CN1788838A - Method and device for producing hydrate and hydrate slurry using supersonic wave - Google Patents
Method and device for producing hydrate and hydrate slurry using supersonic wave Download PDFInfo
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Abstract
本发明涉及用超声波生产水合物及水合物浆的装置与方法，主要应用于制冷空调储能石油、天然气工业等液(气)体—液体反应的强化结晶反应、超声波混合反应，特别是科研和中试。所述的装置，包括超声波发生器、水合物/浆反应器、气/液瓶、真空泵、恒温水浴箱、加水箱，为变幅杆浸入式系统。本发明首次把超声波波引入水合物浆反应中，在此基础上设计了一个适合于能够在高压下生产水合物及水合物浆的超声波反应器。
The invention relates to a device and method for producing hydrate and hydrate slurry by using ultrasonic waves, which are mainly used in the enhanced crystallization reaction and ultrasonic mixing reaction of liquid (gas) body-liquid reactions in refrigeration, air conditioning, energy storage, petroleum and natural gas industries, especially for scientific research and Pilot test. The device includes an ultrasonic generator, a hydrate/slurry reactor, a gas/liquid bottle, a vacuum pump, a constant temperature water bath, and a water adding tank, and is a horn immersion system. The present invention introduces ultrasonic wave into hydrate slurry reaction for the first time, and designs an ultrasonic reactor suitable for producing hydrate and hydrate slurry under high pressure.
Description
Technical field
The present invention relates to produce the apparatus and method of hydrate and hydrate slurry, be mainly used in reinforcement crystallization reaction, ultrasonic wave hybrid reaction, particularly scientific research and the pilot scale of liquid (gas) body-liquid reactions such as refrigeration air-conditioner energy storage oil, gas industry with ultrasonic wave.
Background technology
Ultrasonic wave is that the compressional wave by a series of density interphases constitutes, and by liquid medium to around propagate.When ultrasonic energy is enough high, will produce ultrasonic cavitation.The ultrasonic cavitation bubble produces down (be liquid drawn back and form the hole) mutually under the sound wave negative pressure in the sound wave negative pressure, their immediately collapse under thing followed sound wave malleation acts on mutually again.About 0.1 μ s of the life-span of cavitation bubble, when cavitation bubble collapses, can discharge huge energy, and the about 110m/s of generation speed, microjet with intense impact power, make collision density up to 1.5kg/cm2, supervene the high temperature of hundreds of atmospheric high pressure and thousands of degree.These conditions can promote disturbance and the boundary between non-even practising physiognomy to upgrade, thereby quicken mass transfer and diabatic process between the interface.The ultrasound-enhanced effect of chemical reaction and physical process mainly is because energy effect and mechanical effect that the ultrasonic cavitation of liquid produces cause.
The application of power ultrasonic on industry (as ultrasonic cleaning, welding, processing), medical science (as ultrasonic physiotherapy, control cancer), biology (as the ultrasonic big molecule of DNA of successfully shearing), chemistry (as depolymerization, catalysis), chemical industry (as ultrasonic crystallization, atomizing, precipitation) is very extensive, introduces ultrasonic wave and mainly have and regulate crystal size, improve size distribution, shorten the effect of nucleation crystallization time in crystallization process.
Gas hydrate adopts circulating pump to produce disturbance or the short gas hydrate generation of mechanical agitation usually at present, yet disturbance removes consumes energy, and efficient is lower, boot time is longer, and degree of supercooling is bigger, and hydrate generates also inhomogeneous, particle size distribution is big, and the hydrate slurry of generation is difficult to carry.
Summary of the invention
The objective of the invention is to utilize existing ultrasonic technology and high pressure resistant quartz glass, provide a kind of ultrasonic wave that can under high pressure utilize to be used for studying hydrate and hydrate slurry device.
Device with ultrasonic wave production hydrate and hydrate slurry of the present invention comprises supersonic generator, hydrate/slurry reactor, gas/liquid bottle, vavuum pump, constant water bath box, adds water tank;
Described supersonic generator is made up of the ultrasonic wave generator controller, transducer, the luffing bar that link to each other successively, and the end of luffing bar is a ultrasonic probe, and insertion hydrate/slurry reactor also immerses in the reaction system; By the transducer ultrasonic waves transmitted, the transmitting terminal of process luffing bar is that ultrasonic probe is transmitted directly in hydrate/slurry reactor; The ultrasound source frequency setting is 10k-50kHz, and power is 0-10kW, can hyperacoustic input power of linear as required adjusting and action time;
Be connected to hydrated reactant on described hydrate/slurry reactor and inject valve and emptying valve; Screen pack is equipped with in the bottom of hydrate/slurry reactor;
Described gas/liquid bottle links to each other with hydrate/slurry reactor by three-way pipe, valve with vavuum pump;
In the described constant water bath box heat exchanger is housed, links to each other with refrigerator by pipeline; Constant water bath box links to each other with hydrate/slurry reactor by pump, valve; Constant water bath box is connected to temperature controller; The temperature range of water bath with thermostatic control be 0-15 ℃ adjustable, guarantee that whole hydro-combination process does not freeze;
The described water tank that adds links to each other with constant water bath box by pump, valve.
The main body of described hydrate/slurry reactor is quartz glass or sapphire cylinder, by sealing ring, bolting between upper flange lid and lower flange cover; The luffing bar is by sealing ring and be bolted to upper flange and cover.
The shape of ultrasonic probe of the present invention can change as required.Ultrasonic probe is the transmitting terminal by the luffing bar (also claiming speed converter) of ultrasonic transduction driving, and by the transducer ultrasonic waves transmitted, its transmitting terminal of process is transmitted directly in the reactor.The particle vibration amplitude or the sound intensity of luffing rod end surface are controlled by the electrical power that changes the input transducer.Utilization sound changing-breadth system can obtain the high power density of w/cm2 up to a hundred on its radiation end face.The major advantage of this luffing bar immersion system have following some: (1) is compared with the ultrasonic cleaning machine, in treat liquid, not only can obtain much higher ultrasonic power density, also can eliminate the energy loss that ultrasonic wave causes fully when passing tank and drag.(2) can be reaction liquid bigger power density excursion is provided, so that therefrom seek to determine best ultrasound wave irradiation condition.(3) can reach coupling preferably between ultrasound intensity and the irradiation liquid capacity, in the hope of obtaining optimum efficiency.
The reactor of this device uses high voltage bearing quartz glass or sapphire, and is visual, according to different thickness, and can withstand voltage 0-40MPa.Quartz glass or sapphire cylinder are corrosion-resistant, and light transmittance is 80%, can observe the response situation of hydrate by it.
Because constant temperature system can drop to the temperature of reactor subzero 20 ℃, quartz glass or sapphire can keep performance at low temperatures, so this device also can carry out low temperature test.
Device of the present invention also can add output current adjuster and power output logger in supersonic generator, can continuous linear adjusting power output, write down power output simultaneously, and therefore can real-time processing data, tracking reaction process.
Another object of the present invention provides a kind of method of producing hydrate and hydrate slurry with ultrasonic wave.
Method of producing hydrate and hydrate slurry with ultrasonic wave of the present invention may further comprise the steps:
A) nitrogen cylinder is injected valve by hydrated reactant and link to each other, hydrate/slurry reactor is carried out leak test with hydrate/slurry reactor;
B) vavuum pump is linked to each other with hydrate/slurry reactor by valve, hydrate/slurry reactor is vacuumized;
C) once more pipeline and hydrated reactant being injected valve is connected, earlier in connecting pipe, fill with water, to guarantee keeping vacuum in the reactor, the other end with connecting pipe inserts under the water surface of the open container that fills water then, open hydrated reactant and inject valve, water is inhaled under the effect of siphon in hydrate/slurry reactor;
D) the gas/liquid bottle is connected input gas or liquid with hydrate/slurry reactor by valve;
E) constant water bath box is adjusted to the temperature that hydrate generates, after design temperature is stable, hydrate/slurry reactor is put into water bath with thermostatic control, the turn-on data acquisition system, and pick up counting;
F) when hydrate/slurry reactor temperature drop to setting bath temperature and stable after, setting ultrasonic wave action time is 1-5 second, the interruption unlatching cycle of setting supersonic generator is 3-10;
G) by the transducer ultrasonic waves transmitted, the transmitting terminal of process luffing bar is that ultrasonic probe is transmitted directly in hydrate/slurry reactor; The ultrasound source frequency setting is 10k-50kHz, and power is 0-10kW, can hyperacoustic input power of linear as required adjusting and action time;
H) after the ultrasonic wave effect was finished, hydrate or hydrate slurry generated in hydrate/slurry reactor.
Among the step G, can pass through output current adjuster and the continuous linear adjusting power output of power output logger, write down ultrasonic power output simultaneously.
During reaction, earlier system is vacuumized, close pumped vacuum systems then, utilize vacuum to suck a certain amount of distilled water, and then vacuumize, note vacuumizing and to be extracted into distilled water below the saturated vapor pressure of temperature at that time, ratio according to hydrate in the hydrate slurry, add certain hydration reaction gas (liquid), vacuumize again, back several times repeatedly general equal satisfying the demands.
After exhausting vacuum and adding reaction, water bath with thermostatic control is adjusted to design temperature, after design temperature is stable, reactor is put into water bath with thermostatic control, the turn-on data acquisition system, and pick up counting; When the hydration system drops to the bath temperature of setting and when stablize a period of time, set ultrasonic wave action time, be interrupted and open supersonic generator, the hydrate slurry generation.Increase the concentration of hydrate slurry if desired, open valve, allow a certain amount of water flow out.Reduce the concentration of hydrate slurry if desired, open pump, add a certain amount of water to reactor.When the hydrate total overall reaction was finished in the reactor, the hydrate granule size determined whether to open ultrasonic wave and time length in the hydrate slurry by observing.
Beneficial effect of the present invention has:
1. first ultrasound waves is introduced in the hydrate slurry reaction, designed a ultrasound reactor that is suitable under high pressure to produce hydrate and hydrate slurry on this basis.
2. applied range, temperature and pressure can be measured, and the ultrasonic power linearity is adjustable.
3. adopted the integration design, compact conformation.
Description of drawings
Fig. 1 is overall structure figure of the present invention;
Fig. 2 is the structural representation of hydrate of the present invention/slurry reactor.
The specific embodiment
Device with ultrasonic wave production hydrate and hydrate slurry of the present invention as shown in Figure 1, comprises supersonic generator, hydrate/slurry reactor 5, gas/liquid bottle 6, vavuum pump 7, constant water bath box 8, adds water tank 11;
Described supersonic generator is made up of the ultrasonic wave generator controller 1, transducer 2, the luffing bar 3 that link to each other successively, and the end of luffing bar 3 is a ultrasonic probe 4, and insertion hydrate/slurry reactor 5 also immerses in the reaction system; By transducer 2 ultrasonic waves transmitted, the transmitting terminal of process luffing bar 3 is that ultrasonic probe 4 is transmitted directly in hydrate/slurry reactor 5; The ultrasound source frequency setting is 10k-50kHz, and power is 0-10kW, can hyperacoustic input power of linear as required adjusting and action time;
Be connected to hydrated reactant on described hydrate/slurry reactor 5 and inject valve f5 and emptying valve f4; Screen pack 26 is equipped with in the bottom of hydrate/slurry reactor 5;
Described gas/liquid bottle 6 links to each other with hydrate/slurry reactor 5 by three-way pipe, valve f3 with vavuum pump 7;
In the described constant water bath box 8 heat exchanger 9 is housed, links to each other with refrigerator 10 by pipeline; Constant water bath box 8 links to each other with hydrate/slurry reactor 5 with b3, valve f1 by pump b1; Constant water bath box 8 is connected to temperature controller t1; The temperature range of water bath with thermostatic control be 0-15 ℃ adjustable, guarantee that whole hydro-combination process does not freeze;
The described water tank 11 that adds links to each other with constant water bath box 8 by pump b2, valve f2.
As shown in Figure 2, the main body of described hydrate/slurry reactor 5 is quartz glass or sapphire cylinder 21, is fixed between upper flange lid 22 and the lower flange lid 23 by sealing ring 24, bolt 25; Luffing bar 3 is fixed on the upper flange lid 22 by sealing ring 27 and bolt 28.
Output current adjuster and power output logger are installed in the described supersonic generator, can continuous linear adjusting power output, write down power output simultaneously.
Use as the device among Fig. 1, the method with ultrasonic wave is produced hydrate and hydrate slurry may further comprise the steps:
A) nitrogen cylinder is injected valve f5 by hydrated reactant and link to each other, hydrate/slurry reactor 5 is carried out leak test with hydrate/slurry reactor 5;
B) vavuum pump 7 is linked to each other with hydrate/slurry reactor 5 by valve f3, hydrate/slurry reactor 5 is vacuumized;
C) once more pipeline and hydrated reactant being injected valve f5 is connected, earlier in connecting pipe, fill with water, to guarantee keeping vacuum in the reactor, the other end with connecting pipe inserts under the water surface of the open container that fills water then, open hydrated reactant and inject valve f5, water is inhaled under the effect of siphon in hydrate/slurry reactor 5;
D) gas/liquid bottle 6 is connected input gas or liquid with hydrate/slurry reactor 5 by valve f3;
E) constant water bath box 8 is adjusted to the temperature that hydrate generates, after design temperature is stable, hydrate/slurry reactor 5 is put into water bath with thermostatic control, the turn-on data acquisition system, and pick up counting;
F) when temperature in hydrate/slurry reactor 5 drop to setting bath temperature and stable after, setting ultrasonic wave action time is 1-5 second, the interruption unlatching cycle of setting supersonic generator is 3-10;
G) by transducer 2 ultrasonic waves transmitted, the transmitting terminal of process luffing bar 3 is that ultrasonic probe 4 is transmitted directly in hydrate/slurry reactor 5; The ultrasound source frequency setting is 10k-50kHz, and power is 0-10kW, can hyperacoustic input power of linear as required adjusting and action time;
H) after the ultrasonic wave effect was finished, hydrate or hydrate slurry generated in hydrate/slurry reactor 5.
Among the step G,, write down ultrasonic power output simultaneously by output current adjuster and the continuous linear adjusting power output of power output logger.
Embodiment one:
Designed an experimental provision by Fig. 1, wherein the ultrasound source frequency is 15kHz, and 1000 watts of peak power outputs are linear adjustable.Reactor volume 460ml, cross-sectional reactor area 38.5cm
2, reactor is made up of quartz-glass cylinder, upper flange lid, lower flange lid, hydrated reactant injection valve and emptying valve.Quartz-glass cylinder is corrosion-resistant, and light transmittance is 80%, and barrel bore is 70mm, thick 3mm, and long 130mm can observe the response situation of hydrate by it.Blind flange is formed by the whole car system of stainless steel material, and upper flange covers thick 13mm, and lower flange covers thick 8mm.Blind flange connects to come the seal glass cylinder by bolt, O RunddichtringO up and down.Ultrasonic probe is connected sealing by bolt, silicon rubber O type circle with the upper flange lid.
The reactant of this embodiment is water and liquid HCFC-141b, generates hydrate slurry during reaction, and the mass ratio of water and HCFC-141b is 6: 1, and the hydrate slurry concentration of generation is 46.3%.Can suitably add some surfactants in order to accelerate reaction process.Set water-bath earlier before the experiment beginning, open refrigeration system temperature is dropped to the needed temperature of experiment, with preparing certain density aqueous solution rinse reactor, vacuumize then, then a certain amount of aqueous solution that has prepared concentration, utilize vacuum in the sucting reaction device, vacuumize again, do not remain in the reaction, can add a small amount of gaseous state HCFC-141b in order to guarantee air, take out vacuum again one time, add required HCFC-141b at last.After the temperature constant 2 hours, configure excusing from death wave power, action time, open ultrasonic wave.The result shows that ultrasonic wave can obviously reduce the degree of supercooling that hydrate generates, and improves formation speed, the hydrate epigranular, and the hydrate slurry of formation is stable fine and smooth.The result has proved that this device can promote hydration reaction reliably.
Embodiment two:
Designed an experimental provision by Fig. 1, wherein the ultrasound source frequency is 25kHz, and 1500 watts of peak power outputs are linear adjustable.Reactor volume 78.5ml, cross-sectional reactor area 19.6cm2, reactor is made up of sapphire glass cylinder, upper flange lid, lower flange lid, hydrated reactant injection valve and emptying valve.The sapphire glass cylinder is corrosion-resistant, and light transmittance is 90%, and barrel bore is 50mm, thick 5mm, and long 40mm can observe the response situation of hydrate by it.Blind flange is formed by the whole car system of stainless steel material, and upper flange covers thick 13mm, and lower flange covers thick 8mm.Blind flange connects to come the seal glass cylinder by bolt, O RunddichtringO up and down.Ultrasonic probe is connected sealing by bolt, silicon rubber O type circle with the upper flange lid.
The reactant of this embodiment is water and liquid HFC-134a, all generates hydrate during reaction, and the mass ratio of water and HFC-134a is 2.55: 1.Can suitably add some surfactants in order to accelerate reaction process.Set bath temperature earlier before the experiment beginning, open refrigeration system temperature is dropped to the needed temperature of experiment, with preparing certain density aqueous solution rinse reactor, vacuumize then, then a certain amount of aqueous solution that has prepared concentration, utilize vacuum in the sucting reaction device, vacuumize again, do not remain in the reaction, can add a small amount of gaseous state HFC-134a in order to guarantee air, take out vacuum again one time, add required HFC-134a at last.After the temperature constant 2 hours, configure excusing from death wave power, action time, open ultrasonic wave.The result shows that ultrasonic wave can make hydrate generate fast, and the total overall reaction thing forms hydrate.The result has proved that this device can generate hydrate reliably.
Claims (5)
1, a kind of device with ultrasonic wave production hydrate and hydrate slurry is characterized in that: comprise supersonic generator, hydrate/slurry reactor (5), gas/liquid bottle (6), vavuum pump (7), constant water bath box (8), add water tank (11);
Described supersonic generator is made up of the ultrasonic wave generator controller (1), transducer (2), the luffing bar (3) that link to each other successively, and the end of luffing bar (3) is ultrasonic probe (4), and insertion hydrate/slurry reactor (5) also immerses in the reaction system; By transducer (2) ultrasonic waves transmitted, the transmitting terminal of process luffing bar (3) is that ultrasonic probe (4) is transmitted directly in hydrate/slurry reactor (5); The ultrasound source frequency setting is 10k-50kHz, and power is 0-10kW, can hyperacoustic input power of linear as required adjusting and action time;
Be connected to hydrated reactant on described hydrate/slurry reactor (5) and inject valve (f5) and emptying valve (f4); Screen pack (26) is equipped with in the bottom of hydrate/slurry reactor (5);
Described gas/liquid bottle (6) links to each other with hydrate/slurry reactor (5) by three-way pipe, valve (f3) with vavuum pump (7);
Heat exchanger (9) is housed in the described constant water bath box (8), links to each other with refrigerator (10) by pipeline; Constant water bath box (8) links to each other with hydrate/slurry reactor (5) by pump (b1, b3), valve (f1); Constant water bath box (8) is connected to temperature controller (t1); The temperature range of water bath with thermostatic control be 0-15 ℃ adjustable, guarantee that whole hydro-combination process does not freeze;
The described water tank (11) that adds links to each other with constant water bath box (8) by pump (b2), valve (f2).
2, device according to claim 1, it is characterized in that: the main body of described hydrate/slurry reactor (5) is quartz glass or sapphire cylinder (21), is fixed between upper flange lid (22) and the lower flange lid (23) by sealing ring (24), bolt (25); Luffing bar (3) is fixed on the upper flange lid (22) by sealing ring (27) and bolt (28).
3, device according to claim 1 and 2 is characterized in that: output current adjuster and power output logger are installed in the described supersonic generator, can continuous linear adjusting power output, and write down power output simultaneously.
4, a kind of method of producing hydrate and hydrate slurry with ultrasonic wave is characterized in that, may further comprise the steps:
A) nitrogen cylinder is injected valve (f5) by hydrated reactant and link to each other, hydrate/slurry reactor (5) is carried out leak test with hydrate/slurry reactor (5);
B) vavuum pump (7) is linked to each other with hydrate/slurry reactor (5) by valve (f3), hydrate/slurry reactor (5) is vacuumized;
C) once more pipeline and hydrated reactant being injected valve (f5) is connected, earlier in connecting pipe, fill with water, to guarantee keeping vacuum in the reactor, the other end with connecting pipe inserts under the water surface of the open container that fills water then, open hydrated reactant and inject valve (f5), water is inhaled under the effect of siphon in hydrate/slurry reactor (5);
D) gas/liquid bottle (6) is connected input gas or liquid with hydrate/slurry reactor (5) by valve (f3);
E) constant water bath box (8) is adjusted to the temperature that hydrate generates, after design temperature is stable, hydrate/slurry reactor (5) is put into water bath with thermostatic control, the turn-on data acquisition system, and pick up counting;
F) when temperature in hydrate/slurry reactor (5) drop to setting bath temperature and stable after, setting ultrasonic wave action time is 1-5 second, the interruption unlatching cycle of setting supersonic generator is 3-10;
G) by transducer (2) ultrasonic waves transmitted, the transmitting terminal of process luffing bar (3) is a ultrasonic probe
(4) be transmitted directly in hydrate/slurry reactor (5); The ultrasound source frequency setting is 10k-50kHz, and power is 0-10kW, can hyperacoustic input power of linear as required adjusting and action time;
H) after the ultrasonic wave effect was finished, hydrate or hydrate slurry generated in hydrate/slurry reactor (5).
5, method according to claim 4 is characterized in that: among the step G, by output current adjuster and the continuous linear adjusting power output of power output logger, write down ultrasonic power output simultaneously.
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| CNB2004100773383A CN100341615C (en) | 2004-12-15 | 2004-12-15 | Method and device for producing hydrate and hydrate slurry using supersonic wave |
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| CNB2004100773383A CN100341615C (en) | 2004-12-15 | 2004-12-15 | Method and device for producing hydrate and hydrate slurry using supersonic wave |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101225338B (en) * | 2007-12-19 | 2011-03-23 | 中国科学院广州能源研究所 | Method and device for rapid preparation of natural gas hydrate by static supergravity |
| CN102085472A (en) * | 2010-12-16 | 2011-06-08 | 中国科学院高能物理研究所 | Reduced pressure distillation ultrasonic reactor |
| CN106556687A (en) * | 2016-11-21 | 2017-04-05 | 中国石油大学(华东) | Weak cementing non-diagenesis hydrate acoustics and saturation degree synchronous testing device and method |
| CN107899530A (en) * | 2017-12-15 | 2018-04-13 | 中南民族大学 | A kind of organic chemical synthesis reactor of integration operation |
| CN109589654A (en) * | 2018-12-14 | 2019-04-09 | 中国科学院广州能源研究所 | A kind of gas hydrate slurry separator and method based on air bearing and siphon synergistic effect |
| CN114082574A (en) * | 2021-11-25 | 2022-02-25 | 中国科学院长春应用化学研究所 | Feeding unit for ultrasonic spraying equipment for water electrolysis and fuel cell membrane electrode preparation |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| WO2015087268A2 (en) * | 2013-12-12 | 2015-06-18 | Indian Institute Of Technology Madras | Systems and methods for gas hydrate slurry formation |
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2004
- 2004-12-15 CN CNB2004100773383A patent/CN100341615C/en not_active Expired - Fee Related
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101225338B (en) * | 2007-12-19 | 2011-03-23 | 中国科学院广州能源研究所 | Method and device for rapid preparation of natural gas hydrate by static supergravity |
| CN102085472A (en) * | 2010-12-16 | 2011-06-08 | 中国科学院高能物理研究所 | Reduced pressure distillation ultrasonic reactor |
| CN102085472B (en) * | 2010-12-16 | 2013-02-13 | 中国科学院高能物理研究所 | Reduced pressure distillation ultrasonic reactor |
| CN106556687A (en) * | 2016-11-21 | 2017-04-05 | 中国石油大学(华东) | Weak cementing non-diagenesis hydrate acoustics and saturation degree synchronous testing device and method |
| CN107899530A (en) * | 2017-12-15 | 2018-04-13 | 中南民族大学 | A kind of organic chemical synthesis reactor of integration operation |
| CN107899530B (en) * | 2017-12-15 | 2024-06-11 | 中南民族大学 | Organic chemical synthesis reactor of integration operation |
| CN109589654A (en) * | 2018-12-14 | 2019-04-09 | 中国科学院广州能源研究所 | A kind of gas hydrate slurry separator and method based on air bearing and siphon synergistic effect |
| CN114082574A (en) * | 2021-11-25 | 2022-02-25 | 中国科学院长春应用化学研究所 | Feeding unit for ultrasonic spraying equipment for water electrolysis and fuel cell membrane electrode preparation |
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| CN100341615C (en) | 2007-10-10 |
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