雅克拉凝析油气田油水界面甲烷天然释放及其源示踪

为评价油气田天然释放CH₄对大气CH₄源与汇的贡献, 采用静态箱法实地监测了新疆塔里木盆地雅克拉凝析油气田油水界面处甲烷的释放通量, 并采用在线大气甲烷碳同位素制样系统与稳定同位素质谱仪联机测试了通量箱甲烷碳同位素组成.结果表明, 由于油水界面边水活跃程度不同, 甲烷通量在空间变化很大, 最高的日释放通量达2.28 mg/m2·d, 最低-1.32 mg/m2·d, 日平均释放通量0.51 mg/m2·d, 标准偏差达1.23 mg/m2·d.油水界面处甲烷通量日变化规律基本相同, 凌晨至清晨时达到相对高点, 随后逐渐降低, 下午至傍晚时段为释放低值甚至负值, 夜晚时分又逐渐增加.通量箱中甲烷δ13C组成白天随甲烷浓度的线性降低而逐渐偏重, 夜晚δ13C随着甲烷浓度的线性增加而逐渐偏重.可见, 油水界面边水活跃, 其上方的土壤形成相对氧化的环境, 油气藏甲烷及烃类在向地表运移的过程中不断被土壤吸收氧化, 仅有少量运移至地表并逸散到大气中, 局部甚至均被吸收氧化, 而成为大气甲烷的汇.      

土壤甲烷及其碳同位素地球化学特征

本文重点对我国干旱-半干旱区油气异常区和非油气区地表土壤甲烷的碳同位素组成进行了分析;据此,对土壤、重烃及甲烷的碳同位素地球化学特征进行了讨论。     

Methane exchange between coal-bearing basins and the atmosphere: the Ruhr Basin and the Lower Rhine Embayment, Germany

A precise knowledge of methane exchange processes is required to fully understand the recent rise of atmospheric methane concentration. Three of these processes take place at the lithosphere/atmosphere boundary: bacterial consumption of methane and emission of bacterial or thermogenic methane. This study was initiated to quantify these processes on a regional scale in the Ruhr Basin and the Lower Rhine Embayment. Since these areas are subject to bituminous coal and lignite mining, natural and anthropogenically-induced methane exchange processes could be studied. The methane emission and consumption rates and their carbon isotope signal were measured at the lithosphere/atmosphere boundary using flux chambers. On most of the soils studied, methane consumption by bacteria was identified. Thermogenic methane was released only at some of the natural faults examined. In active and abandoned bituminous coal mining areas methane emissions were restricted to small areas, where high emission rates were measured. The carbon isotope composition of methane at natural faults and in mining subsidence troughs was typical of thermogenic methane (−45 to −32 ‰ δ¹³C). Methane exchange balancing revealed that natural methane emissions from these two basins represent no source of atmospheric importance. However, methane release by upcast mining shafts dominates the methane exchange processes and is by about two orders of magnitude greater than methane consumption by bacterial oxidation in the soils.     

Geochemical insights into contribution of petroleum hydrocarbons to the formation of hydrates in the Taixinan Basin,the South China Sea

Methane hydrate in the South China Sea(SCS)has extensively been considered to be biogenic on the basis of itsδ13C and δD values.Although previous efforts have greatly been made,the contribution of thermogenic oil/gas has still been underestimated.In this study,biomarkers and porewater geochemical parameters in hydrate-free and hydrate-bearing sediments in the Taixinan Basin,the SCS have been measured for evaluating the contribu-tion of petroleum hydrocarbons to the formation of hydrate deposits via a comparative study of their source inputs of organic matters,environmental conditions,and microbial activities.The results reveal the occurrence of C14-C16 branched saturated fatty acids(bSFAs)with relatively high concentrations from sulfate-reducing bacteria(SRBs)in hydrate-bearing sediments in comparison with hydrate-free sediments,which is in accord with the positive δ13C values of dissolved inorganic carbon(DIC),increasing methane concentrations,decreasing alka-linity,and concentration fluctuation of ions(Cl-,Br,SO2-,Ca2+,and Mg2+).These data indicate the relatively active microbial activities in hydrate-bearing sediments and coincident variations of environmental conditions.Carbon isotope compositions of bSFAs(-34.0％o to-21.2％o),n-alkanes(-34.5％o to-29.3％o),and methane(-70.7％o to-69.9％o)jointly demonstrate that SRBs might thrive on a different type of organic carbon rather than methane.Combining with numerous gas/oil reservoirs and hydrocarbon migration channels in the SCS,the occurrence of unresolved complex mixtures(UCMs),odd-even predominance(OEP)values(about 1.0),and biomarker patterns suggest that petroleum hydrocarbons from deep oil/gas reservoirs are the most probable carbon source.Our new results provide significant evidence that the deep oil/gas reservoirs may make a contribution to the formation of methane hydrate deposits in the SCS.     

Methane flux from miniseepage in mud volcanoes of SW Taiwan: Comparison with the data from Italy,Romania, and Azerbaijan

Mud volcanoes (MVs) are considered important methane (CH₄) sources for the atmosphere; gas is not only released from macro-seepage, i.e., from craters and visible gas bubbling manifestations, but also from invisible and pervasive exhalation from the ground, named miniseepage. CH₄ flux related to miniseepage was measured only in a few MVs, in Azerbaijan, Italy, Japan, Romania and Taiwan. This study examines in detail the flux data acquired in 5 MVs and 1 “dry” seep in SW Taiwan, and further compares with other 23 MVs in Italy, Romania and Azerbaijan. Miniseepage from the six manifestations in SW Taiwan MVs and seeps annually contribute at least 110 tons of methane directly to the atmosphere, and represents about ∼80% of total degassing during a quiescent period. Combining miniseepage flux and geo-electrical data from the Wu-shan-ding MV revealed a possible link between gas flux and electrical resistivity of the vadose zone. This suggests that unsaturated subsoil is a preferential zone for shallow gas accumulation and seepage to the atmosphere. Besides, miniseepage flux in Chu-huo everlasting fire decreases by increasing the distance from the main gas channeling zone and molecular fractionation (methane/ethane ratio) is higher for lower flux seepage, consistently with what observed in other MVs worldwide. Measurements from Azerbaijan, Italy, Romania, and Taiwan converge to indicate that miniseepage is directly proportional to the vent output and it is a significant component of the total methane budget of a MV. A miniseepage vs. macro-seepage flux equation has been statistically assessed and it can be used to estimate theoretically at least the order of magnitude of the flux of miniseepage for MVs of which only the flux from vents was evaluated, or will be evaluated in future. This will allow a more complete and objective quantification of gas emission in MVs, thus also refining the estimate of the global methane emission from geological sources.     

若尔盖高原沼泽湿地CH4排放研究

若尔盖高原沼泽湿地海拔 3400 m，面积 4038km²，是我国面积最大的高原沼泽湿地分布区。2001年 5～9月的非冰冻期，其主要沼泽类型木里苔草沼泽的CH₄排放通量范围是 0.51～ 8.20 m g/（m ²· h），平均值为 2.87 m g/（m ²· h）；乌拉苔草沼泽CH₄排放通量范围是 0.36～10.04 m g/（m ²· h），平均值为 4.51 m g/（m ²· h）。在空间分布上，不同沼泽类型之间CH₄排放通量具有一定的差异。在季节变化上，没有明显的排放高峰。根据代表性观测点的CH₄平均排放量、日数和沼泽总面积推算，非冰冻期若尔盖高原沼泽湿地CH₄的排放量为 0.052Tg/a。     

祁连山冻土区天然气水合物岩心顶空气组分与同位素的指示意义——以DK-9孔为例

通过对祁连山冻土区天然气水合物DK-9孔不同深度岩心顶空气中的烃类气体组分及甲烷、乙烷的C同位素分析测试,对比分析了岩心顶空气组分含量变化与天然气水合物及其异常层段、油气显示层段、断层或破碎带分布之间的空间关系,探讨了顶空气组分对天然气水合物及其异常现象、油气显示现象、烃类气体运移作用及顶空气同位素对气体成因的指示意义。结果显示,岩心顶空气中烃类气体含量高的深度段180.26~308.50m、356.45~399.32m、458.55~508.65m与天然气水合物及其异常层段、油气显示层段具有较好的对应关系,其高值区间可作为天然气水合物、油气显示的一种指示。距断层或破碎带产出位置不同的岩心顶空气组分含量变化显示,不同级次的断裂系统为烃类气体向上运移提供了通道,部分可为天然气水合物提供一定的赋存空间;甲烷、乙烷C同位素数据显示气体以热解成因为主,部分为混合成因。     

Comparison study of methane emissions from landfills with different landfill covers

Atmospheric methane, a more effective heat-trapping gas than CO₂ that may affect climate change, has its greatest man-made source in the US from municipal solid waste (MSW) landfills. Consequently, the wise management of landfills can reduce these greenhouse gas emissions to the atmosphere. Methane from modern MSW landfills built with composite covers is frequently vented directly to the atmosphere. Biofiltration of landfill gas could oxidize CH₄ to CO₂ and water. Methane oxidation in old landfills with conventional soil covers can be effective in reducing the amount of CH₄ emitted. In this study, comparison of methane emissions from three different landfill covers was conducted. Methane emissions from old landfills constructed with conventional soil covers, modern MSW landfills constructed with composite covers, and modern MSW landfills constructed with composite covers plus biofilters were calculated using the calculated CH₄ oxidation rates. The results showed that an average of only 14% of the generated CH₄ was emitted from landfills with modern composite covers plus biofilters, and an average of 85% of the generated CH₄ was emitted from landfills with conventional covers when 100% of the generated CH₄ emissions to the atmosphere from landfills with modern composite covers was assumed. By comparing the CH₄ emission rates from three different landfill types, the use of a properly sized biofilter should be an effective technique to reduce CH₄ emissions from landfills across the USA and potentially in many other areas of the world.     

Methane oxidation capacity of methanotrophs isolated from different soil ecosystems

Methane is one of the potential greenhouse gases contributing to global climate change, with a global warming potential of about 25 times than that of carbon dioxide. Aerobic methane oxidation (methanotrophy) is the key process that counteracts emission of methane to atmosphere. In this study, methane oxidation capacity of different methane-oxidizing bacteria (methanotrophs) isolated from six different ecosystems was investigated. Methanotrophic consortium isolated from dumpsite proved to be most effective in oxidizing methane. Initially, methane oxidation rate was found to be 0.72 ± 0.036 mM/day; in course of the study consortium M5 showed an increase in methane oxidation rate up to 1.7 ± 0.016 mM/day. A maximum of 0.78 mol of CO₂ production was found during methane oxidation in methanotrophs from dumpsite (M5). While varying temperatures, methane oxidation rate was in the range of 1.3–1.7 mM/day which has been found in the temperature range of 30–40 °C. Even at higher temperature (50 °C), 0.076 ± 0.14 mM of the methane was utilized per day. Methane oxidation was assessed by Michaelis–Menten kinetics. By varying the methane concentration, methane oxidation was studied and kinetic parameters such as V _max and K _m were derived using Lineweaver–Burk plot and found to be 1.497 mM/day and 2.23 mM, respectively. In methane mitigation approach, Methane soil sink is very essential because a balance between methane production by methanogens and consumption by methanotrophs plays an important role in methane emission reduction. Enhancing the methane soil sink will be a cost-effective method to cut down methane emission.     

Methane microseepage from different sectors of the Yakela condensed gas field in Tarim Basin,Xinjiang, China

Methane microseepage is the result of natural gas migration from subsurface hydrocarbon accumulations to the Earth’s surface, and it is quite common in commercial petroleum fields. While the role of microseepage as a pathfinder in petroleum exploration has been known for about 80 a, its significance as an atmospheric CH₄ source has only recently been studied, and flux data are currently available only in the USA and Europe. With the aim of increasing the global data-set and better understanding flux magnitudes and variabilities, microseepage is now being extensively studied in China. A static flux chamber method was recently applied to study microseepage emissions into the atmosphere in four different sectors of the Yakela condensed gas field in Tarim Basin, Xinjiang, China, and specifically in: (a) a faulted sector, across the Luntai fault systems; (b) an oil–water interface sector, at the northern margin of the field; (c) an oil–gas interface sector, in the middle of the field; (d) an external area, outside the northern gas field boundaries. The results show that positive CH₄ fluxes are pervasive in all sectors and therefore, only part of the CH₄ migrating from the deep oil–gas reservoirs is consumed in the soil by methanotrophic oxidation. The intensity of gas seepage seems to be controlled by subsurface geologic settings and lateral variabilities of natural gas pressure in the condensed gas field. The highest CH₄ fluxes, up to ∼14 mg m⁻² d⁻¹ (mean of 7.55 mg m⁻² d⁻¹) with higher spatial variability (standard deviation, σ: 2.58 mg m⁻² d⁻¹), occur in the Luntai fault sector. Merhane flux was lower in the oil–water area (mean of 0.53 mg m⁻² d⁻¹) and the external area (mean of 1.55 mg m⁻² d⁻¹), and at the intermediate level in the gas–oil sector (mean of 2.89 mg m⁻² d⁻¹). These values are consistent with microseepage data reported for petroleum basins in the USA and Europe. The build-up of methane concentration in the flux chambers is always coupled with an enrichment of ¹³C, from δ¹³C₁ of −46‰ to −42.5‰ (VPDB), which demonstrates that seeping methane is thermogenic, as that occurring in the deep Yakela reservoir. Daily variations of microseepage are very low, with minima in the afternoon, corresponding to higher soil temperature (and higher methanotrophic consumption), and maxima in the early morning (when soil temperatures are lowest). A preliminary and rough estimate of the total amount of CH₄ exhaled from the Yakela field is in the order of 10² tonnes a⁻¹.     

珠江口盆地恩平凹陷CO2成藏特征与成藏过程

珠江口盆地恩平凹陷北部潜山披覆带首次发现了规模富集的CO2气层,但分布局限,平面上主要分布在A油田1井区,纵向上主要分布在珠江组上段,其次是珠海组,其他层系和构造高点未见CO2富集.CO2气藏含量普遍在92％以上,δ13C为?8.735‰～?3.024‰,3He/4He介于5.75×10?6～8.16×10?6之间,为...     

地质成因的甲烷释放对大气的影响

地质成因自然源的甲烷释放在整个大气甲烷估算中起着非常重要的作用,它既是不含放射性14C甲烷源(死碳源)缺失部分的重要代表,也是甲烷重碳源的重要部分.概述了国内外关于地质成因甲烷释放对大气甲烷源与汇影响的研究进展,详述了来自地质成因化石燃料泄漏的人为甲烷释放以及来自沉积盆地(含油气盆地)、泥火山、地热区、海洋和甲烷水合物的地质自然源甲烷释放对大气甲烷源与汇的贡献及其影响因素;说明由于地质成因甲烷分布的区域性、不均匀性和时空的高度变化性,以及目前地质成因甲烷的通量估算仅建立在区域性的少量甲烷通量测试基础上,造成了地质成因甲烷释放通量估算的高度不确定性;指出研究中国西北地区油气田集聚区的甲烷释放通量,对油气田地质成因甲烷释放通量的估算具有重要意义.     

徐家围子断陷深层天然天的形成

通过对松辽盆地徐家围子断陷深层天然气的地质和地球化学分析,揭示了天然气的成因特征和形成过程。该区天然气的分子组成和同位素组成均显示出较大的变化,甲烷是天敢中的主要组分,质量分数在５７．４％－９８．２％之间,平均为９０．１％,主要非烃气体是ＣＯ２和Ｎ２,平均质量分数分别为４．９％和３．２％,且ＣＯ２质量分数变化范围较大,气体同位素分析结果表明,甲烷同位素显示煤型气特征,而乙烷和丙烷的同位素显示油型 的特征,表明徐家子深部除煤和ＩＩＩ型干酪根作为主要气源外,仍有一定含量趋于生油的ＩＩ型干酪根作为次要气源,实测和计算结果证实天然气主要是有机质在高成熟阶段形成的产物,运移过程中和成藏后的次生变化使天然气的组成和同位素面目变得非常复杂,尤其是由盖层微渗漏造成的蒸发分馏的作用使同位素出现例转,徐家围子断陷深层煤型气的发现为     

徐家围子断陷深层天然气的形成

通过对松辽盆地徐家围子断陷深层天然气的地质和地球化学分析 ,揭示了天然气的成因特征和形成过程。该区天然气的分子组成和同位素组成均显示出较大的变化 ,甲烷是天然气中的主要组分 ,质量分数在 57.4 % - 98.2 %之间 ,平均为 90 .1%。主要非烃气体是CO2 和N2 ,平均质量分数分别为 4 .9%和 3.2 % ,且CO2 质量分数变化范围较大。气体同位素分析结果表明 ,甲烷同位素显示煤型气特征 ,而乙烷和丙烷的同位素显示油型气的特征 ,表明徐家围子深部除煤和Ⅲ型干酪根作为主要气源外 ,仍有一定含量趋于生油的Ⅱ型干酪根作为次要气源 ,实测和计算结果证实天然气主要是有机质在高成熟阶段形成的产物。运移过程中和成藏后的次生变化使天然气的组成和同位素面目变得非常复杂 ,尤其是由盖层微渗漏造成的蒸发分馏作用使同位素出现倒转。徐家围子断陷深层煤型气的发现为该区油气勘探展示出了更广阔的前景。     

中国煤炭甲烷管控与减排潜力

甲烷是最主要的非二氧化碳温室气体,受到越来越多的重视。煤炭甲烷是我国最主要的甲烷排放源类型,我国也是世界煤炭甲烷排放量最大的国家,煤炭甲烷的有效排放管控与高效开发利用兼具温室气体减排、能源气体开发利用和灾害气体防治三重意义。基于系统调研和研究工作积累,概述了煤炭甲烷排放管控背景,总结了全球与代表性国家煤炭甲烷排放及其管控现状,阐释了我国煤炭甲烷开发利用与排放管控历程及发展趋势,讨论和前瞻了我国煤炭甲烷减排路径与减排潜力。已有研究工作表明:我国煤炭甲烷排放主要来自煤炭地下开采风排瓦斯,且较长时期内仍是我国煤炭甲烷的主要来源;随着我国关闭矿井增多,由此产生的关闭矿井甲烷排放量呈增长趋势,是我国煤炭甲烷不容忽视的来源。随着碳中和目标的提出,温室气体减排的政策导向逐渐成为我国煤炭甲烷排放管控的重点,明确了煤炭甲烷减排方向。我国煤炭甲烷排放管控形成了以煤层气勘探开发利用、煤矿瓦斯抽采利用、关闭/废弃矿井瓦斯抽采利用、乏风瓦斯利用等全浓度利用,煤炭采前、采中和采后全周期利用为特征的关键技术路径。我国煤炭甲烷排放管控面临巨大压力和严峻挑战,诸多政策、机制、技术问题亟待破解。突破复杂地质条件适配性煤层...     

含油气盆地地质甲烷释放研究综述

目前地质甲烷在国际上引起了广泛的关注。地质甲烷的释放在整个大气甲烷的源与汇的研究具有重要的意义。它既为不含放射性~(14)C甲烷源缺失部分提供了可能的解释,也为全球气候变暖的研究提供了科学依据。含油气盆地的甲烷是地质甲烷中的重要组成部分。本文概述了国内外含油气盆地甲烷释放的研究,详述了含油气盆地甲烷的源以及运移机制;阐述了目前对于地质甲烷研究的常用监测手段及其优缺点;并对全球含油气盆地的甲烷通量估算进行了总结。但是由于含油气盆地甲烷的通量估算是建立在区域性的部分甲烷通量测试基础上,仍然具有较大的不确定性。有效地结合甲烷的各种监测手段,在全球更多更广区域开展含油气盆地CH_4通量测量,是未来的发展方向和热点。我国是油气生产的大国之一,但相关的探究很少,因此,在我国开展含油气盆地甲烷释放通量的研究将有助于进一步完善全球含油气盆地甲烷数据库,对全球甲烷的源和汇的精确估算具有重要作用和意义。     

海洋中溶存甲烷研究进展

CH₄是大气中的重要微量气体，对全球变暖和大气化学有重要作用。海洋是大气甲烷的重要源和汇。开展海洋中溶存甲烷的研究，有助于了解海洋对大气甲烷和全球变化的贡献。综述了海洋中溶存甲烷的研究现状，着重介绍了海洋中溶存甲烷的分布特征、海气交换通量的估算及其生物地球化学循环，并探讨了该领域研究中存在的问题。     

广州地区稻田甲烷排放及中国稻田甲烷排放的空间变化

１９９３年在广州地区采用中国科学院大气物理研究所研制的自动采集和分析系统测量了稻田甲烷的排放率，首次获得了占我国２０－２５％左右水稻收获面积的华南地区稻田甲烷排放特征值。从而宏观地使我国五个主要水稻生态区的甲烷排放率都有了实测资料。稻田甲烷排放率的季节变化主要与气温及灌溉水状态的变化的较大关系，日变化规律以下午出现极大为主。本实验田的甲烷排放率低。     

Methane production from bicarbonate and acetate in an anoxic marine sediment

Methane production from ¹⁴C-labelled bicarbonate and acetate was measured over the top 28 cm of anoxic Cape Lookout Bight sediments during the summer of 1983. The depth distribution and magnitude of summed radioisotopically determined rates compare well with previous measurements of total methane production and the sediment-water methane flux. Methane production from CO₂ reduction and acetate fermentation accounts for greater than 80% of the total production rate and sediment-water flux.Methane production from bicarbonate was found to occur in all depth intervals sampled except those in the top 2 cm, whereas significant methane production from acetate only occurred at depths below 10 cm where sulfate was exhausted. Acetate provided 20 to 29% of the measured methane production integrated over the top 30 cm of the sediments.     

沁水煤层气田高阶煤解吸气碳同位素分馏特征及其意义

沁水盆地是我国煤层气勘探开发的重要有利区,沁水煤层气田位于盆地东南部。对采自沁水煤层气田两口井的煤开展了罐解吸实验。结果表明,该地区煤层气解吸速率很快,96 h后解吸气量都达到了总解吸气量的60%~85%,720 h后解吸过程基本结束;解吸气量大,平均在18 m3/t以上。煤层气解吸过程中甲烷发生碳同位素分馏,δ13C1值变化与解吸率呈良好的线性关系,参考这种正相关关系曲线,定期监视煤层气降压排采过程中甲烷δ13C1值的变化情况,可以大致推测出该地区煤层气解吸率,从而预测煤层气的采出程度。跟踪测试沁水煤层气田A1和A1-3井在试采过程的甲烷δ13C1变化情况,推测现在采出的煤层气可能主要是煤层裂隙中以游离形式存在的煤层气,表明该区煤层气稳产性较好,资源前景广阔。