CN113295628A - Device for simultaneously detecting black carbon, organic carbon and gas - Google Patents
Device for simultaneously detecting black carbon, organic carbon and gas Download PDFInfo
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- CN113295628A CN113295628A CN202010110063.8A CN202010110063A CN113295628A CN 113295628 A CN113295628 A CN 113295628A CN 202010110063 A CN202010110063 A CN 202010110063A CN 113295628 A CN113295628 A CN 113295628A
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- 239000003738 black carbon Substances 0.000 title claims abstract description 42
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 34
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 28
- 238000010521 absorption reaction Methods 0.000 claims abstract description 37
- 239000007789 gas Substances 0.000 claims abstract description 31
- 239000002245 particle Substances 0.000 claims abstract description 28
- 230000003287 optical effect Effects 0.000 claims abstract description 19
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 claims abstract description 17
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 claims abstract description 17
- 239000012528 membrane Substances 0.000 claims description 3
- 239000000126 substance Substances 0.000 claims description 2
- 238000005259 measurement Methods 0.000 abstract description 8
- 238000010895 photoacoustic effect Methods 0.000 abstract description 2
- 229910002092 carbon dioxide Inorganic materials 0.000 description 7
- 238000004867 photoacoustic spectroscopy Methods 0.000 description 7
- 230000008859 change Effects 0.000 description 6
- 238000000034 method Methods 0.000 description 6
- 239000000443 aerosol Substances 0.000 description 5
- 230000005855 radiation Effects 0.000 description 4
- 238000002474 experimental method Methods 0.000 description 3
- 239000013618 particulate matter Substances 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- 238000001514 detection method Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 230000036541 health Effects 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 210000002345 respiratory system Anatomy 0.000 description 2
- 230000035945 sensitivity Effects 0.000 description 2
- 239000000725 suspension Substances 0.000 description 2
- 239000010409 thin film Substances 0.000 description 2
- 208000024172 Cardiovascular disease Diseases 0.000 description 1
- 238000000149 argon plasma sintering Methods 0.000 description 1
- 208000006673 asthma Diseases 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 231100000481 chemical toxicant Toxicity 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 201000010099 disease Diseases 0.000 description 1
- 208000037265 diseases, disorders, signs and symptoms Diseases 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000005180 public health Effects 0.000 description 1
- 230000002685 pulmonary effect Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000000241 respiratory effect Effects 0.000 description 1
- 230000029058 respiratory gaseous exchange Effects 0.000 description 1
- 238000004611 spectroscopical analysis Methods 0.000 description 1
- 239000003440 toxic substance Substances 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
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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
- G01N21/17—Systems in which incident light is modified in accordance with the properties of the material investigated
- G01N21/25—Colour; Spectral properties, i.e. comparison of effect of material on the light at two or more different wavelengths or wavelength bands
- G01N21/31—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry
- G01N21/314—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry with comparison of measurements at specific and non-specific wavelengths
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- G—PHYSICS
- G01—MEASURING; TESTING
- 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
- G01N21/17—Systems in which incident light is modified in accordance with the properties of the material investigated
- G01N21/1702—Systems in which incident light is modified in accordance with the properties of the material investigated with opto-acoustic detection, e.g. for gases or analysing solids
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- G—PHYSICS
- G01—MEASURING; TESTING
- 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
- G01N21/17—Systems in which incident light is modified in accordance with the properties of the material investigated
- G01N21/1702—Systems in which incident light is modified in accordance with the properties of the material investigated with opto-acoustic detection, e.g. for gases or analysing solids
- G01N2021/1704—Systems in which incident light is modified in accordance with the properties of the material investigated with opto-acoustic detection, e.g. for gases or analysing solids in gases
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- G01—MEASURING; TESTING
- 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
- G01N21/17—Systems in which incident light is modified in accordance with the properties of the material investigated
- G01N21/25—Colour; Spectral properties, i.e. comparison of effect of material on the light at two or more different wavelengths or wavelength bands
- G01N21/31—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry
- G01N21/314—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry with comparison of measurements at specific and non-specific wavelengths
- G01N2021/3148—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry with comparison of measurements at specific and non-specific wavelengths using three or more wavelengths
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- G—PHYSICS
- G01—MEASURING; TESTING
- 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
- G01N21/17—Systems in which incident light is modified in accordance with the properties of the material investigated
- G01N21/25—Colour; Spectral properties, i.e. comparison of effect of material on the light at two or more different wavelengths or wavelength bands
- G01N21/31—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry
- G01N21/314—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry with comparison of measurements at specific and non-specific wavelengths
- G01N2021/3155—Measuring in two spectral ranges, e.g. UV and visible
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Abstract
The invention discloses a device for simultaneously detecting black carbon, organic carbon and gas (certain gas such as nitrogen dioxide). Based on the photoacoustic effect, the invention uses a plurality of groups of lasers with different wavelengths, the lasers generate photoacoustic signals through the photoacoustic cell, and the plurality of groups of lasers can respectively measure black carbon, organic carbon and certain gas. The light intensity of the four lasers is modulated at different frequencies, the phase-locked amplifier demodulates the photoacoustic signals with corresponding wavelengths according to different modulation frequencies, and absorption coefficients of the particles at different wavelengths are inverted. According to different optical absorption characteristics of the black carbon and the organic carbon, the black carbon and the organic carbon are distinguished and measured. Compared with the traditional black carbon instrument, the invention provides a new technical means for directly detecting various natural suspended state particles on line, does not need to use a filter to collect the particles, reduces the influence on light intensity signals and improves the measurement accuracy.
Description
Technical Field
The invention belongs to the field of optical spectroscopy, and particularly relates to a device for simultaneously detecting black carbon, organic carbon and nitrogen dioxide based on a photoacoustic spectroscopy technology.
Background
The emissions of automobile exhaust and the like contain black carbon, organic carbon and some harmful gases. Black carbon and organic carbon in atmospheric particulates play an important role in climate change and environmental pollution. Atmospheric particulates directly affect the earth's gas system by scattering and absorbing solar radiation energy. Atmospheric particulates are transmitted to the pulmonary membranes of human bodies through respiratory tracts and permeate into respiratory systems, so that severe diseases such as respiratory asthma, cardiovascular diseases and the like are caused, and public health and safety are influenced. The greenhouse effect of black carbon is one third of that of carbon dioxide, and the effect on climate warming exceeds that of methane. The black carbon can strongly adsorb organic pollutants and heavy metals in the environment, is a transport carrier of toxic chemical substances, enters a human body through respiration, and seriously influences the health and safety of people. Research shows that 50% of aerosol radiation absorption in a specific ultraviolet-visible light band is derived from organic carbon, and the capability of the organic carbon to absorb short-wave radiation and the influence on atmospheric radiation balance still need to be further researched. In the atmosphere, organic carbon can be continuously oxidized, coagulated and nucleated due to the change of temperature, humidity and other environments to form photochemical smog, thereby affecting the health and safety of people.
At present, the main methods for monitoring the concentration of the atmospheric particulates comprise a ray attenuation method and a light scattering method, but the two methods cannot effectively distinguish black carbon and organic carbon components in the atmospheric particulates. The traditional technology for measuring black carbon and organic carbon is a black carbon instrument based on a filter technology, the black carbon instrument collects particulate matters by using a filter, and the concentration of the particulate matters is calculated by measuring the attenuation of the transmitted light intensity of the filter. The interaction of incident light and particles is influenced by multiple scattering and shadow of the filter, so that the accuracy of the measurement result of the instrument is reduced, and the technology enriches various aerosols in the measurement process, causes the form change of aerosol particles, changes the optical characteristics of the aerosols and leads the measurement accuracy of the filter technology to be 20-30%.
The photoacoustic spectroscopy technology based on the photoacoustic effect is a method for directly detecting the absorption characteristics of particles, has no background absorption, and is widely applied to the absorption characteristic measurement of the particles. The photoacoustic spectroscopy technology overcomes the filter influence in the filter technology, and the detection accuracy is improved to 5-10%. Therefore, the invention provides a device for simultaneously detecting black carbon and organic carbon based on the photoacoustic spectroscopy technology, and the device can simultaneously measure the change of the concentration of pollutant nitrogen dioxide in the environment.
Disclosure of Invention
Object of the Invention
The invention mainly provides a device for simultaneously detecting black carbon, organic carbon and certain gas (taking nitrogen dioxide as an example below) based on photoacoustic spectroscopy, and provides a new technical means for directly detecting particles in various natural suspension states on line without using a filter to collect the particles.
The technical scheme adopted by the invention
In order to solve the influence of a filter in the prior art on the measurement of particulate matters, the invention provides a device for simultaneously detecting black carbon, organic carbon and nitrogen dioxide based on photoacoustic spectroscopy, and the detection accuracy is improved to 5-10%.
The invention discloses a device for simultaneously detecting black carbon, organic carbon and nitrogen dioxide based on photoacoustic spectroscopy, which comprises a laser, a signal generator, a reflector, a band-pass optical filter, a photoacoustic cell, a preamplifier, a phase-locked amplifier, a data acquisition card, an optical power meter, an air inlet switching module and a sample pump. Light emitted by the first laser, the second laser, the third laser and the fourth laser is coupled together after passing through the reflecting mirror and the plurality of optical band-pass filters, enters the photoacoustic cell and is detected by the optical power meter; the light emitted by the first laser, the second laser, the third laser and the fourth laser is subjected to intensity modulation according to the signal frequency generated by the signal generator, the signal generated by the signal generator is connected with the phase-locked amplifier, a microphone is arranged in the photoacoustic cell and serves as a detector, the microphone is connected with the preamplifier, the output end of the preamplifier is connected with the phase-locked amplifier, and the output signal end of the phase-locked amplifier is collected by the data acquisition card and sent to the computer for storage; the air inlet switching module switches the first air inlet and the second air inlet to enable particles (black carbon and organic carbon) and nitrogen dioxide to separately enter the photoacoustic cell, and the air inlet rate is measured by the sample pump
In a further specific implementation, the first laser, the second laser, the third laser, and the fourth laser have wavelength bands of 880nm, 660 nm, 450 nm, and 405 nm, respectively, the light intensity is modulated at different frequencies, but all the light intensities are near the resonant frequency of the photoacoustic cell, and can generate corresponding photoacoustic signals, and the lock-in amplifier demodulates the material absorption coefficient measured by each laser according to different reference frequencies.
In a further specific implementation, the air inlet may also have a switching module, and an electromagnetic valve is adopted to enable an air sample (containing particulate matters and gas) and an air sample after filtering the particulate matters to respectively enter the photoacoustic cell, and a phase difference between two channel signals is a photoacoustic signal of the particulate matters.
In a further implementation, the photoacoustic signal of the particles generated by the first laser is used for inverting the black carbon concentration (at the wavelength of the first laser, the absorption of the particles is mainly caused by black carbon), and the photoacoustic signal of the particles generated by the second laser, the third laser and the fourth laser is used for inverting the absorption coefficient of the organic carbon after subtracting the photoacoustic signal corresponding to the measured black carbon concentration (which can be characterized by 2 constants K and ACC in formula (2)). And the absorption coefficients of the organic carbon measured by the second laser, the third laser and the fourth laser are used for further determining the characteristic of the optical absorption of the organic carbon along with the change of the wavelength. In the embodiment where the optical filter is switchable and has a filter with a thin film, the photoacoustic signal generated by the third laser can be directly used to invert the concentration of nitrogen dioxide.
In a further embodiment, the plurality of optical band-pass filters are incident at an angle (e.g., 45).
The invention has the advantages of
Compared with the prior art, the invention has the advantages that the invention avoids the collection of particles by using a filter of a traditional black carbon instrument, can directly detect particles in various natural suspension states on line, and reduces the measurement error to 5-10%; the four lasers are controlled to have different resonant frequencies in the photoacoustic cells, and simultaneously the absorption of the particles at four wavelengths is measured through the photoacoustic cells, so that the particle measurement accuracy is improved; the invention can detect black carbon, organic carbon and nitrogen dioxide simultaneously.
Drawings
FIG. 1 is a schematic view of the structure of the present invention.
Fig. 2 is a schematic diagram of the modulation frequency distribution of four lasers.
Description of reference numerals:
in fig. 1: 1-a first laser (880 nm); 2-a second laser (660 nm); 3-a third laser (450 nm); 4-fourth laser (405 nm); 5-a reflector; 6-optical band-pass filter; 7-an optical band-pass filter; 8-an optical band-pass filter; 9-a membrane filter; 10-a first air inlet; 11-air inlet II; 12-an intake air switching module; 13-sample pump; 14-a photoacoustic cell; 15-an optical power meter; 16-a preamplifier; 17-a lock-in amplifier; 18-a data acquisition card; 19-a computer; 20-signal generator.
Detailed Description
The present invention will be further described with reference to the following embodiments.
A device for simultaneously detecting black carbon, organic carbon and gas (taking nitrogen dioxide as an example) is characterized in that light intensities of lasers 1, 2,3 and 4 are respectively modulated at different resonant frequencies of a photoacoustic cell 14, and a phase-locked amplifier 17 demodulates acoustic signals caused by the corresponding lasers according to different laser modulation frequencies. The device adopts an air inlet switching module 12, and an air inlet I10 and an air inlet II 11 are switched with each other once every a period of time. When the air inlet 10 is switched to, particulate matters in the air are filtered by the thin film filter 9, the device measures the absorption of the gas in the air at 880nm, 660 nm, 450 nm and 405 nm, the gas absorption measured by the laser 3 is the absorption of nitrogen dioxide, and the concentration of the nitrogen dioxide in the air can be inverted according to the gas photoacoustic signal of the laser 3 demodulated by the phase-locked amplifier 17. When the gas inlet I11 is switched to the gas inlet II, particles and gas in the air enter the photoacoustic cell at the same time, the device measures the common absorption of the particles and the gas in the air, and the photoacoustic signal (the particles and the gas) measured at the moment is subtracted from the gas photoacoustic signal at the gas inlet I10 to obtain the photoacoustic absorption signal of the particles. The particle photoacoustic absorption signal generated by the laser 1 is used for inverting the black carbon concentration, the particle photoacoustic absorption signal generated by the black carbon and the organic carbon is measured by the lasers 2,3 and 4, and the particle photoacoustic signal generated by the second laser, the third laser and the fourth laser is used for inverting the organic carbon absorption coefficient after subtracting the photoacoustic signal corresponding to the measured black carbon concentration (which can be represented by 2 constants K and ACC in the formula (2)).
The invention is used for detecting pollutants black carbon, organic carbon and nitrogen dioxide simultaneously, and the specific concentrations of black carbon, organic carbon and nitrogen dioxide are inverted in the following specific description. Within the photoacoustic cell, the acoustic signal generated by the sample absorbing the energy of the incident light can be expressed as:
SPAS = P × M × Ccell×α + Sb (1)
in the formula SPASPhotoacoustic signal intensity (V) generated for absorption of light energy by particles or gases; p is laser power (W); m is the sensitivity of the microphone sensor (mV/Pa); ccellIs the cell constant (Pa.m.W) of the photoacoustic cell 14-1) The capacity of the photoacoustic cell for converting photon energy into photoacoustic signals is represented in relation to factors such as geometric parameters of the photoacoustic cell 14 and the like; absorption coefficient of sample alpha (Mm)-1)= α0× C, α0Is the absorption coefficient per sample concentration, C is the sample concentration, and when the sample is an aerosol, alpha is0The unit is g/m2C in g/m3(ii) a When the sample is a gas molecule, alpha0Has the unit of Mm-1Ppbv, with the unit C being ppbv; sbIs a background noise signal (V).
According to equation (1), the sensitivity (M) of the microphone sensor is a known parameter, the photoacoustic signal strength (S)PAS) Background noise signal (S)b) And laser power (P) is a parameter measured in an experiment, the photoacoustic cell constant can be calibrated by using gas with known concentration, and the absorption coefficient (alpha) of the particulate matter under four wavelengths (880 nm, 660 nm, 450 nm and 405 nm) can be measured in the experiment. The mass absorption coefficient alpha of black carbon at 880nm wavelength0Is 7.8 g/m2And combining the experimentally measured absorption coefficient (alpha) of the black carbon at the wavelength of 880nm, the mass concentration of the black carbon in the air can be obtained. The absorption coefficients of the black carbon and the organic carbon follow the law of power function along with the change of wavelength in the ultraviolet-visible light-near infrared band:
α=K·λ-ACC （2）
lambda is the wavelength, and K is the constant, and ACC is the absorption ngstrm coefficient of particulate matter, and the absorption angstrm coefficient of black carbon is 1, combines the absorption coefficient (alpha) of black carbon at 880nm wavelength, obtains the absorption coefficient of black carbon at 660 nm, 450 nm and 405 nm wavelength, and the absorption coefficient of the particulate matter measured in the experiment at 660 nm, 450 nm and 405 nm wavelength subtracts black carbon absorption coefficient and just is the absorption coefficient of organic carbon, and the organic carbon absorption coefficient that laser 2,3,4 measured is used for further confirming the characteristic that organic carbon optical absorption changes with the wavelength. The nitrogen dioxide concentration can be deduced from the gas absorption coefficient measured at a wavelength of 450 nm.
In this embodiment, the modulation frequencies of the lasers-1, 2,3 and 4 should be at the resonant frequency of the photoacoustic cell, and the modulation frequencies of the frequencies are different by 20Hz, as shown in FIG. 2.
Claims (4)
1. A device for simultaneously detecting black carbon, organic carbon and gas is characterized by comprising a plurality of groups of lasers (taking 4 lasers as an example below) with at least four different wavelengths, a reflector, a plurality of optical band-pass filters, a film filter, a first air inlet, a second air inlet, an air inlet switching module, a sample pump, a photoacoustic cell, an optical power meter, a preamplifier, a phase-locked amplifier, a data acquisition card, a computer and a signal generator; light emitted by the first laser, the second laser, the third laser and the fourth laser is incident to the photoacoustic cell and then detected by the optical power meter; the light emitted by the first laser, the second laser, the third laser and the fourth laser is subjected to intensity modulation according to the signal frequency generated by the signal generator, the signal generated by the signal generator is connected with the phase-locked amplifier, an acoustic detector (such as a microphone) is arranged in the photoacoustic cell, the acoustic detector is connected with the preamplifier, the output end of the preamplifier is connected with the phase-locked amplifier, and the output signal end of the phase-locked amplifier is collected by the data acquisition card and sent to the computer for storage; the gas inlet switching module switches the gas inlet I and the gas inlet II to enable particles (black carbon and organic carbon) and gas to be detected (such as nitrogen dioxide) to separately enter the photoacoustic cell, and the gas inlet speed is controlled by the sample pump.
2. The apparatus according to claim 1, wherein the gas to be detected is nitrogen dioxide, and the apparatus is characterized in that the first laser, the second laser, the third laser, and the fourth laser have wavelength bands of 880nm, 660 nm, 450 nm, and 405 nm, respectively, the light intensity is modulated at different frequencies, but all around the resonant frequency of the photoacoustic cell, and can generate corresponding photoacoustic signals, and the lock-in amplifier demodulates the absorption coefficient of the substance measured by each laser according to different reference frequencies.
3. The apparatus according to claim 1, wherein the air inlet switching module employs a solenoid valve to make the air sample (containing particles and gas) and the air sample filtered by the membrane filter enter the photoacoustic cell respectively, and the difference between the two channels of photoacoustic signals is a photoacoustic signal of the particles.
4. The device as claimed in claim 1, wherein the light emitted from the first, second, third and fourth lasers passes through the reflecting mirror and the plurality of optical band pass filters and then is coupled together and simultaneously incident on the photoacoustic cell, or each laser passes through the photoacoustic cell sequentially by using a switch, and the plurality of optical band pass filters are incident at a certain angle (e.g. 45 °).
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