海湾区海水中的溶存甲烷 Ⅱ.浓度、海气交换通量

本文基于日本东京湾、伊势湾和浜名湖的调查资料，详细地比较了这3个海湾海水中的溶存甲烷浓度、饱和度。表层海水中，溶存甲烷浓度以供名湖最高，达95nmol／dm3，伊势湾和东京湾相近，分别为41nmol／dm3和37nmol／dm3；其表层测定浓度是其平衡浓度的13～78倍，并分别计算了这3个海湾中甲烷的海气交换通量；用平均值外推法得出全球海洋环境中总的甲烷海气交换通量为6．3Tg／a。     

海湾区海水中的溶存甲烷：Ⅱ.浓度,海气交换通量

本文基于日本东京湾，伊势湾和浜名湖的调查资料，详细地比较了这３个海湾海水中的溶存甲烷浓度，饱和度，表层海水中，溶存甲烷浓度以滨名湖最高，达９５ｎｍｏｌ／ｄｍ＾３，伊势湾和东京湾相近，分别为４１ｎｍｏｌ／ｄｍ＾３和３７ｎｍｏｌ／ｄｍ＾３；其表层测定浓度是其平衡深度的１３－７８倍，并分别计算了这３个海湾中甲烷的海气交换通量；用平均值外推法得出全球海洋环境中总的甲烷海气交换通量为６．３Ｔｇ／ｇ。     

春季东海溶存氧化亚氮的分布和海气交换通量

于2011年5至6月在东海采集不同深度海水样品,研究了其中溶存氧化亚氮(N2O)的分布并估算其海-气交换通量。结果表明,春季东海表层海水中溶存N2O浓度范围为6.31~11.88 nmol/L,平均值为(9.13±1.45)nmol/L;底层海水中N2O浓度范围为7.53~39.75 nmol/L,平均值为(13.71±7.76)nmol/L。随着深度的增加,N2O浓度逐渐升高。温度是影响春季东海N2O分布的主要因素,N2O浓度与温度呈负相关关系。长江冲淡水和黑潮水是东海N2O的重要来源。东海表层海水中N2O的饱和度范围为92.5%~139.3%,平均值为118.5%±10.3%,绝大多数站位都处于过饱和状态,因此,春季东海是大气N2O的净源。利用LM86公式和W92公式求得东海的海-气交换通量分别为(4.96±6.12)μmol/(m2·d)和(10.25±17.18)μmol/(m2·d),初步估算出东海年释放N2O通量约为0.061~0.127 Tg/a,占全球海洋释放总量的2.0%,远高于其所占的面积比0.2%。     

三亚河与三亚湾溶存N_2O分布特征与影响因素研究

2008年4月在三亚河设置24h观测连续站,10月在三亚湾设置13个采样站,同时采集大气、表层和底层海水样品,运用静态顶空气相色谱法对海水中溶存N2O的浓度进行了测定。结果表明,三亚湾海水中溶存N2O的浓度范围为7.57—15.04nmol/L,饱和度范围为101.8%—202.2%,均处于过饱和状态,明显受到三亚河水人为污染的影响;三亚河N2O浓度日变化范围在12.7—17.6nmol/L,饱和度范围在170.9%—236.9%,全天也均处于高度过饱和状态,表明三亚河和三亚湾都是大气N2O的源。对三亚河和三亚湾N2O浓度与盐度,营养盐的关系进行相关分析可得,其与盐度之间的关系为负相关,与硝酸盐,亚硝酸盐,氨盐的关系为正相关。此外还利用Liss提出的双层模型计算了三亚河和三亚湾的N2O海-气交换通量,分别为5.71—11.63μmol/(m2·d)、0.33—8.26μmol/(m2·d),表明三亚河与三亚湾水体中N2O的过饱和现象主要来源于城市污水的影响。     

春季西北太平洋水体中甲烷和氧化亚氮的分布及海气交换通量

于2010年5—6月搭乘日本KH10-1航次,对西北太平洋两个不同深度站位甲烷(CH4)和氧化亚氮(N2O)的垂直分布及海气交换通量进行了研究。结果显示:研究海域表层海水中CH4和N2O浓度分别为(2.55±0.22)nmol/L和(7.50±1.11)nmol/L,饱和度分别为126%和116%,均处于轻度过饱和状态。在垂直方向上,CH4浓度分布呈现次表层极大的特征,次表层以下CH4浓度随深度增加逐渐减小。CH4次表层极大值可能是由于细菌利用甲基化合物进行好氧产生和在悬浮颗粒物、浮游动物或其他海洋生物肠道内厌氧微环境产生的综合作用造成的。N2O浓度随深度的增加而增大,在跃层下部达到最大值,N2O与溶解氧的垂直分布呈镜像关系。水体中N2O主要通过硝化过程产生。利用LM86和W92公式计算得到CH4的海气交换通量分别为(0.76±0.57)μmol/(m2·d)和(1.57±0.67)μmol/(m2·d),N2O的海气交换通量分别为(1.96±0.24)μmol/(m2·d)和(3.08±0.38)μmol/(m2·d),因此西北太平洋是大气CH4和N2O的净源。     

夏秋季南海北部陆坡区氧化亚氮的分布、产生及海-气交换通量

分别于2014年10月和2015年6月对南海北部陆坡区进行了调查,研究了其溶存氧化亚氮(N_2O)的分布、产生并估算了其海-气交换通量。结果表明:秋季南海北部表层海水中溶解N_2O浓度为(8.19±0.79)nmol/L,饱和度为132.5%±13.4%;夏季表层海水中溶解N_2O浓度为(7.72±0.56)nmol/L,饱和度为135.5%±9.7%。夏季由于受到珠江冲淡水的影响,表层N_2O浓度随盐度升高呈降低趋势,秋季调查区域东北部受到穿过吕宋海峡的黑潮分支表层水的影响,N_2O浓度较低。结合文献资料,南海北部陆坡区表层N_2O浓度季节变化特征为春末秋季夏季,同一季节,南海陆坡区的N_2O浓度高于其他区域。温度是影响N_2O分布的重要因素,ΔN_2O与表观耗氧量(apparent oxygen utilization,AOU)和NO_3~ˉ的显著相关说明硝化作用是南海水体中N_2O产生的主要机制,由此估算硝化作用的N_2O产率分别为秋季0.033%,夏季0.035%。利用N2000和W2014公式分别估算了该区域秋季和夏季N_2O的海-气交换通量:秋季为1.81—23.81(11.11±6.52,平均值±SD,下同)(N2000)和1.73—24.38(11.30±6.81)(W2014),夏季为1.01—21.57(7.04±6.10)(N2000)和0.75—22.69(6.94±6.49)(W2014),单位均为μmol/(m~2·d)。初步估算出南海北部陆坡N_2O释放量为0.055Tg/a,约占全球海洋总释放量的0.39%,远高于其面积比,说明南海北部陆坡是N_2O释放的活跃海域,是大气N_2O的重要源。     

大亚湾海水中N2O的分布特征与通量的初步研究

2004年1月(冬季)和4月(春季)在大亚湾海域设置15个采样站,采集大气和海水样品,运用静态顶空气相色谱法测定了大气和海水中溶存N2O的浓度并对其分布特征和海-气通量进行了初步研究。结果显示,海水中N2O浓度范围在10.90—40.54 nmol.L-1,饱和度为122%—454%,处于过饱和状态;N2O浓度在湾的中部分布较为均匀,大鹏岙、核电站、范和港顶和澳头等受人类活动影响较大的沿岸浓度较高,最大值出现在龙歧河口。海-气通量为0.05—0.78μmol.(m2.d)-1。海水中N2O浓度与NH4 的含量之间有较为显著的正相关性,河口与核电站是N2O的排放源,说明人类活动影响了大亚湾海水中N2O的分布。     

桑沟湾春、秋季溶存CH4的分布及海-气交换通量

分析2013-10,2014-05和2015-05对桑沟湾3个航次的调查中采集的表、底层海水样品,研究该海域海水中溶解CH_4的分布特征及海-气交换通量。结果表明:春、秋季桑沟湾水体中CH_4浓度范围为3.0356.4nmol·L~(-1),底层浓度高于表层。由于水温的季节变化和陆源输入的影响,秋季表、底层平均CH_4浓度是春季的37倍。受养殖活动的影响,贝藻混养区表、底层CH_4均高于其他养殖区和湾外。2013-10,2014-05和2015-05桑沟湾表层海水CH_4的平均饱和度分别为(2 704±2 532)%,(330±276)%和(858±417)%,表现为秋季高于春季。根据W2014公式估算出桑沟湾春、秋季表层海水CH_4海-气交换通量范围为3.919.9μmol·m~(-2)·d~(-1),根据N2000公式估算出春、秋季表层海水CH_4海-气交换通量范围为5.520.6μmol·m~(-2)·d~(-1),表明春、秋季桑沟湾是大气CH_4的源区。     

桑沟湾溶存N2O的分布和海气交换通量的季节变化

于2006年4月至2007年1月对桑沟湾海域进行了4个航次的调查,采集表层海水样品,研究了该海域表层海水中溶解N_2O的分布特征及海气交换通量的季节变化,结果表明:桑沟湾表层海水中溶解N_2O浓度和饱和度存在一定的季节性变化,浓度表现为冬季最高而饱和度为夏季最高.利用Liss和Merlivat公式(LM86)以及Wanninkhof公式(W92)估算了该海湾海水中N_2O的年平均海-气交换通量,分别为0.2 μmol/(m~2·d)±0.1 μmol/(m~2·d)和1.5 μmol/(m~2·d)±1.0 μmol/(m~2·d).     

胶州湾海水甲烷氧化速率的水平与垂直变化初步研究

系统考察2014年4月胶州湾海水中甲烷的氧化速率。通过一系列的海水培养实验,采用气相—稳定同位素比值质谱仪(GC-IRMS)追踪了培养样品中δ13 CH4的变化,计算了胶州湾海水的甲烷氧化速率(MOX)。结果表明:胶州湾表层水中甲烷的氧化速率的变化范围为3.7~255.5nmol·L~(-1)·d~(-1),平均值为(104.7±89.7)nmol·L~(-1)·d~(-1)。底层水中甲烷的氧化速率的变化范围为38.2~227.1nmol·L~(-1)·d~(-1),平均值为(148.9±76.2)nmol·L~(-1)·d~(-1)。总体而言,在胶州湾东部和西部,特别是海泊河口、洋河河口附近的水域,表层海水中甲烷氧化速率的分布都明显呈现出近岸高,远岸低的趋势。胶州湾甲烷的氧化速率与溶解无机碳浓度的变化以及甲酸的含量呈较明显的线性正相关。根据甲烷氧化速率估算出胶州湾氧化甲烷的量为1.15×108 mol/a,该值相当于胶州湾甲烷海-气通量的6.4~14.3倍。     

The distribution of methane in the Tokyo-wan

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The influence of coupling mode of methane leakage and debris input on anaerobic oxidation of methane

Anaerobic oxidation of methane(AOM) is an important biogeochemical process, which has important scientific significance for global climate change and atmospheric evolution. This research examined the δ~(34)S, terrigenous clastic indices of TiO_2 and Al_2O_3, and times for formation of the Ba front at site SH1, site SH3 and site 973-4 in the South China Sea. Three different coupling mechanisms of deposition rate and methane flux were discovered. The different coupling mechanisms had different effects on the role of AOM. At site 973-4, a high deposition rate caused a rapid vertical downward migration of the sulphate–methane transition zone(SMTZ), and the higher input resulted in mineral dissolution. At site SH3, the deposition rate and methane flux were basically in balance,so the SMTZ and paleo-SMTZ were the most stable of any site, and these were in a slow process of migration. At site SH1, the methane flux dominated the coupled mode, so the movement of the SMTZ at site SH1 was consistent with the general understanding. Understanding the factors influencing the SMTZ is important for understanding the early diagenesis process.     

The global importance and context of methane escape from the seabed

Seabed fluid flow includes volcanic and hydrothermal fluid emissions from ocean spreading centres, island arcs, and intra-plate volcanism, and groundwater flows in some coastal areas. Of direct concern to this paper is the escape of methane from the seabed. Escaping methane may be of microbial, thermogenic or abiogenic origin. Escapes occur in all seas and oceans, in coastal waters, on continental shelves, slopes and rises, the deep oceans, and deep ocean trenches. These represent a variety of geological contexts on passive continental margins, at convergent plate margins (accretionary wedges) and transform plate boundaries. Seepage is clearly widespread, and it contributes methane to the biosphere, the hydrosphere and the atmosphere, thus making up an important part of the global carbon cycle.     

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.     

Estimating the global flux of methane into the atmosphere and its seasonal variations

A new method of estimating the global fluxes of methane into the Earth’s atmosphere is proposed. This method allows one to take into account the whole spectrum of methane sources irrespectively of their location and calculate seasonal variations in methane fluxes. The results of numerical calculations of the amount of methane emitted into the atmosphere on the basis of this method are supported by data obtained from field measurements. In the Northern Hemisphere (NH), during fall, maximum concentrations of CH₄ are due to methane sources in the arctic region which have not been taken into account before. For the condition of balance between the emission and sink of methane to be fulfilled, the total capacity of its sources amounts to no less than ～530 Tg/year for the NH and ～470 Tg/year for the Southern Hemisphere (SH). The results of our calculations and an analysis of the behavior of the concentration and mass of methane in the Earth’s hemispheres show that the global flux of methane from the surfaces of the lithosphere and ocean into the atmosphere may amount to more than ～1000 Tg/year.     

Meio-epifaunal wood colonization in the vicinity of methane seeps

In deep-sea environments, plant remains of several origins are found, including branches, twigs, leaves, and wood pieces, among others. As most of the deep-sea bottoms are oligotrophic and nutrient-limited, plant remains provide an oasis of localized organic enrichment and a substrate for colonization. Sunken wood was suggested to play an important evolutionary role in the diversification of chemosynthetic ecosystems, possibly representing stepping stones for the colonization between vent and seep ecosystems. In order to understand colonization processes of the Pacific Costa Rican meio-epifaunal assemblages associated with sunken wood, a field experiment was conducted on Mound 12 (8°55.778′N, 84°18.730′W) at ~1,000 m water depth. Woodblocks were placed in four different habitats (Mussel beds, tube worms, near mussel beds, rubble bottoms), and different local environmental conditions (seepage-active and seepage-inactive sites). Seven experimental Douglas fir woodblocks (each 1,047 cm² in surface area) were deployed from the R/V Atlantis using the manned submersible Alvin in February 2009 and recovered after 10.5 months in January 2010. Sample processing and analyses led to a data set of abundance (total 9,951 individuals) and spatial distribution of nine meio-epifaunal higher taxa/groups. Meio-epifaunal densities on individual woodblocks ranged from 3 to 26 ind.10 cm². Copepods accounted for the highest abundances (75.1%), followed by nauplii larvae (11.7%) and nematodes (9.8%). The maximum number of individuals (26.3 ind.10 cm⁻²) was found in blocks placed in seepage-inactive areas (near active mussel beds) in contrast to 2.9 ind.10 cm⁻² in active areas (within a mussel bed). A hierarchical cluster analysis grouped blocks according to seepage activity and not to habitat, but tests of similarity showed no significant differences in higher taxon composition and abundances, probably owing either to substrate homogeneity or low sample size. Copepods were the most abundant representatives, suggesting that this group is one of the most successful in colonizing in the early stage of succession, in this case while hardwood substrates are not yet decomposed or bored by bivalves.     

真光层海水过饱和甲烷的来源及机制探讨

真光层海水中普遍存在甲烷过饱和现象,尤其是天然气水合物区真光层的甲烷明显异常。由于临近海气界面,真光层过饱和甲烷与大气甲烷排放及全球温室效应密切相关。目前,对真光层海水的过饱和甲烷来源仍没有统一的认识。综合前人研究成果梳理了真光层海水过饱和甲烷的来源,归纳了真光层海水过饱和甲烷现象形成的影响因素,进一步探讨了原位微生物可能参与的甲烷代谢机制。真光层过饱和甲烷可能来源于沉积物、临近河流或原位微生物,且受区域、季节、营养盐等多种因素的影响。由于受氧气影响,真光层海水甲烷产生的代谢机制有其特殊性,目前推测微生物可能依旧利用常规的产甲烷途径,它们存在于海水微厌氧环境中,或自身形成抵抗氧气影响的能力;此外,微生物也可能选择对氧不敏感的新的产甲烷途径。因此,针对天然气水合物区真光层甲烷过饱和现象,开展甲烷的来源和代谢机制的研究,以期为天然气水合物试采与开发的环境评价提供理论支撑,并为探究海水甲烷对大气及全球气候的影响提供理论依据。     

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.     

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。