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Coupled carbon and sulfur isotope behaviors and other geochemical perspectives into marine methane seepage

Acta Oceanologica Sinica 2017年第6期36卷 12-22页

作者： LIU Lihua FU Shaoying ZHANG Mei guan hongxiang WU Nengyou Key Laboratory of Gas Hydrate Guangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou 510640China guangzhou Marine Geological Survey Guangzhou 510760China The Key Laboratory of Gas Hydrate of Ministry of Land and Resources Qingdao Institute of Marine GeologyQingdao 266071China Laboratory for Marine Mineral Resources Qingdao National Laboratory for Marine Science and TechnologyQingdao 266071China

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 HaS 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.

关键词： marine seepage authigenic minerals carbon isotopes sulfur isotopes numerical simulation

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Detection and indication of 1,3,4-C27-29 triol in the sediment of northern South China Sea

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Science China Earth Sciences 2016年第6期59卷 1187-1194页

作者： ZHU XiaoWei MAO ShengYi WU NengYou JIA GuoDong SUN YongGe guan hongxiang WU DaiDai Key Laboratory of Marginal Sea Geology South China Sea Institute of OceanologyCASGuangzhou 510301China Key Laboratory of Marginal Sea Geology Guangzhou Institute of GeochemistryCASGuangzhou 510640China Key Laboratory of Gas Hydrate Guangzhou Institute of Energy ConversionCASGuangzhou 510640China Department ofGeosciences Zhejiang UniversityHangzhou 310037China guangzhou Center for Gas Hydrate Research CASGuangzhou 510640China

After the detection of the 1,20,21-C29 long-chain triol in some sediments and freshwater pteridophytes, in this study a new homologous long-chain triol, 1,3,4-C27-29, is detected for the first time in the Site4B core sediment in the northern South China Sea. The hydroxyl location and length of the carbon chain of this newly discovered triol differ from those of 1,20,21-C29 triol. The test results of its molecular distribution and individual carbon isotope reveal that 1,3,4-C29triol has a good correlation with n-C26-30 even carbon-numbered long-chain fatty alcohols, with R2 （n=68） values of 0.905, 0.929 and 0.903, respectively, and its carbon isotope composition, at -32.3%o_1.9%o, is similar to that of rt-C26.30, at -29.13%o^0.87%o, -32.98%o^1.28%o, and -32.98%o^1.28%o. 1,3,4-C29 triol from the Site4B core sediment and terrigenous long-chain fatty alcohol （n-C26.34） show highly consistent distribution trends in the entire section; thus, the former could serve as a proxy indicator of the terrigenous input. Considering that the 1,20,21-C29 triol in previous research belongs to Azolla, which are fresh water pteridophytes, the 1,3,4-C27-29 triol identified in this study might have similar biogenetic derivation. Thus, determination of its biogenic area and growing environment could provide potential organic geochemical evidence supporting the terrigenous input and source in the northern South China Sea.

关键词： Long-chain triol Northern South China Sea Terrigenous input

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Lipid Biomarkers and Their Stable Carbon Isotopes in Ancient Seep Carbonates from SW Taiwan, China

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Acta Geologica Sinica(English Edition) 2019年第1期93卷 167-174页

作者： guan hongxiang XU Lanfang WANG Qinxian CHEN Duofu WU Nengyou MAO Shengyi Key Laboratory of Gas Hydrate Guangzhou Institute of Energy Conversion Chinese Academy of Sciences Laboratory for Marine Mineral Resources Qingdao National Laboratory for Marine Science and Technology University of Chinese Academy of Sciences Shanghai Engineering Research Center of Hadal Science and Technology College of Marine Sciences Shanghai Ocean University

Four massive brecciated, chimney-like, and slender pipe network carbonate samples(JA-4, JA-5, JX-8 and BG-12) were collected from southwestern Taiwan, which were suggested to have formed as a result of anaerobic oxidization of methane(AOM). Considering that the environmental conditions of the carbonates precipitation and the sources of carbon and organic matter need to be further declared, molecular fossils and compound-specific carbon isotopic investigations of the carbonates were conducted in this study. According to lipid biomarkers of 2,6,10,15,19-pentamethyleicosane(PMI) and squalane diagnostic to methanotrophic archaea, as well as the extremely low δ^(13)C values(as low as -1^(13).4‰) detected in samples JA-4, JA-5 and JX-8, these carbonates were revealed to be a result of AOM. Based on the varied δ^(13)C values of characteristic archaea biomarkers in specific samples, biogenic methane was proposed to be responsible for the formation of samples JA-4 and JA-5, whereas a mixed carbon source of ^(13)C-depleted methane and ^(13)C-enriched residual CO_2 from methanogenesis was suggested for the carbonate of JX-8 due to the co-occurrence of a highly positive δ^(13) C_(carb) value(+8‰) and a moderate ^(13)C depletion of PMI. The low content of AOM-related biomarkers and the absence of indicators for ANME-2 suggested that these carbonates were formed in weak seep settings. By comparison, no typical lipid biomarkers for methanotrophic archaea was detected in carbonate BG-12. The short-chain and long-chain n-alkanes accounted for 30% and 45% of all hydrocarbons, respectively, with a CPI value of 1.2, suggesting that the n-alkanes were derived from both marine organisms and terrestrial inputs. A low thermal maturity could be revealed by the incomplete equilibrium value of the C^(31)αβ 22S/(22S+22R) ratio(0.5), and the carbonate BG-12 was probably deposited in a suboxic condition indicated by a value of Pr/Ph ratio(2.5).

关键词： methane seeps lipid biomarkers anaerobic oxidation of methane weak seep settings

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Alcohol compounds in Azolla imbricata and potential source implication for marine sediments

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Science China Earth Sciences 2017年第2期60卷 348-359页

作者： MAO ShengYi ZHU XiaoWei WU NengYou JIA GuoDong SUN YongGe guan hongxiang WU DaiDai Key Laboratory of Gas Hydrate Guangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou 510640China Key Laboratory of Marginal Sea Geology South China Sea Institute of OceanologyChinese Academy of SciencesGuangzhou 510301China The Key Laboratory of Gas Hydrate Ministry of Land andResourcesQingdao Institute of Marine GeologyQingdao 266071China School of Ocean and Earth Sciences Tongji UniversityShanghai 200092China Department of Geosciences Zhejiang UniversityHangzhou 310037China guangzhou Center for Gas Hydrate Research Chinese Academy of SciencesGuangzhou 510640China

This study investigated the composition of long-chain alkyl diols, triols, sec-alcohols, hydroxyl acids, and other hydroxylated compounds in Azolla imbricata and compared the organic alcohol components of Azolla filiculoides, Azolla microphylla, and South China Sea （SCS） sediments in order to investigate the possible indication of Azolla being the biological source of diols and triols in SCS sediment. Large amounts of diols, monohydroxy acids, and sec-alcohols with internal hydroxy groups at ω20 were detected in the three types of Azolla. Among these, 1,ω20-diol and ω20-hydroxy acid exhibited strong even-odd predominance distribution, whereas co20-sec-alcohol exhibited strong odd-even predominance distribution. In addition, small amounts of diols, triols, and dihydroxy acids with internal hydroxy groups at 9, 10 or ω9, ω 10 were detected, among which the chain length of C29 was predominate. Compounds having similar structures as those in Azolla reflected a similar biosynthetic pathway： ω20-hydroxy acid exhibiting even-odd predominance distribution is decarboxylated to ω20-sec-alcohol exhibiting odd-even predominance distribution and converted to 1, ω20-diol with even-odd predominance distribution by acyl reduction; ω9,ω10-hydroxy acid is converted to 1,20,21（1, ω9, ω10）-triol by acyl reduction, and then converted to 9,10-diol by hydrogenation and dehydration. The alcohol components in A. imbricata were clearly not the biological source of 1,13/1,14/1,15-C28, 30, 32 diols and 1,3,4-C27.29 triols in the SCS sediment. Certain marine diatoms might be the source of 1,14-C28.30 diol in inshore sediment, but the biological source of diols and triols in the SCS sediment requires further investigation.

关键词： A. imbricata Long-chain alkyl diols Long-chain alkyl triols Hydroxy acids SCS sediment

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Methane seepage intensities traced by sulfur isotopes of pyrite and gypsum in sediment from the Shenhu area,South China Sea

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Acta Oceanologica Sinica 2018年第7期37卷 20-27页

作者： ZHANG Mei LU Hongfeng guan hongxiang LIU Lihua WU Daidai WU Nengyou Key Laboratory of Gas Hydrate Guangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou 510640China guangzhou Marine Geological Survey Guangzhou 510760China Laboratory for Marine Mineral Resources Qingdao National Laboratory for Marine Science and TechnologyQingdao 266061China Key Laboratory of Gas Hydrate Qingdao Institute of Marine GeologyMinistry of Land and ResourcesQingdao 266071China

The northern slope of the South China Sea is a gas-hydrate-bearing region related to a high deposition rate of organic-rich sediments co-occurring with intense methanogenesis in subseafloor *** oxidation of methane（AOM） coupled with bacterial sulfate reduction results in the precipitation of solid phase minerals in seepage sediment,including pyrite and *** aggregates of pyrites and gypsums are observed between the depth of 667 and 850 cm below the seafloor（cmbsf） in the entire core sediment of HS328 from the northern South China *** pyrites are tubes consisting of framboidal cores and outer *** aggregates occur as rosettes and spheroids consisting of *** of them grow over pyrite,indicating that gypsum precipitation postdates pyrite *** sulfur isotopic values（δ^34 S） of pyrite vary greatly（from –46.6‰ to –12.3‰ V-CDT） and increase with ***,the pyrite in the shallow sediments resulted from organoclastic sulfate reduction（OSR） and is influenced by AOM with *** relative high abundance and δ^34 S values of pyrite in sediments at depths from 580 to 810 cmbsf indicate that this interval is the location of a paleo-sulfate methane transition zone（SMTZ）.The sulfur isotopic composition of gypsum（from–25‰ to –20.7‰） is much lower than that of the seawater sulfate,indicating the existence of a 34 S-depletion source of sulfur species that most likely are products of the oxidation of pyrites formed in *** oxidation is controlled by ambient electron acceptors such as MnO2,iron（Ⅲ） and oxygen driven by the SMTZ location shift to great *** δ^34 S values of gypsum at greater depth are lower than those of the associated pyrite,revealing downward diffusion of 34 S-depleted sulfate from the mixture of oxidation of pyrite derived by OSR and the seawater *** sulfates also lead to an increase of calcium ions from the dissolution of calcium carbonate mineral,which will be favor to the formatio

关键词： pyrite tube authigenic gypsum sulfur isotopes methane seepage northern South China Sea

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Last glacial terrestrial vegetation record of leaf wax n-alkanols in the northern South China Sea:Contrast to scenarios from longchain n-alkanes

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Acta Oceanologica Sinica 2022年第8期41卷 22-30页

作者： Shengyi Mao Guodong Jia Xiaowei Zhu Nengyou Wu Daidai Wu hongxiang guan Lihua Liu CAS Key Laboratory of Gas Hydrate Guangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou 510640China Southern Marine Science and Engineering guangdong Laboratory(guangzhou) Guangzhou 511458China State Key Laboratory of Marine Geology Tongji UniversityShanghai 200092China Key Laboratory of Ocean and Marginal Sea Geology South China Sea Institute of OceanologyChinese Academy of SciencesGuangzhou 510301China Key Laboratory of Gas Hydrate of Ministry of Natural Resources Qingdao Institute of Marine GeologyQingdao 266237China Laboratory for Marine Mineral Resources Pilot National Laboratory for Marine Science and Technology(Qingdao)Qingdao 266237China

Long-chain n-alkanols and n-alkanes in core sediments from the northern South China Sea(SCS)were measured to make a comparison during terrestrial vegetation reconstruction from~42 ka to~7 *** results showed that terrestrial vegetation record from long-chain n-alkanes matched well with previous studies in nearby cores,showing that more C_(4)plants developed during the Last Glacial Maximum(LGM)and C_(3)plants dominated in the interglacial ***,these scenarios were not revealed by terrestrial vegetation reconstruction using long-chain n-alkanols,which showed C_(3)plant expansion during the *** discrepancy during the interglacial period could be attributed to the aerobic degradation of functionalized long-chain n-alkanols in the oxygen-rich bottom water,resulting in poor preservation of terrestrial vegetation *** the other hand,the different advantages of functionalized n-alkanols and non-functional n-alkanes to record local and distal vegetation signals,respectively,may offer a potential explanation for the contradiction during the LGM when the SCS was characterized by low-oxygen deep ***,large variations on n-alkyl lipid compositions in C_(3)/C_(4)plants could play a part in modulating sedimentary long-chain n-alkanols and n-alkanes toward different vegetation signals,thereby suggesting that caution must be taken in respect to the terrestrial vegetation reconstruction using long-chain n-alkanes and long-chain n-alkanols.

关键词： South China Sea long-chain n-alkanols long-chain n-alkanes Last Glacial Maximum terrestrial vegetation record

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Fatty-acids and their δ^(13)C characteristics of seep carbonates from the northern continental slope of Gulf of Mexico

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Chinese Science Bulletin 2010年第8期55卷 730-735页

作者： guan hongxiang FENG Dong WU NengYou CHEN DuoFu ROBERTS H H WU DaiDai CAS Key Laboratory of Marginal Sea Geology State Key Laboratory of Organic Geochemistry Guangzhou Institute of Geochemistry Chinese Academy of Sciences Guangzhou 510640 China CAS Key Lab of Renewable Energy and Gas Hydrate Guangzhou Institute of Energy Conversion Chinese Academy of Sciences Guangzhou 510640 China Graduate University of Chinese Academy of Sciences Beijing 100049 China Coastal Studies Institute Louisiana State University Baton Rouge LA 70803 USA

Here we reported the fatty-acids and their δ13 C values in seep carbonates collected from Green Canyon lease block 185 (GC 185;Sample GC-F) at upper continental slope (water depth:～540 m),and Alaminos Canyon lease block 645 (GC 645;Sample AC-E) at lower continental slope (water depth:～2200 m) of the Gulf of *** than thirty kinds of fatty acids were detected in both *** fatty acids are maximized at C *** is a clear even-over-odd carbon number predominance in carbon number *** fatty acids are mainly composed of n-fatty acids,iso-/anteiso-fatty acids and terminally branched odd-numbered fatty acids (iso/anteiso).The low δ13 C values (-39.99‰ to -32.36‰) of n-C 12:0,n-C 13:0,i-C 14:0 and n-C 14:0 suggest that they may relate to the chemosynthetic communities at seep *** unsaturated fatty acids n-C 18:2 and C 18:1 △9 have the same δ13 C values,they may originate from the Beggiatoa/*** other fatty acids,the terminally branched fatty acids (iso/anteiso) show lower δ13 C values (as low as -63.95‰) suggesting a possible relationship to sulfate reducing bacteria,which is common during anaerobic oxidation of methane at seep sites.

关键词：脂肪酸含量碳酸盐岩大陆坡氨基酸 C值墨西哥湾渗透国际标准化组织

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Lipid biomarker composition in surface sediments from the Carlsberg Ridge near the Tianxiu Hydrothermal Field

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Acta Oceanologica Sinica 2021年第8期40卷 53-64页

作者： Shengyi Mao hongxiang guan Lihua Liu Xiqiu Han Xueping Chen Juan Yu Yongge Sun Yejian Wang CAS Key Laboratory of Gas Hydrate Guangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou 510640China Key Laboratroy of Submarine Geosciences&Second Institute of Oceanography Ministry of Natural ResourcesHangzhou 310012China School of Environmental and Chemical Engineering Shanghai UniversityShanghai 200444China Institute of Environmental and Biogeochemistry(eBig) School of Earth SciencesZhejiang UniversityHangzhou 310027China

Hydrothermal venting has a profound effect on the chemical and biological properties of local and distal seawater and sediments. In this study, lipid biomarkers were analyzed to examine the potential influence of hydrothermal activity on the fate of organic matter(OM) in surface sediments around Tianxiu Hydrothermal Field in the Carlsberg Ridge(CR), Northwest Indian Ocean. By comparing the biomarker distributions of the samples with that of other typical hydrothermal sediments in the mid ocean ridge, it is shown that the location of the samples is not affected by the hydrothermal activity. The relatively low abundances of terrestrial n-alkyl lipids and riverine1,15-C_(32) diol suggested a minor contribution of terrigenous OM to the study area. The bacteria contributed predominantly to sedimentary marine OM;however, other marine source organisms, e.g., eukaryotes(i.e.,phytoplankton and fungi) could not be completely neglected. The marine-originated biomarkers showed significantly variable distributions between the two sediments, suggesting different dynamic physical and biogeochemical processes controlling the fate of marine OM. This study identified various diagnostic biomarkers(5,5-diethyl alkanes, diols and β-OH FAs), which may have significant environmental implications for future works in this region.

关键词： Carlsberg Ridge Tianxiu Hydrothermal Field surface sediments biomarkers

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Composition and origin of lipid biomarkers in the surface sediments from the southern Challenger Deep, Mariana Trench

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Geoscience Frontiers 2019年第1期10卷 351-360页

作者： hongxiang guan Linying Chen Min Luo Lihua Liu Shengyi Mao Huangmin Ge Mei Zhang Jiasong Fang Duofu Chen Key Laboratory of Gas Hydrate Guangzhou Institute of Energy Conversion Chinese Academy of Sciences Laboratory for Marine Geology Qingdao National Laboratory for Marine Science and Technology Shanghai Engineering Research Center of Hadal Science and Technology College of Marine Sciences Shanghai Ocean University

The surface sediments collected from the southern Mariana Trench at water depths between ca.4900 m and 7068 m were studied using lipid biomarker analyses to reveal the origin and distribution of organic matters. For all samples, an unresolved complex mixture(UCM) was present in the hydrocarbon fractions, wherein resistant component tricyclic terpanes were detected but C_(27)-C _(29) regular steranes and hopanes indicative of a higher molecular weight range of petroleum were almost *** biomarker distribution patterns suggested that the UCM and tricyclic terpanes may be introduced by contamination of diesel fuels or shipping activities and oil seepage elsewhere. The well-developed faults and strike-slip faults in the Mariana subduction zone may serve as passages for the petroleum hydrocarbons. In addition, the relative high contents of even n-alkanes and low Carbon Preference Indices indicated that the n-alkanes were mainly derived from bacteria or algae. For GDGTs, the predominance of GDGT-0 and crenarchaeol, together with low GDGT-0/Crenarchaeol ratios(ranging from0.86 to 1.64), suggests that the GDGTs in samples from the southern Mariana Trench were mainly derived from planktic Thaumarchaeota. However, the high GDGT-0/crenarchaeol ratio(10.5) in sample BC07 suggests that the GDGTs probably were introduced by methanogens in a more anoxic environment. Furthermore, the n-alkanes C_(19)-C_(22) and the n-fatty acids C_(20:0)-C_(22:0) were depleted in^(13)C by 3‰ compared to n-alkanes C_(16)-C_(18) and the n-fatty acids C_(14:0)-C_(18:0), respectively, which was interpreted to result from the preferential reaction of fatty acid fragments with carbon "lighter" terminal carboxyl groups during carbon chain elongation from the precursors to products. The abundance of total alkanes, carboxylic acids, alcohols and total lipids were generally increased along the down-going seaward plate, suggesting the lateral organic matter inputs play an important role in organic matt

关键词： Mariana Trench Lipid biomarkers Organic matter Topography Hydrodynamics

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Research on an Intelligent Decision Support System for a Conceptual Innovation Design of Pumping Units Based on TRIZ

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Petroleum Science 2006年第1期3卷 85-91页

作者： Zhang Peng He Chuan guan hongxiang Gai Feng Qi Bin The Southwest Petroleum Institute Chengdu Sichuan 610500 China

Attention is concentrated on how to perform the innovative design during the process of pumping unit conceptual design, and how to enhance design efficiency and inspire creativity. Aiming at the shortages of conceptual design, introducing the theory of inventive problem solving （TRIZ） into the mechanical product design for producing innovative ideas, and using the advanced computer-aided technique, the intelligent decision support system （IDSS） based on TRIZ （TRIZ-IDSS） has been constructed. The construction method, system structure, conceptual production, decisionmaking and evaluation of the problem solving subsystem are discussed. The innovative conceptual design of pumping units indicates that the system can help the engineers open up a new space of thinking, overcome the thinking inertia, and put forward innovative design concepts. This system also can offer the scientific instructions for the innovative design of mechanical products.

关键词： Pumping units innovative conceptual design TRIZ intelligent decision support system

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