CN102435567A - Method for measuring gas component concentration in inverse calculation mode based on differential optical absorption spectrum - Google Patents
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- 238000000034 method Methods 0.000 title claims abstract description 40
- 238000000862 absorption spectrum Methods 0.000 title claims abstract description 35
- 230000003287 optical effect Effects 0.000 title abstract description 4
- 239000007789 gas Substances 0.000 claims abstract description 62
- 238000010521 absorption reaction Methods 0.000 claims abstract description 48
- 238000001658 differential optical absorption spectrophotometry Methods 0.000 claims abstract description 28
- 230000003595 spectral effect Effects 0.000 claims abstract description 15
- 238000005259 measurement Methods 0.000 claims abstract description 8
- 238000004458 analytical method Methods 0.000 claims abstract description 5
- 238000001228 spectrum Methods 0.000 claims description 17
- 238000012417 linear regression Methods 0.000 claims description 15
- 238000001514 detection method Methods 0.000 claims description 7
- 239000000523 sample Substances 0.000 claims description 7
- 238000003556 assay Methods 0.000 claims description 6
- 239000000428 dust Substances 0.000 claims description 4
- 230000001419 dependent effect Effects 0.000 claims description 3
- 239000008187 granular material Substances 0.000 claims description 3
- 230000010354 integration Effects 0.000 claims description 3
- 238000012887 quadratic function Methods 0.000 claims description 3
- 239000004071 soot Substances 0.000 claims description 3
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 abstract description 5
- 239000003546 flue gas Substances 0.000 abstract description 5
- 239000003344 environmental pollutant Substances 0.000 abstract 1
- 231100000719 pollutant Toxicity 0.000 abstract 1
- 238000005516 engineering process Methods 0.000 description 8
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 6
- 238000011160 research Methods 0.000 description 6
- 239000000203 mixture Substances 0.000 description 5
- 238000012544 monitoring process Methods 0.000 description 5
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 4
- 238000013461 design Methods 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000003500 flue dust Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 239000000779 smoke Substances 0.000 description 2
- 239000005436 troposphere Substances 0.000 description 2
- 241000139306 Platt Species 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 238000002835 absorbance Methods 0.000 description 1
- 230000002745 absorbent Effects 0.000 description 1
- 239000002250 absorbent Substances 0.000 description 1
- 239000011358 absorbing material Substances 0.000 description 1
- 238000003915 air pollution Methods 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 239000012141 concentrate Substances 0.000 description 1
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- 238000012827 research and development Methods 0.000 description 1
- 238000005070 sampling Methods 0.000 description 1
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Abstract
The invention relates to a method for measuring gas component concentration in an inverse calculation mode based on a differential optical absorption spectrum. In the method for measuring the gas component concentration in the inverse calculation mode based on the differential optical absorption spectrum, a mathematic model is established and solved by a least square method, the contents of various pollutants in flue gas can be recorded in real time, and the gas which comprises unknown components can be determined. Meanwhile, the invention provides a solution scheme aiming at main factors which influence the precision of differential optical absorption spectroscopy (DOAS), analysis errors due to spectral line shift can be effectively reduced, and the precision problem of the gas component concentration measurement in which absorption spectral lines are superposed is solved.
Description
Technical field
The present invention relates to a kind of absorption line has the assay method of overlapping gas component concentrations.
Background technology
The eighties in 20th century, Platt etc. are applied to difference absorption spectrum technology (DOAS) in the atmospheric research of troposphere.From then on, the DOAS technology has obtained fast development, and many research institutions are according to the research characteristics of oneself, Application of DO AS technical design instrument.These application comprise air pollution monitoring, volcanic gas analyse atmos troposphere, stratosphere gas composition monitoring etc.
To the end of the eighties; The DOAS technology is extensively approved as the gas detection means; OPSIS company has confirmed the basic structure of DOAS system, and other companies also release the commercial DOAS system of oneself one after another, and on structure, hardware, software algorithm, have proposed a lot of improvement thinkings.Nineteen ninety, Axelson etc. have at first adopted Cassegrain telescope designs simplification device.1992, John M.C etc. adopted photodiode array (PDA) to replace photomultiplier (PMT), gather spectroscopic data fast, and had realized the robotization of measuring.Nineteen ninety-five, Theo Brauers etc. has improved between the pixel that the PDA detector brings difference to the influence of measurement result.1996; Stutz etc. improve the retrieving concentration method, in order to eliminate spectral shift, stretching and the compression influence to measuring, adopt least square and nonlinear Levenberg-Marquardt method; The algorithm that replaces the pure linearity of forefathers has improved the accuracy of measurement result.2000, Ahilleas etc. proposed the retrieving concentration method to high meticulous spectrum.Different structure, different detectors, the proposition of algorithms of different and application have promoted the development of DOAS technology.
At present, the DOAS systematic research mainly concentrates on Sweden (the OPSIS_DOAS system of OPSIS AB company), Germany (the HMT DOAS system of Heidelberg university and the exploitation of Hoffmann company), the U.S. (the DOAS2000 system of thermal environment research institute), France (the DOAS system of Environment SA exploitation) and Russia states such as (the DOAS 4R of Eridan-1 Science & Technology Center exploitation).
The DOAS technology just is being based on gas with various has differing absorption spectrum to light, is called gas " fingerprint " absorption characteristic to light, distinguishes different materials, measures their concentration.
In atmospheric research; As shown in Figure 1; The light beam that light source sends
is through the decay of certain light path; Light intensity after the decay of drawing can be arranged in principle; But ignored the existence of a lot of other delustring factors in the actual measurement Chinese style; The Rayleigh scattering (
) that comprises gas molecule; Gasoloid Mie scattering (
) and atmospheric disturbance factors such as
, adopt the Lambert-Beer's law of revising to be written as:
Wherein: the delustring that
expression is caused by Rayleigh scattering: incident light dimension less than the particulate of optical wavelength on after the scattering scattered light go out and the lambda1-wavelength same light; Mainly be the scattering owing to air molecule in atmosphere, light is scattered out light path and can't be received." absorption " cross section that Rayleigh scattering is brought can be expressed from the next:
C representes atmospheric molecular concentration, δ
0≈ 4.4 * 10
-16Cm
2Nm
4
The delustring that
expression is caused by Mie scattering: the scattering that when incident light runs into the diameter particulate suitable with lambda1-wavelength, takes place; Mainly be a large amount of particulates that exist in the air, flue dust etc. cause.Mie scattering can be expressed as:
An original smoke absorption spectrum has not only comprised the absorption spectrum of dusty gas, has also comprised its delustring factor information, and when light during through the flue gas of certain light path, and the light intensity attenuation that is caused by Rayleigh scattering and Mie scattering is often greater than molecule absorption.These have all hindered the application Lambert-Beer's law and have directly measured flue gas concentration on principle.For the concentration that obtains all gases need be separated various decay factors.A basic thought of DOAS technology is exactly to be divided into two parts to the absorption cross section of gas:
Wherein: on behalf of absorption cross section,
slowly change part with wavelength to be called broadband spectral,
represent absorption cross section to change rapidly partly to be called narrow-band spectrum with wavelength.And Rayleigh scattering in the atmospheric attenuation, Mie scattering and atmospheric disturbance all slowly change with wavelength, and this two-part separation can realize through certain mathematical processing, utilizes the arrowband part that does not contain Rayleigh scattering and Mie scattering information to calculate absorbing material concentration.Order:
Then have
Wherein: all change composition slowly with wavelength to have comprised absorption spectrum in
,
comprised with the fast composition that changes of wavelength.This separation can fit realization (like Fig. 2) with certain digital filtering or polynomial expression.
Thereby have:
Eliminated flue dust for this, the absorption formula of factor affecting such as greasy dirt analyzes that wherein gas componant and content are just easier again.
The present invention seeks to and will therefore need measure the sulphuric dioxide absorption spectrum the monitoring of sulfur dioxide gas body burden in the flue, NO is as influencing SO at ultraviolet band
2The main flue gas that absorbs, its absorption cross section spectrum also need measured.
Different temperatures, under the different resolution condition, the absorption cross section of sulphuric dioxide is repeatedly measured by forefathers.Wameck has measured the interval SO of 185-315nm
2Absorption spectra.People such as Joens have measured 197-240nm and the interval SO of 228-339nm
2Absorption cross section.McGee etc. have measured the interval SO of 300-325nm under 295K and the 210K temperature
2Absorption cross section, and pointed out the influence of temperature to absorption cross section.Tompson has measured the high-resolution SO of 265-331nm
2Absorption cross section.Ahmed and Kumar have measured 188-231nm and 278-320nmSO
2Absorption spectrum.People such as A.C.Vandaele utilize high-resolution to get fourier spectrometer and have measured the SO of wavelength at 250-370nm
2Absorption cross section.
Equally, for the absorption cross section of NO, 200-230nm wave band absorption cross section when Trada H measured 700K, when Mellqvist J has measured 298K and 670K, 200-230nm wave band absorption cross section.
Fig. 3, Fig. 4 are to 340nm wave band, SO 200
2The absorption curve of gas.NO is as shown in Figure 5 at 200-230nm wave band absorption cross section.
Can know SO from Fig. 3～Fig. 5
2With NO in this wavelength band of 200～230nm, significantly overlap of spectral lines is arranged comparatively.Because the dusty gas of usually measuring all is the mixed gas of two kinds of gases, how in combination gas, carry out active data and separate, be the key factor that final measuring accuracy is measured in influence.
Summary of the invention
In order to solve the problem of difference absorption spectrum technology (DOAS) precision; The purpose of this invention is to provide a kind of gas component concentrations inverting and calculate assay method based on difference absorption spectrum; This method proposed solution to influence technological (DOAS) accuracy factors of difference absorption spectrum, solved the precision problem that absorption line has the mensuration of overlapping gas component concentrations.
In order to realize above-mentioned purpose, the technical scheme below the present invention has adopted:
Assay method is calculated in gas component concentrations inverting based on difference absorption spectrum, and this method comprises the steps:
1) light source sends the incident light of light intensity for
; Through gas absorption and soot dust granule scattering, arriving the end of probe light intensity after the gas disturbance has according to Lambert-Beer's law:
2) light that intensity is
is received by the detection system of spectra re-recorded through behind the spectrograph slit; Because the diffraction spectrum shape of slit changes, this process is the convolution of spectral signal and apparatus function H:
3) according to the resolution of spectrometer, what detection system write down is certain interval interior light intensity integration:
4) owing to adopt bifocal path structure, the ratio of light path and the reference path of in spectra collection, directly being absorbed is the absorption spectrum of gas;
To I
'And I
0Ratio take the logarithm:
S wherein
i' (j) the i.e. Difference Absorption structure of i kind gas;
Gather light intensity through output after the monochromator system by photodetector, the DOAS data handling procedure is found the solution parameter c exactly
iProcess, utilize least square method to find the solution.
As further improvement; Above-mentioned least square method is found the solution the absorption that has comprised n kind gas in spectral line of hypothesis; On the spectrum of being studied, can get m usually; Individual sampled point; M>n, system of equations
is exactly a ultra positive definite system of equations like this, for all sampled points in the spectral line following system of equations is arranged: order
System of equations
The equation number is greater than the independent variable number in the following formula; Whole process can mathematical description be: known dependent variable is that Difference Absorption intensity relies on n independent variable, the Difference Absorption cross section of n kind gas, and oneself knows that large sample adds up to m now; M passage or sampled point; Ask the influence coefficient of each independent variable, obviously this is a multiple linear regression model, is the regression coefficient that will calculate;
The definite of multiple linear regression model coefficient can utilize least square fitting, can be the one-variable linear regression problem with the multiple linear regression problem reduction, and its model is:
Through m group measurement data (x1, y1) ... (xm ym) confirms regression coefficient a and b; If accurate linear relationship is arranged between x and the Y;
then should be arranged; I=1,2...m; But because measuring error and other influence of random disturbance; Generally
; Therefore confirm that another straight line promptly confirms one group of a and b, make on this straight line " approaching " all data points; Here introduce residual error (ei, i=1,2 ... M) describe the degree of " approaching ", residual error is exactly the deviation of observed value Y and regressand value y;
Least square method selects a and b to make E exactly, reaches minimum, and at this moment the regression straight line of gained and all observed value are the most approaching; Because Q is the quadratic function about a and b, so its minimum value must exist, according to the method for asking extreme value in the infinitesimal analysis, a and b should satisfy the equation group:
Find the solution this system of equations and promptly can obtain regression coefficient a and b; For multiple linear regression, according to the least square principle; According to the least square principle, finding the solution above-mentioned system of equations has:
Can obtain all gases concentration.
The present invention is directed at present domestic to the main existing inconvenience of method that adopts the gas sampling fiting chemical to analyze of flue dusty gas monitoring; And the low present situation of accuracy; Research and development has the overlapping real-time checkout equipment of gas component concentrations gas concentration based on the absorption line of DOAS (DOAS); Ultraviolet-visible DOAS (DOAS) is a kind of novel online smoke emissioning pollution thing feasible method of monitoring automatically; It can carry out continuous coverage to multiple gases simultaneously under the prerequisite that does not change the tested sample composition.To the absorption spectra data that obtains by Computer Processing, but the content of all contaminations in the real time record flue gas and is judged the gas of principal component not.Simultaneously, this patent has proposed solution to influence technological (DOAS) accuracy factors of difference absorption spectrum, can reduce the analytical error that spectral line shift brings effectively, has solved the precision problem that absorption line has the mensuration of overlapping gas component concentrations.
Description of drawings
Fig. 1 is the ultimate principle figure of DOAS technical measurement.
Fig. 2 is the collection of illustrative plates of the arrowband part and the broadband part of absorption spectrum absorption cross section.
Fig. 3 is SO
2At 200-230nm wave band absorption cross section collection of illustrative plates.
Fig. 4 is SO
2At 280-320nm wave band absorption cross section collection of illustrative plates.
Fig. 5 is that NO is at 200-230nm wave band absorption cross section.
The DOAS system of Fig. 6 flue of the present invention.
Fig. 7 is 961ppm concentration SO
2Absorption spectrum.
Fig. 8 is 961ppmSO
2Difference absorption spectrum.
Fig. 9 is 200-230nm wave band SO
2With NO blended absorbent spectrum.
Figure 10 is 200-230nm wave band SO
2With NO mixing difference absorption spectrum.
Embodiment
DOAS system according to the described flue of Fig. 6; Light source sends the incident light of light intensity for
; Through gas absorption and soot dust granule scattering, arriving the end of probe light intensity after the gas disturbance has according to Lambert-Beer's law:
The light that intensity is
is through being received by the detection system of spectra re-recorded behind the spectrograph slit, because the diffraction spectrum shape of slit changes.This process is the convolution of spectral signal and apparatus function H:
According to the resolution of spectrometer, what detection system write down is certain interval interior light intensity integration:
This paper contrived experiment is owing to adopt bifocal path structure, and the ratio of light path and the reference path of in spectra collection, can directly being absorbed is the absorption spectrum of gas.
To I
'And I
0Ratio take the logarithm:
S wherein
i' (j) the i.e. Difference Absorption structure of i kind gas.
Gather light intensity through output after the monochromator system by photodetector, the DOAS data handling procedure is found the solution parameter c exactly
iProcess, utilize least square method to find the solution.
Above-mentioned least square method is found the solution the absorption that has comprised n kind gas in spectral line of hypothesis; On the spectrum of being studied, can get m usually; Individual sampled point; M>n; System of equations
is exactly a ultra positive definite system of equations like this, for all sampled points in the spectral line following system of equations is arranged: order
，
，
(7)
System of equations
The equation number is greater than the independent variable number in the following formula; Whole process can mathematical description be: known dependent variable is that Difference Absorption intensity relies on n independent variable, the Difference Absorption cross section of n kind gas, and oneself knows that large sample adds up to m now; M passage or sampled point; Ask the influence coefficient of each independent variable, obviously this is a multiple linear regression model, is the regression coefficient that will calculate;
The definite of multiple linear regression model coefficient can utilize least square fitting, can be the one-variable linear regression problem with the multiple linear regression problem reduction, and its model is:
Through m group measurement data (x1, y1) ... (xm ym) confirms regression coefficient a and b; If accurate linear relationship is arranged between x and the Y;
then should be arranged; I=1,2...m; But because measuring error and other influence of random disturbance; Generally
; Therefore confirm that another straight line promptly confirms one group of a and b, make on this straight line " approaching " all data points; Here introduce residual error (ei, i=1,2 ... M) describe the degree of " approaching ", residual error is exactly the deviation of observed value Y and regressand value y;
Least square method selects a and b to make E exactly, reaches minimum, and at this moment the regression straight line of gained and all observed value are the most approaching; Because Q is the quadratic function about a and b, so its minimum value must exist, according to the method for asking extreme value in the infinitesimal analysis, a and b should satisfy the equation group:
Find the solution this system of equations and promptly can obtain regression coefficient a and b; For multiple linear regression, according to the least square principle; According to the least square principle, finding the solution above-mentioned system of equations has:
(11)
Can obtain all gases concentration.
With the experimentation is the process of resolving of example explanation algorithm, with SO
2Overlapping gas is arranged as practical measuring examples with these two kinds of NO at 200 to 230nm wave bands.
In gas cell, charging into concentration respectively is 152ppm, 195ppm, 295ppm, the standard SO of 961ppm and 1970ppm
2Gas, and on the quartz glass of absorption cell both sides, be coated with and spread dust, other delustring factors in the greasy dirt analog flue.Their absorption spectrum (is example with 961ppm) of record is like Fig. 7 in 280 to 320nm wave bands; Red curve is the casual part that changes of absorption spectrum among the figure; It is that match obtains through quintic curve by the absorption spectrum that collects; Article two, to subtract each other the gas difference absorption spectrum that is absorbed be fast variations (Fig. 8) in the spectrum to curve, realizes separating of absorption spectra data and background data.
For single composition SO that plants
2Gas system of equations (8) can be written as:
(9)
Wherein
is light path; Be known quantity, can find the solution c with least square method equally and make the system of equations variance after finding the solution:
minimum.
According to experimental data, substitution
formula least square method solves sulfur dioxide concentration.
Arrive 230nm wave band, SO 200
2All have absorption with NO, 260ppm sulphuric dioxide and the nitric oxide production mixed gas absorption spectrum of 940ppm (as shown in Figure 9) have been gathered in experiment.
Fit through five times equally and subtract each other, obtain shown in the difference absorption spectrum (like Figure 10).
According to inversion algorithm as stated, utilize least square method to find the solution, system of equations (8) can be written as:
(10)
Wherein A is the absorption spectrum absorbance data,
Be sulphuric dioxide Difference Absorption cross-section data, corresponding c
1Be sulphuric dioxide concentration to be measured,
Be nitric oxide production Difference Absorption cross-section data, corresponding c
2Be nitrogen monoxide concentration to be measured, inversion solution gets:
C
1=247.4ppm, C
2=965.2ppm and actual concentrations ratio error mutually are respectively 4.85% and 2.68%.
Claims (2)
1. calculate assay method based on the gas component concentrations inverting of difference absorption spectrum, it is characterized in that this method comprises the steps:
1) light source sends the incident light of light intensity for
; Through gas absorption and soot dust granule scattering, arriving the end of probe light intensity after the gas disturbance has according to Lambert-Beer's law:
2) light that intensity is
is received by the detection system of spectra re-recorded through behind the spectrograph slit; Because the diffraction spectrum shape of slit changes, this process is the convolution of spectral signal and apparatus function H:
3) according to the resolution of spectrometer, what detection system write down is certain interval interior light intensity integration:
4) adopt bifocal path structure, the ratio of light path and the reference path of in spectra collection, directly being absorbed is the absorption spectrum of gas;
To I
'And I
0Ratio take the logarithm:
S wherein
i' (j) the i.e. Difference Absorption structure of i kind gas;
Gather light intensity through output after the monochromator system by photodetector, the DOAS data handling procedure is found the solution parameter c exactly
iProcess, utilize least square method to find the solution.
2. assay method is calculated in the gas component concentrations inverting based on difference absorption spectrum according to claim 1; It is characterized in that least square method finds the solution the absorption that has comprised n kind gas in spectral line of hypothesis; On the spectrum of being studied, can get m usually; Individual sampled point; M>n, system of equations
is exactly a ultra positive definite system of equations like this, for all sampled points in the spectral line following system of equations is arranged: order
System of equations
The equation number is greater than the independent variable number in the following formula; Whole process can mathematical description be: known dependent variable is that Difference Absorption intensity relies on n independent variable, the Difference Absorption cross section of n kind gas, and oneself knows that large sample adds up to m now; M passage or sampled point; Ask the influence coefficient of each independent variable, obviously this is a multiple linear regression model, is the regression coefficient that will calculate;
The definite of multiple linear regression model coefficient can utilize least square fitting, can be the one-variable linear regression problem with the multiple linear regression problem reduction, and its model is:
Through m group measurement data (x1, y1) ... (xm ym) confirms regression coefficient a and b; If accurate linear relationship is arranged between x and the Y;
then should be arranged; I=1,2...m; But because measuring error and other influence of random disturbance; Generally
; Therefore confirm that another straight line promptly confirms one group of a and b, make on this straight line " approaching " all data points; Here introduce residual error (ei, i=1,2 ... M) describe the degree of " approaching ", residual error is exactly the deviation of observed value Y and regressand value y;
Least square method selects a and b to make E exactly, reaches minimum, and at this moment the regression straight line of gained and all observed value are the most approaching; Because Q is the quadratic function about a and b, so its minimum value must exist, according to the method for asking extreme value in the infinitesimal analysis, a and b should satisfy the equation group:
Find the solution this system of equations and promptly can obtain regression coefficient a and b; For multiple linear regression, according to the least square principle; According to the least square principle, finding the solution above-mentioned system of equations has:
Can obtain all gases concentration.
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Application publication date: 20120502 |