CN107551954A - A kind of method that fast hydrating gas storage is realized using hydrophobically modified foam metal - Google Patents
A kind of method that fast hydrating gas storage is realized using hydrophobically modified foam metal Download PDFInfo
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- CN107551954A CN107551954A CN201710699035.2A CN201710699035A CN107551954A CN 107551954 A CN107551954 A CN 107551954A CN 201710699035 A CN201710699035 A CN 201710699035A CN 107551954 A CN107551954 A CN 107551954A
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Abstract
The invention discloses a kind of method that fast hydrating gas storage is realized using hydrophobically modified foam metal.Liquid-phase system is injected into hydrophobic foam metal inside hole by the present invention, the gas storage medium of hydrophobically modified foam metal liquid feeding phase system is obtained, gas storage medium is placed in atmosphere, is 3 ~ 30 MPa in pressure, temperature is at 0 ~ 20 DEG C, and gas generates hydrate in gas storage medium and carries out gas storage；The gas includes one or more of methane, ethane, propane, nitrogen, oxygen, carbon monoxide or carbon dioxide.It is an advantage of the current invention that heat conduction skeleton of the foam metal as static hydrated body system, can export the hydration heat in the system of lodging in rapidly；After surface carries out hydrophobic treatment, liquid can not fully soak hydrophobically modified foam metal surface, and the space of liquid-solid contact may act as the passage of methane diffusion, so as to effectively improve the contact area of gas-liquid two-phase.
Description
Technical field
The present invention relates to gas hydrate technical field, and in particular to one kind is realized quick using hydrophobically modified foam metal
It is hydrated the method for gas storage.
Background technology
Gas hydrate is by hydrone and a series of micro-molecular gas, such as methane, ethane, propane, carbon dioxide, hydrogen
Gas etc., a kind of non-stoichiometric crystal inclusion complex formed under conditions of cryogenic high pressure.Wherein, hydrone is as main body
Molecule, polyhedron lattice network is built by hydrogen bond action；Gas molecule is entered in hydrone cage, led to as guest molecule
Cross the interaction of gas molecule and hydrone（Mainly Van der Waals force）It is stabilized and maintains the cagelike structure, thus gas water
Compound is also known as Study of Clathrate Hydrates.Meanwhile find substantial amounts of gas hydrate in deep seafloor and plateau permanent freezing layer
Hide, thus it was found from the fact that hydrate Tibetan being present from Storage mechanism and nature according to two aspects, hydrate gas stores up
The technology of depositing is practicable.
Hydrate gas storing technology has following items advantage：1st, gas hydrate has higher volume gas storage close
Degree, according to calculating 1 m3SI types hydrate can store about 180 m3Methane gas；2nd, gas hydrate may be implemented in mesolow, freezing point bar
Gas storage under part, it is not necessary to the ultra-low temperature surroundings of liquefaction gas storage method are provided and compress the hyperbaric environment of gas storage method.In additive
In the presence of, the phase balance condition of gas hydrate will move to high-temperature low-pressure area, it is meant that gas storage process is more prone to carry out；3、
Hydrate gas storing technology is safer for common storing technology, when external environment gives hydrate thermostimulation
Or after Pressure stimulation, gas hydrate due to self-shield effect can maintenance system to a certain extent stability；4th, it is hydrated
Thing method storage gas technology raw material main component is pure water, and cost is low and green.
The core of hydrate gas storing technology is Fast back-projection algorithm gas hydrate.In conventional gas lanthanum chloride hydrate mistake
Cheng Zhong, gases at high pressure contact the moment of cryogenic liquid, and gas-liquid interface will form one layer of hydrate film, and add the biography of gas diffusion
Matter resistance；In addition, easily accumulating hydration heat inside gas storage medium, system temperature rise is unfavorable for being hydrated quickly entering for gas storage process
OK.In order to solve the above problems, currently used reinforcement technique mainly includes stirring, injection and bubbling etc., but outside machine
The increase of tool equipment will improve gas storage process cost and energy consumption.Methane hydrate in static systems should be thus given priority at present to give birth to
Into reinforcement technique.
A series of additives such as surfactant, amino acid etc. are introduced in pure aquatic system can reduce gas-liquid two-phase interface
Power, while increase the solubility of methane gas in the solution.In addition, some scholars report formed in the presence of surfactants it is coarse
Non- homogeneous hydrate film, methane gas can be still diffused among liquid-phase system along intermembrane space.Thus learn in surfactant
And in the presence of the additive such as amino acid can efficient hardening static state hydrated body system mass transport process.
Foam metal is introduced into static gas storage system, liquid is filled into foam metal internal void, and hydro-combination process enters
Its internal heat accumulated can be exported into external source rapidly along heat-conducting metal skeleton during row.Foam metal surface is carried out
After hydrophobically modified, its moistened surface degree is reduced, and methane gas can be diffused into internal system along the gap in liquid-solid contact face,
So as to add the exposure level of gas-liquid two-phase, hydration gas storage efficiency is effectively improved.
The content of the invention
Present invention aims to overcome that existing gas storage technology cost height, high energy consumption, gas storage efficient the shortcomings that, it is proposed that
Hydrophobically modified foam metal is introduced in static hydrated body system as gas storage medium.
Porous foam metal can be as the heat conduction skeleton of static hydrated body system, the hydration heat that will can be lodged in system rapidly
Remove, improve hydration rate；The introducing of hydrophobic coating can make liquid can not fully infiltrate the surface of hydrophobically modified foam metal, gas
Body molecule can be diffused along the space in liquid-solid contact face, that is, increase vapor-liquid two phases contact area, when shortening hydration induction
Between, effectively improve gas storage rate and gas-storing capacity that the static state is hydrated storing gas system.
The present invention is achieved through the following technical solutions.
A kind of method that fast hydrating gas storage is realized using hydrophobically modified foam metal, liquid-phase system is injected into hydrophobic bubble
In foam metal inside hole, the gas storage medium of hydrophobically modified foam metal liquid feeding phase system is obtained, gas storage medium is placed in gas
It is 3 ~ 30 MPa in pressure, temperature is that gas generates hydrate in gas storage medium and stored up at 0 ~ 20 DEG C in atmosphere
Gas；The gas includes one or more of methane, ethane, propane, nitrogen, oxygen, carbon monoxide or carbon dioxide.
In the above method, the foam metal includes one or more of foamed aluminium, foam copper or nickel foam.
In the above method, the foam metal carries out hydrophobic treatment, its surface coating last layer hydrophobic coating.
In the above method, the hydrophobic coating includes one or more of alkyl hydrosulfide, silicon fluoride.
In the above method, the alkyl hydrosulfide includes the chain alkyl mercaptan that carbon number on alkyl chain is ten to 18；It is described
Silicon fluoride includes the long-chain silicon fluoride that fluorinated volume carbon number on 11 fluorine to 17 fluorine, the silicon fluoride main chain is eight to 12,
The oxy radical of the silicon fluoride is one to three methoxy or ethoxy.
In the above method, the liquid-phase system include pure water, surfactant solution, in Freamine Ⅲ it is a kind of with
On.
In the above method, the solvent in described surfactant solution includes the alkane that carbon number on alkyl chain is ten to 18
Base sulfate, alkylsulfonate or alkylbenzenesulfonate.
In the above method, amino acid in described Freamine Ⅲ include leucine, isoleucine or phenylalanine and
Its derivative.
In the above method, all kinds of concentration of polymer solution scopes are 0.001wt% ~ 30wt% in the liquid-phase system.
The preparation method of hydrophobically modified foam metal of the present invention, i.e., by porous bubble under 25-80 DEG C of environment temperature
Foam metal is dipped in oxidizing solution（Hydrogenperoxide steam generator or potassium persulfate solution）, one layer of oxide is formed on its surface
Layer.After be drawn off, clean and after natural air drying, then in the hydrophobic coating being dipped under 40-150 DEG C of environment temperature.1~
Taken out after 5h, then thermally treated obtain hydrophobically modified foam metal.
It is of the present invention to realize fast hydrating gas storage using hydrophobically modified foam metal, comprise the following steps：
（1）Hydrophobic foam metal and liquid are added into autoclave；
（2）It is 0.1 MPa that vacuum is evacuated to gas circuit system, after with low-pressure gas purging autoclave in 2-3 times, into kettle
Being passed through gas makes its pressure it is 0 ~ 20 DEG C to set autoclave environment temperature in the MPa of 3 MPa ~ 30.Work as autoclave
After interior temperature, pressure remained steady, gas hydrate generation terminates.
The present invention is relative to advantage possessed by prior art and beneficial effect：
The present invention can not weaken the premise of the foam metal capacity of heat transmission, by carrying out hydrophobically modified, hydrophobic painting to its surface
Layer presence can reduce infiltration degree of the liquid to foam metal surface, increase the approach of gas diffusion, you can be effectively increased gas-
Liquid two-phase contact area, shorten hydration induction time.And in hydro-combination process, the hydration heat accumulated inside static systems can pass through
Metal heat-conducting skeleton is exported into external source rapidly, greatly increases hydration rate.
The present invention is easy to be thrown to large industrialized and produce to work as to method of modifying simple possible used in foam metal
In.
Present invention process flow is simple to operation, and raw material and product are pollution-free, suitable for large scale industry gas storage process.
Embodiment
Specific elaboration in further detail is made to the present invention below by embodiment.
In following examples, the preparation method of hydrophobically modified foam metal, i.e., foamed aluminium is dipped to quality at 40 DEG C
Concentration is 30wt% hydrogenperoxide steam generator, and layer of oxide layer is formed on its surface.After be drawn off, clean and natural air drying after,
The mass concentration for being dipped to 60 DEG C again is in 0.6wt% lauryl mercaptan solution.Taken out after 1 ~ 3h, then it is thermally treated
Hydrophobically modified foam metal can be obtained.
Embodiment 1
By surface coating lauryl mercaptan hydrophobically modified foamed aluminium put down gently to volume be 300 mL autoclaves in, it is rear past
About 30 mL deionized waters are added in kettle, each connecting pipeline in reactor and gas circuit is vacuumized, until its vacuum is up to 0.1
MPa.Methane gas is then passed to, environment temperature where regulation reactor is 1 DEG C, pressure 8MPa, carries out constant volume reaction.Air inlet
Pressure has a slow reduction afterwards, and after 300 min, temperature in the kettle is flown up, and pressure substantially reduces, and methane hydrate starts largely
Generation.After undergoing 100 min again, temperature in the kettle, pressure are gradually steady, and methane hydrate generation terminates.Opened from methane hydrate
Begin largely to generate and terminate to hydration reaction, the whole process used time, volumetric reserve was about 120 V/V in 8 h or so.Compared to experiment
Under the conditions of time of static pure aquatic system synthesizing methane hydrate substantially shorten, gas-storing capacity substantially rises.
Comparative example 1
About 30 mL deionized waters are added into autoclave, each connecting pipeline in reactor and gas circuit is vacuumized, until its
Vacuum is up to 0.1 MPa.Methane gas is then passed to, environment temperature where regulation reactor is 1 DEG C, and pressure is 8 MPa, is carried out
Constant volume reacts.Pressure begins with slow reduction after air inlet, after undergoing about 2000 min, and becomes in kettle without obvious temperature, pressure
Change.Its volumetric reserve is about 15 V/V.
Embodiment 2
By surface coating lauryl mercaptan hydrophobically modified foamed aluminium put down gently to volume be 300 mL autoclaves in, it is rear past
About 30 mL0.03wt% sodium dodecyl sulfate solutions are added in kettle, each connecting pipeline in reactor and gas circuit are vacuumized, directly
To its vacuum up to 0.1 MPa.Methane gas is then passed to, environment temperature where regulation reactor is 1 DEG C, and pressure is 8 MPa,
Carry out constant volume reaction.After the min of temperature in the kettle pressure stability about 5, temperature is flown up, and pressure substantially reduces, and methane hydrate is opened
Begin largely to generate.After undergoing 20 min again, temperature in the kettle, pressure are gradually steady, and methane hydrate generation terminates.It is hydrated from methane
Thing starts a large amount of generations and terminated to hydration reaction, and the whole process used time, volumetric reserve was about 160 V/V in 30 min or so, with
Greatly shortened under same experimental conditions with the time of pure water synthesizing methane hydrate, and its gas-storing capacity is closer to sI type hydrates
Preferable gas-storing capacity.
Comparative example 2
About 30 mL 0.03wt% sodium dodecyl sulfate solutions are added into autoclave, to respectively connecting in reactor and gas circuit
Adapter line vacuumizes, until its vacuum is up to 0.1 MPa.Methane gas is then passed to, environment temperature where regulation reactor is 1
DEG C, pressure is 8 MPa, carries out constant volume reaction.After the min of temperature in the kettle pressure stability about 30, temperature is flown up, and pressure is obvious
Reduce, methane hydrate starts largely to generate.After undergoing 60 min again, temperature in the kettle, pressure are gradually steady, methane hydrate life
Into end.A large amount of generations to hydration reaction terminates since methane hydrate, and the whole process used time is in 90 min or so, volume storage
Amount about 150 V/V, reserves relative ideal.
Embodiment 3
By surface coating lauryl mercaptan hydrophobically modified foamed aluminium put down gently to volume be 300 mL autoclaves in, it is rear past
About 30 mL0.03wt% sodium dodecyl sulfate solutions are added in kettle, each connecting pipeline in reactor and gas circuit are vacuumized, directly
To its vacuum up to 0.1 MPa.Methane gas is then passed to, environment temperature where regulation reactor is 1 DEG C, and pressure is 4 MPa,
Carry out constant volume reaction.After the min of temperature in the kettle pressure stability about 10, temperature is flown up, and pressure substantially reduces, methane hydrate
Start a large amount of generations.After undergoing 40 min again, temperature in the kettle, pressure are gradually steady, and methane hydrate generation terminates.From methane water
Compound starts a large amount of generations and terminated to hydration reaction, and the whole process used time, volumetric reserve was about 157 V/V in 50 min or so,
With being greatly shortened under same experimental conditions with the time of pure water synthesizing methane hydrate, and its gas-storing capacity is hydrated closer to sI types
The preferable gas-storing capacity of thing.
Embodiment 4
By surface coating lauryl mercaptan hydrophobically modified foamed aluminium put down gently to volume be 300 mL autoclaves in, it is rear past
About 30 mL 0.03wt% sodium dodecyl sulfate solutions are added in kettle, each connecting pipeline in reactor and gas circuit are vacuumized, directly
To its vacuum up to 0.1 MPa.Methane gas is then passed to, environment temperature where regulation reactor is 3 DEG C, and pressure is 8 MPa,
Carry out constant volume reaction.After the min of temperature in the kettle pressure stability about 15, temperature is flown up, and pressure substantially reduces, methane hydrate
Start a large amount of generations.After undergoing 40 min again, temperature in the kettle, pressure are gradually steady, and methane hydrate generation terminates.From methane water
Compound starts a large amount of generations and terminated to hydration reaction, and the whole process used time, volumetric reserve was about 150 V/V in 40 min or so,
With being greatly shortened under same experimental conditions with the time of pure water synthesizing methane hydrate, reserves are comparatively preferable.
Embodiment 5
By surface coating lauryl mercaptan hydrophobically modified foamed aluminium put down gently to volume be 300 mL autoclaves in, it is rear past
About 30 mL0.8wt% leucine solutions are added in kettle, each connecting pipeline in reactor and gas circuit is vacuumized, until its vacuum
Up to 0.1 MPa.Methane gas is then passed to, environment temperature where regulation reactor is 1 DEG C, and pressure is 8 MPa, and it is anti-to carry out constant volume
Should.After the min of temperature in the kettle pressure stability about 8, temperature is flown up, and pressure substantially reduces, and methane hydrate starts a large amount of lifes
Into.After undergoing 28 min again, temperature in the kettle, pressure are gradually steady, and methane hydrate generation terminates.It is big since methane hydrate
Amount generation terminates to hydration reaction, and the whole process used time, volumetric reserve was about 155 V/V, with identical experiment in 40 min or so
Under the conditions of greatly shortened with the time of pure water synthesizing methane hydrate, and its gas-storing capacity closer to sI type hydrates ideal storage
Tolerance.
Embodiment 6
By surface coating lauryl mercaptan hydrophobically modified foamed aluminium put down gently to volume be 300 mL autoclaves in, it is rear past
About 30 mL 0.03wt% sodium dodecyl sulfate solutions are added in kettle, each connecting pipeline in reactor and gas circuit are vacuumized, directly
To its vacuum up to 0.1 MPa.Carbon dioxide is then passed to, environment temperature where regulation reactor is 5 DEG C, pressure 4
MPa, carry out constant volume reaction.After the min of temperature in the kettle pressure stability about 20, temperature is flown up, and pressure substantially reduces, methane water
Compound starts largely to generate.After undergoing 33 min again, temperature in the kettle, pressure are gradually steady, and methane hydrate generation terminates.From first
Alkane hydrate starts a large amount of generations and terminated to hydration reaction, and the whole process used time, volumetric reserve was about 150 in 60 min or so
Greatly shortened under V/V, with same experimental conditions with the time of pure water synthesizing methane hydrate, and its gas-storing capacity is closer to sI types
The preferable gas-storing capacity of hydrate.
The above embodiment of the present invention is only intended to clearly illustrate example of the present invention, and is not to the present invention
Embodiment restriction.For those of ordinary skill in the field, can also make on the basis of the above description
Other various forms of changes or variation.There is no necessity and possibility to exhaust all the enbodiments.It is all the present invention
All any modification, equivalent and improvement made within spirit and principle etc., should be included in the protection of the claims in the present invention
Within the scope of.
Claims (9)
- A kind of 1. method that fast hydrating gas storage is realized using hydrophobically modified foam metal, it is characterised in that note liquid-phase system Enter into hydrophobic foam metal inside hole, obtain the gas storage medium of hydrophobically modified foam metal liquid feeding phase system, gas storage is situated between Matter is placed in atmosphere, is 3 ~ 30 MPa in pressure, temperature is that gas generates hydration in gas storage medium at 0 ~ 20 DEG C Thing carries out gas storage；The gas include in methane, ethane, propane, nitrogen, oxygen, carbon monoxide or carbon dioxide it is a kind of with On.
- 2. the method for fast hydrating gas storage is realized using hydrophobically modified foam metal according to claim 1, it is characterised in that The foam metal includes one or more of foamed aluminium, foam copper or nickel foam.
- 3. the method for fast hydrating gas storage is realized using hydrophobically modified foam metal according to claim 1, it is characterised in that The foam metal carries out hydrophobic treatment, its surface coating last layer hydrophobic coating.
- 4. the method for fast hydrating gas storage is realized using hydrophobically modified foam metal according to claim 3, it is characterised in that The hydrophobic coating includes one or more of alkyl hydrosulfide, silicon fluoride.
- 5. the method for fast hydrating gas storage is realized using hydrophobically modified foam metal according to claim 4, it is characterised in that The alkyl hydrosulfide includes the chain alkyl mercaptan that carbon number on alkyl chain is ten to 18；The silicon fluoride includes fluorinated volume ten One fluorine to 17 fluorine, carbon number is eight to 12 long-chain silicon fluoride on the silicon fluoride main chain, the oxy radical of the silicon fluoride For one to three methoxy or ethoxy.
- 6. the method for fast hydrating gas storage is realized using hydrophobically modified foam metal according to claim 1, it is characterised in that described Liquid-phase system includes one or more of pure water, surfactant solution, Freamine Ⅲ.
- 7. the method for fast hydrating gas storage is realized using hydrophobically modified foam metal according to claim 6, it is characterised in that described Surfactant solution in solvent include alkyl chain on carbon number be ten to 18 alkyl sulfate, alkylsulfonate or alkane Base benzene sulfonate.
- 8. the method for fast hydrating gas storage is realized using hydrophobically modified foam metal according to claim 6, it is characterised in that described Freamine Ⅲ in amino acid include leucine, isoleucine or phenylalanine and its derivative.
- 9. the method for fast hydrating gas storage is realized using hydrophobically modified foam metal according to claim 6, it is characterised in that described All kinds of concentration of polymer solution scopes are 0.001wt% ~ 30wt% in liquid-phase system.
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Cited By (3)
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| CN108373137A (en) * | 2018-01-13 | 2018-08-07 | 华南理工大学 | A method of carrying out hydration hydrogen storage using propane hydrate powder |
| CN110090544A (en) * | 2019-04-03 | 2019-08-06 | 华南理工大学 | It is a kind of to strengthen hydration separation CH using porous particle4/CO2Method |
| CN114702995A (en) * | 2022-04-06 | 2022-07-05 | 中国科学院广州能源研究所 | Gas hydrate synthesis method and device |
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Application publication date: 20180109 |