CN115266969A - Ozone source analysis method based on precursor receptor model and box model - Google Patents
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- 239000011159 matrix material Substances 0.000 claims description 2
- 238000004088 simulation Methods 0.000 abstract description 6
- 238000004451 qualitative analysis Methods 0.000 abstract 1
- 238000004445 quantitative analysis Methods 0.000 abstract 1
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- 230000006872 improvement Effects 0.000 description 8
- 150000003254 radicals Chemical class 0.000 description 8
- 238000001514 detection method Methods 0.000 description 7
- IOVCWXUNBOPUCH-UHFFFAOYSA-N Nitrous acid Chemical compound ON=O IOVCWXUNBOPUCH-UHFFFAOYSA-N 0.000 description 5
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- 238000004364 calculation method Methods 0.000 description 3
- 239000002028 Biomass Substances 0.000 description 2
- -1 NOx Chemical class 0.000 description 2
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Abstract
The invention discloses an ozone source analysis method based on a precursor receptor model and a box model. The method is an analysis method for qualitatively and quantitatively analyzing atmospheric ozone pollution sources based on real-time observation data, and specifically comprises the steps of measuring the concentration and other parameters of pollutants in the environment, inputting the concentration of Volatile Organic Compounds (VOCs) into a receptor model for source analysis, inputting the pollutants and other parameters into a box model for calculating the ozone generation rate of pollutants of different species at a specific moment, and finally obtaining the ozone generation rates of different sources at different moments by combining with a VOCs component spectrum obtained by the precursor receptor model. The method realizes qualitative and quantitative analysis of the source of the ozone precursor, improves the accuracy of model simulation, and enables the model simulation to be more suitable for the real atmospheric pollution process.
Description
Technical Field
The invention relates to the technical field of atmospheric environment protection, in particular to an ozone source analysis method based on a precursor receptor model and a box model.
Background
Ozone (O) in atmosphere3) The pollution is becoming more and more serious and becoming an important pollutant affecting the air quality. In the environment, the generation of ozone is influenced by precursors such as Volatile Organic Compounds (VOCs) and nitrogen oxides (NOx), and exhibits a high nonlinear dependence. Thereby accurately polluting ozoneThe source is qualitative and quantitative, and has important significance for pollution prevention, control and decision making.
The current models for simulating the concentration and generation of ozone in the atmosphere mainly comprise an air quality mode and a box mode. The air quality model, while able to identify the contribution of regional transport to ozone, may suffer from accuracy and hysteresis and uncertainty in boundary layer simulation using emission lists. The box mode can accurately simulate the atmospheric pollution change condition in the observation station area, and air pollutants (VOCs, NOx, CO and SO) observed in real time are used2、HONO、CH4) And other parameters (temperature, pressure, humidity, NO)2Photolysis rate) to simulate the generation rate and the consumption rate of ozone in the atmosphere, and can accurately reflect the real situation of a research area.
At present, the related patents of the source of ozone pollution, such as qualitative and quantitative, are few. An observation method recommended by technical guidelines (trial) for analyzing ozone sources in ambient air organized by science and technology standards department of the ecological environment department in 2018 is a main method for analyzing ozone sources in China at present. The method is based on a receptor model to obtain a source component spectrum of VOCs and Maximum Increment Reactivity (MIR) of the VOCs, and ozone generation potentials of different VOCs emission sources are calculated to perform ozone source analysis. The MIR values used are fixed conditions that are most sensitive to ozone generation in a certain area, and usually deviate from the actual atmospheric conditions in the area under investigation and do not reasonably simulate the daily evolution of ozone. Chinese patent document CN110057983A discloses an ozone source analysis method based on observed data and chemical mechanism, which includes data acquisition (in which the VOCs data are acquired off-line) and model simulation. In the model simulation part, the analysis result of the VOCs source is input into the atmospheric chemical reaction mechanism again, and the contribution of the emission source to ozone generation is indirectly obtained based on the ozone generation relative increment activity of different emission reduction scenes of a single source. According to the method, damage to free radical balance in the box model after emission source emission reduction is ignored, and a simulation result is deviated from an actual situation. Therefore, in order to improve the accuracy of the ozone source analysis, improvements and improvements to the existing methods are required.
Disclosure of Invention
In view of the above problems in the prior art, the present invention provides an ozone source analysis method based on a precursor receptor model and a cassette model. The method needs a conventional precursor receptor model and a box model for calculating ozone generation kinetics, and specifically comprises the following steps:
step one, measuring real-time air pollutant concentration data and meteorological parameters and simultaneously measuring NO2Real-time photolysis rate constants;
step two, inputting the concentration data of VOCs in the air pollutants into a precursor receptor model in real time to obtain VOCs component spectrums of different sources, namely the relative contributions of VOCs of different sources;
step three, carrying out the step two and simultaneously carrying out air pollutant concentration data and NO2The real-time photolysis rate constant and meteorological parameters are input into a box model on line, and HO generated by the reaction of each species2 and RO2The rate of the free radicals is marked in the whole process, and RO generated by different VOCs under the real atmospheric condition is simulated2Reaction rate with NO, HO2Rate of reaction with NO and NO, HO2 and RO2To obtain the ozone generation rate of the VOCs in the atmosphere;
and step four, applying the VOCs component spectrum to the ozone generation rates of the VOCs to obtain the ozone generation rates of different sources, so as to realize qualitative and quantitative source analysis of the VOCs of the pollutants.
As a further improvement of the invention, in the second step, the precursor receptor model adopts a conventional orthogonal matrix factor analysis model (PMF model) or a chemical mass balance model (CMB).
As a further improvement of the invention, the box model in step three is a box model for calculating ozone generation kinetics, and specifically, the box model for calculating ozone generation kinetics adopts a conventional photochemical box model.
As a further improvement of the present invention, the calculation formula of the ozone generation rates of different VOCs species in the atmosphere in step three is as follows:
in the formula ,
ozone generation Rate for VOC species j, [ NO]、[HO2]、[RO2]Respectively represent NO and HO2、RO2The concentration of (a) in (b),
represents HO2And the rate of reaction of the NO and the nitrogen,
represents RO generated by VOC species j2Rate of reaction with NO, wherein RO2React with NO to form RO and NO2No reaction to form organic nitrates is involved.
As a further improvement of the present invention, the calculation formula of applying the spectrum of the components of the VOCs to the ozone generation rate of the VOCs in step four is as follows:
wherein ,
for the i < th > VOC source comprising n species at a particular time to ozone generation rate,
the relative contribution of VOC species j to the ith VOC source, which results from step two;
represents the RO generated by VOC species j2 and HO2Sum of reaction rates with NO, which results from step three.
As a further improvement of the invention, in step one, the method comprises the steps of using a gas chromatograph, a trace gas analyzer andthe methane analyzer continuously collects and analyzes ambient air to obtain real-time VOCs, NOx, CO and SO2HONO and CH4The concentration data of (c).
As a further refinement of the present invention, step a pair of real-time collected air samples were analyzed using gas chromatography to obtain data on the concentration of 117 ozone precursor VOCs.
Compared with the prior art, the ozone source analysis method based on the precursor receptor model and the box model can really analyze the pollution source which contributes greatly to ozone generation and the reasonable daily variation characteristic, has the advantages of easiness in operation and high accuracy, wherein the precursor receptor model and the box model are operated independently and do not interfere with each other, and the ozone generation dynamics obtained by the box model reflects the actual atmospheric conditions.
Drawings
FIG. 1 is a flow chart of a method for ozone source analysis based on a precursor receptor model and a cassette model according to one embodiment of the present invention;
FIG. 2 is a schematic diagram of a method for calculating ozone generation rate in an ozone source analysis method based on a precursor receptor model and a box model according to an embodiment of the present invention;
fig. 3 is a schematic diagram of daily variation and percentage of ozone generation rates of different ozone sources obtained by an ozone source analysis method based on a precursor receptor model and a box model according to an embodiment of the present invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are some, but not all, embodiments of the present invention. All other embodiments, which can be obtained by a person skilled in the art without making any creative effort based on the embodiments in the present invention, belong to the protection scope of the present invention.
Embodiment one, ozone source analysis method based on precursor receptor model and box model
As shown in FIG. 1, the invention provides an ozone source analysis method based on a precursor receptor model and a box model, which comprises the following specific steps:
the method comprises the following steps of firstly, carrying out real-time sampling analysis on the concentration of VOCs in the atmosphere by using a gas chromatograph, and calibrating 117 VOCs components by using ozone precursors (PAMs and TO-15) TO obtain the concentration and detection limit of 117 VOCs in the atmosphere; use of gas and methane analyzers for other pollutants and free radicals (including NOx, CO, SO)2、HONO、CH4) The concentration of (c); using weather stations and NO2The analyzer obtains real-time temperature, humidity, atmospheric pressure and NO2The rate of photolysis.
And step two, inputting the concentrations of 117 VOCs and the uncertainty calculated by using the detection limit into a precursor receptor model to obtain component spectrums of the VOCs under different sources, namely the relative contributions of the VOCs under different sources.
Step three, carrying out step two and simultaneously adding all pollutants (VOCs, NOx, CO and SO)2、 HONO、CH4) Concentration data and other parameters (temperature, pressure, humidity, NO)2Photolysis rate) into a box model to simulate the generation of RO from different species of VOCs under real atmospheric conditions2Reaction rate with NO, HO2Rate of reaction with NO and NO, HO2 and RO2To thereby obtain the ozone generation rate. As shown in fig. 2, the kinetic principle of ozone generation according to step three is: in the atmosphere, VOCs generate HO under the action of illumination, OH free radicals and oxygen2 and RO2Free radicals, HO2 and RO2Free radical promoted formation of NO2Finally NO under light irradiation2Reacts with oxygen to generate ozone. Meanwhile, the main calculation formula of the ozone generation rates of different VOCs types in the atmosphere is as follows:
in the formula ,
is the ozone generation rate of VOC species j, [ NO]、[HO2]、[RO2]Respectively represent NO and HO2、RO2The concentration of (a) in (b),
represents HO2And the rate of reaction of the NO and the nitrogen,
represents RO generated by VOC species j2The rate of reaction with NO. Wherein RO2React with NO to form RO and NO2No reaction to form organic nitrates is involved.
Step four, substituting the VOCs component spectrum and the ozone generation rate at different moments
Thereby calculating the ozone generation rate of different sources at different time. The ozone generation rate refers to the rate at which ozone is generated by different ozone precursors in the model, and is related to the actual atmospheric ozone concentration. Wherein,
for the i < th > VOC source comprising n species at a particular time to ozone generation rate,
is the relative contribution of VOC species j to the ith VOC source,
represents the RO generated by VOC species j2 and HO2Sum of reaction rates with NO.
Example II, analysis of ozone source in winter in certain industrial city in northern China
As shown in fig. 3, the method of the first embodiment is used to analyze the source of ozone in winter in an industrial city in north of china, and the specific steps are as follows:
step one, carrying out real-time sampling analysis on the concentration of VOCs in the atmosphere by using a gas chromatograph, and calibrating 117 VOCs components by using ozone precursors (PAMs and TO-15) TO obtain the concentration and detection limit of 117 VOCs in the atmosphere; at the same time, other pollutants and free radicals (including NOx, CO, SO) are obtained by using a gas analyzer and a methane analyzer2、HONO、CH4) The concentration of (c); using weather stations and NO2The analyzer obtains real-time temperature, humidity, atmospheric pressure and NO2The rate of photolysis.
And step two, inputting the concentrations of 117 VOCs and the uncertainty calculated by using the detection limit into a precursor receptor model to obtain component spectrums of the VOCs under different sources. When the concentration of the species is lower than the detection limit, using 5/6 of the detection limit as the uncertainty of the species at the current moment; when the species concentration is higher than the detection limit, the use
The current uncertainty is calculated. Where the correlation between VOCs species observation and prediction is good (R)2＝0.7,P<0.01). The precursor receptor model resolves six pollution sources, and the spectra of the VOCs components (relative contributions of VOCs from different sources) are: biomass combustion sources (6.4 ppbv, 19.8%), industrial combustion sources (9.0ppbv, 27.8%), vehicle exhaust gas sources (2.8ppbv, 8.6%), cooking sources (3.9ppbv, 12.0%), solvent use sources (7.5ppbv, 23.1%), and pharmaceutical plant discharge sources (2.8ppbv, 8.6%).
Step three, carrying out step two and simultaneously adding all pollutants (VOCs, NOx, CO and SO)2、 HONO、CH4) Concentration data and other parameters (temperature, pressure, humidity, NO)2Photolysis rate) into a box model to simulate the generation of RO from different species of VOCs under real atmospheric conditions2Reaction rate with NO, HO2Rate of reaction with NO and NO, HO2 and RO2To obtain the ozone generation rate.
Step four, the VOCs component spectrum is subjected to deodorization at different timesOxygen generation rate substitution
Thereby calculating the ozone generation rate of different sources at different time. Finally, as shown in FIG. 3, we have observed that the ozone generation rate of the biomass combustion source during the observation period was 0.9 ppbv/h, accounting for 13.7% of the total ozone generation rate. The largest proportion of the ozone generating agent is an industrial combustion source, the daily average value of the ozone generating rate is 2.3ppbv/h, and the proportion is 34.8%. Followed by solvent emission source (1.4 ppbv/h, 21.2%), vehicle exhaust gas source (1.3 ppbv/h, 19.7%), cooking source (0.5 ppbv/h, 7.6%), and pharmaceutical factory exhaust gas source (0.2 ppbv/h, 3.0%). Meanwhile, as shown in fig. 3, the method of the first embodiment can give a characteristic of the obvious daily variation of the ozone generation rates of all the sources, and the ozone generation rates of all the sources in the winter of the city are obviously increased from nine am until eleven am reaches a peak value and then gradually decreased until six pm of the day, and the ozone generation rates of all the sources are close to zero.
Therefore, in the second embodiment, the ozone source obtained in winter in an industrial city in north china is mainly from the industrial combustion source, and the ozone generation rate during the observation period accounts for 19.7% although the concentration of the tail gas source of the motor vehicle is low, which means that the method in the first embodiment can not only explain the regional ozone pollution generation factor, but also reveal the highly reactive species in the ozone pollution.
And (4) conclusion:
the ozone source analysis method based on the precursor receptor model and the box model has the following beneficial effects:
1. the invention adopts gas chromatography automatic analysis and online real-time observation, relates to 117 VOCs in the atmosphere, and has the characteristics of simple operation, strong timeliness and wide coverage range.
2. The invention uses the online data to be input into the precursor receptor model and the box model in parallel, so that the results of the precursor receptor model and the box model are not interfered with each other, the time can be effectively saved, and meanwhile, the method for marking the ozone generation rate based on the observed box model does not bring extra errors of free radicals and the ozone generation rate.
3. The precursor source of the ozone is qualitatively and quantitatively determined by using the precursor receptor model result and the box model result, and an important scientific basis is provided for explaining the regional ozone pollution generating factors and the atmospheric pollution treatment.
The above is only a preferred embodiment of the present invention, and is not intended to limit the present invention, and various modifications and changes will occur to those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (7)
1. The method for analyzing the ozone source based on the precursor receptor model and the box model is characterized by comprising the following steps of:
step one, measuring real-time air pollutant concentration data and meteorological parameters and measuring NO simultaneously2Real-time photolysis rate constants;
inputting VOCs concentration data in air pollutants into a precursor receptor model to obtain VOCs component spectrums of different sources, namely the relative contributions of the VOCs of different sources;
step three, when the step two is implemented, the air pollutant concentration data and NO are processed2The real-time photolysis rate constant and meteorological parameters are input into a box model on line, and HO is generated by reacting each species2 and RO2The rate of the free radicals is marked in the whole process, and RO generated by different VOCs under the real atmospheric condition is simulated2Reaction rate with NO, HO2Rate of reaction with NO and NO, HO2 and RO2To obtain the ozone generation rate of the VOCs in the atmosphere;
and step four, applying the VOCs component spectrum to the ozone generation rates of the VOCs to obtain ozone generation rates of different sources, so as to realize qualitative and quantitative source analysis of the pollutants VOCs.
2. The method of claim 1, wherein the precursor receptor model in step two is an orthogonal matrix factorial analysis model.
3. The method of claim 1, wherein the cassette model in step three is a cassette model for calculating ozone generation kinetics, and the cassette model for calculating ozone generation kinetics is a photochemical cassette model.
4. The method of claim 1, wherein the ozone generation rates for different VOCs species in the atmosphere in step three are calculated as follows:
in the formula ,
is the ozone generation rate of VOC species j, [ NO]、[HO2]、[RO2]Respectively represent NO and HO2、RO2The concentration of (a) is higher than (b),
represents HO2And the rate of reaction of the NO and the nitrogen,
represents RO generated by VOC species j2Rate of reaction with NO, wherein RO2React with NO to form RO and NO2No reaction to form organic nitrates is involved.
5. The method of claim 1 wherein the step four applies the spectra of the VOCs components to the ozone generation rates of the VOCs as follows:
wherein ,
for the i < th > VOC source comprising n species at a particular time to ozone generation rate,
the relative contribution of VOC species j to the ith VOC source, which resulted from step two;
represents the RO generated by VOC species j2 and HO2Sum of reaction rates with NO, which results from step three.
6. The method of claim 1, wherein in step one, by using a gas chromatograph, a trace gas analyzer and a methane analyzer to continuously collect and analyze ambient air, real-time VOCs, NOx, CO, SO are obtained2HONO and CH4The concentration data of (c).
7. The method of claim 6, wherein in step one, gas chromatography is used on a real-time collected air sample to obtain 117 ozone precursor VOCs concentration data.
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