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Coupled carbon and sulfur isotope behaviors and other geochemical perspectives into marine methane seepage
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Lihua LIU1, *, Shaoying FU2, Mei ZHANG1, Hongxiang GUAN1, Nengyou WU3, 4
Acta Oceanologica Sinica | 2017, 36(6) : 12 - 22
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Acta Oceanologica Sinica | 2017, 36(6): 12-22
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Coupled carbon and sulfur isotope behaviors and other geochemical perspectives into marine methane seepage
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Lihua LIU1, *, Shaoying FU2, Mei ZHANG1, Hongxiang GUAN1, Nengyou WU3, 4
Affiliations
  • 1 Key Laboratory of Gas Hydrate, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China
  • 2 Guangzhou Marine Geological Survey, Guangzhou 510760, China
  • 3 The Key Laboratory of Gas Hydrate of Ministry of Land and Resources, Qingdao Institute of Marine Geology, Qingdao 266071, China
  • 4 Laboratory for Marine Mineral Resources, Qingdao National Laboratory for Marine Science and Technology, Qingdao 266071, China
Published: 2017-06-01 doi: 10.1007/s13131-017-0998-y
Outline
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Methane seepage is the signal of the deep hydrocarbon reservoir. The determination of seepage is significant to the exploration of petroleum, gas and gas hydrate. The seepage habits microbial and macrofaunal life which is fueled by the hydrocarbons, the metabolic byproducts facilitate the precipitation of authigenic minerals. The study of methane seepage is also important to understand the oceanographic condition and local ecosystem. The seepage could be active or quiescent at different times. The geophysical surveys and the geochemical determinations reveal the existence of seepage. Among these methods, only geochemical determination could expose message of the dormant seepages. The active seepage demonstrates high porewater methane concentration with rapid SO42– depleted, low H2S and dissolved inorganic carbon (DIC), higher rates of sulfate reduction (SR) and anaerobic oxidation of methane (AOM). The quiescent seepage typically develops authigenic carbonates with specific biomarkers, with extremely depleted 13C in gas, DIC and carbonates and with enriched 34S sulfate and depleted 34S pyrite. The origin of methane, minerals precipitation, the scenario of seepage and the possible method of immigration could be determined by the integration of solutes concentration, mineral composition and isotopic fractionation of carbon, sulfur. Numerical models with the integrated results provide useful insight into the nature and intensity of methane seepage occurring in the sediment and paleo-oceanographic conditions. Unfortunately, the intensive investigation of a specific area with dormant seep is still limit. Most seepage and modeling studies are site-specific and little attempt has been made to extrapolate the results to larger scales. Further research is thus needed to foster our understanding of the methane seepage.

marine seepage  /  authigenic minerals  /  carbon isotopes  /  sulfur isotopes  /  numerical simulation
Lihua LIU, Shaoying FU, Mei ZHANG, Hongxiang GUAN, Nengyou WU. Coupled carbon and sulfur isotope behaviors and other geochemical perspectives into marine methane seepage[J]. Acta Oceanologica Sinica, 2017 , 36 (6) : 12 -22 . DOI: 10.1007/s13131-017-0998-y
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1 Introduction of marine methane seepage
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Marine seepage is formed by the release of deep pressurized pore fluids and considered to be a signal pointing directly to deep hydrocarbon reservoirs. Seep occurs at nm to 3 000 m depth of between a few meters and several kilometers. Escaped gaseous and aqueous hydrocarbons mostly methane supports overlain microbial communities. The metabolic byproducts of microorganisms facilitate the precipitation of authigenic minerals, the minerals provide solid substrates for habitation of macrofaunal organisms (Formolo and Lyons, 2013; Grupe et al., 2015). The macrofaunal activities enhance solute transport and influence the redox zonation of sediments through irrigation and geochemical reactions (Hutchens et al., 2010; Meile et al., 2001). The upwelling flow, the micro- and macro-communities and the solid minerals form a unique ecosystem of methane seepage. This ecosystem and the biogeochemical relationships drive the cycling of carbon, sulfur and other elements. The investigation of seepage is thus an elegant approach to study the local element cycle, to trace the paleoceanographic conditions and guide offshore exploration for hydrocarbon deposits (Judd et al., 2002).
Methane seeps occur where the overpressured fluids rise to the sediment surface through cracks and fissures accompanied sometimes by visible evidences. The most obvious evidence is gas flares. The flares could be identified by observation and multi-beam sonar system (Hovland et al., 2012; Jensen et al., 2002; Judd et al., 2002; Martens et al., 1999). Pockmarks and mud volcanos is another identification (Hovland et al., 2012; Nelson et al., 1979) and could be recognized by the high-resolution multi-beam systems and echo sounder electro-magnetic methods (Hovland et al., 2012; Judd et al., 2002; Röemer et al., 2012; Talukder et al., 2013). Microbial mats, seep-related chemosynthetic animals and authigenic minerals are also visible signals of seeps (Barry et al., 1997; Boetius and Suess, 2004; Feng et al., 2015; Hovland et al., 2012; Joye et al., 2010; Knittel et al., 2005). Above visual quantifications could be revealed by remotely operated vehicle (ROV), by seismic and hydroacoustic surveys (Regnier et al., 2011; Röemer et al., 2012; Talukder et al., 2013).
Worldwide scientists have investigated prospective areas of methane seeps during the past decades (Foucher et al., 2009; Han et al., 2013; Paull et al., 2008; Rollet et al., 2006; Yin et al., 2003). The investigation suggests that methane seeps have been reported from (1) every see and ocean; (2) a broad range of oceanographic settings from the coast to the deep ocean; (3) a wide variety of geological environments (Judd, 2003).
2 Geochemical properties of marine methane seepage
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Geochemical properties indicate the seepage especially suitable for the dormant and ancient seepage. High concentrations of methane, even higher than saturated concentration have been determined in many seeping areas (Archer, 2007; Huang et al., 2008; Lim et al., 2011). The high concentration fuels the geochemical reactions and accompanied by a specific isotopic distribution. The coupled processes of geochemical reactions and microorganism activities form the metabolic foundation of marine seeps. The seeps could be revealed by the composition of minerals, the distribution of solutes and isotopic fractionations of elements (Joye et al., 2010; Treude et al., 2007). Dormant or ancient seepage may only be delineated by geochemical signals, e.g., authigenic mineral, solutes distribution, ionic and stable isotopic composition (Bayon et al., 2007; Cook et al., 2011; Feng and Chen, 2015; Han et al., 2008; Malone et al., 2002; van Dongen et al., 2007).
2.1 Authigenic minerals
The presence of authigenic minerals and mineral aggregates indicates a high upwelling flux and the active of microorganism. Among the authigenic minerals, carbonate is the commonest one and has been well investigated (Bouloubassi et al., 2006; Gieskes et al., 2005; Greinert et al., 2002; Luff et al., 2005). The carbonates are mainly aragonite, Mg-calcite and (proto)-dolomite, also Fe- and Mn-carbonates (Haas et al., 2010; Han et al., 2008). Various carbonates appear under different geochemical conditions and the formation of carbonates is mediated by the activities of microorganism (Han et al., 2014; Liebetrau et al., 2014). Other authigenic minerals, e.g., pyrite (FeS2), gypsum (CaSO4·2H2O), barite (BaSO4) and greigite (Fe3S4) have also been reported (Greinert et al., 2001; Joye et al., 2010; Lin et al., 2016a, c ; Peckmann et al., 2001; Sassen et al., 2004; van Dongen et al., 2007; Vanneste et al., 2013). The association of carbonates with gas emissions and populations of chemosynthetic faunas has been a widely used criterion to identify the hydrocarbon seeps (Feng and Chen, 2015; Feng et al., 2015; Suess, 2014).
2.2 Distribution of solutes in interstitial water
The distribution of solutes in interstitial water may directly point the seepage. Methane seepages typically harbor communities of micro- and macro-organism, which mediates the anaerobic oxidation of methane (AOM) to produce HCO3– and HS–. HCO3– is the main part of dissolved inorganic carbon (DIC=[CO32–]+[HCO3–]+[CO2]+[H2CO3]) which could precipitate with metallic ion as carbonate. In the active seep site, porewater CH4 and dissolved organic carbon (DOC) concentrations are thus high with significant NH4+, rapid SO42– depleted, low H2S and DIC, higher rates of sulfate reduction (SR) and AOM (Knittel and Boetius, 2009; Treude et al., 2005). The high rates of methaneogenesis are associated with either abundant natural gas or deep hydrocarbon reservoir. The high methanotrophic rate is accompanied by the high DIC and the recrystallization of carbonates (Boetius et al., 2000; Knittel and Boetius, 2009). The depth of sulfate-methane reaction zone reveals the intensity of upwelling flux (Chuang et al., 2013; Lin et al., 2016c; Luff and Wallmann, 2003). For the inactive or quiescent seepages the distribution of solutes provide limit signal with the geological time (Haeckel et al., 2004). Only carbonate and isotopic fractionations of elements preserve more messages (Ge et al., 2015; Novikova et al., 2015). Some models have been used to quantitatively describe the seepage and the model work will be introduced below (Liu et al., 2016a; Luff et al., 2004; Wallmann et al., 2006).
2.3 Stable isotopic fractionation
The stable isotopes and biomarkers have been the advanced criteria for recognizing ancient seeps (Bohrmann et al., 1998; Feng et al., 2015; Formolo and Lyons, 2013; Gieskes et al., 2005; Hu et al., 2015; Lin et al., 2016c; Lu et al., 2015; Sivan et al., 2007). The fractionation of element isotopes during uptake and metabolism of methanogens and methanotrophy is controlled primarily by the source material and kinetic isotope effects (Feng et al., 2015; Novikova et al., 2015; Whiticar, 1999).
2.3.1 Stable isotope of carbon
(1) Methane gas
Except for methane, hydrogen sulfide and carbon dioxide has been determined in headspace (Himmler et al., 2015; Joye et al., 2010; Kastner et al., 1998; Malone et al., 2002; Suess, 2005). However, only a few sites reported isotopic composition of methane and hydrogen sulfide. The reported gaseous δ13C were listed in Tables 1 and 2 (for sulfide) and marked in Figs 1 and 2 (for sulfide).
Biogenic methane gas commonly shows an extremely negative δ13C value of –110‰ to –50‰ and the thermogenic methane is generally, but not exclusively, enriched in 13C (>–50‰), the mixture located in the transition region (Joye et al., 2010; Whiticar, 1999).
(2) Dissolved inorganic carbon (DIC)
The δ13C in DIC has been widely investigated. The values were listed in Table 1 and shown in Fig. 1. Normal δ13CDIC value of ocean water is around 2‰ (Faure, 1986). The anaerobic oxidation of methane with medium of microorganism will obtain low δ13C of around –20‰ to –50‰ (Hu et al., 2015; Kastner et al., 1998; Lin et al., 2001; Malone et al., 2002; Martens et al., 1999; Roalkvam et al., 2011). Generally, δ13C values of DIC are higher than gaseous methane in a certain sites since the lightest fraction could preferentially escape to gaseous or react.
However, in the inactive seepages, both the distribution of solutes and the isotopic data provide limit message, further information have to recur the signature of solid carbonates.
(3) Authigenic carbonate
A direct consequence of methane consumption is the precipitation of carbonates with depleted 13C (Grupe et al., 2015; Magalhães et al., 2012). The values in remnant bacterial mats could be –81.6‰ (Novikova et al., 2015). Some δ13C of the carbonates are listed in Table 1. Most seepage carbonates show a higher δ13C than gaseous methane and similar to that of DIC (Aloisi et al., 2004; Berndt et al., 2014; Cook et al., 2011; Feng and Chen, 2015; Formolo and Lyons, 2013; Formolo et al., 2004; Himmler et al., 2015; Malone et al., 2002; Treude et al., 2005; Wang et al., 2013). This scheme may be due to the fractionation during evaporation and metabolism. Cold-seep carbonates are characterized by a negative δ13C value, most are between 0‰ to –40‰ or even lower (Tong et al., 2013), and the lowest one was –61‰ in the Southwest African continental margin (Grupe et al., 2015). This value clearly indicates the methane derived carbonates. A high value of 0‰–29‰ was determined in a down core profile in a pockmark area of Niger Delta (Bayon et al., 2007) which could be a geothermal or non-methane driven source.
(4) Biomarkers
Abundant fossilized microbes are preserved in seep carbonates (Cook et al., 2011; Elvert et al., 2000; Guan et al., 2016; Han et al., 2008; Peckmann and Thiel, 2004). Fossilized biomarkers could be extracted with distinctive carbonate fabrics and stable isotope signatures. The extractants could reveal the biogeochemical route and environmental conditions of ancient seep sites. The oldest biomarker recorded in the 300-million-year-old limestone (Birgel et al., 2008; Suess, 2014). The characteristic biomarkers in ancient seep environments are 13C-depleted archaeal isoprenoids, linear and methyl-branched carbon skeletons and hopanoids of bacterial origin (Peckmann and Thiel, 2004). Beyond above species, a wide range of biomarkers, including fatty acids, isoprenoidal and non-isoprenoidal ether lipids and hopanoids have also been determined in cold seeps (Pancost et al., 2001; Schouten et al., 1998; Stadnitskaia et al., 2003, 2005; van Dongen et al., 2007). Above biomarkers are greatly depleted 13C (–40‰ to –140‰), the lightest could be lower than –140.8‰ in a cold seep from the northern South China Sea (Ge et al., 2015). A high value of 32‰ for n-alkanes from iron sulfide nodules (saturated hydrocarbon) could be due to the non-methane source. However, extreme variability over narrow spatial and temporal scales within short distances (m) is common for active and dormant seeps (Formolo and Lyons, 2013; Li et al., 2007).
2.3.2 Stable isotope of sulfur
Isotopic fractionation of sulfur suggests the existence and evolution of seepage because both the degradation of organic carbon and AOM are accompanied by microbial sulfate reduction (Boudreau, 1996; Lin et al., 2016a, b ; Luff et al., 2000). Microorganisms have long been known to fractionate isotopes during their sulfur metabolism. Both 34S and 18O which will be introduced next have been used as indicators of the origin and geochemical routine of seep site (Aharon and Fu, 2000, 2003; Faure, 1986; Feng et al., 2015; Formolo and Lyons, 2013; Kastner et al., 1998).
Some of the published δ34S values were listed in Table 2 and Fig. 2. A few values reported gaseous sulfur and hydrogen sulfide and substantial liquid phase, and sulfate in porewater. The extreme high or low value of isotopic fraction appears in the reactive area which indicates the seepage. The range of gaseous hydrogen sulfide was –20‰ to 25‰ depending on the local formation, sulfur source and metabolic processes. Most dissolved sulfate in pore water have δ34S value similar to seawater which is about 20‰ and the maximum could be 70.8‰ in the intensive sulfate reduction area in the Gulf of Mexico (Aharon and Fu, 2003). Pyrite, typically occurring as a framboidal crystal aggregate is the most common non-carbonate mineral in methane seep (Lin et al., 2016b; Peckmann and Thiel, 2004) another one is gypsum (Lin et al., 2016a). Figure 2 and Table 2 show clearly that δ34Spyrite cover a broad range of 47‰ to –45‰ (Lin et al., 2016a; Peckmann and Thiel, 2004) which indicated the complex source and synthesis of pyrite. Most solid phase including pyrite, total reduced inorganic sulfur and acid volatile sulfur. Elemental sulfur obtained light sulfur mainly around 0‰ to –20‰. However, the different among various solid phases is only the extraction method. The mechanism of the formation and fractionation is still unclear, further research is needed.
2.3.3 Stable isotope of oxygen
The δ18O values were reported for carbonate, gypsum, sulfate and interstitial water samples. The determination of 18O in seepage is limit and scattered, the data are listed in Table 3 (Aharon and Fu, 2000; Aharon et al., 1992; Davidson et al., 1978; Faure, 1986; Feng and Chen, 2015; Himmler et al., 2015; Kastner et al., 1998; Malone et al., 2002; Matsumoto, 2000; Novikova et al., 2015; Tong et al., 2013). Most carbonate δ18O lies between 0‰–10‰, only the cold seep area in the Gulf of Mexico shows a high value of 35.33‰ (Formolo et al., 2004). One reported δ18O in gypsum was 5.3‰–12.3‰ in the Shenhu Area, SCS (Lin et al., 2016c). The mineralogy of the authigenic minerals and the source of fluid is probably the main influence on the δ18O (Cook et al., 2011). Two interstitial water samples were around zero, and the samples in active area showed a higher level. The high level could be more than 20‰ which may due to the lighter portion preferentially enter the gaseous phase (Aharon and Fu, 2000).
3 Episodes of methane seepage
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The methane seepage in one site may spurt several times over geologic time. Several layers of methane-derived carbonates are direct evidence of the episode (Magalhães et al., 2012). The episode could be determined by the age of carbonates and paleo-environmental condition. The seep carbonates with a series of consecutive U/Th dating has been reported in the northern South China Sea which established the periods of seep events (Feng and Chen, 2015; Han et al., 2014). Different lithologic groups evidenced the extensive episodes (Magalhães et al., 2012) and the fluctuation of depleted δ13C record several leaching events during glacial intervals (Hyun et al., 2014). If the sulfate methane transition zone is deep in the seafloor, the authigenic carbonates formed much older than the episode of methane flux (Cook et al., 2011; Novikova et al., 2015). Periodic, catastrophic release of stored methane in gas hydrates implicated also climate change scenarios (Dickens et al., 1995; Hyun et al., 2014; Ménot and Bard, 2010). However, the seep activity is also affected by tidal, sea level, climate change and orbital. Detailed investigation is needed to identify the episode and causes of seepage.
4 Numerical simulation of the seepage
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Simulation tools have greatly improved our quantitative understanding of seepage and help us to reconstruct the environmental conditions in marine sediments. The processes from methaneogenesis to methantrophy have been extensively modeled (Aloisi et al., 2004; Arning et al., 2011; Meysman et al., 2003; Reed et al., 2011; Scholz et al., 2011). The benthic fluxes of dissolved inorganic carbon (DIC) and alkalinity (TA) and carbonate deposition has been estimated from coastal sediments (Boudreau, 1996; Krumins et al., 2013; Luff et al., 2000, 2005). Currently simulations could define the path of geochemical reactions and mineralization and evaluate the kinetic reaction rate (Liu et al., 2016b). However, the knowledge about the episode and the cycle of seepage is still limit and further research is necessary.
5 Conclusions
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For the exploration of hydrocarbon reservoir, the investigation of seepage is an elegant method. The study of seepage contributes also to the reconstruction of paleoceanographic and environmental conditions. During the past decades, we got some knowledge about methane source, methane reaction, consumption and the episodes of seep. Generally, the survey of seepage starts from the geophysical reconnaissance to the geochemical determination. The geochemical determination, e.g., methane gas, DIC, carbonates and biomarkers could be used to evaluate the geological background, the geochemical reactions and the mechanism of compound immigration. The seepage could be active or dormant and the geochemical prospection is a suitable approach especially for the dormant seepage. Unfortunately, it is impossible to determine the source neither the transport mechanism with one element isotopic ratio or one phase distribution. The combination of carbon, sulfur and oxygen isotope behaviors with other geochemical determination is always necessary. With the integrated field and geochemical determination, model could quantitatively describe the kinetic reactions, the formation of minerals and the flux of seepage. Eventually we may better understand the system, predicate the leaching events and access the climate effect of methane seepage. However, the intensive investigation of a specific area for methane seepage, especially for dormant seep is still limit. Most seepage investigation tends nevertheless to be site-specific since the geological formations are highly variable even between two adjacent cores separated by less than a meter, and little attempt has been made to extrapolate the results to larger scales. Further research is thus needed to foster our understanding of the methane seepage.
Funding
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  • The National Natural Science Foundation of China under contract No. 41376076; the Natural Science Foundation of Guangdong Province under contract No. 2015A030313718; the Scientific Cooperative Project by China National Petroleum Corporation and Chinese Academy of Sciences under contract No. 2015A-4813; the National Marine Geological Project, China Geological Survey under contract No. GZH2012006003.
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Appendix
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doi: 10.1007/s13131-017-0998-y
  • Receive Date：2016-04-12
  • Online Date：2026-04-14
  • Published：2017-06-01
Article Data
Affiliations
History
  • Received：2016-04-12
  • Accepted：2016-09-27
Funding
The National Natural Science Foundation of China under contract No. 41376076; the Natural Science Foundation of Guangdong Province under contract No. 2015A030313718; the Scientific Cooperative Project by China National Petroleum Corporation and Chinese Academy of Sciences under contract No. 2015A-4813; the National Marine Geological Project, China Geological Survey under contract No. GZH2012006003.
Affiliations
    1 Key Laboratory of Gas Hydrate, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China
    2 Guangzhou Marine Geological Survey, Guangzhou 510760, China
    3 The Key Laboratory of Gas Hydrate of Ministry of Land and Resources, Qingdao Institute of Marine Geology, Qingdao 266071, China
    4 Laboratory for Marine Mineral Resources, Qingdao National Laboratory for Marine Science and Technology, Qingdao 266071, China

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表12种不同金属材料的力学参数
科
Family		 属数
Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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