Anaerobic oxidation of methane coupled to sulfate reduction: Consortium characteristics and application in co-removal of H2S and methane

Anaerobic sludge from a sewage treatment plant was used to acclimatize microbial colonies capable of anaerobic oxidation of methane (AOM) coupled to sulfate reduction. Clone libraries and fluorescence in situ hybridization were used to investigate the microbial population. Sulfate-reducing bacteria (SRB) (e.g., Desulfotomaculum arcticum and Desulfobulbus propionicus) and anaerobic methanotrophic archaea (ANME) (e.g., Methanosaeta sp. and Methanolinea sp.) coexisted in the enrichment. The archaeal and bacterial cells were randomly or evenly distributed throughout the consortia. Accompanied by sulfate reduction, methane was oxidized anaerobically by the consortia of methane-oxidizing archaea and SRB. Moreover, CH₄ and SO₄^2 ? were consumed by methanotrophs and sulfate reducers with CO₂ and H₂S as products. The H₃CSH produced by methanotrophy was an intermediate product during the process. The methanotrophic enrichment was inoculated in a down-flow biofilter for the treatment of methane and H₂S from a landfill site. On average, 93.33% of H₂S and 10.71% of methane was successfully reduced in the biofilter. This study tries to provide effective method for the synergistic treatment of waste gas containing sulfur compounds and CH₄.     

Detailed in-furnace measurements with reburning of superfine pulverized coal in high CO2 concentration

This paper presents detailed measurements of gaseous species during the reburning process with high CO₂ concentration in a bench-scale furnace. Superfine pulverized coal, with the average particle size below or around 20 μm, is used as the reburning fuel. The data of flue gas concentration (NO_x, HCN, NH₃, CH₄, O₂, CO, CO₂ etc.) is obtained in order to reveal the intrinsic connection between NO_x emissions and other influential gaseous species at different positions of the furnace. The finding concludes that the advantage of superfine pulverized coal with regard to NO reduction is more efficient in homogeneous stage rather than heterogeneous stage. Meanwhile, the evolution of HCN and CH₄ agrees well with each stage of NO reduction, which indicates that these gaseous species are favorable for NO abatement. Eventually, oxygen consumption rate for superfine pulverized coal is relatively faster, conducive to strengthen both homogeneous and heterogeneous NO reduction under CO₂ reburning condition.     

Turnover of dissolved organic carbon fuels nocturnal CO2 emissions from a headwater catchment reservoir, Southeastern China: Effects of ecosystem metabolism on source partitioning of CO2 emissions

Dam reservoirs in headwater catchments, as critical zones for their proximity to terrestrial sources, play important roles in dissolved organic carbon (DOC) cycling. However, the effects of ecosystem metabolism (EM) on DOC cycling are not well known. Here, in-situ diurnal and monthly observations were conducted to measure EM (including gross primary production (GPP), ecosystem respiration (ER) and heterotrophic respiration (HR)), DOC turnover and CO₂ emissions in a headwater catchment reservoir in Southeastern China in 2020. Our study showed the nocturnal CO₂ emission rate was about twice as high as in daytime, and was strongly driven by EM. The values for DOC turnover velocity ranged from 0.10 to 1.59 m/day, and the average DOC turnover rate was 0.13 day⁻¹, with the average removal efficiency of 12%. The contribution of respired DOC to daily CO₂ emissions ranged from 17% to 61%. The accumulated efficiencies were estimated to be 13% for the selected 15 reservoirs throughout the Changjiang River network, corresponding to about 0.34 Tg C/year of the respired DOC. The modified CO₂ flux was 0.75 Tg C/year, and respired DOC accounted for about 45% of total emitted CO₂ from the 15 larger reservoirs. Our research emphasizes the necessity of incorporating the effects of EM into studies of reservoir DOC removal and CO₂ emissions.     

Carbonate-induced enhancement of phenols degradation in CuS/peroxymonosulfate system: A clear correlation between this enhancement and electronic effects of phenols substituents

This study investigated the enhancement effects of dissolved carbonates on the peroxymonosulfate-based advanced oxidation process with CuS as a catalyst. It was found that the added CO₃²⁻ increased both the catalytic activity and the stability of the catalyst. Under optimized reaction conditions in the presence of CO₃²⁻, the degradation removal of 4-methylphenol (4-MP) within 2 min reached 100%, and this was maintained in consecutive multi-cycle experiments. The degradation rate constant of 4-MP was 2.159 min⁻¹, being 685% greater than that in the absence of CO₃²⁻ (0.315 min⁻¹). The comparison of dominated active species and 4-MP degradation pathways in both CO₃²⁻-free and CO₃²⁻-containing systems suggested that more CO₃•⁻/¹O₂ was produced in the case of CO₃²⁻deducing an electron transfer medium, which tending to react with electron-rich moieties. Meanwhile, Characterization by X-ray photoelectron spectroscopic and cyclic voltammetry measurement verified CO₃²⁻ enabled the effective reduction of Cu²⁺ to Cu⁺. By investigating the degradation of 11 phenolics with different substituents, the dependence of degradation kinetic rate constant of the phenolics on their chemical structures indicated that there was a good linear relationship between the Hammett constants σ_p of the aromatic phenolics and the logarithm of k in the CO₃²⁻-containing system. This work provides a new strategy for efficient removal of electron-rich moieties under the driving of carbonate being widely present in actual water bodies.     

Methane emission via sediment and water interface in the Bohai Sea, China

Sediment is recognized as the largest reservoir and source of methane (CH₄) in the ocean, especially in the shallow coastal areas. To date, few data of CH₄ concentration in sediment have been reported in the China shelf seas. In this study, we measured CH₄ concentration in sediment and overlying seawater columns, and conducted an incubation experiment in the Bohai Sea in May 2017. CH₄ concentration was found to be ranged from 3.075 to 1.795 μmol/L in sediment, which was 2 to 3 orders of magnitude higher than that in overlying seawater columns. The surface sediment was an important source of CH₄, while bottom seawater acted as its sink. Furthermore, the net emission rate via sediment water interface (SWI) was calculated as 2.45 μmol/(m²∙day) based on the incubation experiment at station 73, and the earthquake may enhance CH₄ release from sediment to seawater column in the eastern Bohai Sea.     

Component regulation in novel La-Co-O-C composite catalyst for boosted redox reactions and enhanced thermal stability in methane combustion

A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation. It was demonstrated that Co₃O₄ phase was the main component in regulation. The combined results of X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption of oxygen (O₂-TPD), temperature-programmed reduction of hydrogen (H₂-TPR), temperature-programmed desorption of ammonia/carbon dioxide (NH₃/CO₂-TPD) revealed that component regulation led to more oxygen vacancies and exposure of surface Co²⁺, lower surface basicity and optimized acidity, which were beneficial for adsorption of active oxygen species and activation of methane molecules, resulting in the excellent catalytic oxidation performance. Especially, the (3.5)LC-C (3.5 is Co-to-La molar ratio) showed the optimum activity and the T₅₀ and T₉₀ (the temperature at which the CH₄ conversion rate was 50% and 90%, respectively) were 318 and 367°C, respectively. Using theoretical calculations and in situ diffuse reflection infrared Fourier transform spectroscopy characterization, it was also found that the catalytic mechanism changes from the “Rideal-Eley” mechanism to the “Two-term” mechanism depending on the temperature windows in which the reaction takes place. Besides, the use of the “Flynn-Wall-Ozawa” model in thermoanalytical kinetics revealed that component regulation simultaneously optimized the decomposition activation energy, further expanding the application scope of carbon-containing composites.     

Applying a new method for direct collection, volume quantification and determination of N2 emission from water

The emission of N₂ is important to remove excess N from lakes, ponds, and wetlands. To investigate the gas emission from water, Gao et al. (2013) developed a new method using a bubble trap device to collect gas samples from waters. However, the determination accuracy of sampling volume and gas component concentration was still debatable. In this study, the method was optimized for in situ sampling, accurate volume measurement and direct injection to a gas chromatograph for the analysis of N₂ and other gases. By the optimized new method, the recovery rate for N₂ was 100.28% on average; the mean coefficient of determination (R²) was 0.9997; the limit of detection was 0.02%. We further assessed the effects of the new method, bottle full of water, vs. vacuum bag and vacuum vial methods, on variations of N₂ concentration as influenced by sample storage times of 1, 2, 3, 5, and 7 days at constant temperature of 15°C, using indices of averaged relative peak area (%) in comparison with the averaged relative peak area of each method at 0 day. The indices of the bottle full of water method were the lowest (99.5%-108.5%) compared to the indices of vacuum bag and vacuum vial methods (119%-217%). Meanwhile, the gas chromatograph determination of other gas components (O₂, CH₄, and N₂O) was also accurate. The new method was an alternative way to investigate N₂ released from various kinds of aquatic ecosystems.     

Effect of C/N ratio, aeration rate and moisture content on ammonia and greenhouse gas emission during the composting

Gaseous emission (N₂O, CH₄ and NH₃) from composting can be an important source of anthropogenic greenhouse gas and air pollution. A laboratory scale orthogonal experiment was conducted to estimate the effects of C/N ratio, aeration rate and initial moisture content on gaseous emission during the composting of pig faeces from Chinese Ganqinfen system. The results showed that about 23.9% to 45.6% of total organic carbon (TOC) was lost in the form of CO₂ and 0.8% to 7.5% of TOC emitted as CH₄. Most of the nitrogen was lost in the form of NH₃, which account for 9.6% to 32.4% of initial nitrogen. N₂O was also an important way of nitrogen losses and 1.5% to 7.3% of initial total nitrogen was lost as it. Statistic analysis showed that the aeration rate is the most important factor which could affect the NH₃ (p = 0.0189), CH₄ (p = 0.0113) and N₂O (p = 0.0493) emissions significantly. Higher aeration rates reduce the CH₄ emission but increase the NH₃ and N₂O losses. C/N ratio could affect the NH₃ (p = 0.0442) and CH₄ (p = 0.0246) emissions significantly, but not the N₂O. Lower C/N ratio caused higher NH₃ and CH₄ emissions. The initial moisture content can not influence the gaseous emission significantly. Most treatments were matured after 37 days, except a trial with high moisture content and a low C/N ratio.     

Dramatic decline of observed atmospheric CO2 and CH4 during the COVID-19 lockdown over the Yangtze River Delta of China

The temporal variation of greenhouse gas concentrations in China during the COVID-19 lockdown in China is analyzed in this work using high resolution measurements of near surface △CO₂, △CH₄ and △CO concentrations above the background conditions at Lin'an station (LAN), a regional background station in the Yangtze River Delta region. During the pre-lockdown observational period (IOP-1), both △CO₂ and △CH₄ exhibited a significant increasing trend relative to the 2011-2019 climatological mean. The reduction of △CO₂, △CH₄ and △CO during the lockdown observational period (IOP-2) (which also coincided with the Chinese New Year Holiday) reached up to 15.0 ppm, 14.2 ppb and 146.8 ppb, respectively, and a reduction of △CO₂/△CO probably due to a dramatic reduction from industrial emissions. △CO₂, △CH₄ and △CO were observed to keep declining during the post-lockdown easing phase (IOP-3), which is the synthetic result of lower than normal CO₂ emissions from rural regions around LAN coupled with strong uptake of the terrestrial ecosystem. Interestingly, the trend reversed to gradual increase for all species during the later easing phase (IOP-4), with △CO₂/△CO constantly increasing from IOP-2 to IOP-3 and finally IOP-4, consistent with recovery in industrial emissions associated with the staged resumption of economic activity. On average, △CO₂ declined sharply throughout the days during IOP-2 but increased gradually throughout the days during IOP-4. The findings showcase the significant role of emission reduction in accounting for the dramatic changes in measured atmospheric △CO₂ and △CH₄ associated with the COVID-19 lockdown and recovery.     

低温等离子体氧化甲烷的实验研究

采用电容耦合等离子体对干空气中的甲烷进行氧化实验,对甲烷的分解效率、反应产物进行了分析。并且和放置催化剂时进行对比,结果表明放置催化剂后,甲烷的分解效率明显提高,反应产物中CO2 的选择性增加。甲烷的最终氧化产物都为CO、CO2 和H2 O。     

准好氧填埋工艺氧气浓度对甲烷与二氧化碳浓度的影响研究

构建了准好氧填埋模拟装置,在其产气相对稳定期间,测定填埋装置内不同点位的ψ(O₂),ψ(CH₄)和ψ(CO₂),并用数学模型对ψ(O₂)与ψ(CH₄)和ψ(CO₂)之间的关系进行拟合.结果表明:随着ψ(O₂)的增加,上层ψ(CH₄)呈对数规律下降,而ψ(CO₂)呈线性规律下降;中层ψ(CH₄)和ψ(CO₂)均呈指数规律下降;下层ψ(CH₄)呈指数规律下降,而ψ(CO₂)先保持在34%左右波动,当ψ(O₂)大于1.8%后呈指数规律下降.上层主要为好氧带,ψ(CH₄)低于ψ(CO₂);中层主要为兼氧带,当ψ(O₂)小于5.8%时ψ(CH₄)高于ψ(CO₂),而当ψ(O₂)大于5.8%时ψ(CH₄)低于ψ(CO₂);下层主要为厌氧带,当ψ(O₂)小于2.8%时ψ(CH₄)高于ψ(CO₂),而当ψ(O₂)大于2.8%时ψ(CH₄)低于ψ(CO₂).      

磁场对厌氧除Cr(Ⅵ)工艺产气组成的影响及其机理分析

研究了磁场对优势菌去除Cr(Ⅵ)生物系统出水pH与ρ(COD_(Cr))以及产气中ρ(H_2S),ρ(NH_3),ρ(H_2),ρ(CH_4),ρ(CO_2)和ρ(VOCs)的影响. 结果表明:磁场系统(系统B)出水pH均比无磁系统(系统A)略低;系统B对COD_(Cr)的消耗效率明显高于系统A;磁场的引入能抑制H_2S和NH_3的产生. 在初始ρ[Cr(Ⅵ)]从30 mg/L增至60 mg/L时,系统A和B产气组分中的ρ(H_2S)和ρ(NH_3)均有所增大,增幅分别为28.67%～32.87%和62.65%～70.89%;初始ρ[Cr(Ⅵ)]为30 mg/L时,系统B产气中的ρ(CH_4)为系统A的3.1倍,其ρ(CO_2)比系统A高33.33%,ρ(VOCs)比系统A低14.75%;初始ρ[Cr(Ⅵ)]增至60 mg/L时,两系统产气中的ρ(CH_4)相等,ρ(CO_2)均有所下降,ρ(VOCs)均明显升高. 两系统产气中均未检出H_2. 从生理生化过程角度分析了磁场影响厌氧产气过程的机理.     

炭黑尾气中可燃气态污染物的净化及余热利用

研究炭黑生产尾气中可燃气态污染物CO、H₂及CH₄等的净化及其余热利用。研究结果表明,采用直接燃烧法,不仅可将炭黑尾气中可燃气态污染物转化为无害的物质CO₂和H_2,O,并可回收利用燃烧热,使炭黑生产余热利用率提高40％以上。直接燃烧装置可采用低热值尾气余热锅炉,并配置发电机组,即炭黑尾气发电。经济技术评价表明,采用直接燃烧法和炭黑尾气发电,其经济效益和环境效益十分可观。     

黔中喀斯特石漠化地区土壤温室气体浓度的时空分布特征

2006~2007年对喀斯特石漠化地区土壤剖面中CO2、N2O和CH4的浓度分布进行观测.结果表明,土壤剖面中CO2、N2O和CH4浓度分别介于530.2~31512.6、0.27~0.67和0.1~3.5μL.L-1.总体上,自地表向下,CO2和N2O浓度逐渐增大,CH4浓度则为逐渐减小,但在阴冷潮湿的10、11月和1月,15cm以下土层中CO2和N2O浓度随着深度的增加逐渐减小,CH4浓度则明显增加.土壤温度、水分同时影响剖面中CO2、N2O和CH4的时空分布,但影响效应以及作用的土层深度有所不同.相关分析结果表明,土壤中CO2和N2O浓度的时空分布显著正相关(r为0.780~0.894,p0.05~0.01),相关关系受环境因子的影响;CO2和CH4的时空分布则呈显著负相关关系(r=330,p0.01);N2O和CH4的空间分布为互逆关系,但只在土壤水分较大月份达到显著水平(r为-0.829~-0.956,p0.05~0.01).     

Flow characteristic and wastewater treatment performance of a pilot-scale airlift oxidation ditch

A pilot-scale airlift oxidation ditch using bubble diffuser and baffle as aerator was operated in a wastewater treatment plant (WWTP) to investigate its flow characteristic and wastewater treatment performance. Compared with the conventional oxidation ditch process, effective depth and oxygen utilization efficiency of this new process was improved by underwater aeration. Furthermore, it had a reversed velocity distribution, which decreased from the bottom to the top on vertical section. Velocity measurement showed that a velocity over 0.2 m/s at the bottom was sufficient to prevent sludge settlement during long term operation. Application of these concepts would save land area and energy consumption by about 25%–50% and 55%, respectively. In this new system, organic biodegradation and nitrification could be well achieved. Denitrification could occur steadily in the straight part by adjusting the airflow rate. An average TN removal rate of 63% was achieved with dissolved oxygen (DO) concentrations between 0.6 mg/L and 1.5 mg/L. The main pollutants in the effluent could meet the strictest discharge standard (COD<50 mg/L, NH₄ ⁺−N < 5 mg/L, and TN < 15 mg/L) in China now.     

沼泽湿地CO2、CH4、N2O排放对氮输入的响应

利用静态暗箱-气象色谱法，选取小叶章沼泽化草甸进行野外原位试验，研究氮输入对沼泽湿地CO2、CH4和N2O等3种温室气体排放的影响,结果表明：氮输入对沼泽湿地CO2和CH4排放有明显影响，其季节排放总量分别是对照处理的1.3和2.5倍，但对CO2和CH4的季节变化模式无明显影响；氮输入对N2O的排放强度和季节变化模式均有显著影响,CO2排放通量与5cm深土壤温度存在显著的正相关关系，与地表温度和1.5m气温存在指数关系，而CH4和N2O排放与温度之间没有显著的相关性．在20、100和500年时间尺度上氮输入处理的CH4和N2O全球增温潜势（GWP）分别比对照处理增加了150％、150％和80％，表明氮输入在长、短时间尺度上都是增强CH4和N2O的温室效应的。     

塑料玩具中邻苯二甲酸酯类环境激素检测方法研究

文章建立了一种对塑料玩具中5种邻苯二甲酸酯类物质同时分离和检测的高效液相色谱分析法。以shim-pack VP-ODS(4.6mm×150mm,5μm)为分离柱;以甲醇-水(体积比:90:10)为流动相,流速:1.0mL/min,检测波长:230nm。该方法所测得的5种邻苯二甲酸酯类物质在0.5～1000mg/L内具有良好的线性,相关系数r=0.9996,检出限达0.34～0.96μg/L,平均回收率在93.00%～105.23%。在对样品提取和纯化的基础上,对塑料玩具中邻苯二甲酸酯类物质进行了分析,结果令人满意。     

液相催化氧化法净化H2S实验研究

采用液相催化氧化法净化H2 S尾气。研究了铁离子浓度、氧含量和表面活性剂等因素在H2 S的净化中对吸收液净化效率和硫容量的影响。实验结果表明 ,用铁离子作催化剂 ,添加表面活性剂后 ,对低氧含量的尾气 ,吸收液具有较高的净化效率和较大的硫容量 ;当吸收液的硫容量达到饱和时 ,可通入空气进行再生循环使用。这一方法对H2 S尾气的污染治理及硫的回收利用具有重要的现实意义。