CN102998152A - Device for collecting light hydrocarbon component in rock sample - Google Patents

Device for collecting light hydrocarbon component in rock sample Download PDF

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Publication number
CN102998152A
CN102998152A CN2012104654547A CN201210465454A CN102998152A CN 102998152 A CN102998152 A CN 102998152A CN 2012104654547 A CN2012104654547 A CN 2012104654547A CN 201210465454 A CN201210465454 A CN 201210465454A CN 102998152 A CN102998152 A CN 102998152A
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China
Prior art keywords
sample
light hydrocarbon
gas
pipeline
rock
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Pending
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CN2012104654547A
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Chinese (zh)
Inventor
张水昌
胡国艺
刘建宪
黄凌
张文龙
徐宜瑞
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Petrochina Co Ltd
China Petroleum and Natural Gas Co Ltd
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China Petroleum and Natural Gas Co Ltd
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Priority to CN2012104654547A priority Critical patent/CN102998152A/en
Publication of CN102998152A publication Critical patent/CN102998152A/en
Pending legal-status Critical Current

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Abstract

The invention relates to a device for collecting light hydrocarbon component in a rock sample. The collecting device comprises a sealed smashed sample tank, the smashed sample tank comprises a gas inlet and a gas outlet, rock blocks and smashed sample metal blocks are arranged in the smashed sample tank; the gas inlet is communicated to a gas carrying mechanism by a gas inlet pipeline; the gas outlet is communicated with a sealed sample bottle by a gas outlet pipeline; the sample bottle is placed in a heat insulation low temperature tank containing liquid nitrogen; and an exhaust pipeline is arranged in the sample bottle and is internally provided with a gas flowmeter, a cold trap and a vacuum pump in sequence. The collecting device is obvious in collecting effect and good in repeatability; rock samples can be smashed in low-temperature and sealed environment, and since low temperature sampling is adopted, the loss minimization of the light hydrocarbon in the sampling process is ensured; the use of a great quantity of chemical reagents which can pollute the environment is avoided in the collection process; the collecting device is wide in range of collectable light hydrocarbon and high in recovery rate of light hydrocarbon samples; and in addition, the collecting device has the characteristics of being simple in structure, convenient and quick to operate and low in cost.

Description

The gathering-device of light hydrocarbon component in the rock sample
Technical field
The invention relates to the lighter hydrocarbons collection technique of lighter hydrocarbons content and isotope value in the applied geochemistry methods analyst rock of petroleum geology exploration field, relate in particular to the gathering-device of light hydrocarbon component in a kind of rock sample with cryogenic seal crushing function.
Background technology
Lighter hydrocarbons refer to give birth to, carbon number is less than 15 hydrocarbon compound in oil-saturated reservoir rock or the petroleum gas, and carbon number is more than or equal to the corresponding heavy hydrocarbon that is called as of 15 hydrocarbon compound.Lighter hydrocarbons are the important component part of hydrocarbon component in rock gas, oil and the rock sample normally.For lighter hydrocarbons contained in rock gas and the oil, utilize the method for gas chromatography can be with they compartment analysises well.But in the at present various analysis experiments for life, the contained hydrocarbon compound of oil-saturated reservoir rock, often be subject to the restriction of experimental analysis technology, most lighter hydrocarbons in the sample pre-treatments stage all by the people for losing, be difficult to quantitative test and estimate its accurate content in rock sample, and then missed many Useful Informations.As everyone knows, in the evaluation of hydrocarbon resources amount, need accurately to know the content of the hydrocarbon component of gamut in the rock sample, just can make resource evaluation more can reflect actual conditions, and the content of lighter hydrocarbons and running parameter can be used to estimate abundance, type and the degree of ripeness of oil source rock organic matter in the rock sample, therefore, the light hydrocarbon component in Correct Analysis and the study of rocks sample is very necessary.
Be used at present measuring rock light hydrocarbon compound ripe be the pyrolysis gas chromatography (Pyro-GC) technology.This analytical technology is that the rock sample that will pulverize is placed in the special pyrolysis annex on the gas chromatograph injection port, rock sample is heated to 200-300 ℃, the lighter hydrocarbons compound component that is included in the rock sample is evaporated by heat, by cooling it is captured by chromatographic column after entering injection port with carrier gas, then carry out stratographic analysis by temperature programme.For example, Chinese patent 02113247.X adopts the disseminated organic matter in the intensification heat hydrocarbon source rock, make the hydrocarbon component desorption after being heated to uniform temperature that is adsorbed on the organic matter in the rock become organic hydrocarbon gas, with inorganic gas as: nitrogen, hydrogen, helium etc. are done carrier gas it are written in the collection tube of a low-temperature space, make its cohesion become liquid hydrocarbon and then are used for other analysis.The advantage of this technology is easy and simple to handle, and analytical cycle is shorter; Shortcoming is to cause the volatilization of part lighter hydrocarbons in broken sample process, and the diffusion conditions of lighter hydrocarbons is inconsistent in heating process, causes collected light ends fractionation incomplete, and the as a result repeatability of quantitative test is relatively poor.
Chinese patent 02160133.X employing is hermetically sealed, the low boiling point solvent cold-draw is put forward technology, carries out the sealing extracting of rock sample under the normal temperature, can prepare the various hydrocarbons that comprise light ends fractionation, thereby can carry out the analytical test of multiple analysis project.The core technology of this rock sealing hydrocarbon extraction instrument is that rock is in the following pulverizing of hermetically sealed condition limit extracting.Lower in working order, the paddle wheel High Rotation Speed produces larger centrifugal force, makes granular rock sample in the cylindrical shell with solvent strenuous exercise upwards, and firmly encircle with blade, the cylinder inboard wall of High Rotation Speed and top cover of cylinder body produces strong collision, thereby granular rock sample is pulverized.Simultaneously, in the process of High Rotation Speed, solvent will be ground in the rock sample of powder the hydrocarbons drawer out.The weak point of this instrument is the crushing effect of hard rock not good enough, such as limestone, tight sand etc.In addition, because the part in the closed barrel is more, residue is difficult for cleaning up.
Deficiency for above-mentioned technology, Chinese patent 200310103219.6 does up and down with hardness much larger than the steel ball of any rock hardness that straight reciprocating motion smashes rock sample in the O-ring barrel, the hydrocarbons of the Powdered rock sample adsorption that in this process, is crashed to pieces simultaneously also under the effect of motion solvent by solvent extraction.This technology to smash effect better, particle diameter can reach more than 90% greater than the powder rock sample more than 100 orders.And since the cylindrical vessel integral sealing, therefore also free of losses of light hydrocarbon material in the rock in sample making course.After each sample preparation finishes in addition, clean to the residue in the sealed cylindrical container also easy cleaning.But above-mentioned two kinds of devices all need be used the organic solvent freon-11 that environment is had obvious contamination in leaching process, and this reagent must pass through purifying before use, and the purified product of gained is answered the inclusion-free chromatographic peak through gas chromatographic analysis.In addition, in the situation that lighter hydrocarbons content is less, the product of above-mentioned two kinds of extraction elements also needs the liquid-concentrating instrument in Chinese patent 200510056779.X to process and obtains lighter hydrocarbons extraction concentrate.Although this liquid-concentrating instrument is airtight container and the generation negative pressure of can bleeding the solvent of evaporation is taken out, because what adopt is the water-cooled system, higher environment temperature will cause carbon number less than 6 light hydrocarbon component by scattering and disappearing in various degree, affect accuracy and the repeatability of quantitative analysis results.
Thus, the inventor relies on experience and the practice of being engaged in for many years relevant industries, proposes the gathering-device of light hydrocarbon component in a kind of rock sample, to overcome the defective of prior art.
Summary of the invention
The object of the present invention is to provide the gathering-device of light hydrocarbon component in a kind of rock sample, the collecting effect of this gathering-device obviously, good reproducibility, and have simple in structure, easy to operate, quick, the characteristics that use cost is cheap.
The object of the present invention is achieved like this, the gathering-device of light hydrocarbon component in a kind of rock sample, described gathering-device comprises the broken sample tank body of a sealing, and described broken sample tank body is provided with air intake opening and gas outlet, is provided with rock block and broken sample derby in the described broken sample tank body; Described air intake opening is communicated to carrier gas mechanism by admission line; Described gas outlet is communicated with the sample bottle of a sealing by the pipeline of giving vent to anger, described sample bottle is placed on one and fills in the adiabatic cryostat, of liquid nitrogen; Also be provided with the pipeline of bleeding in the described sample bottle, be provided with successively gas meter, cold-trap and vacuum pump in this pipeline of bleeding.
In a better embodiment of the present invention, described broken sample tank body is arranged in the constant temperature oven, and described constant temperature oven two side is respectively equipped with the perforation that can pass admission line and give vent to anger pipeline.
In a better embodiment of the present invention, the pipeline of giving vent to anger between described constant temperature oven and sample bottle has wrapped heat-insulation layer.
In a better embodiment of the present invention, described carrier gas mechanism includes the switch valve that is communicated with admission line, and this switch valve one end connects a vacuum meter, and this switch valve other end connects a carrier gas gas cylinder by a gas gauge.
In a better embodiment of the present invention, be provided with nitrogen or helium in the described carrier gas gas cylinder; Described flow rate of carrier gas is lower than 10 ml/min.
In a better embodiment of the present invention, described broken sample tank body is made of tank cylinder and cover; Described rock block and broken sample derby are arranged in the tank cylinder, and the sealing of tank cover lid is located on the tank cylinder; Described air intake opening and gas outlet are separately positioned on the cover, the top of described air intake opening and gas outlet is fixed with the dottle pin of being made by silastic material, described admission line and the pipeline of giving vent to anger pass respectively described dottle pin conducting in air intake opening and gas outlet, and the bottom of described air intake opening and gas outlet is fixed with metallic sieve.
In a better embodiment of the present invention, described metallic sieve is 100~400 purpose screen clothes.
In a better embodiment of the present invention, described broken sample derby is cylindric, and its diameter is 10cm; Thickness is 2cm.
In a better embodiment of the present invention, the bottleneck of described sample bottle is provided with plug, and the described pipeline of giving vent to anger is arranged in described plug with the pipeline of bleeding; The pipeline of giving vent to anger passes plug and extends the sample bottle bottom.
From the above mentioned, in the rock sample of the present invention the gathering-device collecting effect of light hydrocarbon component obviously, good reproducibility; Rock sample is pulverized under low temperature, airtight environment, owing to being the low temperature sampling, has guaranteed that the lost of lighter hydrocarbons minimizes in the sampling process; In collection process, need not use the chemical reagent of a large amount of contaminated environment; The collectable lighter hydrocarbons scope of this gathering-device is wider, and the recovery of lighter hydrocarbons sample is higher; In addition, also have simple in structure, easy to operate, quick, the characteristics that use cost is cheap.
Description of drawings
The following drawings only is intended to the present invention done and schematically illustrates and explain, not delimit the scope of the invention.Wherein:
Fig. 1: be the structural representation of the gathering-device of light hydrocarbon component in the rock sample of the present invention.
Embodiment
Understand for technical characterictic of the present invention, purpose and effect being had more clearly, now contrast description of drawings the specific embodiment of the present invention.
As shown in Figure 1, the present invention proposes the gathering-device 100 of light hydrocarbon component in a kind of rock sample, and described gathering-device 100 comprises the broken sample tank body 1 of a sealing, and described broken sample tank body 1 is made of tank cylinder 11 and cover 12; Be provided with rock block 2 and broken sample gold in the described tank cylinder 11 and bend piece 3, cover 12 gland bonnets are located on the tank cylinder 11; Described cover 12 is provided with air intake opening 121 and gas outlet 122; The top of described air intake opening 121 and gas outlet 122 is fixed with the dottle pin 13 of being made by silastic material, the bottom of described air intake opening 121 and gas outlet 122 is fixed with metallic sieve 14, to prevent that rock dust from entering gas outlet and blocking pipeline with gas, described metallic sieve 14 is 100~400 purpose screen clothes, above described dottle pin 13, adopt " manually fastened " set nut of gas chromatographic sample introduction mouth that dottle pin 13 is fixing, with having externally threaded hollow nut that screen cloth 14 is fixing below screen cloth 14; One admission line, 1211 one ends are communicated with carrier gas mechanism 4, its other end passes described dottle pin 13 conductings in air intake opening 121, described carrier gas mechanism 4 includes the switch valve 41 that is communicated with admission line 1211, these switch valve 41 1 ends connect a vacuum meter 42, these switch valve 41 other ends connect a carrier gas gas cylinder 44 by a gas gauge 43, by the switching effect of switch valve 41, admission line 1211 alternately is communicated with vacuum meter 42 and rain glass 43, carrier gas gas cylinder 44; In the described carrier gas gas cylinder 44 nitrogen or helium are housed; Described flow rate of carrier gas is lower than 10 ml/min; The one pipeline 1221 one ends of giving vent to anger are communicated with the sample bottle 5 of a sealing, and its other end passes described dottle pin 13 conductings in the gas outlet 122; Described sample bottle 5 is placed on one and fills in the adiabatic cryostat, 6 of liquid nitrogen 61; Also be provided with the pipeline 7 of bleeding in the described sample bottle 5, be provided with successively gas meter 71, cold-trap 72 and vacuum pump 73 in this pipeline 7 of bleeding.Described broken sample tank body 1 is arranged in the constant temperature oven 8, and described constant temperature oven 8 two sides are respectively equipped with the perforation that can pass admission line 1211 and the pipeline 1221 of giving vent to anger; The pipeline 1221 of giving vent to anger between described constant temperature oven 8 and sample bottle 5 has wrapped heat-insulation layer 1222.
From the above mentioned, in the rock sample of the present invention the gathering-device collecting effect of light hydrocarbon component obviously, good reproducibility, and have simple in structure, easy to operate, quick, the characteristics that use cost is cheap.
Further, in the present embodiment, described broken sample derby 3 is cylindric (round pie), and its diameter is 10cm; Thickness is 2cm.The bottleneck of described sample bottle 5 is provided with plug 51, and the described pipeline 1221 of giving vent to anger is arranged in described plug 51 with the pipeline 7 of bleeding; The pipeline 1221 of giving vent to anger passes plug 51 and extends the bottom of sample bottle 5.
The use procedure of the gathering-device of light hydrocarbon component is as follows in the rock sample of the present invention:
(1) screws off the cover 12 of broken sample tank body 1, with dottle pin 13 with metallic sieve 14 installs respectively and fixing (because employed dottle pin 13 is to annotate film by the high quality silicon elastomeric material to make, even under 350 ℃ to 400 ℃ high temperature, gas conduit through syringe needle is housed repeatedly punctures and also can guarantee good sealing effectiveness), pour an amount of liquid nitrogen cooling into and remove air in the tank body after clean broken sample derby 3 packed into, then add an amount of biotite gneiss sample 2, after liquid nitrogen volatilization fully, screw cover 12 and make broken sample tank body 1 sealing;
(2) whole broken sample tank body 1 is placed the crushing grinding system equipment (be existing equipment, the crushing grinding system equipment that adopts New Zealand ROCKLABS company to produce in the present embodiment, its model is: pulverized 1-5 minute BOYK MK3/RING MILL/C+PB), utilize the grinding between rock sample and the derby to make rock fragmentation become 80-100 purpose particle with effect of impact;
(3) bottleneck of gas chromatography sample bottle 5 seals with sillicon rubber blocking 51, liquid nitrogen 61 coolings in the insulated cryostat, 6 of bottle.The pipeline 1221 of giving vent to anger that is communicated with the gas outlet 122 of broken sample tank body 1 and gas phase chromatographic sample bottle 5 extends the bottom of sample bottle 5, and constant temperature oven 8 outsides to the pipeline of giving vent to anger of the bottleneck of sample bottle 5 is wrapped to form heat-insulation layer 1222 with insulation material.The bottleneck of gas chromatography sample bottle 5 is communicated with gas meter 71 by another pipeline 7 of bleeding, and the other end of flowmeter 71 is communicated with cold-trap 72 and vacuum pump 73;
(4) start vacuum pump 73, be lower than 10 ml/min with flowmeter 71 adjustments of gas flow velocitys, the air intake opening 121 that vacuumizes after 5 minutes broken sample tank body 1 is connected to switch valve 41 by admission line 1211 terminal syringe needles, switching by valve 41 can be communicated with vacuum meter 42 and rain glass 43 respectively, and the carrier gas output pressure of carrier gas gas cylinder 44 is adjusted to 0.1-0.2MPa by rain glass 43;
(5) be communicated with vacuum meter 42 and broken sample tank bodies 1 by valve 41, by the control device (not shown) temperature of constant temperature oven 8 risen to 300 ℃;
(6) with behind valve 41 connection rain glass 43, carrier gas gas cylinder 44 and the broken sample tank bodies 1 carrier gas slowly being entered in the tank body 1.Inflate after 2 minutes again vacuum meter 42 and broken sample tank body 1 are communicated with, be evacuated to vacuum tightness and be about 8 * 10-2MPa;
(7) operation in the repeating step (6) is twice; By the operation that repeatedly vacuumizes and be filled with carrier gas most of light hydrocarbon component is pumped down in the gas chromatography sample bottle 5, light hydrocarbon gas solidifies at gas chromatography sample bottle 5 internal coolings;
(8) temperature of constant temperature oven 8 is down to room temperature;
The syringe needle that (9) will stretch into the pipeline 1221 of giving vent to anger of broken sample tank body 1 gas outlet 122 is extracted, and immerses in the solvent of 0.5-1mL, and described solvent can be methylene chloride or carbon disulphide, utilizes the vacuum action of vacuum pump 73 with in the solvent suction sample bottle 5;
(10) gas chromatography sample bottle 5 is taken out from liquid nitrogen 61, cover bottle cap for subsequent use;
(11) close vacuum pump 73.
In above-mentioned collection process, the temperature constant of constant temperature oven 8 is at 300 ℃, by repeatedly vacuumizing and be filled with the operation of carrier gas, make light hydrocarbon component be pumped down to gas chromatography sample bottle 5 places, liquid nitrogen 61 in the adiabatic cryostat, 6 are used to provide low temperature environment, make the components such as lighter hydrocarbons that arrive gas chromatography sample bottle 5 be condensed out and then reach the purpose of collection.The lighter hydrocarbons sample of condensation can wash out with methylene chloride, carbon disulphide equal solvent in the pipeline of giving vent to anger of the gas outlet 122 that is communicated with broken sample tank body 1 and gas phase chromatographic sample bottle 5, is used for chromatogram or chromatography-mass spectroscopy quantitative test and lighter hydrocarbons isotope analysis.
The gathering-device of light hydrocarbon component compared with prior art has following advantage in the rock sample of the present invention:
(1) the each accessible rock sample amount of this gathering-device is larger, owing to being the low temperature sampling, has guaranteed that the lost of lighter hydrocarbons minimizes in the sampling process.
(2) rock sample is pulverized under low temperature, airtight environment.
(3) processing and fabricating of this gathering-device is simple, need not use the chemical reagent of a large amount of contaminated environment in the collection process.
(4) the collectable lighter hydrocarbons scope of this gathering-device is wider, and the recovery of lighter hydrocarbons sample is higher.
(5) the lighter hydrocarbons sample of this gathering-device collection can be used for multiple light hydrocarbon analysis project, for example chromatogram or chromatography-mass spectroscopy quantitative test and lighter hydrocarbons isotope analysis.
The above only is the schematic embodiment of the present invention, is not to limit scope of the present invention.Any those skilled in the art, the equivalent variations of having done under the prerequisite that does not break away from design of the present invention and principle and modification all should belong to the scope of protection of the invention.

Claims (9)

1. the gathering-device of light hydrocarbon component in the rock sample, it is characterized in that: described gathering-device comprises the broken sample tank body of a sealing, and described broken sample tank body is provided with air intake opening and gas outlet, is provided with rock block and broken sample derby in the described broken sample tank body; Described air intake opening is communicated to carrier gas mechanism by admission line; Described gas outlet is communicated with the sample bottle of a sealing by the pipeline of giving vent to anger, described sample bottle is placed on one and fills in the adiabatic cryostat, of liquid nitrogen; Also be provided with the pipeline of bleeding in the described sample bottle, be provided with successively gas meter, cold-trap and vacuum pump in this pipeline of bleeding.
2. the gathering-device of light hydrocarbon component in the rock sample as claimed in claim 1, it is characterized in that: described broken sample tank body is arranged in the constant temperature oven, and described constant temperature oven two side is respectively equipped with the perforation that can pass admission line and give vent to anger pipeline.
3. the gathering-device of light hydrocarbon component in the rock sample as claimed in claim 2, it is characterized in that: the pipeline of giving vent to anger between described constant temperature oven and sample bottle has wrapped heat-insulation layer.
4. the gathering-device of light hydrocarbon component in the rock sample as claimed in claim 1, it is characterized in that: described carrier gas mechanism includes the switch valve that is communicated with admission line, this switch valve one end connects a vacuum meter, and this switch valve other end connects a carrier gas gas cylinder by a gas gauge.
5. the gathering-device of light hydrocarbon component in the rock sample as claimed in claim 4 is characterized in that: be provided with nitrogen or helium in the described carrier gas gas cylinder; Described flow rate of carrier gas is lower than 10 ml/min.
6. the gathering-device of light hydrocarbon component in the rock sample as claimed in claim 1, it is characterized in that: described broken sample tank body is made of tank cylinder and cover; Described rock block and broken sample derby are arranged in the tank cylinder, and the sealing of tank cover lid is located on the tank cylinder; Described air intake opening and gas outlet are separately positioned on the cover, the top of described air intake opening and gas outlet is fixed with the dottle pin of being made by silastic material, described admission line and the pipeline of giving vent to anger pass respectively described dottle pin conducting in air intake opening and gas outlet, and the bottom of described air intake opening and gas outlet is fixed with metallic sieve.
7. the gathering-device of light hydrocarbon component in the rock sample as claimed in claim 1, it is characterized in that: described metallic sieve is 100~400 purpose screen clothes.
8. the gathering-device of light hydrocarbon component in the rock sample as claimed in claim 1, it is characterized in that: described broken sample derby is cylindric, and its diameter is 10cm; Thickness is 2cm.
9. the gathering-device of light hydrocarbon component in the rock sample as claimed in claim 1, it is characterized in that: the bottleneck of described sample bottle is provided with plug, and described pipeline and the pipeline of bleeding of giving vent to anger is arranged in described plug; The pipeline of giving vent to anger passes plug and extends the sample bottle bottom.
CN2012104654547A 2012-11-16 2012-11-16 Device for collecting light hydrocarbon component in rock sample Pending CN102998152A (en)

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CN104535361A (en) * 2014-12-15 2015-04-22 中国石油天然气股份有限公司 Hydrocarbon inclusion component low-temperature sampling system and sampling method
CN106153374A (en) * 2015-04-21 2016-11-23 中国石油化工股份有限公司 A kind of sealing crushes degasser
CN106596218A (en) * 2016-11-23 2017-04-26 中国石油天然气股份有限公司 Preparation method of light hydrocarbons in rocks
CN112393940A (en) * 2019-08-16 2021-02-23 中国石油天然气股份有限公司 Fast and efficient collecting device and method for light hydrocarbon components of gold tube thermal simulation product
CN112857931A (en) * 2021-01-08 2021-05-28 闫春会 Food safety inspection is with system appearance device
CN112892808A (en) * 2021-01-14 2021-06-04 杨锦宏 Extraction element is smashed to plant negative pressure
CN114113440A (en) * 2021-11-19 2022-03-01 中国石油大学(北京) System and method for capturing and analyzing volatile hydrocarbon in natural gas hydrate reservoir

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Cited By (9)

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Publication number Priority date Publication date Assignee Title
CN104535361A (en) * 2014-12-15 2015-04-22 中国石油天然气股份有限公司 Hydrocarbon inclusion component low-temperature sampling system and sampling method
CN104535361B (en) * 2014-12-15 2017-03-08 中国石油天然气股份有限公司 A kind of hydrocarbon inclusion component low temperature sampler and sampling method
CN106153374A (en) * 2015-04-21 2016-11-23 中国石油化工股份有限公司 A kind of sealing crushes degasser
CN106153374B (en) * 2015-04-21 2018-11-23 中国石油化工股份有限公司 It is a kind of to seal broken degasser
CN106596218A (en) * 2016-11-23 2017-04-26 中国石油天然气股份有限公司 Preparation method of light hydrocarbons in rocks
CN112393940A (en) * 2019-08-16 2021-02-23 中国石油天然气股份有限公司 Fast and efficient collecting device and method for light hydrocarbon components of gold tube thermal simulation product
CN112857931A (en) * 2021-01-08 2021-05-28 闫春会 Food safety inspection is with system appearance device
CN112892808A (en) * 2021-01-14 2021-06-04 杨锦宏 Extraction element is smashed to plant negative pressure
CN114113440A (en) * 2021-11-19 2022-03-01 中国石油大学(北京) System and method for capturing and analyzing volatile hydrocarbon in natural gas hydrate reservoir

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Application publication date: 20130327