海底沉积物-水界面溶解甲烷渗漏通量原位观测研究进展

海底沉积物-水界面溶解甲烷渗漏不仅是海底天然气水合物的存在标志和分解释放途径,也是冷泉生物群落的物质和能量来源,因其对海洋环境乃至全球变化的可能重要影响而日益引起人们关注,而海底原位观测及渗漏甲烷通量估算是理解上述问题的关键。目前国际上有两种较为成熟的海底甲烷通量观测方法:1流体渗漏速率原位测量配以室内甲烷浓度分析;2底栖室流体连续取样配以室内甲烷浓度分析,前者能灵敏反应冷泉渗漏速率的时序变化,而后者具有较高的甲烷通量测量准确度。随着甲烷传感器技术的发展,原位测量方法将大大提高甲烷通量测量精度、时间和分辨率。在可移动式观测平台上搭载甲烷传感器,同时进行近海底界面微尺度甲烷浓度梯度测量和湍流观测,不仅能够精细刻画近海底甲烷浓度变化、渗漏通量变化,并且非封闭环境能够最大限度地避免沉积物-水界面遭受扰动,使观测数据更接近海底真实环境,这成为未来海底原位观测的主要发展方向之一。除此之外,特征冷泉生物群落的分布已被广泛应用于将个别测量站位的观测结果扩展到整个区域的甲烷渗漏流量估算。目前,国外学者已经对部分典型海底冷泉区进行了渗漏甲烷通量估算,发现每个渗漏系统每年通过溶解形式向海水释放甲烷量约为6×103~1.35×107 mol,并且甲烷渗漏在时间上和空间上都是多变的,但还没能将单个冷泉系统的通量估算延伸到更大的时空尺度,这成为深入研究海底甲烷储库及其在全球碳循环和气候变化中的作用的瓶颈之一。     

海底冷泉区沉积物-水界面甲烷通量原位观测研究进展

海底沉积物-水界面作为冷泉跨圈层活动最关键的界面，近年来已成为冷泉区碳循环研究调查的重点目标。为准确获取海洋沉积物-水界面的流体通量，客观重建界面环境过程，评估环境效应，必须发展一整套精确、高效、科学的水下原位甲烷通量测量技术。综述了当前海洋冷泉区沉积物-水界面甲烷通量研究的意义与价值，详细介绍了多种较为成熟的海洋沉积物-水界面甲烷原位通量测试技术工作原理、使用方法和优缺点等，如测试游离气泡态甲烷通量的渗漏帐篷、声学反射、时序影像等技术方法，原位溶解态甲烷膜脱气技术的甲烷传感器、激光拉曼光谱测量方法等，同时对全球该领域已经调查的地区、研究现状和进展进行了详细的介绍。最后从技术层面对这一研究领域未来的发展方向和趋势进行展望，以期为未来国内海洋冷泉区沉积物-水界面甲烷通量原位观测研究提供思路与方向借鉴。     

南海F站位冷泉水体中的溶解甲烷

目前对南海北部陆坡的F站位冷泉的研究多从地质和生物角度开展,而冷泉羽流在水平和垂直方向上的扩散范围尚不清晰,其影响因素尚不明确。针对该问题,于2021年6月6~23日搭乘“科学”轮对该冷泉海域的溶解甲烷进行调查,使用搭载遥控无人潜水器(Remote Operated Vehicle,ROV)和温盐深系统(Conductivity,Temperature,Depth,CTD)的采水瓶采集了该冷泉及邻近水体中从近海底(距底2.5 m)至表层(5~10 m)多个层位的水样,并使用气相色谱仪在现场分析了水样中溶解甲烷的含量。结果表明,溶解甲烷在覆盖喷口的生物繁茂区水体中的含量为6 590~11 300 nmol/L,在生物稀少的毗邻区迅速降至85.0~354.8 nmol/L。水柱剖面的测量结果显示冷泉喷口区1 000 m以深的水体中溶解甲烷含量高于背景区,而1 000 m以浅的水体中溶解甲烷的含量与背景区相同(2.01~3.90 nmol/L);自喷口区顺流向下1 500 m处,甲烷羽流信号消失。综上结果,甲烷羽流的水平扩散距离≤1 500 m,上升高度≤125 m。溶解甲烷的含量在生物繁茂区的迅速降低是由于底栖生物对溶解甲烷的摄食所致,而其在繁茂区之外扩散过程中的逐渐降低是海水湍流混合导致的稀释效应所致。     

基于光学技术的水下气泡探测实验研究

热液/冷泉溢出含有硫化氢、甲烷、二氧化碳等化学成分的气泡。实验室模拟海底热液/冷泉资源溢出气泡环境搭建了实验平台,以甲烷气体为实验气体,在黑暗环境下用高速光电探测器对气泡后向散射光进行接收,用拉曼光谱仪实现甲烷气体气泡后向散射光的拉曼检测,并与计算拉曼光谱比较。由结果可知激光拉曼光谱可以探测到气泡后向散射光,并识别气泡中含有的气体成分。通过探测气泡成分,从而判定这些气泡是否来自海底热液/冷泉等甲烷资源溢出。这样的探测方式,探测准确率高,缓解探测深度,同时避免探测设备直接与海底资源直接接触而造成的寿命缩减,为将来的海洋探测与实际应用打下了良好的基础。     

海洋钻探对甲烷渗漏的影响:以南海北部天然气水合物钻探GMGS2-16站位为例

目前世界上许多国家对海洋天然气水合物开展了调查和试开采,但是对水合物开发与海底甲烷渗漏之间的关系缺乏了解。本文依托我国第二次天然气水合物钻探航次(GMGS2),对GMGS2-16钻孔开展了两次钻后甲烷渗漏调查。第一次使用水下机器人(ROV)在该孔开钻之前、钻探过程中及完钻67天内进行了4次海底观察,其中开钻之前未发现海底甲烷渗漏,而在完钻后的两次海底观察中,发现大量气泡从废弃井口冒出。第二次使用船载多波束在该孔完钻18个月后开展水体调查,发现水体中存在火焰状的高回波强度,表明水体中存在气体羽状流,指示海底发生了甲烷渗漏。地震剖面显示该站位水合物赋存层下伏游离气,甲烷渗漏可能是由于钻探打通了海底与该游离气层,形成了甲烷气体运移的优势通道,造成海底甲烷渗漏。多波束水体数据显示甲烷气泡从海底溢出,在海面以下约650m处消失,表明甲烷气体在通过水体的过程中被完全溶解,因此,钻探导致的甲烷渗漏对大气的影响较小。未来随着井壁的坍塌以及水合物在井内的形成,气体运移的优势通道将会完全关闭,甲烷渗漏终止。     

海底天然气水合物及冷泉流体渗漏的原位观测技术

海底天然气水合物藏是天然的巨型碳储藏库,是深部甲烷等烃类气体运移至海底过程中暂时的碳储,是地球碳循环过程的重要一环。冷泉通常与海底天然气水合物藏分解密切相关,是深源或浅层气及水合物分解气在海底发生渗漏的现象。该文根据国内外天然气水合物及冷泉系统勘查的最新动向,综述了与水合物及冷泉流体渗漏相关的羽状流、运移通道、海底微地形地貌等要素的海底原位观测技术,主要包括：走航式及坐底式原位观测、海面及低空渗漏甲烷观测、海底可视化观测、与水合物及冷泉相关的海底观测网络等。综合使用原位观测技术可以更细致、全面地描绘水合物和冷泉系统的时空“景象”,更好地协助厘清海底渗漏甲烷的归趋,拓展人类对深海独特生命绿洲的认知。     

深海冷泉古菌厌氧甲烷氧化研究进展

在富含甲烷水合物的海相冷泉沉积物中, 古菌厌氧甲烷氧化作用(anaerobic oxidation of methane, AOM)越来越受到人们的重视。目前普遍认为, AOM是由嗜甲烷古菌和硫酸盐还原菌共同调节的生物地球化学过程。16S rRNA基因分析表明, 包括AEME-1、AEME-2和AEME-3在内的多种甲烷古菌参与了AOM的过程, 它们广泛分布于全球大洋海底缺氧带。AOM过程与全球环境变化密切相关, 从深海底部冷泉区向上渗漏的甲烷气体, 绝大部分在穿透缺氧带沉积层过程中被甲烷氧化古菌所消耗, 有效减少了具有强烈温室效应的甲烷气体向大气的释放。对AOM生物地球化学过程的研究, 在认识冷泉系统碳酸盐的形成机理、控制强温室气体甲烷从海底的渗漏和开发可燃冰新能源等方面具有重要意义。     

海底冷泉区气泡流量流速的声学探测机理研究

海洋冷泉区常含有巨大资源前景和引发环境灾害的天然气水合物,并发育有依赖于流体化学自养能和养分的特异生物群,研究其泄漏气体的流量和流速,具有重要的资源和环境意义。冷泉区存在大量气泡幕,首先根据声波穿过气泡幕时会产生强烈衰减的特征,对穿过不同气泡流量的声波进行探测,得到气泡流量和声波衰减呈线性比例关系;其次,利用相关流量法对放置于不同深度的两路接收信号进行互相关分析,计算出气泡流的上升速度。在此基础上通过声学探测所得声波幅值,反演出气泡流量;并由气泡的上升速度和流量得出气泡的分布范围,为海洋冷泉区气泡流速流量探测提供了新的方法。     

南海冷泉分布特征及油气地质意义

在系统收集和分析南海海底冷泉资料基础上,应用浅剖和多波束水体影像技术识别海底冷泉,结合地质条件综合研究南海冷泉分布特征,进而分析探讨其油气地质意义。研究结果表明,南海冷泉分布广泛,神狐、东沙西南部、东沙东北部、琼东南、西沙海槽、南沙南部和越南沿岸等海域均发现冷泉,冷泉分布水深为200~3 000m。海底冷泉与深部油气乃至浅层天然气水合物资源有着密切的成因联系。冷泉及其伴生物(冷泉碳酸盐岩)的探测与识别对海洋油气勘探,尤其是天然气水合物勘查的指示作用明显。浅剖和多波束水体影像技术不仅可以探测和识别冷泉,而且两者结合可实现低成本、高效率的海底地质异常体(冷泉碳酸盐岩、泥底辟及气烟囱等)的声学异常探测,极大地提高了海洋油气勘探及天然气水合物勘查的成功率。     

海底甲烷缺氧氧化与冷泉碳酸盐岩沉淀动力学研究进展

海底缺氧带甲烷氧化作用是一个重要的甲烷生物地球化学过程,已被许多地球化学现象所证实。甲烷缺氧氧化有效地减少了渗漏到海水和大气中的甲烷通量,但目前仅有的数据还不能很好地限定甲烷缺氧氧化在全球甲烷循环和全球碳循环中的作用。甲烷缺氧氧化的机理还存在争议,很可能是一个“反甲烷生成”过程。在许多天然气渗漏发育区域,由于甲烷缺氧氧化作用引起环境碱度的增加而沉淀冷泉碳酸盐岩,在海底表层沉积物中形成块状碳酸盐岩结壳。但冷泉碳酸盐岩生成所需的物理化学和生物地球化学条件在很大程度上还不清楚。数值计算表明,孔隙水中溶解足够量的甲烷、冷泉渗漏强度适中、较小的生物扰动作用有利于冷泉碳酸盐岩的生成,而过高的沉积速率则抑制冷泉碳酸盐岩结壳的生成。因此,海底发育冷泉碳酸盐岩可以指示天然气渗漏系统的演化特征。     

冷泉系统甲烷气体渗漏的声学特征及潜在环境效应

The amount of methane leaked from deep sea cold seeps is enormous and potentially affects the global warming,ocean acidification and global carbon cycle. It is of great significance to study the methane bubble movement and dissolution process in the water column and its output to the atmosphere. Methane bubbles produce strong acoustic impedance in water bodies, and bubble strings released from deep sea cold seeps are called "gas flares"which expressed as flame-like strong backscatter in the water column. We characterized the morphology and movement of methane bubbles released into the water using multibeam water column data at two cold seeps. The result shows that methane at site I reached 920 m water depth without passing through the top of the gas hydrate stability zone(GHSZ, 850 m), while methane bubbles at site II passed through the top of the GHSZ(597 m) and entered the non-GHSZ(above 550 m). By applying two methods on the multibeam data, the bubble rising velocity in the water column at sites I and II were estimated to be 9.6 cm/s and 24 cm/s, respectively. Bubble velocity is positively associated with water depth which is inferred to be resulted from decrease of bubble size during methane ascending in the water. Combined with numerical simulation, we concluded that formation of gas hydrate shells plays an important role in helping methane bubbles entering the upper water bodies, while other factors, including water depth, bubble velocity, initial kinetic energy and bubble size, also influence the bubble residence time in the water and the possibility of methane entering the atmosphere. We estimate that methane gas flux at these two sites is 0.4×10~6–87.6×10~6 mol/a which is extremely small compared to the total amount of methane in the ocean body, however, methane leakage might exert significant impact on the ocean acidification considering the widespread distributed cold seeps. In addition, although methane entering the atmosphere is not observed, further research is still needed to understand its potential impact on increasing methane concentration in the surface seawater and gas-water interface methane exchange rate, which consequently increase the greenhouse effect.     

Compositional changes in natural gas bubble plumes: observations from the Coal Oil Point marine hydrocarbon seep field

Detailed measurements of bubble composition, dissolved gas concentrations, and plume dynamics were conducted during a 9-month period at a very intense, shallow (22-m water depth) marine hydrocarbon seep in the Santa Barbara Channel, California. Methane, carbon dioxide, and heavier hydrocarbons were lost from rising seep bubbles, while nitrogen and oxygen were gained. Within the rising seawater bubble plume, dissolved methane concentrations were more than 4 orders of magnitude greater than atmospheric equilibrium concentrations. Strong upwelling flows were observed and bubble-rise times were ~40 s, demonstrating the rapid exchange of gases within the bubble plume.     

Contributions to atmospheric methane by natural seepages on the U.K. continental shelf [Mar. Geol. 137 (1997) 165–189]

Natural gas seepages occur on the United Kingdom's continental shelf and although published reports suggest that they are very rare, the petroleum industry has identified, but not publicly reported, many more. There is also very little data on the flux of gas from seabed seepages, and even less on the contribution of seepages to atmospheric concentrations of gases such as methane.

Potential gas source rocks include Quaternary and Tertiary peats as well as petroliferous source rocks such as the Carboniferous Coal Measures and the Upper Jurassic Kimmeridge Clays. There are also other organic-rich sediments which are potential source rocks. Together these cover a considerable part of the U.K. continental shelf.

Analogue seismic reflection (pinger) profiles acquired during the British Geological Survey's regional mapping programme have been reviewed to identify water column targets including fish and plumes of gas bubbles. The ability to distinguish targets is critical to an assessment of the distribution of gas seepages. Both theoretical predictions of target identity and the habits of shoaling fish have been investigated in order to identify a method of distinction.

Data from seabed seepages and measurements of seepage rates have been used to establish likely ranges of gas flux rates and the sizes of gas bubbles. The likelihood that a rising bubble will survive and escape into the atmosphere is determined primarily by bubble size and water depth; methane, the principal constituent of seepage gas, is relatively unreactive and sparingly soluble.

The studies have enabled a new estimate of the distribution of gas seepages on the U.K. continental shelf, and of the contribution to atmospheric methane levels. The results suggest that natural gas seepages are significantly more important as a source of methane than had hitherto been established. It is estimated that between 120,000 and 3.5 mtonnes of methane per year come from a continental shelf area of about 600,000 km². This represents between 2% and 40% of the total United Kingdom methane emission. It is suggested that similar contributions arise from other continental shelf areas worldwide, and that geological sources of atmospheric methane are more significant than is generally acknowledged.     

Seismic imaging of the Formosa Ridge cold seep site offshore of southwestern Taiwan

Multi-scale reflection seismic data, from deep-penetration to high-resolution, have been analyzed and integrated with near-surface geophysical and geochemical data to investigate the structures and gas hydrate system of the Formosa Ridge offshore of southwestern Taiwan. In 2007, dense and large chemosynthetic communities were discovered on top of the Formosa Ridge at water depth of 1125 m by the ROV Hyper-Dolphin. A continuous and strong BSR has been observed on seismic profiles from 300 to 500 ms two-way-travel-time below the seafloor of this ridge. Sedimentary strata of the Formosa Ridge are generally flat lying which suggests that this ridge was formed by submarine erosion processes of down-slope canyon development. In addition, some sediment waves and mass wasting features are present on the ridge. Beneath the cold seep site, a vertical blanking zone, or seismic chimney, is clearly observed on seismic profiles, and it is interpreted to be a fluid conduit. A thick low velocity zone beneath BSR suggests the presence of a gas reservoir there. This “gas reservoir” is shallower than the surrounding canyon floors along the ridge; therefore as warm methane-rich fluids inside the ridge migrate upward, sulfate carried by cold sea water can flow into the fluid system from both flanks of the ridge. This process may drive a fluid circulation system and the active cold seep site which emits both hydrogen sulfide and methane to feed the chemosynthetic communities.     

The hydroacoustic method for the quantification of the gas flux from a submersed bubble plume

This article presents an inverse hydroacoustic method for the remote quantification of the total gas flux transported from an underwater bubble plume. The method includes the surveying of the bubble plume by a vertically looking echo sounder and the calculation of the flux using the spatial distribution of the ultrasound backscattering at a fixed depth. A simplified parameterization containing only a few parameters is introduced to describe the empirical bubble size distribution. The linear correlation between the backscattering cross section of the bubble stream and the vertical gas flux is found. The calculation procedure takes into account the occurrence of a gas hydrate film at the bubble’s surface. The influence of different parameters on the accuracy of the method is investigated. The resolution volume of the echo sounder corresponding to the fixed distance is considered as a two-dimensional spatial window. The method was applied to quantify the total convective methane flux at the Haakon-Mosby mud volcano (HMMV) depth 1280 m. The calculated values of the total flux near the bottom (100–400 t/year) are in good agreement with the independently estimated flux for the single bubble jet observed from the ROV (70 t/year). These calculations also show significant temporal variability of the flux at the HMMV. The total flux was found to vary by about a factor of 2–3 within time scales of days.     

High-resolution mapping of shallow gas accumulations and gas seeps in San Simón Bay (Ría de Vigo, NW Spain). Some quantitative data

San Simón Bay in the innermost part of the Ría de Vigo is characterized by an abundance of very shallow gas accumulations and methane seeps. During the expeditions of April–June–September 2004 within the Spanish-funded Gs2G project, detailed very high-resolution seismic and field investigations were carried out to study the shallow gas and the seeps. Direct gas fluxes also were measured from bubble streams. For the first time, the surface area and gas front depth of a shallow gas field has been mapped and quantified in the inner bay of Ría de Vigo. This field overlaps spatially with the distribution of Holocene mud within the bay. Seismic data show 3.6 km² affected by acoustic turbidity but this surface can be extended up to 9.5 km² of San Simón’s muddy subtidal area. Mounded turbidity superimposed on the main gas field has been mapped and characterized as anthropogenically (mussel rafts) mediated gas accumulations. Different acoustic anomalies have been identified and interpreted as being due to gas escapes from the present seabed sediment. The very high resolution of the seismic data makes it possible to identify a new type of seep, here named ‘acoustic smoke.’ A direct relationship can be observed between the gas front of accumulations and escape features, both acoustic seeps and pockmarks. The methane flux has been estimated from the subtidal environment in San Simón based on detected acoustic targets and direct measurements of current bubble flow. The total estimated methane flux from the seabed into the water column ranges from 10.1 to 48.8 t/year, and into the atmosphere from 7.0 to 34.2 t/year. The intertidal San Simón environment is also actively venting methane, as indicated by the presence of bubbling during high tide and white patches of Beggiatoa sp.     

南海北部甲烷渗漏活动存在的证据:近底层海水甲烷高浓度异常

用吹扫-捕集法对东沙群岛西南和西沙海槽附近海域5个站位水柱中的甲烷浓度进行了测定,在其中的3个站位发现了甲烷高浓度异常。在东沙群岛西南海域的E105A和E106两站位近底层海水中甲烷浓度均出现异常增加,其值分别为4.25和10.64 nmol/dm3。在西沙海槽附近的E413站位甲烷异常出现在1 750,1 900和2 050 m深的近底层水中,浓度分别达5.17,8.48和8.70 nmol/dm3。在近底层海水中出现的甲烷高浓度异常是由于沉积物下部甲烷渗漏活动造成的,结合前人在这两个海域沉积物的地球物理和化学调查资料,认为可能是与冷泉渗漏或天然气水合物分解有关。2007年5月在探测到甲烷高浓度明显异常的东沙群岛西南神弧海域,获得了天然气水合物的实物样品,但是西沙海槽附近海域近底层水的甲烷高浓度异常是来源于天然气水合物还是来源于冷泉需要进一步加以确认。     

The evidence for the existence of methane seepages in the northern South China Sea: abnormal high methane concentrations in bottom waters

The methane concentration of water samples at five stations collected by the CTD rosette water sampler in the areas of southwest Dongsha Islands and the Xisha Trough was analyzed by the gas-stripping method on aboard ship. It shows abnormal high methane concentrations in near bottom water samples at three stations. In the southwest Dongsha Islands area, the methane conc.entration of 4. 25 and 10. 64 nmol/dm3 occurs in near bottom water samples at Stas E105A and El06, respectively. In the Xisha Trough area, the high methane concentrations of 5. 17, 8.48 and 8.70 nmol/dm3 in water depths of 1 750, 1 900 and 2 050 m, respectively, have been observed at Sta. F413. It is believed that the abnormal high methane concentrations are generated from the leakage of methane from sediments. Combining with previous geophysical and geochemical data from these two areas, this was probably related to the submarine gas hydrates decomposition and cold seep system. In May 2007, gas hydrate samples were successfully obtained by the drilling in the Shenhu Sea area located in the southwest Dongsha Islands area. It is called for further drilling surveys to confirm the existence of gas hydrate and cold seep system in the Xisha Trough as early as possible.     

Estimation of methane fluxes from bottom sediments of Lake Baikal

Methane bubble fluxes in gas flares from bottom sediments in Lake Baikal were estimated for the first time using hydroacoustic methods. Earlier work has demonstrated the occurrence of gas seeps both inside and outside of areas where bottom simulating reflectors were identified in seismic profiles. Fluxes ranged from 14 to 216 tons per year, with the flux for the entire area of the central and southern basins ranging from 1,400 to 2,800 tons per year. Comparison with other water bodies showed that fluxes from the most intensive Baikal flares were similar to those in the Norwegian and Okhotsk seas. Gas hydrates decompose at the lower boundary of the gas hydrate stability zone due to sedimentation. Calculation of the amount of methane produced due to sedimentation gave a total of between 2,600 and 14,000 tons per year for the central and southern basins of the lake. Based on rough estimation, the total flux from shallow- and deep-water gas seeps is similar to the amount of methane produced due to sedimentation. This suggests that gas hydrates possibly occupy much more than 10?% of the pore volume near the base of the gas hydrate stability zone, or that there are other reasons for gas hydrate dissociation and bubble flux from these bottom sediments.     

Breakup of deep-water methane bubbles

During the Russian Academy of Sciences “MIRI na Baikale. 2008–2009” expedition, deep-water experiments on methane bubbles emerging from the lake bottom at depth of 1400 and 860 meters were carried out. Bubbles escaping the seabed were caught by a trap, which was an inverted glass. Entering in the trap, bubbles became covered by a gas hydrate envelope and then after a time period collapsed into a number of gas hydrate solid fragments. Due to positive buoyancy, fragments remained in the top part of a trap, exhibiting properties of a powder. The glass’s bottom was replaced with a 1 mm mesh grid, allowing the finest gas hydrate particles to sift through the grid, rising upwards. It is proposed that bubble collapse into fragments is related to the pressure drop in the bubble in the course of formation of the gas hydrate envelope. No visible changes in the gas hydrate powder were observed in the course of lifting it to a depth of 380 meters. Shallower than 380 meters, i.e., outside the zone of gas hydrate stability, decomposition of the gas hydrate powder into methane gas was observed.