WO2015085829A1 - 一种快速形成气体水合物的喷雾装置 - Google Patents
一种快速形成气体水合物的喷雾装置 Download PDFInfo
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- WO2015085829A1 WO2015085829A1 PCT/CN2014/089123 CN2014089123W WO2015085829A1 WO 2015085829 A1 WO2015085829 A1 WO 2015085829A1 CN 2014089123 W CN2014089123 W CN 2014089123W WO 2015085829 A1 WO2015085829 A1 WO 2015085829A1
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- gas
- liquid mixing
- hydrate
- sprayer
- liquid
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- 239000007921 spray Substances 0.000 title claims abstract description 40
- 230000015572 biosynthetic process Effects 0.000 title claims abstract description 37
- 150000004677 hydrates Chemical class 0.000 title abstract description 7
- 239000007788 liquid Substances 0.000 claims abstract description 90
- 238000002156 mixing Methods 0.000 claims abstract description 65
- 239000012047 saturated solution Substances 0.000 claims abstract description 24
- 239000012530 fluid Substances 0.000 claims abstract description 20
- 238000002360 preparation method Methods 0.000 claims abstract description 17
- NMJORVOYSJLJGU-UHFFFAOYSA-N methane clathrate Chemical compound C.C.C.C.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O NMJORVOYSJLJGU-UHFFFAOYSA-N 0.000 claims description 41
- 239000000243 solution Substances 0.000 claims description 33
- 238000012360 testing method Methods 0.000 claims description 15
- 238000012545 processing Methods 0.000 claims description 13
- 238000000926 separation method Methods 0.000 claims description 10
- 239000006199 nebulizer Substances 0.000 claims description 9
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- 238000002474 experimental method Methods 0.000 claims description 3
- 239000007789 gas Substances 0.000 description 89
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 26
- 238000000034 method Methods 0.000 description 21
- 230000006698 induction Effects 0.000 description 15
- 239000000203 mixture Substances 0.000 description 7
- 238000003756 stirring Methods 0.000 description 7
- 238000003786 synthesis reaction Methods 0.000 description 5
- 238000005516 engineering process Methods 0.000 description 4
- 238000010907 mechanical stirring Methods 0.000 description 4
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- 238000013019 agitation Methods 0.000 description 3
- 239000007864 aqueous solution Substances 0.000 description 3
- 230000005587 bubbling Effects 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000005265 energy consumption Methods 0.000 description 3
- 238000004904 shortening Methods 0.000 description 3
- 238000005507 spraying Methods 0.000 description 3
- JRMUNVKIHCOMHV-UHFFFAOYSA-M tetrabutylammonium bromide Chemical compound [Br-].CCCC[N+](CCCC)(CCCC)CCCC JRMUNVKIHCOMHV-UHFFFAOYSA-M 0.000 description 3
- 238000000889 atomisation Methods 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
- 238000004090 dissolution Methods 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 238000005411 Van der Waals force Methods 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
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- 230000002349 favourable effect Effects 0.000 description 1
- 230000036571 hydration Effects 0.000 description 1
- 238000006703 hydration reaction Methods 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 238000003760 magnetic stirring Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
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- B01D53/002—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by condensation
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- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
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- C10L2290/00—Fuel preparation or upgrading, processes or apparatus therefore, comprising specific process steps or apparatus units
- C10L2290/18—Spraying or sprinkling
Definitions
- the present invention relates to a spray device for rapidly forming a gas hydrate.
- Gas Hydrate is a mixture of ice-like crystals formed by small molecules of water molecules and guest gases. It is usually formed under low temperature and high pressure conditions. Water molecules are connected by hydrogen bonds to form a series of different sizes and structures. Polyhedral pores, in which different size guest molecules enter these pores and are stably present under the action of van der Waals forces. Different guest molecules form gas hydrates with different phase equilibrium conditions.
- hydrates are selective for different guest molecules, and phase equilibrium conditions of milder guest molecules can preferentially enter gas hydrate formation, resulting in
- the change of the gas component in the hydrate phase and the gas phase is more likely to form a gas hydrate component in the hydrate phase, and is thinner in the gas phase, so that the hydrate method can be used to separate from the gas mixture.
- Gas and purify the gas Compared with traditional gas separation technologies (such as chemical absorption, physical adsorption, membrane separation, etc.), hydrate separation gas technology has the advantages of lower energy consumption and more environmental protection. Therefore, research on hydrate synthesis gas technology is in the world. The scope has become a hot spot, and the process and application of gas separation by hydrate method is the key to the technology's shift to industrial application.
- the process research of gas separation by hydrate method is subject to gas hydrate formation rate and gas separation efficiency.
- the formation rate of gas hydrate is a key factor that restricts the separation process of hydrate method.
- one of the key factors affecting gas hydrate formation is the gas-water contact area. The larger the contact surface area of gas and water, the more favorable the dissolution of gas in the water phase, and the fugacity of gas in the water phase will increase accordingly, thereby further increasing the driving force for gas hydrate formation, providing a rapid gas hydrate formation. condition.
- the gas hydrate is usually formed by a stirring method, a spraying method, a bubbling method, etc., and the purpose of these methods is to promote the thorough mixing of the gas and water and to increase the gas-water contact area.
- the stirring method has two kinds of mechanical stirring and electromagnetic stirring.
- the mechanical stirring is suitable for the larger volume reactor, the stirring speed can always be maintained, and the electromagnetic stirring is limited by the magnetic work. It is only suitable for small reactors, and the stirring speed is The formation of hydrates and the increase in the consistency of the system decrease. However, magnetic stirring makes it easier to seal the system, which is especially important in high pressure environments.
- the spraying method is to spray water into a gas-filled reaction vessel through a spray pipe, form a water-in-water form in space, and promote gas-water contact; bubbling method
- the gas is passed through the bubble generating disc and entered into the reaction vessel containing water in the form of bubbles to form a water-inflated form to promote gas-water contact.
- gas-water contact caused by the stirring method, the spray method, and the bubbling method is much larger than the microscopic nucleation scale in scale, resulting in gas-water contact.
- the area is not large enough, and the gas-water contact is not sufficient, which is not enough to significantly increase the gas hydrate formation rate to meet the demand for process production.
- the present invention is directed to a key problem that restricts the rapid formation of gas hydrates - full contact of gas and water, and provides a spray device for rapidly forming a gas hydrate, which is atomized into 5-10 ⁇ m droplets by thoroughly mixing the gas and water.
- the gas-water contact surface area is significantly increased, the fugacity of the gas in the water phase is improved, the gas hydrate formation driving force is improved, the gas hydrate formation induction time is shortened, and the gas hydrate formation speed is improved.
- a gas hydrate-forming spray device mainly comprises a stable gas supply system connected by a pipeline or a line, a saturated solution preparation system, a gas-liquid mixed sprayer, a temperature control system and a data acquisition and processing system;
- the system consists of a test gas cylinder, a CO 2 gas cylinder, a pressure reducing valve and a booster pump, the stable gas supply system supplying gas to the saturated solution preparation system and the gas-liquid mixed atomizer;
- the saturated solution preparation system is from the solution tank and the pressurization a pump composition, the saturated solution preparation system provides a saturated solution to the gas-liquid mixing atomizer;
- the gas-liquid mixing atomizer mainly comprises a high-speed fluid chamber and a gas-liquid mixing chamber communicating with the high-speed fluid chamber, and is disposed in the gas-liquid mixing chamber.
- the atomizer is connected to the gas-liquid mixing chamber of the gas-liquid mixed sprayer through a pressure reducing valve and a gas flow meter; two gas lines are arranged at the top of the CO 2 gas cylinder, and one of the gas lines is
- the booster pump is in communication with the bottom of the solution tank, and the other gas line is in communication with the top of the solution tank; the solution tank is connected to the high-speed fluid chamber of the gas-liquid mixing sprayer by the booster pump
- the temperature control system includes a temperature control cooling system and a constant temperature chamber disposed at the periphery of the solution tank and the gas-liquid mixed sprayer, and the temperature control system controls temperature changes of the solution tank and the gas-liquid mixed sprayer;
- the data collection and processing comprises a liquid flow meter, a gas flow meter, a data collector and a computer processing system, wherein the data acquisition and processing system is used for controlling, collecting, storing and analyzing the stable gas supply system, the saturated solution preparation system, and the gas-liquid mixed sprayer. And temperature control
- the gas-liquid mixing sprayer is hollow inside, and the inner wall is symmetrically provided with a trapezoidal protrusion to divide the interior of the gas-liquid mixing atomizer into a high-speed fluid chamber and a gas-liquid mixing chamber which are connected to each other; and the convexity of the gas-liquid mixing chamber close to the high-speed fluid chamber
- the gas supply inlet is provided at the beginning, and the gas-liquid mixing atomizer further comprises a spray head disposed at the outer end of the atomizer and a distributor distributed on the spray head.
- the atomizer is fixedly coupled to the wall of the gas-liquid mixing sprayer via a threaded joint and a gasket.
- the spray head is annular and detachable, and the spray head is preferably connected to the atomizer through an inner spiral.
- the distributor has an inner diameter of 0.04 to 1.0 mm.
- the present invention also protects the application of the rapid gas hydrate forming spray device for thermodynamic and kinetic experiments in rapid continuous hydrate gas separation and rapid gas hydrate formation.
- the upper working pressure of the device can reach 8MPa, and high-pressure gas-liquid mixing can be performed;
- the device realizes pressure atomization, and the atomization speed is fast.
- the atomized droplets are distributed in the range of 5-10 ⁇ m, and the droplets are enclosed in the gas environment in the device to form a water-in-water contact mode.
- the gas-water contact surface area is effectively improved, and the induction time of gas hydrate formation is significantly shortened under appropriate temperature and pressure conditions, and the gas hydrate can be formed instantaneously, and can be widely applied to rapid continuous hydrate gas separation and gas hydrate rapid formation. Thermodynamic and kinetic experiments.
- the device realizes the full mixing of gas and liquid in the gas-liquid mixing chamber by spraying, does not need to consume energy, effectively reduces the total energy consumption of gas hydrate formation, and improves the energy consumption efficiency of gas hydrate formation.
- the device is easy to use, the annular spray head is detachable and replaceable, and the internal rotary thread type connection mode can not only realize the change of the ring diameter according to the process requirement, but also can clean the nozzle at any time to prevent the nozzle from being blocked.
- Figure 1 is a schematic view of a spray device of the present invention
- Figure 2 is a cross-sectional view of the gas-liquid mixing sprayer of the present invention.
- Figure 3 is a schematic view of a distributor of an annular spray head
- test cylinder 1, test cylinder; 3, booster pump; 4, CO 2 cylinder; 2 , 5, 6, 10, 12, 14, 17, 19, 20, 21, 24, valve; 7, constant temperature room; 8, solution tank; 9, deionized water; 11, booster pump; 13, liquid flow meter; 15, gas-liquid mixed sprayer; 16, temperature control cooling system; 18, pressure reducing valve; 22, gas flow meter; , data collector; 25, computer processing system; 26, high-speed fluid chamber; 27, gas-liquid mixing chamber; 28, threaded joint; 29, spray head; 30, distributor; 31, gas flow inlet; 33; washers.
- a rapid gas hydrate forming spray device mainly comprises a stable gas supply system connected by a pipeline or a line, a saturated solution preparation system, a gas-liquid mixed atomizer 15, a temperature control system, and data acquisition and processing.
- a system comprising: a test gas cylinder containing a test gas, a CO 2 gas cylinder 4 for preparing a saturated solution, a pressure reducing valve 18, and a booster pump 3; the saturated solution preparation system is composed of a solution
- the tank 8 and the booster pump 11 are composed;
- the gas-liquid mixing sprayer 15 mainly includes a high-speed fluid chamber 26, a gas-liquid mixing chamber 27 communicating with the high-speed fluid chamber 26, and an atomizer 32 disposed in the gas-liquid mixing chamber 27.
- the test gas cylinder 1 is connected to the gas-liquid mixing chamber 27 of the gas-liquid mixing sprayer 15 via a pressure reducing valve 18 and a gas flow meter 22; two gas lines, one of which is disposed at the top of the CO 2 gas cylinder 4
- the pipeline communicates with the bottom of the solution tank 8 via the booster pump 3, and the other gas pipeline communicates with the top of the solution tank 8 via the valve 21; the solution tank 8 passes through the valve 10, the booster pump 11, the valve 12, and the liquid in sequence.
- the flow meter 13 is in communication with the high velocity fluid chamber 26 of the gas-liquid mixing nebulizer 15
- the temperature control system includes a temperature control cooling system 16 and a thermostatic chamber 7 disposed at the periphery of the solution tank 8 and the gas-liquid mixing nebulizer 15, the temperature control system controlling the temperature change of the solution tank 8 and the gas-liquid mixing nebulizer 15;
- the data acquisition and processing system includes a liquid flow meter 13, a gas flow meter 22, a data collector 23, and a computer processing system 25.
- the stabilized gas supply system supplies a gas to a saturated solution preparation system or a gas-liquid mixed atomizer 15, which supplies a saturated solution to the gas-liquid mixing atomizer 15, which controls the solution tank 8 and the gas-liquid mixed sprayer 15 Temperature change, the data acquisition and processing system is used to control, collect, store and analyze the temperature, pressure, gas flow, liquid of the stable gas supply system, the saturated solution preparation system, the gas-liquid mixed sprayer 15 and the temperature control system Traffic data.
- the gas-liquid mixing sprayer 15 is hollow inside, the inner wall is symmetrically provided with trapezoidal protrusions to divide the interior of the gas-liquid mixing sprayer 15 into a high-speed fluid chamber 26 and a gas-liquid mixing chamber 27 that communicate with each other;
- a gas inflow port 31 is disposed in the gas-liquid mixing chamber 27 near the convex end of the high-speed fluid chamber 26, and the gas-liquid mixing nebulizer 15 further includes an atomizer 32 disposed in the gas-liquid mixing chamber 27, and is disposed in the mist.
- the spray head 29 at the outer end of the chemist 32 and the distributor 30 are evenly distributed on the spray head 29.
- the atomizer 32 is fixedly coupled to the wall of the gas-liquid mixing sprayer 15 via a threaded joint 28 and a gasket 33.
- the spray head 29 is annular and is detachable from the atomizer 32 by an inner spiral.
- the distributor 30 has an inner diameter of 0.04 to 1.0 mm.
- CO 2 cylinder 4 CO 2 pressurized gas enters at the booster pump 3 from the bottom of the solution tank 8, 8 and the solution tank 9 built some of deionized water and mixed thoroughly dissolved, then the solution tank 8 The top outlet flows back into the CO 2 cylinder 4 via valve 21 to effect a cycle of CO 2 . After 3 hours, the solution tank is formed inside.
- test gas in the test cylinder 1 directly enters the gas-liquid mixing chamber 27 of the gas-liquid mixing sprayer 15 under the action of a vacuum valve 18 through the pressure reducing valve 18, the valve 20, and the gas flow meter 22 to realize gas supply; the stable gas supply
- the test gas supplied by the system and the saturated solution of CO 2 provided by the saturated solution preparation system are fully mixed in the gas-liquid mixing chamber 27, and the fully mixed gas-liquid system enters the atomizer 32 to form a spray of 5-10 ⁇ m.
- the mist droplets enter the spray head 29, and are injected into the gas hydrate reactor at a constant pressure through a distributor 30 having an inner diameter of 0.04 to 1.0 mm.
- the temperature control system controls temperature changes of the solution tank 8 and the gas-liquid mixed sprayer 15; the data acquisition and processing system controls, collects, stores and analyzes the stable gas supply system, the saturated solution preparation system, the gas-liquid mixed sprayer 15 and Temperature, pressure, gas flow, and liquid flow data of the temperature control system.
- the CO 2 gas circulates in the solution tank 8, and is sufficiently mixed with the 0.29 mol% TBAB solution, and after three hours, a CO 2 saturated TBAB aqueous solution is formed.
- the saturated TBAB aqueous solution is pressurized to 3.5 MPa by the booster pump 11 and then enters the high-speed fluid chamber 26 of the gas-liquid mixing sprayer 15 at a high speed to form a vacuum in the gas-liquid mixing chamber 27, and the test gas in the gas cylinder 1 is tested (volume ratio is 40.0).
- the induction time of gas hydrate formation by the same gas and solution system is nearly 10 times shorter than that of mechanical agitation.
- test gas in the test cylinder 1 was a CO 2 /H 2 mixture having a volume ratio of 18.0/82.0%.
- the induction time of gas hydrate formation by the same gas and solution system is nearly 18 times shorter than that of mechanical agitation.
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Analytical Chemistry (AREA)
- Engineering & Computer Science (AREA)
- General Chemical & Material Sciences (AREA)
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Abstract
Description
Claims (7)
- 一种快速形成气体水合物的喷雾装置,其特征在于,主要包括由管路或线路连接的稳定供气系统、饱和溶液制备系统、气液混合喷雾器(15)、控温系统和数据采集及处理系统;所述稳定供气系统由试验气瓶(1)、CO2气瓶(4)、减压阀(18)和增压泵(3)组成,所述稳定供气系统向饱和溶液制备系统和气液混合喷雾器(15)提供气体;所述饱和溶液制备系统由溶液罐(8)和增压泵(11)组成,所述饱和溶液制备系统向气液混合喷雾器(15)提供饱和溶液;所述气液混合喷雾器(15)内部主要包括高速流体腔(26)、跟高速流体腔(26)连通的气液混合腔(27),设在气液混合腔(27)内的雾化器(32);所述试验气瓶(1)经减压阀(18)、气体流量计(22)跟气液混合喷雾器(15)的气液混合腔(27)连通;所述CO2气瓶(4)顶端设有两气体管路,其中的一气体管路经增压泵(3)跟溶液罐(8)的底部连通,另一气体管路跟溶液罐(8)的顶部连通;所述溶液罐经增压泵(11)跟气液混合喷雾器(15)的高速流体腔(26)连通;所述控温系统包括温控制冷系统(16)和设在所述溶液罐(8)、气液混合喷雾器(15)外围的恒温室(7),所述控温系统控制溶液罐(8)和气液混合喷雾器(15)的温度变化;所述数据采集及处理系统包括液体流量计(13)、气体流量计(22)、数据采集器(23)和电脑处理系统(25),所述数据采集及处理系统用来控制、采集、保存和分析所述稳定供气系统、饱和溶液制备系统、气液混合喷雾器和控温系统的温度、压力、气体流量、液体流量数据。
- 根据权利要求1所述的快速形成气体水合物的喷雾装置,其特征在于,所述气液混合喷雾器(15)内部中空,内壁对称设有梯形凸起将所述气液混合喷雾器(15)内部分割为互相连通的高速流体腔(26)和气液混合腔(27);所述气液混合腔(27)内靠近高速流体腔(26)的凸起端设有气体流入口(31),所述气液混合喷雾器(15)还包括设在雾化器(32)外端的喷雾头(29)、喷雾头(29)上均布的分布器(30)。
- 根据权利要求2所述的快速形成气体水合物的喷雾装置,其特征在于,所述喷雾头(29)为环形,可拆卸。
- 根据权利要求2或3所述的快速形成气体水合物的喷雾装置,其特征在于,所述喷雾头(29)跟雾化器(32)通过内螺旋纹连接。
- 根据权利要求2或3所述的快速形成气体水合物的喷雾装置,其特征在于,所述分布器(30)内径为0.04~1.0mm。
- 根据权利要求1所述的快速形成气体水合物的喷雾装置,其特征在于,所述雾化器(32)经螺纹连接头(28)和垫圈(33)跟气液混合喷雾器(15)的壁固定连接。
- 上述任一权利要求所述的快速形成气体水合物的喷雾装置的应用,其特征在于应用于快速连续水合物法气体分离和气体水合物快速形成的热力学和动力学实验。
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US14/765,463 US20160271579A1 (en) | 2013-12-10 | 2014-10-22 | Spraying device for quickly forming gas hydrates |
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CN201310670233.8A CN103623766B (zh) | 2013-12-10 | 2013-12-10 | 一种快速形成气体水合物的喷雾装置 |
CN201310670233.8 | 2013-12-10 |
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PCT/CN2014/089123 WO2015085829A1 (zh) | 2013-12-10 | 2014-10-22 | 一种快速形成气体水合物的喷雾装置 |
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Cited By (1)
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CN112844275A (zh) * | 2020-11-05 | 2021-05-28 | 东北石油大学 | 一种用于分层多级水合物浆制备的反应釜以及制备方法 |
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CN103623766B (zh) * | 2013-12-10 | 2015-03-11 | 中国科学院广州能源研究所 | 一种快速形成气体水合物的喷雾装置 |
CN105502289B (zh) * | 2014-09-24 | 2018-06-29 | 中国石油大学(北京) | 一种催化裂化干气中氢气的分离方法及其系统 |
CN204746272U (zh) * | 2015-06-30 | 2015-11-11 | 江苏宏博机械制造有限公司 | 水合物气液固三相分离的实验装置 |
US20190291048A1 (en) * | 2016-05-20 | 2019-09-26 | Khalifa University of Science and Technology | Bulk separation of undesired components from gas mixtures |
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WO2019106908A1 (ja) * | 2017-11-29 | 2019-06-06 | 東芝ライフスタイル株式会社 | 微細気泡発生器、洗濯機および家電機器 |
CN108102754A (zh) * | 2017-12-15 | 2018-06-01 | 浙江海洋大学 | 一种天然气水合物反应装置 |
CN110044676B (zh) * | 2019-04-24 | 2022-01-14 | 上海汉克威自动化科技有限公司 | 一种用于丙烯腈装置氧分析仪样品气体预处理系统及方法 |
CN112111308B (zh) * | 2020-09-21 | 2021-03-12 | 青岛科技大学 | 一种水合物生产-输运一体式连续反应装置 |
CN114432945B (zh) * | 2020-10-20 | 2023-01-10 | 中国石油化工股份有限公司 | 水合物法联合膜法的连续气体分离系统及其扰动装置 |
CN113074974B (zh) * | 2021-03-26 | 2022-11-04 | 北京石油化工学院 | 一种管式气液雾化混合器混合性能测试装置及方法 |
CN113354202B (zh) * | 2021-06-11 | 2023-04-28 | 宜兴市荣盛达环保有限公司 | 一种高浓度有机工业废水处理与循环利用集成系统 |
CN114314511A (zh) * | 2022-02-09 | 2022-04-12 | 河南农业大学 | 一种基于水合物法的生物氢气提纯装置 |
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