CN112551807A - Treatment method and treatment system for three-gas combined production flowback fluid - Google Patents
Treatment method and treatment system for three-gas combined production flowback fluid Download PDFInfo
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Abstract
The invention provides a method for treating three-gas combined production flowback fluid. Compared with the prior art, the invention utilizes an advanced oxidation method, a zero-valent iron reduction method and a microbiological method to cooperatively treat the three-gas combined production return liquid, utilizes soil in the system to intercept and filter particles in the three-gas combined production return liquid, utilizes plants to absorb organic matters in the three-gas combined production return liquid, utilizes microorganisms to decompose organic pollutants in the three-gas combined production return liquid, and utilizes an adsorbent to remove ions such as fluorine, arsenic, iron, manganese and the like in the three-gas combined production return liquid, has simple and reliable operation, low operation cost and small floor area, and is suitable for in-situ treatment of the output water of a single-port gas well field in the three-gas combined production well field.
Description
Technical Field
The invention belongs to the technical field of environmental engineering, and particularly relates to a treatment method and a treatment system for three-gas combined production flowback liquid.
Background
Due to the particularity of geological structures, most unconventional natural gas fields (such as the east edge of the Ordors basin and the south gas field of the Qin basin) in China contain coal beds, sandstone beds and shale beds. By adopting the 'three-gas' co-production technology, the natural gas resource can be comprehensively developed by selecting a proper technology according to the 'three-gas' co-production characteristics in different areas, so that not only can the comprehensive development and the facility sharing be realized, but also the exploitation cost can be greatly reduced and the exploitation efficiency of the resource can be improved.
The hydraulic fracturing is the core technology of unconventional natural gas, and in the process of 'three-gas combined production', a fracturing fluid containing fine sand and multi-component chemical additives is injected into a target gas-rich stratum through a shaft by using a surface high-pressure pump to perform fracturing so as to achieve the purpose of releasing natural gas in the stratum. The hydraulic fracturing process can produce a large amount of flowback fluid.
The flowback fluid after fracturing operation contains solid particles in stratum and coal bed, residual additives such as thickening agent, cross-linking agent, pH value regulator, bactericide and the like, has complex components, high viscosity, high organic matter content and poor biodegradability, and can cause serious harm to the environment, especially water environment if the flowback fluid is directly discharged without effective treatment. Due to the complex components of the flowback fluid, no mature treatment technology and process exist.
At present, the main treatment of the flowback liquid comprises a coagulating sedimentation method, an advanced oxidation method, a biochemical method and the like, and the discharge reaching the standard is often difficult to realize.
Disclosure of Invention
In view of this, the technical problem to be solved by the present invention is to provide a method and a system for treating a three-gas combined production flowback liquid, which are simple and easy to operate, reliable in operation, good in treatment effect, and thorough in removal of organic pollutants.
The invention provides a method for treating three-gas combined production flowback fluid, which comprises the following steps:
s1) precipitating the three-gas combined production flowback fluid to obtain a precipitated flowback fluid;
s2) carrying out micro-electrolysis treatment on the precipitated flowback liquid to obtain the micro-electrolysis treated flowback liquid;
s3) carrying out oxidation reaction on the return liquid subjected to micro-electrolysis treatment and a hydrogen peroxide solution to obtain the return liquid subjected to oxidation treatment;
s4) adjusting the pH value of the waste liquid after the oxidation treatment to be neutral or alkalescent for coagulating sedimentation to obtain the waste liquid after coagulating sedimentation;
s5) carrying out zero-valent iron reduction treatment on the flowback liquid after the coagulating sedimentation to obtain a flowback liquid after the zero-valent iron reduction treatment;
s6) treating the flowback liquid subjected to zero-valent iron reduction treatment by microorganisms to obtain a microbiologically treated flowback liquid;
s7) treating the flowback liquid after the microbial treatment by wetland microbes to obtain effluent.
Preferably, the pH value of the return liquid during the micro-electrolysis treatment in the step S2) is 3-3.5; the micro-electrolysis treatment time is 90-120 min.
Preferably, the micro-electrolysis treatment in the step S2) is performed with aeration; the gas-water ratio of aeration is (3-3.5): 1.
preferably, the mass concentration of the hydrogen peroxide solution in the step S3) is 25% to 30%; the mass of the hydrogen peroxide solution is 0.1-0.2% of the mass of the flow-back fluid after micro-electrolysis treatment; the time of the oxidation reaction is 90-120 min.
Preferably, the pH value of the oxidized flowback liquid in the step S4) is adjusted to 7-8; the coagulating sedimentation time is 120-150 min.
Preferably, the mass ratio of the zero-valent iron to the activated carbon in the zero-valent iron reduction treatment in the step S5) is (1.5-2.5): 1; the time for the zero-valent iron reduction treatment is 100-200 min.
Preferably, the mass ratio of the zero-valent iron to the activated carbon in the zero-valent iron reduction treatment in step S5) is 2: 1.
Preferably, the time for the microbial treatment in the step S6) is 120-180 min.
The invention also provides a treatment system of the three-gas combined production flowback fluid, which comprises the following steps:
a sedimentation tank;
the micro-electrolysis reactor is communicated with the water outlet of the sedimentation tank;
the Fenton reactor is communicated with the water outlet of the micro-electrolysis reactor;
the coagulating sedimentation device is communicated with a water outlet of the Fenton reactor;
the zero-valent iron reaction device is communicated with the water outlet of the coagulating sedimentation device;
the microbial reactor is communicated with a water outlet of the zero-valent iron reaction device;
and the wetland is communicated with the water outlet of the microbial reactor.
The invention provides a method for treating three-gas combined production flowback fluid, which comprises the following steps: s1) precipitating the three-gas combined production flowback fluid to obtain a precipitated flowback fluid; s2) carrying out micro-electrolysis treatment on the precipitated flowback liquid to obtain the micro-electrolysis treated flowback liquid; s3) carrying out oxidation reaction on the return liquid subjected to micro-electrolysis treatment and a hydrogen peroxide solution to obtain the return liquid subjected to oxidation treatment; s4) adjusting the pH value of the waste liquid after the oxidation treatment to be neutral or alkalescent for coagulating sedimentation to obtain the waste liquid after coagulating sedimentation; s5) carrying out zero-valent iron reduction treatment on the flowback liquid after the coagulating sedimentation to obtain a flowback liquid after the zero-valent iron reduction treatment; s6) treating the flowback liquid subjected to zero-valent iron reduction treatment by microorganisms to obtain a microbiologically treated flowback liquid; s7) treating the flowback liquid after the microbial treatment by wetland microbes to obtain effluent. Compared with the prior art, the invention utilizes an advanced oxidation method, a zero-valent iron reduction method and a microbiological method to cooperatively treat the three-gas combined production return liquid, utilizes soil in the system to intercept and filter particles in the three-gas combined production return liquid, utilizes plants to absorb organic matters in the three-gas combined production return liquid, utilizes microorganisms to decompose organic pollutants in the three-gas combined production return liquid, and utilizes an adsorbent to remove ions such as fluorine, arsenic, iron, manganese and the like in the three-gas combined production return liquid, has simple and reliable operation, low operation cost and small floor area, and is suitable for in-situ treatment of the output water of a single-port gas well field in the three-gas combined production well field.
Drawings
Fig. 1 is a schematic diagram of a three-gas combined production flowback fluid treatment system provided by the invention.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The invention provides a treatment system of three-gas combined production flowback fluid, which comprises:
a sedimentation tank;
the micro-electrolysis reactor is communicated with the water outlet of the sedimentation tank;
the Fenton reactor is communicated with the water outlet of the micro-electrolysis reactor;
the coagulating sedimentation device is communicated with a water outlet of the Fenton reactor;
the zero-valent iron reaction device is communicated with the water outlet of the coagulating sedimentation device;
the microbial reactor is communicated with a water outlet of the zero-valent iron reaction device;
and the wetland is communicated with the water outlet of the microbial reactor.
Referring to fig. 1, fig. 1 is a schematic diagram of a three-gas-combined flow-back liquid treatment system provided by the present invention.
The invention also provides a method for treating the three-gas combined production flowback fluid by adopting the treatment system, which comprises the following steps: s1) precipitating the three-gas combined production flowback fluid to obtain a precipitated flowback fluid; s2) carrying out micro-electrolysis treatment on the precipitated flowback liquid to obtain the micro-electrolysis treated flowback liquid; s3) carrying out oxidation reaction on the return liquid subjected to micro-electrolysis treatment and a hydrogen peroxide solution to obtain the return liquid subjected to oxidation treatment; s4) adjusting the pH value of the waste liquid after the oxidation treatment to be neutral or alkalescent for coagulating sedimentation to obtain the waste liquid after coagulating sedimentation; s5) carrying out zero-valent iron reduction treatment on the flowback liquid after the coagulating sedimentation to obtain a flowback liquid after the zero-valent iron reduction treatment; s6) treating the flowback liquid subjected to zero-valent iron reduction treatment by microorganisms to obtain a microbiologically treated flowback liquid; s7) treating the flowback liquid after the microbial treatment by wetland microbes to obtain effluent.
After the suspended matters of the return liquid are removed by precipitation; the organic pollutant degradation of the flowback liquid is removed by utilizing the combined process of iron-carbon micro-electrolysis and Fenton, and meanwhile, the biodegradability of the treated effluent can be improved and the toxicity of the produced effluent can be reduced; reducing by utilizing zero-valent iron to remove residual organic pollutants in the produced water, and further improving the biodegradability of the flowback liquid; carrying out microbial treatment on the produced water after reduction treatment; the produced water after the microbial treatment enters an ecological wetland, and the final treatment of the 'three-gas combined mining' return fluid is completed by utilizing the substrate and the organisms in the wetland. The method is easy to implement, simple and convenient to operate, reliable to operate, good in treatment effect and thorough in organic pollutant removal, and the treated effluent can directly reach the standard and be discharged or recycled.
The present invention is not particularly limited in terms of the source of all raw materials, and may be commercially available.
Precipitating the three-gas combined recovery flow-back liquid to obtain a precipitated flow-back liquid; the precipitation treatment is preferably carried out in a reprecipitation tank; removing larger particles and suspended matters in the sedimentation tank through sedimentation; the time of the precipitation treatment is preferably 200-240 min.
Carrying out micro-electrolysis treatment on the precipitated flowback liquid to obtain micro-electrolysis treated flowback liquid; the microelectrolytic treatment is preferably carried out in a microelectrolytic reactor; the pH value of the return liquid after precipitation during micro-electrolysis treatment is preferably 3-3.5; in the invention, the pH value is preferably adjusted by adopting an inorganic acid solution with the mass fraction of 2-25%; the mass fraction of the inorganic acid solution is more preferably 5 to 25%, still more preferably 10 to 25%, and most preferably 15 to 20%; the inorganic acid solution is preferably one or more of hydrochloric acid, sulfuric acid and nitric acid; the micro-electrolysis treatment is preferably carried out while aeration is carried out; the gas-water ratio of aeration is preferably (3-3.5): 1; the time of the micro-electrolysis treatment is preferably 90-120 min.
Carrying out oxidation reaction on the return liquid subjected to micro-electrolysis treatment and a hydrogen peroxide solution to obtain oxidized return liquid; the oxidation reaction is preferably carried out in a Fenton reactor; the mass concentration of the hydrogen peroxide solution is preferably 25-30%, and more preferably 30%; the mass of the hydrogen peroxide solution is preferably 0.1-0.2% of that of the return liquid after micro-electrolysis treatment; the oxidation reaction is preferably carried out under stirring conditions; the stirring is preferably carried out by means of aeration; the gas-water ratio of aeration is preferably (3-3.5): 1; the time of the oxidation reaction is preferably 90-120 min.
Adjusting the pH value of the flow-back liquid after the oxidation treatment to be neutral or alkalescent for coagulating sedimentation to obtain a flow-back liquid after coagulating sedimentation; in the invention, the pH value of the oxidized flowback liquid is preferably adjusted to 7-8; in the invention, sodium hydroxide solution is adopted to adjust the pH value; the concentration of the sodium hydroxide solution is preferably 0.5-2 mol/L, and more preferably 1-2 mol/L; in the coagulating sedimentation treatment process, preferably, a coagulant is added firstly, after the reaction is carried out for 3-6 min, a flocculating agent is added, the reaction is carried out for 6-8 min, then the precipitation is carried out, and formed floc is removed through precipitation; the coagulant is preferably polyaluminium chloride and/or polyferric sulfate; the addition amount of the coagulant is preferably 10-50 mg/L; the flocculating agent is preferably one or more of nonionic polyacrylamide, anionic polyacrylamide and cationic polyacrylamide; the addition amount of the flocculating agent is preferably 1-3 mg/L; the time for the coagulating sedimentation treatment is preferably 120-150 min; larger suspended matters can be removed through coagulating sedimentation.
Reducing the flow-back liquid after the coagulating sedimentation by using zero-valent iron to obtain the flow-back liquid after the zero-valent iron reduction; the zero-valent iron reduction treatment is preferably carried out in a zero-valent iron reaction device; zero-valent iron and active carbon are filled in the zero-valent iron reaction device; the mass ratio of the zero-valent iron to the activated carbon is preferably (1.5-2.5) to 1, more preferably 2: 1; the time for the zero-valent iron reduction treatment is preferably 100-200 min.
Fenton advanced oxidation generates OH free radicals with extremely strong activity in reaction, and then macromolecules and refractory organic matters in water are oxidized and degraded into low-toxicity or non-toxic micromolecular substances, even into CO through addition, substitution, electron transfer, bond breaking and the like between the free radicals and organic compounds2And H2O, having "broad spectrum"; the reductive treatment of wastewater by zero-valent iron has many limitations, so that macromolecular refractory organic matters in the flowback liquid need to be firstly decomposed into micromolecular organic matters, and then the treatment by the zero-valent iron is carried out to improve the treatment efficiency.
Treating the flowback liquid subjected to zero-valent iron reduction treatment by microorganisms to obtain a flowback liquid subjected to microorganism treatment; the microbial treatment is preferably carried out in a microbial reactor; the time of the microbial reaction is preferably 120-180 min. And further removing the residual organic pollution in the flowback liquid through microbial reaction.
Treating the flowback liquid subjected to the microbial treatment by using wetland microbes to obtain effluent; organic pollutants in water are degraded by using microorganisms in the wetland, and F, Fe, Mn and other ions in the water can be removed by using the wetland adsorption, so that the treated effluent can be directly discharged or recycled.
The invention utilizes an advanced oxidation method, a zero-valent iron reduction method and a microbiological method to cooperatively treat the 'three-gas combined production' return fluid, utilizes soil in a system to intercept and filter particles in the 'three-gas combined production' return fluid, utilizes plants to absorb organic matters in the 'three-gas combined production' return fluid, utilizes microorganisms to decompose organic pollutants in the 'three-gas combined production' return fluid, utilizes an adsorbent to remove fluorine, arsenic, iron, manganese and other ions in the 'three-gas combined production' return fluid, has simple and reliable operation, low operation cost and small floor area, and is suitable for the 'three-gas combined production' well site to treat the produced water of a single-mouth gas well in situ.
In order to further explain the present invention, the following describes in detail a treatment method and a treatment system for a three-gas combined production flowback fluid provided by the present invention with reference to an embodiment.
The reagents used in the following examples are all commercially available.
Example 1
a. And discharging the three-gas combined mining return liquid into a sedimentation tank, and settling in the sedimentation tank to remove larger particles and suspended matters in the three-gas combined mining return liquid.
b. The three-gas combined production return fluid without larger particles and suspended matters is pumped into a micro-electrolysis reactor, the pH value of the three-gas combined production return fluid is adjusted to 3.0 in the micro-electrolysis reactor, and meanwhile, aeration is carried out in the reactor, and the three-gas combined production return fluid stays in the micro-electrolysis reactor for 100 min.
c. Feeding the 'three-gas combined production' flowback liquid after micro-electrolysis reaction into a Fenton reactor, and simultaneously adding 30% of H into the reaction2O2The addition amount is 1.5 per mill of the treatment water amount, and the return liquid of the three-gas combined production stays in the Fenton reactor for 90 min.
d. Adjusting the pH of the Fenton-treated 'three-gas-combined-production' return liquid to 7-8 by using 1mol/L sodium hydroxide aqueous solution, then feeding the return liquid into a coagulating sedimentation device, adding 30mg/LPAC into the coagulating sedimentation device for reaction for 5min, then adding 2mg/LPAM, and feeding the return liquid into a sedimentation tank for sedimentation after reacting for 6 min; staying in the coagulating sedimentation device for 120min and then entering a zero-valent iron reaction device.
e. Effluent water after removing suspended matters and particles in water through coagulating sedimentation stays in a zero-valent iron reaction device for 120min, zero-valent iron and granular activated carbon are filled in the zero-valent iron reaction, and the mass ratio of the zero-valent iron to the activated carbon is 2: 1.
f. The produced water after the zero-valent iron reaction stays in the microbial reactor for 160min, the residual organic pollution in the produced water is further removed through the microbial reaction, and the effluent enters the wetland;
g. after the effluent of the microbial bioreactor enters the wetland, the microorganisms in the wetland are utilized to degrade residual organic pollutants in the water, meanwhile, the wetland is utilized to adsorb and remove F, Fe and Mn ions in the water, and the treated effluent can be discharged or recycled.
According to the steps, the case of treating the flowback fluid of a certain coal bed gas field in Shanxi is treated, the COD of the flowback fluid containing the fracturing fluid is 6700mg/l, the COD of the flowback fluid after being precipitated in a primary sedimentation tank is 6530mg/l, the flowback fluid enters a micro-electrolysis reactor after being subjected to pH regulation, the COD of the effluent after reaction is 3970mg/l, the COD of the effluent after reaction is 2350mg/l after reaction in a Fenton reactor, the effluent after coagulation precipitation enters a zero-valent iron reactor, the effluent after being treated by the zero-valent iron reactor is 1220mg/l, the effluent enters a biochemical reactor, the COD of the effluent after biochemical treatment is 230mg/l, the effluent is further treated by a wetland, and the final COD of the effluent is 48mg/l, so that the discharge standard is reached.
According to the case of treating the flowback fluid of a certain coal bed gas field in Shaanxi, the COD of the flowback fluid containing the fracturing fluid is 4650mg/l, the COD of the flowback fluid after being precipitated by a primary sedimentation tank is 4530mg/l, the flowback fluid enters a micro-electrolysis reactor after being subjected to pH regulation, the COD of the effluent after reaction is 2765mg/l, the COD of the effluent after reaction enters a Fenton reactor for reaction is 1950mg/l, the effluent after coagulation precipitation enters a zero-valent iron reactor, the COD of the effluent after being treated by the zero-valent iron reactor is 890mg/l, the effluent enters a biochemical reactor, the COD of the effluent after biochemical treatment is 180mg/l, the effluent is further treated by a wetland, and the COD of the final effluent is 42mg/l, so that the discharge standard is reached.
Claims (9)
1. A treatment method of three-gas combined production flowback fluid is characterized by comprising the following steps:
s1) precipitating the three-gas combined production flowback fluid to obtain a precipitated flowback fluid;
s2) carrying out micro-electrolysis treatment on the precipitated flowback liquid to obtain the micro-electrolysis treated flowback liquid;
s3) carrying out oxidation reaction on the return liquid subjected to micro-electrolysis treatment and a hydrogen peroxide solution to obtain the return liquid subjected to oxidation treatment;
s4) adjusting the pH value of the waste liquid after the oxidation treatment to be neutral or alkalescent for coagulating sedimentation to obtain the waste liquid after coagulating sedimentation;
s5) carrying out zero-valent iron reduction treatment on the flowback liquid after the coagulating sedimentation to obtain a flowback liquid after the zero-valent iron reduction treatment;
s6) treating the flowback liquid subjected to zero-valent iron reduction treatment by microorganisms to obtain a microbiologically treated flowback liquid;
s7) treating the flowback liquid after the microbial treatment by wetland microbes to obtain effluent.
2. The treatment method according to claim 1, wherein the pH value of the flowback liquid during the micro-electrolysis treatment in the step S2) is 3-3.5; the micro-electrolysis treatment time is 90-120 min.
3. The process according to claim 1, wherein the microelectrolysis treatment in step S2) is carried out with aeration; the gas-water ratio of aeration is (3-3.5): 1.
4. the treatment method according to claim 1, wherein the mass concentration of the hydrogen peroxide solution in the step S3) is 25-30%; the mass of the hydrogen peroxide solution is 0.1-0.2% of the mass of the flow-back fluid after micro-electrolysis treatment; the time of the oxidation reaction is 90-120 min.
5. The treatment method according to claim 1, wherein the pH value of the oxidized flowback liquid in the step S4) is adjusted to 7-8; the coagulating sedimentation time is 120-150 min.
6. The treatment method according to claim 1, wherein the mass ratio of the zero-valent iron to the activated carbon in the zero-valent iron reduction treatment in step S5) is (1.5-2.5): 1; the time for the zero-valent iron reduction treatment is 100-200 min.
7. The treatment method according to claim 6, wherein the mass ratio of the zero-valent iron to the activated carbon in the zero-valent iron reduction treatment in step S5) is 2: 1.
8. The method as claimed in claim 1, wherein the time for the microbial treatment in step S6) is 120-180 min.
9. A three gas recovery combined flowback fluid treatment system is characterized by comprising:
a sedimentation tank;
the micro-electrolysis reactor is communicated with the water outlet of the sedimentation tank;
the Fenton reactor is communicated with the water outlet of the micro-electrolysis reactor;
the coagulating sedimentation device is communicated with a water outlet of the Fenton reactor;
the zero-valent iron reaction device is communicated with the water outlet of the coagulating sedimentation device;
the microbial reactor is communicated with a water outlet of the zero-valent iron reaction device;
and the wetland is communicated with the water outlet of the microbial reactor.
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| CN102786186A (en) * | 2012-08-09 | 2012-11-21 | 杨德敏 | Shale gas fracturing flow-back waste liquid treatment method |
| WO2015194739A1 (en) * | 2014-06-20 | 2015-12-23 | 우진건설주식회사 | Waste water treatment method using micro-electrolysis reaction, and micro-electrolysis material thereof |
| CN105668948A (en) * | 2016-04-11 | 2016-06-15 | 中国矿业大学 | Treating method for coal-bed gas field produced water |
| CN109209268A (en) * | 2018-10-19 | 2019-01-15 | 中国石油集团渤海钻探工程有限公司 | The method that drain is returned in acidification is handled using reproducibility iron powder |
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