CN106474919B - Modular unit of the large area along face DBD synergistic catalyst removing NOx - Google Patents

Modular unit of the large area along face DBD synergistic catalyst removing NOx Download PDF

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Publication number
CN106474919B
CN106474919B CN201610939904.XA CN201610939904A CN106474919B CN 106474919 B CN106474919 B CN 106474919B CN 201610939904 A CN201610939904 A CN 201610939904A CN 106474919 B CN106474919 B CN 106474919B
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catalyst
gas
system
line style
electrode
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CN201610939904.XA
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CN106474919A (en
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王文春
赵紫璐
杨德正
袁皓
张丽
王森
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大连理工大学
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Abstract

Large area removes NO along face DBD synergistic catalystxModular unit, belong to plasma technique application field.It is inserted in the line style ground electrode dead earthing of medium tube, array line style high-field electrode is embedded, and forms creeping discharge region.Array line-line electrode (1) merging exoelectrical reaction room (2), forms modularization electric discharge-removing means, and synergistic catalyst removes NOx.Discharge plasma is motivated by power-supply system (4) and is generated, and guarantees the power output of power supply using matching system (3).Inline diagnosis, the NO provided using gas detecting system (6) air supply system (5) are carried out along face DBD to the large area of generation using electricity diagnostic system (7) and optical diagnostic system (8)xTreatment effect is diagnosed, and is characterized using Catalyst Characterization System (9) to catalyst, and study the Synergistic Mechanisms of plasma and catalyst.

Description

Large area removes NO along face DBD synergistic catalystxModular unit

Technical field

The invention belongs to plasma technique application fields.More particularly to it is a kind of utilize array line-line electrode, by Match system guarantees the power-supply system excitation of power output, generates large area surface discharge plasma, and synergistic catalyst is handled NOxModularization discharge-remove experimental provision.

Technical background

In recent years, catalytic eliminating NOxNo matter in terms of laboratory research, or in terms of technical application, all obtain wide General concern.For traditional catalytic eliminating method usually to catalyst requirement with higher, material requested is expensive, and device is complicated, And in practical applications, the problems such as how preventing catalyst poisoning, there is still a need for more perfect solutions.Plasma body cooperative catalysis Agent removes NOxTechnology has good effect for removing gaseous pollutant since there are a large amount of active species for discharge plasma Fruit, and structure is simple, installation cost is low.Simultaneously as the desorption of active specy, same for catalyst poisoning phenomenon There is good improvement.The device of plasma body cooperative catalyst removal gaseous pollutant, main wired-cartridge type, filling bed type etc., Belong to space discharging structure.

Surface discharge plasma has in terms of the control of aerospace airflow on surface, gas-solid-liquid tri-state It is widely used.Especially surface dielectric barrier discharge, traditional structure be, dielectric-slab be clipped in high-field electrode and ground electrode it Between, plane discharge plasma is generated in the two sides of dielectric-slab.However, with the development of plasma technology with application background Increasingly sophisticated, the creeping discharge of traditional " sandwich " structure is gradually unable to satisfy the demand of technical application.Firstly, " sandwich " is tied Structure need to be built in planar structure, and flat plasma can only be generated, and can not be applied on space scale;Secondly, " Sanming City Control " machining area of structure when expanding or shrinking on demand, needs to redesign, processing discharging structure, and it is costly and time consuming It is long, it is difficult to form modularization structure device.

Summary of the invention

In order to solve conventional catalyst removing NOxMethod cost of material is high, apparatus structure is complicated, catalyst is vulnerable, and " three The creeping discharge of Mingzhi " structure is difficult to be applied on space scale, realizes, diagnoses large area discharge and have difficulties etc. and ask Topic, the present invention provides a kind of large area to remove NO along face DBD synergistic catalystxModular unit and experimental method, mainly By array line-line electrode, reaction chamber, matching system, power-supply system, air supply system, gas detecting system, electricity diagnosis system System, optical diagnostic system and Catalyst Characterization System composition;Array line-line electrode is mainly arranged by multiple arrays Line style high-field electrode, medium tube, line style ground electrode and fixing piece composition;Wherein, medium tube and line style ground electrode are tubulose knot Structure, line style high-field electrode include solid metal stud;The internal diameter of medium tube is consistent with the outer diameter of line style ground electrode;Line style ground electrode It is inserted in medium tube, medium tube array arrangement, line style high-field electrode is inserted into the gap between medium tube;It is made of insulation board Upper fixing element and lower fixing piece be individually fixed on the top and bottom in enclosed reaction chamber made of insulating materials;Upper fixation Part and lower fixing piece are provided with hole, and the length of line style high-field electrode is greater than the distance between upper fixing element and lower fixing piece;Line style High-field electrode, medium tube top pass through the hole of upper fixing element, and are fixed on upper fixing element;Line style high-field electrode and line style The lower end of electrode passes through the hole of lower fixing piece, and is fixed on lower fixing piece;The top of each line style high-field electrode connects Array high-field electrode is formed on to the metal plate between upper fixing element and reaction chamber;The matched system of array high-field electrode connects Connect power-supply system;Ground electrode terminal plate is fixed between lower fixing piece and reaction chamber, each line style ground electrode and ground electrode wiring Plate connection, and pass through ground electrode wiring plate earthing;Uniform gas board is the sieve plate of uniformly distributed pore, and two mutually isostructural uniform gas boards are parallel Electrode two sides in array line-line electrode are fixed on by the corresponding hole slot of lower fixing piece in reaction chamber front and back sides, are catalyzed Agent is placed in the gap formed between uniform gas board and electrode;Former and later two sides of reaction chamber are symmetrically provided with several and penetrating are used for The stomata that gas passes through;Air supply system is divided to two gas circuits, and the road A is passed through gas detecting system, and the road B passes through reaction chamber again through stomata It is passed through gas detecting system, on-line checking is carried out to reacting gas concentration;Large area surface dielectric barrier discharge is along medium tube table Face occurs between line style high-field electrode and line style ground electrode, forms region of discharge;The side of reaction chamber is provided with quartz observing window, Electricity diagnostic system and the optical diagnostic system popped one's head in linear optical fiber carry out discharge plasma by quartz observing window Inline diagnosis;Before optical diagnostics, the part photosensitive element of linear optical fiber probe is blocked, while observing spectrum, determines photosensitive member The corresponding relationship of part and spatially resolved spectroscopy;Matching system is adjusted, voltage, current waveform are stablized, spectral intensity reaches maximum value, Guarantee the power output of power-supply system;Catalyst Characterization System characterizes the catalyst in electric discharge-elimination reaction.

Air supply system is mainly made of gas cylinder, mass flowmenter, heating furnace;Gas cylinder includes NOxGas and carrier gas, carrier gas one As be nitrogen, according to experiment needs, a certain amount of oxygen or hydrogen etc. can also be added;The flow and component of reaction gas are by quality stream Meter control, temperature is by Heating Furnace Control.

Gas detecting system is nitrogen-oxide analyzer, or gas chromatograph, is pressed between reaction chamber and gas detecting system Temperature control equipment need to be increased;According to General N OxThe temperature requirement of elimination reaction, temperature control equipment are usually cooling device.

Electricity diagnostic system is mainly by high-voltage probe, current probe and digital oscilloscope composition;Voltage signal is by connection High-voltage probe between line style high-field electrode and power-supply system on conducting wire passes to digital oscilloscope, and current signal is by connection Current probe between line style ground electrode and ground connection on conducting wire passes to digital oscilloscope;Real-time discharge voltage and electric discharge electricity Stream signal is measured and is shown by digital oscilloscope.

Optical diagnostic system is mainly popped one's head in by linear optical fiber, quartz lens, optical fiber, High Resolution Grating Monochromator, charge Coupled apparatus and computer composition;Wherein, High Resolution Grating Monochromator, charge-coupled device and computer are placed in bilayer screen Cover interior, and dead earthing;Linear optical fiber probe and quartz lens are fixed on optical platform by optical bench, face region of discharge Domain acquires optical signal by quartz observing window;Optical signal is collected by optical fiber, is divided into High Resolution Grating Monochromator Light, the monochromatic optical signal after light splitting is converted into digital signal by charge-coupled device, finally by computer disposal, with spectrogram Form is presented.

Grating used is 2400l/m and 1200l/m, and corresponding blaze wavelength is respectively 350nm and 500nm;Utilize spectrum When scheming to determine active specy classification and intensity, the grating of 1200l/m, 500nm need to be selected, to obtain bigger wave-length coverage;Benefit When determining the vibration temperature and rotation temperature of plasma with spectrogram, the grating of 2400l/m, 350nm need to be selected, to obtain more Clearly rotational band.

The daylighting element of linear optical fiber probe is in linear array, each element can independently, be collected simultaneously optical signal, light letter Number after quartz lens focuses, the spatially resolved spectroscopy of discharge plasma can be collected.

Catalyst Characterization System is X-ray diffractometer or high power transmission electron microscope or Fourier infrared spectrograph, or can be with Measure skeleton spectrum, the INFRARED SPECTRUM of adsorption species etc. of catalyst.

Uniform gas board bore dia, spacing are no more than 2mm.Uniform gas board can be added in pairs in the reaction chamber, at this time catalyst It can be individually placed between the uniform gas board added.

Power-supply system is also possible to the pulse power either AC power source.

Linear optical fiber probe had both can be used in optical diagnostic system, and traditional round fibre-optical probe also can be used.

Large area removes NO along face DBD synergistic catalystxModular unit experimental method include the following steps:

Step 1: two classes of assembling discharge-remove module: only comprising array line-line electrode in the reaction chamber of I generic module, II generic module then adds catalyst on this basis;

Step 2: plasma discharging bulk properties diagnoses: utilizing I generic module and gas circuit B, using electricity diagnostic system and have The optical diagnostic system of linear optical fiber probe carries out inline diagnosis to discharge plasma, blocks the part sense of linear optical fiber probe Optical element, while spectrum is observed, it determines the corresponding relationship of photosensitive element and spatially resolved spectroscopy, matching system is adjusted, so that electric Pressure, current waveform are stablized, and spectral intensity reaches maximum value;

Step 3: primary condition measures: determining the component and flow of gas using mass flowmenter, utilize heating stove heating Gas simultaneously keeps constant temperature, measures NO using gas detecting system and gas circuit AxEntrance concentration is characterized using Catalyst Characterization System Original catalyst, if having used self-supporting piece in characterization, need to be characterized in electric discharge-removing atmosphere it is pretreated from Support chip, and the characterization spectrum of self-supporting piece is deducted in analysis of catalyst characterization time spectrum;

Step 4: control group: using I generic module and gas circuit B measurement only plasma to NOxRemoval effect, utilize II Generic module measurement only plasma to the synergy of catalyst, using II generic module and gas circuit B measurement only catalyst to NOx's Removal effect, and utilize the catalyst after the reaction of Catalyst Characterization System (9) characterization;

Step 5: experimental group: using II generic module and gas circuit B measurement plasma body cooperative catalyst to NOxRemoving effect Fruit, and utilize the catalyst after Catalyst Characterization System characterization reaction.

The beneficial effects of the present invention are: (1) utilizes array line-line electrode, large area array creeping discharge is obtained Plasma establishes electric discharge-removing modular device;(2) area of discharge plasma can extension by array and mould The increase of block and increase;(3) technical application of surface discharge plasma is extended into space scale;(4) there is linear optical fiber The optical diagnostic system of probe can obtain the discharge plasma spectrum with spatial discrimination;(5) matching system is utilized, is adjusted The capacitance for saving load, guarantees the output power of power supply;(6) discharge plasma is applied to association by electric discharge-removing module With catalyst removal nitrogen oxides.

Detailed description of the invention

Fig. 1 is the structural diagram of the present invention.

Fig. 2 is array line-line electrode structural schematic diagram.

Fig. 3 is merging array line-line electrode exoelectrical reaction room.

Fig. 4 is feeder.

Fig. 5 is electricity diagnostic system.

Fig. 6 is the optical diagnostic system popped one's head in linear optical fiber.

In figure: 1. array lines-line electrode;2. reaction chamber;3. matching system;4. power-supply system;5. air supply system;6. gas Physical examination examining system;7. electricity diagnostic system;8. optical diagnostic system;9. Catalyst Characterization System;101. line style high-field electrode; 102. medium tube;103. line style ground electrode;104. ground electrode terminal plate;105. upper fixing element;106. lower fixing piece;107. even gas Plate;108. uniform gas board fixing piece;201. quartz observing windows;202. stomata;203. reactive tank;501. gas cylinder;502. mass flow Meter;503. heating furnace;701. digital oscilloscope;702. high-voltage probe;703. current probe;801. quartz lens;802. line style Fibre-optical probe;803. optical fiber;804. charge-coupled device;805. High Resolution Grating Monochromator;806. computer.

Specific embodiment

The present invention is further described with specific embodiment with reference to the accompanying drawing.

Array line-line electrode 1 is by array line style high-field electrode 101, medium tube 102, line style ground electrode 103, ground electricity Pole terminal plate 104, upper fixing element 105, lower fixing piece 106, uniform gas board 107 and uniform gas board fixing piece 108 form;Line style it is electric Pole 103 is inserted into lower fixing piece 106 one by one and is fixed, and accesses ground electrode terminal plate 104 with screw, makes ground electrode by conducting wire 104 dead earthing of terminal plate;By 102 sets of the same number of medium tube outside each line style ground electrode 103;Array line style is high Piezoelectricity pole 101 is inserted into upper fixing element 105 and is fixed, and each stud of array line style high-field electrode 101 is inserted into Jie respectively Between matter pipe 102, region of discharge is formed;Uniform gas board 107 is fixed on region of discharge two sides by uniform gas board fixing piece 108;By leading Line connects array line style high-field electrode 101, matching system 3 and power-supply system 4.

Stud size that array line style high-field electrode 101 includes, material are identical, the outer diameter one in gap and medium tube 102 It causes, the internal diameter of medium tube 102 is consistent with the diameter of line style ground electrode 103, and the thickness range of medium tube 102 is 1~1.5mm.Battle array The radial dimension of the stud that column line style high-field electrode 101 includes, line style ground electrode 103 and medium tube 102 can be in several millimeters To within the scope of more than ten millimeter, and axial dimension can be in tens cm ranges.Line style ground electrode 103 and medium tube 102 Number is consistent, can be one more compared with the stud number that array line style high-field electrode 101 includes, and can also lack one.Array Formula line style high-field electrode 101, line style ground electrode 103 and ground electrode terminal plate 104 can be by conduction materials such as white steel, brass, red coppers Material is made, and medium tube 102 can be the dielectric substances such as quartz, polytetrafluoroethylene (PTFE), ceramics, upper fixing element 105, lower fixing piece 106, uniform gas board fixing piece 108 then can be the insulating materials such as organic glass, wood.

Reaction chamber 2 includes quartz observing window 201, reactive tank 202 and stomata 203;Quartz observing window 201 is good due to it Translucency, the spectral characteristic of plasma in reaction chamber 2 can be measured in electric discharge-elimination reaction;Reactive tank 202 can be placed Array line-line electrode 101, uniform gas board 107, catalyst, can also be vacant according to experiment needs, and quantity can be according to reality It tests depending on demand;Stomata 202 is uniformly distributed in the two sides of reaction chamber, and the air flue of formation is perpendicular to region of discharge;Array line style High-field electrode 1 is placed in reaction chamber 2, constitutes electric discharge-removing module;Wherein, uniform gas board 107 can also be individually placed at reaction chamber 2 reactive tank 203 can be filled when the electric conductivity of catalyst is lower, carrier granular is less small in uniform gas board 107 and region of discharge Between domain, i.e., " one-part form ";If the electric conductivity of catalyst is enough to influence electric discharge, carrier is powdered, it can be individually placed in anti- It answers in slot 203, i.e. " two-part ".The selection of " one-part form " and " two-part ", should also be according to laboratory in addition to considering conditions above Or industrial application select.

Matching system 3 is made of adjustable resistance, capacitor, inductance, so that load matches with power supply, to guarantee power supply The power output of system 4.Matching value is then by the strength and stability of current-voltage waveform or spatial-resolved emission spectra come really It is fixed, i.e., when power-supply system 4 is certain, matching system 3 is adjusted, so that voltage current waveform is stable and current value reaches maximum, or The intensity of emission spectra of spatial discrimination reaches most strong, stability reaches best.

Power-supply system 4 can be nanosecond pulse power supply, be also possible to sine ac power supply.Wherein, nanosecond pulse power supply can To submit in positive negative direction for identical burst pulse voltage waveform is generated, pulse rise time is about 30-40ns, and pulsewidth is about 60ns, peak impulse voltage are continuously adjusted within the scope of 0-60kV, and pulse recurrence frequency is continuously adjusted within the scope of 0-400Hz. Nanosecond pulse power supply is placed in double layer screen case, shielded box and dead earthing.It is good that sine ac power supply can produce repeatability Sinusoidal ac corrugating, centre frequency are continuously adjusted within the scope of 0~15kHz, and voltage peak-to-peak value is within the scope of 0-40kV It is continuously adjustable.Since pulse voltage has precipitous rising edge and shorter pulse duration, so that electronics is in rapid increase Electric field in largely accelerated, and the lower ion of the larger mobility of quality and neutral particle are then difficult extremely short Energy is obtained in time, warm-up movement degree is almost unchanged, and the plasma generated is kept close to the state in room temperature.And The voltage of sine ac power supply is in continuous wave, when the temperature of discharge plasma can be with frequency, voltage peak-to-peak value, electric discharge Between etc. factors and increase.Therefore, when plasma of the needs generation close to room temperature, nanosecond pulse power supply is selected;When for putting When the temperature requirement of electro-plasma is not high, sine ac power supply can be selected.

Air supply system 5 is made of gas cylinder 501, mass flowmenter 502, heating furnace 503, and gas cylinder 501 includes NOxGas and Carrier gas, carrier gas are generally nitrogen, according to experiment needs, can also add a certain amount of oxygen or hydrogen etc.;The flow of reaction gas and Component is controlled by mass flowmenter 502, and temperature is controlled by heating furnace 503;Air supply system 501 is divided to two gas circuits, and the road A is passed through gas Detection system 6, the road B are passed through gas detecting system 6 after electric discharge-removing module again.

Gas detecting system 6 is generally nitrogen-oxide analyzer, or gas chromatograph, according to the sample temperature of instrument requirements, Increase temperature control equipment on demand before air inlet;According to General N OxThe temperature requirement of elimination reaction, temperature control equipment are usual For cooling device;If analysis instrument carries cooling device, can not also add.

Electricity diagnostic system 7 is made of high-voltage probe 702, current probe 703 and digital oscilloscope 701;Voltage signal warp It crosses the high-voltage probe 702 for being connected between array line style high-field electrode 101 and power-supply system 4 on conducting wire and passes to number and show Wave device, current signal pass to number by the current probe 703 on conducting wire between being connected to line style ground electrode 103 and being grounded and show Wave device 701;Real-time discharge voltage and discharge current signal are measured and are shown by digital oscilloscope 701.

Optical diagnostic system 8 is by linear optical fiber probe 802, quartz lens 801, optical fiber 803, High Resolution Grating Monochromator 805, charge-coupled device 804 and computer 806 form.Wherein, High Resolution Grating Monochromator 805, charge-coupled device 804 and computer 806 be placed in double layer screen room, and dead earthing.Linear optical fiber probe 802 is different from traditional fiber probe Place is that the element of acquisition optical signal whose forwardmost end portions linearly arranges, and optical signal, can after the focusing of quartz lens 801 To collect the spatially resolved spectroscopy of discharge plasma.When acquiring optical signal, linear optical fiber probe 802 and quartz lens 801 It is fixed on optical platform by optical bench, face region of discharge.Optical signal is collected by optical fiber 803, into high-resolution gration Monochromator 805 is divided, and the monochromatic optical signal after light splitting is converted into digital signal by charge-coupled device 804, finally by The processing of computer 806, is presented in the form of spectrogram.Wherein, common grating has 2400l/m and 1200 l/m, blaze wavelength point It Wei not 350nm and 500nm.When determining active specy classification and intensity using spectrogram, the biggish grating of blaze wavelength need to be selected, To obtain bigger wave-length coverage;When determining the vibration temperature and rotation temperature of plasma using spectrogram, resolution need to be selected The higher grating of rate, to obtain clearer rotational band.

Catalyst Characterization System 9 is generally X-ray diffractometer or high power transmission electron microscope or Fourier infrared spectrograph, can With skeleton spectrum, the INFRARED SPECTRUM of adsorption species etc. for measuring catalyst;According to the work of the spectrogram of measurement and discharge plasma Property species diagnosis, can analyze the reaction mechanism of plasma body cooperative catalyst.

Large area removes NO along face DBD synergistic catalystxModular unit specific experiment method, including walk as follows It is rapid:

Step 1: two classes of assembling discharge-remove module: only comprising array line-line electrode in the reaction chamber 2 of I generic module 1, II generic module then adds catalyst on this basis;

When assembly array formula line-line electrode 1, line style ground electrode 103 need to be inserted into one by one to fixed in lower fixing piece 106, use Screw accesses ground electrode terminal plate 104, passes through conducting wire dead earthing;In each line style by 102 sets of the same number of medium tube Outside electrode 103;Array line style high-field electrode 101 be inserted into it is fixed in upper fixing element 105, and by array line style high-field electrode 101 each stud, which is respectively embedded into, to be covered between the medium tube 102 outside line style ground electrode 103;Uniform gas board 107 is placed in region of discharge Two sides, it is fixed by uniform gas board fixing piece 108;Array line style high-field electrode 101, matching system 4 and power supply are connected by conducting wire System 5;Assembled array line-line electrode 1 is placed in reaction chamber 2, adds catalyst as desired, forms electric discharge- Remove module.

Step 2: plasma discharging bulk properties diagnoses: utilizing I generic module and gas circuit B, utilize electricity diagnostic system 7 and band There is the optical diagnostic system 8 of line style fibre-optical probe 802 to carry out inline diagnosis to discharge plasma, determines that linear optical fiber is popped one's head in 802 photosensitive element and the corresponding relationship of spectrum, the Current Voltage obtained using measurement, emission spectrum are adjusted matching system 3, made Electric discharge device is obtained to match with power-supply system 4;

When measuring electrology characteristic, electricity diagnostic system 7 need to be started;High-voltage probe 702 and current probe 703 are connected respectively To oscillograph 701, high-voltage probe 702 is connected in electric discharge high-voltage end, and current probe 703 is connected in electric discharge ground terminal, opens oscillograph 701 With voltage, electric current inputting channel, range is adjusted to maximum, determines triggering mode and signal averaging number;

When measuring optical characteristics, optical diagnostic system 8 need to be started;Adjust linear optical fiber probe 802 and quartz lens 801 Optical platform is fixed in position, so that the optical signal that discharge plasma issues imports light after converging by quartz lens 801 Fibre 803 opens High Resolution Grating Monochromator 805, charge-coupled device 804 and computer 806, starts Solis software, presses Suitable grating model is selected according to measurement demand, determines spectral measurement wave-length coverage and time for exposure, waits high-resolution gration Monochromator 805 and charge-coupled device 804, which are cooled to -70 DEG C or less, can carry out next step operation;Meanwhile in measurement space point Before distinguishing spectrum, the part photosensitive element of linear optical fiber probe 802 is blocked, obtained spectral signal is observed, determines linear optical fiber The corresponding relationship for the unit spectral signal that each photosensitive element of probe 802 and measurement obtain;

When adjusting matching system 3, it need to be needed according to measurement, first selection power supply type and parameter;Power-supply system 4 is opened, Keep power supply type and parameter certain, what the voltage and current and optical diagnostic system 8 recorded by electricity diagnostic system 7 recorded Emission spectrum determines the matching value of matching system 3.

Step 3: primary condition measures: determining the component and flow of gas using mass flowmenter 502, utilize heating furnace 503 heat gas simultaneously keep constant temperature, measure NO using gas detecting system 6 and gas circuit AxEntrance concentration utilizes catalyst characterization System 9 characterizes original catalyst, and pretreated self-supporting piece in electric discharge-removing atmosphere;

Characterization processing before original catalyst when, need to according to measurement need selecting catalyst characterization system 9 spectra resolution Rate, accumulative frequency, sweep time, and remained unchanged in entire measurement process;Tabletting or self-supporting piece needed for measurement are existed It is pre-processed in electric discharge-removing atmosphere, adjusts the processing time, measure the bone of corresponding reaction procatalyst, tabletting or self-supporting piece Frame spectrum and adsorbing species infrared spectroscopy;When the skeleton of analysis of catalyst or adsorbing species, tabletting or self-supporting piece need to be deducted Characterize spectrogram.

Step 4: control group: using I generic module and gas circuit B measurement only plasma to NOxRemoval effect, utilize II Generic module measurement only plasma to the synergy of catalyst, using II generic module and gas circuit B measurement only catalyst to NOx's Removal effect, and utilize the catalyst after the characterization reaction of Catalyst Characterization System 9;

Step 5: experimental group: using II generic module and gas circuit B measurement plasma body cooperative catalyst to NOxRemoving effect Fruit, and utilize the catalyst after the characterization reaction of Catalyst Characterization System 9.

Present invention uses the energisation modes with matching system, adjust matching value by diagnostic system to guarantee power supply Power output, to guarantee the area and stability of electric discharge.In terms of the diagnosis of active specy, since present invention uses have The spatial discrimination optical diagnostic system of linear optical fiber probe, both can with the active specy classification of on-line measurement discharge plasma and Relative intensity, and the emission spectrum of different discharge positions can be determined simultaneously, be conducive to expanding electric discharge geometric area, increasing and put When electricity-removing module number, real-time diagnosis spatially is carried out for the actual strength, area, stability of electric discharge.

Embodiment 1:

Catalytic mechanical is ground into graininess and is sieved, guarantee has a diameter larger than uniform gas board aperture 107, and is less than even gas The gap of plate 107 and region of discharge, is characterized;In N2In atmosphere, with gas flow 200ml/min, 300 DEG C of gas temperature, It is characterized after pretreatment self-supporting piece 30min;Self-supporting piece spectrogram is subtracted, original catalyst spectrogram S is obtainedo

Assemble two classes discharge-remove module.

I generic module is connected into circuit, gas circuit, adjusts inlet gas component, NOxFor 1000ppm, N2For Balance Air, gas stream 200ml/min is measured, 300 DEG C of temperature, measures reaction gas entrance concentration CoWith exit concentration Cp, and its photoelectric characteristic is detected, it determines Matching value.

II generic module is connected into gas circuit, adjusts inlet gas component, NOxFor 1000ppm, N2For Balance Air, gas flow 200ml/min, 300 DEG C of temperature, measurement outlet concentration Cc, catalyst is characterized after 30min, obtains spectrogram Sc

II generic module is connected into circuit, gas circuit, is only passed through Balance Air N2, gas flow 200ml/min, 300 DEG C of temperature, etc. Gas ions characterize catalyst, obtain spectrogram S with after catalyst action 30minp

II generic module is connected into circuit, gas circuit, adjusts inlet gas component, NOxFor 1000ppm, N2For Balance Air, gas Flow 200ml/min, 300 DEG C of temperature, plasma body cooperative catalyst treatment gas, measurement outlet concentration Ccp, characterize after 30min Catalyst obtains spectrogram Scp

Wherein, NOxEntrance concentration be Co, only catalyst is to NOxRemoval efficiency be (Cc-Co)/Co* 100%, only plasma Body is to NOxRemoval efficiency be (Cp-Co)/Co* 100%, plasma body cooperative catalyst is to NOxRemoval efficiency be (Ccp-Co)/Co* 100%;Original catalyst spectrogram is So, only catalyst removal NOxSpectrogram be Sc, the only spectrogram of plasma body cooperative catalyst For Sp, plasma body cooperative catalyst removal NOxSpectrogram be Scp

In the present embodiment, array line style high-field electrode 101 contains 19 identical studs with Bai Gangwei material. Line style ground electrode 103 is equally 20 independent cylindrical bodies, there are threaded apertures for wiring at column bottom with Bai Gangwei material With.Ground electrode terminal plate 104 is white steel part, there is 20 threaded through-holes, the size of through-hole and position and line style ground electrode 103 matchings.It medium tube 102 totally two ten, is covered outside 20 line style ground electrodes 103 one by one, material is polytetrafluoroethylene (PTFE).Catalysis Agent is adsorption catalyst natural zeolite.

Claims (8)

1. large area removes NO along face DBD synergistic catalystxModular unit, mainly by array line-line electrode (1), reaction Room (2), matching system (3), power-supply system (4), air supply system (5), gas detecting system (6), electricity diagnostic system (7), light Learn diagnostic system (8) and Catalyst Characterization System (9) composition;It is characterized by: array line-line electrode (1) is mainly by more Line style high-field electrode (101), medium tube (102), line style ground electrode (103) and the fixing piece composition of a array arrangement;Its In, medium tube (102) and line style ground electrode (103) they are tubular structure, and line style high-field electrode (101) includes solid metal stud; The internal diameter of medium tube (102) is consistent with the outer diameter of line style ground electrode (103);Line style ground electrode (103) is inserted in medium tube (102) In, medium tube (102) array arrangement, line style high-field electrode (101) is inserted into the gap between medium tube (102);By insulating Upper fixing element made of plate (105) and lower fixing piece (106) are individually fixed in enclosed reaction chamber made of insulating materials (2) On top and bottom;Upper fixing element (105) and lower fixing piece (106) are provided with hole, and the length of line style high-field electrode (101) is greater than The distance between upper fixing element (105) and lower fixing piece (106);Line style high-field electrode (101), medium tube (102) top pass through The hole of upper fixing element (105), and be fixed on upper fixing element (105);Line style high-field electrode (101) and line style ground electrode (103) lower end passes through the hole of lower fixing piece (106), and is fixed on lower fixing piece (106);Each line style high-field electrode (101) top is all connected to form array high-field electrode on the metal plate between upper fixing element (105) and reaction chamber (2); The matched system of array high-field electrode (3) connects power-supply system (4);Ground electrode terminal plate (104) is fixed on lower fixing piece (106) between reaction chamber (2), each line style ground electrode (103) connect with ground electrode terminal plate (104), and passes through ground electrode Terminal plate (104) ground connection;Uniform gas board (107) is the sieve plate of uniformly distributed pore, and two mutually isostructural uniform gas boards (107) are parallel to instead Room (2) front and back sides are answered, by the corresponding hole slot of lower fixing piece (106), are fixed on electrode two in array line-line electrode (1) Side, catalyst are placed in the gap formed between uniform gas board (107) and electrode;Reaction chamber (2) former and later two sides are symmetrically provided with Several penetrating stomatas (202) passed through for gas;Air supply system (5) is divided to two gas circuits, and the road A is passed through gas detecting system (6), the road B is passed through gas detecting system (6) by reaction chamber (2) through stomata (202) again, is examined online to reacting gas concentration It surveys;Large area surface dielectric barrier discharge is along medium tube (102) surface in line style high-field electrode (101) and line style ground electrode (103) occur between, form region of discharge;The side of reaction chamber (2) is provided with quartz observing window (201), electricity diagnostic system (7) Discharge plasma is carried out by quartz observing window (201) with the optical diagnostic system (8) with linear optical fiber probe (802) Inline diagnosis;Before optical diagnostics, the part photosensitive element of linear optical fiber probe (802) is blocked, while observing spectrum, determines sense The corresponding relationship of optical element and spatially resolved spectroscopy;It adjusts matching system (3), stablizes voltage, current waveform, spectral intensity reaches Maximum value guarantees the power output of power-supply system (4);Catalyst Characterization System (9) characterizes the catalysis in electric discharge-elimination reaction Agent.
2. large area according to claim 1 removes NO along face DBD synergistic catalystxModular unit, it is characterised in that Air supply system (5) is mainly made of gas cylinder (501), mass flowmenter (502), heating furnace (503);Gas cylinder (501) includes NOxGas Body and carrier gas, carrier gas are nitrogen, according to experiment needs, can also add a certain amount of oxygen or hydrogen;The flow and group of reaction gas Divide and controlled by mass flowmenter (502), temperature is controlled by heating furnace (503).
3. large area according to claim 1 removes NO along face DBD synergistic catalystxModular unit, it is characterised in that Gas detecting system (6) is nitrogen-oxide analyzer, or gas chromatograph, between reaction chamber (2) and gas detecting system (6) Increase temperature control equipment on demand;According to NOxThe temperature requirement of elimination reaction, temperature control equipment are cooling device.
4. large area according to claim 1 removes NO along face DBD synergistic catalystxModular unit, it is characterised in that Electricity diagnostic system (7) is mainly by high-voltage probe (702), current probe (703) and digital oscilloscope (701) composition;Voltage letter Number number is passed to by the high-voltage probe (702) for being connected between line style high-field electrode (101) and power-supply system (4) on conducting wire Oscillograph, current signal are passed to by being connected to the current probe (703) between line style ground electrode (103) and ground connection on conducting wire Digital oscilloscope (701);Real-time discharge voltage and discharge current signal are measured and are shown by digital oscilloscope (701).
5. large area according to claim 1 removes NO along face DBD synergistic catalystxModular unit, it is characterised in that Optical diagnostic system (8) is mainly popped one's head in (802) by linear optical fiber, quartz lens (801), optical fiber (803), high-resolution gration list Color instrument (805), charge-coupled device (804) and computer (806) composition;Wherein, High Resolution Grating Monochromator (805), electricity Lotus coupled apparatus (804) and computer (806) are placed in double layer screen room, and dead earthing;Linear optical fiber pop one's head in (802) and Quartz lens (801) is fixed on optical platform by optical bench, face region of discharge, acquires light by quartz observing window (201) Signal;Optical signal is collected by optical fiber (803), is divided into High Resolution Grating Monochromator (805), the monochrome after light splitting Optical signal is converted into digital signal by charge-coupled device (804), is finally handled by computer (806), in the form of spectrogram It presents.
6. large area removes NO along face DBD synergistic catalyst according to claim 1 or 5xModular unit, feature Be the daylighting element of linear optical fiber probe (802) in linear array, each element can independently, be collected simultaneously optical signal, light Signal can collect the spatially resolved spectroscopy of discharge plasma after quartz lens (801) focus.
7. large area according to claim 1 removes NO along face DBD synergistic catalystxModular unit, feature exists In: uniform gas board (107) is added in pairs in reaction chamber (2), at this time catalyst be individually placed at the uniform gas board (107) added it Between.
8. large area according to claim 2 removes NO along face DBD synergistic catalystxModular unit, it is characterised in that Experimental method includes the following steps:
Step 1: two classes of assembling discharge-remove module: only comprising array line-line electrode in the reaction chamber (2) of I generic module (1), II generic module then adds catalyst on this basis;
Step 2: plasma discharging bulk properties diagnoses: utilizing I generic module and gas circuit B, using electricity diagnostic system (7) and have The optical diagnostic system (8) of linear optical fiber probe (802) carries out inline diagnosis to discharge plasma, blocks linear optical fiber probe (802) part photosensitive element, while spectrum is observed, determine the corresponding relationship of photosensitive element and spatially resolved spectroscopy, adjusting Match system (3), so that voltage, current waveform are stablized, spectral intensity reaches maximum value;
Step 3: primary condition measures: determining the component and flow of gas using mass flowmenter (502), utilize heating furnace (503) heat gas and constant temperature is kept, gas detecting system (6) and gas circuit A is utilized to measure NOxEntrance concentration utilizes catalyst Characterization system (9) characterizes original catalyst, if having used self-supporting piece in characterization, needs to be characterized in electric discharge-removing gas Pretreated self-supporting piece in atmosphere, and the characterization spectrum of self-supporting piece is deducted in analysis of catalyst characterization time spectrum;
Step 4: control group: using I generic module and gas circuit B measurement only plasma to NOxRemoval effect, utilize II generic module Measurement only plasma to the synergy of catalyst, using II generic module and gas circuit B measurement only catalyst to NOxRemoving effect Fruit, and utilize the catalyst after the reaction of Catalyst Characterization System (9) characterization;
Step 5: experimental group: using II generic module and gas circuit B measurement plasma body cooperative catalyst to NOxRemoval effect, and Utilize the catalyst after the reaction of Catalyst Characterization System (9) characterization.
CN201610939904.XA 2016-10-25 2016-10-25 Modular unit of the large area along face DBD synergistic catalyst removing NOx CN106474919B (en)

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