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CN109826606B - Method and device for intermittent in-situ exploitation of oil shale by alternately fracturing high-temperature fluid and low-temperature fluid - Google Patents

Method and device for intermittent in-situ exploitation of oil shale by alternately fracturing high-temperature fluid and low-temperature fluid Download PDF

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CN109826606B
CN109826606B CN201910117012.5A CN201910117012A CN109826606B CN 109826606 B CN109826606 B CN 109826606B CN 201910117012 A CN201910117012 A CN 201910117012A CN 109826606 B CN109826606 B CN 109826606B
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oil shale
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张广清
郑学林
邢岳堃
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China University of Petroleum Beijing
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Abstract

本申请提供了一种高低温流体交替压裂间断原位开采油页岩的方法及装置,该方法包括如下步骤:采用高温流体对油页岩储层进行压裂,以使油页岩储层产生预定长度的人工主裂缝。停止高温流体压裂油页岩储层,并使高温流体加热油页岩储层,在达到第一预定时间后,返排高温流体。采用液氮对油页岩储层进行压裂,以使人工主裂缝两侧产生次级裂缝,同时液氮气化产生氮气,进而使次级裂缝两侧产生多级裂缝。封闭井口,在达到第二预定时间后,开启井口,返排氮气,以使油页岩储层形成一系列相互连通的缝网。本申请既能够实现油页岩中的干酪根转化为油气资源,又能够有效提高油页岩储层的渗透性,可以实现油页岩大规模原位开采。

Figure 201910117012

The present application provides a method and device for intermittently fracturing oil shale in situ by alternating high and low temperature fluids. The method includes the following steps: fracturing an oil shale reservoir with a high temperature fluid, so as to make the oil shale reservoir An artificial main fracture of predetermined length is created. The high temperature fluid is stopped from fracturing the oil shale reservoir, the high temperature fluid is allowed to heat the oil shale reservoir, and after the first predetermined time is reached, the high temperature fluid is flown back. Liquid nitrogen is used to fracturing oil shale reservoirs to generate secondary fractures on both sides of artificial main fractures, while liquid nitrogen gasification produces nitrogen gas, which in turn produces multi-level fractures on both sides of secondary fractures. The wellhead is closed, and after reaching a second predetermined time, the wellhead is opened to flow back nitrogen, so that a series of interconnected fracture networks are formed in the oil shale reservoir. The present application can not only realize the transformation of kerogen in oil shale into oil and gas resources, but also can effectively improve the permeability of oil shale reservoir, and can realize large-scale in-situ mining of oil shale.

Figure 201910117012

Description

高低温流体交替压裂间断原位开采油页岩的方法及装置Method and device for intermittent in-situ production of oil shale by alternating fracturing of high and low temperature fluids

技术领域technical field

本申请属于油页岩储层水力压裂技术领域,特别涉及一种利用高低温流体交替压裂间断原位开采油页岩的方法及装置。The application belongs to the technical field of hydraulic fracturing of oil shale reservoirs, and in particular relates to a method and a device for in-situ production of oil shale using alternating fracturing discontinuities of high and low temperature fluids.

背景技术Background technique

目前,我国油页岩开采技术相对落后,油页岩开发基本上全部采用地上干馏技术,油收率低,难以满足大规模开发应用,且污染问题突出。因此,相关学者开展了油页岩地下干馏技术的攻关研究,以促进油页岩的大规模开发和利用。由于油页岩比较致密,渗透率极低,油页岩储层中的干酪根在地下经过热解之后产生的可开采的油气资源很难通过储层进入井筒,因此,需要对油页岩储层进行改造。水力压裂技术是目前对非常规油气储层进行有效改造最常用的手段,因此可以采用水力压裂技术对油页岩储层进行改造。油页岩储层一般埋藏比较深,在地层高温高压的作用下,油页岩会表现出热塑性,因此,常规水力压裂在油页岩储层中产生的水力裂缝比较单一,储层改造效果不好。At present, my country's oil shale mining technology is relatively backward, and oil shale development basically adopts above-ground dry distillation technology. The oil yield is low, it is difficult to meet the large-scale development and application, and the pollution problem is prominent. Therefore, relevant scholars have carried out research on the underground dry distillation technology of oil shale to promote the large-scale development and utilization of oil shale. Because the oil shale is relatively tight and has extremely low permeability, it is difficult for the recoverable oil and gas resources generated by the kerogen in the oil shale reservoir to enter the wellbore through the reservoir after being pyrolyzed underground. layers are remodeled. Hydraulic fracturing technology is currently the most commonly used method for effective stimulation of unconventional oil and gas reservoirs. Therefore, hydraulic fracturing technology can be used to stimulate oil shale reservoirs. Oil shale reservoirs are generally buried deep. Under the action of high temperature and high pressure in the formation, oil shale will show thermoplasticity. Therefore, the hydraulic fractures generated by conventional hydraulic fracturing in oil shale reservoirs are relatively simple, and the effect of reservoir stimulation is relatively simple. not good.

发明内容SUMMARY OF THE INVENTION

为了克服现有技术的上述缺陷,本发明所要解决的技术问题是提供一种高低温流体交替压裂间断原位开采油页岩的方法及装置,其既能够实现油页岩中的干酪根转化为油气资源,又能够有效提高油页岩储层的渗透性,可以实现油页岩大规模原位开采。In order to overcome the above-mentioned defects of the prior art, the technical problem to be solved by the present invention is to provide a method and device for in-situ production of oil shale by alternating fracturing of high and low temperature fluids, which can not only realize kerogen transformation in oil shale For oil and gas resources, it can effectively improve the permeability of oil shale reservoirs, and can realize large-scale in-situ mining of oil shale.

本发明的具体技术方案是:The concrete technical scheme of the present invention is:

本发明提供一种高低温流体交替压裂间断原位开采油页岩的方法,包括如下步骤:The invention provides a method for producing oil shale in situ by alternating fracturing of high and low temperature fluids, comprising the following steps:

采用高温流体对油页岩储层进行压裂,以使所述油页岩储层产生预定长度的人工主裂缝;fracturing the oil shale reservoir with high temperature fluid, so that the oil shale reservoir produces artificial main fractures of predetermined length;

停止高温流体压裂所述油页岩储层,并使高温流体加热所述油页岩储层,在达到第一预定时间后,返排高温流体;Stop the high temperature fluid fracturing the oil shale reservoir, make the high temperature fluid heat the oil shale reservoir, and after reaching a first predetermined time, flow back the high temperature fluid;

采用液氮对所述油页岩储层进行压裂,以使所述人工主裂缝两侧产生次级裂缝,同时液氮气化产生氮气,进而使所述次级裂缝两侧产生多级裂缝;Fracturing the oil shale reservoir with liquid nitrogen, so that secondary fractures are generated on both sides of the artificial primary fracture, and nitrogen gas is generated by gasification of liquid nitrogen, thereby generating multi-level fractures on both sides of the secondary fracture;

封闭井口,在达到第二预定时间后,开启井口,返排氮气,以使所述油页岩储层形成一系列相互连通的缝网。The wellhead is closed, and after reaching a second predetermined time, the wellhead is opened to flow back nitrogen, so that the oil shale reservoir forms a series of interconnected fracture networks.

在一个优选的实施方式中,在所述油页岩储层形成一系列相互连通的缝网后,对所述油页岩储层进行第一次开采。In a preferred embodiment, after the oil shale reservoir forms a series of interconnected fracture networks, the oil shale reservoir is first produced.

在一个优选的实施方式中,在对所述油页岩储层进行第一次开采后,继续采用高温流体对油页岩储层进行压裂,以使所述人工主裂缝继续向前延伸;In a preferred embodiment, after the oil shale reservoir is produced for the first time, the oil shale reservoir is continuously fractured with high temperature fluid, so that the artificial main fracture continues to extend forward;

停止高温流体压裂所述油页岩储层,并使高温流体加热所述油页岩储层,在达到第一预定时间后,返排高温流体;Stop the high temperature fluid fracturing the oil shale reservoir, make the high temperature fluid heat the oil shale reservoir, and after reaching a first predetermined time, flow back the high temperature fluid;

采用液氮对所述油页岩储层进行压裂,以使向前延伸的人工主裂缝两侧产生次级裂缝,同时液氮气化产生氮气,进而使次级裂缝两侧产生多级裂缝;Fracturing the oil shale reservoir with liquid nitrogen, so that secondary fractures are generated on both sides of the artificial main fracture extending forward, and nitrogen gas is generated by the gasification of liquid nitrogen, thereby generating multi-level fractures on both sides of the secondary fracture;

封闭井口,在达到第二预定时间后,开启井口,返排氮气,以使所述油页岩储层进一步形成相互连通的缝网;closing the wellhead, and after reaching the second predetermined time, opening the wellhead to flow back nitrogen, so that the oil shale reservoir further forms a network of interconnected fractures;

在所述油页岩储层进一步形成相互连通的缝网后,对所述油页岩储层进行第二次开采。After the oil shale reservoir further forms an interconnected fracture network, the oil shale reservoir is produced for the second time.

在一个优选的实施方式中,所述预定长度根据所述油页岩储层中产油物质的含量而定。In a preferred embodiment, the predetermined length is determined according to the content of oil-producing substances in the oil shale reservoir.

在一个优选的实施方式中,所述液氮的温度为-196℃。In a preferred embodiment, the temperature of the liquid nitrogen is -196°C.

在一个优选的实施方式中,所述高温流体的温度在300-500℃之间。In a preferred embodiment, the temperature of the high temperature fluid is between 300-500°C.

在一个优选的实施方式中,所述高温流体为过热蒸汽。In a preferred embodiment, the high temperature fluid is superheated steam.

在一个优选的实施方式中,所述第一预定时间取决于所述油页岩储层中干酪根热解速率。In a preferred embodiment, the first predetermined time depends on the pyrolysis rate of kerogen in the oil shale reservoir.

在一个优选的实施方式中,所述第二预定时间为7天。In a preferred embodiment, the second predetermined period of time is 7 days.

另外,本发明还提供一种采用上述任一项所述的高低温流体交替压裂间断原位开采油页岩的方法的高低温流体交替压裂间断原位开采油页岩的装置,包括:In addition, the present invention also provides a device for in-situ production of oil shale with alternating high and low temperature fluid fracturing and discontinuous in-situ production of oil shale using any of the above-mentioned methods for alternately fracturing and intermittently producing oil shale with high and low temperature fluids, including:

第一压裂模块,其被配置为采用高温流体对油页岩储层进行压裂,以使所述油页岩储层产生预定长度的人工主裂缝;a first fracturing module configured to fracturing an oil shale reservoir with a high temperature fluid to create an artificial primary fracture of a predetermined length in the oil shale reservoir;

加热模块,其被配置为停止高温流体压裂所述油页岩储层,并使高温流体加热所述油页岩储层,在达到第一预定时间后,返排高温流体;a heating module configured to stop the high temperature fluid fracturing the oil shale reservoir, make the high temperature fluid heat the oil shale reservoir, and after reaching a first predetermined time, flow back the high temperature fluid;

第二压裂模块,其被配置为采用液氮对所述油页岩储层进行压裂,以使所述人工主裂缝两侧产生次级裂缝,同时液氮气化产生氮气,进而使次级裂缝两侧产生多级裂缝;The second fracturing module is configured to use liquid nitrogen to fract the oil shale reservoir, so as to generate secondary fractures on both sides of the artificial main fracture, and simultaneously gasify the liquid nitrogen to generate nitrogen, thereby causing the secondary fractures There are multi-level cracks on both sides of the crack;

连通模块,其被配置为封闭井口,在达到第二预定时间后,开启井口,返排氮气,以使所述油页岩储层形成一系列相互连通的缝网。The communication module is configured to close the wellhead, and after reaching the second predetermined time, open the wellhead and flow back nitrogen gas, so that the oil shale reservoir forms a series of interconnected fracture networks.

另外,本发明还提供一种高低温流体交替压裂间断原位开采油页岩的装置,包括存储器和处理器,存储器中存储计算机程序,所述计算机程序在被所述处理器执行时,实现以下步骤:如上述任一项所述的高低温流体交替压裂间断原位开采油页岩的方法。In addition, the present invention also provides a device for intermittently fracturing oil shale in situ alternately with high and low temperature fluids, comprising a memory and a processor, wherein a computer program is stored in the memory, and when the computer program is executed by the processor, the The following steps: the method for producing oil shale in situ by alternate fracturing of high and low temperature fluids as described in any of the above.

借由以上的技术方案,本申请的有益效果在于:By the above technical solutions, the beneficial effects of the present application are:

本发明采用高温流体压裂,既能够产生较长的人工裂缝,又能够加热油页岩促使裂缝周围油页岩中的干酪根转化为油气资源。采用低温流体压裂,能够在已经形成的裂缝两侧产生次级裂缝和/或多级裂缝,为开采油气资源提供必要的渗流通道。在完成每一次高低温流体压裂后,均进行一段时间的开采,能够避免再次注入的高低温流体对已经形成的油气资源造成污染。The invention adopts high temperature fluid fracturing, which can not only generate long artificial fractures, but also heat the oil shale to promote the kerogen in the oil shale around the fractures to be converted into oil and gas resources. Using low-temperature fluid fracturing can generate secondary fractures and/or multi-level fractures on both sides of the formed fractures, providing necessary seepage channels for the exploitation of oil and gas resources. After each high and low temperature fluid fracturing is completed, the exploitation is carried out for a period of time, which can avoid the pollution of the formed oil and gas resources caused by the high and low temperature fluid injected again.

本发明提供的利用高低温流体交替压裂间断原位开采油页岩的方法及装置,既能够实现油页岩中的干酪根转化为油气资源,又能够有效提高油页岩储层的渗透性,通过高低温流体交替压裂能够不断增大油页岩储层改造范围,通过间断开采不断提高采收率,为实现油页岩大规模原位开采提供理论依据。The method and device for in-situ production of oil shale by utilizing high and low temperature fluids alternately fracturing discontinuities provided by the present invention can not only realize the transformation of kerogen in oil shale into oil and gas resources, but also effectively improve the permeability of oil shale reservoirs , through the alternating fracturing of high and low temperature fluids, the stimulation range of oil shale reservoirs can be continuously increased, and the recovery rate can be continuously improved by intermittent mining, which provides a theoretical basis for realizing large-scale in-situ mining of oil shale.

参照后文的说明和附图,详细公开了本申请的特定实施方式,指明了本申请的原理可以被采用的方式。应该理解,本申请的实施方式在范围上并不因而受到限制。在所附权利要求的精神和条款的范围内,本申请的实施方式包括许多改变、修改和等同。With reference to the following description and drawings, specific embodiments of the present application are disclosed in detail, indicating the manner in which the principles of the present application may be employed. It should be understood that the embodiments of the present application are not thereby limited in scope. Embodiments of the present application include many changes, modifications and equivalents within the spirit and scope of the appended claims.

针对一种实施方式描述和/或示出的特征可以以相同或类似的方式在一个或更多个其它实施方式中使用,与其它实施方式中的特征相组合,或替代其它实施方式中的特征。Features described and/or illustrated for one embodiment may be used in the same or similar manner in one or more other embodiments, in combination with, or instead of features in other embodiments .

应该强调,术语“包括/包含”在本文使用时指特征、整件、步骤或组件的存在,但并不排除一个或更多个其它特征、整件、步骤或组件的存在或附加。It should be emphasized that the term "comprising/comprising" when used herein refers to the presence of a feature, integer, step or component, but does not exclude the presence or addition of one or more other features, integers, steps or components.

附图说明Description of drawings

在此描述的附图仅用于解释目的,而不意图以任何方式来限制本申请公开的范围。另外,图中的各部件的形状和比例尺寸等仅为示意性的,用于帮助对本申请的理解,并不是具体限定本申请各部件的形状和比例尺寸。本领域的技术人员在本申请的教导下,可以根据具体情况选择各种可能的形状和比例尺寸来实施本申请。在附图中:The drawings described herein are for explanatory purposes only and are not intended to limit the scope of the present disclosure in any way. In addition, the shapes and proportions of the components in the figures are only schematic and are used to help the understanding of the present application, and do not specifically limit the shapes and proportions of the components of the present application. Under the teachings of the present application, those skilled in the art can select various possible shapes and proportions according to specific conditions to implement the present application. In the attached image:

图1为本申请实施方式的高低温流体交替压裂间断原位开采油页岩的方法流程图;1 is a flow chart of a method for producing oil shale in situ by alternating high and low temperature fluid fracturing intermittently according to an embodiment of the application;

图2为本申请实施方式的高低温流体交替压裂间断原位开采油页岩的装置模块图;2 is a block diagram of a device for intermittently producing oil shale in situ by alternating high and low temperature fluid fracturing according to an embodiment of the application;

图3为本发明高温油页岩储层中垂直于井筒方向的人工裂缝示意图;3 is a schematic diagram of an artificial fracture perpendicular to the wellbore direction in the high-temperature oil shale reservoir of the present invention;

图4为本发明液氮辅助压裂多级裂缝示意图。FIG. 4 is a schematic diagram of the liquid nitrogen-assisted fracturing multi-stage fracture of the present invention.

以上附图的附图标记:1、人工主裂缝;2、井筒;3、多级裂缝;4、压裂管柱;5、次级裂缝;6、三级裂缝;7、四级裂缝;8、n级裂缝。Reference numerals of the above drawings: 1, artificial main fracture; 2, wellbore; 3, multi-level fracture; 4, fracturing string; 5, secondary fracture; 6, tertiary fracture; 7, quaternary fracture; 8 , n-level cracks.

具体实施方式Detailed ways

下面将结合本申请实施方式中的附图,对本申请实施方式中的技术方案进行清楚、完整地描述,显然,所描述的实施方式仅仅是本申请一部分实施方式,而不是全部的实施方式。基于本申请中的实施方式,本领域普通技术人员在没有作出创造性劳动前提下所获得的所有其他实施方式,都属于本申请保护的范围。The technical solutions in the embodiments of the present application will be clearly and completely described below with reference to the accompanying drawings in the embodiments of the present application. Obviously, the described embodiments are only a part of the embodiments of the present application, but not all of the embodiments. Based on the embodiments in the present application, all other embodiments obtained by those of ordinary skill in the art without creative work fall within the protection scope of the present application.

需要说明的是,当元件被称为“设置于”另一个元件,它可以直接在另一个元件上或者也可以存在居中的元件。当一个元件被认为是“连接”另一个元件,它可以是直接连接到另一个元件或者可能同时存在居中元件。本文所使用的术语“垂直的”、“水平的”、“左”、“右”以及类似的表述只是为了说明的目的,并不表示是唯一的实施方式。It should be noted that when an element is referred to as being "disposed on" another element, it can be directly on the other element or intervening elements may also be present. When an element is referred to as being "connected" to another element, it can be directly connected to the other element or intervening elements may also be present. The terms "vertical", "horizontal", "left", "right" and similar expressions used herein are for the purpose of illustration only and do not represent the only embodiment.

除非另有定义,本文所使用的所有的技术和科学术语与属于本申请的技术领域的技术人员通常理解的含义相同。本文中在本申请的说明书中所使用的术语只是为了描述具体的实施方式的目的,不是旨在于限制本申请。本文所使用的术语“和/或”包括一个或多个相关的所列项目的任意的和所有的组合。Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the technical field to which this application belongs. The terms used herein in the specification of the present application are for the purpose of describing particular embodiments only, and are not intended to limit the present application. As used herein, the term "and/or" includes any and all combinations of one or more of the associated listed items.

如图1所示,本发明的实施方式提供一种高低温流体交替压裂间断原位开采油页岩的方法,该方法包括如下步骤:As shown in FIG. 1 , an embodiment of the present invention provides a method for intermittently fracturing oil shale in situ by alternating high and low temperature fluids. The method includes the following steps:

S1:采用高温流体对油页岩储层进行压裂,以使所述油页岩储层产生预定长度的人工主裂缝1;S1: fracturing an oil shale reservoir with a high-temperature fluid, so that an artificial main fracture 1 of a predetermined length is generated in the oil shale reservoir;

S2:停止高温流体压裂所述油页岩储层,并使高温流体加热所述油页岩储层,在达到第一预定时间后,返排高温流体;S2: stop the high-temperature fluid fracturing the oil shale reservoir, make the high-temperature fluid heat the oil shale reservoir, and flow back the high-temperature fluid after reaching a first predetermined time;

S3:采用液氮对所述油页岩储层进行压裂,以使所述人工主裂缝1两侧产生次级裂缝5,进而使次级裂缝5两侧产生多级裂缝3;S3: fracturing the oil shale reservoir with liquid nitrogen, so that secondary fractures 5 are generated on both sides of the artificial primary fracture 1, and then multi-level fractures 3 are generated on both sides of the secondary fracture 5;

S4:封闭井口,在达到第二预定时间后,开启井口,返排氮气,以使所述油页岩储层形成一系列相互连通的缝网。S4: The wellhead is closed, and after the second predetermined time is reached, the wellhead is opened to flow back nitrogen, so that the oil shale reservoir forms a series of interconnected fracture networks.

在本实施方式中,如图3和图4所示,首先利用压裂管柱4向井筒2内注入高温流体,以对油页岩储层进行压裂。所述高温流体可以为过热蒸汽,且其温度可以在300-500℃之间,这样该油页岩储层会产生一条预定长度的人工主裂缝1。在通常情况下,该人工主裂缝1垂直于地层最小主地应力方向。所述预定长度需要根据油页岩储层中干酪根等产油物质的含量而定。例如,如果储层产油物质含量较高,那么预定长度可以短一些。但是预定长度的最低要求是,储层在经过预定长度的高低温流体压裂之后,得到的可采油气资源具有开采价值。In this embodiment, as shown in FIG. 3 and FIG. 4 , firstly, high-temperature fluid is injected into the wellbore 2 by using the fracturing string 4 to fract the oil shale reservoir. The high temperature fluid can be superheated steam, and its temperature can be between 300-500°C, so that the oil shale reservoir will generate an artificial main fracture 1 with a predetermined length. Under normal circumstances, the artificial main fracture 1 is perpendicular to the direction of the minimum main in-situ stress of the formation. The predetermined length needs to be determined according to the content of oil-producing substances such as kerogen in the oil shale reservoir. For example, if the reservoir has a higher oil-producing material content, the predetermined length may be shorter. However, the minimum requirement of the predetermined length is that the recoverable oil and gas resources obtained after the reservoir is fracturing with high and low temperature fluids of the predetermined length have the exploitation value.

然后,需要停泵静置,使得高温流体加热周围油页岩储层,且加热的过程需要维持第一预定时间,这样能够充分加热人工主裂缝1周围的油页岩,促进油页岩中的干酪根转化为油气资源。在到达第一预定时间后,需要返排高温流体,避免随后注入的液氮的超低温作用造成高温流体发生相变,导致人工主裂缝1堵塞。需要进行说明的是,所述第一预定时间取决于所述油页岩储层中干酪根热解速率。Then, the pump needs to be stopped to stand still, so that the high-temperature fluid heats the surrounding oil shale reservoir, and the heating process needs to be maintained for a first predetermined time, which can fully heat the oil shale around the artificial main fracture 1 and promote the oil shale in the oil shale. Kerogen is converted into oil and gas resources. After reaching the first predetermined time, the high-temperature fluid needs to be flowed back to avoid the phase transition of the high-temperature fluid caused by the ultra-low temperature action of the subsequently injected liquid nitrogen, resulting in the blockage of the artificial main fracture 1 . It should be noted that the first predetermined time depends on the pyrolysis rate of kerogen in the oil shale reservoir.

在返排高温流体结束后,采用液氮对所述油页岩储层进行压裂,液氮可以通过压裂管柱4注入井筒2后,会进入人工主裂缝1,人工主裂缝1两侧的高温油页岩在液氮的超低温作用下(-196℃)会产生巨大的热应力,使得其两侧高温油页岩(300℃)破裂产生次级裂缝5。同时液氮气化产生高压氮气促进次级裂缝5再次延伸,进而使次级裂缝5两侧产生多级裂缝3。该多级裂缝3可以包括次级裂缝5周围的三级裂缝6,三级裂缝6周围的四级裂缝7,以此类推,(n-1)级裂缝周围的n级裂缝8,其中n≥2,且n为正整数。例如,在特殊情况下,当n=2时,(n-1)级裂缝为人工主裂缝1,n级裂缝8为次级裂缝5。需要强调的是,此时人工主裂缝1在液氮的作用下,也会稍微向前延伸一部分,进而次级裂缝5和多级裂缝3的产生也是同时发生的。After the high temperature fluid flowback is completed, the oil shale reservoir is fracturing with liquid nitrogen. After the liquid nitrogen can be injected into the wellbore 2 through the fracturing string 4, it will enter the artificial main fracture 1, and the two sides of the artificial main fracture 1 Under the ultra-low temperature of liquid nitrogen (-196 °C), the high-temperature oil shale will generate huge thermal stress, causing the high-temperature oil shale (300 °C) on both sides to rupture and produce secondary fractures5. At the same time, the high-pressure nitrogen gas generated by the liquid nitrogen gasification promotes the re-extension of the secondary crack 5, thereby causing multi-level cracks 3 on both sides of the secondary crack 5. The multi-level cracks 3 may include tertiary cracks 6 around the secondary cracks 5, quaternary cracks 7 around the tertiary cracks 6, and so on, n-level cracks 8 around the (n-1) level cracks, where n≥ 2, and n is a positive integer. For example, in a special case, when n=2, the (n-1)-level fracture is the artificial primary fracture 1, and the n-level fracture 8 is the secondary fracture 5. It should be emphasized that at this time, under the action of liquid nitrogen, the artificial main crack 1 will also slightly extend forward, and the secondary crack 5 and the multi-level crack 3 also occur simultaneously.

最后,需要封闭井口静置,待液氮全部转化为氮气,会进一步促进裂缝延伸,在达到第二预定时间(大约7天左右)后,开启井口,返排氮气,既能避免氮气污染油气资源,又能降低缝网内的压力,便于油气资源在缝网中流动。这样最终可以形成一系列相互连通的复杂缝网。Finally, it is necessary to close the wellhead and let it stand. After the liquid nitrogen is completely converted into nitrogen, it will further promote fracture extension. After reaching the second predetermined time (about 7 days), the wellhead is opened to flow back nitrogen, which can avoid nitrogen pollution of oil and gas resources. It can also reduce the pressure in the fracture network and facilitate the flow of oil and gas resources in the fracture network. This can eventually form a series of interconnected complex seam networks.

在所述油页岩储层形成一系列相互连通的缝网后,需对所述油页岩储层进行第一次开采,避免再次注入的高低温流体对已经形成的油气资源造成污染。此处的污染不仅包括氮气、高温流体等外来物质对油气资源的污染,还包括温度作用对已产生的油气资源成分的影响,以及再次注入高低温流体压裂后返排压裂物质时将油气资源携带出去造成油气资源损失。After a series of interconnected fracture networks are formed in the oil shale reservoir, the oil shale reservoir needs to be exploited for the first time, so as to avoid the re-injected high and low temperature fluids from polluting the formed oil and gas resources. The pollution here includes not only the contamination of oil and gas resources by foreign substances such as nitrogen and high-temperature fluids, but also the influence of temperature on the composition of the oil and gas resources that have been generated, and the oil and gas will be removed when the fracturing material is re-injected with high-low temperature fluids after fracturing. Carrying out resources will cause the loss of oil and gas resources.

在对所述油页岩储层进行第一次开采后,重复上述步骤,继续采用高温流体对油页岩储层进行压裂,以使所述人工主裂缝1继续向前延伸。然后停止高温流体压裂所述油页岩储层,并使高温流体加热所述油页岩储层,在达到第一预定时间后,返排高温流体。接着,采用液氮对所述油页岩储层进行压裂,以使向前延伸的人工主裂缝1两侧产生新的次级裂缝5,同时液氮气化产生氮气,进而使新的次级裂缝5两侧产生多级裂缝3。最后封闭井口,在达到第二预定时间后,开启井口,返排氮气,以使所述油页岩储层进一步形成相互连通的缝网。在所述油页岩储层进一步形成相互连通的缝网后,对所述油页岩储层进行第二次开采。采用间歇式开采能够最大程度地避免上述污染情况发生。此处的间歇式开采包括第一次开采、第二次开采,和如若需要以后重复步骤中的开采方式。After the first exploitation of the oil shale reservoir, the above steps are repeated, and the oil shale reservoir is continuously fracturing with high temperature fluid, so that the artificial main fracture 1 continues to extend forward. Then stop the high temperature fluid fracturing the oil shale reservoir, make the high temperature fluid heat the oil shale reservoir, and after reaching the first predetermined time, the high temperature fluid is flowed back. Next, fracturing the oil shale reservoir with liquid nitrogen, so that new secondary fractures 5 are generated on both sides of the artificial main fracture 1 extending forward, and simultaneously the liquid nitrogen is gasified to generate nitrogen, thereby causing new secondary fractures Multi-level cracks 3 are generated on both sides of the crack 5 . Finally, the wellhead is closed, and after reaching the second predetermined time, the wellhead is opened to flow back nitrogen, so that the oil shale reservoir further forms a network of interconnected fractures. After the oil shale reservoir further forms an interconnected fracture network, the oil shale reservoir is produced for the second time. The use of intermittent mining can minimize the occurrence of the above-mentioned pollution. The intermittent mining here includes the first mining, the second mining, and the mining mode in the subsequent steps repeated if necessary.

进一步地,还可以再次重复上述步骤,利用高低温流体交替压裂间断原位开采油页岩,这样可以不断增大油页岩储层的改造范围,不断提高油页岩的采收率。Further, the above steps can be repeated again, and the oil shale can be produced in situ by alternate fracturing of high and low temperature fluids, which can continuously increase the stimulation range of the oil shale reservoir and continuously improve the recovery rate of the oil shale.

如上所述的利用高低温流体交替压裂间断原位开采油页岩的方法,其中,在完成每一次油气开采之后,需要再次注入高温流体压裂,新的人工主裂缝1会在已有人工主裂缝1的基础上再次进行延伸,从而可以增大储层改造范围。接着再次注入液氮压裂,新的人工主裂缝1两侧会产生次级裂缝5和/或多级裂缝3,可以增加油气资源渗流通道。The method for in-situ production of oil shale using alternating fracturing of high and low temperature fluids as described above, wherein, after each oil and gas exploitation is completed, it is necessary to inject high temperature fluid for fracturing again, and the new artificial main fracture 1 will be in the existing artificial fracture. On the basis of the main fracture 1, it is extended again, so that the scope of reservoir stimulation can be enlarged. Then the liquid nitrogen is injected for fracturing again, and secondary fractures 5 and/or multi-level fractures 3 will be generated on both sides of the new artificial main fracture 1, which can increase the seepage channels of oil and gas resources.

本发明的高低温流体交替压裂间断原位开采油页岩的方法采用先注高温流体再注液氮压裂主要有两个方面的原因。其一,先注入高温流体能够给油页岩储层进行加热,使得压裂区域油页岩达到较高的温度,既能够促进油页岩中的干酪根等转化为可采油气资源,又能够获得与液氮温度相差很大的温度差,从而可以提高液氮压裂过程中产生的热应力,产生更多分支裂缝。In the method of the present invention for fracturing intermittently in situ oil shale by alternating high and low temperature fluids, there are two main reasons for first injecting high temperature fluid and then injecting liquid nitrogen for fracturing. First, injecting high-temperature fluid first can heat the oil shale reservoir, so that the oil shale in the fracturing area can reach a higher temperature, which can not only promote the transformation of kerogen in the oil shale into recoverable oil and gas resources, but also enable the oil shale to reach a higher temperature. A temperature difference that is very different from the liquid nitrogen temperature can be obtained, so that the thermal stress generated during the liquid nitrogen fracturing process can be increased, and more branched fractures can be generated.

其二,如果先注入液氮压裂会在井筒周围产生许多方向随机的细小裂缝,后注入高温流体进行压裂时,压裂液首先进入液氮压裂得到细小裂缝中,沿着细小裂缝扩展,不易形成较长的人工主裂缝1,导致压裂改造区域小。先注入高温流体压裂能够首先获得较长的人工主裂缝1,再注入液氮能够在人工主裂缝1周围产生细小裂缝,即能够增大改造区域,又能够提高压裂改造效果。Second, if liquid nitrogen is injected for fracturing first, many small fractures with random directions will be generated around the wellbore. When high-temperature fluid is injected later for fracturing, the fracturing fluid will first enter the liquid nitrogen fracturing to obtain small fractures and expand along the small fractures. , it is not easy to form a long artificial main fracture 1, resulting in a small fracturing area. Injecting high-temperature fluid for fracturing first can obtain long artificial main fractures 1 first, and then injecting liquid nitrogen can generate small fractures around artificial main fractures 1, which can not only increase the reformed area, but also improve the fracturing effect.

而且,本申请的高低温流体交替压裂间断原位开采油页岩的方法得到的人工主裂缝1两侧分支裂缝少,长度便于控制,而直接采用液氮压裂得到的人工裂缝长度很难进行控制。这是由于首先采用高温流体对油页岩储层进行压裂,人工裂缝扩展主要受地层三向应力控制,此时产生的人工主裂缝1垂直于地层最小主地应力方向,因此可以根据压裂液排量、现场施工压力曲线以及地层岩石力学性质参数等估算人工裂缝的长度。而采用液氮直接进行压裂,得到的人工裂缝包括原来人工主裂缝1的延伸和多级分支裂缝的产生,其中,人工主裂缝1的延伸和多级分支裂缝的产生是同时发生的,分支裂缝产生的原因主要是热应力和流体压力的作用。Moreover, the artificial main fracture 1 obtained by the method for intermittently producing oil shale in situ by alternating high and low temperature fluid fracturing of the present application has few branch fractures on both sides, and the length is easy to control, while the length of the artificial fracture obtained directly by liquid nitrogen fracturing is difficult to achieve Take control. This is because the high temperature fluid is used to fracturing the oil shale reservoir first, and the expansion of artificial fractures is mainly controlled by the three-dimensional stress of the formation. The length of artificial fractures is estimated by the liquid displacement, on-site construction pressure curve, and mechanical properties of formation rock. The artificial fractures obtained by direct fracturing with liquid nitrogen include the extension of the original main artificial fracture 1 and the generation of multi-level branched fractures. The cause of cracks is mainly the effect of thermal stress and fluid pressure.

另外,基于同一发明构思,本发明实施例中还提供了一种高低温流体交替压裂间断原位开采油页岩的装置,如下面的实施例所述。由于一种高低温流体交替压裂间断原位开采油页岩的装置解决问题的原理与一种高低温流体交替压裂间断原位开采油页岩的方法相似,因此高低温流体交替压裂间断原位开采油页岩的装置的实施可以参见高低温流体交替压裂间断原位开采油页岩的方法的实施,重复之处不再赘述。以下所使用的,术语“单元”或者“模块”可以实现预定功能的软件和/或硬件的组合。尽管以下实施例所描述的装置较佳地以软件来实现,但是硬件,或者软件和硬件的组合的实现也是可能并被构想的。In addition, based on the same inventive concept, the embodiments of the present invention also provide a device for intermittently fracturing and intermittently producing oil shale in situ with high and low temperature fluids, as described in the following embodiments. Because the principle of a device for intermittently producing oil shale by alternating high and low temperature fluid fracturing is similar to that of a method for intermittently producing oil shale in situ by alternating high and low temperature fluid fracturing. For the implementation of the device for in-situ production of oil shale, reference may be made to the implementation of the method for intermittent in-situ production of oil shale by alternating high and low temperature fluid fracturing, and the repetition will not be repeated. As used below, the term "unit" or "module" may be a combination of software and/or hardware that implements a predetermined function. Although the apparatus described in the following embodiments is preferably implemented in software, implementations in hardware, or a combination of software and hardware, are also possible and contemplated.

如图2所示,本申请的实施例中还提供一种高低温流体交替压裂间断原位开采油页岩的装置,该装置包括:As shown in FIG. 2 , an embodiment of the present application also provides a device for intermittently fracturing and intermittently producing oil shale in situ with high and low temperature fluids. The device includes:

第一压裂模块101,其被配置为采用高温流体对油页岩储层进行压裂,以使所述油页岩储层产生预定长度的人工主裂缝1。The first fracturing module 101 is configured to fract the oil shale reservoir with high temperature fluid, so that the oil shale reservoir generates artificial main fractures 1 of predetermined length.

加热模块102,其被配置为停止高温流体压裂所述油页岩储层,并使高温流体加热所述油页岩储层,在达到第一预定时间后,返排高温流体。The heating module 102 is configured to stop the high temperature fluid from fracturing the oil shale reservoir, to cause the high temperature fluid to heat the oil shale reservoir, and to flow back the high temperature fluid after a first predetermined time.

第二压裂模块103,其被配置为采用液氮对所述油页岩储层进行压裂,以使所述人工主裂缝1两侧产生次级裂缝5,同时液氮气化产生氮气,进而使次级裂缝5两侧产生多级裂缝3。The second fracturing module 103 is configured to use liquid nitrogen to fract the oil shale reservoir, so as to generate secondary fractures 5 on both sides of the artificial main fracture 1, and simultaneously gasify the liquid nitrogen to generate nitrogen gas, and further Multi-level cracks 3 are generated on both sides of the secondary crack 5 .

连通模块104,其被配置为封闭井口,在达到第二预定时间后,开启井口,返排氮气,以使所述油页岩储层形成一系列相互连通的缝网。The communication module 104, which is configured to close the wellhead, open the wellhead after a second predetermined time period, and flow back nitrogen gas to form a series of interconnected fracture networks in the oil shale reservoir.

在优选的实施方式中,该装置还包括第一开采模块,其被配置为在所述油页岩储层形成一系列相互连通的缝网后,对所述油页岩储层进行第一次开采。In a preferred embodiment, the apparatus further includes a first production module configured to perform a first production run on the oil shale reservoir after the oil shale reservoir forms a series of interconnected fracture networks mining.

在优选的实施方式中,该装置还包括:In a preferred embodiment, the device further comprises:

第三压裂模块,其被配置为在对所述油页岩储层进行第一次开采后,继续采用高温流体对油页岩储层进行压裂,以使所述人工主裂缝1继续向前延伸。The third fracturing module is configured to continue fracturing the oil shale reservoir with high temperature fluid after the first production of the oil shale reservoir, so that the artificial main fracture 1 continues to develop toward the oil shale reservoir. front extension.

继续加热模块,其被配置为停止高温流体压裂所述油页岩储层,并使高温流体加热所述油页岩储层,在达到第一预定时间后,返排高温流体。The continuing heating module is configured to stop the high temperature fluid fracturing the oil shale reservoir, and cause the high temperature fluid to heat the oil shale reservoir, and after a first predetermined time, flow back the high temperature fluid.

第四压裂模块,其被配置为采用液氮对所述油页岩储层进行压裂,以使向前延伸的人工主裂缝1两侧产生次级裂缝5,同时液氮气化产生氮气,进而使次级裂缝5两侧产生多级裂缝3。a fourth fracturing module, which is configured to use liquid nitrogen to fract the oil shale reservoir, so as to generate secondary fractures 5 on both sides of the forward-extending artificial main fracture 1, and simultaneously gasify the liquid nitrogen to generate nitrogen, Further, multi-level cracks 3 are generated on both sides of the secondary crack 5 .

继续连通模块,其被配置为封闭井口,在达到第二预定时间后,开启井口,返排氮气,以使所述油页岩储层进一步形成相互连通的缝网。The continuous communication module is configured to close the wellhead, and after reaching the second predetermined time, open the wellhead and flow back nitrogen gas, so that the oil shale reservoir further forms an interconnected fracture network.

第二开采模块,其被配置为在所述油页岩储层进一步形成相互连通的缝网后,对所述油页岩储层进行第二次开采。The second production module is configured to perform a second production on the oil shale reservoir after the oil shale reservoir is further formed with an interconnected fracture network.

在优选的实施方式中,所述预定长度根据所述油页岩储层中产油物质的含量而定。In a preferred embodiment, the predetermined length is based on the content of oil-producing substances in the oil shale reservoir.

在优选的实施方式中,所述液氮的温度为-196℃。In a preferred embodiment, the temperature of the liquid nitrogen is -196°C.

在优选的实施方式中,所述高温流体的温度在300-500℃之间。In a preferred embodiment, the temperature of the high temperature fluid is between 300-500°C.

在优选的实施方式中,所述高温流体为过热蒸汽。In a preferred embodiment, the high temperature fluid is superheated steam.

在优选的实施方式中,所述第一预定时间取决于所述油页岩储层中干酪根热解速率。In a preferred embodiment, the first predetermined time depends on the rate of kerogen pyrolysis in the oil shale reservoir.

在优选的实施方式中,所述第二预定时间为7天。In a preferred embodiment, the second predetermined period of time is 7 days.

另外,本发明的实施例中还提供一种高低温流体交替压裂间断原位开采油页岩的装置,其包括存储器和处理器,存储器中存储计算机程序,所述计算机程序在被所述处理器执行时,实现以下步骤:如上述任一项所述的高低温流体交替压裂间断原位开采油页岩的方法。In addition, an embodiment of the present invention also provides a device for intermittently fracturing oil shale in situ by alternating high and low temperature fluids, which includes a memory and a processor, and a computer program is stored in the memory, and the computer program is processed by the When the device is executed, the following steps are implemented: the method for intermittently producing oil shale in situ by alternating fracturing of high and low temperature fluids according to any one of the above.

在另外一个实施方式中,还提供了一种软件,该软件用于执行上述实施例及优选实施方式中描述的技术方案。In another embodiment, a software is also provided, and the software is used to execute the technical solutions described in the above embodiments and preferred embodiments.

在另外一个实施方式中,还提供了一种存储介质,该存储介质中存储有上述软件,该存储介质包括但不限于:光盘、软盘、硬盘、可擦写存储器等。In another embodiment, a storage medium is also provided, and the above-mentioned software is stored in the storage medium, and the storage medium includes but is not limited to: an optical disk, a floppy disk, a hard disk, a rewritable memory, and the like.

从以上的描述中,可以看出,本发明实施方式实现了如下技术效果:本发明采用高温流体压裂,既能够产生较长的人工裂缝,又能够加热油页岩促使裂缝周围油页岩中的干酪根转化为油气资源。采用低温流体压裂,能够在已经形成的裂缝两侧产生次级裂缝和/或多级裂缝,为开采油气资源提供必要的渗流通道。在完成每一次高低温流体压裂后,均进行一段时间的开采,能够避免再次注入的高低温流体对已经形成的油气资源造成污染。From the above description, it can be seen that the embodiments of the present invention achieve the following technical effects: the present invention adopts high-temperature fluid fracturing, which can not only generate long artificial fractures, but also heat the oil shale to promote the oil shale around the fractures. of kerogen into oil and gas resources. Using low-temperature fluid fracturing can generate secondary fractures and/or multi-level fractures on both sides of the formed fractures, providing necessary seepage channels for the exploitation of oil and gas resources. After each high and low temperature fluid fracturing is completed, the exploitation is carried out for a period of time, which can avoid the pollution of the formed oil and gas resources caused by the high and low temperature fluid injected again.

本发明提供的利用高低温流体交替压裂间断原位开采油页岩的方法及装置,既能够实现油页岩中的干酪根转化为油气资源,又能够有效提高油页岩储层的渗透性,通过高低温流体交替压裂能够不断增大油页岩储层改造范围,通过间断开采不断提高采收率,为实现油页岩大规模原位开采提供理论依据。The method and device for in-situ production of oil shale by utilizing high and low temperature fluids alternately fracturing discontinuities provided by the present invention can not only realize the transformation of kerogen in oil shale into oil and gas resources, but also effectively improve the permeability of oil shale reservoirs , through the alternating fracturing of high and low temperature fluids, the stimulation range of oil shale reservoirs can be continuously increased, and the recovery rate can be continuously improved by intermittent mining, which provides a theoretical basis for realizing large-scale in-situ mining of oil shale.

显然,本领域的技术人员应该明白,上述的本发明实施例的各模块或各步骤可以用通用的计算装置来实现,它们可以集中在单个的计算装置上,或者分布在多个计算装置所组成的网络上,可选地,它们可以用计算装置可执行的程序代码来实现,从而,可以将它们存储在存储装置中由计算装置来执行,并且在某些情况下,可以以不同于此处的顺序执行所示出或描述的步骤,或者将它们分别制作成各个集成电路模块,或者将它们中的多个模块或步骤制作成单个集成电路模块来实现。这样,本发明实施例不限制于任何特定的硬件和软件结合。Obviously, those skilled in the art should understand that each module or each step of the above-mentioned embodiments of the present invention may be implemented by a general-purpose computing device, and they may be centralized on a single computing device, or distributed in multiple computing devices. network, they can optionally be implemented with program code executable by a computing device, so that they can be stored in a storage device and executed by the computing device, and in some cases, can be different from the The illustrated or described steps are performed in order, either by fabricating them separately into individual integrated circuit modules, or by fabricating multiple modules or steps of them into a single integrated circuit module. As such, embodiments of the present invention are not limited to any particular combination of hardware and software.

以上所述仅为本发明的优选实施例而已,并不用于限制本发明,对于本领域的技术人员来说,本发明实施例可以有各种更改和变化。凡在本发明的精神和原则之内,所作的任何修改、等同替换、改进等,均应包含在本发明的保护范围之内。The above descriptions are only preferred embodiments of the present invention, and are not intended to limit the present invention. For those skilled in the art, various modifications and changes may be made to the embodiments of the present invention. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present invention shall be included within the protection scope of the present invention.

Claims (8)

1. A method for alternately fracturing discontinuous in-situ extraction oil shale by high and low temperature fluids is characterized by comprising the following steps:
fracturing an oil shale reservoir by using high-temperature fluid to enable the oil shale reservoir to generate artificial main fractures with preset lengths;
stopping the high-temperature fluid from fracturing the oil shale reservoir, enabling the high-temperature fluid to heat the oil shale reservoir, and returning the high-temperature fluid after the first preset time is reached;
fracturing the oil shale reservoir by adopting liquid nitrogen to generate secondary cracks on two sides of the artificial main crack, and simultaneously gasifying the liquid nitrogen to generate nitrogen so as to generate multi-stage cracks on two sides of the secondary cracks;
closing the well mouth, opening the well mouth after the second preset time is reached, and back-discharging nitrogen so as to enable the oil shale reservoir to form a series of communicated seam nets; after the oil shale reservoir forms a series of interconnected seam nets, performing first mining on the oil shale reservoir;
after the oil shale reservoir is mined for the first time, continuously fracturing the oil shale reservoir by using high-temperature fluid so as to enable the artificial main fracture to continue to extend forwards;
stopping the high-temperature fluid from fracturing the oil shale reservoir, enabling the high-temperature fluid to heat the oil shale reservoir, and returning the high-temperature fluid after the first preset time is reached;
fracturing the oil shale reservoir by adopting liquid nitrogen to generate secondary cracks on two sides of the artificial main crack extending forwards, and simultaneously gasifying the liquid nitrogen to generate nitrogen so as to generate multi-stage cracks on two sides of the secondary cracks;
closing the well mouth, opening the well mouth after the second preset time is reached, and back-discharging nitrogen so as to further form a mutually communicated seam network in the oil shale reservoir;
after the oil shale reservoir further forms a communicated seam network, performing secondary exploitation on the oil shale reservoir;
the temperature of the high-temperature fluid is between 300 and 500 ℃.
2. The method of claim 1, wherein the predetermined length is determined by the amount of oleaginous matter in the oil shale reservoir.
3. The method of alternately fracturing interrupted in situ recovery oil shale with high and low temperature fluids according to claim 1, wherein the temperature of the liquid nitrogen is-196 ℃.
4. The method of alternately fracturing interrupted in situ recovery oil shale with high and low temperature fluids according to claim 1, wherein the high temperature fluid is superheated steam.
5. The method of alternately fracturing interrupted in situ mined shale with high and low temperature fluids according to claim 1, wherein the first predetermined time is dependent upon a rate of kerogen pyrolysis in the oil shale reservoir.
6. The method of alternately fracturing interrupted in situ recovery oil shale with high and low temperature fluids according to claim 1, wherein the second predetermined time is 7 days.
7. An apparatus for alternately fracturing an interrupted in situ mined oil shale by high and low temperature fluids using the method for alternately fracturing an interrupted in situ mined oil shale as claimed in any one of the preceding claims, comprising:
a first fracturing module configured to fracture an oil shale reservoir with a high temperature fluid to cause the oil shale reservoir to produce artificial primary fractures of a predetermined length;
a heating module configured to stop the high temperature fluid from fracturing the oil shale reservoir and cause the high temperature fluid to heat the oil shale reservoir, the high temperature fluid being flowback after reaching a first predetermined time;
the second fracturing module is configured to fracture the oil shale reservoir by adopting liquid nitrogen so as to generate secondary fractures on two sides of the artificial main fracture, and simultaneously gasify the liquid nitrogen to generate nitrogen gas so as to generate multi-stage fractures on two sides of the secondary fractures;
the communication module is configured to close the well mouth, open the well mouth after a second preset time is reached, and back discharge nitrogen so that the oil shale reservoir forms a series of communicated seam nets;
the temperature of the high-temperature fluid is between 300 and 500 ℃.
8. An apparatus for alternate high and low fluid fracturing of discontinuous in situ produced oil shale, comprising a memory and a processor, the memory having stored therein a computer program which when executed by the processor performs the steps of: a method of alternately fracturing intermittent in situ mined oil shale by high and low temperature fluids as claimed in any of claims 1 to 6.
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