~(15)N示踪法测定海洋反硝化速率中~(29)N_2浓度的准确定量

利用15 N示踪法实测南海水体反硝化速率的研究发现,培养水样在长时间密闭放置过程中也会受到外界空气的污染,且其29N2/28N2比值恒定为0.007 35。根据空气背景中29N2/28N2比值恒定的特征,提出基于质量平衡关系校正空气N2污染的方法,通过将样品实测29N2浓度扣除由外界空气贡献的29N2浓度,可获得由生物反硝化作用所产生的29N2准确浓度,进而可计算出准确的反硝化速率。经空气29N2背景校正后,29N2浓度的偏差明显小于未经校正的结果,且29N2浓度与培养时间之间的线性相关性显著加强,凸显出空气29N2背景校正是获取准确反硝化速率的关键。鉴于15 N示踪法已被广泛应用于海洋水体与沉积物反硝化速率的测定中,所提出的空气29N2背景校正方法具有重要的意义。     

海水反硝化和厌氧氨氧化速率同步测定的15N示踪法及其应用

反硝化与厌氧氨氧化作用是海洋结合态氮迁出的主要途径,15N示踪法是定量反硝化和厌氧氨氧化作用的新方法,它具有灵敏度高、可同步测量反硝化与厌氧氨氧化速率的优点.本研究开展了一系列方法学实验,以确定高纯氦气驱赶水样所含气体的时间、超声赶气时间、同位素比值质谱仪测量N2含量的精度、N2含量及其同位素组成测定的工作曲线以及示踪剂的最佳添加量等,从而确立起15N示踪同步测定海水反硝化和厌氧氨氧化速率的方法.所建立方法测量N2含量的相对标准偏差小于8%,可满足海洋反硝化与厌氧氨氧化速率测定的需要.应用该方法实测了厦门筼筜湖富氧与缺氧水体的反硝化与厌氧氨氧化速率,结果表明,缺氧底层水的反硝化速率[4.10～5.47μmol/（dm3·d）]比富氧表层水[0.43～0.46μmol/（dm3·d）]明显来得高,但缺氧底层水的厌氧氨氧化速率[0.00～0.12μmol/（dm3·d）]则比富氧表层水的速率[0.52～0.67μmol/（dm3·d）]低得多.     

利用稳定同位素(15N)示踪技术研究浮游藻类氮素吸收速率特征

浮游藻类对溶解态氮的吸收同化是湖泊氮生物循环和水体富营养化发生机制探讨的关键环节。本文通过~(15)N稳定同位素添加实验以铜绿微囊藻(Microcystis aeruginosa)、海链藻(Thalassiosira sp.)、卡德藻(Tetraselmis sp.)、剧毒卡尔藻(Karlodinium veneficum)以及盐水隐藻(Rhodomonas salina)为研究对象,从浮游藻类氮素吸收时间、营养盐基质以及藻种差异三个方面研究五种藻类对铵氮(NH_4~+-N)、硝氮(NO_3~--N)、尿素氮(Urea-N)三种形态氮的吸收特征。研究发现:(1)浮游藻类对三种形态氮的吸收均在1h时吸收速率最高,其氮素吸收过程为快速吸收。(2)浮游藻类优先吸收还原态氮,其中NH_4~+-N吸收速率最高,当培养周期为1d和4d时浮游藻类对NH_4~+-N吸收速率的均值分别为4.05和4.15μmol/(L·h);浮游藻类对Urea-N吸收相对偏好系数为25.18—713.42,表现出对小分子溶解态有机氮的特定偏好性。(3)不同藻种对氮素吸收具有不同特征,其中,剧毒卡尔藻对三种形态氮的吸收速率均为最高,而铜绿微囊藻的吸收速率均为最低;不同藻种不同培养时间氮素吸收速率差异与浮游藻类生长周期等特性有关。不同浮游藻类对不同形态氮素表现出吸收特异性,对水体氮负荷和浮游藻类水华优势种形成将产生重要影响。     

基于双还原体系与膜进样质谱快速测定15N加富水样中15NO3-的方法

海洋中的氮循环是海洋生物地球化学研究的热点领域之一,而硝化过程是氮循环的关键一环,准确获取硝化速率对于丰富海洋氮循环的认识至关重要。¹⁵N标记同位素技术是目前国际上最为广泛使用的硝化速率测定方法,该方法的核心在于准确测定¹⁵N加富样品产生的¹⁵NO₂^-和¹⁵NO₃^-的含量,但目前的方法普遍存在测试时间较长、测试成本较高、所需样品体积较大或者检测限较高等问题。研究以低成本的膜进样质谱作为¹⁵N加富样品测试设备,建立了基于镉柱与氨基磺酸双还原体系测定¹⁵N加富样品中¹⁵NO₃^-含量的方法。经条件优化实验确定的具体方法:采用1 mol/L HCl配制15 mmol/L的氨基磺酸（SA）作为反应试剂除去样品原有的NO₂^-,然后利用镉柱将¹⁵NO     

辽河口海域N2O分布特征和海气通量研究

于2007年5月份(枯水期)和8月份(丰水期)采集辽河口区域大气样品及水样,应用气相色谱及静态顶空法测定大气及海水中溶解N₂O的浓度,并计算不同站位的N₂O通量。结果表明:辽河口区域水体中溶解N₂O浓度存在着明显的时空变化,5月份河口区域水体中N₂O浓度高于8月份,且河流段溶解N₂O浓度大于近海岸海域。水中溶解N₂O浓度及溶解氧浓度呈显著的负相关关系。在枯水期和丰水期,所有站位的N₂O均处于过饱和状态,N₂O气体从水体向大气排出,辽河口区域是大气中N₂O的一个排放源。     

苏北滨海湿地互花米草潮滩CO2,CH4和N2O通量的日变化规律

The invasions of the alien species such as Spartina alterniflora along the northern Jiangsu coastlines have posed a threat to biodiversity and the ecosystem function.Yet,limited attention has been given to their potential influence on greenhouse gas(GHG) emissions,including the diurnal variations of GHG fluxes that are fundamental in estimating the carbon and nitrogen budget.In this study,we examined the diurnal variation in fluxes of carbon dioxide(CO_2),methane(CH_4),and nitrous oxide(N2O) from a S.alterniflora intertidal flat in June,October,and December of 2013 and April of 2014 representing the summer,autumn,winter,and spring seasons,respectively.We found that the average CH_4 fluxes on the diurnal scale were positive during the growing season while negative otherwise.The tidal flat of S.alterniflora acted as a source of CH_4 in summer(June) and a combination of source and sink in other seasons.We observed higher diurnal variations in the CO_2 and N_2O fluxes during the growing season(1 536.5 mg CO_2 m~(–2) h~(–1) and 25.6 μg N_2O m~(–2) h~(–1)) compared with those measured in the non-growing season(379.1 mg CO_2 m~(–2) h~(–1) and 16.5 μg N_2O m~(–2) h~(–1)).The mean fluxes of CH_4 were higher at night than that in the daytime during all the seasons but October.The diurnal variation in the fluxes of CO_2 in June and N_2O in December fluctuated more than that in October and April.However,two peak curves in October and April were observed for the diurnal changes in CO_2 and N_2O fluxes(prominent peaks were found in the morning of October and in the afternoon of April,respectively).The highest diurnal variation in the N_2O fluxes took place at 15:00(86.4 μg N_2O m~(–2) h~(–1)) in June with an unimodal distribution.Water logging in October increased the emission of CO_2(especially at nighttime),yet decreased N_2O and CH_4 emissions to a different degree on the daily scale because of the restrained diffusion rates of the gases.The seasonal and diurnal variations of CH_4 and CO_2 fluxes did not correlate to the air and soil temperatures,whereas the seasonal and diurnal variation of the fluxes of N_2O in June exhibited a significant correlation with air temperature.When N_2O and CH_4 fluxes were converted to CO_2-e equivalents,the emissions of N_2O had a remarkable potential to impact the global warming.The mean daily flux(MF) and total daily flux(TDF) were higher in the growing season,nevertheless,the MF and TDF of CO_2 were higher in October and those of CH_4 and N_2O were higher in June.In spite of the difference in the optimal sampling times throughout the observation period,our results obtained have implications for sampling and scaling strategies in estimating the GHG fluxes in coastal saline wetlands.     

黑石礁海域生物碳、氮稳定同位素组成的研究

稳定同位素技术是研究生态系统中物质循环与能量流动的有效技术。利用稳定同位素技术研究了黑石礁海域浮游植物和6种海洋生物的δ13 C和δ15组成、营养位置、空间分布和月份变化。结果显示:浮游植物的δ15 C远低于其他物种,不同物种的δ13 C和δ15 N存在明显的差异,且有交叉现象,表明他们同化了不同的碳源;物种的δ15 N值空间差异较大而δ13 C值空间差异不明显,且δ15 N值与距离排污口的远近有关系,越靠近排污口δ15 N越大,与人类活动营养物质的输入有关系,可以用δ15 N监测人类活动对海洋生物的影响;孔石莼的δ15 N月平均变化很大,浮游植物δ15 N值基本没有变化,其他物种没有发生很大的变化;孔石莼是适合短期监测人类活动对海洋影响的物种。     

热带北太平洋西部固氮速率及固氮微生物组成

In the present study, we report N_2 fixation rate(~(15)N isotope tracer assay) and the diazotroph community structure(using the molecular method) in the western tropical North Pacific Ocean(WTNP)(13°–20°N, 120°–160°E). Our independent evidence on the basis of both in situ N_2 fixation activity and diazotroph community structure showed the dominance of unicellular N_2 fixation over majority of the WTNP surface waters during the sampling periods.Moreover, a shift in the diazotrophic composition from unicellular cyanobacteria group B-dominated to Trichodesmium spp.-dominated toward the western boundary current(Kuroshio) was also observed in 2013. We hypothesize that nutrient availability may have played a major role in regulating the biogeography of N_2 fixation.In surface waters, volumetric N_2 fixation rate(calculated by nitrogen) ranged between 0.6 and 2.6 nmol/(L·d) and averaged(1.2±0.5) nmol/(L·d), with 10 μm size fraction contributed predominantly(88%±6%) to the total rate between 135°E and 160°E. Depth-integrated N_2 fixation rate over the upper 200 m ranged between 150 μmol/(m~2·d)and 480 μmol/(m~2·d)(average(225±105) μmol/(m~2·d). N_2 fixation can account for 6.2%±3.7% of the depthintegrated primary production, suggesting that N_2 fixation is a significant N source sustaining new and export production in the WTNP. The role of N_2 fixation in biogeochemical cycling in this climate change-vulnerable region calls for further investigations.     

基于反转法的O2 -CO2 输运性质预测

采用反转法计算得到了O₂-CO₂混合气体新的势能参数.在此基础上,根据分子动力学理论,计算了混合气体在零密度下的输运性质,包括黏度系数、热扩散系数和热扩散因子,计算的温度范围为273.15—3273.15 K.与实验值比较表明,计算结果可以满足实际工程应用.     

南海NO2-N薄层的研究

1982年6月和1985年6月调查表明,在南海东部和南部海区次表层存在NO₂-N薄层,分别约占总测站84%和71%,薄层平均厚度分别为20.5m和34.5m,NO₂-N平均含量为0.23μmol/dm³和0.19μmol/dm³,NO₂-N薄层中心位置分别是69m和71m。本文对NO₂-N薄层的成因、分布及亚硝酸氮的来源和影响其含量的主要因素等进行了研究。     

Comparative assessment of nitrogen fixation rate by 15N2 tracer assays in the South China Sea

Nitrogen fixation is one of the most important sources of new nitrogen in the ocean and thus profoundly affects the nitrogen and carbon biogeochemical processes. The distribution, controlling factors, and flux of N₂ fixation in the global ocean remain uncertain, partly because of the lack of methodological uniformity. The 15N₂ tracer assay (the original bubble method → the 15N₂-enriched seawater method → the modified bubble method) is the mainstream method for field measurements of N₂ fixation rates (NFRs), among which the original bubble method is the most frequently used. However, accumulating evidence has suggested an underestimation of NFRs when using this method. To improve the availability of previous data, we compared NFRs measured by three 15N₂ tracer assays in the South China Sea. Our results indicate that the relationship between NFRs measured by the original bubble method and the 15N₂-enriched seawater method varies obviously with area and season, which may be influenced by incubation time, diazotrophic composition, and environmental factors. In comparison, the relationship between NFRs measured by the original bubble method and the modified bubble method is more stable, indicating that the N₂ fixation rates based on the original bubble methods may be underestimated by approximately 50%. Based on this result, we revised the flux of N₂ fixation in the South China Sea to 40 mmol/(m2·a). Our results improve the availability and comparability of literature NFR data in the South China Sea. The comparison of the 15N₂ tracer assay for NFRs measurements on a larger scale is urgently necessary over the global ocean for a more robust understanding of the role of N₂ fixation in the marine nitrogen cycle.     

N2O Production, Nitrification and Denitrification in an Estuarine Sediment

The mechanisms regulating N₂O production in an estuarine sediment (Tama Estuary, Japan) were studied by comparing the change in N₂O production with those in nitrification and denitrification using an experimental continuous-flow sediment–water system with¹⁵N tracer (¹⁵N-NO−3 addition). From Feburary to May, both nitrification and denitrification in the sediment increased (246 to 716 μmol N m⁻² h⁻¹and 214 to 1260 μmol N m⁻² h⁻¹, respectively), while benthic N₂O evolution decreased slightly (1560 to 1250 nmol N m⁻² h⁻¹). Apparent diffusion coefficients of inorganic nitrogen compounds and O₂at the sediment–water interface, calculated from the respective concentration gradients and benthic fluxes, were close to the molecular diffusion coefficients (0·68–2·0 times) in February. However, they increased to 8·8–52 times in May except for that of NO−2, suggesting that the enhanced NO−3 and O₂supply from the overlying water by benthic irrigation likely stimulated nitrification and denitrification. Since the progress of anoxic condition by the rise of temperature from February to May (9 to 16 °C) presumably accelerated N₂O production through nitrification, the observed decrease in sedimentary N₂O production seems to be attributed to the decrease in N₂O production/occurrence of its consumption by denitrification. In addition to the activities of both nitrification and denitrification, the change in N₂O metabolism during denitrification by the balance between total demand of the electron acceptor and supply of NO−3+NO−2 can be an important factor regulating N₂O production in nearshore sediments.     

The density functional calculations on the structural and electronic properties of the endohedral fullerene dimer (N2@C60)2

The generalised gradient approximation based on density functional theory is used to study the structural and electronic properties of the endohedral fullerene dimer (N₂@C₆₀)₂. Four N atoms sit at the cage centres in the form of two N_2 molecules. The density of states and Mulliken charge analysis explore that the energy levels from -6 to -10 eV are mainly influenced by the N₂ molecules.     

Cu2+/SnO2复合纳米光催化剂的制备及其对海洋柴油污染物的降解

采用化学沉淀法成功制备了Cu2+/SnO2复合纳米光催化剂,采用XRD、SEM等测试手段对复合纳米光催化剂的粒径、形态等进行表征。在紫外光条件下,分别改变催化剂掺杂比、催化剂煅烧温度、催化剂投加量、柴油初始含量和光照时间等单因素,探究不同条件对Cu2+/SnO2复合纳米光催化剂降解海洋柴油污染物的影响。结果表明,自制复合纳米光催化剂可以有效降解海水中的柴油污染物,在紫外光作用下,于400℃下煅烧Cu/Sn掺杂比为0. 03的Cu2+/SnO2复合纳米光催化剂、投加量为0. 2 g/dm3、柴油初始含量为0. 15 g/dm3、H2O2溶液含量为0. 2 g/dm3、溶液的p H为7、光照时间3 h时效果最好,海水中柴油的去除率最高,达到86. 98%。Cu2+/SnO2复合纳米光催化剂用聚丙烯纳米球负载后可以实际应用于海洋中,便于回收。     

相变存储材料Ge1Sb2Te4和Ge2Sb2Te5薄膜的结构和电学特性研究

采用射频磁控溅射方法制备了两种用于相变存储器的Ge₁Sb₂Te₄和Ge₂Sb₂Te₅相变薄膜材料,对其结构、电学输运性质和恒温下电阻随时间的变化关系进行了比较和分析.X射线衍射(XRD)和原子力显微镜(AFM)的结果表明:随着退火温度的升高,Ge₁Sb₂Te₄薄膜逐步晶化,由非晶态转变为多晶态,表面出现均匀的、     

镉和汞两种重金属离子对四角蛤蜊血细胞DNA损伤的初步研究

利用彗星电泳技术,研究了不同胁迫浓度和胁迫时间下,Cd2+和Hg2+对四角蛤蜊(Mactra veneriformis)血细胞DNA损伤的情况.研究结果显示,50、100和200μg/L Cd2+胁迫14天不能造成四角蛤蜊血细胞DNA损伤.10、20和40μg/L Hg2+胁迫均能明显损伤血细胞DNA,并且DNA损伤程...