CN111088023A - High-temperature-resistant polyacrylamide gel plugging agent and preparation method and application thereof - Google Patents
High-temperature-resistant polyacrylamide gel plugging agent and preparation method and application thereof Download PDFInfo
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Abstract
The invention relates to the technical field of oil exploitation, and provides a high-temperature-resistant polyacrylamide gel plugging agent, and a preparation method and application thereof. The high-temperature resistant polyacrylamide gel plugging agent comprises: acrylamide polymer, water-soluble urea-formaldehyde resin, organic chromium, an oxygen scavenger, a urea compound and water, wherein the urea compound has a structure shown in a formula (1) and/or a formula (2), R1And R2Each independently selected from hydrogen or 2-propynyl; r3、R4And R5Each independently selected from oxygen, sulfur or imino. The high-temperature resistant polyacrylamide gel plugging agent provided by the invention is simple in preparation method, can effectively plug a steam channeling channel for a long time (30-90 days) at a higher temperature (150-.
Description
Technical Field
The invention relates to the technical field of oil exploitation, in particular to a high-temperature-resistant polyacrylamide gel plugging agent, and a preparation method and application thereof.
Background
Steam stimulation is the main mode of heavy oil development, is considered to be a conventional, economical and effective method and is widely used by heavy oil fields. Along with the progress of the multiple times of huff and puff stages, the water invasion and steam channeling are serious, the water content of the oil well is greatly increased, different degrees of influence are brought to the thermal recovery of the heavy oil reservoir, and the thermal recovery effect is deteriorated. The high water content of an oil well in the thermal recovery process of a heavy oil reservoir becomes a main problem influencing the thermal recovery effect. At present, one of the most effective methods for solving the problem is to use a gel plugging agent to block a steam channeling channel and improve the utilization degree and recovery ratio of thick oil.
The existing gel plugging agent is compounded and injected into a stratum by taking a polyacrylamide aqueous solution as a thickening agent and phenolic resin as a crosslinking agent, and is crosslinked in situ at the deep part of the stratum to form gel for plugging water. However, the technology is only suitable for the environment below 120 ℃, and cannot stably block water for a long time in a high-temperature steam huff and puff environment, because the system is unstable at high temperature, the working fluid enters the stratum and is excessively crosslinked in the early stage to be dehydrated, and the working fluid is thermally degraded in the later stage. Therefore, for the water shutoff operation of the steam huff and puff of the heavy oil reservoir, the construction success rate is not high, the oil increasing effective period is short, and the oil increasing effect is limited. The gel plugging agent which is effective for a long time at a higher temperature and in a longer time range is a current technical difficulty and needs to be broken through urgently.
Disclosure of Invention
Aiming at the problem that the existing gel blocking agent can not be effectively applied to higher temperature and realize longer-time water blocking, the invention aims to provide a novel high-temperature-resistant polyacrylamide gel blocking agent and a preparation method and application thereof. The high-temperature-resistant polyacrylamide gel plugging agent can effectively plug a steam channeling channel in a higher-temperature environment and in a longer time range, and realizes the high-efficiency development of a heavy oil reservoir.
According to a first aspect of the present invention, the present invention provides a high temperature resistant polyacrylamide gel plugging agent, comprising: acrylamide polymer, water-soluble urea-formaldehyde resin, organic chromium, an oxygen scavenger, a urea compound and water, wherein the urea compound has a structure shown in a formula (1) and/or a formula (2),
wherein R is1And R2Each independently selected from hydrogen or 2-propynyl; r3And R4Each independently oxygen, sulfur or imino;
based on the total weight of the high-temperature resistant polyacrylamide gel plugging agent, the content of the urea compound is 0.1-2 wt%.
According to a second aspect of the present invention, the present invention provides a method for preparing the high temperature resistant polyacrylamide gel blocking agent, which comprises:
(1) dissolving acrylamide polymer in water to obtain polymer water solution;
(2) and adding water-soluble urea-formaldehyde resin, organic chromium, a urea compound and an oxygen scavenger into the polymer aqueous solution, and stirring until the mixture is dissolved to obtain the high-temperature-resistant polyacrylamide gel plugging agent.
According to a third aspect of the invention, the invention provides an application of the high-temperature-resistant polyacrylamide gel plugging agent in heavy oil steam stimulation thermal recovery.
The high-temperature resistant polyacrylamide gel plugging agent provided by the invention is simple in preparation method, can effectively plug a steam channeling channel for a long time (30-90 days) at a higher temperature (150-. Compared with the existing gel plugging agent, the gel plugging agent has higher plugging rate and longer plugging time, and can be suitable for large pore path plugging operation in heavy oil steam huff and puff thermal recovery operation.
Detailed Description
The endpoints of the ranges and any values disclosed herein are not limited to the precise range or value, and such ranges or values should be understood to encompass values close to those ranges or values. For ranges of values, between the endpoints of each of the ranges and the individual points, and between the individual points may be combined with each other to give one or more new ranges of values, and these ranges of values should be considered as specifically disclosed herein.
According to a first aspect of the present invention, the present invention provides a high temperature resistant polyacrylamide gel blocking agent, comprising: acrylamide polymer, water-soluble urea-formaldehyde resin, organic chromium, an oxygen scavenger, a urea compound and water.
In the present invention, the urea compound has a structure represented by formula (1) and/or formula (2),
wherein R is1And R2Each independently selected from hydrogen or 2-propynyl, R3And R4Each independently oxygen, sulfur or imino.
Preferably, the urea compound is one or more of urea, 2-propynyl urea, biuret, thiobiuret and 2-imino-4-thiobiuret.
More preferably, the urea-based compound is urea. Urea has a smaller molecular weight and volume relative to its dimer (e.g., biuret) and its substituted compounds (e.g., 2-propynyl urea), has less steric hindrance and better mobility when reacted in the gellant system, and is somewhat better able to compete with polyacrylamide-based polymers during condensation reactions with water-soluble urea-formaldehyde resins.
In the invention, the content of the urea compound is 0.1-2 wt%, preferably 0.2-1 wt%, based on the total weight of the high temperature resistant polyacrylamide gel blocking agent.
In the present invention, the kind and amount of the acrylamide-based polymer may be selected with reference to the prior art, and the acrylamide-based polymer may be synthesized according to the prior art or commercially available. For the present invention, preferably, the acrylamide-based polymer is one or more of partially hydrolyzed polyacrylamide, partially hydrolyzed methylene polyacrylamide, acrylamide/acrylic acid/AMPS sodium salt copolymer, and acrylamide/acrylic acid/acrylonitrile sodium salt copolymer. Wherein the partially hydrolyzed polyacrylamide and the acrylamide/acrylic acid/AMPS sodium salt copolymer are available from Shandong Baumo et al.
Preferably, the viscosity average molecular weight of the acrylamide polymer is 800 to 3500 ten thousand, more preferably 1000 to 3000 ten thousand; the degree of hydrolysis of the acrylamide-based polymer is 8 to 35%, more preferably 10 to 25%.
In the present invention, the degree of hydrolysis is measured by the method for measuring the degree of hydrolysis of partially hydrolyzed polyacrylamide according to the national standard GB/T12005.6-1989.
Preferably, the content of the acrylamide polymer is 0.1-2 wt%, more preferably 0.2-1 wt%, based on the total weight of the high temperature resistant polyacrylamide gel blocking agent.
In the invention, the water-soluble urea-formaldehyde resin is linear urea-formaldehyde resin, and is preferably obtained by polymerizing formaldehyde and urea monomers in a molar ratio of 1.0-3.0:1 under an alkaline condition. Typically, the water-soluble urea-formaldehyde resin obtained by the reaction is a solid-liquid mixture with a pH value of more than 9 and a solid content of more than 40 wt%.
Preferably, the content of the water-soluble urea-formaldehyde resin is 0.1-2 wt%, more preferably 0.2-1 wt%, based on the total weight of the high-temperature resistant polyacrylamide gel plugging agent.
In the present invention, the organic chromium is preferably one or more of chromium acetate, chromium oxalate, chromium lactate, chromium propionate, chromium malonate, and chromium citrate, and more preferably chromium lactate. The organic acid chromium can be prepared according to the prior art, and according to an embodiment of the invention, chromium (II) is firstly reacted with sodium nitrite, reduced to chromium (III) and then complexed with an organic acid (preferably one or more of acetic acid, oxalic acid, lactic acid, propionic acid, malonic acid and citric acid), wherein the molar ratio of the reaction of chromium (II) and sodium nitrite is 1/4-1/3, the molar ratio of the complexation of the reaction of chromium (III) and the organic acid is 1/50-1/10, the obtained organic chromium is dark green solution, the pH value is 4-10, and the effective content of chromium (III) is more than 2%.
Preferably, the content of the organic chromium is 0.01 to 2 weight percent, more preferably 0.03 to 1.5 weight percent based on the total weight of the high-temperature resistant polyacrylamide gel plugging agent.
In the invention, the oxygen scavenger can reduce the oxidative degradation of the polymer in the system, and the type and the dosage of the oxygen scavenger can be selected according to the prior art. In the present invention, preferably, the oxygen scavenger is one or more of sodium thiosulfate, sodium sulfite, sodium bisulfite, sodium hydrosulfite, isoascorbic acid and thiourea.
Preferably, the weight of the oxygen scavenger is 0.05-1 wt% based on the total weight of the high temperature resistant polyacrylamide gel plugging agent.
In the present invention, water is used as the solvent and reaction medium in the high temperature resistant polyacrylamide gel blocking agent system, and the selection of the solvent and the reaction medium is not particularly limited in the present invention. The degree of mineralization of water is usually less than 500 mg, and can be natural water, such as rivers, lakes, atmospheric water, seawater, groundwater and the like, and artificial water, such as tap water, distilled water, deionized water or heavy water. In the present invention, the water content is 91 to 99.64 wt%, preferably 94.5 to 99.32 wt%, based on the total weight of the high temperature resistant polyacrylamide gel blocking agent.
In the invention, the content of each component in the high-temperature resistant polyacrylamide gel plugging agent is calculated by the feeding amount.
The high-temperature resistant polyacrylamide gel plugging agent is particularly suitable for plugging a steam channeling pipeline in the process of steam huff and puff thermal thickened oil recovery. Specifically, hydroxyl in the water-soluble urea-formaldehyde resin and an amide group of the acrylamide polymer can undergo an in-situ dehydration condensation reaction at a high temperature, so that the acrylamide polymer is crosslinked; meanwhile, the organic chromium in the system coordinates with the carboxyl of the acrylamide polymer, so that the acrylamide polymer is crosslinked, the system gradually forms gel along with the reaction, and a steam channeling pipeline is blocked in the process of steam huff and puff thermal recovery of thick oil. In addition to the above reaction, the urea compound contained in the system can also undergo a dehydration condensation reaction with the water-soluble urea resin, and the possible reaction mechanism is as follows (taking the urea compound represented by formula (1) as an example):
therefore, the urea compound competes with the condensation reaction of the acrylamide polymer and the water-soluble urea-formaldehyde resin, so that the crosslinking speed of the acrylamide polymer is reduced, and the crosslinking reaction of the acrylamide polymer can be continuously carried out for a long time. Through determination, the high-temperature resistant polyacrylamide gel plugging agent can form gel within one day at the high temperature of 150 ℃ to form plugging.
In addition, the addition of the urea compound reduces the density of crosslinking active points in the system, inhibits the dehydration phenomenon caused by excessive crosslinking of the acrylamide polymer, can adjust the distance between the crosslinking active points, slows down the degree of coverage of the crosslinking active points, improves the crosslinking efficiency, increases the strength of gel formed by the crosslinking system, and enables the formed gel system to be stable at a higher temperature.
According to a second aspect of the present invention, the present invention provides a method for preparing the high temperature resistant polyacrylamide gel blocking agent according to the first aspect of the present invention, the method comprising:
(1) dissolving acrylamide polymer in water to obtain polymer water solution;
(2) and adding water-soluble urea-formaldehyde resin, organic chromium, a urea compound and an oxygen scavenger into the polymer aqueous solution, and stirring until the urea-formaldehyde resin, the organic chromium, the urea compound and the oxygen scavenger are completely dissolved to obtain the high-temperature-resistant polyacrylamide gel plugging agent.
According to a third aspect of the invention, the invention provides an application of the high-temperature-resistant polyacrylamide gel plugging agent in heavy oil steam stimulation thermal recovery. As mentioned above, the high temperature resistant polyacrylamide gel plugging agent is particularly suitable for plugging a steam channeling pipeline in the process of steam huff and puff thermal heavy oil recovery.
According to the invention, the application may comprise: and injecting the high-temperature-resistant polyacrylamide gel plugging agent into the stratum, so that the high-temperature-resistant polyacrylamide gel plugging agent is crosslinked in situ in the stratum to form gel.
Under the environment of steam huff and puff thermal recovery of thickened oil, the gel plugging agent formed by the high-temperature resistant polyacrylamide gel plugging agent can be kept for 30-90 days at the temperature of 150-180 ℃.
The present invention will be described in detail below by way of examples.
Example 1
This example is used to illustrate the high temperature resistant polyacrylamide gel blocking agent and the preparation method thereof.
At room temperature, 20 g of partially hydrolyzed polyacrylamide (viscosity average molecular weight 800 ten thousand, degree of hydrolysis 8%) is dissolved in 1L of water, and the mixture is stirred at 500 rpm until the partially hydrolyzed polyacrylamide is completely dissolved; and then sequentially adding 20 g of water-soluble urea-formaldehyde resin (the molar ratio of formaldehyde to urea is 2.8), 20 g of chromium acetate, 10 g of urea and 10 g of sodium thiosulfate, and stirring until the mixture is completely dissolved to obtain the high-temperature-resistant polyacrylamide gel plugging agent.
The blocking performance of the high temperature resistant polyacrylamide gel blocking agent at 150 ℃ for 60 days of standing time is tested, and the results are shown in table 1.
The Darcy principle is applied to the test of the plugging performance, and the prior art can be specifically referred to. The method for testing the plugging performance comprises the following steps:
filling a simulated core (the diameter d of the core is 25mm, the length L of the core is 200mm), injecting water into the core at the flow rate of 2 ml/min after vacuumizing, and measuring the permeability (k) before core plugging0) (ii) a Then to the coreInjecting 1.0-1.5PV of the high-temperature-resistant polyacrylamide gel plugging agent of the embodiment into the model, plugging two ends of the core by using a plug, placing the core into a constant temperature box at 150 ℃ for standing for 60 days, injecting water again until the pressure is stable, recording the reading on a pressure gauge to obtain injection pressure difference, and calculating the permeability (k') after the core is plugged so as to calculate the plugging rate;
for convenience of description and explanation, k will be given0And k' are collectively called as core permeability k, and the calculation formula is as follows:
wherein Q is the injection rate, mL · s-1(ii) a μ is the fluid viscosity, mPa · s; a is the cross section area of the sand-filled model in cm2,A=πd2(ii)/4; Δ P is the injection pressure difference, 10-1MPa;k,μm2。
example 2
This example is used to illustrate the high temperature resistant polyacrylamide gel blocking agent and the preparation method thereof.
At room temperature, 4 g of acrylamide/acrylic acid/AMPS sodium salt copolymer (viscosity average molecular weight is 2500 ten thousand, hydrolysis degree is 20%) is dissolved in 1L of water, and stirring is carried out at a speed of 500 revolutions per minute until the acrylamide/acrylic acid/AMPS sodium salt copolymer is completely dissolved; 4 g of water-soluble urea-formaldehyde resin (the molar ratio of formaldehyde to urea is 2.8), 2 g of chromium lactate, 2 g of urea and 2 g of isoascorbic acid are sequentially added and stirred until all the components are dissolved, so that the high-temperature-resistant polyacrylamide gel plugging agent of the embodiment is obtained.
The plugging rates of the high-temperature resistant polyacrylamide gel plugging agent under the conditions of 150 ℃/60 days, 150 ℃/75 days, 150 ℃/90 days, 165 ℃/60 days and 180 ℃/60 days are tested, the test method is the same as that of example 1, and the test results are shown in tables 1 and 2.
Example 3
This example is used to illustrate the high temperature resistant polyacrylamide gel blocking agent and the preparation method thereof.
At room temperature, 1 g of acrylamide/acrylic acid/AMPS sodium salt copolymer (viscosity average molecular weight is 3500 ten thousand, hydrolysis degree is 35%) is dissolved in 1L of water, and the mixture is stirred at 500 revolutions per minute until the acrylamide/acrylic acid/AMPS sodium salt copolymer is completely dissolved; and then sequentially adding 1 g of water-soluble urea-formaldehyde resin (the molar ratio of formaldehyde to urea is 2.8), 0.1 g of chromium oxalate, 1.5 g of urea and 0.5 g of sodium bisulfite, and stirring until the mixture is completely dissolved to obtain the high-temperature resistant polyacrylamide gel plugging agent.
The blocking rate of the high temperature resistant polyacrylamide gel blocking agent is tested at the temperature of 150 ℃ and the standing time of 60 days, the test method is the same as that of example 1, and the test results are shown in table 1.
Example 4
This example is used to illustrate the high temperature resistant polyacrylamide gel blocking agent and the preparation method thereof.
At room temperature, 4 g of acrylamide/acrylic acid/AMPS sodium salt copolymer (viscosity average molecular weight is 2500 ten thousand, hydrolysis degree is 20%) is dissolved in 1L of water, and stirring is carried out at 500 revolutions per minute until the acrylamide/acrylic acid/AMPS sodium salt copolymer is completely dissolved; and then, sequentially adding 4 g of water-soluble urea-formaldehyde resin (the molar ratio of formaldehyde to urea is 2.8), 2 g of chromium lactate, 5 g of biuret and 2 g of isoascorbic acid, and stirring until the mixture is completely dissolved to obtain the high-temperature-resistant polyacrylamide gel plugging agent.
The blocking rate of the high temperature resistant polyacrylamide gel blocking agent is tested at the temperature of 150 ℃ and the standing time of 60 days, the test method is the same as that of example 1, and the test results are shown in table 1.
Example 5
This example is used to illustrate the high temperature resistant polyacrylamide gel blocking agent and the preparation method thereof.
At room temperature, 20 g of partially hydrolyzed polyacrylamide (viscosity average molecular weight 800 ten thousand, degree of hydrolysis 8%) is dissolved in 1L of water, and the mixture is stirred at 500 rpm until the partially hydrolyzed polyacrylamide is completely dissolved; and then sequentially adding 20 g of water-soluble urea-formaldehyde resin (the molar ratio of formaldehyde to urea is 2.8), 20 g of chromium acetate, 20 g of urea and 10 g of sodium thiosulfate, and stirring until the mixture is completely dissolved to obtain the high-temperature-resistant polyacrylamide gel plugging agent.
The blocking rate of the high temperature resistant polyacrylamide gel blocking agent is tested at the temperature of 150 ℃ and the standing time of 60 days, the test method is the same as that of example 1, and the test results are shown in table 1.
Comparative example 1
At room temperature, 4 g of acrylamide/acrylic acid/AMPS sodium salt copolymer (viscosity average molecular weight 2000 ten thousand, hydrolysis degree 22%) is dissolved in 1L of water, and the mixture is stirred at a speed of 500 revolutions per minute until the acrylamide/acrylic acid/AMPS sodium salt copolymer is completely dissolved; 4 g of water-soluble urea-formaldehyde resin (the molar ratio of formaldehyde to urea is 2.0), 2 g of chromium lactate and 2 g of isoascorbic acid are added in sequence and stirred until the mixture is completely dissolved, so as to obtain the high-temperature resistant polyacrylamide gel plugging agent of the comparative example.
The blocking rate of the high temperature resistant polyacrylamide gel blocking agent is tested at the temperature of 150 ℃ and the standing time of 60 days, the test method is the same as that of example 1, and the test results are shown in table 1.
Plugging rate test results:
TABLE 1
Note: table 1 shows the results of the test of the plugging rate (150 ℃ C./60 days) of examples and comparative examples.
TABLE 2
Note: table 2 shows the results of the plugging rate tests of example 2 under different test conditions.
As can be seen from Table 1, the high temperature resistant polyacrylamide gel block agents of examples 1 to 5 have higher blocking rates than the gel block agent composition without urea compound, compared to the polyacrylamide gel block agent without urea compound of comparative example 1, under the condition of standing at 150 ℃ for 60 days. As can be seen from Table 2, the high temperature resistant polyacrylamide gel plugging agent can stably exist for at least 90 days at 150 ℃, and a higher plugging rate is maintained; can be stably stored for at least 60 days when the temperature is increased to 180 ℃. Therefore, the high-temperature-resistant polyacrylamide gel plugging agent is applied to heavy oil steam huff-puff thermal recovery, can effectively plug a steam channeling channel at a high temperature (150-.
The preferred embodiments of the present invention have been described above in detail, but the present invention is not limited thereto. Within the scope of the technical idea of the invention, many simple modifications can be made to the technical solution of the invention, including combinations of various technical features in any other suitable way, and these simple modifications and combinations should also be regarded as the disclosure of the invention, and all fall within the scope of the invention.
Claims (12)
1. The high-temperature-resistant polyacrylamide gel plugging agent is characterized by comprising the following components in percentage by weight: acrylamide polymer, water-soluble urea-formaldehyde resin, organic chromium, an oxygen scavenger, a urea compound and water, wherein the urea compound has a structure shown in a formula (1) and/or a formula (2),
wherein R is1And R2Each independently selected from hydrogen or 2-propynyl, R3And R4Each independently selected from oxygen, sulfur or imino;
based on the total weight of the high-temperature resistant polyacrylamide gel plugging agent, the content of the urea compound is 0.1-2 wt%.
2. The high-temperature resistant polyacrylamide gel plugging agent according to claim 1, wherein the content of the urea compound is 0.2-1 wt% based on the total weight of the high-temperature resistant polyacrylamide gel plugging agent.
3. The high temperature resistant polyacrylamide gel blocking agent according to claim 1 or 2, wherein the urea compound is one or more of urea, 2-propynyl urea, biuret, thiobiuret and 2-imino-4-thiobiuret, preferably urea.
4. The high-temperature resistant polyacrylamide gel plugging agent according to claim 1 or 2, wherein the content of the acrylamide polymer is 0.1-2 wt%, the content of the water-soluble urea-formaldehyde resin is 0.1-2 wt%, the content of the organic chromium is 0.01-2 wt%, and the content of the oxygen scavenger is 0.05-1 wt%, based on the total weight of the high-temperature resistant polyacrylamide gel plugging agent.
5. The high-temperature-resistant polyacrylamide gel plugging agent according to claim 1 or 4, wherein the water-soluble urea-formaldehyde resin is prepared from formaldehyde and urea according to the weight ratio of 1-3: 1, is polymerized.
6. The high temperature resistant polyacrylamide gel blocking agent according to claim 1 or 4, wherein the acrylamide polymer is one or more of partially hydrolyzed polyacrylamide, partially hydrolyzed methylene polyacrylamide, acrylamide/acrylic acid/AMPS sodium salt copolymer and acrylamide/acrylic acid/acrylonitrile sodium salt copolymer.
7. The high-temperature resistant polyacrylamide gel block agent according to claim 6, wherein the viscosity-average molecular weight of the acrylamide polymer is 800-3500 ten thousand; the hydrolysis degree of the acrylamide polymer is 8-35%.
8. The high-temperature-resistant polyacrylamide gel blocking agent according to claim 1 or 4, wherein the oxygen scavenger is one or more of sodium thiosulfate, sodium sulfite, sodium bisulfite, sodium hydrosulfite and erythorbic acid.
9. The high-temperature-resistant polyacrylamide gel blocking agent according to claim 1 or 4, wherein the organic chromium is one or more of chromium acetate, chromium oxalate, chromium lactate, chromium propionate, chromium malonate and chromium citrate, preferably chromium lactate.
10. A method for preparing the high temperature resistant polyacrylamide gel blocking agent of any one of claims 1-9, wherein the method comprises:
(1) dissolving the acrylamide polymer in water to obtain a polymer aqueous solution;
(2) and adding water-soluble urea-formaldehyde resin, organic chromium, a urea compound and an oxygen scavenger into the polymer aqueous solution, and stirring until the mixture is dissolved to obtain the high-temperature-resistant polyacrylamide gel plugging agent.
11. Use of the high temperature resistant polyacrylamide gel block of any one of claims 1-9 in heavy oil steam stimulation thermal recovery.
12. The application of claim 11, wherein the application comprises: and injecting the high-temperature-resistant polyacrylamide gel plugging agent into the stratum, so that the high-temperature-resistant polyacrylamide gel plugging agent is crosslinked in situ in the stratum to form gel.
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