以甲醇为碳源生物反硝化过程释放一氧化二氮的试验研究

污水生物反硝化脱氮过程是一氧化二氮(N2O)的重要释放源之一.试验采用序批式反应器以甲醇为碳源(电子供体),硝酸盐(NO3--N)为电子受体驯化反硝化菌,并采用批处理试验研究不同电子受体、不同碳氮(C/N)比和不同初始亚硝酸盐(NO2--N)质量浓度条件下N2O释放情况.在典型周期试验和批处理试验中均能检测到N2O的释放.以NO2--N为电子受体时会释放较多的N2O,而以NO3--N为电子受体时释放的N2O相对较少.不同C/N比通过影响反硝化菌的活性进而影响N2O的释放,反硝化菌的活性和N2O的释放量均随着C/N比的降低而降低.N2O的释放量随着初始NO2--N质量浓度的增加而增加,一定浓度范围内的NO2--N会增强反硝化菌的活性.初始NO2--N质量浓度与N2O的释放量具有较好的指数相关性.     

Effects of temperature change and tree species composition on N2O and NO emissions in acidic forest soils of subtropical China

Tree species and temperature change arising from seasonal variation or global warming are two important factors influencing N2O and NO emissions from forest soils. However, few studies have examined the effects of temperatures(5–35℃) on the emissions of forest soil N2O and NO in typical subtropical region. A short-term laboratory experiment was carried out to investigate the influence of temperature changes(5–35℃) on soil N2O and NO emissions under aerobic conditions in two contrasting(broad-leaved and coniferous) subtropical acidic forest types in China. The results showed that the temporal pattern of N2O and NO emissions between the three lower temperatures(5℃, 15℃, and 25℃) and 35℃ was significantly different for both broad-leaved and coniferous forest soils. The effects of temperature on soil N2O and NO emission rates varied between broad-leaved and coniferous forest soils. Both N2O and NO emissions increased exponentially with an increase in temperature in the broad-leaved forest soil. However, N2O and NO emissions in the coniferous forest soil were not sensitive to temperature change between 5℃ and 25℃. N2O and NO emission rates were significantly higher in the broad-leaved forest soil as compared with the coniferous forest soil at all incubation temperatures except 5℃. These results suggest that the broad-leaved forest could contribute more N2O and NO emissions than the coniferous forest for most of the year in the subtropical region of China.     

Nitrous oxide reductase gene (nosZ) and N2O reduction along the littoral gradient of a eutrophic freshwater lake

Lake littoral zones are characterized by heterogeneity in the biogeochemistry of nutrient elements. This study aimed to explore the relationship between the nitrous oxide reductase gene (nosZ)-encoding denitrifier community composition/abundance and N2O reduction. Five samples (deep sediment, near-transition sediment, transition site, near-transition land and land soil) were collected along a littoral gradient of eutrophic Baiyangdian Lake, North China. To investigate the relationship between the nosZ-encoding denitrifier community structure and N2O reduction, the nosZ-encoding denitrifier community composition/abundance, potential denitrification rate (DNR) and potential N2O production rate (pN2O) were investigated using molecular biological technologies and laboratory incubation experiments. The results showed that the average DNR of sediments was about 25 times higher than that of land soils, reaching 282.5 nmol N/(g dry weight (dw)·hr) and that the average pN2O of sediments was about 3.5 times higher than that of land soils, reaching 15.7 nmol N/(g dw·hr). In the land area, the nosZ gene abundance showed a negative correlation with the N2O/(N2O+N2) ratio, indicating that nosZ gene abundance dominated N2O reduction both in the surface soils of the land area and in the soil core of the transition site.Phylogenetic analysis showed that all the nosZ sequences recovered from sediment clustered closely with the isolates Azospirillum largimobile and Azospirillum irakense affiliated to Rhodospirillaceae in alpha-Proteobacteria, while about 92.3% (12/13) of the nosZ sequences recovered from land soil affiliated to Rhizobiaceae and Bradyrhizobiaceae in α-Proteobacteria. The community composition of nosZ gene-encoding denitrifiers appeared to be coupled with N2O reduction along the littoral gradient.     

Preparation, characterization and application of CuCrO2/ZnO photocatalysts for the reduction of Cr(VI)

The delafossite CuCrO₂ elaborated by sol-gel from 40 nm diameter colloid is optically active in the visible region. It is characterized physically and photoelectrochemically. The microstructure is fairly homogenous with a mean crystallite size of ca. 2 μm. The optical gap (1.30 eV), determined from the diffuse reflectance, is well suited to the sunlight spectrum. The Mott Schottky plot is characteristic of P-type conductivity with a flat band potential of -0.26 V_SCE. As application, the photoreduction of chromate is successfully achieved in air-equilibrated suspension CuCrO₂/ZnO (1/1). CuCrO₂ is photoactivated by visible light and the electrons in the conduction band (-1.34 V_SCE) are injected to ZnO. In the presence of salicylic acid, a conversion of Cr(VI) to Cr(III) of 57% is obtained under optimal conditions (pH 3 at 25℃, 5×10^-4 mol/L) because of the HCrO₄^- dark adsorption onto ZnO (4HCrO₄^- + 3C₇H₆O₃ + 18O₂ + 16H⁺ → 4Cr³⁺ + 21CO₂ + 19H₂O, ΔG⁰ = -557 kcal/mol). Prolonged illumination is accompanied by a deceleration in the photoactivity owing to the competitive water reduction, an issue of energetic concern. The hetero-system exhibits self sensitization for hydrogen production with an evolution rate of 149 μmol/(hr·g).     

Nitrous oxide emissions from black soils with different pH

N₂O fluxes as a function of incubation time from soil with different available N contents and pH were determined. Cumulative carbon dioxide (CO₂) emissions were measured to indicate soil respiration. A 144-hr incubation experiment was conducted in a slightly acidic agricultural soil (pH_H2O 5.33) after the pH was adjusted to four different values (3.65, 5.00, 6.90 and 8.55). The experiments consisted of a control without added N, and with NH₄⁺-N and NO₃^--N fertilization. The results showed that soil pH contributed significantly to N₂O flux from the soils. There were higher N₂O emissions in the period 0-12 hr in the four pH treatments, especially those enhanced with N-fertilization. The cumulative N₂O-N emission reached a maximum at pH 8.55 and was stimulated by NO₃^--N fertilization (70.4 μg/kg). The minimum emissions appeared at pH 3.65 and were not stimulated by NO₃^--N or NH₄⁺-N fertilization. Soil respiration increased significantly due to N-fertilization. Soil respiration increased positively with soil pH (R² = 0.98, P < 0.01). The lowest CO₂-C emission (30.2 mg/kg) was presented in pH 3.65 soils without N-fertilization. The highest CO₂-C emissions appeared in the pH 8.55 soils for NH₄⁺-N fertilization (199 mg/kg). These findings suggested that N₂O emissions and soil respiration were significantly influenced by low pH, which strongly inhibits soil microbial nitrification and denitrification activities. The content of NO₃^--N in soil significantly and positively affected the N₂O emissions through denitrification.     

催化铁强化低碳废水生物反硝化过程的探讨

研究了低碳氮比条件下催化铁耦合生物反硝化的脱氮效率以及N2O产生.结果表明,相对常规低碳氮比反硝化,催化铁耦合组能大大提高硝酸根的转化率,但产生亚硝态氮积累,总氮去除率变化不大.耦合组N2O释放量高于常规生物对照组,源于亚铁氧化物与亚硝酸根的化学反应,但最高累积量小于8%,且可继续生物还原为N2.催化铁可以消除体系的溶解氧和降低氧化还原电位,对维持缺氧反硝化环境有利.     

昼夜增温对大豆田土壤N2O排放的影响

通过田间试验,用静态箱-气相色谱法测定N2O排放通量,研究昼夜增温对大豆田土壤N2O排放的影响.结果表明,增温没有改变大豆田土壤N2O排放通量的季节性变化规律.整个生长季,与对照相比,增温土壤N2O平均排放通量增加了17.31%(P=0.019),累积排放量显著增加了20.27%(P=0.005).对照与增温处理土壤N2O排放通量与土壤温湿度均呈显著性相关关系,对照与增温土壤的N2O排放温度敏感系数分别为3.75和4.10.整个生育期,增温显著增加了植株地上和总生物量、叶片硝酸还原酶活性和全氮含量,显著降低了叶片NO3--N含量;显著增加了土壤NO3--N含量,但对土壤有机碳及全氮含量没有显著影响.本研究表明,昼夜增温显著增加了大豆田土壤N2O的排放.     

优化施氮对河套灌区氧化亚氮排放和氨挥发的影响

以河套灌区盐化潮土为研究对象,采用静态暗箱-气相色谱法和通气法研究了4个施肥处理(不施肥(CK)、传统施肥(CON)、优化处理1(OPT1,减氮53.3%)、优化处理2(OPT2,减氮53.3%+硝化抑制剂))对河套灌区玉米农田氧化亚氮(N_2O-N)排放、氨挥发(NH_3-N)损失和玉米产量的影响.结果表明:氮肥减量显著降低了土壤N_2O-N排放和NH_3-N挥发;相比于CON处理,OPT1处理的N_2O-N排放量和NH_3-N挥发量分别降低了45.2%和68.8%(p0.05),但N_2O-N损失氮素比率增加了9.7%(p0.05).施用硝化抑制剂可显著降低土壤N_2O-N排放,与OPT1处理相比,OPT2处理可降低34.6%(p0.05)的N_2O-N排放和41.5%(p0.05)的N_2O-N损失氮素比率,但NH_3-N挥发增加了47.5%(p0.05).OPT1处理显著降低了玉米产量,降幅达22.1%(p0.05),而OPT2处理相对于OPT1处理增产32.9%(p0.05),与传统施肥处理无差异.因此,综合N_2O-N排放、NH_3-N挥发及玉米产量可知,OPT2是较为合理的施肥措施,值得在河套灌区推广.     

高盐高碱环境下硝化反硝化过程及N2O产生特征

采用稳定运行在高盐高碱环境厌氧/好氧/缺氧(A_n/O/A)模式下的序批式生物膜反应器(SBBR),考察在不同碳氮比(C/N)条件下,硝化反硝化过程及N_2O产生特征.结果表明,在C/N为5、2和对照组(C/N=0)时,总氮去除率分别为(98. 17±0. 42)%、(65. 78±2. 47)%和(44. 08±0. 27)%; N_2O的产生量分别为(32. 07±2. 03)、(21. 81±0. 85)和(17. 32±0. 95) mg·L~(-1); N_2O转化率(N_2O产生量在去除总氮中的比例)分别为(29. 75±0. 93)%、(30. 04±2. 17)%和(41. 69±0. 80)%.高盐高碱条件下,亚硝酸盐氧化菌(NOB)受到很强的抑制作用,硝化过程基本停留在亚硝酸盐阶段.由于高盐高碱环境对N_2O还原酶活性的抑制,使得异养反硝化过程产生了大量N_2O,随着碳氮比的增大,有更多的碳源用于反硝化过程,因而总氮去除率和N_2O产生量均随之增加.随着碳氮比的增大,N_2O转化率随之降低,这可能是由于异养反硝化过程氮素还原酶对电子的竞争所形成的,碳氮比越高,电子竞争越弱.高通量测序表明:在SBBR中,氨氧化细菌(AOB)被富集,而几乎不存在NOB;优势异养反硝化菌属主要是Thauera、Azoarcus和Gemmobacter.     

亚硝酸盐对聚磷菌吸磷效果的影响

以厌氧/好氧生化反应器中的聚磷菌为实验对象,探讨了亚硝酸盐对聚磷菌吸磷效果的影响.结果表明:低浓度NO₂^--N可以作为聚磷菌的电子受体,实现NO₂^--N型反硝化除磷,但吸磷总量和吸磷速率明显低于NO₃^--N型反硝化除磷的效果;当NO₂^--N和NO₃^--N共存于缺氧环境时,NO₂^--N对NO₃^--N型反硝化除磷的除磷总量和速率没有影响,但会降低NO₃^--N的消耗量;NO₂^--N型反硝化除磷污泥的好氧吸磷量和速率均低于传统A/O厌氧放磷污泥的效果,但由于它经历了缺氧吸磷和好氧吸磷2个阶段,因此,从吸磷总量或出水水质看,二者相差不大.     

凤眼莲对富营养化水体硝化、反硝化脱氮释放N2O的影响

以往有关大型水生漂浮植物消减富营养化水体氮(N)的研究主要侧重于植物对N的吸收效果,而忽略了硝化、反硝化反应途径对水体脱氮的贡献.基于此,本研究中借助具创新性的收集凤眼莲种植水体释放N₂O的装置和方法,通过模拟实验研究了凤眼莲对富营养化水体硝化、反硝化脱氮中间产物N₂O的影响.结果表明,凤眼莲可以促进富营养化水体的硝化、反硝化、成对硝化-反硝化反应过程,在本实验条件下凤眼莲种植水体在整个培养期内释放的N₂O气体浓度累积升高幅度较大,为453~4055 nL·L^-1(未加硝化抑制剂处理),通过释放N₂O而脱除氮素的量占整个水体N消减量的1.36%,为相应未种植凤眼莲水体的4.31倍.种植凤眼莲水体试验期间释放N₂O-N的量与水体氨态氮或硝态氮浓度的变化量均存在显著相关关系(p<0.05),说明N₂O释放量受到水体中NH₄⁺、NO₃^-浓度变化的影响.种植凤眼莲在实验中后期可以增加水体中硝化、反硝化细菌的数量,但其数量远低于凤眼莲根系附着的硝化反硝化细菌.水体中反硝化细菌数量与水体释放N₂O浓度之间并无显著相关性,说明种植凤眼莲水体反硝化脱氮释放N₂O过程可能主要是由根系共生微生物驱动的.     

Nitrous oxide emissions from a maize field during two consecutive growing seasons in the North China Plain

Nitrous oxide (N₂O) emissions from a maize field in the North China Plain (Wangdu County, Hebei Province, China) were investigated using static chambers during two consecutive maize growing seasons in the 2008 and 2009. The N₂O pulse emissions occurred with duration of about 10 days after basal and additional fertilizer applications in the both years. The average N₂O fluxes from the CK (control plot, without crop, fertilization and irrigation), NP (chemical N fertilizer), SN (wheat straw returning plus chemical N fertilizer), OM- 1/2N (chicken manure plus half chemical N fertilizer) and OMN (chicken manure plus chemical N fertilizer) plots in 2008 were 8.51, 72.1, 76.6, 101, 107 ng N/(m²·sec), respectively, and in 2009 were 33.7, 30.0 and 35.0 ng N/(m²·sec) from CK, NP and SN plots, respectively. The emission factors of the applied fertilizer as N₂O-N (EFs) were 3.8% (2008) and 1.1% (2009) for the NP plot, 3.2% (2008) and 1.2% (2009) for the SN plot, and 2.8% and 2.2% in 2008 for the OM-1/2N and OMN plots, respectively. Hydromorphic properties of the investigated soil (with gley) are in favor of denitrification. The large differences of the soil temperature and water-filled pore space (WFPS) between the two maize seasons were suspected to be responsible for the significant yearly variations. Compared with the treatments of NP and SN, chicken manure coupled with compound fertilizer application significantly reduced fertilizer loss rate as N₂O-N.     

Experimental study of NO2 reduction in N2/Ar and O2/Ar mixtures by pulsed corona discharge

Non-thermal plasma technology has been regarded as a promising alternative technology for NOx removal. The understanding of NO2 reduction characteristics is extremely important since NO2 reduction could lower the total NO oxidation rate in the plasma atmosphere. In this study, NO2 reduction was experimentally investigated using a non-thermal plasma reactor driven by a pulsed power supply for different simulated gas compositions and operating parameters. The NO2 reduction was promoted by increasing the specific energy density （SED）, and the highest conversion rates were 33.7%, 42.1% and 25.7% for Ar, N2/Ar and O2/Ar, respectively. For a given SED, the NO2 conversion rate had the order N2/Ar 〉 Ar 〉 02/Ar. The highest energy yield of 3.31 g/kWh was obtained in N2/Ar plasma and decreased with increasing SED; the same trends were also found in the other two gas compositions. The conversion rate decreased with increasing initial NO2 concentration. Furthermore, the presence of N2 or O2 led to different reaction pathways for NO2 conversion due to the formation of different dominating reactive radicals.     

N2O emission from nitrogen removal via nitrite in oxic-anoxic granular sludge sequencing batch reactor

Bionitrification is considered to be a potential source of nitrous oxide （N2O） emissions, which are produced as a by-product during the nitrogen removal process. To investigate the production of N2O during the process of nitrogen removal via nitrite, a granular sludge was studied using a labscale sequence batch reactor operated with real-time control. The total production of N2O generated during the nitrification and denitrification processes were 1.724 mg/L and 0.125 mg/L, respectively, demonstrating that N2O is produced during both processes, with the nitrification phase generating larger amount. In addition, due to the NEO-N mass/oxidized ammonia mass ratio, it can be concluded that nitrite accumulation has a positive influence on N2O emissions. Results obtained from PCRDGGE analysis demonstrate that a specific Nitrosomonas microorganism is related to N2O emission.     

SBR双颗粒污泥系统脱氮除磷性能研究

以模拟废水为研究对象,对SBR双颗粒污泥系统的脱氮除磷性能进行了考察.试验结果表明,A₂N双颗粒污泥系统能使硝化菌和聚磷菌分别在各自最佳的环境中生长,有利于系统脱氮除磷的稳定和高效运行,可控制性也得到了提高.在COD为300 mg·L^-1条件下,系统对COD的平均去除率达到78.8%,大部分COD被聚磷菌用来合成PHA;当溶解氧控制在3.55~4.90 mg·L^-1和5.60~6.60 mg·L^-1之间时,硝化SBR对氨氮的去除率分别为87.0%和94.5%.除磷SBR仅设置缺氧段时,磷去除率为72%;增设后曝气段后,磷去除率增至85%.NO_x^--N(NO₂^--N+ NO₃^--N)的去除主要发生在缺氧段,在反硝化除磷时作为电子受体被去除,平均去除率为90.6%.     

Nitrous oxide emission fromagricultural lands in Russia

Nitrous oxide (N₂O) atmospheric emission from differentagricultural soil types in Russia was evaluated based on published data onsingle input of nitrogen (N) fertilizers. For most of experiments the rates offertilization varied from 40 to 75 and from 160 to 264 kg/ha in activematter and they were considered separately. The higher rates ofsynthetic fertilizers (160 to 264 kg/ha) reduced relative gaseous loss ofN as N₂O (N₂O-N). Evidently, if nitrate (NO₃) concentrationswere high, the low content of organic carbon (C) and oxygen (O) restricted soilmicrobiological activity and consequently formation of N₂O. Themajority of gaseous loss of N₂O-N occurred within 140 days afterthe input of fertilizers. The N₂O emission factors derived forchernozem and soddy podzolic soil are 0.0126 and 0.0238 kgN₂O-N/kg N respectively. In 1990, the use of N fertilizers innational agriculture caused the release of 53 Gg N₂O-N thatconstituted 6% of global N₂O emission. Later on, the emissiondropped because of decreased use of N fertilizers, and in 1998 itwas almost 21% of the 1990 level.     

城市污水生物脱氮系统出水经氯胺消毒形成NDMA的影响因素研究

为了考察城市污水回用时氯消毒过程中NDMA的形成,以2套生物脱氮实验装置厌氧/缺氧/好氧(A/A/O)和缺氧/好氧(A/O)的二沉池出水为对象,研究了氯胺消毒过程中氯胺剂量、pH、NO2--N和NO3--N浓度对N-亚硝基二甲胺(NDMA)形成的影响.结果表明,二沉池出水中仍然含有微量的NDMA前体物,导致了氯胺消毒过程中NDMA的形成,而且NDMA的浓度会随氯胺浓度的增加呈线性增加;在中性或稍偏碱性(pH 7～8)的条件下,NDMA生成量最大;二沉池出水中NO2--N和NO3--N的浓度对NDMA的含量皆不会产生明显影响.     

Effect of pretreatment on Pd/Al2O3 catalyst for catalytic oxidation of o-xylene at low temperature

The effect of pretreatment on Pd/Al₂O₃ catalysts for the catalytic oxidation of o-xylene at low temperature was studied by changing the pretreatment and testing conditions. The fresh and pretreated Pd/Al₂O₃ catalysts were characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD). The results showed that the pretreatment dramatically changed the Pd/PdO ratio and then significantly affected the Pd/Al₂O₃ activity; while the pretreatment had not much influence on Pd particle size. The Pd/Al₂O₃ pre-reduced at 300℃/400℃, which has fully reduced Pd species, showed the highest activity; while the fresh Pd/Al₂O₃, which has fully oxidized Pd species, presented the worst performance, indicating the Pd chemical state plays an important role in the catalytic activity for the o-xylene oxidation. It is concluded that metallic Pd is the active species on the Pd/Al₂O₃ catalyst for the catalytic oxidation of o-xylene at low temperature.     

Cover crop effects on nitrous oxide emission from a manure-treated Mollisol

Agriculture contributes 40–60% of the total annual N₂O emissions to the atmosphere. Development of management practices to reduce these emissions would have a significant impact on greenhouse gas levels. Non-leguminous cover crops are efficient scavengers of residual soil NO₃, thereby reducing leaching losses. However, the effect of a grass cover crop on N₂O emissions from soil receiving liquid swine manure has not been evaluated. This study investigated: (i) the temporal patterns of N₂O emissions following addition of swine manure slurry in a laboratory setting under fluctuating soil moisture regimes; (ii) assessed the potential of a rye (Secale cereale L.) cover crop to decrease N₂O emissions under these conditions; and (iii) quantified field N₂O emissions in response to either spring applied urea ammonium nitrate (UAN) or different rates of fall-applied liquid swine manure, in the presence or absence of a rye/oat winter cover crop. Laboratory experiments investigating cover crop effects N₂O emissions were performed in a controlled environment chamber programmed for a 14 h light period, 18 °C day temperature, and 15 °C night temperature. Treatments with or without a living rye cover crop were treated with either: (i) no manure; (ii) a phosphorus-based manure application rate (low manure): or (iii) a nitrogen-based manure application rate (high manure). We observed a significant reduction in N₂O emissions in the presence of the rye cover crop. Field experiments were performed on a fine-loamy soil in Central Iowa from October 12, 2005 to October 2, 2006. We observed no significant effect of the cover crop on cumulative N₂O emissions in the field. The primary factor influencing N₂O emission was N application rate, regardless of form or timing. The response of N₂O emission to N additions was non-linear, with progressively more N₂O emitted with increasing N application. These results indicate that while cover crops have the potential to reduce N₂O emissions, N application rate may be the overriding factor.     

城市污水处理厂缺氧池短程反硝化现象及影响因素研究

调研了北方某城市污水处理厂缺氧池亚硝态氮积累的现象.该污水处理厂采用传统厌氧/缺氧/好氧（A/A/O）工艺,在缺氧池中存在稳定的短程反硝化过程,且缺氧池中亚硝态氮积累率最高可达88.4%.16S rRNA高通量测序分析表明Saccharibacteria_genera_incertae_sedis和Thauera可能是导致该厂缺氧池亚硝态氮积累的主要菌种,而短程反硝化现象出现的主要原因可能为外加碳源乙酸钠和系统较高的pH值.取活性污泥在COD/NO₃^--N为2~5条件下进行反硝化批次试验,结果表明硝态氮的还原速率均高于亚硝态氮的还原速率,且最大硝态氮到亚硝态氮的转换率均在50%左右.但碳源充足时,积累的NO₂^-会在NO₃^-被还原完后继续发生还原反应,从而导致最终亚硝态氮积累效果变差.本研究,以乙酸钠为碳源,COD/NO₃^--N为3可使反硝化过程获得最高亚硝态氮积累.因此,控制合适COD/NO₃^--N或缺氧反应时间是短程反硝化工艺运行的关键控制参数.本研究可为实际污水处理厂构建短程反硝化并进一步耦合厌氧氨氧化技术提供参考.