing and chemicals analysis by GC-MS exhibited that methanol was an intermediate product released to extracellular environment and acted as the electronic carrier to drive the EET in methane oxidation. Extracellular electron transfer was achieved through the collaboration of DAMO bacteria, Methylocystis sp., and Pseudomonas sp. Anthraquinone 2-sulfonic acid ester (AQS) could improve the rate of electron transfer to the extracellular space, especially in the EMN-0.5 reaction system. This study provides a new understanding of AMO consortium metabolism in BES and may provide a scientific basis for developing methane control technology.

Escape and functional alterations of microbial aerosol particles containing Pseudomonas sp. during wastewater treatment.

Wastewater treatment plants (WWTP) are considered sources of bioaerosols emission that negatively affects the surrounding atmosphere. This study focused on Pseudomonas sp. Emissions in bioaerosols from a WWTP that adopts the A2O treatment process, and their inactivation through ultraviolet (UV) radiation. High-throughput sequencing was used to assay the microbial population, and functional composition profiles were predicted using 16 S rRNA sequencing data with PICRUSt2. Recorded emission levels of airborne bacteria and Pseudomonas sp. In WWTP were 130 ± 83-6113 ± 3015 CFU/m3 and 0-6431 ± 1945 CFU/m3, respectively. Bioaerosol emissions presented site-related and temporal variation. Over 80% of Pseudomonas sp. Were attached to coarse particles with sizes over 2.1 µm. Bioaerosol concentration and particle-size distribution in the air were closely related to ambient temperature, relative humidity, light intensity, and wind speed. Exposure to 45.67 µW/cm3 UV radiation led to a significant decline in bioaerosol concentrations in the air, and reduction rate reached 89.16% and 95.77% for airborne bacteria and Pseudomonas sp., respectively. The results suggested that UV radiation can be an effective method in reducing bioaerosols. Compared with other bacteria, Pseudomonas stutzeri and Bacillus sp. Are more resistant to UV radiation. The abundance of antibiotic resistance genes noticeably receded when exposed to UV irradiation. The relative abundance of cationic antimicrobial peptide resistance, categorized under human diseases in KEGG (level 3), significantly decreased in Pseudomonas sp. After 120 min of UV irradiation. This study provides a novel insight into the control of bioaerosol emissions carrying pathogenic bacteria.

Emission behavior and impact assessment of gaseous volatile compounds in two typical rural domestic waste landfills.

Landfill sites are sources of gaseous volatile compounds. The dumping area (LDA) and leachate storage pool (LSP) of two typical rural domestic waste landfill sites in north China (NLF) and southwest China (SLF) were investigated. We found that 45, 46, 61 and 68 volatile organic compounds (VOC) were present in the air of NLF-LDA, NLF-LSP, SLF-LDA, and SLF-LSP, respectively. And there were 27, 29, 35 and 37 kinds of odorous compounds being detected. Oxygenated compounds (>48.88%), chlorinated compounds (>6.85%), and aromatics (>5.46%), such as organic acid, 1-chlorobutane, and benzene, were the most abundant compounds in both landfills. The SLF-LDA had the highest olfactory effect, with a corresponding total odor activity value of 29,635.39. The ozone-formation potential analysis showed that VOCs emitted from SLF landfills had significantly higher potential for ozone formation than those from NLF landfills, with ozone generation potentials of 166.02, 225.86, 2511.82, and 1615.99 mg/m3 for the NLF-LDA, NLF-LSP, SLF-LDA, and SLF-LSP, respectively. Higher chronic toxicity and cancer risk of VOCs were found in the SLF according to method of Risk Assessment Information System. Based on the sensitivity analysis by the Monte Carlo method, concentrations of benzene, propylene oxide, propylene, trichloroethylene, and N-nitrosodiethylamine, along with exposure duration, daily exposure time, and annual exposure frequency, significantly impacted the risk levels. We provide a scientific basis, which reflects the need for controlling and reducing gaseous pollutants from landfills, particularly rural residential landfills, which may improve rural sanitation.

Dispersion, olfactory effect, and health risks of VOCs and odors in a rural domestic waste transfer station.

The impact of odorous gases emitted from refuse transfer stations has always been a concern raised by the surrounding residents. The emitted volatile organic compounds (VOCs) and odors were investigated in a rural solid waste transfer station (RSWTS) located in Southwest China. A total of 70 VOCs were identified and quantified. The total VOCs (TVOCs) concentrations varied from 848.38 to 31193.24 µg/m3. Inorganic odor and greenhouse gases concentrations ranged from 39.11 to 470.14 µg/m3 and 1.03-525.42 µg/m3, respectively. Oxygenated compounds contributed the most (58.25%) to the VOCs. Among the oxygenated compounds, ketones, esters, and ethers were the dominant categories, accounting for 67.5%, 12.70%, and 11.85%, respectively. The key odorants included propionaldehyde, hexanaldehyde, propionic acid, acetaldehyde, and disopropyl ether. N-nitrosodiethylamine, acrylonitrile, and 1,3-Butadiene were the three main carcinogens that pose considerable risk to human health. Allyl chloride was the most non-carcinogenic pathogen among the VOCs detected in RSWTS. With diffusion in the downwind direction, the concentration of VOCs decreased gradually, and their risks weakened accordingly. At the sampling site of RSWTS-10, located 100 m away from RSWTS, acrylonitrile and 1,3-Butadiene still presented an unacceptable carcinogenic risk to human health. This study provides new data for assessing the emission characteristics, olfactory effects, and health risks of trace VOCs, especially those released from RSWTS.

Conversion and speculated pathway of methane anaerobic oxidation co-driven by nitrite and sulfate.

Anaerobic sludge from sewage treatment was employed to derive a microbial colony that is capable of anaerobic oxidation of methane coupled with sulfate reduction and denitrification. Investigations revealed that methane can be oxidized with sulfate reduction and denitrification. When sulfate and nitrite acted as electron acceptors together, the rates and amount of methane conversion were higher than that when sulfate or nitrite alone was employed as an electron acceptor. The oxidation rate and amount of methane conversion reached 1.9 mg/(d•gVSS) and 22.24 mg, respectively. Methanotrophic bacteria, such as M. oxyfera, and Methylocystis sp., sulfate-reducing bacteria (SRB), e.g. Desulfosporosinus sp., and Desulfuromonas sp.; and denitrification bacteria, such as Hyphomicrobium sp., and Diaphorobacter sp., presented in the bacterial community. Anaerobic methanotrophic archaea (ANME), including Methanosaeta sp. and Methanobacterium sp. were found in the archaeal community. These findings indicate the coexistence of ANME, SRB and denitrification bacteria in the system. Nitrite reduction coupled with methane oxidation was performed independently by M. oxyfera during which limited oxygen generated. The oxygen released may be utilized by methanotrophic bacteria to produce organics, which could be used by denitrifying bacteria to reduce nitrite. Methanotrophic archaea could also oxidize methane to carbon dioxide or organics by reverse methanogenesis whereas sulfate was reduced to sulfide by SRB. This study opens possibility for biotechnological process of sulfate reduction and denitrification with methane as electron donor and provides a method for the synergistic treatment of wastewater containing sulfate/nitrite and waste gas containing methane.

Emission, dispersion, and potential risk of volatile organic and odorous compounds in the exhaust gas from two sludge thermal drying processes.

Emissions of odorous and volatile organic compounds (VOCs) were investigated between two sludge drying methods. A total of 37 chemical compounds were identified and quantified from the off-gases from sludge drying by indirect drying method. The total number of VOCs detected ranged from 3.45 × 10-3 to 4.53 mg/m3, which includes benzene series, volatile organic sulfur, and nitrogenous organic compounds. High emissions were found in the exhaust gas released from drying workshop that used direct drying method. Sulfur dioxide, aromatics, and chlorinated compounds were dominant. Based on the olfactory effect analysis and cancer risk assessment, the main odor-causing gaseous pollutants were methyl mercaptan and methyl sulfide (for indirect sludge drying process) and SO2 (for direct sludge drying process), while the dominant carcinogens were benzene, carbon tetrachloride, chloroform, and methylene. This study provides new insights into the emission characteristics, olfactory effects, and cancer risks of VOCs and odorous compounds in the exhaust gas from thermal sludge drying processes.

Microbial aerosol particles in four seasons of sanitary landfill site: Molecular approaches, traceability and risk assessment.

Landfill sites are regarded as prominent sources of bioaerosols for the surrounding atmosphere. The present study focused on the emission of airborne bacteria and fungi in four seasons of a sanitary landfill site. The main species found in bioaerosols were assayed using high-throughput sequencing. The SourceTracker method was utilized to identify the sources of the bioaerosols present at the boundary of the landfill site. Furthermore, the health consequences of the exposure to bioaerosols were evaluated based on the average daily dose rates. Results showed that the concentrations of airborne bacteria in the operation area (OPA) and the leakage treatment area (LTA) were in the range of (4684 ± 477)-(10883 ± 1395) CFU/m3 and (3179 ± 453)-(9051 ± 738) CFU/m3, respectively. The average emission levels of fungal aerosols were 4026 CFU/m3 for OPA and 1295 CFU/m3 for LTA. The landfill site received the maximum bioaerosol load during summer and the minimum during winter. Approximately 41.39%- 86.24% of the airborne bacteria had a particle size of 1.1 to 4.7 µm, whereas 48.27%- 66.45% of the airborne fungi had a particle size of more than 4.7 µm. Bacillus sp., Brevibacillus sp., and Paenibacillus sp. were abundant in the bacterial population, whereas Penicillium sp. and Aspergillus sp. dominated the fungal population. Bioaerosols released from the working area and treatment of leachate were the two main sources that emerged in the surrounding air of the landfill site boundary. The exposure risks during summer and autumn were higher than those in spring and winter.

Electrochemical system for anaerobic oxidation of methane by DAMO microbes with nitrite as an electron acceptor.

Denitrifying anaerobic methane oxidation (DAMO) is an important microbial metabolic process that simultaneously converts of methane and nitrite. In this study, electrochemical systems were investigated for DAMO with nitrite as an electron acceptor. The results showed that the auxiliary voltage enhanced anaerobic methane oxidation and nitrite reduction. The greatest methane conversion (26.61 mg L-1 d-1) was obtained at an auxiliary voltage of 1.6 V (EMN-1.6). Isotope tracing indicated that carbon dioxide was the oxidation product of methane, and methanol was the intermediate. The power density reached 0.60 (for EMN-0.5, the bioreactor with a voltage of 0.5 V) and 3.77 mW m-2 (for EMN-1.6). DAMO microbes, Methylocystis sp., and Methylomonas sp. were identified as methanotrophs. Rhodococcus sp., Hyphomicrobium sp., and Thiobacillus sp. were the dominant denitrifying bacteria. The conversion pathway was speculated to be as follows: methane was oxidized to carbon dioxide and nitrite was reduced to nitrogen. The two processes were independently completed by DAMO bacteria and oxygen was simultaneously generated. For the electron transfer pathway, methanotrophs utilized the oxygen released by DAMO bacteria to convert methane into organic matter (e.g. methanol). These organic compounds were utilized by Pseudoxanthomonas sp. and Pseudomonas sp., and the generated electrons were then released to the outside of the cells and transferred to the anode. Denitrifying bacteria received electrons at the cathode, transferred them to the interior of the cell, and then converted nitrite into nitrogen. This research explored an effective consortium and a method for methane and nitrogen removal.

Trace volatile compounds in the air of domestic waste landfill site: Identification, olfactory effect and cancer risk.

Landfill sites are regarded as sources of volatile compounds (VOCs) and odors emitted to the atmosphere. Surface emissions of VOCs and odors were investigated in a rural domestic waste landfill site located in southwest China. A total of 76 chemical compounds belonging to 3 chemical families were identified and quantified. The total number of VOCs (TVOC) detected ranged from 18.1 to 806.3 mg/m3, while odorous gases and greenhouse gases ranged from 0.4 to 21.2 and 0-100.5 mg/m3, respectively. High emissions were found in the air surrounding the leachate storage pool (LSP) and dumping area (DPA). The dominant species of VOCs were hexaldehyde, m-xylene, propylene oxide, acetophenone, and 2-butanone. The traceability analysis showed that the odors and VOCs diffused to the downwind boundary mainly came from the DPA and LSP. According to the olfactory effect analysis and cancer risk assessment, the main odor-causing gaseous pollutants were hydrogen sulfide, propionic acid, styrene, and 2-pentanone, while benzene, trichlorethylene, and 1,3-butadiene were the dominant carcinogens. This study provides new insights into the emission characteristics, olfactory effects, and cancer risks of VOCs and odors emitted from rural domestic solid waste landfill sites.

Comparison and application of biofilter and suspended bioreactor in removing gaseous o-xylene.

Two bioreactors, suspended-growth bioreactors (SPB) and biofilter (BF), were compared for the performances in removing gaseous o-xylene. Their efficiencies were investigated by varying the o-xylene loadings, gas flow rates, and gas-water ratios. High-throughput techniques were applied for the microbial populations assay. The conversion rate of carbon in o-xylene was calculated, and the relationship between biomass and removal efficiencies was also analyzed. Results indicated that both the SPB and BF could effectively treat gases containing o-xylene. The average removal efficiencies were 91.8% and 93.5%, respectively. The elimination capacity of the BF was much higher than that of the SPB when the intake load was below 150 g m-3 h-1. When the o-xylene loadings were over 150 g m-3 h-1, both the SPB and BF achieved similar o-xylene removal rates. The maximum elimination capacities were 28.36 g m-3 h-1 for the SPB and 30.67 g m-3 h-1 for BF. The SPB was more sensitive to the changes in the gas flow rate. Results of microbial assay indicated that bacteria e.g. Mycobacterium sp. and Rhodanobacter sp. might play important roles in removing o-xylene in the SPB, while the bacteria Pseudomonas sp., Sphingomonas sp., and Defluviicoccus sp., and the fungi Aspergillus sp. and Scedosporium sp., were the o-xylene degraders in the BF. The successful application of the integrated bioreactor in treating gases containing o-xylene exhausted from the electroplating plant indicated that the integration of SPB and BF could be an effective method for removing VOCs with Henry coefficient in the range of 0.01-1.

Auxiliary voltage enhanced microbial methane oxidation co-driven by nitrite and sulfate reduction.

In this study, single-chamber bioelectrochemical reactors (EMNS) were used to investigate the methane oxidation driven by sulfate and nitrite reduction with the auxiliary voltage. Results showed that the methane oxidation was simultaneously driven by sulfate and nitrite reduction, with more methane being converted using the auxiliary voltage. When the voltage was 1.6 V, the maximum removal rate was achieved at 8.05 mg L-1 d-1. Carbon dioxide and methanol were the main products of methane oxidation. Simultaneously, nitrogen, nitrous oxide, sulfur ions, and hydrogen sulfide were detected as products of sulfate and nitrite reduction. Microbial populations were analyzed by qPCR and high-throughput sequencing. The detected methanotrophs included Methylocaldum sp., Methylocystis sp., Methylobacter sp. and M. oxyfera. The highest abundance of M. oxyfera was (3.97 ± 0.32) × 106 copies L-1 in the EMNS-1.6. The dominant nitrite-reducing bacteria were Ignavibacterium sp., Hyphomicrobium sp., Alicycliphilus sp., and Anammox bacteria. Desulfovibrio sp., Desulfosporosinus sp. and Thiobacillus sp. were related to the sulfur cycle. Ignavibacterium sp., Thiobacillus sp. and Desulfovibrio sp. may transfer electrons with electrodes using humic acids as the electronic shuttle. The possible pathways included (1) Methane was mainly oxidized to carbon dioxide and dissolved organic matters by methanotrophs utilizing the oxygen produced by the disproportionation in the cells of M. oxyfera. (2) Nitrite was reduced to nitrogen by heterotrophic denitrifying bacteria with dissolved organic compounds. (3) Desulfovibrio sp. and Desulfosporosinus sp. reduced sulfate to sulfur ions. Thiobacillus sp. oxidized sulfur ions to sulfur or sulfate using nitrite as the electron acceptor.

[Particle Size Distribution and Population Characteristics of Airborne Bacteria Emitted from a Sanitary Landfill Site].

Sanitary landfill is a commonly-used method for solid waste disposal. In the process of landfilling, e. g. dumping, stacking, pushing, and compacting, a large number of bioaerosols with pathogenic bacteria will be generated. That can result in air pollution and significant harm to human health if these pathogens are released into the air. Sampling sites were set up in a domestic waste sanitary landfill in North China to collect airborne bacteria in the air. Airborne bacteria, particle size distributions, and populations were analyzed, and the influence of meteorological parameters (temperature, relative humidity (RH), and wind speed (WS)) on the emission of airborne bacteria was also investigated. Results showed that the concentrations of airborne bacteria in the working area and the coverage area were (5437±572) CFU·m-3 and (2707±396) CFU·m-3, respectively. The emission level in the leachate treatment area was the highest, with an average of 9460 CFU·m-3. The concentration of airborne bacteria showed clear seasonal variation, being was much higher in summer than that in the other seasons. Redundancy analysis (RDA) demonstrated that RH, temperature, and WS affected the number of airborne bacteria in the air. The peaks in the airborne particle size distribution were 2.1-4.7 µm in the working area and 0.65-2.1 µm in the coverage area. Most of the airborne bacteria released from the leachate treatment processes were larger than 4.7 µm. Moraxellaceae, Bacillus aerius, Arcobacter, and Aeromonas were potential or opportunistic pathogens detected from the airborne bacteria samples. Effective measures should be taken to reduce the amount of bacterial aerosol emitted to the air in landfill working areas and in the leachate of treatment areas. Operators of landfill machinery and leachate treatment facilities should consider personal protection measures and should reduce their exposure to microbial aerosols in order to prevent disease.

Long-term nitrate removal through methane-dependent denitrification microorganisms in sequencing batch reactors fed with only nitrate and methane.

Denitrifying anaerobic methane oxidation (damo) bioprocesses can remove nitrate using methane as the electron donor, which gains great concern due to the current stringent discharge standard of nitrogen in wastewater treatment plants. To obtain an engineering acceptable nitrogen removal rate (NRR) and demonstrate the long-term stable ability of damo system under conditions of nitrate and methane, two sequencing batch reactors (SBRs) fed with only nitrate and methane were operated for more than 600 days at 30 °C. The NRR of 21.91 ± 0.73 mg NO3--N L-1 day-1 was obtained which is, to the best of our knowledge, the highest rate observed in the literatures under such conditions. The temperature was found to significantly affect the system performance. Furthermore, the microbial community was analyzed by using real-time PCR technique. The results showed that the microbial consortium contained damo archaea and bacteria. These two microbes cooperated to maintain the long-term stability. And the number of damo archaea was higher than that of damo bacteria with the ratio of 1.77. By using methane as the electron donor, damo archaea reduced nitrate to nitrite coupled to methane oxidation and damo bacteria reduce the generated nitrite to nitrogen gas. The first step of nitrate to nitrite taken by damo archaea might be the limiting step of this cooperation system. SBR could be a suitable reactor configuration to enrich slow-growing microbes like damo culture. These results demonstrated the potential application of damo processes for nitrogen removal of wastewater containing low C/N ratios.