CN104291334A - Method for promoting growth of gas hydrate - Google Patents
Method for promoting growth of gas hydrate Download PDFInfo
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- CN104291334A CN104291334A CN201410460643.4A CN201410460643A CN104291334A CN 104291334 A CN104291334 A CN 104291334A CN 201410460643 A CN201410460643 A CN 201410460643A CN 104291334 A CN104291334 A CN 104291334A
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Abstract
The invention provides a method for promoting growth of a gas hydrate. According to the method, a gas is blown into a gas hydrate promoter solution; and at the temperature of 0-20 DEG C and at the pressure of 0-15 MPa, stirring is carried out at the rotating speed of 400-600r/min so as to obtain a gas hydrate, wherein the gas hydrate promoter solution is an aqueous solution of an amphoteric perfluoroalkyl ether betaine surfactant with the concentration being 100-1,000 ppm. By the method for promoting growth of the gas hydrate, nucleation and clustering of the gas hydrate can effectively be promoted, and induction time is shortened. In addition, surface tension of the gas hydrate is reduced remarkably, reaction time is shortened, production cost is low, and the promotion effect is more excellent.
Description
Technical field
The present invention relates to a kind of method promoting growth of aerial hydrate, particularly a kind of method promoting carbon dioxide hydrate growth, belongs to oil recovery technical field.
Background technology
Along with the continuous increase of energy-output ratio, a large amount of industrial gaseous wastees is directly drained in air, wherein CO
2the arch-criminal causing Greenhouse effect, therefore, CO
2seizure and Plugging Technology Applied seem particularly important.Traditional CO
2the equipment volume that recovery method ubiquity uses is huge, the shortcoming that cost of investment is higher.
Gas hydrate is gas (N
2, CO
2, CH
4, C
2h
6deng) and a kind of cage type crystalline compounds of generating under cryogenic high pressure condition of water.In gas hydrate, form lattice structure between water molecules by stronger hydrogen bonded, gas molecule utilizes the Van der Waals force between water molecules to be filled in interlattice cage.
In recent years, hydrate reclaims, seals CO up for safekeeping
2technology obtains extensive concern both domestic and external.With other CO
2capture method is compared, and hydrate seals CO up for safekeeping
2technology has the following advantages: the gas-storing capacity sealing trapping up for safekeeping is large; Formation condition easily realizes; Can to reuse and safe and reliable.But the generation due to gas hydrate is similar to one crystallisation process slowly, wherein along with complex processes such as gas-liquid-solid three-phase mass-and heat-transfers, research finds, existing hydrate sends out the method for sealing gas up for safekeeping, the induction time of ubiquity gas hydrate is long, and generating rate is slow, the shortcoming of long reaction time, and the existence due to liquid-vapo(u)r interface place hydrate film hinders gas and enters liquid phase, reaction cannot be carried out continuously.
The method that current hydrate seals gas up for safekeeping generally adopts gas hydrate accelerant, for realizing generating continuously fast of gas hydrate, and improves gas storage density.But, existing gas hydrate accelerant more or less have that induction time is long, application conditions is harsh, cost is high, application art is complicated, addition is high and corresponding facilitation effect difference and the shortcoming such as application is single.
In sum, provide a kind of and obviously can shorten induction time, the method for growth of aerial hydrate of speed of reaction that improves gas hydrate is one of this area problem demanding prompt solution.
Summary of the invention
In order to solve the problem, the object of the present invention is to provide a kind of method promoting growth of aerial hydrate, the method can promote the generation of gas hydrate effectively, reduce gas hydrate balance each other a little, shorten induction time, improve speed of reaction and the gas storage density of gas hydrate.
In order to achieve the above object, the invention provides a kind of method promoting growth of aerial hydrate, the method comprises the following steps:
Gas is passed in gas hydrate accelerant solution, temperature be 0-20 DEG C (being preferably 2-10 DEG C), pressure is under the condition of 0-15MPa (being preferably 1.5-10MPa), stir 3-13min (being preferably 5min) with the rotating speed of 400-600r/min (being preferably 550r/min), obtain gas hydrate;
Wherein, the aqueous solution of described gas hydrate accelerant solution to be concentration the be both sexes perfluoroalkyl ethers beet alkali surface activator of 100-1000ppm.
In the method for promotion growth of aerial hydrate provided by the invention, preferably, be in the reactor of 500mL at cubic capacity, the volume ratio of gas hydrate accelerant solution and gas is 1/30-1/220:1.
According to the specific embodiment of the present invention, wherein, the volume ratio of its gas hydrate accelerant solution and gas and the cubic capacity of reactor, liquid inlet volume, temperature and pressure are relevant, here only provide its liquid gas volume ratio with described condition and 500mL reactor, its liquid gas volume ratio is 1/30-1/220:1.
In the method for promotion growth of aerial hydrate provided by the invention, preferably, the both sexes perfluoroalkyl ethers beet alkali surface activator of employing comprises fluorocarbon surfactant Intechem-01 (FC-01).
In the method for promotion growth of aerial hydrate provided by the invention, preferably, the gas of employing comprises CO
2, CH
4, C
2h
6or N
2deng, more preferably, the gas of employing is CO
2.
In the method for promotion growth of aerial hydrate provided by the invention, preferably, the aqueous solution of gas hydrate accelerant solution used to be concentration the be both sexes perfluoroalkyl ethers beet alkali surface activator of 100ppm, 500ppm or 1000ppm.
The gas hydrate accelerant used in the method for promotion growth of aerial hydrate provided by the invention can be dissolved in majority of organic solvent, has good composite effect.In cationic in acidic medium, in anionic in alkaline medium, be aobvious both sexes in the medium of 6-8 at pH, effectively can promote gas hydrate nucleation cluster, shorten induction time, and significantly reduce the surface tension of gas hydrate, the surface tension of the gas hydrate using it to be formed is not more than 16.8mN/m under application of temperature and applying pressure, gas-liquid molecule is fully contacted, Reaction time shorten.
The method of promotion growth of aerial hydrate provided by the invention, specifically comprises the following steps:
Step one: gas hydrate generating apparatus is vacuumized to remove unnecessary gas with vacuum pump, the pumpdown time is 5min, then by gas hydrate accelerant injected slurry volume be 500mL autoclave in;
Step 2: open thermostatical water bath, initial temperature and pressure are set, after the temperature-stable in autoclave, injection experiments gas, after air inlet terminates, opens and stirs (400-600r/min), gas hydrate generates fast, in gas hydrate generative process, the data such as record temperature and pressure, obtain gas hydrate;
Subsequently, treat that gas hydrate generates completely, and pressure is not when changing, exhaust, the record temperature of gas hydrate in decomposition course, pressure, that finds gas hydrate balances each other a little; The solution in autoclave to be extracted before carrying out next group experiment out, and repeatedly clean, guarantee the accurate of gas promoter concentration.
The method of promotion growth of aerial hydrate provided by the invention, compared with the method for existing promotion growth of aerial hydrate, has the following advantages:
The gas hydrate accelerant of the method employing of promotion growth of aerial hydrate provided by the invention obviously can reduce the liquid-gas interface tension force of gas hydrate reaction, promote gas dissolving, shorten induction time, under application of temperature and applying pressure, the surface tension of the gas hydrate obtained is not more than 16.8mN/m, compared with deionized water, reduce 30%;
The gas hydrate accelerant that the present invention uses obviously can shorten the induction time of gas hydrate, CO under experiment condition
2hydrate induction time is about 3-8min, reaction times shorten in average about 20min, and vapor pressure also decreases;
The cost of the gas hydrate accelerant that the present invention uses is low, consumption is few, and because the main additive (both sexes perfluoroalkyl ethers beet alkali surface activator) of this gas hydrate accelerant belongs to the compound containing fluorine structure, side chain ether-containing key is containing fluorine structure, biodegradable, belong to low-carbon environment-friendly gas hydrate accelerant;
The applied range of the method for promotion growth of aerial hydrate provided by the invention, can be applied in fields such as hydrate storage and transportation technology, hydrate separation technology and sea water desaltinations;
The method of promotion growth of aerial hydrate provided by the invention simple to operate.
Accompanying drawing explanation
Fig. 1 is the structural representation of the synthesizer of the gas hydrate of embodiment 1.
Fig. 2 is the change curve of surface tension with concentration of sodium lauryl sulphate (SDS) and fluorocarbon surfactant Intechem-01 (FC-01).
Fig. 3 is the CO in the FC-01 solution of different concns and in SDS (500ppm) solution
2the phase equilibrium line figure that gas hydrate generates.
Fig. 4 is CO in FC-01 and SDS bis-kinds of different solutions systems
2the pressure fall-off curve that hydrate generates.
Main Reference nomenclature:
1 bomb 2 stopping valve 3 high pressure gas drive supercharging device 4 autoclave 5 thermostatical water bath 6 tank 7 magnetic stirring equipment 8 vent valve 9 temperature, pressure monitor station 10 data acquisition unit
Embodiment
In order to there be understanding clearly to technical characteristic of the present invention, object and beneficial effect, existing following detailed description is carried out to technical scheme of the present invention, but can not be interpreted as to of the present invention can the restriction of practical range.
The promotion of the current traditional Surfactant On Hydrate generally adopted be surface tension by reducing liquid-gas interface with the resistance to mass transfer reduced between gas-liquid make gas molecule more easily catch by water molecules.Therefore, the impact of tensio-active agent effects on surface tension force is the important indicator weighing facilitation effect and accelerator level.Fig. 2 is the impact of the concentration effects on surface tension force of sodium lauryl sulphate (SDS) and base ether alcohol ammonium salt type anion surfactant FC-01.As can be seen from Figure 2, under same experimental conditions, when temperature is 25 DEG C, it is more that FC-01 can make the surface tension of liquid-gas interface reduce, and its desired concn is also lower, and therefore, consumption is less.In addition, by the CO of different concns FC-01
2gas hydrate generates phase equilibrium line and SDS (500ppm) phase equilibrium line contrasts, and as shown in Figure 3, Fig. 3 is CO in different concns FC-01 solution and in SDS (500ppm) solution to result
2the phase equilibrium line that gas hydrate generates.As seen from Figure 3, SDS is as kinetics promotor, and it generates on gas hydrate the not impact that balances each other a little mutually, and its vapor pressure has had the decline of certain amplitude under comparatively high temps (> 277K) condition.
Embodiment 1
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, is completed by the synthesizer of gas hydrate, and as shown in Figure 1, detailed process comprises the following steps the structure of this device:
Step one: vacuumized to remove unnecessary gas by whole device with vacuum pump, the pumpdown time is 5min, opens stopping valve 2, the CO in bomb 1
2gas purging gas circulation line 2-3 time, close stopping valve 2, again the gas hydrate accelerant solution (mass concentration is the fluorocarbon surfactant Intechem-01 (FC-01) of 100ppm) of 200mL is injected autoclave 4, magnetic stirring equipment 7 is housed in autoclave 4;
Step 2: open thermostatical water bath 5, arranges that initial temperature is 4 DEG C, after the temperature-stable in the autoclave 4 be in tank 6, tank, built with magnetic stirring equipment 7, opens stopping valve 2, injects CO
2, by high pressure gas drive supercharging device 3, carry out supercharging to gas, make the pressure in still reach set(ting)value 3MPa, after air inlet terminates, close stopping valve 2, open and stir (400-600r/min), general control, at 550r/min, stirs after 5min, CO
2hydrate starts to generate, at CO
2in hydrate formation, the data of temperature and pressure are monitored by temperature, pressure monitor station 9 and by data acquisition unit 10 record;
Step 3: treat CO
2hydrate generates completely, and pressure is not when changing, open vent valve 8, start exhaust, the temperature, pressure of record gas hydrate in decomposition course, by sight glass visor, that finds gas hydrate balances each other a little, the solution in autoclave 4 to be extracted before carrying out next group experiment out, and repeatedly clean, guarantee the accurate of the concentration of gas hydrate accelerant solution.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 8min
2hydrate starts to be formed, and vapor pressure is 2.02MPa.
Comparative example 1
In order under (concentration in Fig. 2 corresponding to lowest surface tension, SDS:240ppm, FC-01:100ppm) condition of relatively optimum concn, observe CO in SDS and FC-01 bis-kinds of different accelerator systems
2the generative process of gas hydrate, has carried out CO in SDS (concentration is 240ppm) solution system
2the generative process experiment of gas hydrate, its control condition is identical with embodiment 1, and difference is the gas hydrate accelerant of employing to be mass concentration be the SDS solution of 240ppm.As shown in Figure 4, Fig. 4 is CO in FC-01 and SDS bis-kinds of different solutions systems to experimental result
2the pressure fall-off curve that hydrate generates, can find from Fig. 4, under optimum concn, the speed of pressure drop in two kinds of systems is substantially identical in the starting stage, but pressure drop rate is apparently higher than SDS solution in the second half section FC-01 system of gas hydrate reaction, this shows at the generating rate of starting stage hydrate substantially identical, and the generating rate in second half section FC-01 solution system is higher than SDS solution, in addition Fig. 4 also shows that in FC-01 system, overall pressure drop amplitude is larger, and it is more thorough that gas hydrate reaction is carried out.
Embodiment 2
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, the synthesizer of the gas hydrate adopting embodiment 1 to provide completes, the fluorocarbon surfactant Intechem-01 (FC-01) of the general gas hydrate accelerant being to adopt with, difference of detailed process and embodiment 1 to be mass concentration be 500ppm.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 6min
2hydrate starts to be formed, and vapor pressure is 1.98MPa.
Embodiment 3
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, the synthesizer of the gas hydrate adopting embodiment 1 to provide completes, the fluorocarbon surfactant Intechem-01 (FC-01) of the general gas hydrate accelerant being to adopt with, difference of detailed process and embodiment 1 to be mass concentration be 1000ppm.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 7.5min
2hydrate starts to be formed, and vapor pressure is 1.87MPa.
Embodiment 4
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, the synthesizer of the gas hydrate adopting embodiment 1 to provide completes, detailed process and embodiment 1 are generally same, difference is the gas hydrate accelerant that adopts to be mass concentration is the fluorocarbon surfactant Intechem-01 (FC-01) of 100ppm, initial temperature is 6 DEG C, and original pressure is 5MPa.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 12min
2hydrate starts to be formed, and vapor pressure is 2.34MPa.
Embodiment 5
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, the synthesizer of the gas hydrate adopting embodiment 1 to provide completes, the fluorocarbon surfactant Intechem-01 (FC-01) of the general gas hydrate accelerant being to adopt with, difference of detailed process and embodiment 4 to be mass concentration be 500ppm.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 5min
2hydrate starts to be formed, and vapor pressure is 2.18MPa.
Embodiment 6
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, the synthesizer of the gas hydrate adopting embodiment 1 to provide completes, the fluorocarbon surfactant Intechem-01 (FC-01) of the general gas hydrate accelerant being to adopt with, difference of detailed process and embodiment 4 to be mass concentration be 1000ppm.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 6.5min
2hydrate starts to be formed, and vapor pressure is 2.09MPa.
Embodiment 7
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, the synthesizer of the gas hydrate adopting embodiment 1 to provide completes, detailed process and embodiment 1 are generally same, difference is the gas hydrate accelerant that adopts to be mass concentration is the fluorocarbon surfactant Intechem-01 (FC-01) of 100ppm, and initial temperature is 2 DEG C.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 4min
2hydrate starts to be formed, and vapor pressure is 1.67MPa.
Embodiment 8
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, the synthesizer of the gas hydrate adopting embodiment 1 to provide completes, the fluorocarbon surfactant Intechem-01 (FC-01) of the general gas hydrate accelerant being to adopt with, difference of detailed process and embodiment 7 to be mass concentration be 500ppm.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 3.5min
2hydrate starts to be formed, and vapor pressure is 1.55MPa.
Embodiment 9
Present embodiments provide a kind of promotion CO
2the method of hydrate growth, the synthesizer of the gas hydrate adopting embodiment 1 to provide completes, the fluorocarbon surfactant Intechem-01 (FC-01) of the general gas hydrate accelerant being to adopt with, difference of detailed process and embodiment 7 to be mass concentration be 1000ppm.
The method of the promotion growth of aerial hydrate that the present embodiment provides, reaction starts CO after about 6min
2hydrate starts to be formed, and vapor pressure is 1.72MPa.
Claims (9)
1. promote a method for growth of aerial hydrate, the method comprises the following steps:
In gas hydrate accelerant solution, pass into gas, be 0-20 DEG C in temperature, and pressure is under the condition of 0-15MPa, stirs 3-13min, obtain gas hydrate with the rotating speed of 400-600r/min;
Wherein, the aqueous solution of described gas hydrate accelerant solution to be concentration the be both sexes perfluoroalkyl ethers beet alkali surface activator of 100-1000ppm.
2. the method for promotion growth of aerial hydrate according to claim 1, is characterized in that, is in the reactor of 500mL at cubic capacity, and the volume ratio of described gas hydrate accelerant solution and described gas is 1/30-1/220:1.
3. the method for promotion growth of aerial hydrate according to claim 1, is characterized in that, described both sexes perfluoroalkyl ethers beet alkali surface activator comprises fluorocarbon surfactant Intechem-01.
4. the method for promotion growth of aerial hydrate according to claim 1, is characterized in that, described temperature is 2-10 DEG C.
5. the method for promotion growth of aerial hydrate according to claim 1, is characterized in that, described gas comprises CO
2, CH
4, C
2h
6or N
2.
6. the method for promotion growth of aerial hydrate according to claim 1, wherein, described gas is CO
2.
7. the method for promotion growth of aerial hydrate according to claim 1, wherein, described pressure is 1.5-10MPa.
8. the method for promotion growth of aerial hydrate according to claim 1, wherein, described stirring stirs 5min under the rotating speed of 550r/min.
9. the method for promotion growth of aerial hydrate according to claim 1, wherein, the aqueous solution of described gas hydrate accelerant solution to be concentration the be both sexes perfluoroalkyl ethers beet alkali surface activator of 100ppm, 500ppm or 1000ppm.
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Cited By (6)
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| CN104857891A (en) * | 2015-05-20 | 2015-08-26 | 常州大学 | Hydrate promoter and preparation method thereof |
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| CN106914122A (en) * | 2017-04-18 | 2017-07-04 | 长沙紫宸科技开发有限公司 | It is continuously separated hydrate accelerant, the device and method of carbon dioxide in flue gas |
| CN109735373A (en) * | 2019-03-11 | 2019-05-10 | 中国科学院青岛生物能源与过程研究所 | A kind of preparation method of methane hydrate |
| CN112108096A (en) * | 2020-10-26 | 2020-12-22 | 河南理工大学 | Natural gas hydrate synthesis device and method integrating multiple strengthening methods |
| CN113817442A (en) * | 2020-06-18 | 2021-12-21 | 中国石油化工股份有限公司 | Dynamic hydrate accelerant, application and gas storage and transportation method |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN113817442A (en) * | 2020-06-18 | 2021-12-21 | 中国石油化工股份有限公司 | Dynamic hydrate accelerant, application and gas storage and transportation method |
| CN113817442B (en) * | 2020-06-18 | 2022-09-27 | 中国石油化工股份有限公司 | Dynamic hydrate accelerant, application and gas storage and transportation method |
| CN112108096A (en) * | 2020-10-26 | 2020-12-22 | 河南理工大学 | Natural gas hydrate synthesis device and method integrating multiple strengthening methods |
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Application publication date: 20150121 |