孙龙德,冯子辉,江航,曾花森
SUN Longde,FENG Zihui,JIANG Hang,ZENG Huasen

• 1:多资源协同陆相页岩油绿色开采全国重点实验室
• 2:中国石油天然气集团有限公司
• 3:中国石油大庆油田有限责任公司勘探开发研究院
• 4:中国石油勘探开发研究院

摘要(Abstract)：

氢能是全球能源转型发展的重要载体，与人工制氢相比，天然氢气的开采不仅具有成本上的优势，也是实现能源完全脱碳的关键。松辽盆地作为大型陆内裂谷盆地，具备勘探天然氢气的潜力。首次系统梳理松辽盆地北部中下部含油气组合和深部含气组合中天然氢的含量，分析天然氢气的空间分布特征，初步探讨了天然氢气的来源、形成机制及控制因素。结果表明：松辽盆地含氢天然气（φ（H_2）>1.0%）在中央坳陷区普遍发育，氢体积分数为1.00%～85.54%，其中富氢天然气（φ（H_2）>10.0%）主要在深部含气组合，试气产量在微量和1 444 m~3/d之间，沿控陷断裂附近分布；松辽盆地天然氢气主要来源于深部富铁岩层的水-岩作用，氢气的形成和供给具有可持续性，具备形成天然氢气聚集的物质基础；基底以上富氢气藏的形成受沟通至地幔的控陷断裂、深大断裂控制，油藏和天然气藏对富氢气体有稀释和破坏作用，未来天然氢气藏的勘探应该避开油气充注的有利区；深化对盆地深部壳-幔结构及无机地球化学作用过程的认识，是未来松辽盆地天然氢气勘探的重要科学议题。研究成果可为松辽盆地天然氢气的勘探提供理论指导。
Hydrogen energy is an important carrier for global energy transition and development. Compared to artificially producing hydrogen, the exploitation of natural hydrogen not only has advantage of low cost, but also is the key in realizing complete decarbonization of energy. As a large intracontinental rift basin, Songliao Basin has potential for exploring natural hydrogen. Natural hydrogen content of middle and lower oil-and gas-bearing assemblages and deep gas-bearing assemblages in northern Songliao Basin is systematically summarized for the first time to preliminarily analyze spatial distribution characteristics, source, genesis mechanism and controlling factors of natural hydrogen. The results show that hydrogen-bearing natural gas(φ(H_2)>1.0%) widely develops in Central Depression of Songliao Basin, with hydrogen content of 1.00%～85.54%, of which hydrogen-rich gas(φ(H_2)>10.0%) are mainly in deep gas-bearing assemblages, with gas production ranging from trace to 1 444 m~3/d and distribution near riftcontrolling faults.Natural hydrogen in Songliao Basin is mainly generated by water-rock reaction in deep iron-rich rocks, with sustainable hydrogen generation and supply, providing material basis for natural hydrogen accumulation.The formation of hydrogen-rich gas reservoirs above basement is controlled by rift-controlling faults and deep large faults connecting to the mantle. Oil and natural gas reservoirs have dilution and destructive impact on hydrogen-rich gas. Future exploration of natural hydrogen gas reservoirs should avoid favorable areas with oil and gas charge.Deepening the understanding of deep crust-mantle structure and inorganic geochemical processes in the basin is an important scientific subject for future natural hydrogen exploration in Songliao Basin. The research provides theoretical guidance for exploration of natural hydrogen in Songliao Basin.

关键词(KeyWords)： 松辽盆地;天然氢气;成因机制;水-岩作用;蛇纹岩化作用
Songliao Basin;natural hydrogen;genesis mechanism;water-rock reaction;serpentinization

Abstract:

Keywords:

基金项目(Foundation): 中央引导地方科技发展专项“黑龙江省致密油和泥岩油成藏研究重点实验室建设项目”（ZY20B13）

作者(Author): 孙龙德,冯子辉,江航,曾花森
SUN Longde,FENG Zihui,JIANG Hang,ZENG Huasen

DOI: 10.19597/J.ISSN.1000-3754.202403001

参考文献(References)：

• [1] OSSELIN F,SOULAINE C,FAUGUEROLLES C,et al. Orange hydrogen is the new green[J].Nature Geoscience, 2022, 15(10):765-769.
• [2]窦立荣，刘化清，李博，等.全球天然氢气勘探开发利用进展及中国的勘探前景[J].岩性油气藏，2024,36(2):1-14.DOU Lirong,LIU Huaqing,LI Bo,et al. Global natural hydrogen exploration and development situation and prospects in China[J]. Lithologic Reservoirs,2024,36(2):1-14.
• [3] HAND E. Hidden hydrogen[J]. Science,2023,379(6633):630-636.
• [4] NEAL C,STANGER G. Hydrogen generation from mantle source rocks in Oman[J]. Earth and Planetary Science Letters,1983,66(1-3):315-320.
• [5] PETERSEN H C. Does natural hydrogen exist[J]. International Journal of Hydrogen Energy,1990,15(1):55.
• [6] MAIGA O, DEVILLE E, LAVAL J, et al. Characterization of the spontaneously recharging natural hydrogen reservoirs of Bourakebougou in Mali[J]. Scientific Reports, 2023, 13:11876.
• [7] ZGONNIK V. The occurrence and geoscience of natural hydrogen:A comprehensive review[J]. Earth-Science Reviews, 2020,203:103140.
• [8]孟庆强，金之钧，孙冬胜，等.高含量氢气赋存的地质背景及勘探前景[J].石油实验地质，2021,43(2):208-216.MENG Qingqiang,JIN Zhijun,SUN Dongsheng,et al. Geological background and exploration prospects for the occurrence of high-content hydrogen[J]. Petroleum Geology&Experiment,2021,43(2):208-216.
• [9]孟凡超，崔岩，张曰静，等.松辽盆地基底石英脉中无机成因气的地球化学特征及指示意义[J].天然气工业，2020,40(10):29-37.MENG Fanchao,CUI Yan,ZHANG Yuejing,et al. Geochemical characteristics of abiogenic gas in the quartz veins in the basement rocks of the Songliao Basin and their indicative significance[J]. Natural Gas Industry,2020,40(10):29-37.
• [10] HAN S B,XIANG C H,DU X,et al. Geochemistry and origins of hydrogen-containing natural gases in deep Songliao basin,China:Insights from continental scientific drilling[J]. Petroleum Science,2024,21(2):741-751.
• [11] HORSFIELD B,MAHLSTEDT N,WENIGER P,et al. Molecular hydrogen from organic sources in the deep Songliao Basin,PR China[J]. International Journal of Hydrogen Energy,2022,47(38):16750-16774.
• [12]王璞珺，赵然磊，蒙启安，等.白垩纪松辽盆地：从火山裂谷到陆内拗陷的动力学环境[J].地学前缘，2015,22(3):99-117.WANG Pujun,ZHAO Ranlei,MENG Qi’an,et al. The Cretaceous Songliao Basin:Dynamic background from volcanic rift to interior sag basin[J]. Earth Science Frontiers,2015,22(3):99-117.
• [13]冯志强，董立，童英，等.蒙古-鄂霍茨克洋东段关闭对松辽盆地形成与演化的影响[J].石油与天然气地质，2021,42(2):251-264.FENG Zhiqiang,DONG Li,TONG Ying,et al. Impacts of the closure of eastern Mongolia-Okhotsk Ocean on formation and evolution of Songliao Basin[J]. Oil&Gas Geology, 2021, 42(2):251-264.
• [14] WANG F,XU W L,GAO F H,et al. Precambrian terrane within the Songnen-Zhangguangcai Range Massif, NE China:Evidence from U-Pb ages of detrital zircons from the Dongfengshan and Tadong groups[J].Gondwana Research,2014,26(1):402-413.
• [15]裴福萍，许文良，杨德彬，等.松辽盆地基底变质岩中锆石U-Pb年代学及其地质意义[J].科学通报，2006,51(24):2881-2887.PEI Fuping, XU Wenliang, YANG Debin, et al. Zircon U-Pb geochronology of basement metamorphic rocks in the Songliao Basin[J]. Chinese Science Bulletin,2006,51(24):2881-2887.
• [16]章凤奇，陈汉林，董传万，等.松辽盆地北部存在前寒武纪基底的证据[J].中国地质，2008,35(3):421-428.ZHANG Fengqi, CHEN Hanlin,DONG Chuanwan,et al. Evidence for the existence of Precambrian basement under the northern Songliao Basin[J]. Geology in China, 2008, 35(3):421-428.
• [17]尹永康.松辽盆地三叠纪基底地质年代学与岩石学研究及其构造意义[D].长春：吉林大学，2022.YIN Yongkang. Geochronology and Petrology of Triassic basement of the Songliao Basin:Implications for regional tectonics[D].Changchun:Jilin University,2022.
• [18]王小军，白雪峰，陆加敏，等.松辽盆地北部油气勘探新领域、新类型及资源潜力[J].石油学报，2023,44(12):2091-2103.WANG Xiaojun,BAI Xuefeng,LU Jiamin,et al. New fields,new types and resource potentials of oil-gas exploration in northern Songliao Basin[J]. Acta Petrolei Sinica, 2023, 44(12):2091-2103.
• [19] COVENEY R M,GOEBEL E D,ZELLER E J,et al. Serpentinization and the origin of hydrogen gas in Kansas[J]. AAPG Bulletin,1987,71(1):39-48.
• [20]韩双彪，唐致远，杨春龙，等.天然气中氢气成因及能源意义[J].天然气地球科学，2021,32(9):1270-1284.HAN Shuangbiao, TANG Zhiyuan, YANG Chunlong, et al.Genesis and energy significance of hydrogen in natural gas[J].Natural Gas Geoscience,2021,32(9):1270-1284.
• [21] MILKOV A V. Molecular hydrogen in surface and subsurface natural gases:Abundance,origins and ideas for deliberate exploration[J]. Earth-Science Reviews,2022,230:104063.
• [22] PRINZHOFER A,TAHARA CISSE C S,DIALLO A B. Discovery of a large accumulation of natural hydrogen in Bourakebougou(Mali)[J]. International Journal of Hydrogen Energy, 2018,43(42):19315-19326.
• [23] GUELARD J,BEAUMONT V,ROUCHON V,et al. Natural H2in Kansas:Deep or shallow origin[J]. Geochemistry, Geophysics,Geosystems,2017,18(5):1841-1865.
• [24] MOINE B N,BOLFAN-CASANOVA N,RADU I B,et al. Molecular hydrogen in minerals as a clue to interpret?D variations in the mantle[J]. Nature Communications,2020,11:3604.
• [25] LIN L H,SLATER G F,LOLLAR B S,et al. The yield and isotopic composition of radiolytic H2, a potential energy source for the deep subsurface biosphere[J]. Geochimica et Cosmochimica Acta,2005,69(4):893-903.
• [26] SUZUKI N,SAITO H,HOSHINO T. Hydrogen gas of organic origin in shales and metapelites[J]. International Journal of Coal Geology,2017,173:227-236.
• [27]孟庆强.地质体中天然氢气成因识别方法初探[J].石油实验地质，2022,44(3):552-558.MENG Qingqiang. Identification method for the origin of natural hydrogen gas in geological bodies[J]. Petroleum Geology&Experiment,2022,44(3):552-558.
• [28]冯志强，刘永江，李伟民，等.大兴安岭阿尔山迈罕特乌拉蛇绿混杂岩形成时代及其地质意义[J].地质科学，2021,56(2):508-532.FENG Zhiqiang,LIU Yongjiang,LI Weimin,et al. Geochronology and regional implication of Manhantewula ophiolitic mélange in Arxan, the Great Xing’an Range[J]. Chinese Journal of Geology,2021,56(2):508-532.
• [29] ARROUVEL C,PRINZHOFER A. Genesis of natural hydrogen:New insights from thermodynamic simulations[J]. International Journal of Hydrogen Energy,2021,46(36):18780-18794.
• [30]迟元林，云金表，庞庆山.徐家围子断陷CO2气藏形成地质机制研究[J].大庆石油地质与开发，2000,19(3):1-3.CHI Yuanlin,YUN Jinbiao,PANG Qingshan. Geological mechanism of the formation of CO2 reservoir of Xujiaweizi rift[J].Petroleum Geology&Oilfield Development in Daqing,2000,19(3):1-3.
• [31]付广，吕延防，王剑秦.徐家围子断陷CO2气成藏与分布的主控因素及有利区预测[J].断块油气田，2002,19(3):1-4.FU Guang, LüYanfang, WANG Jianqin. Main factors controlling the formation and distribution of carbon dioxide gas reservoirs and favorable areas prospecting in Xujiaweizi depression[J].Fault-Block Oil&Gas Field,2002,19(3):1-4.
• [32]戴金星，邹才能，张水昌，等.无机成因和有机成因烷烃气的鉴别[J].中国科学D辑：地球科学，2008,38(11):1329-1341.DAI Jinxing,ZOU Caineng,ZHANG Shuichang,et al. Discrimination of abiogenic and biogenic alkane gases[J]. Science in China(Series D)-Earth Sciences,2008,38(11):1329-1341.
• [33] SUGISAKI R,MIMURA K. Reply to the comment by J.F. Kenney on Mantle hydrocarbons:Abiotic or biotic[J]. Geochimica et Cosmochimica Acta,1995,59(18):3859-3861.
• [34] WEATHERBEE G D,BARTHOLOMEW C H. Hydrogenation of CO2 on groupⅧmetals：Ⅳ. Specific activities and selectivities of silica-supported Co,Fe,and Ru[J]. Journal of Catalysis,1984,87(2):352-362.
• [35] MURRAY J,CLéMENT A,FRITZ B,et al. Abiotic hydrogen generation from biotite-rich granite:A case study of the Soultzsous-Forêts geothermal site, France[J]. Applied Geochemistry,2020,119:104631.
• [36] LE BAS M J,STRECKEISEN A L. The IUGS systematics of igneous rocks[J]. Journal of the Geological Society, 1991, 148(5):825-833.
• [37]张钊，黄丰，许继峰，等.松科二井早白垩世早期玄武安山岩的发现及地质意义[J].岩石学报，2022,38(6):1756-1770.ZHANG Zhao,HUANG Feng,XU Jifeng, et al. Discovery and geological implications of the Early Cretaceous basaltic andesites in SK2 borehole[J]. Acta Petrologica Sinica,2022,38(6):1756-1770.
• [38] LOLLAR B S, ONSTOTT T C, LACRAMPE-COULOUME G,et al. The contribution of the Precambrian continental lithosphere to global H2 production[J]. Nature, 2014, 516(7531):379-382.
• [39] NEWELL K D,DOVETON J H,MERRIAM D F,et al. H2-rich and hydrocarbon gas recovered in a deep Precambrian well in northeastern Kansas[J]. Natural Resources Research, 2007,16(3):277-292.
• [40]王成善，高远，王璞珺，等.松辽盆地国际大陆科学钻探：白垩纪恐龙时代陆相地质记录[J].地学前缘，2024,31(1):412-430.WANG Chengshan,GAO Yuan,WANG Pujun,et al. International continental scientific drilling project of the Songliao Basin:Terrestrial geological records of the Cretaceous dinosaur age[J]. Earth Science Frontiers,2024,31(1):412-430.
• [41] PRINZHOFER A, CACAS-STENTZ M-C. Natural hydrogen and blend gas:A dynamic model of accumulation[J]. International Journal of Hydrogen Energy,2023,48(57):21610-21623.