CN108120681A - A kind of measurement HO2Transfer efficiency and RO2The apparatus and method for disturbing size - Google Patents
A kind of measurement HO2Transfer efficiency and RO2The apparatus and method for disturbing size Download PDFInfo
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- CN108120681A CN108120681A CN201711386354.4A CN201711386354A CN108120681A CN 108120681 A CN108120681 A CN 108120681A CN 201711386354 A CN201711386354 A CN 201711386354A CN 108120681 A CN108120681 A CN 108120681A
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- G—PHYSICS
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- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
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- G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
- G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
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Abstract
The invention discloses a kind of measurement HO2Transfer efficiency and RO2The device of size is disturbed, including radical source module, modular converter and fluorescence detection module；The radical source module includes lamp source, first gas flow duct and second gas flow duct, the lamp source, which is arranged in, closes at the position of the first gas flow duct, and the first gas flow duct and the second gas flow duct are interconnected and between the two equipped with CO gas feeds and hydrocarbon gas import；The modular converter includes conversion chamber and the NO gas supply mechanisms connected with the conversion chamber；The fluorescence detection module includes OH cell fluorescence detections ponds and HO2The fluorescence detection pond of cell, the OH cell fluorescence detections pond are connected with the second gas flow duct, and the conversion chamber is connected with the OH cell fluorescence detections pond, the HO2The fluorescence detection pond of cell is connected with the conversion chamber.The configuration of the present invention is simple, it is easy to operate, and also measurement accuracy is high, can widely be applied.
Description
Technical field
The invention belongs to atmosphere environment supervision fields, relate in particular to a kind of measurement HO2Transfer efficiency and RO2Interference
The apparatus and method of size.
Background technology
At present, the discharge of China's Megapolis atmosphere pollution has obtained effective control, however, with haze and photochemistry
The air secondary pollution problem that smog pollution is characterized but increasingly is shown especially, and secondary pollution has become the anti-of current China's atmosphere pollution
Control emphasis.There are free radical such as OH, HO of many high reaction activities during atmospheric photochemistry2、RO2Deng wherein OH freedom
Base is most important oxidant in air.Outside OH free radicals are except through the direct source of the photodissociation such as ozone, HONO, also
There is important secondary source.The secondary source of OH free radicals is exactly based on the chemical looping reaction generation between free radical,
Middle HO2Free radical is one of important secondary source of OH free radicals.HO in air2Free radical is 50~100 times of left sides of OH free radicals
The right side, HO2Free radical can by with NO react generation OH, in order to deeper into understand atmospheric oxidn process and the whole world air
Quality, be to HO2Free radical measurement is studied.HO2It is intermediate product important in atmospheric chemistry process, is primary pollution
The important medium of removal and secondary pollution generation, the formation of numerous secondary pollutions are all closely related with it.Therefore, realize
HO in FAGE systems2The measurement of free radical transfer efficiency is to realize a breakthrough of peroxy radical real-time online measuring in air
The research of property.
Due to peroxy radical it is difficult to be detected by method measured directly, gas flaring laser Induced Fluorescence Technology
(FAGE) it is that a kind of current application more widely measures HO indirectly by the method for chemical conversion2The method of free radical.In HO2
Measurement process in, RO2Free radical can also react generation OH free radicals with NO, so can be to HO2The measurement of free radical brings one
Fixed interference.Due to, there are many disturbing factors, realizing HO in air in field testing2The accurate measurement of free radical is always one
Hang-up.The present apparatus can be not only realized to HO in system2It is dry can also to understand some for the accurate measurement of free radical transfer efficiency
It disturbs in the presence of factor to HO in FAGE systems2The size that free radical measurement affects.
The content of the invention
The technical problems to be solved by the invention are to provide a kind of measurement HO2Transfer efficiency and RO2Disturb the device of size
And method.
In order to solve the above-mentioned technical problem, the present invention adopts the following technical scheme that：A kind of measurement HO2Transfer efficiency and RO2
The device of size is disturbed, including radical source module, modular converter and fluorescence detection module；
The radical source module includes lamp source, first gas flow duct and second gas flow duct, the lamp source arrangement
It is closing at the position of the first gas flow duct, the first gas flow duct is mutually interconnected with the second gas flow duct
Lead to and be equipped with CO gas feeds and hydrocarbon gas import between the two；
The modular converter includes conversion chamber and the NO gas supply mechanisms connected with the conversion chamber；
The fluorescence detection module includes OH cell fluorescence detections ponds and HO2The fluorescence detection pond of cell, the OH
Cell fluorescence detections pond is connected with the second gas flow duct, and the conversion chamber is connected with the OH cell fluorescence detections pond,
The HO2The fluorescence detection pond of cell is connected with the conversion chamber.
Further, the lamp source is covered with housing, and the housing is equipped with purge gas import and purge gas exports.
Further, the housing is socketed in the first gas flow duct.
Further, lens and diaphragm are equipped in the housing.
Further, the lower end of the second gas flow duct is covered with gas chamber, the OH cell fluorescence detections pond and institute
Air chamber sealing connection is stated, is connected with this with the second gas flow duct, the gas chamber is equipped with Waste gas outlet.
Further, the NO gas supply mechanisms include tee pipe coupling, flowmeter and two positioned opposite and difference
The pin hole shape NO air inlet pipe connected with the conversion chamber, two the pin hole shape NO air inlet pipe, the flowmeters pass through described three
Connection for bbreather pipe is interconnected.
Further, the NO gas flow directions in the pin hole shape NO air inlet pipe are flowed with the gas in the conversion chamber
Direction is vertical.
Further, further include and the HO2The vacuum pump of the fluorescence detection pond connection of cell.
Using above-mentioned measurement HO2Transfer efficiency and RO2The measurement HO that the device of size is disturbed to realize2Transfer efficiency
Method comprises the following steps：
(1) it is passed through N into first gas flow duct2、O2、H2The mixed gas of O three is opened lamp source, is supplied by NO gases
NO gases are passed through into conversion chamber to mechanism, the fluorescence signal that OH cell fluorescence detections pond is detected is denoted as SOH, HO2Cell's
The fluorescence signal that fluorescence detection pond is detected, is denoted as SNO；
(2) it is passed through N into first gas flow duct2、O2、H2The mixed gas of O three, open lamp source, by CO gases into
Mouth is passed through CO gases into second gas flow duct, and NO gases, OH cell are passed through into conversion chamber by NO gas supply mechanisms
The fluorescence signal that fluorescence detection pond is detected, is denoted as SCO, HO2The fluorescence signal that the fluorescence detection pond of cell is detected, is denoted as
SCO, NO；
(3) formula is passed throughHO is obtained2The transfer efficiency α of free radical.
Using above-mentioned measurement HO2Transfer efficiency and RO2The measurement RO that the device of size is disturbed to realize2Disturb the side of size
Method comprises the following steps：
(1) radical source module is not passed through any gas, and the fluorescence signal that OH cell fluorescence detections pond is detected is denoted as
S0；
(2) it is passed through N into first gas flow duct2、O2、H2The mixed gas of O three, open lamp source, by CO gases into
Mouth is passed through CO gases into second gas flow duct, and NO gases, HO are passed through into conversion chamber by NO gas supply mechanisms2cell
The fluorescence signal that detects of fluorescence detection pond, be denoted as SCO, NO；
(3) it is passed through N into first gas flow duct2、O2、H2The mixed gas of O three opens lamp source, passes through nytron
Object gas feed is passed through hydrocarbon gas into second gas flow duct, is led to by NO gas supply mechanisms into conversion chamber
Enter NO gases, the fluorescence signal that OH cell fluorescence detections pond is detected is denoted as SR, work as SRTend to S0When, illustrate OH and hydrocarbonization
It closes object to react completely, at this time HO2The fluorescence signal that the fluorescence detection pond of cell is detected, is denoted as SR, NO；
(4) formula is passed throughIt is obtained when there are a certain amount of RO2During free radical, to measuring HO2Interference
Size β.
Beneficial effects of the present invention are embodied in：
Apparatus of the present invention are based on gas flaring laser Induced Fluorescence Technology, are resonated by two fluorescence detection ponds to free radical
The fluorescence signal that transition generates synchronizes measurement, can realize known concentration HO2Conversion effect of the free radical in FAGE systems
The measurement of rate, then extends in air (HO2And RO2) number of free radical measurement, while the device can realize difference
RO2Free radical is to HO in FAGE systems2The measurement of interference effect.
In addition apparatus of the present invention are at low cost, and it is succinct convenient to operate, and has established the measurement to peroxy radical in air, has applied
Prospect is good, and apparatus of the present invention can also generate different types of RO2Free radical, therefore can there are a certain amount of in apparent FAGE systems
RO2To HO during free radical2The interference size of free radical measurement.
Measurement HO provided by the invention2Transfer efficiency and RO2The method for disturbing size, it is simple for process, it is easy to operate, and
And measurement accuracy is high, can widely be applied.
Description of the drawings
Fig. 1 is the structure diagram of one embodiment of the invention.
In attached drawing the mark of each component for：11 lamp sources, 12 first gas flow ducts, 13 second gas flow ducts, 14 CO gas
Body import, 15 hydrocarbon gas imports, 16 housings, 161 purge gas imports, the outlet of 162 purge gas, 17 gas chambers, 171
Waste gas outlet, 21 conversion chambers, 22 tee pipe couplings, 23 flowmeters, 24 pin hole shape NO air inlet pipe, 31 OH cell fluorescence detections
Pond, 32HO2The fluorescence detection pond of cell, 4 vacuum pumps.
Specific embodiment
The present invention will be described in detail below with reference to the accompanying drawings and in conjunction with the embodiments.It should be noted that in the feelings not conflicted
Under condition, the feature in embodiment and embodiment in the application can be mutually combined.
Referring to Fig. 1.
Present invention measurement HO2Transfer efficiency and RO2Disturb size device, including radical source module, modular converter and
Fluorescence detection module；
The radical source module includes lamp source 11, first gas flow duct 12 and second gas flow duct 13, the lamp
Source 11, which is arranged in, closes on (the specific distance of " closing on " is so as to effectively carry out photodissociation) described first gas flow duct 12
At position, the first gas flow duct 12 and the second gas flow duct 13 be interconnected and be equipped between the two CO gases into
Mouth 14 and hydrocarbon gas import 15；
The modular converter includes conversion chamber 21 and the NO gas supply mechanisms connected with the conversion chamber 21；
The fluorescence detection module includes OH cell fluorescence detections pond 31 and HO2The fluorescence detection pond 32 of cell, the OH
Cell fluorescence detections pond 31 is connected with the second gas flow duct 13, the conversion chamber 21 and the OH cell fluorescence detections
Pond 31 connects, the HO2The fluorescence detection pond 32 of cell is connected with the conversion chamber 21.
In the present invention, radical source module is generating OH, HO2Free radical, and OH free radicals is clear by other reactions
It removes or converts；Modular converter is realizing HO2Free radical and RO2The conversion of free radical.Concrete principle is as follows：
First gas flow duct and second gas flow duct are used for carrying out sample collection and series of chemical, generally adopt
It is made of quartz ampoule, a certain proportion of N is passed through into first gas flow duct2、O2、H2The mixed gas of O three, in lamp source (one
As select mercury lamp) under the effect of light of 185nm, synchronous photodissociation H2O and O2The HO of equivalent can be generated2With OH free radicals；
When being passed through certain density CO gases into second gas flow duct by CO gas feeds, pass through reaction equation OH
+CO→HO2+CO2By the OH radical conversions in system into HO2Free radical；By radical source mould OH radical conversions in the block into
HO2Free radical avoids loss of the OH free radicals of high activity in transmission process；
When the hydrocarbon gas for being passed through appropriate concentration into second gas flow duct by hydrocarbon gas import
Body (methane, ethylene etc.), alkane hydrocarbon is mainly by reaction equation RH+OH → R+H2O、R+O2+M→RO2+ M (R=
CH4、C2H4Deng), OH free radicals are converted into RO2Free radical, and alkene hydrocarbon is mainly converted by addition reaction
Into RO2Free radical, the OH free radicals RO different from the generation of different types of hydrocarbon reaction2Free radical, and certain anti-
Since OH free radicals are different from hydrocarbon reaction rate in seasonable, the RO of generation2The amount of free radical is also different.
And when middle NO gases are passed through into conversion chamber by NO gas supply mechanisms, then pass through reaction equation RO2+NO→RO+
NO2、RO+O2→R,O+HO2、HO2+NO→OH+NO2Or other reaction paths are by RO in system2、HO2Radical conversion into OH from
By base, the RO in sampling air flow is detected2Free radical is to HO in system2The size of free radical measurement interference；
Two fluorescence detection ponds can measure OH free radicals and resonant transition generation occurs under the laser irradiation of 308nm simultaneously
Fluorescence signal (i.e. fluorescent photon number), with reference to above operation, according to two fluorescence detection pond detecting under different operating
Fluorescence signal can measure HO in FAGE systems2Transfer efficiency and RO2Disturb size.Measuring method is as described below.
In one embodiment, the lamp source 11 is covered with housing 16, and the housing 16 is equipped with 161 He of purge gas import
Purge gas outlet 162.In use, purge gas is passed through from purge gas (generally nitrogen) import, purge gas outlet
Discharge, effect one is the temperature stabilization that can maintain lamp source, and two can be prevented from absorption of the oxygen to 185nm light.
In one embodiment, the housing 16 is socketed in the first gas flow duct 12.It so designs, housing and one
Gas flow duct is combined together, easy to install and use.
In one embodiment, lens and diaphragm are equipped in the housing 16.The effect of lens ensures that lamp source is launched
Just for parallel radiation in sample gas, the effect of diaphragm is can to adjust the power of lamp source light.
In one embodiment, the lower end of the second gas flow duct 13 is covered with gas chamber 17, and the OH cell fluorescence is visited
It surveys pond 31 to connect with the gas chamber 17 sealing, be connected with this with the second gas flow duct 13, the gas chamber is equipped with exhaust gas
Floss hole 171.It so designs, not only facilitates the unwanted exhaust gas of discharge, but also can avoid being put into gas in flow duct and be formed
Turbulent flow avoids more collision losses.
In one embodiment, the NO gas supply mechanisms include tee pipe coupling 22, flowmeter 23 and two opposite cloth
The pin hole shape NO air inlet pipe 24 put and connected respectively with the conversion chamber 21, two the pin hole shape NO air inlet pipe 24, the streams
Gauge 23 is interconnected by the tee pipe coupling 22.So design, so design, can make NO gases evenly into turn
Change room, and flowmeter can control the flow velocity and concentration for being passed through NO, preferred mass flowmeter (MFC) of the present invention.
In one embodiment, in the NO gas flow directions in the pin hole shape NO air inlet pipe 24 and the conversion chamber 21
Gas flow direction is vertical, can realize peroxy radical and the effective collision of NO, and can efficiently weaken flow perturbation to OH from
The interference measured by base, avoids its collision loss, to realize HO2The accurate measurement of free radical lays the foundation.
In one embodiment, further include and the HO2The vacuum pump 4 that the fluorescence detection pond 32 of cell connects.Vacuum pump is used
The power that drive gas flow is moved is provided.
HO is measured using the present invention2Transfer efficiency and RO2The measurement HO that the device of size is disturbed to realize2Transfer efficiency
Method, comprise the following steps：
(1) it is passed through N into first gas flow duct 122、O2、H2The mixed gas of O three opens lamp source 11, passes through NO gas
Body feed mechanism is passed through NO gases into conversion chamber 21, and such mixed gas generates OH and HO in first gas flow duct 122
Free radical, then HO2Free radical changes into OH free radicals, the fluorescence that OH cell fluorescence detections pond 31 is detected in conversion chamber
Signal is denoted as SOH, HO2The fluorescence signal that the fluorescence detection pond 32 of cell is detected, is denoted as SNO；
(2) it is passed through N into first gas flow duct 122、O2、H2The mixed gas of O three opens lamp source 11, passes through CO gas
Body import 14 is passed through CO gases into second gas flow duct 13, and NO gas is passed through into conversion chamber 21 by NO gas supply mechanisms
Body, such mixed gas generate OH and HO in first gas flow duct 122Free radical, then OH free radicals are in second gas stream
HO is changed into dynamic pipe 132Free radical, therefore it is pumped into the only HO in fluorescence detection pond 312Free radical, OH cell fluorescence are visited
The fluorescence signal that pond 31 is detected is surveyed, is denoted as SCO, HO2The fluorescence signal that the fluorescence detection pond 32 of cell is detected, is denoted as SCO, NO；
(3) formula is passed throughHO is obtained2The transfer efficiency α of free radical.
It considers OH and NO in entire reaction process in the formula there are back reaction generation HONO and to cause OH free radicals
Part influence of the loss to transfer efficiency and certain density CO is passed through into flow duct is in order to by radical source module
In OH radical conversions into HO2Free radical avoids the OH free radicals of the high activity in transmission process from being lost.It so can be more accurate
The true HO calculated in FAGE systems2The transfer efficiency of free radical.
HO is measured using the present invention2Transfer efficiency and RO2The measurement RO that the device of size is disturbed to realize2Disturb size
Method comprises the following steps：
(1) radical source module is not passed through any gas, the fluorescence signal that OH cell fluorescence detections pond 31 is detected, note
For S0, S0For background signal；
(2) it is passed through N into first gas flow duct 122、O2、H2The mixed gas of O three opens lamp source 11, passes through CO gas
Body import 14 is passed through CO gases into second gas flow duct 13, and NO gas is passed through into conversion chamber 21 by NO gas supply mechanisms
Body, HO2The fluorescence signal that the fluorescence detection pond 32 of cell is detected, is denoted as SCO, NO；
(3) it is passed through N into first gas flow duct 122、O2、H2The mixed gas of O three opens lamp source 11, by hydrocarbon
Chemical compound gas import 15 is passed through hydrocarbon gas into second gas flow duct 13, by NO gas supply mechanisms to turn
Change in room 21 and be passed through NO gases, such mixed gas generates OH and HO in first gas flow duct 122Free radical, then OH from
By base RO is changed into second gas flow duct 132Free radical, therefore be pumped into fluorescence detection pond 31 and contain RO2、HO2
Free radical, the fluorescence signal that OH cell fluorescence detections pond 31 is detected, is denoted as SR, work as SRTend to S0When, illustrate OH and hydrocarbonization
It closes object to react completely, at this time HO2The fluorescence signal that the fluorescence detection pond 32 of cell is detected, is denoted as SR, NO；
(4) formula is passed throughIt is obtained when there are a certain amount of RO2During free radical, to measuring HO2Interference
Size β.
The above method can facilitate and accurately calculate variety classes RO2Free radical is to HO in FAGE systems2Free backbone
Disturb size.
It should be understood that example as described herein and embodiment are not intended to limit the invention, this field only for explanation
Technical staff can make various modifications or variation according to it, within the spirit and principles of the invention, any modification for being made,
Equivalent substitution, improvement etc., should all be included in the protection scope of the present invention.
Claims (10)
1. a kind of measurement HO2Transfer efficiency and RO2Disturb the device of size, it is characterised in that：Including radical source module, turn
Change the mold block and fluorescence detection module；
The radical source module includes lamp source, first gas flow duct and second gas flow duct, and the lamp source, which is arranged in, faces
At the position of the nearly first gas flow duct, the first gas flow duct and the second gas flow duct be interconnected and
CO gas feeds and hydrocarbon gas import are equipped between the two；
The modular converter includes conversion chamber and the NO gas supply mechanisms connected with the conversion chamber；
The fluorescence detection module includes OH cell fluorescence detections ponds and HO2The fluorescence detection pond of cell, the OH cell fluorescence
Detection pond is connected with the second gas flow duct, and the conversion chamber is connected with the OH cell fluorescence detections pond, described
HO2The fluorescence detection pond of cell is connected with the conversion chamber.
2. measurement HO as described in claim 12Transfer efficiency and RO2Disturb the device of size, it is characterised in that：The lamp
Source is covered with housing, and the housing is equipped with purge gas import and purge gas exports.
3. measurement HO as claimed in claim 22Transfer efficiency and RO2Disturb the device of size, it is characterised in that：The shell
Body is socketed in the first gas flow duct.
4. measurement HO as claimed in claim 2 or claim 32Transfer efficiency and RO2Disturb the device of size, it is characterised in that：It is described
Lens and diaphragm are equipped in housing.
5. the measurement HO as described in claim 1 or 2 or 32Transfer efficiency and RO2Disturb the device of size, it is characterised in that：
The lower end of the second gas flow duct is covered with gas chamber, and the OH cell fluorescence detections pond is connected with the air chamber sealing, with
This is connected with the second gas flow duct, and the gas chamber is equipped with Waste gas outlet.
6. the measurement HO as described in claim 1 or 2 or 32Transfer efficiency and RO2Disturb the device of size, it is characterised in that：
It is positioned opposite and respectively connected with the conversion chamber that the NO gas supply mechanisms include tee pipe coupling, flowmeter and two
Pin hole shape NO air inlet pipe, two the pin hole shape NO air inlet pipe, the flowmeters are interconnected by the tee pipe coupling.
7. the measurement HO as described in claim 1 or 2 or 32Transfer efficiency and RO2Disturb the device of size, it is characterised in that：
NO gas flow directions in the pin hole shape NO air inlet pipe are vertical with the gas flow direction in the conversion chamber.
8. the measurement HO as described in claim 1 or 2 or 32Transfer efficiency and RO2Disturb the device of size, it is characterised in that：
It further includes and the HO2The vacuum pump of the fluorescence detection pond connection of cell.
9. a kind of measurement HO2Transfer efficiency method, which is characterized in that employ as any one of claim 1 to 8
Measurement HO2Transfer efficiency and RO2The device of size is disturbed, is comprised the following steps：
(1) it is passed through N into first gas flow duct2、O2、H2The mixed gas of O three opens lamp source, and machine is supplied by NO gases
Structure is passed through NO gases into conversion chamber, and the fluorescence signal that OH cell fluorescence detections pond is detected is denoted as SOH, HO2The fluorescence of cell
The fluorescence signal that detection pond is detected, is denoted as SNO；
(2) it is passed through N into first gas flow duct2、O2、H2The mixed gas of O three, open lamp source, by CO gas feeds to
CO gases are passed through in second gas flow duct, NO gases, OH cell fluorescence are passed through into conversion chamber by NO gas supply mechanisms
The fluorescence signal that detection pond is detected, is denoted as SCO, HO2The fluorescence signal that the fluorescence detection pond of cell is detected, is denoted as SCO, NO；
(3) formula is passed throughHO is obtained2The transfer efficiency α of free radical.
10. a kind of measurement RO2The method for disturbing size, which is characterized in that employ as described in any item of the claim 1 to 8
Measure HO2Transfer efficiency and RO2The device of size is disturbed, is comprised the following steps：
(1) radical source module is not passed through any gas, and the fluorescence signal that OH cell fluorescence detections pond is detected is denoted as S0；
(2) it is passed through N into first gas flow duct2、O2、H2The mixed gas of O three, open lamp source, by CO gas feeds to
CO gases are passed through in second gas flow duct, NO gases, HO are passed through into conversion chamber by NO gas supply mechanisms2Cell's is glimmering
The fluorescence signal that optical detection pond is detected, is denoted as SCO, NO；
(3) it is passed through N into first gas flow duct2、O2、H2The mixed gas of O three opens lamp source, passes through hydrocarbon gas
Body import is passed through hydrocarbon gas into second gas flow duct, and NO is passed through into conversion chamber by NO gas supply mechanisms
Gas, the fluorescence signal that OH cell fluorescence detections pond is detected, is denoted as SR, work as SRTend to S0When, illustrate OH and hydrocarbon
It reacts completely, at this time HO2The fluorescence signal that the fluorescence detection pond of cell is detected, is denoted as SR, NO；
(4) formula is passed throughIt is obtained when there are a certain amount of RO2During free radical, to measuring HO2The size of interference
β。
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| CN113281311A (en) * | 2020-02-20 | 2021-08-20 | 北京大学 | Online detection device and method for organic peroxy radicals in atmosphere |
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