CN108128755B - Drum-type dielectric barrier discharge water mist hydrogen peroxide preparation device - Google Patents

Drum-type dielectric barrier discharge water mist hydrogen peroxide preparation device Download PDF

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CN108128755B
CN108128755B CN201810055198.1A CN201810055198A CN108128755B CN 108128755 B CN108128755 B CN 108128755B CN 201810055198 A CN201810055198 A CN 201810055198A CN 108128755 B CN108128755 B CN 108128755B
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hydrogen peroxide
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power supply
water
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CN108128755A (en
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刘昌裕
陈秉岩
戚家程
刘子豪
田泽
朱昌平
蒋永锋
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Changzhou Campus of Hohai University
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    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B15/00—Peroxides; Peroxyhydrates; Peroxyacids or salts thereof; Superoxides; Ozonides
    • C01B15/01—Hydrogen peroxide
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Abstract

The invention discloses a drum-type dielectric barrier discharge water mist hydrogen peroxide preparation device, which comprises a motor control unit, a motor driving unit, a motor transmission mechanism in the transmission and discharge unit, a gas recovery unit, a hydrogen peroxide collection unit, a spectrum detection unit, a programmable AC/DC power supply, a PDM high-voltage excitation power supply and an auxiliary power supply. The invention adopts the dielectric barrier discharge principle to prepare hydrogen peroxide, adopts a roller-crawler type integrated production mode, realizes a full-automatic production mode of obtaining a product hydrogen peroxide through oxygen and water and collecting the product hydrogen peroxide, and realizes the function of quickly preparing the hydrogen peroxide.

Description

Drum-type dielectric barrier discharge water mist hydrogen peroxide preparation device
Technical Field
The invention relates to a drum-type dielectric barrier discharge water mist hydrogen peroxide preparation device, and belongs to the technical field of hydrogen peroxide preparation.
Background
The hydrogen peroxide is a green oxidant, the reaction product is pollution-free, can chemically react with most substances, has the characteristics of high reaction speed, small reaction dosage and controllable reaction, and is widely applied to the fields of bleaching industry, synthesis industry, electroplating industry, three-waste treatment, food, pharmaceutical industry and the like.
At present, the anthraquinone method is mainly adopted to produce hydrogen peroxide (H) in industry2O2) The anthraquinone method for producing hydrogen peroxide has the serious problems of complex process, large equipment investment, environmental pollution and the like, and also has the defects of large reactor volume and long single production period; in addition, the problems of catalyst pulverization, agglomeration, anthraquinone degradation, low hydrogen efficiency, catalyst poisoning and the like can not be avoided in the production process. The method for directly synthesizing hydrogen peroxide from oxyhydrogen by adopting noble metal supported catalysts such as palladium, gold and the like has the defects of unavailable combination of high selectivity and high conversion rate, impurity-containing products, difficult separation and the like.
Disclosure of Invention
The technical problem to be solved by the invention is to overcome the defects of the prior art and provide a drum-type DBD water mist hydrogen peroxide preparation device, hydrogen peroxide is prepared by adopting a Dielectric Barrier Discharge (DBD) principle, a full-automatic production mode that the product hydrogen peroxide is collected by oxygen and water is realized by adopting a drum-crawler-type integrated production mode, and the function of quickly preparing hydrogen peroxide is realized.
In order to solve the technical problems, the invention provides a drum-type dielectric barrier discharge water mist hydrogen peroxide preparation device which comprises a sealed box body, an air inlet unit, a water supply unit, a transmission and discharge unit, a water mist generation unit, a motor driving unit, a motor control unit, a gas recovery unit, a hydrogen peroxide collection unit, a spectrum detection unit, a programmable AC/DC power supply, a PDM high-voltage excitation power supply and an auxiliary power supply, wherein the sealed box body is provided with a gas inlet and outlet; wherein, the transmission and discharge unit, the water mist generation unit, the hydrogen peroxide collection unit and the spectrum detection unit are arranged in the sealed box body; the sealed box body is provided with an air outlet and a water outlet;
the gas inlet unit consists of a gas pump, a gas source, an adjusting valve and a gas flowmeter, wherein the gas pump pumps gas with a certain flow rate from the gas source into the water mist generating unit to provide oxygen with a certain flow rate for the hydrogen peroxide preparation device; the water supply unit consists of a water tank, a water pump, an adjusting valve and a liquid flowmeter, and the water pump pumps water with a certain flow rate from the water tank to the water mist generation unit; the water mist generating unit is an atomizing nozzle and is used for generating water mist jet; the transmission and discharge unit comprises a motor transmission mechanism and a DBD unit; the motor transmission mechanism consists of a servo motor and a series of servo motor transmission mechanisms, and the DBD unit consists of a high-voltage roller electrode and a strip-shaped low-voltage electrode; the transmission and discharge unit and the water mist generation unit jointly form a hydrogen peroxide generation unit, the center of a motor shaft sleeve is collinear with the centers of all high-pressure roller electrode rotating shafts, the radius of a high-pressure roller electrode is equal to that of a motor driving wheel, a transmission film is firstly sleeved on the high-pressure roller electrode and a motor shaft sleeve, the position of the high-pressure roller electrode in a sealed box body is fixed, the motor is horizontally moved until the transmission film is tightened, a discharge gap is formed between the high-pressure roller electrode and a strip-shaped low-voltage electrode, and the water film is discharged under the action of a PDM high-voltage excitation power supply; the spectrum detection unit is a spectrum probe and is used for detecting the relative spectral intensity of hydroxyl generated in the discharge gap; the programmable AC/DC power supply is used for setting the input voltage of the PDM high-voltage excitation power supply and the power of the whole system; the PDM high-voltage excitation power supply is an excitation power supply of a hydrogen peroxide generator; the auxiliary power supply is used for supplying power to the motor driving unit; the hydrogen peroxide collecting unit collects hydrogen peroxide by adopting a collecting tank, and the collected hydrogen peroxide needs to be subjected to a series of enrichment and purification; the gas recovery unit enables gas which is not completely reacted to enter the compressor from the gas outlet through the circulating pipeline and be pressurized to the gas pump, and therefore the gas is introduced into the device again;
the atomizing nozzle is provided with two input ends of liquid and oxygen, the liquid input end is connected with a water pump of the water supply unit through a water supply pipeline, the oxygen input end is connected with a gas pump of the gas inlet unit through a gas supply pipeline, and the oxygen passing through the gas inlet unit and the water provided by the water supply unit are mixed in the water mist generating unit to form water mist jet flow which enters the transmission and discharge unit; the collecting tank is arranged at a position which is 10-30cm away from the center of the roller at the rightmost end, and the scraper plate is tightly close to the transmission film; the spectrum probe is placed 3-12mm above the transmission film and beside any one low-voltage electrode, and the horizontal distance between the spectrum probe and the low-voltage electrode is 10-30 mm; the auxiliary power supply supplies power to the motor driving unit, the motor control unit is connected with the motor driving unit, and the motor driving unit is connected with the transmission and discharge unit; the hydrogen peroxide generating unit is connected with the gas recovery unit, and the gas recovery unit is connected with the gas inlet unit; the auxiliary power supply is connected with a programmable AC/DC power supply, and the programmable AC/DC power supply is connected with a PDM high-voltage excitation power supply; the negative electrode of the PDM high-voltage excitation power supply is connected with a strip-shaped low-voltage electrode of the DBD reactor, the positive electrode of the PDM high-voltage excitation power supply is connected with a high-voltage roller electrode of the DBD reactor, and an insulating sleeve is sleeved on the high-voltage roller electrode to serve as a dielectric layer;
the distance H between the atomizing nozzle and the transmission film satisfies the following formula:
Figure BDA0001553543400000021
wherein, the range of alpha is 60 degrees to 120 degrees, and S is the length of the high-voltage roller electrode;
the running speed v, the duty ratio D and the distance L between the adjacent high-voltage roller electrodes of the transmission film2Satisfies the following formula:
L2＝(2N+1)DTm,jv
wherein N is a non-zero natural number, Tm,jFor one period of the power density modulation,
Figure BDA0001553543400000022
Ton,jis the discharge time in one power regulation period.
The distance between the high-voltage roller electrode and the strip-shaped low-voltage electrode is 0.5-2.5 cm; the high-voltage roller electrode and the strip-shaped low-voltage electrode are both made of stainless steel materials.
The sealing box body is made of plastic or organic glass insulating materials.
The discharge medium layer is made of polytetrafluoroethylene or rubber.
The whole structure of the collecting tank is a U-shaped groove without a cover, the rear plate is a scraper and 10-30mm higher than the front plate, the rear plate has an inclination of 30-75 degrees, and any sides of the left side and the right side of the U-shaped groove are opened, so that the scraped hydrogen peroxide flows into the sealed box body and flows out of the water outlet of the sealed box body for collection.
The liquid flowmeter adopts an electromagnetic flowmeter or a rotor flowmeter; the gas flowmeter adopts a pore plate flowmeter with pressure compensation, a small-flow vortex shedding flowmeter or a v-cone flowmeter.
The atomizing nozzle described above was a GA-series fan nozzle from PNR corporation.
The duty ratio D is 0.1-0.5.
The thickness of the water film formed on the transmission film by the water mist is adjusted to be within the range of 0.1 mm-0.5 mm by adjusting the water flow of the water supply pipeline and the air flow of the air supply pipeline.
The yield of the hydrogen peroxide is adjusted by adjusting the rotating speed of the motor and the frequency, the voltage amplitude or the discharge power of the PDM high-voltage excitation power supply.
The invention achieves the following beneficial effects:
the invention adopts DBD principle to prepare hydrogen peroxide, adopts roller-crawler type integrated production mode, realizes full-automatic production mode of obtaining products from raw materials and collecting products, and realizes the function of quickly preparing hydrogen peroxide.
The invention leads the gas which is not completely reacted into the device again for recycling, thereby reducing the production cost.
The invention uses the hydrogen peroxide generated by scraping with the scraper to be collected in the collecting tank, and the circulation is carried out in such a way, so that the hydrogen peroxide is efficiently generated.
Drawings
FIG. 1 is a schematic view of the overall structure of the apparatus of the present invention;
FIG. 2 is a schematic view showing the connection of the components of the apparatus of the present invention;
FIG. 3 is a schematic diagram of a DBD unit;
FIG. 4 is a schematic structural view of a hydrogen peroxide collecting unit;
FIG. 5 is a schematic view of an atomizing nozzle;
FIG. 6 is a schematic view of an atomizing nozzle installation;
FIG. 7 is a waveform diagram of the power supply of the PDM high-voltage excitation power supply;
fig. 8 is a flow chart of the operation of the apparatus of the present invention.
Detailed Description
The invention is further described below. The following examples are only for illustrating the technical solutions of the present invention more clearly, and the protection scope of the present invention is not limited thereby.
As shown in fig. 1 and 2, the drum-type dielectric barrier discharge water mist hydrogen peroxide preparation device of the invention comprises an air inlet unit, a water supply unit, a transmission and discharge unit, a water mist generation unit, a motor driving unit, a motor control unit, a gas recovery unit, a hydrogen peroxide collection unit, a spectrum detection unit, a programmable AC/DC power supply, a PDM high-voltage excitation power supply, an auxiliary power supply and the like. In particular, the method comprises the following steps of,
the gas inlet unit mainly comprises a gas pump 7, a gas source 18, an adjusting valve 2 and a gas flowmeter 6, wherein the gas pump 7 pumps gas with a certain flow from the gas source 18 into the water mist generating unit to provide oxygen with a certain flow for the whole system to be used as a raw material for preparing hydrogen peroxide; the water supply unit mainly comprises a water tank 1, a water pump 3, an adjusting valve 2 and a liquid flowmeter 4, wherein the water pump 3 extracts water with a certain flow from the water tank 1 to the water mist generation unit; the transmission and discharge unit comprises a motor transmission mechanism and a DBD unit, the motor transmission mechanism consists of a servo motor and a series of servo motor transmission mechanisms, and the servo motor has good response characteristic, good high-speed performance and strong overload resistance; the DBD unit in the transmission and discharge unit adopts a roller stainless steel electrode as a high-voltage electrode, the low-voltage electrode adopts a stainless steel strip electrode, and the distance between the high-voltage electrode and the low-voltage electrode is 0.5-2.5cm, so that the DBD unit is used for discharging a water film on the surface of the film to generate high-concentration hydrogen peroxide; a plurality of DBD cells may be provided, as in fig. 2, as two pairs of high voltage electrodes and low voltage electrodes, i.e., two DBD cells. The center of the motor shaft sleeve is collinear with the centers of all the high-voltage roller electrode rotating shafts, the radius of the high-voltage roller electrode is equal to that of a driving wheel of the motor, the radius of a roller is R, the radius of the rotating shaft is R, a transmission film 13 is firstly sleeved on the high-voltage roller electrode 17 and the motor 15 shaft sleeve, the position of the high-voltage roller electrode 17 in a sealed box body 14 is fixed, the position of the motor 15 can move horizontally, the motor is moved to be tightened to the transmission film 13, if a belt is loosened in the operation process, the motor is moved to be tightened to the transmission film, and then the tight connection of the transmission film, the motor shaft sleeve and the high-voltage roller electrode is.
The spectrum detection unit is used for detecting the relative spectral intensity of the specific active species generated by the discharge; the programmable AC/DC power supply is used for setting the input voltage of the PDM high-voltage excitation power supply and the power of the whole system; the PDM (power density modulation) high-voltage excitation power supply is used as an excitation power supply of the hydrogen peroxide generator, and the power supply power density, the voltage and the discharge intensity of the PDM high-voltage excitation power supply can be adjusted, so that the power supply condition of the reactor is changed along with the working mode of the PDM high-voltage excitation power supply; the auxiliary power supply mainly supplies power to the motor transmission unit; the hydrogen peroxide collecting unit adopts a collecting tank for collection, the collected hydrogen peroxide has low purity, and high-concentration hydrogen peroxide is obtained through a series of enrichment and purification processes; the gas recovery unit pressurizes the incompletely reacted gas to the air pump 7 through the compressor 19 through the gas outlet 20 and the circulating pipeline 9, so that the incompletely reacted gas is introduced into the device again for recycling, and the production cost is reduced.
The connection relationship among the parts is as follows: the gas inlet unit and the water supply unit are combined into one path, and oxygen gas passing through the gas inlet unit and water provided by the water supply unit are mixed in the water mist generating unit to form water mist jet flow which enters the transmission and discharge unit; the water mist generating unit and the transmission and discharge unit jointly form a hydrogen peroxide generating unit, and the hydrogen peroxide collecting unit is connected with the hydrogen peroxide generating unit; the auxiliary power supply supplies power to the motor driving unit, the motor control unit is connected with the motor driving unit, and the motor driving unit is connected with the transmission and discharge unit; the hydrogen peroxide generating unit is connected with the gas recovery unit, and the gas recovery unit is connected with the gas inlet unit; the auxiliary power supply is connected with a programmable AC/DC power supply, the programmable AC/DC power supply is connected with a PDM high-voltage excitation power supply, and the PDM high-voltage excitation power supply is connected with a DBD unit of the transmission and discharge unit.
As shown in fig. 2, the whole device is accommodated in the sealed box body 14 to perform a sealing function, the sealed box body 14 is provided with an air outlet and a water outlet 10, and the material can be plastic, organic glass and other insulating materials;
the DBD unit is a DBD reactor which is composed of a high-voltage roller electrode and a strip-shaped low-voltage electrode, the specific connection structure is shown in figure 3, the negative electrode of a PDM high-voltage excitation power supply is connected with a strip-shaped low-voltage electrode 16 of the DBD reactor, the positive electrode of the PDM high-voltage excitation power supply is connected with a high-voltage roller electrode 17 of the DBD reactor, an insulating sleeve is sleeved on the high-voltage roller electrode to serve as a dielectric discharge layer 11, the material can be polytetrafluoroethylene, rubber and the like, and the length of the high-voltage roller electrode is S. The high-voltage roller electrode and the strip-shaped low-voltage electrode are both made of stainless steel materials. When the transmission film carrying the water film passes through the discharge gap, the two electrodes discharge to generate hydrogen peroxide.
The water mist generating unit is an atomizing nozzle 5, the atomizing nozzle comprises a nozzle base, a fixing screw cap and a nozzle, the nozzle is arranged on the nozzle base through the fixing screw cap, and further, the nozzle is a fan-shaped nozzle.
The atomizing nozzle is provided with two input ends of liquid and oxygen, a liquid flowmeter 4 is arranged on the liquid input end and a water supply pipeline of a water pump of the water supply unit, and the liquid flowmeter adopts an electromagnetic flowmeter or a rotor flowmeter; and a gas flowmeter 6 is arranged on a gas supply pipeline of the oxygen input end and a gas pump of the gas inlet unit, and the gas flowmeter adopts a pore plate flowmeter, a small-flow vortex shedding flowmeter or a v-cone flowmeter with pressure compensation.
Fig. 5 is a schematic structural view of a fan-shaped atomizing nozzle, the nozzle of the present invention can adopt a GA series fan-shaped nozzle of PNR company, a unique ultra-short body design, effectively solves the installation problem of a narrow space, a uniform atomizing effect and an impact force with moderate strength can be well applied in the present invention, in addition, the present invention selects the series "1/4" standard spray amount type ", and there are a plurality of choices of engineering plastic materials besides the standard metal material in the material aspect, the present invention adopts stainless steel SUS303, stainless steel SUS316L, PVC, PP or PTFE and other materials, wherein the external dimensions are as follows: the nozzle height H was 12mm, the thread length H1 was 7mm, and WS represents a fan-shaped water mist nozzle.
FIG. 6 is a schematic view of the installation of the fan-shaped nozzle, wherein the distance H between the fan-shaped nozzle and the transmission film satisfies the following formula:
Figure BDA0001553543400000051
wherein alpha ranges from 60 DEG to 120 DEG, and S is the length of the high-voltage roller electrode.
The spectrum detection unit (8 in figure 2) is arranged 3-12mm above the transmission film 13, is horizontally spaced from the low-voltage electrodes by 10-30mm, can be arranged near any one low-voltage electrode to detect the relative spectrum intensity of hydroxyl generated in the discharge gap, and uses the relative light quantum yield of the hydroxyl to evaluate the energy efficiency ratio of the device.
The collecting tank 12 is shown in fig. 4, the whole structure of the collecting tank is a uncovered U-shaped groove, the rear plate is a scraper and is 10-30mm higher than the front plate, the scraper has an inclination of 30-75 degrees so as to scrape the hydrogen peroxide film, any side of the left side and the right side is open, the scraped hydrogen peroxide film flows into the sealed box body and flows out of a water outlet of the sealed box body for collection, the collecting tank is arranged at a position 10-30cm away from the center of the roller at the rightmost end, the scraping tip of the scraper is in good contact with the thin film, and when the attached hydrogen peroxide film passes through the scraper, the hydrogen peroxide film is scraped into the collecting tank for collection.
FIG. 7 is a typical supply waveform, T in the figure, for a PDM high voltage excitation power supplym,jFor a PDM power supply with fixed frequency, T is the power density modulation period, called power regulation period for shortm,jIs stationary. To in the figuren,jIs the discharge time in a power regulation period, and consists of a plurality of power supply periods at Tm,jWhile stationary, by changing Ton,jThe supply energy can be changed by changing the supply duration. Defining duty ratio as D ═ Ton,jAnd Tm,jThe ratio of (a) to (b).
Because the hydrogen peroxide is unstable and easy to decompose, if the treated hydrogen peroxide is repeatedly discharged, the hydrogen peroxide is decomposed, the energy efficiency ratio of the hydrogen peroxide generated by a system is reduced, and similarly, if the water on the transmission film is not subjected to discharge treatment in a power regulation period, the yield of products is reduced. The PDM power supply has the characteristics of discontinuous discharge, adjustable discharge frequency, variable number of power supply cycles and the like, and the key point of the invention is to match the relationship among the characteristics of the PDM high-voltage excitation power supply, the rotating speed of a motor and the electrode spacing and improve the energy efficiency ratio of hydrogen peroxide generation to the maximum extent.
The matching principle is as follows: the running speed of the transmission film is v, and the distance between the motor and the adjacent high-voltage roller electrode is L1The distance between adjacent high-voltage roller electrodes is L2As in fig. 2.
The length L of the transmission film to be operated in the discharge time of one power regulation periodonComprises the following steps:
Lon＝DvTm,j (1)
the length L of the transmission film to be operated in the non-discharge time of one power regulation periodoffComprises the following steps:
Loff＝(1-D)vTm,j(2)
the relationship between the angular speed omega of the motor and the rotating speed n is as follows:
Figure BDA0001553543400000052
the linear speed v of the motor rotation is as follows:
Figure BDA0001553543400000053
wherein, R is the radius of the driving wheel of the motor, and the transmission speed v of the motor is the running speed of the transmission film.
Duty ratio D, motor rotation linear speed v, and distance L between adjacent high-voltage roller electrodes2The following formula is required to be satisfied:
L2＝(2N+1)DTm,jv (5)
wherein N is a non-zero natural number.
In summary, the control unit of the motor sets the rotation linear velocity of the motor according to the formula (5) and the signal and duty ratio of the power frequency, so as to achieve the purpose of matching and efficiently generate hydrogen peroxide.
In practical application, when N is 2, the duty ratio D is 0.5, and the time T of one power regulation periodm,j10ms, 4 power-adjusting periods are needed when the film passes through the two electrodes, and the radius R of the driving wheel of the motor is 0.2mDistance L between two electrodes2When the rotation speed is 0.52m, the rotation linear speed v of the motor at the moment can be determined to be 21m/s, and the corresponding rotation speed n is 16.7r/s, namely 1000 r/min. In practical application, D can be 0.1-0.5, and the rotation speed n can be 700 r/min-1300 r/min.
The working process of the device of the invention is as follows:
checking whether a motor system works normally, and starting a motor, a motor driving unit and a motor control unit to perform pre-starting; checking whether the transmission film is loose, and if so, adjusting the tightening screw to tighten so as to ensure that the transmission film is tightly attached to the lower collecting tank scraper; the water tank is filled with water, the two valves are opened, and the air pump and the water pump are opened.
Before hydrogen peroxide is prepared, a motor system is started, when water in a water tank is uniformly sprayed onto a transmission film through an atomizing nozzle after being mixed with oxygen coming from a gas supply pipeline through a water supply pipeline, a PDM high-voltage excitation power supply is turned on to discharge, the transmission film bearing the water can become hydrogen peroxide through high-voltage discharge when a discharge gap exists, at the moment, the transmission film bearing the hydrogen peroxide is scraped into a collecting tank to be collected through the hydrogen peroxide film by a scraper when the transmission film bearing the hydrogen peroxide is tightly attached to the collecting tank below. The spectral probe is placed beside the discharge gap and is used for monitoring the spectral intensity of hydroxyl radicals and the like generated in the discharge gap.
When the device can stably run, the rotating speed of the motor and series parameters of the PDM high-voltage excitation power supply can be adjusted, the parameters of the PDM high-voltage excitation power supply, such as frequency, voltage amplitude, discharge power and the like, can be changed, the DBD (direct double-diffused metal) strength, the active free radical, ultraviolet rays, oxygen atoms and hydroxyl yield can be adjusted, and therefore the yield of hydrogen peroxide is changed. Such as: the content of oxygen atoms and hydroxyl groups is different under different discharge powers, and the yield of hydrogen peroxide and the energy efficiency ratio are completely different when the rotating speed of the transmission film is the same. The output duty ratio of the internal controller of the PDM high-voltage excitation power supply is changed, so that the discharge power of the plasma DBD is changed.
The flow of the water mist from the atomizing nozzle can be changed by changing the flow of the water supply pipeline and the air flow of the air supply pipeline. Experiments show that the thickness of a water film formed on the thin film by the water mist and the treatment time in the discharge gap influence the treatment effect. Usually, the thickness of the water film is preferably 0.1mm to 0.5mm, if the water film is too thin, the yield of hydrogen peroxide is low, and if the water film is too thick, water is thrown out of the film due to the rotation of the transmission film. With the increase of the rotation speed of the transmission film, the detention time of water molecules in the discharge gap is reduced, and the water molecules can not fully react.
The invention adopts the dielectric barrier discharge principle to prepare hydrogen peroxide, can be accompanied with a series of photochemical reactions in the discharge reaction process, can directly utilize a spectral instrument to monitor the variety change and the concentration change of various substances in the reaction process, particularly monitor the change of various substances in a reaction system caused by the change of parameters, for example, the yield of the hydrogen peroxide can be quantitatively reflected according to the relative spectral intensity of hydroxyl radicals in the discharge process, and some adjustments such as discharge parameters, the rotating speed of a motor and the thickness of a water film are carried out to improve the yield.
Fig. 8 is a process flow diagram for hydrogen peroxide preparation, which mainly includes the process flows of water mist jet, discharge treatment, product collection and purification, residual gas recovery and the like. Water and gas to be treated are introduced into a water mist generating unit in the sealed box body, water mist jet flow is generated after atomization, the water mist jet flow is uniformly brushed on a transmission film through an atomizing nozzle by a water guiding brush, and dielectric barrier discharge is carried out in an oxygen environment to generate hydrogen peroxide. In the hydrogen peroxide generation unit, the rotating speed of the motor and the electrical parameters of the PDM high-voltage excitation power supply, such as voltage amplitude, power supply frequency, duty ratio and the like, can be adjusted, and the effect of hydrogen peroxide generation of the device is different under different physical parameters. The hydrogen peroxide generated by the hydrogen peroxide generating unit is collected by the hydrogen peroxide collecting tank, the concentration of the hydrogen peroxide generated by one-time discharge is low, and enrichment, separation and purification are needed if high-concentration hydrogen peroxide is needed.
The above description is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, several modifications and variations can be made without departing from the technical principle of the present invention, and these modifications and variations should also be regarded as the protection scope of the present invention.

Claims (9)

1. The drum-type dielectric barrier discharge water mist hydrogen peroxide preparation device is characterized by comprising a sealed box body, an air inlet unit, a water supply unit, a transmission and discharge unit, a water mist generation unit, a motor driving unit, a motor control unit, a gas recovery unit, a hydrogen peroxide collection unit, a spectrum detection unit, a programmable AC/DC power supply, a PDM high-voltage excitation power supply and an auxiliary power supply; wherein, the transmission and discharge unit, the water mist generation unit, the hydrogen peroxide collection unit and the spectrum detection unit are arranged in the sealed box body; the sealed box body is provided with an air outlet and a water outlet;
the gas inlet unit consists of a gas pump, a gas source, an adjusting valve and a gas flowmeter, wherein the gas pump pumps gas with a certain flow rate from the gas source into the water mist generating unit to provide oxygen with a certain flow rate for the hydrogen peroxide preparation device; the water supply unit consists of a water tank, a water pump, an adjusting valve and a liquid flowmeter, and the water pump pumps water with a certain flow rate from the water tank to the water mist generation unit; the water mist generating unit is an atomizing nozzle and is used for generating water mist jet; the transmission and discharge unit comprises a motor transmission mechanism and a DBD unit; the motor transmission mechanism consists of a servo motor and a series of servo motor transmission mechanisms, and the DBD unit consists of a high-voltage roller electrode and a strip-shaped low-voltage electrode; the transmission and discharge unit and the water mist generation unit jointly form a hydrogen peroxide generation unit, the center of a motor shaft sleeve is collinear with the centers of all high-pressure roller electrode rotating shafts, the radius of a high-pressure roller electrode is equal to that of a motor driving wheel, a transmission film is firstly sleeved on the high-pressure roller electrode and a motor shaft sleeve, the position of the high-pressure roller electrode in a sealed box body is fixed, the motor is horizontally moved until the transmission film is tightened, a discharge gap is formed between the high-pressure roller electrode and a strip-shaped low-voltage electrode, and the water film is discharged under the action of a PDM high-voltage excitation power supply;
the spectrum detection unit is a spectrum probe and is used for detecting the relative spectral intensity of hydroxyl generated in the discharge gap; the programmable AC/DC power supply is used for setting the input voltage of the PDM high-voltage excitation power supply and the power of the whole system; the PDM high-voltage excitation power supply is an excitation power supply of a hydrogen peroxide generator; the auxiliary power supply is used for supplying power to the motor driving unit; the hydrogen peroxide collecting unit collects hydrogen peroxide by adopting a collecting tank, and the collected hydrogen peroxide needs to be subjected to a series of enrichment and purification; the gas recovery unit enables gas which is not completely reacted to enter the compressor from the gas outlet through the circulating pipeline and be pressurized to the gas pump, and therefore the gas is introduced into the device again;
the atomizing nozzle is provided with two input ends of liquid and oxygen, the liquid input end is connected with a water pump of the water supply unit through a water supply pipeline, the oxygen input end is connected with a gas pump of the gas inlet unit through a gas supply pipeline, and the oxygen passing through the gas inlet unit and the water provided by the water supply unit are mixed in the water mist generating unit to form water mist jet flow which enters the transmission and discharge unit; the collecting tank is arranged at a position which is 10-30cm away from the center of the roller at the rightmost end, and the scraper plate is tightly close to the transmission film; the thickness of a water film formed on the transmission film by the water mist is adjusted to be within the range of 0.1 mm-0.5 mm by adjusting the water flow of the water supply pipeline and the air flow of the air supply pipeline;
the spectrum probe is placed 3-12mm above the transmission film and beside any one low-voltage electrode, and the horizontal distance between the spectrum probe and the low-voltage electrode is 10-30 mm; the auxiliary power supply supplies power to the motor driving unit, the motor control unit is connected with the motor driving unit, and the motor driving unit is connected with the transmission and discharge unit; the hydrogen peroxide generating unit is connected with the gas recovery unit, and the gas recovery unit is connected with the gas inlet unit; the auxiliary power supply is connected with a programmable AC/DC power supply, and the programmable AC/DC power supply is connected with a PDM high-voltage excitation power supply; the negative electrode of the PDM high-voltage excitation power supply is connected with a strip-shaped low-voltage electrode of the DBD reactor, the positive electrode of the PDM high-voltage excitation power supply is connected with a high-voltage roller electrode of the DBD reactor, and an insulating sleeve is sleeved on the high-voltage roller electrode to serve as a dielectric layer;
the distance H between the atomizing nozzle and the transmission film satisfies the following formula:
Figure FDA0002757765150000011
wherein, the range of alpha is 60 degrees to 120 degrees, and S is the length of the high-voltage roller electrode;
the running speed v, the duty ratio D and the distance L between the adjacent high-voltage roller electrodes of the transmission film2Satisfies the following formula:
L2＝(2N+1)DTm,jv
wherein N is a non-zero natural number, Tm,jFor one period of the power density modulation,
Figure FDA0002757765150000021
Ton,jis the discharge time in one power regulation period.
2. The roller type dielectric barrier discharge water mist hydrogen peroxide preparation device according to claim 1, wherein the distance between the high-voltage roller electrode and the strip-shaped low-voltage electrode is 0.5-2.5 cm; the high-voltage roller electrode and the strip-shaped low-voltage electrode are both made of stainless steel materials.
3. The roller type dielectric barrier discharge water mist hydrogen peroxide preparation device according to claim 1, wherein the sealed box body is made of plastic or organic glass insulating material.
4. The roller type dielectric barrier discharge water mist hydrogen peroxide preparation device according to claim 1, wherein the discharge dielectric layer is made of polytetrafluoroethylene or rubber.
5. The drum-type dielectric barrier discharge water mist and hydrogen peroxide preparation device as claimed in claim 1, wherein the collecting tank is in an uncovered U-shaped groove in the whole structure, the rear plate is a scraper and 10-30mm higher than the front plate, and has an inclination of 30-75 degrees, and any side of the left side and the right side of the U-shaped groove is open, so that the scraped hydrogen peroxide flows into the sealed box body and flows out of a water outlet of the sealed box body for collection.
6. The roller type dielectric barrier discharge water mist hydrogen peroxide preparation device according to claim 1, wherein the liquid flowmeter is an electromagnetic flowmeter or a rotor flowmeter; the gas flowmeter adopts a pore plate flowmeter with pressure compensation, a small-flow vortex shedding flowmeter or a v-cone flowmeter.
7. The roller type dielectric barrier discharge water mist hydrogen peroxide preparation device according to claim 1, wherein the atomizing nozzles are GA series fan nozzles of PNR company.
8. The roller type dielectric barrier discharge water mist and hydrogen peroxide preparation device according to claim 1, wherein the duty ratio D is 0.1-0.5.
9. The roller type dielectric barrier discharge water mist hydrogen peroxide preparation device according to claim 1, wherein the yield of hydrogen peroxide is adjusted by adjusting the rotating speed of a motor and the frequency, voltage amplitude or discharge power of a PDM high-voltage excitation power supply.
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IL258383A (en) * 2018-03-26 2018-05-31 Riskin Yefim Method and device for conversion of water into hydrogen peroxide

Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4272345A (en) * 1979-08-09 1981-06-09 Leach Sam L Energy conservation technique
CN1546367A (en) * 2003-11-28 2004-11-17 大连理工大学 Method and device for directly synthesizing hydrogen peroxide at room temperature
CN102583697A (en) * 2012-03-15 2012-07-18 大连海事大学 Dielectric barrier discharge water treatment device and dielectric barrier discharge water treatment method
CN103482735A (en) * 2013-09-09 2014-01-01 河海大学常州校区 Water spray discharge air plasma jet processing device and high-voltage power source thereof
CN103693714A (en) * 2014-01-10 2014-04-02 重庆大学 High-pressure atomizing dielectric barrier discharge plasma water treatment device
CN105858617A (en) * 2016-04-08 2016-08-17 复旦大学 Device and method for preparing hydrogen peroxide by using plasma discharge
CN106794988A (en) * 2014-05-05 2017-05-31 塞尼斯有限责任公司 Purified hydrogen peroxide gas method for generation and device

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4272345A (en) * 1979-08-09 1981-06-09 Leach Sam L Energy conservation technique
CN1546367A (en) * 2003-11-28 2004-11-17 大连理工大学 Method and device for directly synthesizing hydrogen peroxide at room temperature
CN102583697A (en) * 2012-03-15 2012-07-18 大连海事大学 Dielectric barrier discharge water treatment device and dielectric barrier discharge water treatment method
CN103482735A (en) * 2013-09-09 2014-01-01 河海大学常州校区 Water spray discharge air plasma jet processing device and high-voltage power source thereof
CN103693714A (en) * 2014-01-10 2014-04-02 重庆大学 High-pressure atomizing dielectric barrier discharge plasma water treatment device
CN106794988A (en) * 2014-05-05 2017-05-31 塞尼斯有限责任公司 Purified hydrogen peroxide gas method for generation and device
CN105858617A (en) * 2016-04-08 2016-08-17 复旦大学 Device and method for preparing hydrogen peroxide by using plasma discharge

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
Review of the methods to form hydrogen peroxide in electrical discharge plasma with liquid water;Bruce R Locke,et al.;《Plasma Sources Science and Technology》;20110412;第20卷;034006 *

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