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| 1 | 页岩气运移过程中的碳同位素分馏:机理、表征及意义显示文摘页岩原位含气量和吸附气/游离气比例是页岩气资源评价的2个关键参数,因此受到了广泛关注.然而,业已提出评价上述关键参数的多种方法均未得到广泛认可.甲烷在运移过程中的碳同位素分馏效应为有效区分不同赋存状态气体(吸附气、游离气)运移过程并最终确定这2个参数提供了全新的途径.文章通过页岩气运移模拟实验发现,页岩气解析/生产过程中甲烷碳同位素分馏存在4个阶段:游离气压差渗流阶段(Ⅰ)、吸附-游离转换阶段(Ⅱ)、吸附气解吸阶段(Ⅲ)和浓度差扩散阶段(Ⅳ).解耦实验揭示了甲烷运移过程中各单一作用(压差渗流、吸附-解吸和扩散)的碳同位素分馏效应.结合Amoco曲线拟合法和碳同位素分馏方法,文章进一步评价了页岩气解析/生产过程中吸附气/游离气比例动态变化,结果表明:第Ⅰ阶段产出的气体主要为游离气,甲烷碳同位素值(δ13C1)基本保持不变,且与气源值(13C10)相近;第Ⅱ阶段,游离气比例降低,吸附气比例增加,δ13C1值逐渐变轻;随着游离气的大量消耗,吸附气占据主导地位(接近100%),碳同位素分馏进入第Ⅲ阶段,δ13C1值逐渐变重;第Ⅳ阶段,残留在页岩基质内的吸附气在浓度差作用下向外扩散,该阶段δ13C1值再次变轻并最终稳定在一个较轻值.此外,文章还建立了定量描述页岩气解吸与扩散的动力学模型. | 李文镖 卢双舫 李俊乾 张鹏飞 王思远 冯文俊 魏永波 | 2020 | 中国科学:地球科学2020，50，4： | 8 |
| 2 | Carbon isotope fractionation during shale gas transport: Mechanism, characterization and significance显示文摘The gas in-place(GIP)content and the ratio of adsorbed/free gas are two key parameters for the assessment of shale gas resources and have thus received extensive attention.A variety of methods have been proposed to solve these issues,however none have gained widespread acceptance.Carbon isotope fractionation during the methane transport process provides abundant information,serving as an effective method for differentiating the gas transport processes of adsorbed gas and free gas and ultimately evaluating the two key parameters.In this study,four stages of methane carbon isotope fractionation were documented during a laboratory experiment that simulated gas transport through shale.The four stages reflect different transport processes:the free gas seepage stage(Ⅰ),transition stage(Ⅱ),adsorbed gas desorption stage(Ⅲ)and concentration diffusion stage(Ⅳ).Combined with the results of decoupling experiments,the isotope fractionation characteristics donated by the single effect(seepage,adsorption-desorption and diffusion)were clearly revealed.We further propose a technique integrating the Amoco curve fit(ACF)method and carbon isotope fractionation(CIF)to determine the dynamic change in adsorbed and free gas ratios during gas production.We find that the gases produced in stage Ⅰ are primarily composed of free gas and that carbon isotope ratios of methane(δ13C1)are stable and equal to the ratios of source gas(13C 10).In stage Ⅱ,the contribution of free gas decreases,while the proportion of adsorbed gas increases,and the δ13C1 gradually becomes lighter.With the depletion of free gas,the adsorbed gas contribution in stage Ⅲ reaches 100%,and the δ13C1 becomes heavier.Finally,in stage Ⅳ,the desorbed gas remaining in the pore spaces diffuses out under the concentration difference,and the δ13C1 becomes lighter again and finally stabilizes.In addition,a kinetic model for the quantitative description of isotope fractionation during desorption and diffusion was established. | Wenbiao LI Shuangfang LU Junqian LI Pengfei ZHANG Siyuan WANG Wenjun FENG Yongbo WEI | 2020 | Science China Earth Sciences2020，63，5： | 4 |
| 3 | 页岩气/煤层气运移过程中的同位素分馏研究进展显示文摘从同位素分馏特征与影响因素、分馏机理与定量表征模型和地质应用等3方面对页岩气/煤层气运移过程中的同位素分馏研究进展进行综述。研究发现,页岩气/煤层气完整产出过程中的同位素分馏表现为“稳定—变轻—变重—再变轻”的4阶段特征,这与页岩/煤层孔隙内复杂的气体运移方式密切相关。页岩/煤层内气体运移机制包括渗流、扩散和吸附/解吸,其中压差驱动的体相渗流基本不产生同位素分馏,而扩散和吸附/解吸过程中的同位素分馏显著。现有的同位素分馏模型包括纯扩散分馏模型、扩散、吸附/解吸耦合模型和多尺度多机制耦合模型,模型计算结果表明,天然气运移过程中的同位素分馏主要受控于岩石孔隙结构、吸附能力和初始/边界条件。目前,同位素分馏模型已成功应用于评价页岩/煤岩原位含气量和吸附气/游离气比例等关键参数,同时在气井生产状态判识和产能变化趋势预测等方面展现出一定的应用前景。下一步研究应重点关注:①天然气运移过程不同组分碳、氢同位素组成的协同演化规律;②生—排—运—聚—散全过程同位素分馏的整体表征;③复杂孔-裂隙系统内天然气运移过程同位素分馏的定量表征及应用。 | 李文镖 卢双舫 李俊乾 魏永波 赵圣贤 张鹏飞 王子轶 李霄 王峻 | 2022 | 石油勘探与开发2022，49，5： | 1 |
| 4 | Prediction of decline in shale gas well production using stable carbon isotope technique显示文摘Prediction of shale gas production is a challenging task because of the complex fracture-pore networks and gas flow mechanisms in shale reservoirs.Empirical methods,which are used in the industry to forecast the future production of shale gas,have not been assessed sufficiently to warrant high confidence in their results.Methane carbon isotopic signals have been used for producing gas wells,and are controlled by physical properties and physics-controlling production;they serve as a unique indicator of the gas production status.Here,a workable process,which is combined with a gas isotope interpretation tool(also known as a numerical simulator),has been implemented in Longrnaxi shale gas wells to predict the production decline curves.The numerical simulator,which takes into account a convection-diffu-sion-adsorption model for the matrix and a convection model for fractures in^(13)CH_(4) and ^(12)CH_(4) isotopologues,was used to stabilize the carbon isotope variation in the produced gas to elucidate gas recovery.Combined with the production rates of the four developing wells,the total reserves ranged from 1.72×10^(8) to 2.02×10^(8) m^(3),which were used to constrain the trend of two-segment produc-tion decline curves that exhibited a transition from a hyperbolic equation to an exponential one within 0.82-0.89 year.Two-segment production decline curves were used to forecast future production and estimate ultimate recovery. | Shengxian ZHAO Shujuan KANG Majia ZHENG Shuangfang LU Yunfeng YANG Huanxu ZHANG Yongyang LIU Ziqiang XIA Chenglin ZHANG Haoran HU Di ZHU | 2021 | Frontiers of Earth Science2021，15，4： | 1 |
| 5 | Research progress on isotopic fractionation in the process of shale gas/coalbed methane migration显示文摘The research progress of isotopic fractionation in the process of shale gas/coalbed methane migration has been reviewed from three aspects: characteristics and influencing factors, mechanism and quantitative characterization model, and geological application. It is found that the isotopic fractionation during the complete production of shale gas/coalbed methane shows a four-stage characteristic of “stable-lighter-heavier-lighter again”, which is related to the complex gas migration modes in the pores of shale/coal. The gas migration mechanisms in shale/coal include seepage, diffusion, and adsorption/desorption. Among them, seepage driven by pressure difference does not induce isotopic fractionation, while diffusion and adsorption/desorption lead to significant isotope fractionation. The existing characterization models of isotopic fractionation include diffusion fractionation model, diffusion-adsorption/desorption coupled model, and multi-scale and multi-mechanism coupled model. Results of model calculations show that the isotopic fractionation during natural gas migration is mainly controlled by pore structure, adsorption capacity, and initial/boundary conditions of the reservoir rock. So far, the isotope fractionation model has been successfully used to evaluate critical parameters, such as gas-in-place content and ratio of adsorbed/free gas in shale/coal etc. Furthermore, it has shown promising application potential in production status identification and decline trend prediction of gas well. Future research should focus on:(1) the co-evolution of carbon and hydrogen isotopes of different components during natural gas migration,(2) the characterization of isotopic fractionation during the whole process of gas generation-expulsion-migration-accumulation-dispersion, and(3) quantitative characterization of isotopic fractionation during natural gas migration in complex pore-fracture systems and its application. | LI Wenbiao LU Shuangfang LI Junqian WEI Yongbo ZHAO Shengxian ZHANG Pengfei WANG Ziyi LI Xiao WANG Jun | 2022 | Petroleum Exploration and Development2022，49，5： | 1 |
| 6 | 烷烃碳同位素对页岩含气性的指示意义——以四川盆地及周缘龙马溪组为例显示文摘以四川盆地及周缘龙马溪组为例,分析了烷烃碳同位素平面分布特征以及倒转情况,定量研究了烷烃碳同位素值与热演化程度、埋藏深度及含气量之间的关系,并探讨了造成不同区块烷烃碳同位素倒转程度差异的主要原因。结果表明:(1)龙马溪组页岩气组分具有典型的干气特征:CH_(4)含量介于95.32%~99.59%,平均为98.44%;C_(2)H6含量较少,介于0.09%~0.74%,平均为0.52%;C_(3)H8含量普遍很低。(2)烷烃碳同位素表现为自盆地边缘向盆地中心逐渐变轻的特征,δ^(13)C_(1)值介于-36.9‰~-26.7‰,平均为-30.27‰;δ^(13)C_(2)值介于-42.8‰~-31‰,平均为-34.9‰;δ^(13)C_(3)值介于-50.5‰~-33.1‰,平均为-37.28‰。(3)整体上,四川盆地及周缘龙马溪组页岩气烷烃碳同位素具有完全倒转(δ^(13)C_(1)>δ^(13)C_(2)>δ^(13)C_(3))的特征,页岩气成藏过程中干酪根裂解气与滞留烃裂解气的混合可能是导致烷烃碳同位素发生倒转的主要原因。(4)同位素定量分馏模型显示滞留烃裂解气在页岩气中的占比多大于60%,指示两种裂解气混合比不同是造成烷烃碳同位素倒转程度差异的主要原因;整体上,随滞留烃裂解气含量的增多,δ^(13)C_(2)值减小,烷烃碳同位素倒转程度增大,页岩的含气量也逐渐增加。 | 廖芸 郭艳琴 陈志鹏 王芳 王高成 邹辰 马瑶 | 2021 | 海相油气地质2021，26，3： | 1 |
| 7 | 丙烷分子内碳同位素示踪作用显示文摘分子内同位素可标定物质来源、形成机理与路径.通过对比世界不同层系/类型天然气丙烷与有机质(Ⅰ~Ⅲ型干酪根、原油、nC_(25))热模拟产生的丙烷分子内碳同位素特征发现:(1)实验条件下丙烷演化模式与自然条件下区别极大,源于实验条件下能够全面再现各阶段特征,而自然条件下部分阶段不出现,尤其是油型气丙烷.(2)地质盆地油型气丙烷分子内碳同位素相对稳定,与母质类型、源岩时代、沉积环境等相关,受成熟度影响较小(<3‰),可做绝佳源岩示踪剂.煤成气丙烷由于煤富含支链结构而具有两阶段演化模式,阶段I随成熟度增加中位碳快速变重、边位碳轻微变重,阶段Ⅱ趋近于丙烷理论生成线.(3)丙烷分子内同位素受多种次生/后生作用影响显著,化学氧化致中位碳比边位碳变重幅度快1倍.(4)受Fe2O3等金属氧化物氧化影响,塔里木盆地克深8气藏中的丙烷中位碳明显偏重;而克深13气藏中丙烷被氧化程度弱,源于成藏晚;台盆区塔中45、轮古东、吉拉克、富满等油气藏奥陶系天然气来源一致,但与和田河天然气区别明显.丙烷分子内同位素示踪效应强大,将为深层与复杂构造区油气来源与成藏过程研究提供强有力支撑. | 帅燕华 彭平安 陶小晚 李剑 李芸 熊永强 | 2023 | 科学通报2023，68，36： | 0 |
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