CN109883931B - PM (particulate matter)2.5Online source analysis method and measurement system - Google Patents
PM (particulate matter)2.5Online source analysis method and measurement system Download PDFInfo
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Abstract
The invention discloses a PM2.5 online source analysis method and a measurement system, wherein the measurement system comprises a laser, a polarization beam splitter, a wave plate, a plano-convex cylindrical lens, a measurement cavity, a multi-angle Stokes vector measurement device and a signal acquisition card, wherein the laser, the polarization beam splitter, the wave plate and the plano-convex cylindrical lens are positioned on the same straight line, and a light trap is arranged behind the measurement cavity; the multi-angle Stokes vector measuring device is arranged along the periphery of the measuring cavity and connected with a signal acquisition card, and the signal acquisition card is connected with a computer. The invention can be applied to PM alone2.5Online source parsing; meanwhile, the physical information of the particles acquired by the measurement system can be used together with a single-particle mass spectrometer and jointly applied to PM2.5Online source parsing; the whole system is simple in device and lower in cost; the maximum particle data of 3000 particles can be detected per second, rapid online source analysis monitoring can be realized, and the time resolution reaches the minute level; is suitable for large-scale popularization and application in various regions.
Description
Technical Field
The invention relates to the technical field of environment monitoring devices, in particular to a PM (particulate matter) monitoring device2.5Provided are an online source analysis method and a measurement system.
Background
PM2.5Pollution is a common concern in China and even all over the world, and is closely related to normal travel and physical health of people. With PM2.5Maturity and application of concentration monitoring technology, how to effectively control and reduce PM2.5Pollution has become a major concern to society. PM (particulate matter)2.5The source analysis means qualitative or quantitative recognition of the source of atmospheric particulate pollution in environmental receptors by chemical, physical, mathematical and other methods, is the basis and premise for scientifically and effectively developing dust haze prevention and control, and is an important basis for the national government to make an air quality standard-reaching plan.
Common analytical models for atmospheric particulate sources include emission inventory, diffusion models, and receptor models. The emission list is also called as a source emission list method, which is to investigate and count pollution sources on a specific time and space scale, and establish a pollution source list database according to activity levels and emission factor models of different source classes, so as to evaluate the emission amount of the different source classes to determine main pollution sources. The emission list is mainly used for large regional research of countries, cities and the like, and certain errors exist when the emission list is applied to small regions such as districts, counties, industrial districts and the like; the diffusion model is also called a source model, starts from a pollution source, simulates or predicts the time-space distribution of the concentration of the particulate matters under different meteorological conditions under the condition that the emission amount or emission intensity of each pollution source is determined, estimates the contribution condition of different pollution sources to the concentration of the pollution through simulating the processes of conveying, reacting, clearing and the like of the particulate matters in the horizontal direction and the vertical direction, and can establish a good quantitative relation between the fixed or mobile pollution source and the concentration of the atmospheric particulate matters. The diffusion model has the limitations that the diffusion model depends on local meteorological data, the result inaccuracy is caused by meteorological data errors, the diffusion model cannot be used for an open source with uncertain strength and a large-scale particle open source, and the diffusion model is generally applied to the spatial distribution of primary atmospheric particles in a small area; the receptor model mainly determines the contribution of the pollution source to the receptor by analyzing the chemical compositions of the receptor and the pollution source sample, and can be divided into a source-unknown receptor model and a source-known receptor model according to whether detailed source class information is required or not.
Based on the prior art, the combination of continuous observation and source analysis model of chemical components is PM2.5The main means of online source parsing. Due to PM2.5Due to the complexity of sources and the rapid change of weather systems, the chemical components and concentration levels of the atmospheric pollutants are evolved in real time, the pollution change process of the atmospheric pollutants can not be mastered under high time resolution, and the essential reasons and the formation mechanism of the atmospheric PM2.5 pollution can not be deeply known and monitored, so that the online source analysis can play an important role in early warning, prevention and control of the heavy pollution process conveniently.
At present, there are two kinds of automatic instruments applied to online source analysis: one is based on continuous observation of components of the aerosol mass spectrum; the other is continuous component observation based on 3 types of online instrument combinations, namely an online ion chromatography (water-soluble ions), an online EC/OC and an online heavy metal instrument. In China, aerosol mass spectrometry, particularly single-particle aerosol flight time mass spectrometry (SPAMS), is widely applied to component characteristic analysis and source analysis, while the second research is focused on off-line/on-line method comparison, cause and rule analysis in a heavy pollution process and the like, and the research of applying 3 types of chemical component on-line observation data to a receptor model to analyze a pollution source is rare.
In China, the Hexin PM2.5On line source analysis mass spectrum monitoring system as representative, PM is realized by using single particle mass spectrum detection technology2.5Online source resolution has been developed in more than one hundred cities in China. The system is generally sold at a price of over 400 ten thousand yuan, and mass spectrum information of about 20 particles can be detected every second, but the following problems generally exist in the source analysis system: 1. the price is high, and most of the urban and regional finances cannot be borne, so that the large-scale application is difficult; 2. the chemical characteristic-based receptor analytical model needs to depend on a large amount of chemical composition information of particulate matters and single-particle mass spectrumThe instrument can detect mass spectrum information of about 20 particles at most every second, the data volume is small, and the error of a source analysis result is large easily; 3. with increasingly complex air pollution conditions in China, the source analysis method based on chemical composition characteristics cannot meet all requirements, and particularly, the problem that different pollution sources have collinear characteristics is large in error, so that the online source analysis method based on various information sources and technical means is strengthened to be gradually paid attention by researchers.
The physical characteristics of the particles include particle size, complex refractive index, morphology, structure and the like. In recent years, a source analysis technology based on comprehensive characteristics of particulate matters is more and more emphasized, and physical characteristic information of the particulate matters is gradually applied to source analysis of the particulate matters. The particulate matters emitted from different pollution sources are different in generation mechanism and process, so that the physical characteristic distribution of the particulate matters is different, and thus, large errors are generated in measurement and source analysis.
Disclosure of Invention
The invention aims to solve the technical problem of providing a PM which is low in cost, can quickly analyze online sources and is beneficial to industrialization aiming at the defects of the prior art2.5An online source analysis method and a measurement system.
In order to solve the technical problems, the invention adopts the following technical scheme: PM (particulate matter)2.5The measuring system comprises a laser, a polarization beam splitter, a wave plate, a plano-convex cylindrical lens, a measuring cavity, a multi-angle Stokes direction measuring device and a signal acquisition card, wherein the laser, the polarization beam splitter, the wave plate and the plano-convex cylindrical lens are positioned on the same straight line; one end of the plane of the plano-convex cylindrical lens faces the measuring region, and the other end of the convex surface faces the wave plate; the multi-angle Stokes direction measuring device is arranged along the periphery of the measuring cavity and forms a plurality of scattered light measuring angles of the measured particles in the measuring cavityDegree; the multi-angle Stokes vector measuring device is connected with a signal acquisition card, and the signal acquisition card is connected with a computer.
The core of the system is that single particle polarization physical characteristic information is obtained through polarization detection; and obtaining an online source analysis result by using the polarization physical characteristic information of the particle group through a corresponding algorithm.
Preferably, the measuring angles of the multi-angle stokes vector measuring device include, but are not limited to, 10 degrees, 30 degrees, 60 degrees, 85 degrees and 115 degrees, so that stokes vector detection of multi-angle scattered light can be realized, and the information quantity is rich.
Further, the polarization beam splitter and the wave plate combination can be modulated into any linear polarization, circular polarization and elliptical polarization according to actual measurement requirements.
Further, the stokes vector measuring device measures including but not limited to horizontal linear polarization, vertical linear polarization, 45 degree linear polarization and circular polarization.
PM based on aforementioned measurement system2.5The online source analysis method is an online source analysis algorithm based on the polarization physical characteristics of particulate matters, and is divided into two stages:
the first stage is the establishment of a polarized physical characteristic spectrum of a pollution source, and the process is as follows, wherein m kinds of main pollution sources are provided:
1) scattering PM using multi-angle polarized light2.5The single particle measuring system collects m kinds of particles discharged by pollution sources, and each particle collects n paths of polarization index signals, equivalently uses an n-dimensional polarization physical characteristic vector [ a ]1,a2,...,an]Describing a particulate; respectively counting the probability distribution p of n polarization indexes of each pollution source particulate matteri,jI.e. the j path polarization physical characteristic probability distribution of the ith pollution source particulate matter, defining pi,jThe method comprises the steps that (i is 1,2, the.. multidata m, j is 1,2, the.. multidata n) is collected to be a pollution source multi-dimensional polarization physical characteristic distribution database; p is a radical ofi(aj) The j-th polarization index of the particles is expressed as ajProbability of particulate matter being assigned to the i-th source of pollution, pi(aj) Can pass through the establishedProbability distribution p ofi,jLooking up a database to obtain;
2) respectively calculating the probability P of each particle belonging to each pollution sourceiThe calculation formula is as follows:
(j ═ 1.., n), defines PiThe maximum term is the single particle recognition result of the particulate matter;
3) respectively counting the single particle identification results of M particles for each pollution source, normalizing the counting results to obtain a pollution source polarization identification fingerprint spectrum Ki(i＝1,2,...,m)，KiThe basic form of (A) is: ki＝[k1,k2,...,km]，KiThe physical meaning is as follows: for the i-th pollution source particulate matter, there is k1The single particle in the ratio is identified as coming from the 1 st contamination source, with k2A single particle of a proportion is identified as being from a 2 nd source of contamination. Wherein the content of the first and second substances,
the second stage is PM2.5The algorithm flow of online source analysis is as follows:
1) scattering PM using multi-angle polarized light2.5Single particle measuring device for collecting and measuring PM in ambient air2.5(ii) particulate matter data;
2) calculating the probability P of each particulate matter belonging to each pollution sourceiThe calculation formula is as follows:
(i ═ 1, 2.., m), defines PiThe maximum term is the single particle recognition result of the particulate matter;
3) counting and normalizing the single-particle identification results of all the particles in one measurement period, wherein the result is defined as the polarization identification fingerprint of the currently measured particles and counted as K ═ K1,k2,...,km]The physical meaning of the method is that k is actually measured in the particles1The single particles in the ratio are identified as being from type 1A source of contamination having k2A single particle of a proportion is identified as being from a 2 nd source of contamination. Also satisfies
4) The polarization recognition fingerprint of the actually measured particulate matter is equivalent to the linear superposition of the polarization recognition fingerprint of the known pollution source, which is shown as the following formula:
the online source analytic model is equivalent to solving the optimal solution of the equation
Make | | e | non-calculation2Minimum;
in order to avoid obtaining abnormal conditions such as negative solutions, the following constraint conditions are introduced:
adopting a Lagrange optimization method to solve to obtain an online source analysis result
In step 1) of the first stage, n is ≦ 20.
A pollution source multi-dimensional polarization characteristic distribution database and a pollution source polarization identification fingerprint database which are established in the steps of the first stage are data bases for realizing online source analysis in the second stage; the data spectrum base is related to the actual pollution source lists of all regions, and can be updated regularly according to actual conditions.
The method and the measuring system provided by the invention can be independently applied to PM2.5Online source parsing; meanwhile, the physical information of the particles acquired by the measuring system is used as the chemical components of the existing particlesAn innovative complement to the system, which can be used in conjunction with single particle mass spectrometers for common application to PM2.5Online source parsing; the whole system is simple in device and lower in cost; the maximum particle data of 3000 particles can be detected per second, rapid online source analysis monitoring can be realized, and the time resolution reaches the minute level; is suitable for large-scale popularization and application in various regions.
Drawings
FIG. 1 is a schematic view of a measurement system according to the present invention;
FIG. 2 is a flow chart of the analytic method of the present invention;
FIG. 3 is a flow chart of the establishment of the polarization spectrum library of the pollution source according to the present invention;
FIG. 4 is a flow chart of an online source resolution algorithm of the present invention;
FIG. 5 is a bar graph of statistical results of online analytical testing errors for the mixture of 4 contamination sources according to the present invention.
In fig. 1, 1 is a laser, 2 is a polarization beam splitter, 3 is a wave plate, 4 is a plano-convex cylindrical lens, 5 is a measurement cavity, 6 is a light trap, 10 is a multi-angle stokes vector measuring device, and 11 is a signal acquisition card.
Detailed Description
In this embodiment, referring to fig. 1, the PM2.5 online source analysis method and measurement system includes a laser 1, a polarization beam splitter 2, a wave plate 3, a plano-convex cylindrical lens 4, a measurement cavity 5, a multi-angle stokes direction measurement apparatus 10, and a signal acquisition card 11, where the laser 1, the polarization beam splitter 2, the wave plate 3, and the plano-convex cylindrical lens 4 are located on a straight line, the polarization beam splitter 2 is aligned with an irradiation port of the laser 1, the wave plate 3 is disposed behind the polarization beam splitter 2, the plano-convex cylindrical lens 4 is disposed behind the wave plate 3, the measurement cavity 5 is located behind the plano-convex cylindrical lens 4, a light trap 6 is disposed behind the measurement cavity 5, and the light trap 6, the plano-convex cylindrical lens 4, the wave plate 3, and the polarization beam splitter 2 are located on a straight line; one end of the plane of the plano-convex cylindrical lens 4 faces the measuring cavity 5, and the other end of the convex surface faces the wave plate 3; a multi-angle Stokes-direction measuring device 10 is arranged along the periphery of the measuring chamber 5, which forms five scattered-light measuring angles of the measured particles in the measuring chamber 5, the five angles being theta1、θ2、θ3、θ4、θ5(ii) a The multi-angle Stokes vector measuring device 10 is connected with a signal acquisition card 11, and the signal acquisition card 11 is connected with a computer.
The multi-angle stokes vector measuring device 10 has the advantages that the measuring angles comprise 10 degrees, 30 degrees, 60 degrees, 85 degrees and 115 degrees, other angles can be adopted, the stokes vector detection of multi-angle scattering light can be realized, and the information quantity is rich.
The measuring objects of the multi-angle stokes vector measuring device 10 include, but are not limited to, horizontal linear polarization, vertical linear polarization, 45-degree linear polarization and circular polarization, and multi-dimensional polarization state detection of scattered light is realized.
The polarization beam splitter 2 and the wave plate 3 are combined, including but not limited to horizontal linear polarization, 45-degree linear polarization or circular polarization, and the polarization state of the incident light can be modulated into any linear polarization, circular polarization or elliptical polarization state according to the actual measurement requirement.
Referring to fig. 2, 3 and 4, the core of the system is to acquire single particle polarization physical characteristic information through polarization detection; and obtaining an online source analysis result by using the polarization physical characteristic information of the particle group through a corresponding algorithm.
PM based on aforementioned measurement system2.5The online source analysis method is an online source analysis algorithm based on the polarization physical characteristics of particulate matters, and is divided into two stages:
the first stage is the establishment of a polarized physical characteristic spectrum of a pollution source, and the process is as follows, wherein m kinds of main pollution sources are provided:
1) scattering PM using multi-angle polarized light2.5The single particle measuring system collects m kinds of particles discharged by pollution sources, each particle collects n paths of polarization index signals (n is less than or equal to 20), and equivalently uses an n-dimensional polarization physical characteristic vector [ a ]1,a2,...,an]Describing a particulate; respectively counting the probability distribution p of n polarization indexes of each pollution source particulate matteri,jI.e. the j path polarization physical characteristic probability distribution of the ith pollution source particulate matter, defining pi,j(i 1, 2.. multidot.m; j 1, 2.. multidot.n) as a pollutant sourceA multi-dimensional polarized physical characteristic distribution database; p is a radical ofi(aj) The j-th polarization index of the particles is expressed as ajProbability of particulate matter being assigned to the i-th source of pollution, pi(aj) Can pass through the established probability distribution pi,jLooking up a database to obtain;
2) respectively calculating the probability P of each particle belonging to each pollution sourceiThe calculation formula is as follows:
(j ═ 1.., n), defines PiThe maximum term is the single particle recognition result of the particulate matter;
3) respectively counting the single particle identification results of M particles for each pollution source, normalizing the counting results to obtain a pollution source polarization identification fingerprint spectrum Ki(i＝1,2,...,m)，KiThe basic form of (A) is: ki＝[k1,k2,...,km]，KiThe physical meaning is as follows: for the i-th pollution source particulate matter, there is k1The single particle in the ratio is identified as coming from the 1 st contamination source, with k2A single particle of a proportion is identified as being from a 2 nd source of contamination. Wherein the content of the first and second substances,
the second stage is PM2.5The algorithm flow of online source analysis is as follows:
1) scattering PM using multi-angle polarized light2.5Single particle measuring device for collecting and measuring PM in ambient air2.5(ii) particulate matter data;
2) calculating the probability P of each particulate matter belonging to each pollution sourceiThe calculation formula is as follows:
(i ═ 1, 2.., m), defines PiThe maximum term is the single particle recognition result of the particulate matter;
3) counting and normalizing single-particle recognition results of all particles in one measurement periodAnd defining the result as the polarization recognition fingerprint of the current measured particulate matter, and counting as K ═ K1,k2,...,km]The physical meaning of the method is that k is actually measured in the particles1The single particle in the ratio is identified as coming from the 1 st contamination source, with k2A single particle of a proportion is identified as being from a 2 nd source of contamination. Also satisfies
4) The polarization recognition fingerprint of the actually measured particulate matter is equivalent to the linear superposition of the polarization recognition fingerprint of the known pollution source, which is shown as the following formula:
the online source analytic model is equivalent to solving the optimal solution of the equation
Make | | e | non-calculation2Minimum;
in order to avoid obtaining abnormal conditions such as negative solutions, the following constraint conditions are introduced:
adopting a Lagrange optimization method to solve to obtain an online source analysis result
The method specifically takes raise dust, biomass combustion, coal burning and motor vehicle tail gas as examples, the raise dust, the biomass combustion, the coal burning and the motor vehicle tail gas are four main pollution sources of dust-haze weather generated in autumn and winter in northern areas and account for PM2.5Contaminating the major part. By using the scheme in the invention, the PM is scattered by using multi-angle polarized light2.5Measurement system for Beijing areaMeasuring raised dust (road dust and soil dust), biomass (hay and corn straw) combustion, coal (civil bituminous coal) and motor vehicle tail gas (diesel vehicle) particles with typical representative meanings; by adopting the online source analysis algorithm model in the scheme of the invention, online source analysis of four typical pollution sources of dust emission, biomass combustion, fire coal and motor vehicle tail gas is realized, and partial results are shown in the following table:
in the above table, each row represents the meaning: taking example 1, the instrument measures road dust particles, and the online source analysis result shows that 94.53% is raise dust, 1.86% is biomass combustion, 3.19% is fire coal, 0.7% is motor vehicle exhaust, 0.33% is other particles, and so on.
The four typical emission source particles are mixed according to a set proportion (1% is taken as a step length, the proportion of each pollution source is changed from 0% to 100% in sequence), online source analysis is carried out by adopting the method in the scheme of the invention, an output result is compared with a real proportion in an error mode, and the result is shown in figure 5. From the error statistical result, the online source analysis errors of the invention are basically less than 20%, the average identification absolute error is 6%, and the PM of the invention is proved2.5The online source analysis method and the measurement system are effective.
While the invention has been described in detail, it should be understood that it is not limited to the particular forms disclosed, but is intended to cover all modifications, equivalents, and alternatives falling within the spirit and scope of the invention as defined by the appended claims.
Claims (3)
1. Based on PM2.5PM of online source analysis measuring system2.5The on-line source analysis method includes measuring system including laser, polarization beam splitter, wave plate, plano-convex cylindrical lens, measuring cavity, multi-angle Stokes vector measuring device and signal collecting card, the laser, the polarization beam splitter, the wave plate and the plano-convex cylindrical lens are in one straight line, the polarization beam splitterThe measuring cavity is positioned behind the plano-convex cylindrical lens, the light trap is arranged behind the measuring cavity, and the light trap, the plano-convex cylindrical lens, the wave plate and the polarization beam splitter are positioned on the same straight line; one end of the plane of the plano-convex cylindrical lens faces the measuring region, and the other end of the convex surface faces the wave plate; the multi-angle Stokes vector measuring device is arranged along the periphery of the measuring cavity and forms a plurality of scattered light measuring angles of the measured particles in the measuring cavity; the multi-angle Stokes vector measuring device is connected with a signal acquisition card, the signal acquisition card is connected with a computer, the online source analysis method is an online source analysis algorithm based on particle polarization physical characteristics, and the online source analysis method comprises two stages:
the first stage is the establishment of the polarized physical characteristic spectrum of the pollution source, and the process is as follows: wherein, the main pollution sources are m types:
1) scattering PM using multi-angle polarized light2.5The single particle measuring system collects m kinds of particles discharged by pollution sources, and each particle collects n paths of polarization index signals, equivalently uses an n-dimensional polarization physical characteristic vector [ a ]1,a2,...,an]Describing a particulate; respectively counting the probability distribution p of n polarization indexes of each pollution source particulate matteri,jI.e. the j path polarization physical characteristic probability distribution of the ith pollution source particulate matter, defining pi,jThe method comprises the steps that (i is 1,2, the.. multidata m, j is 1,2, the.. multidata n) is collected to be a pollution source multi-dimensional polarization physical characteristic distribution database; p is a radical ofi(aj) The j-th polarization index of the particles is expressed as ajProbability of particulate matter being assigned to the i-th source of pollution, pi(aj) Can pass through the established probability distribution pi,jLooking up a database to obtain;
2) respectively calculating the probability P of each particle belonging to each pollution sourceiThe calculation formula is as follows:
definition PiThe maximum term is the single particle recognition result of the particulate matter;
3) respectively counting the single particle identification results of M particles for each pollution source, normalizing the counting results to obtain a pollution source polarization identification fingerprint spectrum Ki(i＝1,2,...,m)，KiThe basic form of (A) is: ki＝[k1,k2,...,km]，KiThe physical meaning is as follows: for the i-th pollution source particulate matter, there is k1The single particle in the ratio is identified as coming from the 1 st contamination source, with k2A single particle of a proportion is identified as being from a 2 nd source of contamination. Wherein the content of the first and second substances,
the second stage is PM2.5The algorithm flow of online source analysis is as follows:
1) scattering PM using multi-angle polarized light2.5Single particle measuring device for collecting and measuring PM in ambient air2.5(ii) particulate matter data;
2) calculating the probability P of each particulate matter belonging to each pollution sourceiThe calculation formula is as follows:
definition PiThe maximum term is the single particle recognition result of the particulate matter;
3) counting and normalizing the single-particle identification results of all the particles in one measurement period, wherein the result is defined as the polarization identification fingerprint of the currently measured particles and counted as K ═ K1,k2,...,km]The physical meaning of the method is that k is actually measured in the particles1The single particle in the ratio is identified as coming from the 1 st contamination source, with k2A single particle of a proportion is identified as being from a 2 nd source of contamination. Also satisfies
4) The polarization recognition fingerprint of the actually measured particulate matter is equivalent to the linear superposition of the polarization recognition fingerprint of the known pollution source, which is shown as the following formula:
the online source analytic model is equivalent to solving the optimal solution of the equation
Make | | e | non-calculation2Minimum;
adopting a Lagrange optimization method to solve to obtain an online source analysis result
A pollution source multi-dimensional polarization characteristic distribution database and a pollution source polarization identification fingerprint database which are established in the steps of the first stage are data bases for realizing online source analysis in the second stage; the data spectrum base is related to the actual pollution source lists of all regions, and can be updated regularly according to actual conditions.
2. PM according to claim 12.5The online source analysis method is characterized by comprising the following steps: in step 4) of the second stage, in order to avoid obtaining abnormal conditions such as negative solutions, the following constraint conditions are introduced:
adopting a Lagrange optimization method to solve to obtain an online source analysis result
3. PM according to claim 12.5The online source analysis method is characterized by comprising the following steps: in step 1) of the first stage, n is ≦ 20.
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