CN108238589A - Line plate dielectric barrier discharge automatic adaptation water mist synthesizes hydrogen peroxide plant and method - Google Patents
Line plate dielectric barrier discharge automatic adaptation water mist synthesizes hydrogen peroxide plant and method Download PDFInfo
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- CN108238589A CN108238589A CN201810054602.3A CN201810054602A CN108238589A CN 108238589 A CN108238589 A CN 108238589A CN 201810054602 A CN201810054602 A CN 201810054602A CN 108238589 A CN108238589 A CN 108238589A
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- C—CHEMISTRY; METALLURGY
- 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
- C01B15/027—Preparation from water
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Abstract
The invention discloses a kind of line plate dielectric barrier discharge automatic adaptation water mist synthesis hydrogen peroxide plant and methods.The present apparatus includes：Water mist generates unit, line plate dielectric barrier discharge unit, adjustable power supply unit, electric signal converting unit, data analysis control unit and gas-liquid separation unit, and line plate dielectric barrier discharge unit includes the reactor being made of babinet and line plate electrode；Several line plate electrodes for being parallel to tank floor and orthogonal line electrode and plate electrode are formed are provided in babinet；Line electrode connects the anode of power supply, and plate electrode connects the cathode of power supply.Present apparatus structure novel, obvious processing effect realize the quick function of producing hydrogen peroxide, and simultaneous reactions body product is greatly reduced, can accomplish with production with, additionally will not generation environment pollution, have broad application prospects.
Description
Technical field
The present invention relates to a kind of line plate dielectric barrier discharge automatic adaptation water mists to synthesize hydrogen peroxide plant.
Background technology
Hydrogen peroxide (H2O2) is a kind of important industrial chemicals, is widely used in association with pulp bleaching, electronics industry, at sewage
The fields such as reason, chemical synthesis.Hydrogen peroxide has oxidation, available for fabric, paper pulp, the bleaching of careless Teng's bamboo product, You Jihe
Into and Polymer Synthesizing, organic and inorganic peroxide production, electroplating industry, three-protection design, food and medicine industry etc..
The most of H in the whole world at present2O2Using anthraquinone production, with hydrogen dioxide solution production by anthraquinone process, there are complex process, reactor bodies
Long-pending big, the single process time is long, is also crushed there are catalyst, caking, anthraquinone are degraded, hydrogen imitates low, catalyst poisoning, equipment investment
The serious problems such as big and environmental pollution.Hydrogen-oxygen is directly synthesized by H using the noble-metal-supporteds catalyst such as palladium, gold2O2Have perhaps
More researchs, but the process can not get both there is highly selective with high conversion, generation such as O2Need the drawbacks such as separation.It is non-flat
Weighing apparatus plasma is widely used for material processing and field of environment protection, also has in chemical conversion and synthesis field and well should
Use prospect.With the H of nonequilibrium plasma activation hydrogen-oxygen molecule synthesis2O2Though early in the sixties in last century just it has been reported that but
Generate H2O2Yield it is very low.Since the board-like DBD reactors of plate make simply, H is produced2O2Raw material --- water mist and O2, can
It largely easily obtains, so synthesizing H with the board-like dielectric barrier discharge reactor of plate2O2It can accomplish produce in times of requiring, save into
This, be not confined to large-scale plant production, is being a kind of environmentally friendly synthesis H2O2Method.
Invention content
The technical problems to be solved by the invention are the defects of overcoming the prior art, provide a kind of line plate dielectric barrier discharge
Automatic adaptation water mist synthesizes hydrogen peroxide plant, can quickly produce hydrogen peroxide, simultaneous reactions device is small, does not pollute the environment.
In order to solve the above technical problems, the technical solution adopted by the present invention is as follows：
A kind of line plate dielectric barrier discharge automatic adaptation water mist synthesizes hydrogen peroxide plant, it is characterized in that, including：Adjustable power supply
Unit, electric signal converting unit, hydrogen peroxide generating unit and data analysis controlling unit；
The hydrogen peroxide generating unit generates unit, line plate dielectric barrier discharge unit and gas-liquid separation unit phase by water mist
Intercommunicated composition；
The water mist, which generates unit, uniformly to have one from the gas of external gas source and the input of external liquid source and liquid generation
The water mist of constant current speed；
The line plate dielectric barrier discharge unit handles the water mist production of the water mist generation unit using dielectric barrier discharge
Raw hydrogen peroxide and ozone；
The adjustable power supply unit provides high-voltage pulse excitation for line plate dielectric barrier discharge unit；
Spectrum relative intensity that the electric signal converting unit generates line plate dielectric barrier discharge unit, voltage and current
Signal is separately converted to digital signal and is input in the data analysis control unit；
The signal of the electric signal converting unit that the data analysis control unit analysis receives, analyzes unit energy
The relative quantity of dioxygen water is generated, and passes through and the adjustable power supply unit is controlled to adjust the line plate dielectric barrier discharge unit
Supply voltage, frequency and power density obtain maximum Energy Efficiency Ratio；
The water mist that the line plate dielectric barrier discharge unit exports is passed through in hydrops by the gas-liquid separation unit, by water mist
In gas-liquid separation；
Line plate dielectric barrier discharge unit includes the reactor being made of babinet and line plate electrode；It is provided in babinet several
The line plate electrode formed perpendicular to the line electrode and plate electrode of tank floor；Line electrode connects the anode of power supply, plate electrode connection
The cathode of power supply；Line electrode is more molybdenums, tungsten or nichrome wire arranged in parallel, and plate electrode includes being separately positioned on molybdenum, tungsten
Or the stainless steel substrates outside two sides of nichrome wire formation, polytetrafluoroethylene (PTFE) conduct is provided between line electrode and plate electrode
Block media, molybdenum, tungsten or nichrome wire and stainless steel substrates are as discharge electrode.
A gas-liquid control loop unit is further included, by the gas-liquid control loop unit by the data analysis control unit
Control, to inputting, the water mist generates the gas flow of unit and fluid flow is adjusted.
A gas storage unit is further included, the gas storage unit stores the gas generated after the gas-liquid separation unit work.
A liquid storage unit is further included, the liquid storage unit stores the hydrogen peroxide generated after the gas-liquid separation unit work.
The external gas source generates unit for the water mist and provides oxygen.
The data analysis control unit puts line plate dielectric impedance according to the relative spectral power that spectrometer test obtains
The discharge effect of electric unit is assessed, and the opposite quantum yield of the active material from region of discharge is calculated by following formula
Eer：
Wherein, I is the relative intensity of the emission spectrum of region of discharge, Em,jIt is the confession electric flux in Power Regulation period；
Pass through opposite quantum yield EerEvaluate the yield of active specy.
While the water mist that water mist generates unit generation passes rapidly through the gap between block media, risen using voltage pulse
Electric discharge is generated with high-voltage pulse excitation driving line plate dielectric barrier discharge unit of the fall time for nanosecond, generates electric discharge generation
Object.
Water mist generates unit and uses single or multiple ultrasonic atomizers.
Gas-liquid separation unit includes a babinet that can accommodate hydrops, and lower section sets a filler, filler in babinet
The fine-structure mesh being submerged in hydrops by one between the side wall of babinet one end separates；Water mist is entered by the entrance above babinet in babinet,
And pass through a water mist entrance being always positioned under the liquid level of hydrops and be passed through in hydrops.
A kind of small flow automatic energy adaptation water mist synthesis hydrogen peroxide method of bar array, it is characterized in that,
Water mist, which generates unit, uniformly to have a constant current from the gas of external gas source and the input of external liquid source and liquid generation
The water mist of speed；
The water mist that line plate dielectric barrier discharge unit generates unit using dielectric barrier discharge processing water mist generates hydrogen peroxide
And ozone；
Adjustable power supply unit provides high-voltage pulse excitation for line plate dielectric barrier discharge unit；
Spectrum relative intensity that electric signal converting unit generates line plate dielectric barrier discharge unit, voltage and current signal
Digital signal is separately converted to be input in the data analysis control unit；
The signal of the electric signal converting unit that the analysis of data analysis control unit receives analyzes unit energy generation
The relative quantity of dioxygen water, and pass through the power supply that the adjustable power supply unit is controlled to adjust the line plate dielectric barrier discharge unit
Voltage, frequency and power density obtain maximum Energy Efficiency Ratio；
The water mist that the line plate dielectric barrier discharge unit exports is passed through in hydrops by gas-liquid separation unit, will be in water mist
Gas-liquid separation；
Line plate dielectric barrier discharge unit includes the reactor being made of babinet and line plate electrode；It is provided in babinet several
The line plate electrode formed perpendicular to the line electrode and plate electrode of tank floor；Line electrode connects the anode of power supply, plate electrode connection
The cathode of power supply；Line electrode is more molybdenums, tungsten or nichrome wire arranged in parallel, and plate electrode includes being separately positioned on molybdenum, tungsten
Or the stainless steel substrates outside two sides of nichrome wire formation, polytetrafluoroethylene (PTFE) conduct is provided between line electrode and plate electrode
Block media, molybdenum, tungsten or nichrome wire and stainless steel substrates are as discharge electrode；
Water mist generates the water mist that unit generates and passes rapidly through gap between polytetrafluoroethylene (PTFE), risen using voltage pulse and
High-voltage pulse excitation driving line plate dielectric barrier discharge cell discharge of the fall time for nanosecond, generates discharge product.
The advantageous effect that the present invention is reached：
The present apparatus realizes the quick function of producing hydrogen peroxide, and simultaneous reactions body product is greatly reduced, can accomplish with
Production with, additionally will not generation environment pollution.Present apparatus structure novel, obvious processing effect effectively can be generated quickly simultaneously
H202 has wide utilization prospect.
Description of the drawings
Fig. 1 single unit system frame diagrams；
Fig. 2 single unit system schematic diagrames；
Fig. 3 working-flow figures；
Fig. 4 parameter processing main programs；
Fig. 5 reactor input voltage test schematic diagrams；
Fig. 6 reactor supply current test schematic diagrams；
Fig. 7 Ultraviolet sensor test schematic diagrams；
Fig. 8 water level acquisition test schematic diagrams；
Fig. 9 power supply energy balane subprograms；
Figure 10 quantum yield Energy Efficiency Ratio counting subroutines；
Figure 11 newton hill-climbing algorithm schematic diagrames；
Figure 12 line plate dielectric barrier discharge unitary reactor schematic diagrames；
Figure 13 line plate electrode structure diagrams；
Figure 14 gas-liquid separation unit structure front views；
Figure 15 gas-liquid separation unit structure right views.
Specific embodiment
The invention will be further described below in conjunction with the accompanying drawings.Following embodiment is only used for clearly illustrating the present invention
Technical solution, and be not intended to limit the protection scope of the present invention and limit the scope of the invention.
1 single unit system structure
As depicted in figs. 1 and 2, the invention mainly comprises：External gas source, external liquid source, gas-liquid control loop unit, water mist
Generate unit, line plate dielectric barrier discharge unit, adjustable power supply unit, electric signal converting unit, data analysis control unit, gas
Liquid separative element, liquid storage unit and gas storage unit.
Wherein, external gas source is connected with gas-liquid control loop unit；External liquid source generates unit with water mist and is connected；Gas storage list
Member is connected with gas-liquid control loop unit；Gas-liquid separation unit is connected with gas-liquid control loop unit；Gas-liquid control loop unit
Unit is generated with water mist to be connected；Water mist generates unit and is connected with line plate dielectric barrier discharge unit；Line plate dielectric barrier discharge list
It is first to be connected with adjustable power supply unit；Line plate dielectric barrier discharge unit is connected with electric signal converting unit；Adjustable power supply unit with
Electric signal converting unit is connected；Data analysis control unit is connected with electric signal converting unit；Gas-liquid separation unit and electric signal
Converting unit is connected；Data analysis control unit is connected with gas-liquid control loop unit；Data analysis control unit and adjustable confession
Electric unit is connected；Line plate dielectric barrier discharge unit is connected with gas-liquid separation unit；Gas-liquid separation unit is connected with liquid storage unit.
In the present apparatus, water mist is generated unit and the water mist for uniformly having certain flow rate is generated using the gas and liquid of input；
Gas-liquid control loop unit generates the gas flow and fluid flow of unit by adjusting input water mist, controls the spray stream of generation
Speed and concentration；Line plate dielectric barrier discharge unit generates hydrogen peroxide and ozone using dielectric barrier discharge discharge treatment water mist；Electricity
The spectrum relative intensity that signal conversion unit can generate OH, the voltage and current of line plate dielectric barrier discharge are converted into number
Signal；The information that data analysis control unit can occur according to electric signal converting unit, goes out unit energy according to Algorithm Analysis
The relative quantity of dioxygen water is generated, by adjusting supply voltage, frequency and power density, maximum Energy Efficiency Ratio is obtained, controls simultaneously
The switch conditions of gas-liquid valve；The water mist that line plate dielectric barrier discharge unit exports is passed through in hydrops by gas-liquid separation unit, will
Gas-liquid separation in water mist；Adjustable power supply unit provides high-voltage pulse excitation for line plate dielectric barrier discharge unit；Gas storage unit
It is responsible for the mixture of the gases such as the ozone, the oxygen that are generated after storage work；External gas source provides high-concentration oxygen for device；Liquid storage
Unit is responsible for storing the hydrogen peroxide generated after work；
Gas-liquid control loop unit includes electrode M1, M2, valve V1, valve V2, valve V3 and valve V4.
With reference to Fig. 2 and Fig. 3, electrode M1, M2, water mist generates cell operation after valve V1, V4 are opened, adjustable after waiting for 15 seconds
Power supply unit works, the water mist then generated by line plate dielectric barrier discharge cell processing, and electric signal conversion is single after processing
Member broadcasts data to data analysis control unit and data is analyzed, and analysis result carries out a condition judgment, if best
Then valve V3, V4 opens to adjust height of water level until meeting the requirements condition, and height of water level reaches requirement late gate V5 unlatchings, storage
Liquid unit collects product.Then if not optimum condition then regulates and controls power parameter by data analysis control unit feeds back to telecommunications
Number converting unit gathered data re-starts condition judgment.
2 electric signal converting units
Electric signal converting unit includes supply voltage detection circuit, supply current detection circuit, photoelectric signal transformation circuit
With water level signal conversion circuit.
2.1 voltage signals and current signal conversion
With reference to Fig. 5 and supply voltage detection circuit shown in fig. 6 and supply current detection circuit.In this part for reality
When show the operating power of current device, the present invention has detected the input voltage and electric current of power supply.
The method of measurement voltage that the present invention uses is resitstance voltage divider method, and high voltage waveform is converted into low-voltage wave
Shape is made of high-voltage arm and low-voltage arm.Input voltage VRH is added in whole device, and output voltage is then derived from low resistance R2.
By the voltage signal at R2 both ends by capacitance C1, play the role of eliminating DC component.In addition, due to circuit detection being high
Signal is pressed, occurs instantaneous high pressure spike in order to prevent by bleeder circuit, causes detection circuit short-circuit, damages component situation,
In one TVS pipe D1 of C1 rear ends parallel connection, for importing big voltage, surge power is absorbed, protects test circuit.Collected voltage
Signal carries out rectification by precise rectification circuit, then very effective to AC signal progress by real effective (RMS) conversion circuit
Value conversion.AD637, AD736 or AD737 etc. may be selected in RMS conversion chip.AC signal is become into direct current signal later,
Data analysis control unit is then input to, data analysis control unit can be the MCU of built-in ADC module, carry out signal
Processing.As shown in figure 5, R1, R2 represent the resistance of high voltage arm and low-voltage arm respectively, it is assumed that tested voltage is U, and R2 both ends are electric
It presses as UR2.According to principle of continuity of electric current：
If Fig. 6 is supply current detection circuit.In the present solution, using a current transformer come the electric discharge of sensing device
Electric current.Current transformer is the uniform close air core solenoid being wound on an annular nonmagnetic skeleton, output voltage be proportional to by
Electric current is surveyed to change with time rate.By the plane where the ground wire straight through measuring coil of DBD reactors, induction discharge electric current.
The expression formula of current transformer output voltage is：
In formula:I is tested electric current, and h is skeleton height, and N is coil turn, μ0For space permeability, Rb, Ra are respectively bone
The inside and outside diameter of frame；The voltage induced for the Weak current that Current Transformer measurement obtains is too weak, so will be to collecting
Signal is amplified processing.
In formula (2),It is a constant, is represented with mutual inductance M：
Since current transformer output voltage is directly proportional to the differential of tested electric current, so the voltage exported to it is needed to believe
Number carry out Integral Processing can just obtain the output voltage directly proportional to loop current.The voltage signal of current transformer output first passes through
It crosses a voltage follower U2 and carries out subsequent processing again, the effect of voltage follower U2 is to reduce subsequent conditioning circuit to acquiring signal
Interference.In addition, due to the transformer induced voltage signal very little arrived, the voltage signal output it first passes through an amplification
Circuit U 3 carries out the amplification of signal, using integrating circuit U4.Signal has been converted to one and sensing after integrating circuit U4
The proportional voltage signal of the current signal that arrives, before MCU is transferred signals to, collected voltage signal is by accurate whole
Current circuit carries out rectification, then carries out RMS conversion to AC signal by real effective (RMS) conversion circuit.Real effective
AD637, AD736 or AD737 etc. may be selected in conversion chip.So the workflow of discharge current testing circuit is：First use electric current
Current signal is converted into voltage signal by the discharge current in transformer induced system, then by voltage follower U2 into
Row isolation, is in next step amplified voltage signal by U3, and by precise rectification circuit the signal of amplification is carried out rectification, then lead to
It crosses real effective (RMS) conversion circuit and RMS conversion is carried out to AC signal.AC signal is become into direct current signal later
Data analysis control unit is input to, data analysis control unit can be the MCU of built-in ADC module, and data are acquired
And processing.
The circuit that integrating circuit U4 is formed with peripheral devices in figure plays what current transformer output voltage was integrated
Effect
The voltage signal of current transformer output is after integrating circuit, electric current that obtained voltage signal and its sense
Signal is in linear function relationship.This signal is sent in MCU, the relationship of sensing electric current and voltage can be set, can be put
Discharge current in electrical circuit.
2.2 photoelectric signal transformation circuits
With reference to shown in Fig. 7, in order to measure the activated species of region of discharge and concentration, the present invention utilizes Ultraviolet sensor
Spectral intensity in the active matter of 71 detection reaction device region of discharges, is converted into electric signal by optical signalling, uses Ultraviolet sensor
The voltage signal of 71 outputs represents the relative concentration that active specy generates.Due to the active matter generated during dielectric barrier discharge
Kind meeting sends out the spectrum of multi-wavelength, and the spectrum of OH is primarily upon in the present invention, therefore placed before Ultraviolet sensor 71
Optical filter 72 tentatively filters out spectrum.Optical filter 72 uses ultraviolet bandpass-type optical filter, and ultraviolet bandpass-type optical filter can be with
ET313/25BP (centre wavelength 313nm, bandwidth 25nm), ET325/20BP (centre wavelength 325nm, bandwidth 20nm) are selected,
XBPA310, ZBPA310 (centre wavelength 310nm, bandwidth 10nm).The voltage signal of Ultraviolet sensor is passed through into voltage follower
U7 is isolated, due to Ultraviolet sensor output signal frequency it is higher, so voltage follower U7 using the response time compared with
Fast current mode operational amplifier is used as voltage follower, and the effect of voltage follower is identical with described in Fig. 5 herein.Due to rear
The input impedance of grade operational amplifier is infinitely great, causes the accumulation of charge, it is therefore desirable to the indirect ground resistance with the earth
Release channels of the R12 as energy, high-voltage oscillation, ground resistance R12 are connect with voltage follower U7 output terminals in order to prevent
Resistance R13 is matched, and resistance value is equal.Voltage follower U7 output terminals are connect through feedback resistance R11 with its inverting input.It is purple
The voltage signal of outer sensor output contains DC component, if it be likely to result in directly by the amplifying circuit of rear class
Amplify saturation distortion, therefore use the DC component in capacitance C6 isolation Ultraviolet sensor output signals.Reverse phase is used in next step
Amplifying circuit U8 is amplified the signal amplitude of acquirement.Later by rectification circuit to AC signal is become direct current signal,
RMS conversion is carried out to AC signal by real effective (RMS) conversion circuit again.RMS conversion chip may be selected
AD637, AD736 or AD737 etc..Data analysis control unit is input a signal into later, and data analysis control unit can be interior
The MCU of ADC module is put, data are acquired and are shown.
The corresponding equation of amplifying circuit is：
In formula, V represents that the voltage signal of Ultraviolet sensor output passes through the voltage value of voltage follower, and U8o represents amplification
The voltage value of circuit output, R11For the resistance value of feedback resistance R11, R12Resistance value for ground resistance R12.
2.3 water level signal conversion circuits
As shown in Fig. 8 and Figure 14, in order to measure whether water level reaches expected requirement, the present invention is using in water level acquisition module
Electrode 81 in gas-liquid separation unit water level carry out data acquisition, water level information is converted into electric signal.Voltage comparator
U9 using dual power supply work, when water level meets the requirements, data analysis control unit or MCU receive high level, when water level not
When meeting the requirements, data analysis control unit or MCU receive low level.
3 data analysis control units
3.1 unit
MCU can select STC12C, STM32, STC89 series monolithic of STC Corporation.It recommends and is encapsulated as SOP-
20, microcontroller built-in 8 ADC and universaling I/O port, speed can reach 100kHZ, and 8 tunnel ADC module may be used as button inspection
Survey, liquid pump Rotating speed measring, flow detection, pressure detecting and electromagnetic valve switch detection etc..Electric signal converting unit can be converted
Voltage, electric current, water level and the photosignal crossed are transmitted to the A/D mouths of MCU, and MCU is whole according to the signal control collected later
The operation of a system.
3.2 data analysis
Data analysis control unit according to the relative spectral power that spectrometer test obtains to the discharge effects of DBD devices into
Row assessment.It is represented with the relative spectral power divided by a Power Regulation period consumption energy of hydroxyl radical free radical in region of discharge (OH)
With respect to quantum yield Energy Efficiency Ratio Eer.Therefore, the opposite quantum yield Energy Efficiency Ratio of the active material from region of discharge can be with
It is obtained by following formula：
Wherein I is the relative intensity of the emission spectrum of region of discharge, Em,jIt is the confession electric flux in Power Regulation period.Plasma
The relative concentration of active material is proportionate with the relative intensity of its emission spectrum in region.It therefore, can be by using opposite
Quantum yield EerTo evaluate the yield of active specy.
First, the excitation power supply of DBD is adjusted to PDM powering modes, and discharging condition is set under PDM patterns, including PDM electricity
Source supply voltage, the frequency in Power Regulation period, frequency of supply and power density.Single confession is calculated by the electric discharge terminal found
Then electric periodical energy average value Ed, a obtain always supplying electric flux according to the Power Regulation period and power-up period accumulation calculating that measure
ET.Using the relative spectral power of active specy in spectrometer measurement region of discharge, phase is carried out eventually by newton hill-climbing algorithm
Quantum yield Energy Efficiency Ratio is assessed, so that it is determined that optimum reaction condition.
Such as Fig. 4, parameter processing program is that the data for reading and preserving are carried out calculation processing, and electricity is detected by supply voltage
Road, supply current detection circuit, power supply energy balane subprogram, equivalent parameters counting subroutine, the sub- journey of quantum yield Energy Efficiency Ratio
Sequence respectively obtains supply voltage peak-to-peak value, effective discharge time, micro discharge mean intensity, electric energy is always supplied in system operation time
Amount, single power-up period average energy, reactor equivalent capacity, quantum yield Energy Efficiency Ratio.
Fig. 9 is power supply energy balane subprogram, which obtains the energy of the single power-up period in device operational process
Average value supplies electric flux with total.According to the data that last point of small circuit part obtains, the Li Saru of signal period is carried out
Figure reconstruction.Since in supply current test circuit, current transformer output voltage is directly proportional to the differential of tested electric current, so
The voltage signal exported to it is needed to carry out Integral Processing with regard to the output voltage directly proportional to loop current can be obtained.Due to Lee's Sa
If figure is the curve that two orthogonal vectors are synthesized when doing periodic swinging, the vibration frequency of two vectors is identical, Neng Gouhe
Into the figure of closing.But in vibration processes, the mould of vector is to be not fixed, therefore the feature size of each periods synthesizer has
Difference.When being powered energy balane, need to calculate the area of each period lissajous figures, therefore to carry out figure
The reconstruct of shape simultaneously detaches each period, establishes the rule of image separation.Restructuring procedure is as follows：
With " input voltage " for abscissa data, " supply voltage " is ordinate data, carries out figure reconstruction.It obtains at this time
Be lissajous figures that all power-up periods stack.It is single lissajous figures since single power-up period is corresponding,
It need to carry out signal period image separation.Establishing the data decimation ambit rule of single power-up period lissajous figures reconstruct is：
When drawing Lie groupoid, the voltage applied is selected to rise to the time of zero two consecutive points as a cycle.
After separation reconstruct is carried out to the lissajous figures of single power-up period, the lissajous figures of reconstruct are powered
The integral and calculating of voltage and integral voltage obtains the area Sd, i of lissajous figures.According to the area of Lee's Sa such as, with reference to what is obtained
The confession electric flux of the ENERGY E d, i of single power-up period, power-up period the number ndm, j in a Power Regulation period and Power Regulation period
Em,j.It is added up later according to power-up period number Non, t total in run time to the energy of each power-up period, is
Electric flux is always supplied in run time of uniting.Output is carried out to Ed, a and ET to show.
Figure 10 is opposite quantum yield Energy Efficiency Ratio EerCounting subroutine passes through according in " power supply energy process subprogram "
Handle the power supply ENERGY E in the Power Regulation period of storagem,jOpposite quantum yield Energy Efficiency Ratio E is calculated in dataer, and to result into
Row display output.
It after the step of passing through front obtains discharge parameter, and then is combined with newton hill-climbing algorithm, devises optimal discharge
Effect evaluation method.According to the changing rule of quantum yield, the corresponding discharge parameter in optimal discharge effect is obtained.According to
Newton hill-climbing algorithm finds out best opposite quantum yield Energy Efficiency Ratio EerCorresponding discharging condition determines corresponding parameter area.
It is the XX-Eer figures of climbing hill algorithm as shown in figure 11, horizontal axis represents the power supply ENERGY E in a Power Regulation periodm,j, indulge
Axis represents opposite quantum yield Eer.Climbing hill algorithm is also known as perturbation observation method, passes through putting for constantly regulate exoelectrical reaction system
Electric condition generates E to compare DBD before and after adjustmenterSituation of change, discharging condition is adjusted further according to situation of change, including that can compile
The output voltage of journey AC/DC power supplys, the supply voltage of PDM power supplys, the parameter for electric flux, make discharge reactor be operated in most preferably
Near Energy Efficiency Ratio.It is as follows that climbing hill algorithm specific works situation can be analyzed：
(1) add a disturbance variable in A points, such as change the E for for electric flux, making reactorerReach B points；
(2) improved before detecting causes the opposite quantum yield Energy Efficiency Ratio of reactor to increase for electric flux, continues former
The direction come increases disturbance variable, and reactor is made to be operated in C points；
(3) continue original direction and add disturbance variable, reactor is made to be operated in M points；
(4) continue original direction and add disturbance variable, reactor is made to be operated in D points；
(5) disturbance variable before detecting at this time causes the opposite quantum yield Energy Efficiency Ratio of reactor to reduce, and changes
Direction originally adds disturbance variable, makes the E of reactorerAgain reach M points；
(6) continue original direction and add disturbance variable, reactor is made to be operated in C points；
(7) finally, reactor is in C points, M points, and D points fluctuate between three operating points.
Disturbance variable in algorithm is chosen：Supply voltage, the frequency in Power Regulation period, frequency of supply and power density, make
Best opposite quantum yield Energy Efficiency Ratio can be determined in this way, and can obtain corresponding discharging condition, because
This can determine optimal discharge parameter regulation range.
In newton hill-climbing algorithm, M points are not necessarily E according to determined by the step-length of disturbance variableerPeak, true
After having determined optimal parameter adjustable range C to D, the step-length of disturbance variable is reset with optimum seeking method, according to the following steps
Find out peak：
(1) in (C, M) section Nei Qu midpoints P1, (M, D) section Nei Qu midpoints P2；
(2) when the corresponding functional values of P1 functional value corresponding more than P2, with respect to the maximum of quantum yield Energy Efficiency Ratio
In (P1, M) section, the section of (M, P2) is cast out；
(3) conversely, maximum is in (M, P2) section, cast out (P1, M) section；
(4) when the corresponding functional values of P1 and P2 are equal, maximum in the range of (P1, P2), cast out (C, P1) and (P2,
D section)；(5) midpoint is taken again in remaining section, find P3, P4, continue to change in a manner of step (1) to (4)
In generation, calculates；Until remaining interval range is less than setting valueWhen, algorithm terminates.
3.3 control device
The equipment that can be controlled has the high-voltage pulse power source of gas-liquid valve, adjustable power supply unit, wherein equipment control gas
These parameters of the switch of the fluid valve and supply voltage of high-voltage pulse power source, duty ratio and frequency,
4 line plate dielectric barrier discharge units
Line plate dielectric barrier discharge cellular system is as shown in figure 12, including babinet, line plate electrode.The top of babinet and water mist
The gas outlet for generating unit is connected, and the lower section of babinet is connected with the air inlet of gas-liquid separation unit, if being provided in babinet
The dry line plate electrode being made of line electrode and plate electrode perpendicular to tank floor.Line electrode connects the anode of power supply, plate electrode
Connect power supply cathode, structure is as shown in figure 13, line electrode be molybdenum arranged in parallel, tungsten or nichrome wire 133,
Plate electrode includes the stainless steel substrates 130 being separately positioned on outside two sides that molybdenum, tungsten or nichrome wire are formed, line
Polytetrafluoroethylene (PTFE) is provided between electrode and plate electrode as block media 131, molybdenum, tungsten or nichrome wire 133 and stainless steel
Piece 130 is used as discharge electrode.Polytetrafluoroethylene (PTFE) is tightly attached on 130 medial surface of stainless steel substrates, polytetrafluoroethylene (PTFE) and molybdenum, tungsten or nickel chromium triangle
The space for accommodating air is formed between B alloy wire 133.The region of discharge of the reactor, the gas flow rate in channel can use gas
The cross-sectional area of flow and discharge channel is calculated, and formula can be expressed as：
Wherein v refers to the gas flow rate in channel, and Q represents gas flow (LMin-1), and Ac is the transversal of discharge channel
Area.D, L is the length and width in discharge channel section.
Ac=DL (9)
The optimum flow rate of gas between 2.0-3.5m/s,
It is anti-using high voltage power supply excitation DBD when the water mist of certain flow rate enters this element when under the action of previous unit
Device is answered to discharge, for discharge voltage between 5KV-30KV, reactor can generate the free radical of a large amount of strong oxidizing properties when discharging, can
It synthesizes a large amount of H202 and is combined with water mist, form hydrogen peroxide.
The interelectrode minimum arcing distance d of DBD, atmospheric pressure p and breakdown voltage VBBetween follow Paschen (Paschen '
SLaw) law, i.e.,：
A and B in formula are constant, VBFor breakdown voltage, p is atmospheric pressure, discharging gaps of the d between dielectric layer, and r is
Secondary electron yield；F (pd) represents the Paschen function using pd as variable.Water mist generates the water for the certain flow rate that unit generates
Mist passes rapidly through the gap between quartz medium layer.Use the high-voltage pulse that voltage pulse rising and falling time is nanosecond
Power drives dielectric barrier discharge structure.Under the action of high reduction electric field, make ionization generate electronics occur accelerate, collision and
The chain reactions such as ionization, cause avalanche effect, finally generate dielectric barrier discharge.Between the atom of water mist or molecule and electronics
Collision, is collided between atom and atom, and light and the interaction of atom or molecule etc. can ionize, and generation electronics-from
Son is right；Electronics or ion collision exhaust gas.When dielectric barrier discharge occurs in the offgas as a result, various electric discharges can be generated
Product, including high energy electron, negative ions, free radical, ozone (O3) and ultraviolet light.
DBD key reactions include electron collision, photodissociation and secondary response.Averaged electron energy is in 1- in DBD plasmas
10eV or so.Main reaction is the collision of the electronics under different electron energies：
e+O2→O(1D)+O(1D)+e(Te=0-5eV) (11)
e+H2O→e+H+OH(Te=1-2eV) (12)
DBD plasma generation process is dissociated along with secondary response, H2O and O2 molecules：
O(1D)+H2O→2OH (13)
N2 *+O2→N2+2O(1D) (14)
In heating region, excitation state O energy and N2Molecule reacts, some O energy and O2Generate O3, equation is as follows：
O2+O+M→O3+M (15)
In addition, in the environment of high intensity ultraviolet radiation, mainly photolysis is as follows：
H2O+hv → OH+H (λ=145-246nm) (16)
O2+hv→O+O(1D) (λ=200-220nm) (17)
O3+hv→O2+O(1D)(λ≤320nm) (18)
And the OH generated in the above process be combined with each other, and generates the main matter H of hydrogen peroxide202, equation is as follows：
OH+OH→H2O2 (19)
5 water mists generate unit
Single ultrasonic atomizer generates fogdrop diameter and can be calculated with following formula：
D is liquid-drop diameter in formula；γ is the surface tension of atomized liquid；ρ is fluid density；f1For ultrasonic rate.Water mist
Liquid
Particle diameter is 0.1um-20.0um.
Water mist generates unit and single or multiple ultrasonic atomizers can be used in the design of the present apparatus, to meet small-large flow
Demand.
6 gas-liquid separation units
With reference to shown in Figure 14 and Figure 15, water mist 141 is entered by the air inlet 142 being located above in gas-liquid separation unit, is led to
Enter lower section hydrops, bubble is divided by stainless steel fine-structure mesh 143, it is made to be come into full contact with hydrops, reaches the liquid made in water mist
The fully fused purpose with hydrops, while gas moves upwards due to density is much smaller than liquid, is mixed into overhead gas.Simultaneously because
There is filler 144 in gas-liquid separation unit, 144 height of filler is higher than liquid of inner and outer air pressure when identical in water mist entrance
Outer liquid level, therefore ensure water mist entrance always under the liquid level of liquid.
For the stainless steel fine-structure mesh used, network interface diameter is in the range of 0.1mm-2.0mm.
7 phase feeds choose principle
The present apparatus chooses oxygen as phase feed, due to that, containing most of nitrogen, can be produced in discharge process in air
Raw NO, NO2 detrimental activity substance, reaction mechanism are as follows：
Key reaction includes electron collision, photodissociation and secondary response in discharge process.Electronics is averaged in discharge plasma
Energy is in 1-10eV or so.Main reaction is the collision of the electronics under different electron energies：
e+O2→O(1D)+O(1D)+e(Te=0-5eV) (21)
e+H2O→e+H+OH(Te=1-2eV) (22)
Discharge plasma generates process along with secondary response, H2O and O2Molecule is dissociated：
O(1D)+H2O→2OH (24)
N2 *+O2→N2+2O(1D) (25)
In heating region, excitation state O energy and N2Molecule reacts, and N is reacted with the OH generated.Some O energy and O2Generation
O3, some O3NO is generated with NO2, equation is as follows：
O(1D)+N2→NO+N (26)
N+OH→NO+H (27)
O2+O+M→O3+M (28)
NO+O3→NO2+O2 (29)
In addition, in the environment of high intensity ultraviolet radiation, mainly photolysis is as follows：
H2O+hv → OH+H (λ=145-246nm) (30)
O3+hv→O2+O(1D)(λ≤320nm) (31)
NO2+hv→NO+O2(λ≤420nm) (32)
NO2+hv→N2+O(1D)(λ≤337nm) (33)
NO2Formation HNO soluble in water3, contain NO in solution3, make solution into acidity, and H2O2Into faintly acid, will inhibit
H2O2Generation, reduce its yield.
8 liquid phase feeds choose principle
The present apparatus produces H by gas-liquid mixed atomizing type2O2, raw material is NaCl solution and O2, wherein it is molten to choose NaCl
Liquid is higher than NaOH alkaline solution yields as liquid phase generation raw material, because of H2O2It is weak acid, is reacted in concentrated NaOH solution with OH-
Generate HO2, reaction equation is as follows：
H2O2+OH-→HO2 -+H2O (34)
Therefore, generated H2O2It is consumed by being reacted with NaOH, leads to low-down H2O2Yield.
So the present apparatus is conducive to H using neutral liquids such as NaCl solution or water2O2It generates.
The above is only the preferred embodiment of the present invention, it is noted that for the ordinary skill people of the art
For member, without departing from the technical principles of the invention, several improvement and deformation can also be made, these are improved and deformation
Also it should be regarded as protection scope of the present invention.
Claims (10)
1. a kind of line plate dielectric barrier discharge automatic adaptation water mist synthesizes hydrogen peroxide plant, it is characterized in that, including：Adjustable power supply is single
Member, electric signal converting unit, hydrogen peroxide generating unit and data analysis controlling unit；
The hydrogen peroxide generating unit generates unit by water mist, line plate dielectric barrier discharge unit is mutually interconnected with gas-liquid separation unit
It is logical to form；
The water mist, which generates unit, uniformly to have a constant current from the gas of external gas source and the input of external liquid source and liquid generation
The water mist of speed；
The water mist generation that the line plate dielectric barrier discharge unit handles the water mist generation unit using dielectric barrier discharge is double
Oxygen water and ozone；
The adjustable power supply unit provides high-voltage pulse excitation for line plate dielectric barrier discharge unit；
Spectrum relative intensity that the electric signal converting unit generates line plate dielectric barrier discharge unit, voltage and current signal
Digital signal is separately converted to be input in the data analysis control unit；
The signal of the electric signal converting unit that the data analysis control unit analysis receives, analyzes unit energy generation
The relative quantity of dioxygen water, and pass through the power supply that the adjustable power supply unit is controlled to adjust the line plate dielectric barrier discharge unit
Voltage, frequency and power density obtain maximum Energy Efficiency Ratio；
The water mist that the line plate dielectric barrier discharge unit exports is passed through in hydrops by the gas-liquid separation unit, will be in water mist
Gas-liquid separation；
Line plate dielectric barrier discharge unit includes the reactor being made of babinet and line plate electrode；It is provided in babinet several vertical
In the line plate electrode that the line electrode and plate electrode of tank floor are formed；Line electrode connects the anode of power supply, plate electrode connection power supply
Cathode；Line electrode is more molybdenums, tungsten or nichrome wire arranged in parallel, and plate electrode includes being separately positioned on molybdenum, tungsten or nickel
The stainless steel substrates outside two sides that chromium alloy wire is formed are provided with polytetrafluoroethylene (PTFE) as blocking between line electrode and plate electrode
Medium, molybdenum, tungsten or nichrome wire and stainless steel substrates are as discharge electrode.
2. line plate dielectric barrier discharge automatic adaptation water mist according to claim 1 synthesizes hydrogen peroxide plant, it is characterized in that,
A gas-liquid control loop unit is further included, by the gas-liquid control loop unit by the data analysis control unit control
System, to inputting, the water mist generates the gas flow of unit and fluid flow is adjusted.
3. line plate dielectric barrier discharge automatic adaptation water mist according to claim 1 synthesizes hydrogen peroxide plant, it is characterized in that,
A gas storage unit is further included, the gas storage unit stores the gas generated after the gas-liquid separation unit work.
4. line plate dielectric barrier discharge automatic adaptation water mist according to claim 1 synthesizes hydrogen peroxide plant, it is characterized in that,
A liquid storage unit is further included, the liquid storage unit stores the hydrogen peroxide generated after the gas-liquid separation unit work.
5. line plate dielectric barrier discharge automatic adaptation water mist according to claim 1 synthesizes hydrogen peroxide plant, it is characterized in that,
The external gas source generates unit for the water mist and provides oxygen.
6. line plate dielectric barrier discharge automatic adaptation water mist according to claim 1 synthesizes hydrogen peroxide plant, it is characterized in that,
The relative spectral power that the data analysis control unit is obtained according to spectrometer test is to line plate dielectric barrier discharge unit
Discharge effect is assessed, and the opposite quantum yield E of the active material from region of discharge is calculated by following formulaer：
Wherein, I is the relative intensity of the emission spectrum of region of discharge, Em,jIt is the confession electric flux in Power Regulation period；
Pass through opposite quantum yield EerEvaluate the yield of active specy.
7. line plate dielectric barrier discharge automatic adaptation water mist according to claim 1 synthesizes hydrogen peroxide plant, it is characterized in that,
Water mist generates water mist that unit generates while pass rapidly through the gap between block media, during using voltage pulse raising and lowering
Between for the high-voltage pulse excitation driving line plate dielectric barrier discharge unit of nanosecond generate electric discharge, generate discharge product.
8. line plate dielectric barrier discharge automatic adaptation water mist according to claim 1 synthesizes hydrogen peroxide plant, it is characterized in that,
Water mist generates unit and uses single or multiple ultrasonic atomizers.
9. line plate dielectric barrier discharge automatic adaptation water mist according to claim 1 synthesizes hydrogen peroxide plant, it is characterized in that,
Gas-liquid separation unit includes a babinet that can accommodate hydrops, and lower section sets a filler, filler and babinet one in babinet
The fine-structure mesh being submerged in hydrops by one between the wall of end side separates；Water mist is entered by the entrance above babinet in babinet, and passes through one
The water mist entrance under the liquid level of hydrops is always positioned to be passed through in hydrops.
10. a kind of small flow automatic energy adaptation water mist synthesis hydrogen peroxide method of bar array, it is characterized in that,
Water mist, which generates unit, uniformly to have certain flow rate from the gas of external gas source and the input of external liquid source and liquid generation
Water mist；
The water mist that line plate dielectric barrier discharge unit generates unit using dielectric barrier discharge processing water mist generates hydrogen peroxide and smelly
Oxygen；
Adjustable power supply unit provides high-voltage pulse excitation for line plate dielectric barrier discharge unit；
Spectrum relative intensity that electric signal converting unit generates line plate dielectric barrier discharge unit, voltage and current signal difference
Digital signal is converted into be input in the data analysis control unit；
The signal of the electric signal converting unit that the analysis of data analysis control unit receives analyzes unit energy and generates dioxygen
The relative quantity of water, and pass through the power supply electricity that the adjustable power supply unit is controlled to adjust the line plate dielectric barrier discharge unit
Pressure, frequency and power density obtain maximum Energy Efficiency Ratio；
The water mist that the line plate dielectric barrier discharge unit exports is passed through in hydrops by gas-liquid separation unit, by the gas-liquid in water mist
Separation；
Line plate dielectric barrier discharge unit includes the reactor being made of babinet and line plate electrode；It is provided in babinet several vertical
In the line plate electrode that the line electrode and plate electrode of tank floor are formed；Line electrode connects the anode of power supply, plate electrode connection power supply
Cathode；Line electrode is more molybdenums, tungsten or nichrome wire arranged in parallel, and plate electrode includes being separately positioned on molybdenum, tungsten or nickel
The stainless steel substrates outside two sides that chromium alloy wire is formed are provided with polytetrafluoroethylene (PTFE) as blocking between line electrode and plate electrode
Medium, molybdenum, tungsten or nichrome wire and stainless steel substrates are as discharge electrode；
The water mist that water mist generation unit generates passes rapidly through the gap between polytetrafluoroethylene (PTFE), using voltage pulse raising and lowering
High-voltage pulse excitation driving line plate dielectric barrier discharge cell discharge of the time for nanosecond, generates discharge product.
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103496761A (en) * | 2013-09-09 | 2014-01-08 | 河海大学常州校区 | Plasma-supersonic wave combined water processing apparatus and process flow thereof |
| CN103523856A (en) * | 2013-09-09 | 2014-01-22 | 河海大学常州校区 | Water mist discharge and ultrasound synergetic degradation wastewater treatment device and running method thereof |
| CN105198035A (en) * | 2015-08-13 | 2015-12-30 | 河海大学常州校区 | Variable-frequency power ultrasonic control underwater dense bubble dielectric barrier discharge reactor |
| CN105858617A (en) * | 2016-04-08 | 2016-08-17 | 复旦大学 | Device and method for preparing hydrogen peroxide by using plasma discharge |
-
2018
- 2018-01-19 CN CN201810054602.3A patent/CN108238589A/en not_active Withdrawn
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103496761A (en) * | 2013-09-09 | 2014-01-08 | 河海大学常州校区 | Plasma-supersonic wave combined water processing apparatus and process flow thereof |
| CN103523856A (en) * | 2013-09-09 | 2014-01-22 | 河海大学常州校区 | Water mist discharge and ultrasound synergetic degradation wastewater treatment device and running method thereof |
| CN105198035A (en) * | 2015-08-13 | 2015-12-30 | 河海大学常州校区 | Variable-frequency power ultrasonic control underwater dense bubble dielectric barrier discharge reactor |
| CN105858617A (en) * | 2016-04-08 | 2016-08-17 | 复旦大学 | Device and method for preparing hydrogen peroxide by using plasma discharge |
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