CN1326810A - Normal pressure microwave discharging reactor and appliation in removing nitrogen-oxygen compound thereof - Google Patents

Normal pressure microwave discharging reactor and appliation in removing nitrogen-oxygen compound thereof Download PDF

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Publication number
CN1326810A
CN1326810A CN 00110497 CN00110497A CN1326810A CN 1326810 A CN1326810 A CN 1326810A CN 00110497 CN00110497 CN 00110497 CN 00110497 A CN00110497 A CN 00110497A CN 1326810 A CN1326810 A CN 1326810A
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discharge
reactor
normal pressure
microwave
gas
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CN1173767C (en
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唐军旺
马磊
徐长海
孙孝英
张涛
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Dalian Institute of Chemical Physics of CAS
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Dalian Institute of Chemical Physics of CAS
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Abstract

The normal pressure microwave discharging reactor consists of two parts of microwave feeding mechanism and chemical reactor. it features that the chemical reactor is one double-layered quartz structure including the inner layer of closed-tip conic quartz tube and the outer layer of cylindrical quartz tube with one sandwiched gas passage being formed in between. Below the conic tip of the inner layer quartz tube, there is one quartz grating fixed to the outer layer quartz tube and one layer of quartz wool is set on the quartz grating. The present invention may be used to convert 60% over NOx in gas with high oxygen content into harmless N2 and O2 directly in the condition of no catalyst. The present invention has the advantages of no electrode and additive pollution, etc.

Description

A kind of normal pressure microwave discharge reactor and the application in oxynitrides removes thereof
The present invention relates to directly cause normal pressure microwave discharge and the application in environmental protection thereof.Particularly need not to cause electrode and other initiation material, realized normal pressure microwave stable discharging; And under a large amount of oxygen existence conditions, need not catalyst, and need not additive, a step is with a large amount of NO xBe converted into N 2And O 2
Utilizing corona discharge to remove gas pollutant is a kind of well-known method.People such as Puchkarev have set forth the research of " elimination of toxic gas under discharging condition " comprehensively in international plasma meeting in 1994.Inquired into the elimination of discharge in the Ser.No.08/29595 patent, and applied by Hughes Aircraft company to liquid pollutant.People such as Yamamoto have also described by corona discharge pulse and have eliminated VOC refuses such as (VOCs).U.S.Pat.No.4695358 has also pointed out to remove SO in the waste gas with the high direct voltage discharge xAnd NO x, also remove NO among China patent CN.96199441.x with the high voltage electric field discharge xUtilize fuel oil under the corona discharge state, to remove NO among U.S.Pat.No.5807466 and the U.S.Pat.No.5084078 xAbove discharge technology all belongs to the high direct voltage discharge, shown the higher advantage of its conversion ratio, but shortcoming is obvious, and its capacity usage ratio of pointing out in U.S.Pat.No.5807466 as people such as Wang is lower.
People such as G.E.Vogtlin and B.M.Penetrate is in that " corona discharge removes NO x" summed up the high direct voltage discharge in the literary composition and remove NO xProcess, promptly at first under a large amount of oxygen conditions, NO is being converted into NO 2, then by adding NH 3Or hydro carbons comes absorption of N O 2, form nitrose salt, remove the solid salt particle with deduster or filter again.This method shortcoming is to need to add additive to remove NO x, and the solid salt grain that forms still need handle, and capacity usage ratio is also lower; Problems such as the loss of sparking electrode and electrode fouling are also to be solved simultaneously.
With microwave discharge cracking methane, methane conversion can reach 90% to people such as J.H.Hang and S.L.Suib under condition of negative pressure, but the negative pressure discharge has increased operating equipment and has been unfavorable for its commercial Application.People such as metal research institute of China Chinese Academy of Sciences Cao Li China are in patent No.94110112, and the medium made from refractory ceramics causes microwave discharge.We had also once realized causing microwave discharge with electrode, and came cracking CH with this 4System acetylene, the acetylene yield reaches 60%, but has the serious ablation phenomen of electrode in the experiment.
Microwave discharge is compared than the high direct voltage discharge, and the former active constituent (electronics, negative ions and free radical) is made high frequency oscillation at region of discharge with electromagnetic field, thereby obtained big energy, its temperature is also very high, and the overall gas mean temperature is very low, and this can improve capacity usage ratio greatly; The latter's active constituent region of discharge then do not do the concussion or the concussion frequency very low, be not very big so active group and ensemble average temperature differ, this limited to a certain extent its application, the particularly application aspect chemical industry.
The object of the present invention is to provide a kind of normal pressure microwave discharge reactor, it can need not any initiation material, directly obtains stable normal pressure microwave discharge in gas, is specially adapted to NO xHarmless removing.
The invention provides a kind of normal pressure microwave discharge reactor, form by microwave feed-in mechanism, chemical reactor two parts, it is characterized in that: described chemical reactor is the double-decker of quartzy material, internal layer quartz ampoule (2) is taper, the tip is sealed, outer quartz ampoule (1) is cylindrical, and the chuck of two interlayers forms gas passage; Under internal layer quartz ampoule (2) cone point, be provided with quartzy grid (4) affixed with outer quartz ampoule (1), quartzy grid (4) are gone up and are placed one deck silica wool (3).
Special construction design of the present invention makes to be evenly distributed between reactor internal layer awl point and the quartzy little grid by the discharge of microwave initiation is concentrated.In addition, the present invention introduces region of discharge as excited gas with unstripped gas, and with its discharge of microwave-excitation, microwave discharge power is determined by gas flow, thereby can realize the discharge of normal pressure steady and continuous.Because active group (electronics, negative ions, free radical) temperature is very high in the discharge gas that the present invention causes with microwave, has very big activity, is convenient to other substance reaction or promotes reaction between other material.The mean temperature of discharge gas is very low simultaneously, and the average energy consumption of overall gas is little, helps controlling the degree that reaction is carried out, and can make thalidomide stay the intermediate state.Thereby be suitable for chemical field, particularly be applicable to NO xHarmless removing.Specifically, the present invention can at first will contain NO and a large amount of O 2Mist feed in the quartz discharge device, by this special discharge reactor it is discharged under microwave condition, and then with 60% above NO xBe converted into N 2And O 2
The present invention is electrodeless and secondary pollution such as additive, does not have the catalyst poisoning phenomenon.The existing ripe production specifications of required microwave device help technology and amplify.NO in the unstrpped gas xNO in content and the real waste gas xContent is approaching, even higher.Required discharge reactor also simply is easy to do, and need not add other material in the reaction, and operating procedure is simple, for removing NO x, shown considerable prospect with microwave discharge method, and might carry out widespread adoption.
Below by example in detail the present invention is described in detail.
Accompanying drawing 1. normal pressure microwave discharge reactor schematic diagrames
When accompanying drawing 2. existed at a large amount of oxygen, microwave input power removed NO to discharge xInfluence
Embodiment 1.
As shown in Figure 1, constitute microwave cavity by waveguide (8), coupling window (9), tuning plunger (11), reactor vertically passes resonator, for preventing the leakage of microwave energy, be provided with anti-leak ring (10), make discharge reactor with double-deck quartz ampoule, internal layer quartz ampoule (2) is taper, the sealing of awl point, awl end external diameter 6mm; There are quartzy grid (4) at the 20mm place under internal layer quartz ampoule (2) awl point, and itself and outer quartz ampoule (1) sintering have one deck silica wool (3) to be placed on the quartzy grid (4) together.Outer quartz ampoule (1) is the cylinder of 10mm for internal diameter.Gas is along importing discharge reactor in the inside and outside quartz ampoule chuck.Region of discharge is positioned at internal layer quartz ampoule (2) awl point between the quartzy grid (4).Reaction gas is entered by reaction gas inlet (5), and product gas is overflowed by product gas outlet (6), the electric arc that (7) form for discharge.O in the used discharge gas 2: 0-4%, total gas flow rate 40-120ml/min.
Under embodiment 2. oxygen free conditions, Decomposition of NO in Microwave Discharge
Atmosphere is in the example: NO, 2000ppm; All the other are He, and total gas flow rate is 60ml/min, and discharge stability was surveyed product with gas-chromatography and five proximate analysis instrument and formed after one hour.
Gas composition Microwave input power (W) NO total conversion (%) NO is converted into N 2(%) NO is converted into other (%)
??NO+He ????40—50 ????95.72 ????88.03 ????7.69
When embodiment 3. a large amount of oxygen exist, Decomposition of NO in Microwave Discharge x
Atmosphere is in the example: NO, 2000ppm; O 2, 2%; All the other are He, and total gas flow rate is 60ml/min, and discharge stability was surveyed product with gas-chromatography and five proximate analysis instrument and formed after one hour.
Gas composition Microwave input power (W) NO xTotal conversion (%) ??NO xBe converted into N 2(%) ??NO xBe converted into other (%)
NO+He+O 2 40—50 77.54 ??62.29 ??15.25
Embodiment 4. is with CH 4Replace O 2The time, Decomposition of NO in Microwave Discharge
Atmosphere is in the example: NO, 2000ppm; CH 4, 1600ppm; All the other are He, and total gas flow rate is 60ml/min, and discharge stability was surveyed product with gas-chromatography and five proximate analysis instrument and formed after one hour.
Gas composition Microwave input power (W) NO total conversion (%) NO is converted into N 2(%) NO is converted into other (%)
NO+He+CH 4 ?30—35 ?100 ?76.90 ?23.10
?40—50 ?100 ?80.58 ?19.42
When embodiment 5. existed at a large amount of oxygen, microwave input power removed NO to discharge xInfluence
Atmosphere is in the example: NO, 2000ppm; O 2, 2%; All the other are He, and total gas flow rate is 60ml/min, and discharge stability was surveyed product with gas-chromatography and five proximate analysis instrument and formed (accompanying drawing 2) after one hour.
Thus example as can be seen, when oxygen exists in a large number, still can be with microwave discharge method with 60% above NO xBe converted into non-harmful N 2

Claims (2)

1, a kind of normal pressure microwave discharge reactor, form by microwave feed-in mechanism, chemical reactor two parts, it is characterized in that: described chemical reactor is the double-decker of quartzy material, internal layer quartz ampoule (2) is taper, the tip is sealed, outer quartz ampoule (1) is cylindrical, and the chuck of two interlayers forms gas passage; Under internal layer quartz ampoule (2) cone point, be provided with quartzy grid (4) affixed with outer quartz ampoule (1), quartzy grid (4) are gone up and are placed one deck silica wool (3).
2, the described normal pressure microwave discharge of a kind of claim 1 reactor is at NO xApplication in removing is characterized in that: under the catalyst-free condition, with 60% above NO in the high keto content gas xBe converted into harmless N 2And O 2
CNB001104977A 2000-06-07 2000-06-07 Normal pressure microwave discharging reactor and appliation in removing nitrogen-oxygen compound thereof Expired - Fee Related CN1173767C (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109821372A (en) * 2019-02-21 2019-05-31 东华大学 A kind of microwave induced metal discharge carries out the device and method of denitrating flue gas

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109821372A (en) * 2019-02-21 2019-05-31 东华大学 A kind of microwave induced metal discharge carries out the device and method of denitrating flue gas

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