An underground hydrogen storage physicochemical reaction experiment method and device

Abstract

The application discloses a kind of underground hydrogen storage physicochemical reaction experimental method and device.The method comprises: target pressure value and target reaction time are respectively set for each group of experimental samples;The porosity, permeability and component of core are detected, and the component of core powder and the component of formation water and / or underground crude oil are detected;Hydrogen is introduced into core holder, sand pack and liquid storage bottle;When the reaction time of any one group of experimental samples reaches the preset reaction time, the reacted experimental sample is taken out, and the discharged gas is collected;The component change between hydrogen and discharged gas is compared, the porosity change, permeability change and component change before and after core reaction are compared, and the component change before and after core powder reaction and the component change before and after formation water reaction are compared.The method can quantify the contribution rate of different reaction paths to hydrogen loss, obtain the relationship between pressure change and hydrogen consumption, and the influence of time length on hydrogen consumption, to provide technical support for underground hydrogen storage.

Description

Technical Field

[0001] This invention relates to the field of underground hydrogen storage technology, and in particular to an experimental method and apparatus for the physicochemical reaction of underground hydrogen storage. Background Technology

[0002] Hydrogen energy, as a new energy source that does not rely on fossil fuels, is a clean, low-carbon, and widely applicable renewable energy source with advantages such as abundant reserves, good combustion characteristics, high calorific value, and diverse utilization methods. With the increasing demand for hydrogen energy, the storage capacity of hydrogen also urgently needs to be improved.

[0003] Underground hydrogen storage is a method for large-scale hydrogen storage, offering advantages such as low cost, minimal environmental impact, small land use requirements, and low risk of hydrogen leakage. Hydrogen storage in depleted oil and gas fields utilizes the underground space of already extracted oil and gas fields for hydrogen storage, making it particularly suitable for long-term storage needs. Depleted oil and gas fields possess enormous storage capacity and excellent geological sealing. After years of oil and gas extraction, their geological structures have been thoroughly studied and validated, effectively preventing hydrogen leakage. These fields typically have thick caprock (such as mudstone or salt rock), providing reliable sealing conditions to ensure stable hydrogen storage for years to decades. Furthermore, the infrastructure of depleted oil and gas fields (such as wellheads and pipelines) can be modified and reused, significantly reducing development costs. Due to their large scale, excellent sealing, and high economic efficiency, depleted oil and gas fields are considered an ideal choice for achieving large-scale strategic hydrogen reserves and long-term energy transition, particularly suitable for supporting the sustainable development of the future hydrogen economy. Summary of the Invention

[0004] To expand the selection of experimental methods for the physicochemical reactions of underground hydrogen storage and to enhance the study of the physicochemical reaction mechanism of hydrogen with rocks, minerals, and formation water in abandoned oil and gas reservoirs, this invention provides an experimental method and apparatus for the physicochemical reactions of underground hydrogen storage.

[0005] In a first aspect, embodiments of the present invention provide an experimental method for the physicochemical reaction of underground hydrogen storage, comprising:

[0006] Multiple sets of experimental samples were obtained from the target gas storage facility, and target pressure values ​​and target reaction times were set for each set of experimental samples; each set of experimental samples included cores, core powder, and formation water and / or underground crude oil.

[0007] For each set of experimental samples, the porosity, permeability and composition of the core were tested, as well as the composition of the core powder and the composition of formation water and / or underground crude oil.

[0008] For each experimental sample, the core was saturated with formation water and then placed in a core holder. The core powder was placed in a sand-filling tube, and the formation water and / or underground crude oil were placed in a storage bottle.

[0009] For each set of experimental samples, hydrogen gas was simultaneously introduced into the core holder, the sand filling tube, and the liquid storage bottle, and the pressure and temperature inside the core holder, the sand filling tube, and the liquid storage bottle were kept consistent.

[0010] Adjust the pressure of each group of experimental samples to the corresponding target pressure value;

[0011] Once the reaction time of any group of experimental samples reaches the preset reaction time, the experimental samples after the reaction are taken out and the discharged gas is collected.

[0012] The composition of the emitted gas was detected, and for each set of experimental samples taken out, the porosity, permeability and composition of the core were detected again, as well as the composition of the core powder and the composition of formation water and / or underground crude oil.

[0013] For each group of experimental samples, the compositional changes between hydrogen and the emitted gas were compared, as were the changes in porosity, permeability, and composition before and after the core reaction, the compositional changes of the core powder before and after the reaction, and the compositional changes of the formation water before and after the reaction.

[0014] In one or more optional embodiments, the step of acquiring multiple sets of experimental samples from the target gas storage facility and setting target pressure values ​​and target reaction times for each set of experimental samples includes:

[0015] Obtain multiple sets of experimental samples from the target gas storage facility;

[0016] The target pressure values ​​for each group of experimental samples were set according to an arithmetic sequence.

[0017] The target reaction time for each group of experimental samples was set to be the same.

[0018] In one or more optional embodiments, the step of acquiring multiple sets of experimental samples from the target gas storage facility and setting target pressure values ​​and target reaction times for each set of experimental samples includes:

[0019] Obtain multiple sets of experimental samples from the target gas storage facility;

[0020] Set the target pressure value to be the same for each group of experimental samples;

[0021] The target reaction time for each group of experimental samples was set according to an arithmetic sequence.

[0022] In one or more optional embodiments, the step of acquiring multiple sets of experimental samples from the target gas storage facility and setting target pressure values ​​and target reaction times for each set of experimental samples includes:

[0023] Obtain multiple sets of experimental samples from at least five gas storage facilities, including the first set of experimental samples, the second set of experimental samples, the third set of experimental samples, the fourth set of experimental samples, and the fifth set of experimental samples;

[0024] The target pressure values ​​of the first group of experimental samples, the second group of experimental samples, and the third group of experimental samples are set as an arithmetic sequence, and the target reaction times of the first group of experimental samples, the second group of experimental samples, and the third group of experimental samples are set to be the same;

[0025] The target pressure values ​​of the third group of experimental samples, the fourth group of experimental samples, and the fifth group of experimental samples are set to be the same, and the target reaction times of the third group of experimental samples, the fourth group of experimental samples, and the fifth group of experimental samples are set to an arithmetic sequence.

[0026] In one or more alternative embodiments, the step of detecting the porosity, permeability, and composition of the core sample for each group of experimental samples, and detecting the composition of the core powder and the composition of the formation water, includes:

[0027] For each experimental sample, the porosity and permeability of the core were detected by a pressure-controlled permeability device, the mineral composition of the core at a fixed point was detected by a positioning scanning electron microscope, the composition of the core powder was detected by an X-ray diffractometer, and the composition of formation water and / or underground crude oil was detected by a liquid chromatograph.

[0028] In one or more alternative embodiments, the detection of the components of the discharged gas, and, for each set of experimental samples taken out, the re-detection of the porosity, permeability, and composition of the core, and the detection of the composition of the core powder and the composition of formation water and / or underground crude oil, includes:

[0029] The components of the emitted gas are detected by gas chromatography.

[0030] For each set of experimental samples, the porosity and permeability of the core were detected by a pressure-controlled permeability device, the mineral composition of the core at a fixed point was detected by a positioning scanning electron microscope, the composition of the core powder was detected by an X-ray diffractometer, and the composition of the formation water was detected by a liquid chromatograph.

[0031] In one or more alternative embodiments, prior to the steps of detecting the porosity, permeability, and composition of the core sample for each set of experimental samples, and detecting the composition of the core powder and the formation water, the method further includes:

[0032] The core, core powder, and formation water were sterilized.

[0033] In one or more optional embodiments, after simultaneously introducing hydrogen gas into the core holder, the sand-filling tube, and the liquid storage bottle for each group of experimental samples, and ensuring that the pressure and temperature inside the core holder, the sand-filling tube, and the liquid storage bottle are consistent, the method further includes:

[0034] Circulating pressure is applied to the core holders corresponding to each group of experimental samples using a circulating pressure pump.

[0035] In one or more optional embodiments, the underground hydrogen storage physicochemical reaction experimental method further includes:

[0036] The core holder, the sand-filling pipe, and the liquid storage bottle are placed in a constant temperature explosion-proof box to simulate the reservoir temperature.

[0037] The hydrogen concentration in the constant temperature explosion-proof box is monitored in real time by a hydrogen leak alarm device.

[0038] When the hydrogen leak alarm device detects that the hydrogen concentration in the constant temperature explosion-proof box is greater than a preset threshold, it issues an alarm signal.

[0039] In one or more optional embodiments, the underground hydrogen storage physicochemical reaction experimental method further includes:

[0040] When the hydrogen leak alarm device detects that the hydrogen concentration in the constant temperature explosion-proof box is greater than a preset threshold, it activates the exhaust device to discharge the gas from the constant temperature explosion-proof box.

[0041] Secondly, embodiments of the present invention also provide an underground hydrogen storage physicochemical reaction experimental device, including a hydrogen supply device, multiple hydrogen reaction devices, a constant temperature explosion-proof box, a hydrogen leakage alarm device, and an exhaust device.

[0042] The hydrogen supply device is connected to the multiple sets of hydrogen reaction devices respectively.

[0043] The multiple hydrogen reaction devices and the hydrogen leakage alarm device are installed inside the constant temperature explosion-proof box;

[0044] The exhaust device is located at the ventilation opening of the constant temperature explosion-proof box.

[0045] In one or more alternative embodiments, the hydrogen reaction apparatus includes a main control valve, a flow controller, a core holder, a liquid storage bottle, a sand filling pipe, and a gas recovery pipe;

[0046] The main control valve is connected to the hydrogen supply device;

[0047] The flow controller is connected to the main control valve, the core holder, the liquid storage bottle, and the sand filling pipe, respectively.

[0048] The core holder and the liquid storage bottle are connected to the gas recovery pipe;

[0049] A first switching valve is provided between the flow controller and the core holder, the liquid storage bottle and the sand filling pipe respectively;

[0050] A second switching valve is provided between the gas recovery pipe and the core holder and the liquid storage bottle, respectively.

[0051] The core holder is used to hold the core;

[0052] The storage bottle is used to hold formation water and / or underground crude oil;

[0053] The sand-filled pipe is used to hold core powder.

[0054] In one or more optional embodiments, the underground hydrogen storage physicochemical reaction experimental device further includes a hydrogen storage physicochemical detection device;

[0055] The hydrogen storage physicochemical detection device includes a pressure-covered pore permeation device, a positioning scanning electron microscope, an X-ray diffractometer, a liquid chromatograph, and a gas chromatograph.

[0056] The pressure-controlled permeability device is used to detect the porosity and permeability of the rock core.

[0057] The positioning scanning electron microscope is used to position and scan the rock core, and to obtain the mineral composition of the rock core at a fixed point;

[0058] The X-ray diffractometer is used to scan the core powder and obtain the composition information of the core powder;

[0059] The liquid chromatograph is used to detect formation water and / or underground crude oil, and to obtain compositional information of formation water and / or underground crude oil.

[0060] The gas chromatograph is used to detect gases and obtain information about their composition.

[0061] The beneficial effects of the above-mentioned technical solutions provided in the embodiments of the present invention include at least the following:

[0062] The underground hydrogen storage physicochemical reaction experimental method provided in this embodiment of the invention sets corresponding target pressure values ​​and target reaction times for multiple groups of experimental samples, and simultaneously conducts underground hydrogen storage physicochemical reactions on these experimental samples. This yields the changes in formation water and / or underground crude oil, core samples, and core powder before and after the reaction under different pressure conditions and / or different reaction time lengths. By comparing the compositional changes between hydrogen and the emitted gases, comparing the changes in porosity, permeability, and composition before and after the core reaction, and comparing the compositional changes in core powder and formation water before and after the reaction, the key consumption mechanism of hydrogen in the rock-water system within the reservoir can be clarified. The contribution rate of different reaction pathways to hydrogen loss can be quantified, and the relationship between pressure changes and hydrogen consumption, as well as the impact of time length on hydrogen consumption, can be obtained. This enables the study of the physicochemical reaction mechanism of hydrogen with rock minerals and formation water in abandoned oil and gas reservoirs, providing technical support for underground hydrogen storage and effective guidance for reservoir screening.

[0063] Other features and advantages of the invention will be set forth in the following description, and will be apparent in part from the description, or may be learned by practicing the invention. The objects and other advantages of the invention may be realized and obtained by means of the structures particularly pointed out in the written description and the accompanying drawings.

[0064] The technical solution of the present invention will be further described in detail below with reference to the accompanying drawings and embodiments. Attached Figure Description

[0065] The accompanying drawings are provided to further illustrate the invention and form part of the specification. They are used in conjunction with embodiments of the invention to explain the invention and do not constitute a limitation thereof. In the drawings:

[0066] Figure 1 This is a schematic flowchart of the experimental method for underground hydrogen storage physicochemical reaction provided in an embodiment of the present invention;

[0067] Figure 2 This is a schematic diagram of the underground hydrogen storage physicochemical reaction experimental device provided in an embodiment of the present invention. Detailed Implementation

[0068] Exemplary embodiments of the present disclosure will now be described in more detail with reference to the accompanying drawings. While exemplary embodiments of the present disclosure are shown in the drawings, it should be understood that the present disclosure may be implemented in various forms and should not be limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete, and will fully convey the scope of the disclosure to those skilled in the art.

[0069] In the description of this invention, it should be noted that the terms "center," "upper," "lower," "left," "right," "vertical," "horizontal," "inner," "outer," "far," "near," "front," and "rear," etc., indicating the orientation or positional relationship, are based on the orientation or positional relationship shown in the accompanying drawings and are only for the convenience of describing this invention and simplifying the description, and do not indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation, and therefore should not be construed as a limitation of this invention. Furthermore, the terms "first," "second," and "third" are used for descriptive purposes only and should not be construed as indicating or implying relative importance.

[0070] In the description of this invention, it should be noted that, unless otherwise explicitly specified and limited, the terms "installation," "connection," and "linking" should be interpreted broadly. For example, they can refer to a fixed connection, a detachable connection, or an integral connection; they can refer to a mechanical connection or an electrical connection; they can refer to a direct connection or an indirect connection through an intermediate medium; and they can refer to the internal connection of two components. Those skilled in the art can understand the specific meaning of the above terms in this invention based on the specific circumstances.

[0071] The inventors discovered that hydrogen's chemical reactivity can lead to reactions with underground minerals or formation water, resulting in hydrogen loss. Newly formed minerals may clog pores or consume certain minerals, creating gas leakage channels and affecting the caprock's sealing. However, the reaction mechanism between hydrogen and underground geological rocks, minerals, or formation water is unclear, and the reaction parameters for the physicochemical reactions involved in hydrogen storage are not documented in relevant technologies. This leads to a degree of uncertainty and blind spots in the selection of hydrogen storage facilities.

[0072] Based on this, embodiments of the present invention provide an experimental method and apparatus for the physicochemical reaction of underground hydrogen storage, which will be described in detail below through specific embodiments.

[0073] Example 1

[0074] This invention provides an experimental method for the physicochemical reaction of underground hydrogen storage, referring to... Figure 1 As shown, it includes:

[0075] S101: Obtain multiple sets of experimental samples from the target gas storage facility, and set target pressure values ​​and target reaction times for each set of experimental samples; each set of experimental samples includes cores, core powder, and formation water and / or underground crude oil;

[0076] S102: For each set of experimental samples, detect the porosity, permeability and composition of the core, and detect the composition of the core powder as well as the composition of formation water and / or underground crude oil.

[0077] S103: For each group of experimental samples, after the core is saturated with formation water, it is placed in the core holder 24, the core powder is placed in the sand filling tube 26, and the formation water and / or underground crude oil is placed in the storage bottle 25.

[0078] S104: For each group of experimental samples, hydrogen gas is simultaneously introduced into the core holder 24, the sand filling tube 26 and the liquid storage bottle 25, and the pressure and temperature inside the core holder 24, the sand filling tube 26 and the liquid storage bottle 25 are kept consistent.

[0079] S105: Adjust the pressure of each group of experimental samples to the corresponding target pressure value;

[0080] S106: When the reaction time of any group of experimental samples reaches the preset reaction time, take out the experimental sample after the reaction and collect the gas discharged.

[0081] S107: Detect the composition of the discharged gas, and for each set of experimental samples taken out, re-detect the porosity, permeability and composition of the core, and detect the composition of the core powder as well as the composition of formation water and / or underground crude oil.

[0082] S108: For each group of experimental samples, compare the compositional changes between hydrogen and the exhaust gas, compare the changes in porosity, permeability and composition before and after the core reaction, compare the compositional changes before and after the core powder reaction and the compositional changes before and after the formation water reaction.

[0083] In this embodiment of the invention, each set of experimental samples corresponds to a set of reaction containers. A set of reaction containers includes a core holder, a sand filling pipe, and a liquid storage bottle. By controlling the amount of hydrogen gas introduced into each set of reaction containers, different pressure values ​​can be applied to each set of experimental samples.

[0084] The underground hydrogen storage physicochemical reaction experimental method provided in this embodiment of the invention can be adopted. Figure 2The underground hydrogen storage physicochemical reaction experimental device shown is realized. This device includes a hydrogen supply unit 1 and multiple hydrogen reaction units 2 connected in parallel with the hydrogen supply unit 1. The hydrogen supply unit 1 supplies hydrogen to the multiple hydrogen reaction units 2. The hydrogen supply unit 1 includes an explosion-proof cabinet 12 and gas cylinders 11, which are housed inside the explosion-proof cabinet 12 for storing hydrogen. The hydrogen reaction device 2 includes a main control valve 21, a flow controller 22, a core holder 24, a liquid storage bottle 25, a sand filling pipe 26, and a constant temperature explosion-proof box 3. The main control valve 21 is connected to the gas cylinder 11. The flow controller 22 is connected to the main control valve 21, the core holder 24, the liquid storage bottle 25, and the sand filling pipe 26. A first switching valve 23 is provided between the flow controller 22 and the core holder 24, the liquid storage bottle 25, and the sand filling pipe 26. A second switching valve 27 is provided at the outlet of the core holder 24 and the liquid storage bottle 25. The outlet end of the second switching valve 27 is connected to a gas recovery pipe 28. The core holder 24 is connected to a ring pressure pump (not shown in the figure).

[0085] In this embodiment of the invention, the underground hydrogen storage physicochemical reaction experimental device may further include a hydrogen storage physicochemical detection device. The hydrogen storage physicochemical detection device includes a pressure-controlled porosity and permeability device, a positioning scanning electron microscope (SEM), an X-ray diffractometer, a liquid chromatograph (LC), and a gas chromatograph (GC). The pressure-controlled porosity and permeability device is used to detect the porosity and permeability of the core sample; the positioning SEM is used to position and scan the core sample and obtain the mineral composition at specific points in the core; the X-ray diffractometer is used to scan the core powder and obtain the composition information of the core powder; the LC is used to detect formation water and / or underground crude oil and obtain the composition information of the formation water and / or underground crude oil; and the GC is used to detect gases and obtain the composition information of the gases.

[0086] The underground hydrogen storage physicochemical reaction experimental method provided in this embodiment of the invention sets corresponding target pressure values ​​and target reaction times for multiple groups of experimental samples, and simultaneously conducts underground hydrogen storage physicochemical reactions on these experimental samples. This yields the changes in formation water and / or underground crude oil, core samples, and core powder before and after the reaction under different pressure conditions and / or different reaction time lengths. By comparing the compositional changes between hydrogen and the emitted gases, comparing the changes in porosity, permeability, and composition before and after the core reaction, and comparing the compositional changes in core powder and formation water before and after the reaction, the key consumption mechanism of hydrogen in the rock-water system within the reservoir can be clarified. The contribution rate of different reaction pathways to hydrogen loss can be quantified, and the relationship between pressure changes and hydrogen consumption, as well as the impact of time length on hydrogen consumption, can be obtained. This enables the study of the physicochemical reaction mechanism of hydrogen with rock minerals and formation water in abandoned oil and gas reservoirs, providing technical support for underground hydrogen storage and effective guidance for reservoir screening.

[0087] In this embodiment of the invention, when pressure is used as the sole variable in conducting underground hydrogen storage physicochemical reaction experiments, step S101 involves obtaining multiple sets of experimental samples from the target gas storage facility and setting target pressure values ​​and target reaction times for each set of experimental samples. Specifically, this may include:

[0088] Obtain multiple sets of experimental samples from the target gas storage facility;

[0089] The target pressure values ​​for each group of experimental samples were set according to an arithmetic sequence.

[0090] The target reaction time for each group of experimental samples was set to be the same.

[0091] Each group of experimental samples was placed in a different reaction vessel, and the pressure values ​​in the different reaction vessels were controlled to be an arithmetic sequence. By comparing the changes in the experimental samples before and after the reaction, the effect of pressure on underground hydrogen storage can be obtained.

[0092] In this embodiment of the invention, when the time length is used as the only variable condition for conducting underground hydrogen storage physicochemical reaction experiments, step S101: obtaining multiple sets of experimental samples from the target gas storage facility, and setting target pressure values ​​and target reaction times for each set of experimental samples, specifically may include:

[0093] Obtain multiple sets of experimental samples from the target gas storage facility;

[0094] Set the target pressure value to be the same for each group of experimental samples;

[0095] The target reaction time for each group of experimental samples was set according to an arithmetic sequence.

[0096] Each group of experimental samples was placed in a different reaction vessel, and the pressure in each reaction vessel was kept equal. When the target reaction time of any group of experimental samples was reached, the experimental samples were taken out. By comparing the changes of multiple groups of experimental samples before and after the reaction, the effect of time on underground hydrogen storage can be obtained.

[0097] In this embodiment of the invention, when both pressure and time are used as variables in the underground hydrogen storage physicochemical reaction experiment, step S101: obtaining multiple sets of experimental samples from the target gas storage facility, and setting target pressure values ​​and target reaction times for each set of experimental samples, may specifically include:

[0098] Obtain multiple sets of experimental samples from at least five gas storage facilities, including the first set of experimental samples, the second set of experimental samples, the third set of experimental samples, the fourth set of experimental samples, and the fifth set of experimental samples;

[0099] The target pressure values ​​of the first group of experimental samples, the second group of experimental samples, and the third group of experimental samples are set as an arithmetic sequence, and the target reaction time of the first group of experimental samples, the second group of experimental samples, and the third group of experimental samples is set to be the same;

[0100] The target pressure values ​​of the third group of experimental samples, the fourth group of experimental samples, and the fifth group of experimental samples are set to be the same, and the target reaction times of the third group of experimental samples, the fourth group of experimental samples, and the fifth group of experimental samples are set to an arithmetic sequence.

[0101] By conducting simultaneous physicochemical reaction experiments on five sets of experimental samples for underground hydrogen storage, the effects of pressure and time on the physicochemical reaction of underground hydrogen storage can be obtained at the same time. This will help to study the physicochemical reaction mechanism of hydrogen with rocks, minerals and formation water in abandoned oil and gas reservoirs, and provide technical support for underground hydrogen storage.

[0102] In this embodiment of the invention, each set of experimental samples includes rock cores, rock core powder, and formation water and / or underground crude oil. It is understood that the storage bottle 25 can contain formation water alone, underground crude oil alone, or both simultaneously. If formation water and underground crude oil are contained simultaneously, the ratio of formation water to underground crude oil can be controlled according to the actual simulated conditions, thereby accurately simulating the environment within the gas storage facility and improving the reliability of the experimental results.

[0103] In this embodiment of the invention, before step S102: for each group of experimental samples, the porosity, permeability, and composition of the core sample are detected, and the composition of the core powder and the composition of the formation water are detected, the following may be included:

[0104] Sterilization of the core, core powder, and formation water can eliminate the influence of microorganisms on the physicochemical reaction experiments of underground hydrogen storage.

[0105] In this embodiment of the invention, step S102: For each group of experimental samples, the porosity, permeability, and composition of the core sample are detected, and the composition of the core powder and the composition of formation water and / or underground crude oil are detected. Specifically, this may include:

[0106] For each experimental sample, the porosity and permeability of the core were detected using a pressure-controlled permeability analyzer 201, the composition of the core was detected using a scanning electron microscope 202, the composition of the core powder was detected using an X-ray diffractometer 203, and the composition of formation water and / or underground crude oil was detected using a liquid chromatograph 204. It should be noted that if the formation water is prepared on-site, it is not necessary to detect its composition before the reaction.

[0107] In this embodiment of the invention, before step S104: for each group of experimental samples, hydrogen gas is simultaneously introduced into the core holder 24, the sand filling tube 26, and the liquid storage bottle 25, and before ensuring that the pressure and temperature inside the core holder 24, the sand filling tube 26, and the liquid storage bottle 25 are consistent, the following may also be included:

[0108] Connect the core holder 24, the sand filling tube 26, and the liquid storage bottle 25 to the pressure monitor, and monitor the pressure inside the core holder 24, the sand filling tube 26, and the liquid storage bottle 25 in real time through the pressure monitor.

[0109] In this embodiment of the invention, step S104: For each group of experimental samples, hydrogen gas is simultaneously introduced into the core holder 24, the sand filling tube 26, and the liquid storage bottle 25, ensuring that the pressure and temperature inside the core holder 24, the sand filling tube 26, and the liquid storage bottle 25 are consistent. Specifically, this may include:

[0110] First switching valves 23 are respectively installed at the inlets of the core holder 24, the sand filling pipe 26 and the liquid storage bottle 25;

[0111] Hydrogen gas was simultaneously introduced into the core holder 24, the sand filling pipe 26 and the liquid storage bottle 25, respectively.

[0112] The flow controller 22 controls the flow rate of hydrogen into the core holder 24, the sand filling pipe 26, and the liquid storage bottle 25 respectively. The amount of hydrogen entering the core holder 24, the sand filling pipe 26, and the liquid storage bottle 25 is controlled by opening or closing the corresponding first switch valve 23, so that the pressure in the core holder 24, the sand filling pipe 26, and the liquid storage bottle 25 of the same set of reaction vessels is consistent.

[0113] In this embodiment of the invention, after step S104: for each group of experimental samples, hydrogen gas is simultaneously introduced into the core holder 24, the sand filling tube 26, and the liquid storage bottle 25, and the pressure and temperature inside the core holder 24, the sand filling tube 26, and the liquid storage bottle 25 are kept consistent, the following may also be included:

[0114] An annular pressure is applied to the core holder 24 corresponding to each group of experimental samples by an annular pressure pump. The annular pressure must be 2MPa-3MPa greater than the axial pressure inside the core holder 24 to simulate the real pressure environment of the reservoir.

[0115] In this embodiment of the invention, step S105: adjusting the pressure of each group of experimental samples to the corresponding target pressure value may specifically include:

[0116] A master control valve 21 is installed at the main inlet of each group of reaction vessels;

[0117] The amount of hydrogen gas introduced into each group of reaction vessels is controlled by the main control valve 21, so that the corresponding reaction vessels of each group of experimental samples reach the corresponding target pressure value.

[0118] In this embodiment of the invention, step S106: When the reaction time of any group of experimental samples reaches the preset reaction time, the experimental sample after the reaction is taken out and the discharged gas is collected, which may specifically include:

[0119] For each set of reaction vessels, a second switch valve 27 is provided at the outlet of the core holder 24 and the outlet of the liquid storage bottle 25, and the second switch valve 27 is connected to a gas recovery pipe 28. When the reaction time of any set of experimental samples reaches the preset reaction time, the gas after the reaction can be collected and recovered by opening the second switch valve 27.

[0120] After gas recovery, the reacted core, core powder, formation water, and / or underground crude oil can be extracted.

[0121] In this embodiment of the invention, step S107: Detecting the composition of the discharged gas, and for each group of experimental samples taken out, re-detecting the porosity, permeability, and composition of the core sample, and detecting the composition of the core powder and the composition of formation water and / or underground crude oil, specifically may include:

[0122] The components of the emitted gas were detected by gas chromatograph 205;

[0123] For each set of experimental samples taken out, the porosity and permeability of the core were detected by the overburden permeability device 201, the composition of the core was detected by the positioning scanning electron microscope 202, the composition of the core powder was detected by the X-ray diffractometer 203, and the composition of the formation water was detected by the liquid chromatograph 204.

[0124] In an optional embodiment, the underground hydrogen storage physicochemical reaction experimental method may further include:

[0125] Before the experiment, the core holder 24, the sand filling pipe 26 and the liquid storage bottle 25 were placed in the constant temperature explosion-proof box 3 to simulate the reservoir temperature.

[0126] The hydrogen concentration in the constant temperature explosion-proof box 3 is monitored in real time by the hydrogen leakage alarm device 4.

[0127] When the hydrogen leakage alarm device 4 detects that the hydrogen concentration in the constant temperature explosion-proof box 3 is greater than a preset threshold, it issues an alarm signal.

[0128] In an optional embodiment, the underground hydrogen storage physicochemical reaction experimental method may further include:

[0129] When the hydrogen leakage alarm device 4 detects that the hydrogen concentration in the constant temperature explosion-proof box 3 is greater than the preset threshold, the exhaust device 5 is activated to discharge the gas in the constant temperature explosion-proof box 3.

[0130] To more clearly illustrate the experimental method for underground hydrogen storage physicochemical reactions provided in the embodiments of the present invention, the following preferred embodiments are provided, detailing the application process of this method:

[0131] S1: Select an underground hydrogen storage physicochemical reaction experimental device with 7 sets of hydrogen reaction devices 2, take 49 sets of experimental samples in the target gas storage, and number the 49 sets of experimental samples from 1 to 49.

[0132] S2: Set the target pressure value and target reaction time for each group of experimental samples. The setting results are shown in Table 1 below:

[0133] Table 1. Target pressure values ​​and target reaction times for 49 groups of experimental samples;

[0134]

[0135] S3: Select 7 groups of experimental samples numbered 1-7. For each group of experimental samples, test the porosity, permeability and composition of the core, and test the composition of the core powder as well as the composition of formation water and / or underground crude oil.

[0136] S4: For each group of experimental samples, after the core is saturated with formation water, it is placed into 7 sets of hydrogen reaction devices and hydrogen is introduced into the 7 sets of hydrogen reaction devices. The pressure of the 7 sets of experimental samples is adjusted to the target pressure values ​​corresponding to Table 1.

[0137] S5: After all 7 groups of experimental samples have reached the target reaction time of 5 days, take out the 7 groups of experimental samples after the reaction and collect the gas discharged from each group.

[0138] S6: For each set of experimental samples taken out, detect the composition of the gas emitted, re-detect the porosity, permeability and composition of the core, and detect the composition of the core powder as well as the composition of formation water and / or underground crude oil.

[0139] S7: For each group of experimental samples, compare and record the compositional changes between hydrogen and the exhaust gas, compare and record the changes in porosity, permeability and composition before and after the core reaction, compare and record the compositional changes before and after the core powder reaction and the compositional changes before and after the formation water reaction.

[0140] Continue by selecting seven experimental samples numbered 8-14, and repeating steps S3-S7 according to the target pressure and reaction time set in Table 1. This process is repeated for every seven experimental samples, with one sample placed in the underground hydrogen storage physicochemical reaction experimental device each time, according to the target pressure and reaction time set in Table 1. The second sample is then numbered 8-14, and so on, resulting in a total of 49 experimental samples and corresponding experimental results. Based on these results, the key consumption mechanism of hydrogen in the rock-water system within the reservoir can be clarified, the contribution rate of different reaction pathways to hydrogen loss can be quantified, and the relationship between pressure change and hydrogen consumption, as well as the impact of time on hydrogen consumption, can be obtained. This enables the study of the physicochemical reaction mechanism of hydrogen with rock minerals and formation water in abandoned oil and gas reservoirs, providing technical support for underground hydrogen storage and effective guidance for reservoir screening.

[0141] Example 2

[0142] Based on the same inventive concept, this invention also provides an underground hydrogen storage physicochemical reaction experimental device, referring to... Figure 2 As shown, it includes a hydrogen supply device 1, multiple hydrogen reaction devices 2, a constant temperature explosion-proof box 3, a hydrogen leakage alarm device 4, and an exhaust device 5.

[0143] Hydrogen supply device 1 is connected to multiple hydrogen reaction devices 2 respectively;

[0144] Multiple hydrogen reaction devices 2 and hydrogen leakage alarm devices 4 are installed in a constant temperature explosion-proof box 3;

[0145] The exhaust device 5 is installed at the ventilation opening of the constant temperature explosion-proof box 3.

[0146] In this embodiment of the invention, the underground hydrogen storage physicochemical reaction experimental device corresponds to the underground hydrogen storage physicochemical reaction experimental method described in Example 1. Its specific application process can be referred to the execution process of the underground hydrogen storage physicochemical reaction experimental method described in Example 1. Where it is repeated, it will not be described again.

[0147] In this embodiment of the invention, the hydrogen reaction device includes a main control valve, a flow controller, a core holder, a liquid storage bottle, a sand filling pipe, and a gas recovery pipe. The main control valve is connected to a hydrogen supply device; the flow controller is connected to the main control valve, the core holder, the liquid storage bottle, and the sand filling pipe respectively; the core holder and the liquid storage bottle are connected to the gas recovery pipe; a first switching valve is respectively installed between the flow controller and the core holder, the liquid storage bottle, and the sand filling pipe; a second switching valve is respectively installed between the gas recovery pipe and the core holder and the liquid storage bottle; the core holder is used to hold the core; the liquid storage bottle is used to hold formation water and / or underground crude oil; and the sand filling pipe is used to hold core powder.

[0148] In this embodiment of the invention, the underground hydrogen storage physicochemical reaction experimental device further includes a hydrogen storage physicochemical detection device. The hydrogen storage physicochemical detection device includes a pressure-controlled porosity and permeability device, a positioning scanning electron microscope (SEM), an X-ray diffractometer, a liquid chromatograph (LC), and a gas chromatograph (GC). The pressure-controlled porosity and permeability device is used to detect the porosity and permeability of the core sample; the positioning SEM is used to position and scan the core sample and obtain the mineral composition at specific points in the core; the X-ray diffractometer is used to scan the core powder and obtain the composition information of the core powder; the LC is used to detect formation water and / or underground crude oil and obtain the composition information of the formation water and / or underground crude oil; and the GC is used to detect gases and obtain the composition information of the gases.

[0149] Obviously, those skilled in the art can make various modifications and variations to this invention without departing from its spirit and scope. This disclosure is not limited to the precise structures described above and shown in the accompanying drawings, and various modifications and changes can be made without departing from its scope. The scope of this disclosure is limited only by the appended claims. Thus, if these modifications and variations of the invention fall within the scope of the claims of the invention and their equivalents, the invention is also intended to include these modifications and variations.

Claims

1. An experimental method for the physicochemical reaction of underground hydrogen storage, characterized in that, include: Multiple sets of experimental samples were obtained from the target gas storage facility, and target pressure values ​​and target reaction times were set for each set of experimental samples; each set of experimental samples included cores, core powder, and formation water and / or underground crude oil. For each set of experimental samples, the porosity, permeability and composition of the core were tested, as well as the composition of the core powder and the composition of formation water and / or underground crude oil. For each experimental sample, the core was saturated with formation water and then placed in a core holder. The core powder was placed in a sand-filling tube, and the formation water and / or underground crude oil were placed in a storage bottle. For each set of experimental samples, hydrogen gas was simultaneously introduced into the core holder, the sand filling tube, and the liquid storage bottle, and the pressure and temperature inside the core holder, the sand filling tube, and the liquid storage bottle were kept consistent. Adjust the pressure of each group of experimental samples to the corresponding target pressure value; Once the reaction time of any group of experimental samples reaches the preset reaction time, the experimental samples after the reaction are taken out and the discharged gas is collected. The composition of the emitted gas was detected, and for each set of experimental samples taken out, the porosity, permeability and composition of the core were detected again, as well as the composition of the core powder and the composition of formation water and / or underground crude oil. For each group of experimental samples, the compositional changes between hydrogen and the emitted gas were compared, as were the changes in porosity, permeability, and composition before and after the core reaction, the compositional changes of the core powder before and after the reaction, and the compositional changes of the formation water before and after the reaction.

2. The experimental method for underground hydrogen storage physicochemical reaction according to claim 1, characterized in that, The process of acquiring multiple sets of experimental samples from the target gas storage facility and setting target pressure values ​​and target reaction times for each set of experimental samples includes: Obtain multiple sets of experimental samples from the target gas storage facility; The target pressure values ​​for each group of experimental samples were set according to an arithmetic sequence. The target reaction time for each group of experimental samples was set to be the same.

3. The experimental method for underground hydrogen storage physicochemical reaction according to claim 1, characterized in that, The process of acquiring multiple sets of experimental samples from the target gas storage facility and setting target pressure values ​​and target reaction times for each set of experimental samples includes: Obtain multiple sets of experimental samples from the target gas storage facility; Set the target pressure value to be the same for each group of experimental samples; The target reaction time for each group of experimental samples was set according to an arithmetic sequence.

4. The experimental method for underground hydrogen storage physicochemical reaction according to claim 1, characterized in that, The process of acquiring multiple sets of experimental samples from the target gas storage facility and setting target pressure values ​​and target reaction times for each set of experimental samples includes: Obtain multiple sets of experimental samples from at least five gas storage facilities, including the first set of experimental samples, the second set of experimental samples, the third set of experimental samples, the fourth set of experimental samples, and the fifth set of experimental samples; The target pressure values ​​of the first group of experimental samples, the second group of experimental samples, and the third group of experimental samples are set as an arithmetic sequence, and the target reaction times of the first group of experimental samples, the second group of experimental samples, and the third group of experimental samples are set to be the same; The target pressure values ​​of the third group of experimental samples, the fourth group of experimental samples, and the fifth group of experimental samples are set to be the same, and the target reaction times of the third group of experimental samples, the fourth group of experimental samples, and the fifth group of experimental samples are set to an arithmetic sequence.

5. The experimental method for underground hydrogen storage physicochemical reaction according to claim 1, characterized in that, For each group of experimental samples, the porosity, permeability, and composition of the core sample were measured, as well as the composition of the core powder and the composition of the formation water, including: For each experimental sample, the porosity and permeability of the core were detected by a pressure-controlled permeability device, the mineral composition of the core at a fixed point was detected by a positioning scanning electron microscope, the composition of the core powder was detected by an X-ray diffractometer, and the composition of formation water and / or underground crude oil was detected by a liquid chromatograph.

6. The experimental method for underground hydrogen storage physicochemical reaction according to claim 1, characterized in that, The process of detecting the composition of the emitted gas, and for each set of experimental samples taken out, re-detecting the porosity, permeability, and composition of the core, as well as the composition of the core powder and the composition of formation water and / or underground crude oil, includes: The components of the emitted gas are detected by gas chromatography. For each set of experimental samples, the porosity and permeability of the core were detected by a pressure-controlled permeability device, the mineral composition of the core at a fixed point was detected by a positioning scanning electron microscope, the composition of the core powder was detected by an X-ray diffractometer, and the composition of the formation water was detected by a liquid chromatograph.

7. The experimental method for underground hydrogen storage physicochemical reaction according to claim 1, characterized in that, Before determining the porosity, permeability, and composition of the core sample for each set of experimental samples, and before determining the composition of the core powder and the formation water, the method further includes: The core, core powder, and formation water were sterilized.

8. The experimental method for underground hydrogen storage physicochemical reaction according to claim 1, characterized in that, After simultaneously introducing hydrogen gas into the core holder, the sand-filling tube, and the liquid storage bottle for each group of experimental samples, and ensuring that the pressure and temperature inside the core holder, the sand-filling tube, and the liquid storage bottle are consistent, the process further includes: Circulating pressure is applied to the core holders corresponding to each group of experimental samples using a circulating pressure pump.

9. The experimental method for underground hydrogen storage physicochemical reaction according to claim 1, characterized in that, Also includes: The core holder, the sand-filling pipe, and the liquid storage bottle are placed in a constant temperature explosion-proof box to simulate the reservoir temperature. The hydrogen concentration in the constant temperature explosion-proof box is monitored in real time by a hydrogen leak alarm device. When the hydrogen leak alarm device detects that the hydrogen concentration in the constant temperature explosion-proof box is greater than a preset threshold, it issues an alarm signal.

10. The experimental method for underground hydrogen storage physicochemical reaction according to claim 9, characterized in that, Also includes: When the hydrogen leak alarm device detects that the hydrogen concentration in the constant temperature explosion-proof box is greater than a preset threshold, it activates the exhaust device to discharge the gas from the constant temperature explosion-proof box.

11. An experimental apparatus for underground hydrogen storage physicochemical reaction, characterized in that, Includes hydrogen supply device, multiple hydrogen reaction devices, constant temperature explosion-proof box, hydrogen leakage alarm device and exhaust device; The hydrogen supply device is connected to the multiple sets of hydrogen reaction devices respectively. The multiple hydrogen reaction devices and the hydrogen leakage alarm device are installed inside the constant temperature explosion-proof box; The exhaust device is located at the ventilation opening of the constant temperature explosion-proof box.

12. An underground hydrogen storage physicochemical reaction experimental apparatus according to claim 11, characterized in that, The hydrogen reaction device includes a main control valve, a flow controller, a core holder, a liquid storage bottle, a sand filling pipe, and a gas recovery pipe; The main control valve is connected to the hydrogen supply device; The flow controller is connected to the main control valve, the core holder, the liquid storage bottle, and the sand filling pipe, respectively. The core holder and the liquid storage bottle are connected to the gas recovery pipe; A first switching valve is provided between the flow controller and the core holder, the liquid storage bottle and the sand filling pipe respectively; A second switching valve is provided between the gas recovery pipe and the core holder and the liquid storage bottle, respectively. The core holder is used to hold the core; The storage bottle is used to hold formation water and / or underground crude oil; The sand-filled pipe is used to hold core powder.

13. An underground hydrogen storage physicochemical reaction experimental apparatus as described in claim 12, characterized in that, It also includes a hydrogen storage physicochemical detection device; The hydrogen storage physicochemical detection device includes a pressure-covered pore permeation device, a positioning scanning electron microscope, an X-ray diffractometer, a liquid chromatograph, and a gas chromatograph. The pressure-controlled permeability device is used to detect the porosity and permeability of the rock core. The positioning scanning electron microscope is used to position and scan the rock core, and to obtain the mineral composition of the rock core at a fixed point; The X-ray diffractometer is used to scan the core powder and obtain the composition information of the core powder; The liquid chromatograph is used to detect formation water and / or underground crude oil, and to obtain compositional information of formation water and / or underground crude oil. The gas chromatograph is used to detect gases and obtain information about their composition.

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