CN102295967A - Apparatus for continuously separating carbon dioxide from natural gas through hydrate method, and method thereof - Google Patents
Apparatus for continuously separating carbon dioxide from natural gas through hydrate method, and method thereof Download PDFInfo
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- CN102295967A CN102295967A CN201110176249A CN201110176249A CN102295967A CN 102295967 A CN102295967 A CN 102295967A CN 201110176249 A CN201110176249 A CN 201110176249A CN 201110176249 A CN201110176249 A CN 201110176249A CN 102295967 A CN102295967 A CN 102295967A
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Abstract
The invention discloses an apparatus for continuously separating carbon dioxide from natural gas through a hydrate method, and a method thereof. The apparatus comprises a gas inlet pipe (9), a low temperature water bath (1), a low temperature water tank (2), a gas compressor (3), a liquid pressurizing water pump (4), a gas-liquid mixer (5), a tube type separator (6), a liquid conveying pump (16) and a hydrate decomposition tower (8). The method is characterized in that: water introduced from a water supplement pipe and an addition agent introduced from a reagent adding pipe enter the low temperature water tank, then are subjected to cooling to the hydrate separation temperature; the cooled water and the cooled addition agent are subjected to pressurization; the pressurized water, the pressurized addition agent and the pressurized natural gas enter the gas-liquid mixer to carry out mixing to continuously form a hydrate; the separated hydrate slurry enters the hydrate decomposition tower; the hydrate is subjected to decomposition to recover the solution and the CO2. According to the present invention, a purpose of continuous and rapid removal of the CO2 from the natural gas through the hydrate method is realized; the yield of the CH4 is 100 m<3> per hour.
Description
Technical field
The present invention relates to CO in a kind of hydrate high-efficiency and continuous separating natural gas
2Method and apparatus.
Background technology
Gas hydrate is water and methane, ethane, CO
2And H
2The nonstoichiometry cage shape crystalline substance that micro-molecular gas such as S form under certain temperature and pressure condition claims the cage modle hydrate again.When biogas formed hydrate, middle mutually gas composition of hydrate and gas phase were formed inconsistent, CO
2At the enrichment of hydrate phase, CH
4Enrichment in gas phase realizes CH
4And CO
2Separation.CO in the hydrate partition method separating natural gas
2Can realize the effect such as simplification, technical security environmental protectionization, production stabilization, cheapization of expense of Sweet natural gas decarbonization process, have industrial prospect preferably aspect the Sweet natural gas decarburization.For realizing that the hydrate partition method removes CO in the Sweet natural gas
2Industrialization need be designed the continuous safely and efficiently hydrate of a cover and remove CO in the Sweet natural gas
2Technology.Therefore, research and development hydrate CO in the separating natural gas rapidly and efficiently
2Technology and technology are significant.
At present, hydrate separates the CO in biogas and the Sweet natural gas
2Also there is not the industrial application case.What the research of hydrate divided gas flow was more is the separation of flue gas, N
2And CO
2Form hydrate pressure down at 5 ℃ and differ 25MPa, CH
4And CO
2Form hydrate pressure down at 5 ℃ and differ 2MPa.Because CH
4And CO
2The pressure of generation hydrate differ very little, CO
2Generate under the hydrate condition CH
4Also be easy to generate hydrate, make hydrate separate biogas CO in the Sweet natural gas
2Selectivity to be lower than in the flue gas CO
2Selectivity, remove CO in the Sweet natural gas with hydrate
2, CH
4The ratio that generates hydrate is higher, and separating difficulty is big.Gas hydrate forms will pass through gas dissolving, nucleus generates and crystal growth phase, hydrate can only form at liquid-gas interface, and the membranaceous hydrate that begins to form stops gas further to contact with the aqueous solution, the hydrate generative process becomes gas transmission rate control by speed of reaction control, make the natural formation speed of hydrate very slow, CO in the hydrate separating natural gas
2Inefficiency, can not satisfy industrial needs far away.When in recent years, improve the selectivity that hydrate separates biogas how, improve the hydration rate aspect, domestic and international many scientific research personnel have carried out big quantity research and have obtained very big progress.The direction of studying mainly comprises: on kinetics, adopt the time method that widens CO2 and CH4 formation hydrate, on thermodynamics, interpolation can widen the additive of CH4 and CO2 formation hydrate pressure, improves mass transfer/heat transfer condition, strengthens mixing etc.
The research of CO2 just began in recent years in the hydrate separating natural gas, and document and patent report all concentrate on conceptual phase.For example 2009, Nena Dabrowski etc. designed CO in the multistage equilibrium crystallization flowsheeting hydrate separating natural gas
2, draw hydrate can separating natural gas in CO
2, the problem that needs to solve is the high problem of methane rate of loss.The Shell Oil Co. are CO in hydrate separating natural gas
2Study morely, 2009, Mark van Denderen etc. studied THF, and there are down CO in the hydrate separating natural gas in CTAB, NaCL
2Effect, drawing hydrate can separation of C H
4/ CO
2Gas mixture, but speed of reaction is slow, and the methane loss is more.2009, Michael Golombok etc. were by CO in the dynamics research Sweet natural gas
2Remove, find CO
2The induction time that forms hydrate is more responsive to stir speed (S.S.), along with the increase of stir speed (S.S.), and induction time CO
2Reduce and compare CH
4Hurry up, mixing speed below 500RPM, CO
2The induction time that generates hydrate is greater than CH
4Generate the induction time of hydrate, during stir speed (S.S.) 1000RPM, CO
2Induction time far below CH
4, like this after CO2 generates hydrate, CH
4Or gas, thereby can realize CH
4With CO
2Separation.
The CO2 method only rests on experimental stage at present in the above-mentioned hydrate separating natural gas, does not also realize industrialization.Abroad, particularly Japan, Norway pay much attention to the hydrate isolation technique, and the Shell Oil Co. remove CO in the Sweet natural gas at hydrate
2Study more.But, also use with a certain distance from commercial applications, also have many technical problems to need to solve.Therefore developing the hydrate high-efficiency and continuous removes CO in the Sweet natural gas
2Device highly significant.
Summary of the invention
The object of the present invention is to provide a kind of new Sweet natural gas decarbonization method, a kind of can be efficiently, CO in the separating natural gas continuously
2Method and apparatus, the present invention also is used for other gas delivery of Sweet natural gas such as H
2S separates.
For achieving the above object, the present invention has adopted following technical scheme:
CO in the continuous separating natural gas of a kind of hydrate
2Device, comprise inlet pipe 9, low temperature water-bath 1, low temperature water pot 2, gas compressor 3, liquid booster water pump 4, gas liquid mixer 5, pipe separator 6, liquid delivery pump 16 and decomposition of hydrate tower 8; Described low temperature water pot 2 is provided with and adds reagent mouth, water outlet, water supplement port and liquid-inlet, and water outlet is connected with the liquid-inlet of liquid booster pump 4 with gas liquid mixer 5 successively; Add the reagent mouth and add reagent pipe 18 and link to each other, water supplement port links to each other with filling pipe 17; Be provided with gas pipeline in the described low temperature water pot 2, one end of gas pipeline connects inlet pipe 9, the other end is connected with the gas feed of gas compressor 3 with gas liquid mixer 5 successively, also be provided with cooling water pipeline in the described low temperature water pot 2, the two ends of cooling water pipeline link to each other with first water-in with first water outlet of low temperature water-bath 1 respectively; Described pipe separator 6 comprises tube side and shell side, the entrance of cooling water of shell side links to each other with second water outlet of low temperature water-bath 1, the cooling water outlet of shell side links to each other by pipeline with second water-in of low temperature water-bath 1, pipe connection is passed through in the tube side import of pipe separator 6 and the outlet of gas liquid mixer 5, pipe separator 6 tube sides be provided with pneumatic outlet and liquid exit, the liquid exit of tube side links to each other with the import of decomposition of hydrate tower 8, the top of decomposition of hydrate tower is provided with gas discharge outlet, the bottom is provided with liquid exit, liquid exit is connected to the liquid-inlet of low temperature water pot 2, interlocking in the described decomposition of hydrate tower 8 is provided with column plate, and a well heater 19 is arranged at the bottom.
Described tube side reaches the part that connects with it for straight tube in parallel 10; Shell side is that the outer passage of straight tube reaches the part that connects with it, and shell side is provided with traverse baffle.
Described straight tube is provided with fin 20 outward; Be provided with the fluid scale 12 that circles round in the straight tube.
Circle round height and the caliber ratio of scale 12 of described fluid is that 0.6 ~ 0.7, two fluids circle round between scale distance and caliber than 1.5 ~ 2.0.
Described decomposition of hydrate tower 8 can be plate distillation column.
The pneumatic outlet of described tube side is connected with two pipelines, and one is connected with inlet pipe by pressure valve, constitutes the branch road of inlet pipe, and another connects pressure valve, directly discharges gas.
CO in the continuous separating natural gas of described device
2Method, may further comprise the steps:
(1) water that adds by filling pipe and enter the low temperature water pot together and form mixed solution by adding hydrate accelerant that the reagent pipe adds, water coolant in the low temperature water-bath enters the low temperature water pot mixed solution is cooled to 5 ~ 15 ℃, and mixed solution enters the liquid booster water pump and is pressurized to 2 ~ 7MPa; The CO that contains by the inlet pipe feeding
2Natural gas via low temperature water pot cooling after enter gas compressor, be pressurized to 2 ~ 7MPa; Mixed solution after supercharging and Sweet natural gas enter gas liquid mixer together to be mixed;
(2) mixed gas-liquid mixture enters hydration reaction takes place in the pipe separator, generates hydrate slurry, and an isolated gas part is as product gas CH simultaneously
4Output, another part gas backstreaming is to inlet pipe;
(3) hydrate slurry enters the decomposition of hydrate tower, and hydrate slurry is 20 ~ 40 ℃ of decomposition, the gas CO of generation
2Output, liquid is back to the low temperature water pot through liquid delivery pump, the CO in the promptly continuous separating natural gas
2
The temperature of described low temperature water-bath 1 is 1 ~ 7 ℃.
Described hydrate slurry runs down into the orlop column plate step by step from the superiors' column plate of decomposition of hydrate tower.
There is straight tube in parallel the inside of described pipe separator; The pipe shell journey is provided with traverse baffle, and pipeline has fin outward and is used to strengthen heat exchange.The fluid scale that circles round is installed in the pipeline, and the height of the scale that circles round and caliber are than between 0.6-0.7, and distance and caliber are than between 1.5-2.0 between two scales.Walk gas-liquid mixture in the tubulation, walk heat-eliminating medium outside the pipe.The pipeline parallel connection not only strengthens unit volume gas-liquid mixture heat exchange effect, and avoids the long problem that causes generating the hydrate blocking pipe of pipeline, effectively improves the hydrate separation efficiency; The convection current angle that traverse baffle can improve heat-eliminating medium and straight tube is set, improves heat transfer coefficient.Traverse baffle can also play the effect of supporting tube bank, holding tube distance in addition.Fin has increased the heat interchanging area of tube wall and heat-eliminating medium, the enhance heat transfer effect; The fluid scale that circles round both can increase gas-liquid mixture mobile turbulent extent, increased the gas-liquid mixed effect, strengthened heat transmission and mass transfer, can avoid hydrate to bond at the tube wall face again.
A gas part of coming out from pipe separator is as products C H
4Output, a part enters gas circulation loop, by regulating the ratio of output gas and recycle gas, makes CH in the output gas
4Concentration reach requirement.
The hydrate slurry that comes out from pipe separator enters the decomposition of hydrate tower, decomposition of hydrate tower bottom having heaters.Hydrate slurry enters the decomposition tower internal pressure to be reduced, and conducts heat on column plate simultaneously, and hydrate decomposes under low-voltage high-temperature, the gas CO after the decomposition
2Through the output of cat head pipeline, the liquid after the decomposition enters liquid circulation loop.
The present invention is with respect to advantage and beneficial effect that prior art had:
1, realizes that hydrate removes CO in the Sweet natural gas
2
2, the present invention is provided with the fluid scale that circles round, and it is mobile that gas-liquid mixture is circled round, and increased the solution-air contact area;
3, accelerate the heat and mass transport of reaction process;
4, realize that hydrate removes CO in the Sweet natural gas continuously fast
2
Description of drawings
Fig. 1 is a invention process case device synoptic diagram;
Fig. 2 is the single tube synoptic diagram of pipe separator of the present invention;
Fig. 3 is the fluid installed in the tubulation in the pipe separator fin synoptic diagram that circles round.
The water-bath of 1-low temperature; 2-low temperature water pot; The 3-gas compressor; 4-liquid booster water pump; The 5-gas liquid mixer; The 6-pipe separator; The 7-liquid delivery pump; 8-decomposition of hydrate tower; The 9-inlet pipe; The 10-straight tube; The 11-traverse baffle; The 12-fluid scale 13-gaseous tension variable valve that circles round; 14-gaseous tension variable valve; 15-gaseous tension variable valve; The 16-liquid delivery pump; The 17-filling pipe; 18-adds the reagent pipe; The 19-well heater; The 20-fin.
Embodiment
Below in conjunction with accompanying drawing and case study on implementation content of the present invention is described in further details:
As shown in Figure 1, CO in the continuous separating natural gas of a kind of hydrate
2Device, comprise inlet pipe 9, low temperature water-bath 1, low temperature water pot 2, gas compressor 3, liquid booster water pump 4, gas liquid mixer 5, pipe separator 6, liquid delivery pump (7,16) and decomposition of hydrate tower 8; Described low temperature water pot 2 is provided with and adds reagent mouth, water outlet, water supplement port and liquid-inlet, and water outlet is connected with the liquid-inlet of liquid booster pump 4 with gas liquid mixer 5 successively; Add the reagent mouth and add reagent pipe 18 and link to each other, water supplement port links to each other with filling pipe 17; Be provided with gas pipeline in the described low temperature water pot 2, one end of gas pipeline connects inlet pipe 9, the other end is connected with the gas feed of gas compressor 3 with gas liquid mixer 5 successively, also be provided with cooling water pipeline in the described low temperature water pot 2, the two ends of cooling water pipeline link to each other with first water-in with first water outlet of low temperature water-bath 1 respectively; Described pipe separator 6 comprises tube side and shell side, the entrance of cooling water of shell side links to each other with second water outlet of low temperature water-bath 1, the cooling water outlet of shell side links to each other by pipeline with second water-in of low temperature water-bath 1, pipe connection is passed through in the tube side import of pipe separator 6 and the outlet of gas liquid mixer 5, pipe separator 6 tube sides be provided with pneumatic outlet and liquid exit, the liquid exit of tube side links to each other with the import of decomposition of hydrate tower 8, the top of decomposition of hydrate tower is provided with gas discharge outlet, the bottom is provided with liquid exit, liquid exit is connected to the liquid-inlet of low temperature water pot 2, described decomposition of hydrate tower 8 is a plate distillation column, interlocking is provided with column plate, and a well heater 19 is arranged at the bottom.
Described tube side reaches the part that connects with it for straight tube in parallel 10; Shell side is that the outer passage of straight tube reaches the part that connects with it, and shell side is provided with traverse baffle.Shown in Figure 2, described straight tube is provided with fin 20 outward; Be provided with the fluid scale 12 that circles round in the straight tube.
Among Fig. 3, circle round height and the caliber ratio of scale 12 of described fluid is that 0.6 ~ 0.7, two fluids circle round between scale distance and caliber than 1.5 ~ 2.0.
The pneumatic outlet of described tube side is connected with two pipelines, and one is connected with inlet pipe by pressure valve, constitutes the branch road of inlet pipe, and another connects pressure valve, directly discharges gas.
CO in the continuous separating natural gas of described device
2Method, may further comprise the steps:
(1) water that adds by filling pipe and enter the low temperature water pot together and form mixed solution by adding hydrate accelerant that the reagent pipe adds, water coolant in the low temperature water-bath enters the low temperature water pot mixed solution is cooled to 5 ~ 15 ℃, and mixed solution enters the liquid booster water pump and is pressurized to 2 ~ 7MPa; The CO that contains by the inlet pipe feeding
2Natural gas via low temperature water pot cooling after enter gas compressor, be pressurized to 2 ~ 7MPa; Mixed solution after supercharging and Sweet natural gas enter gas liquid mixer together to be mixed;
(2) mixed gas-liquid mixture enters hydration reaction takes place in the pipe separator, generates hydrate slurry, and an isolated gas part is as product gas CH simultaneously
4Output, another part gas backstreaming is to inlet pipe;
(3) hydrate slurry enters the decomposition of hydrate tower, and hydrate slurry is 20 ~ 40 ℃ of decomposition, the gas CO of generation
2Output, liquid is back to the low temperature water pot through liquid delivery pump, the CO in the promptly continuous separating natural gas
2
The temperature of described low temperature water-bath 1 is 1 ~ 7 ℃.
Described hydrate slurry runs down into the orlop column plate step by step from the superiors' column plate of decomposition of hydrate tower.
Embodiment 2
The implementation case device enters the low temperature water pot together by the water of filling pipe 17 and the hydrate accelerant of doping pipe 18 in use, is cooled to 7 ℃ through low temperature water-bath 1, and liquid booster pump 4 makes hydraulic pressure bring up to 3MPa.The CO that contains by inlet pipe 9
2Natural gas via low temperature water pot, entered gas compressor 3 after the cryogenic liquid in it cooling to make gaseous tension bring up to 3MPa.Enter gas liquid mixer 5 together through liquid that has promotor after the water pump supercharging and the Sweet natural gas after the gas compressor supercharging.Gas and liquid thorough mixing form the water that has a large amount of micro-bubbles thus in gas liquid mixer 5 exits.Then, above-mentioned gas-liquid mixture enters pipe separator, in pipe, carry out turbulent flow circle round mobile, gas and liquid thorough mixing mass transfer and heat transfer in this process, CO
2Separate from gas mixture with the liquid hydration; Gas part after the separation through gaseous tension variable valve 13 as products C H
4Output, a part of gas loops back inlet pipe 9 through gaseous tension variable valve 14, forms gas return path.
Described cooling heat exchange system is provided by the circulating cooling medium of low temperature water-bath 1, and temperature is 5 ℃, and to pipe separator 6 and low temperature water pot 2, temperature raises after heat exchange with pipe connection, loops back low temperature water-bath 1 then and carries out next one circulation.
Described decomposition of hydrate tower 8 bottoms are provided with well heater 19, and well heater provides heat to make decomposition of hydrate in tower.Hydrate slurry in the pipe separator 6 enters the decomposition of hydrate tower through liquid delivery pump 7, and hydrate from the first block of column plate in the top, flows to bottom column plate step by step in tower, and hydrate decomposes step by step.Gas after the decomposition is through 13 outputs of top of tower pipeline, and the liquid after the decomposition loops back the low temperature water pot through fluid discharge pump 16 and carries out next one circulation.The implementation case has following advantage: 1 realizes that hydrate removes CO in the Sweet natural gas
2; 2 have increased the solution-air contact area; 3 accelerate the heat transfer of reaction process; 4 realize that hydrate removes CO in the Sweet natural gas continuously fast
2, CH
4Output 100m3/h.
Claims (9)
1. the device of carbonic acid gas in the continuous separating natural gas of hydrate, it is characterized in that, comprise inlet pipe (9), low temperature water-bath (1), low temperature water pot (2), gas compressor (3), liquid booster water pump (4), gas liquid mixer (5), pipe separator (6), liquid delivery pump (16) and decomposition of hydrate tower (8); Described low temperature water pot (2) is provided with and adds reagent mouth, water outlet, water supplement port and liquid-inlet, and water outlet is connected with the liquid-inlet of liquid booster pump (4) with gas liquid mixer (5) successively; Add the reagent mouth and add reagent pipe (18) and link to each other, water supplement port links to each other with filling pipe (17); Be provided with gas pipeline in the described low temperature water pot (2), one end of gas pipeline connects inlet pipe (9), the other end is connected with the gas feed of gas compressor (3) with gas liquid mixer (5) successively, also be provided with cooling water pipeline in the described low temperature water pot (2), the two ends of cooling water pipeline link to each other with first water-in with first water outlet of low temperature water-bath (1) respectively; Described pipe separator (6) comprises tube side and shell side, the entrance of cooling water of shell side links to each other with second water outlet of low temperature water-bath (1), the cooling water outlet of shell side links to each other by pipeline with second water-in of low temperature water-bath (1), pipe connection is passed through in the outlet of the tube side import of pipe separator (6) and gas liquid mixer (5), pipe separator (6) tube side be provided with pneumatic outlet and liquid exit, the liquid exit of tube side links to each other with the import of decomposition of hydrate tower (8), the top of decomposition of hydrate tower is provided with gas discharge outlet, the bottom is provided with liquid exit, liquid exit is connected to the liquid-inlet of low temperature water pot (2), interlocking in the described decomposition of hydrate tower (8) is provided with column plate, and a well heater (19) is arranged at the bottom.
2. device according to claim 1 is characterized in that, described tube side is straight tube (10) in parallel and the part that connects with it; Shell side is that the outer passage of straight tube reaches the part that connects with it, and shell side is provided with traverse baffle.
3. device according to claim 2 is characterized in that, described straight tube is provided with fin (20) outward; Be provided with the fluid scale (12) that circles round in the straight tube.
4. device according to claim 3 is characterized in that, circle round height and the caliber ratio of scale (12) of described fluid is that 0.6 ~ 0.7, two fluids circle round between scale distance and caliber than 1.5 ~ 2.0.
5. device according to claim 4 is characterized in that, described decomposition of hydrate tower (8) is a plate distillation column.
6. device according to claim 5 is characterized in that, the pneumatic outlet of described tube side is connected with two pipelines, and one is connected with inlet pipe by pressure valve, constitutes the branch road of inlet pipe, and another connects pressure valve, directly discharges gas.
7. application rights requires CO in one of 1 ~ 6 continuous separating natural gas of described device
2Method, it is characterized in that, may further comprise the steps:
(1) water that adds by filling pipe and enter the low temperature water pot together and form mixed solution by adding hydrate accelerant that the reagent pipe adds, water coolant in the low temperature water-bath enters the low temperature water pot mixed solution is cooled to 5 ~ 15 ℃, and mixed solution enters the liquid booster water pump and is pressurized to 2 ~ 7MPa; The CO that contains by the inlet pipe feeding
2Natural gas via low temperature water pot cooling after enter gas compressor, be pressurized to 2 ~ 7MPa; Mixed solution after supercharging and Sweet natural gas enter gas liquid mixer together to be mixed;
(2) mixed gas-liquid mixture enters hydration reaction takes place in the pipe separator, generates hydrate slurry, and an isolated gas part is as product gas CH simultaneously
4Output, another part gas backstreaming is to inlet pipe;
(3) hydrate slurry enters the decomposition of hydrate tower, and hydrate slurry is 20 ~ 40 ℃ of decomposition, the gas CO of generation
2Output, liquid is back to the low temperature water pot through liquid delivery pump, the CO in the promptly continuous separating natural gas
2
8. method according to claim 7 is characterized in that, the temperature of described low temperature water-bath (1) is 1 ~ 7 ℃.
9. method according to claim 8 is characterized in that, described hydrate slurry runs down into the orlop column plate step by step from the superiors' column plate of decomposition of hydrate tower.
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| CN105087093A (en) * | 2014-05-08 | 2015-11-25 | 罗显平 | Method and device for continuous separation of methane, carbon dioxide and hydrogen sulfide from biogas by hydrate method |
| CN106016817A (en) * | 2016-06-08 | 2016-10-12 | 上海理工大学 | Carbon dioxide recovery device based on open type absorption refrigeration cycle |
| CN107325852A (en) * | 2017-05-31 | 2017-11-07 | 常州大学 | A kind of method and its device based on hydrate processing cultivation excreta |
| CN108003952A (en) * | 2017-11-30 | 2018-05-08 | 湘南学院 | A kind of application for the method and phytic acid for preparing hydrate |
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| RU2807822C1 (en) * | 2023-05-03 | 2023-11-21 | Федеральное государственное бюджетное образовательное учреждение высшего образования "Российский химико-технологический университет имени Д.И. Менделеева" (РХТУ им. Д.И. Менделеева) | Method for trapping carbon dioxide from flue gases |
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| CN105087093B (en) * | 2014-05-08 | 2018-08-10 | 罗显平 | Hydrate continuous separation of methane, carbon dioxide, the method for hydrogen sulfide and its device from biogas |
| CN105087093A (en) * | 2014-05-08 | 2015-11-25 | 罗显平 | Method and device for continuous separation of methane, carbon dioxide and hydrogen sulfide from biogas by hydrate method |
| CN106016817B (en) * | 2016-06-08 | 2019-04-30 | 上海理工大学 | A kind of carbon dioxide recovering apparatus based on open absorption refrigeration circulation |
| CN106016817A (en) * | 2016-06-08 | 2016-10-12 | 上海理工大学 | Carbon dioxide recovery device based on open type absorption refrigeration cycle |
| CN107325852A (en) * | 2017-05-31 | 2017-11-07 | 常州大学 | A kind of method and its device based on hydrate processing cultivation excreta |
| CN108003952A (en) * | 2017-11-30 | 2018-05-08 | 湘南学院 | A kind of application for the method and phytic acid for preparing hydrate |
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