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1.
长期以来,研究者在探讨土壤中多环芳烃(PAHs)的降解及修复过程中,缺乏简便有效的手段对化合物的降解动态进行定量研究。前人尝试用投加实验、对比采用降解措施前后污染物的浓度变化、模型计算等方法研究PAHs的降解过程,其结果常互相矛盾,或不能真实反映复杂的实际环境。本文应用单体碳同位素技术对农田土壤中多环芳烃的植物降解过程进行定量表征,采集了某地农田表土作为供试土壤,选择玉米作为供试作物,开展了作物对土壤中PAHs降解及消除过程的研究。气相色谱-质谱分析结果表明,培养所用的玉米原始土及分4批收集的空白土、根际土、非根际土样品中16种PAHs的浓度总和(∑PAHs)平均分别为380.8 ng/g、(281.5±34.7) ng/g、(272.2±11.6) ng/g和(299.8±37.9) ng/g;玉米生长期间,各土壤样品 的∑PAHs均比原始土壤有所下降,但除3环化合物(苊烯、苊、芴、菲、蒽)外,其他化合物并未随玉米的生长表现出显著趋势。与玉米根、叶倾向于富集低环PAHs化合物相对应,可以判断植物对土壤中的低环化合物去除作用最为显著。各采样时期玉米根际土、非根际土和空白土壤样品中多环芳烃单体化合物的碳同位素分馏值(δ13C)在-34.31‰~-23.95‰之间,且除芘外的其他化合物的δ13C值随时间呈现逐步变轻的趋势,波动值位于-0.6‰~-9.0‰之间;本文对于PAHs单体化合物,尤其是4、5环化合物,在玉米降解过程中的碳同位素分馏与浓度变化之间未发现明显关系。考虑3环以下的PAHs化合物更倾向于被降解和清除,且其碳、氢同位素分馏情况更容易被观察到,因此稳定同位素分析更有助于探明该类单体多环芳烃污染物在环境中的迁移、转化规律。  相似文献   

2.
应用单体碳同位素组成追溯多环芳烃（PAHs）类污染物的来源越来越受关注。单体同位素分析中,利用样品预处理减少共流出和未分峰（UCM）,是实现同位素比值准确分析的重要前提。已有分离净化研究较少关注环数小于3的PAHs;或需联合使用高效液相色谱（HPLC）技术,但对实验室条件要求较高。本文期望避免使用HPLC技术,仅通过简单的固相萃取法,实现16种PAHs的分离净化,满足包括低环数在内的PAHs单体碳同位素分析的要求。实验对比了氨基和硅胶两种填料的固相萃取（SPE）小柱,以及正戊烷等10种淋洗溶剂对PAHs的分离净化富集效果。结果表明：氨基小柱中有20%以上的萘和苊不能与烷烃和未分峰完全分离,硅胶SPE小柱除杂效果和分离效果优于氨基小柱。选择1000mg/6mL硅胶SPE小柱,利用6mL正戊烷淋洗UCM和烷烃,5mL正戊烷-二氯甲烷（70：30,V/V）洗脱PAHs。利用气相色谱（GC）对分离净化效果进行初步检验,气体同位素质谱（GC-IRMS）进行单体碳同位素分析。16种PAHs的回收率为79%~128%,相对标准偏差为2%~13%（1σ,n=6）,单体碳同位素比值（δ13C）分析精度为0.1‰~0.75‰,大幅降低了其中UCM和共流出对PAH单体碳同位素分析的干扰,尤其减少了对低环数PAHs单体碳同位素分析的影响,而且净化过程没有造成PAHs单体碳同位素分馏,满足PAHs单体碳同位素分析的要求。  相似文献   

3.
应用气相色谱-气体同位素质谱(GC-C-IRMS)分析正构烷烃单体碳同位素之前,需要对饱和烃样品中正构烷烃和异构烷烃进行预分离、富集,在预分离和富集过程中正构烷烃单体碳同位素是否发生分馏是高精度分析正构烷烃单体碳同位素比值(δ~(13)C)的关键。本文以正构烷烃混合溶液为对象,利用柱色谱、5■分子筛络合、环己烷-正戊烷混合溶剂两次洗脱,GC-C-IRMS分析正构烷烃单体碳同位素,研究前处理过程中正构烷烃单体碳同位素是否发生分馏。结果表明:使用柱色谱分离前后,多数正构烷烃单体碳同位素比值相差-0.2‰～0.2‰;当5■分子筛不完全络合时,未络合的正构烷烃单体碳同位素比值偏重约0.7‰,可能发生了微弱的碳同位素分馏,但并未影响洗脱后的正构烷烃单体碳同位素比值;使用环己烷-正戊烷混合溶剂洗脱前后,碳同位素比值相差-0.2‰～0.5‰,以同样方式洗脱第二次,获得的正构烷烃单体碳同位素比值与模拟样品相差-0.3‰～0.2‰。分析不同回收率(20%)正构烷烃的单体碳同位素比值,处理前后的差值基本在0.3‰以内,可见当正构烷烃回收率低至20%左右时,其单体碳同位素仍未发生明显分馏。柱色谱分离-5■分子筛络合-混合溶剂洗脱方法适用于回收率大于20%的正构烷烃单体碳同位素分析。  相似文献   

4.
海洋沉积物有机碳和稳定氮同位素分析的前处理影响   总被引：2，自引：0，他引：2  
海洋沉积物中的有机碳和稳定氮同位素为海洋古环境和碳氮循环提供了大量信息,然而不同的前处理方法对有机碳和稳定氮同位素测定结果的准确性产生不同程度的影响.笔者通过大量条件实验,分析了前处理过程中影响结果准确性的可能因素.①器皿材质:使用聚丙烯和玻璃离心管进行酸处理所得样品的δ13C和δ15N基本无差别.②干燥方式:样品经热烘干燥会导致样品中轻碳组分和易挥发组分的逸散,引起样品中δ13C的分馏.鲜样和酸处理后样均采用热烘干燥会引起样品中δ15N发生明显分馏.③驱酸方式和洗酸程度:水洗造成溶解性有机碳和氮的损失,致使δ13C和δ15N值较真实值偏正,但酸蒸法不能保证氯离子的有效驱除.洗至中性后的洗酸次数对δ13C影响甚小,但会导致δ15N继续偏正.全程采用冷冻干燥,选用PP离心管作为主要酸处理水洗和干燥的器皿,具有很好的重复性,可获得较理想、准确的δ13C和δ15N测试数值.  相似文献   

5.
为了揭示塔里木盆地海相烃源岩中芳烃分子同位素的地质-地球化学信息,利用逐步增加试剂极性的方法对芳烃馏分进行了进一步的分离,并利用气相色谱同位素质谱(GC-IR-MS)分析技术测定了萘系列和菲系列的单体碳同位素.分析结果显示,芳烃分子碳同位素分布为-47.5‰ ～-17.4‰,其中寒武系-下奥陶统烃源岩的碳同位素为-38.2‰ ～-17.4‰,平均为-26.8‰;其中ML1-1、ML1-2两个样品的碳同位素为-36.8‰ ～-17.4‰,平均为-25.7‰;中-上奥陶统烃源岩为-47.5‰ ～-20.3‰,平均-30.6‰.结果表明,萘系列和菲系列化合物整体上表现为寒武系-下奥陶统烃源岩富集13C,而中-上奥陶统烃源岩更富集12C;在受到异常高温作用或过成熟度阶段,成熟度可能对芳烃的分子碳同位素产生较大影响,使其更富集13C.不同样品的二甲基萘系列化合物的碳同位素分布特征相似,暗示其可能具有相似的碳同位素分馏机制.而三甲基萘、二甲基菲系列化合物的碳同位素分布杂乱,暗示其成因来源可能较为复杂.塔里木盆地两套海相烃源岩中1,6-DMN、1,2,5-TMN、1-MP和1,9-DMP的碳同位素存在明显差异,可以对两套烃源岩进行有效的区分.  相似文献   

6.
对南羌塘侏罗系布曲组和夏里组烃源岩氯仿沥青"A"组分碳同位素分析表明,碳同位素主要受有机母质及沉积环境影响,夏里组烃源岩氯仿沥青"A"组分的碳同位素较重,而布曲组烃源岩氯仿沥青"A"中族组分的碳同位素组成相对较轻。并且它们普遍存在碳同位素逆转现象,夏里组烃源岩氯仿沥青"A"组分的碳同位素逆转表现为:δ13C饱和烃δ13C非烃δ13C芳烃δ13C沥青质,主要受有机质母源控制;布曲组烃源岩氯仿沥青"A"组分的碳同位素逆转表现为:δ13C非烃δ13C沥青质δ13C饱和烃δ13C芳烃,主要与生物降解作用有关。  相似文献   

7.
碳同位素在天然气运移路径示踪中的应用十分广泛,以游离相运移的天然气,运移过程中碳同位素的分馏主要受"质量分馏效应"控制;以水溶相运移的天然气,运移过程中碳同位素的分馏主要受"溶解分馏效应"控制。天然气运移中碳同位素的分馏程度不仅与气体分子质量、气体分子水溶解度等物理化学性质有关,同时也受天然气运移距离、输导层物性等外部环境条件的影响。常用的天然气运移路径示踪参数有δ~(13)C_1、δ~(13)C_2-δ~(13)C_1、δ~(13)CO_2及储集层中自生方解石的碳同位素。对研究现状分析后提出运移相态识别、碳同位素失真分析是应用碳同位素示踪天然气运移路径的基础,非烃碳同位素、多参数对比是碳同位素示踪天然气运移路径研究的未来趋势。  相似文献   

8.
天然气水合物是一种新型的洁净能源。甲烷天然气水合物是储量最丰富的一种类型,常出现在深海中或极地大陆上,其生成的过程中会发生同位素的分馏效应。通过实验室模拟水合物生成的过程,利用天然海水与甲烷或二氧化碳气体反应,以及更接近实际生成环境的甲烷-海水-沉积物动态聚散实验,对甲烷水合物和二氧化碳水合物生成前后δ13C值进行测定,研究水合物生成过程中δ13C的变化情况。实验证明,水合物反应中碳同位素分馏是存在的,其变化程度明显小于氧同位素和氢同位素。甲烷水合物碳同位素的分馏系数αC的值为1000 3~1000 9。二氧化碳水合物生成反应后气相的碳、氧同位素变轻,重同位素趋向于进入水合物中,二氧化碳水合物碳同位素的分馏系数αC的值为1000 7~1001 2。海水中溶解的CO2气体在甲烷水合物形成过程中会被水合物捕获,从而使得δ13CDIC值变小,重的碳同位素趋于进入水合物中,而较轻的碳同位素留在海水中。但由于海水中含有的溶解CO2气体有限,经过多轮水合物动态聚散后δ13CDIC值的变化幅度会越来越小。  相似文献   

9.
为探讨塔里木盆地原油类型和油源问题,运用色谱-同位素质谱分析技术,分析了该盆地塔中、塔北、塔东与库车地区的典型原油轻烃单体烃碳同位素组成。结果表明,不同结构轻烃化合物中,支链烷烃与环己烷系列比环戊烷系列更具明显的成因判识意义。2-甲基环戊烷2 mC_5、3-甲基环戊烷3 mC_5、3-甲基环己烷3 mC_6、环己烷CYC6与甲基环己烷mCYC_6等化合物的δ~(13)C在煤成油最高,δ~(13)C大于-21‰;湖相油次之,δ~(13)C位于-25‰~-22‰之间;再次之为寒武系-下奥陶统海相原油,δ~(13)C位于-27‰~-21‰之间,最轻的为上奥陶统海相原油,δ~(13)C小于-28‰。其碳同位素值可以较好的判别该盆地寒武系-下奥陶统海相油、上奥陶统海相油、湖相油与煤成油。优选的8个特征化合物碳同位素可以作为原油成因类型的划分标志,尤其是2-甲基环戊烷2 mC_5、3-甲基环戊烷3 mC_5、3-甲基环己烷3 mC_6、环己烷CYC6与甲基环己烷mCYC_6等化合物。特征轻烃化合物的碳同位素组成可成为不同成因原油的划分标志。  相似文献   

10.
煤成甲烷碳同位素分馏的动力学模拟   总被引：10，自引：6，他引：4  
主要目的是通过动力学模拟实验与GC-IRMS技术建立煤成甲烷碳同位素分馏的动力学模拟.热解产物中甲烷碳同位素的测定结果表明,同时假定生气过程中同位素分馏系数(α)固定不变和所有产甲烷母质具有相同的初始碳同位素组成(δ13Co)对于解释煤化过程中的碳同位素分馏是不可行的.在本研究中,为了解决陆源有机质的非均质性,应用了两个方法:一是假定对于煤中所有产甲烷前身物具有一个相同的初始碳同位素组成(δ13Co),通过调整各个平行反应的△Ea,i(Ea,i13C-Ea,i12C)来拟合实测甲烷同位素组成的变化;另一个是假定在整个生气过程中同位素分馏系数(α)不变,即△Ea,i为常数,通过改变fi13C来实现与实测甲烷同位素的拟合.动力学计算结果表明,在2℃/Ma的地质升温速率下两种方法具有相似的结果.  相似文献   

11.
多环芳烃单体同位素分析进展   总被引：5，自引：0，他引：5  
多环芳烃(PAHs)单体同位素组成是辨识这类污染物来源,评价其在环境中生物可降解性的重要手段。准确高精度的PAHs单体同位素比值测定有赖于样品预处理方法的改进和相应仪器分析技术的提高。文章综合评述了近年来PAHs单体同位素分析中的预处理方法研究进展,主要包括索氏提取、加速溶剂萃取等提取方法和硅胶、氧化铝柱色谱、固相萃取、凝胶渗透色谱、高效液相色谱、薄层色谱等净化方法;介绍了PAHs单体同位素组成的气相色谱-同位素比值质谱分析方面的研究进展,包括色谱柱头压、进样时间、PTV大体积进样技术等仪器参数的选择和校准同位素内标的选择等数据处理方式。  相似文献   

12.
羊卓雍湖流域湖水稳定同位素循环过程研究   总被引：9，自引：0，他引：9  
基于卓雍错流域2004年降水、河水、湖水中δ18O的监测结果,结合内陆湖水循环稳定同位素蒸发分馏模型,探讨了青藏高原南部羊卓雍湖水中稳定同位素的变化过程.研究表明:羊卓雍现代湖水中-5.9‰的δ18O平均值,相对应于当地相对湿度介于54%~58%的气候条件下,这是湖水蒸发分馏作用的最后结果.此外,入湖河水中δ18O变化也对湖水中平衡δ18O有一定的影响,而湖水温度的直接影响可以乎略.湖水中δ18O对入湖水δ18O的波动的调节能力很强,对于入湖水中δ18O大的波动,只有不到50 a的时间,湖水中稳定同位素会重新达到平衡.  相似文献   

13.
Diamonds from high- and low-MgO groups of eclogite xenoliths from the Jericho kimberlite, Slave Craton, Canada were analyzed for carbon isotope compositions and nitrogen contents. Diamonds extracted from the two groups show remarkably different nitrogen abundances and δ13C values. While diamonds from high-MgO eclogites have low nitrogen contents (5-82 ppm) and extremely low δ13C values clustering at ∼−40‰, diamonds from the low-MgO eclogites have high nitrogen contents (>1200 ppm) and δ13C values from −3.5‰ to −5.3‰.Coupled cathodoluminescence (CL) imaging and SIMS analysis of the Jericho diamonds provides insight into diamond growth processes. Diamonds from the high-MgO eclogites display little CL structure and generally have constant δ13C values and nitrogen contents. Some of these diamonds have secondary rims with increasing δ13C values from −40‰ to ∼−34‰, which suggests secondary diamond growth occurred from an oxidized growth medium. The extreme negative δ13C values of the high-MgO eclogite diamonds cannot be produced by Rayleigh isotopic fractionation of average mantle-derived carbon (−5‰) or carbon derived from typical organic matter (∼−25‰). However, excursions in δ13C values to −60‰ are known in the organic sedimentary record at ca. 2.7 and 2.0 Ga, such that diamonds from the high-MgO eclogites could have formed from similar organic matter brought into the Slave lithospheric mantle by subduction.SIMS analyses of a diamond from a low-MgO eclogite show an outer core with systematic rimwards increases in δ13C values coupled with decreases in nitrogen contents, and a rim with pronounced alternating growth zones. The coupled δ13C-nitrogen data suggest that the diamond precipitated during fractional crystallization from an oxidized fluid/melt from which nitrogen was progressively depleted during growth. Model calculations of the co-variation of δ13C-N yielded a partition coefficient (KN) value of 5, indicating that nitrogen is strongly compatible in diamond relative to the growth medium. δ13C values of diamond cores (−4‰) dictate the growth medium had higher δ13C values than primary mantle-derived carbon. Therefore, possible carbon sources for the low-MgO eclogite diamonds include oxidized mantle-derived (e.g. protokimberlite or carbonatite) fluids/melts that underwent some fractionation during migration or, devolatilized subducted carbonates.  相似文献   

14.
An empirical calibration for the oxygen isotope fractionation between biogenic silica and water was determined for diatom frustules sampled from living diatom communities in the Jemez Mountains of northern New Mexico, USA. Over a temperature range from 5.1 to 37.8 °C, the silica-water fractionation is defined by the equation 1000 ln α(silica-water) = 2.39(±0.13) × 106T−2 + 4.23(±1.49). This relationship is in close agreement with other published silica-water fractionation factors for laboratory cultured diatom samples; however, it is as much as 8‰ lower than equilibrium quartz-water fractionations and 3-4‰ lower than observed silica-water fractionations in diatomaceous silica collected from sediment traps and sediment cores. There are three possible explanations for the disparate silica-water fractionation factors observed in diatom silica: (1) silica does not precipitate in equilibrium with ambient water, (2) silica does precipitate in equilibrium with ambient water, but the silica-water fractionation factor for diatom silica is considerably less than the equilibrium fractionation factor for quartz-water, or (3) silica precipitation is influenced by a ‘vital’ effect, where the δ18O value of the water inside the diatom cell walls is lower than the δ18O values of ambient water.Post-mortem loss of organic material results in an alteration or ‘maturation’ of diatom silica in which silica reequilibrates with a silica-water fractionation closer to the equilibrium quartz-water fractionation. Alteration is likely to occur rapidly after the diatom frustule loses its organic coating, either as it settles through the water column or at the sediment-water interface; δ18O values recorded by paleo-diatom silica therefore do not record growing conditions but more likely record conditions at the sediment-water interface. In the case of lacustrine environments, where the bottom water remains at a nearly constant 4 °C, the reequilibration of diatom silica with bottom conditions could reduce or remove the conflating effects of temperature on δ18O values recorded by paleo-diatom silica and provide direct information on the δ18O value of the lake water.  相似文献   

15.
The reliability of δ13C trends in Neoproterozoic carbonate-dominated successions for regional and global chemostratigraphic correlation is discussed. In the light of recent findings of a predominantly non-marine rare earth element and yttrium signature in most Neoproterozoic carbonates and a comparatively short oceanic residence time of carbon, trends towards enrichment in 13C seen in many of these carbonates are considered to reflect facies variations rather than temporal signals of ocean chemistry. Positive δ13CCarb excursions are explained by elevated bioproductivity and/or increased evaporation in shallow marine, near-coastal, temporarily restricted depositional environments. Examples are provided that illustrate that C isotope trends can be highly ambiguous temporal markers and are in the absence of other chemostratigraphic data, such as Sr isotope ratios, and radiometric age control of only limited use for stratigraphic correlation. The overall enrichment in 13C recorded by most Neoproterozoic carbonates, except for those in close stratigraphic proximity to glacial deposits, is suggested to reflect a dominance of microbially mediated carbonate formation in the Neoproterozoic. This might explain why C isotope chemostratigraphy in Neoproterozoic successions is less reliable than in Phanerozoic successions in which carbonates are, with only few exceptions, biogenic products of shelly fossils.  相似文献   

16.
陆生蜗牛化石稳定同位素组成是一种良好的古环境信息载体,常被用于古环境古气候的重建。由于缺少古环境因子 对蜗牛壳体稳定同位素组成机理性的结论,因此越来越多的研究侧重于对现代蜗牛壳体的环境效应进行探讨。实验室蜗牛 饲养实验则可以通过控制环境因素来确定其对壳体碳酸盐稳定同位素组成的影响程度,从而得到较为确切的结果。该文在 前人的研究基础上,利用Achatina fulica 进行实验室饲养实验。结果表明,在相同的温、湿度下,同种食物喂养的蜗牛壳体 有非常稳定的分馏值,不同食物类型的结果有一定的差异,莴苣叶、玉米粉和饲料喂养的蜗牛壳体相对于食物的分馏值分 别为16.70‰±0.2‰,10.57‰±0.2‰和10.65‰±0.2‰;在20~30℃实验条件下,壳体δ13C并不受环境温度的影响,主要受食 物的影响,并得到两者之间的回归方程为δ13Cs=0.6665δ13Cv+6.2302（n=26）;无机碳酸盐对Achatina fulica 壳体文石δ13C值影 响很少;根据端元组分分析方法的统计结果显示,食物是Achatina fulica 壳体碳同位素组成的主要影响因素,贡献值约为 80％±5％,除此以外,大气CO2的贡献值约为20％±5％。  相似文献   

17.
In this study we determined rubidium isotope ratios in twenty-one commonly used international geological reference materials, including igneous, sedimentary and metamorphic rocks, as well as an IAPSO seawater reference material. All δ87Rb results were obtained relative to the NIST SRM 984 reference material. For most reference materials, Rb was purified using a single column loaded with Sr-spec resin. For reference materials containing low Rb but high mass fractions of matrix elements (such as basic rock and seawater), Rb was purified using two-column chromatography, with the first column packed with AGMP-50 resin and the second column packed with Sr-spec resin. Two methods for instrumental mass bias correction, sample-standard bracketing (SSB) mode, and the combined sample-standard bracketing and Zr internal normalisation (C-SSBIN) method, were compared for Rb isotopic measurements by multi-collector inductively coupled plasma-mass spectrometry (MC-ICP-MS). The long-term reproducibility of Rb isotopic measurements using both methods was similar, better than 0.06‰ (2s, standard deviation) for NIST SRM 984. Significant Rb isotopic fractionation was observed among the reference materials, with an overall variation in δ87Rb values of approximately 0.5‰. The δ87Rb values of igneous rocks ranged from -0.28‰ to +0.06‰, showing a trend from heavier isotopic compositions in mafic rocks to lighter δ87Rb values in the more evolved felsic rocks. The sedimentary and metamorphic rocks had Rb isotope ratios similar to those of igneous rocks. The δ87Rb values of the reference materials related to low-temperature geological processes showed a wider range than those of high-temperature processes. Notably, the IAPSO seawater reference material had a δ87Rb value of +0.14‰, which deviated from that of igneous rocks, and represents the heaviest reservoir of Rb isotopes found thus far on Earth. The comprehensive dataset presented here has the potential to serve for quality assurance purposes, and provide a framework for interlaboratory comparisons of Rb isotope ratios.  相似文献   

18.
In this study, with the method of vacuum extraction, two evaporative processes of soil water and free water under equilibrium condition were simulated. For each sample, water vapor was condensed by liquid nitrogen and was collected in four time intervals. From the analysis of hydrogen and oxygen isotopic compositions of the water collected at different times, it was discovered that the isotope fractionation of soil water also follows the mode, which is just the same as the evaporative process of free water. The relationship between the stable hydrogen and oxygen isotopes in residual water showed that the simulative evaporation line was close to the global meteoric water line (GMWL) under the equilibrium condition at about 20°C. Comparison of the two types of evaporative processes indicated that the isotope fractionation and evaporation velocity of soil water were only slightly modified by the Van der Waals force.  相似文献   

19.
The first data are reported on the carbon isotopic composition of diamond crystals from the Grib pipe kimberlite deposit of the Archangelsk diamond province (ADP). The δ13C value of the crystals ranges from ?2.79 to ?9.61‰. The isotopic composition of carbon was determined in three zoned crystals (δ13C of ?5.8 ?6.96 ‰, ?5.64/ ?5.85 ‰, and ?5.94/ ?5.69 ‰), two “diamond in diamond” samples (diamond inclusion with δ13C of ?4.05 and ?6.34 ‰ in host diamond crystals with δ13C of ?8.05 and ?7.54 ‰, respectively), and two samples of coated diamonds (cores with δ13C of ?6.98 and ?6.78‰ and coats with δ13C of ?7.51 and ?8.01 ‰, respectively). δ13C values were obtained for individual diamond crystals from bort-type aggregates (δ13C of ?4.24/ ?4.05 ‰, ?6.58/ ?7.48 ‰, and ?5.48/ ?6.08 ‰). Correlations were examined between the carbon isotopic composition of diamonds and their crystal morphology; the color; the concentration of nitrogen, hydrogen, and platelet defects; and mineral inclusions content. It was supposed that the observed δ13C variations in the crystals are most likely related to the fractionation of carbon isotopes rather than to the heterogeneity of carbon sources involved in diamond formation. The isotopic characteristics of diamonds from the Grib pipe were compared with those of previously investigated diamonds from the Lomonosov deposit. It was found that diamonds from these relatively closely spaced kimberlite fields are different; this also indicates the existence of spatially localized peculiarities of isotope fractionation in processes accompanying diamond formation.  相似文献   

20.
The stable isotope composition (δ15N and δ18O) of nitrate was measured during Summer 1999 in the anaerobic hypolimnion of eutrophic Lake Lugano (Switzerland). Denitrification was demonstrated by a progressive nitrate depletion coupled to increasing δ15N and δ18O values for residual nitrate. Maximum δ15N and δ18O values amounted to 27.2 and 15.7‰, respectively.15N and 18O enrichment factors for denitrification (ε) were estimated using a closed-system model and a dynamic diffusion-reaction model. Using the Rayleigh equation (closed-system approach), we obtained ε values of −11.2 and −6.6‰ for nitrogen and oxygen, respectively. The average ε values derived using the diffusion-reaction model were determined to be −20.7 ± 3.8 for nitrogen and −11.0 ± 1.7 for oxygen. Both N and O isotope fractionation appeared to be lower when denitrification rates where high, possibly in association with high organic carbon availability. In addition, variations in the isotope effects may be attributed to the variable importance of sedimentary denitrification having only a small isotope effect on the water column. The combined measurement of N and O isotope ratios in nitrate revealed that coupled nitrification-denitrification in the open-water was of minor importance. This is the first study of nitrogen and oxygen isotope effects associated with microbial denitrification in a natural lake. Moreover, this study confirms the high potential of δ18O of nitrate as a valuable biogeochemical tracer in aquatic systems, complementing nitrate δ15N.  相似文献   

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