Source analysis method and system for anthropogenic emissions of VOCs based on receptor model

Abstract

The present invention relates to the technical field of source analysis of atmospheric volatile organic compounds, and a method and system for analyzing the sources of primary anthropogenic emissions of VOCs based on a receptor model, including: constructing a photochemical age parameterization model using the [OH] exposure, the initial isoprene emission concentration, the [OVOCs] observed concentration, the tracer observed concentration, the actual [OVOCs] reaction rate constant, and the tracer reaction rate constant, calculating the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model, observing the anthropogenic emission observed concentration of [NMHCs], obtaining the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs], performing photochemical loss correction and atmospheric diffusion correction on the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] to obtain the initial concentration of primary anthropogenic emissions of [VOCs], and performing VOCs source analysis using the initial concentration of primary anthropogenic emissions of [VOCs] according to the PMF receptor model. The present invention can improve the analytical accuracy of the PMF receptor model for the sources of VOCs in the actual atmosphere.

Description

Technical Field

[0001] The present invention relates to the technical field of source analysis of atmospheric volatile organic compounds, and particularly relates to a method and system for analyzing the sources of primary anthropogenic emissions of VOCs based on a receptor model. Background Art

[0002] The Positive Matrix Factorization (PMF) receptor model is a very effective method for evaluating the sources of VOCs.

[0003] The premise assumption of the PMF receptor model for analyzing the sources of atmospheric volatile organic compounds (referred to as VOCs) is that pollutants do not undergo photochemical reactions from the emission source to the receptor monitoring point. However, in the actual atmospheric environment, when volatile organic compounds are transported from the emission source through the atmosphere to the receptor point for monitoring, they will experience varying degrees of loss, and affected by atmospheric turbulence diffusion, this makes the analysis results of the sources of VOCs in the actual atmosphere using the PMF receptor model deviate. Summary of the Invention

[0004] The present invention provides a method and system for analyzing the sources of primary anthropogenic emissions of VOCs based on a receptor model, and its main purpose is to improve the analysis accuracy of the PMF receptor model for the sources of VOCs in the actual atmosphere.

[0005] To achieve the above purpose, a method for analyzing the sources of primary anthropogenic emissions of VOCs based on a receptor model provided by the present invention includes:

[0006] Obtain the observed concentrations of [OVOCs], the observed concentrations of tracers, and the tracer reaction rate constants, and calculate the OH exposure, the initial emission concentration of isoprene, and the actual reaction rate constant of [OVOCs];

[0007] Construct a photochemical age parameterization model using the OH exposure, the initial emission concentration of isoprene, the observed concentration of [OVOCs], the observed concentration of tracers, the actual reaction rate constant of [OVOCs], and the tracer reaction rate constants;

[0008] Calculate the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model, and use a pre-constructed observation instrument to observe the observed concentration of anthropogenic emissions of [NMHCs] to obtain the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs], where the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] refers to: the theoretical concentration of primary anthropogenic emissions of [OVOCs] and the observed concentration of anthropogenic emissions of [NMHCs];

[0009] Perform photochemical loss correction and atmospheric diffusion correction on the observed concentration of the primary anthropogenic emissions of the full-spectrum [VOCs] to obtain the initial concentration of the primary anthropogenic emissions of [VOCs];

[0010] According to the pre-constructed PMF receptor model, perform source apportionment of VOCs using the initial concentration of the primary anthropogenic emissions of [VOCs]

[0011] Optionally, the calculation of the OH exposure, the initial emission concentration of isoprene, and the actual reaction rate constant of [OVOCs] includes:

[0012] Obtain the emission concentration ratio and the observed concentration ratio of the benzene series species pair, where the two benzene series species in the benzene series species pair have the same source and different chemical activities;

[0013] According to the pre-constructed OH exposure formula, calculate the OH exposure using the emission concentration ratio and the observed concentration ratio;

[0014] Obtain the observed concentration of isoprene, and calculate the initial emission concentration of isoprene using the following formula based on the OH exposure and the observed concentration of isoprene:

[0015]

[0016] Where, represents the initial emission concentration of isoprene, represents the observed concentration of isoprene at time represents the reaction rate constant of isoprene, represents the OH exposure;

[0017] Calculate the photolysis rate of [OVOCs] using the pre-constructed photolysis rate formula;

[0018] According to the photolysis rate of [OVOCs], calculate the actual reaction rate constant of [OVOCs] using the pre-constructed reaction rate formula of [OVOCs].

[0019] Optionally, the OH exposure formula is as follows:

[0020]

[0021] Where, represents the OH exposure, represents the reaction rate constant of species C in the benzene series species pair with the OH radical, represents the reaction rate constant of species B in the benzene series species pair with the OH radical, represents the natural logarithm symbol, represents the ratio of the emission concentrations of species C and species B at time Indicates the observed concentration ratio of species C to species B at the moment.

[0022] Optionally, the photolysis rate formula is as follows:

[0023]

[0024] where represents the photolysis rate of [OVOCs], represents the photolysis rate of [OVOCs] under clear sky conditions, represents the photolysis rate under clear sky conditions, represents the measured photolysis rate.

[0025] Optionally, the OVOCs reaction rate formula is as follows:

[0026]

[0027] where represents the actual [OVOCs] reaction rate constant, represents the reference [OVOCs] reaction rate constant, represents the photolysis rate of [OVOCs], represents the OH radical concentration.

[0028] Optionally, the photochemical age parameterization model is as follows:

[0029]

[0030] where represents the observed concentration of [OVOCs], represents the observed concentration of the tracer, represents the emission ratio variable of [OVOCs] relative to the tracer, represents the tracer reaction rate constant, represents the observed concentration of the tracer, represents the emission ratio variable of the [OVOCs] precursor relative to the tracer, represents the reaction rate variable of the [OVOCs] precursor with the OH radical, represents the emission ratio variable of [OVOCs] relative to the initial isoprene emission concentration, represents the background concentration of [OVOCs].

[0031] Optionally, calculating the theoretical concentration of the primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model includes:

[0032] Using the photochemical age parameterization model, perform non-linear fitting on the actual [OVOCs] reaction rate constant, [OVOCs] observed concentration, tracer observed concentration, OH exposure, and isoprene initial emission concentration, and calculate the emission ratio of [OVOCs] relative to the tracer, the emission ratio of [OVOCs] precursors relative to the tracer, the reaction rate constant of [OVOCs] precursors with OH radicals, the emission ratio of [OVOCs] relative to the isoprene initial emission concentration, and the [OVOCs] background concentration according to the preset least squares method;

[0033] Substitute the emission ratio of [OVOCs] relative to the tracer, the emission ratio of [OVOCs] precursors relative to the tracer, the reaction rate constant of [OVOCs] precursors with OH radicals, the emission ratio of [OVOCs] relative to the isoprene initial emission concentration, and the [OVOCs] background concentration into the photochemical age parameterization model for calculation to obtain the theoretical concentration of primary anthropogenic emissions of [OVOCs].

[0034] Optionally, performing photochemical loss correction and atmospheric diffusion correction on the observed concentration of primary anthropogenic emissions of the full-spectrum [VOCs] to obtain the initial concentration of primary anthropogenic emissions of [VOCs] includes:

[0035] According to the observed concentration of primary anthropogenic emissions of the full-spectrum [VOCs], calculate using the following formula Fitted reaction rate:

[0036]

[0037] where represents the observed concentration of primary anthropogenic emissions of the i-th [VOCs] at time t, represents the emission ratio of the i-th [VOCs] relative to the preset full-spectrum tracer, represents the fitted reaction rate of the i-th [VOCs];

[0038] Obtain Theoretical reaction rate constant, and calculate the empirical coefficient according to the Theoretical reaction rate constant, Fitted reaction rate using the following formula:

[0039]

[0040] where represents the empirical coefficient, represents the theoretical reaction rate constant of the i-th [VOCs];

[0041] According to the empirical coefficient, the initial concentration of primary anthropogenic emissions of [VOCs] is calculated using the following formula:

[0042]

[0043] where represents the initial concentration of primary anthropogenic emissions of the i-th [VOCs].

[0044] Optionally, after calculating the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model, the method further includes:

[0045] Successively extract atmospheric volatile organic compounds from the pre-constructed set of atmospheric volatile organic compounds to obtain multiple groups of tracer-[OVOCs] training sets and multiple groups of tracer-[OVOCs] validation sets of the atmospheric volatile organic compounds. Among them, the tracer training concentration in the tracer-[OVOCs] training set is the independent variable, and the [OVOCs] observed training concentration is the dependent variable. Each group of tracer-[OVOCs] training sets and each group of tracer-[OVOCs] validation sets correspond to the tracer category. The multiple groups of tracer-[OVOCs] validation sets are calculated according to the photochemical age parameterization model. The atmospheric volatile organic compounds belong to non-methane hydrocarbons or oxygenated volatile organic compounds;

[0046] Successively extract the initial machine learning algorithms from the pre-constructed set of machine learning algorithms. The initial machine learning algorithms include: decision tree algorithm, random forest algorithm, extremely randomized tree algorithm, gradient boosting decision tree algorithm, Adaboost algorithm, Catboost algorithm, Xgboost algorithm, LightGBM algorithm;

[0047] Successively extract the tracer-[OVOCs] training sets from the multiple groups of tracer-[OVOCs] training sets;

[0048] Use the tracer-[OVOCs] training set to train the initial machine learning algorithm to obtain the target machine learning algorithm;

[0049] Use the tracer-[OVOCs] validation set to verify the target machine learning algorithm to obtain the prediction accuracy set, and calculate the average prediction accuracy of the prediction accuracy set. The average prediction accuracy in the average prediction accuracy set represents the voting score value of the target machine learning algorithm for the tracer category;

[0050] Summarize the average prediction accuracies corresponding to each group of tracer-[OVOCs] training sets to obtain the average prediction accuracy set;

[0051] Summarize the mean sets of prediction accuracies corresponding to each target machine learning algorithm to obtain multiple sets of mean prediction accuracy sets;

[0052] Use the following formula to calculate the tracer score values based on the multiple sets of mean prediction accuracy sets to obtain a set of tracer score values:

[0053]

[0054] where, represents the tracer score value of the p-th tracer, Q represents the number of target machine learning algorithms, represents the mean prediction accuracy of the q-th target machine learning algorithm for the p-th tracer;

[0055] Extract the maximum tracer score in the set of tracer score values, and identify the tracer category corresponding to the maximum tracer score;

[0056] Take the tracer category corresponding to the maximum tracer score as the target tracer of the atmospheric volatile organic compounds. To achieve the above object, the present invention also provides a source analysis system for primary anthropogenic emissions of VOCs based on a receptor model, including:

[0057] A photochemical age parameterization model construction module, configured to obtain the observed concentration of [OVOCs], the observed concentration of the tracer, and the tracer reaction rate constant, and calculate the OH exposure, the initial isoprene emission concentration, and the actual [OVOCs] reaction rate constant; construct a photochemical age parameterization model by using the OH exposure, the initial isoprene emission concentration, the observed concentration of [OVOCs], the observed concentration of the tracer, the actual [OVOCs] reaction rate constant, and the tracer reaction rate constant;

[0058] An [OVOCs] primary anthropogenic emission observed concentration calculation module, configured to calculate the theoretical concentration of the primary anthropogenic emission of [OVOCs] according to the photochemical age parameterization model, and use a pre-constructed observation instrument to observe the observed concentration of the anthropogenic emission of [NMHCs] to obtain the observed concentration of the primary anthropogenic emission of the full-spectrum [VOCs], where the observed concentration of the primary anthropogenic emission of the full-spectrum [VOCs] refers to: the theoretical concentration of the primary anthropogenic emission of [OVOCs] and the observed concentration of the anthropogenic emission of [NMHCs];

[0059] A [VOCs] primary anthropogenic emission initial concentration calculation module, configured to perform photochemical loss correction and atmospheric diffusion correction on the observed concentration of the primary anthropogenic emission of the full-spectrum [VOCs] to obtain the initial concentration of the primary anthropogenic emission of [VOCs];

[0060] A [VOCs] source analysis module, configured to perform VOCs source analysis according to a pre-constructed PMF receptor model by using the initial concentration of the primary anthropogenic emission of [VOCs].

[0061] To solve the above problems, the present invention further provides an electronic device, which includes:

[0062] a memory storing at least one instruction; and

[0063] a processor that executes the instructions stored in the memory to implement the above-mentioned source analysis method for primary anthropogenic VOC emissions based on the receptor model.

[0064] To solve the above problems, the present invention further provides a computer-readable storage medium, in which at least one instruction is stored, and the at least one instruction is executed by a processor in an electronic device to implement the above-mentioned source analysis method for primary anthropogenic VOC emissions based on the receptor model.

[0065] To solve the problems described in the background art, the present invention first needs to construct a photochemical age parameterization model, and then calculate the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model. Since the photochemical age parameterization model includes known parameters, multiple unknown variables, multiple groups of measurable parameters, and multiple groups of computable parameters. Among them, the known parameters are: tracer reaction rate constants; multiple groups of unknown variables include: the emission ratio variable of [OVOCs] relative to the tracer, the emission ratio variable of [OVOCs] precursors relative to the tracer, the reaction rate variable of [OVOCs] precursors with OH radicals, the emission ratio variable of [OVOCs] relative to the initial emission concentration of isoprene, and the background concentration of [OVOCs]; multiple groups of measurable parameters include: the observed concentration of [OVOCs], the observed concentration of the tracer; multiple groups of computable parameters include: OH exposure, the reference reaction rate constant of [OVOCs], and the initial emission concentration of isoprene. Therefore, the observed concentration of [OVOCs], the observed concentration of the tracer, and the tracer reaction rate constant can be obtained first, and then the OH exposure, the initial emission concentration of isoprene, and the actual reaction rate constant of [OVOCs] can be calculated. At this time, the photochemical age parameterization model can be constructed based on the above-obtained and calculated parameters and multiple groups of unknown variables, and then the theoretical concentration of primary anthropogenic emissions of [OVOCs] can be calculated according to the photochemical age parameterization model. The observed concentration of anthropogenic emissions of [NMHCs] is observed by using a pre-constructed observation instrument to obtain the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs]. Among them, the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] refers to: the theoretical concentration of primary anthropogenic emissions of [OVOCs] and the observed concentration of anthropogenic emissions of [NMHCs]. Due to atmospheric photochemical loss and atmospheric diffusion, the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] needs to be corrected for photochemical loss and corrected for atmospheric diffusion to obtain the initial concentration of primary anthropogenic emissions of [VOCs]. Finally, based on the pre-constructed PMF receptor model, the source analysis of VOCs in primary anthropogenic emissions is completed by using the initial concentration of primary anthropogenic emissions of [VOCs]. Therefore, the present invention can improve the accuracy of the PMF receptor model in analyzing the sources of VOCs in the actual atmosphere. Description of the Drawings

[0066] Figure 1 It is a schematic flowchart of a method for analyzing the sources of primary anthropogenic emissions of VOCs based on a receptor model provided by an embodiment of the present invention;

[0067] Figure 2 It is a functional module diagram of a system for analyzing the sources of primary anthropogenic emissions of VOCs based on a receptor model provided by an embodiment of the present invention;

[0068] Figure 3Schematic diagram of the structure of an electronic device for implementing the method for analyzing the sources of primary anthropogenic emissions of VOCs based on the receptor model provided in an embodiment of the present invention.

[0069] The implementation, functional features, and advantages of the present invention will be further described with reference to the embodiments and the accompanying drawings. Detailed implementation manners

[0070] It should be understood that the specific embodiments described herein are only used to explain the present invention and are not used to limit the present invention.

[0071] An embodiment of the present application provides a method for analyzing the sources of primary anthropogenic emissions of VOCs based on the receptor model. The execution subject of the method for analyzing the sources of primary anthropogenic emissions of VOCs based on the receptor model includes, but is not limited to, at least one of electronic devices such as a server, a terminal, etc. that can be configured to execute the method provided in the embodiment of the present application. In other words, the method for analyzing the sources of primary anthropogenic emissions of VOCs based on the receptor model can be executed by software or hardware installed on a terminal device or a server device, and the software can be a blockchain platform. The server includes, but is not limited to: a single server, a server cluster, a cloud server, or a cloud server cluster, etc.

[0072] Refer to Figure 1 As shown, it is a flowchart of a method for analyzing the sources of primary anthropogenic emissions of VOCs based on the receptor model provided in an embodiment of the present invention. In this embodiment, the method for analyzing the sources of primary anthropogenic emissions of VOCs based on the receptor model includes:

[0073] S1. Obtain the observed concentration of [OVOCs], the observed concentration of tracers, and the reaction rate constant of the tracer, and calculate the OH exposure, the initial emission concentration of isoprene, and the actual reaction rate constant of [OVOCs].

[0074] It can be understood that the observed concentration of [OVOCs] refers to the observed concentration of a certain oxygenated volatile organic compound (Oxygenated Volatile Organic Compounds, abbreviated as OVOCs) at a monitoring site. For example, the observed concentration of acetaldehyde at a certain site is . The observed concentration of the tracer refers to the observed concentration of a compound that can specifically indicate or trace the source and distribution of the oxygenated volatile organic compound at a monitoring site, generally acetylene, , benzene, or toluene. It should be noted that in the embodiments of the present invention, volatile organic compounds refer to non-methane hydrocarbons (NMHCs) and oxygenated volatile organic compounds.

[0075] Furthermore, the reaction rate constant of the tracer indicates the reaction rate constant of the tracer with the OH radical, and the OH exposure can be expressed as , where represents the air mass reaction time. The initial emission concentration of isoprene refers to the concentration of isoprene emitted from the emission source. The actual [OVOCs] reaction rate constant refers to the actual reaction rate constant of oxygenated volatile organic compounds with OH radicals.

[0076] In an embodiment of the present invention, after calculating the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model, the method further includes:

[0077] Successively extract atmospheric volatile organic compounds from a pre-constructed set of atmospheric volatile organic compounds to obtain multiple groups of tracer-[OVOCs] training sets and multiple groups of tracer-[OVOCs] validation sets of the atmospheric volatile organic compounds. Among them, the tracer training concentration in the tracer-[OVOCs] training set is the independent variable, and the [OVOCs] observed training concentration is the dependent variable. Each group of tracer-[OVOCs] training sets and each group of tracer-[OVOCs] validation sets correspond to the tracer category. The multiple groups of tracer-[OVOCs] validation sets are calculated and obtained according to the photochemical age parameterization model. The atmospheric volatile organic compounds belong to non-methane hydrocarbons or oxygenated volatile organic compounds;

[0078] Successively extract initial machine learning algorithms from a pre-constructed set of machine learning algorithms, where the initial machine learning algorithms include: decision tree algorithm, random forest algorithm, extremely randomized tree algorithm, gradient boosting decision tree algorithm, Adaboost algorithm, Catboost algorithm, Xgboost algorithm, LightGBM algorithm;

[0079] Successively extract the tracer-[OVOCs] training sets from the multiple groups of tracer-[OVOCs] training sets;

[0080] Use the tracer-[OVOCs] training set to train the initial machine learning algorithm to obtain a target machine learning algorithm;

[0081] Use the tracer-[OVOCs] validation set to verify the target machine learning algorithm to obtain a prediction accuracy set, and calculate the average prediction accuracy of the prediction accuracy set. Among them, the average prediction accuracy in the average prediction accuracy set represents the voting score value of the target machine learning algorithm for the tracer category;

[0082] Summarize the average prediction accuracies corresponding to each group of tracer-[OVOCs] training sets to obtain an average prediction accuracy set;

[0083] Summarize the average prediction accuracy sets corresponding to each target machine learning algorithm to obtain multiple groups of average prediction accuracy sets;

[0084] Using the following formula, calculate the tracer score value based on the set of mean prediction accuracies of multiple groups to obtain a set of tracer score values:

[0085]

[0086] where represents the tracer score value of the p-th tracer, Q represents the number of target machine learning algorithms, represents the mean prediction accuracy of the q-th target machine learning algorithm for the p-th tracer;

[0087] Extract the maximum tracer score in the set of tracer score values, and identify the tracer category corresponding to the maximum tracer score;

[0088] Take the tracer category corresponding to the maximum tracer score as the target tracer of the atmospheric volatile organic compounds.

[0089] Specifically, the set of atmospheric volatile organic compounds can be: acetaldehyde, acetone, methanol, xylene, styrene, toluene, etc. The multiple sets of tracer-[OVOCs] training sets refer to the set of tracer training concentrations and [OVOCs] observed training concentrations. The tracer training concentration refers to the tracer concentration input to the initial machine learning algorithm for training the initial machine learning algorithm. The [OVOCs] observed training concentration refers to the [OVOCs] observed concentration observed at the monitoring site at the tracer training concentration. The tracer-[OVOCs] validation set refers to the set of multiple sets of tracer validation concentrations and [OVOCs] theoretical validation concentrations. Among them, the [OVOCs] theoretical validation concentration refers to the primary anthropogenic emission theoretical concentration of [OVOCs] calculated according to the photochemical age parameterization model at the tracer validation concentration.

[0090] Furthermore, the prediction accuracy set refers to the prediction error of each set of tracer validation concentrations and [OVOCs] theoretical validation concentrations in the tracer-[OVOCs] validation set under the initial machine learning algorithm. When performing validation, the tracer validation concentration can be first input into the target machine learning algorithm, so as to obtain the [OVOCs] theoretical predicted concentration according to the target machine learning algorithm, and then calculate the prediction accuracy according to the [OVOCs] theoretical validation concentration and the [OVOCs] theoretical predicted concentration. The prediction accuracy can be the reciprocal of the difference between the [OVOCs] theoretical validation concentration and the [OVOCs] theoretical predicted concentration. The mean prediction accuracy refers to the average prediction accuracy of the prediction accuracy set.

[0091] It is understandable that each set of tracer-[OVOCs] training sets corresponds to a tracer category. Therefore, multiple tracer categories correspond to multiple mean prediction accuracies, that is, the set of mean prediction accuracies. Each set of mean prediction accuracies in the multiple sets of mean prediction accuracies corresponds to a target machine learning algorithm.

[0092] For example, when the set of mean prediction accuracies corresponding to the decision tree algorithm is 2, 4, 7, 9 (the corresponding tracers are , benzene, toluene, and acetylene in sequence), the set of mean prediction accuracies corresponding to the random forest algorithm is 1, 2, 4, 6 (the corresponding tracers are acetylene, , benzene or toluene in sequence), and the set of mean prediction accuracies corresponding to the extremely randomized trees algorithm is 3, 4, 6, 7 (the corresponding tracers are acetylene, , benzene or toluene in sequence), the tracer score value of the first tracer is 2 + 1 + 3, the tracer score value of the second tracer is 4 + 2 + 4, the tracer score value of the third tracer is 7 + 4 + 6, and the tracer score value of the fourth tracer is 9 + 6 + 7. At this time, the fourth tracer acetylene is the target tracer of the atmospheric volatile organic compounds. The target tracer refers to the tracer most suitable for the atmospheric volatile organic compounds.

[0093] In the embodiments of the present invention, calculating the OH exposure, the initial emission concentration of isoprene, and the actual [OVOCs] reaction rate constant includes:

[0094] Obtaining the emission concentration ratio and the observed concentration ratio of a benzene series species pair, where the two benzene series species in the benzene series species pair have the same source and different chemical activities;

[0095] According to the pre-constructed OH exposure formula, calculating the OH exposure using the emission concentration ratio and the observed concentration ratio;

[0096] Obtaining the observed concentration of isoprene, and calculating the initial emission concentration of isoprene according to the OH exposure and the observed concentration of isoprene using the following formula:

[0097]

[0098] where, represents the initial emission concentration of isoprene, represents the observed concentration of isoprene at time represents the reaction rate constant of isoprene, represents the OH exposure;

[0099] Calculating the photolysis rate of [OVOCs] using the pre-constructed photolysis rate formula;

[0100] According to the photolysis rate of the OVOCs, the actual [OVOCs] reaction rate constant is calculated using the pre-established OVOCs reaction rate formula.

[0101] It can be understood that the benzene series species pair consists of two benzene series compounds (such as benzene, toluene, and xylene, etc.). For example, ethylbenzene and m,p-xylene, ethylbenzene and o-xylene, benzene and toluene, etc. The two selected benzene series compounds generally have the same source and different atmospheric activities. The emission concentration ratio refers to the initial concentration emission ratio of the benzene series species pair at the start of monitoring, which can be obtained by combining the maximum slope concentration ratio of the benzene series species pair actually observed during the period when no photochemical reaction occurs at night (where the maximum slope concentration ratio is the ratio at the maximum concentration slope of the more reactive benzene series compound to the less reactive benzene series compound in the benzene series species pair), or can be obtained by referring to relevant literature of the emission inventory. The observed concentration ratio refers to the ratio of the observed concentrations of the benzene series species pair at a certain time period from the start of monitoring.

[0102] Specifically, the isoprene observed concentration refers to the observed concentration of isoprene at a monitoring site at a certain moment. The isoprene initial emission concentration refers to the initial emission concentration of isoprene at the emission source. The isoprene reaction rate constant refers to the reaction rate constant of isoprene and OH radicals. The [OVOCs] photolysis rate refers to the photolysis rate of a certain oxygenated volatile organic compound (OVOCs). The actual [OVOCs] reaction rate constant refers to the reaction rate constant of OVOCs and OH radicals after correction.

[0103] In the embodiments of the present invention, the OH exposure formula is as follows:

[0104]

[0105] where, represents the OH exposure, represents the reaction rate constant of species C and OH radicals in the benzene series species pair, represents the reaction rate constant of species B and OH radicals in the benzene series species pair, represents the natural logarithm symbol, represents the emission concentration ratio of species C and species B at time, represents the observed concentration ratio of species C and species B at time.

[0106] Furthermore, the sampling location of the emission concentration ratio is the emission source, and the observation location of the observed concentration ratio is the monitoring site.

[0107] In the embodiments of the present invention, the photolysis rate formula is as follows:

[0108]

[0109] Among them, represents the photolysis rate of [OVOCs], represents the photolysis rate of [OVOCs] under clear sky conditions, represents the photolysis rate under clear sky conditions, represents the measured photolysis rate. The photolysis rate formula is constructed on the premise that the effects of factors such as cloud cover on the photolysis rates of OVOCs and are the same.

[0110] It can be understood that the and can be calculated according to the parameterization method in the chemical reaction mechanism MCN (V3.1.1). The specific formula is as follows:

[0111]

[0112] Among them, , , represent three parameters of different photolysis reactions, which are obtained by N, the photochemical flux, absorption cross-section, and quantum yield under clear sky at an altitude of 0.5 km, and are obtained by fitting using the least squares method. is the solar zenith angle, represents or .

[0113] In the embodiments of the present invention, the reaction rate formula of OVOCs is as follows:

[0114]

[0115] Among them, represents the actual reaction rate constant of [OVOCs], represents the reference reaction rate constant of [OVOCs], represents the photolysis rate of [OVOCs], represents the concentration of OH radicals.

[0116] It should be understood that the reference reaction rate constant of [OVOCs] refers to the reference reaction rate constant of OVOCs with OH radicals.

[0117] S2. Use the OH exposure, initial isoprene emission concentration, [OVOCs] observed concentration, tracer observed concentration, actual [OVOCs] reaction rate constant, and tracer reaction rate constant to construct a photochemical age parameterization model.

[0118] It is understandable that the photochemical age parameterization model refers to the method for estimating atmospheric OVOCs determined by de Gouw et al. The photochemical age parameterization model decomposes the atmospheric concentration of OVOCs into four parts: the theoretical concentration of primary anthropogenic emissions of [OVOCs], the concentration of secondary anthropogenic generation, the concentration of natural source emissions, and the background concentration of [OVOCs]. See the following embodiments for details.

[0119] S3. Calculate the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model, and use a pre-built observation instrument to observe the observed concentration of anthropogenic emissions of [NMHCs] to obtain the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs]. Among them, the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] refers to: the theoretical concentration of primary anthropogenic emissions of [OVOCs] and the observed concentration of anthropogenic emissions of [NMHCs].

[0120] It is understandable that the theoretical concentration of primary anthropogenic emissions of [OVOCs] refers to the theoretical concentration of OVOCs anthropogenically emitted at the emission source calculated according to the photochemical age parameterization model, and the observed concentration of anthropogenic emissions of [NMHCs] refers to the concentration of NMHCs observed at the monitoring site. The observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] refers to the observed concentration of anthropogenic non-methane hydrocarbons (NMHCs) and oxygenated volatile organic compounds at the monitoring site. Among them, atmospheric volatile organic compounds include non-methane hydrocarbons (NMHCs) and oxygenated volatile organic compounds (OVOCs).

[0121] Furthermore, since the NMHCs at the monitoring site directly come from primary emissions, and a part of the OVOCs is directly emitted from anthropogenic sources, and a part is generated by the photochemical reaction of NMHCs, the theoretical concentration of primary anthropogenic emissions of [OVOCs] does not include the concentration of OVOCs generated by the secondary generation of NMHCs.

[0122] In the embodiment of the present invention, the photochemical age parameterization model is as follows:

[0123]

[0124] Among them, represents the observed concentration of [OVOCs], represents the observed concentration of the tracer, represents the emission ratio variable of [OVOCs] relative to the tracer, represents the reaction rate constant of the tracer, represents the observed concentration of the tracer, represents the emission ratio variable of the precursor of [OVOCs] relative to the tracer, Represents the reaction rate variable of [OVOCs] precursors with OH radicals, Represents the emission ratio variable of [OVOCs] relative to the initial emission concentration of isoprene, Represents the background concentration of [OVOCs].

[0125] It can be understood that the emission ratio variable of [OVOCs] relative to the tracer refers to the unknown variable of the ratio of the theoretical concentration of primary anthropogenic emissions of [OVOCs] to the observed concentration of the tracer. The observed concentration of the tracer refers to the observed concentration of the tracer at the monitoring site. The emission ratio variable of [OVOCs] precursors relative to the tracer refers to the unknown variable of the ratio of the emission concentration of OVOCs precursors to the observed concentration of the tracer. The emission ratio variable of [OVOCs] relative to the initial emission concentration of isoprene refers to the unknown variable of the ratio of the theoretical concentration of primary anthropogenic emissions of [OVOCs] to the initial emission concentration of isoprene.

[0126] In an embodiment of the present invention, calculating the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model includes:

[0127] Using the photochemical age parameterization model to perform non-linear fitting on the actual [OVOCs] reaction rate constant, [OVOCs] observed concentration, tracer observed concentration, OH exposure, and initial isoprene emission concentration, and calculating the emission ratio of [OVOCs] relative to the tracer, the emission ratio of [OVOCs] precursors relative to the tracer, the reaction rate constant of [OVOCs] precursors with OH radicals, the emission ratio of [OVOCs] relative to the initial isoprene emission concentration, and the background concentration of [OVOCs] according to the preset least squares method;

[0128] Substituting the emission ratio of [OVOCs] relative to the tracer, the emission ratio of [OVOCs] precursors relative to the tracer, the reaction rate constant of [OVOCs] precursors with OH radicals, the emission ratio of [OVOCs] relative to the initial isoprene emission concentration, and the background concentration of [OVOCs] into the photochemical age parameterization model for calculation to obtain the theoretical concentration of primary anthropogenic emissions of [OVOCs].

[0129] It can be understood that substituting the actual [OVOCs] reaction rate constant, [OVOCs] observed concentration, tracer observed concentration, OH exposure, and initial isoprene emission concentration into the photochemical age parameterization model, and on the basis of minimizing the difference between the [OVOCs] observed concentration and the [OVOCs] theoretical concentration, solving by the least squares method 、 、 And , and then 、 , and Substitute the specific values of into the photochemical age parameterization model, and the theoretical concentration of primary anthropogenic emissions, secondary anthropogenic generation concentration, natural source emission concentration and background concentration of [OVOCs] can be calculated respectively.

[0130] S4. Perform photochemical loss correction and atmospheric diffusion correction on the observed concentration of primary anthropogenic emissions of the full-spectrum [VOCs] to obtain the initial concentration of primary anthropogenic emissions of [VOCs].

[0131] It is understandable that the photochemical loss correction refers to correcting the observed concentration of primary anthropogenic emissions of the full-spectrum [VOCs] for atmospheric photochemical loss, and the atmospheric diffusion correction refers to correcting the observed concentration of primary anthropogenic emissions of the full-spectrum [VOCs] for atmospheric diffusion.

[0132] In the embodiment of the present invention, performing photochemical loss correction and atmospheric diffusion correction on the observed concentration of primary anthropogenic emissions of the full-spectrum [VOCs] to obtain the initial concentration of primary anthropogenic emissions of [VOCs] includes:

[0133] Calculate the fitted reaction rate value according to the observed concentration of primary anthropogenic emissions of the full-spectrum [VOCs] using the following formula:

[0134]

[0135] where represents the observed concentration of primary anthropogenic emissions of the i-th [VOCs] at time t, represents the emission ratio of the i-th [VOCs] relative to the preset full-spectrum tracer, represents the fitted reaction rate value of the i-th [VOCs];

[0136] Obtain the theoretical reaction rate constant, and calculate the empirical coefficient according to the theoretical reaction rate constant, the fitted reaction rate value using the following formula:

[0137]

[0138] where represents the empirical coefficient, represents the theoretical reaction rate constant of the i-th [VOCs];

[0139] Calculate the initial concentration of primary anthropogenic emissions of [VOCs] according to the empirical coefficient using the following formula:

[0140]

[0141] Among them, represents the initial concentration of the i-th primary anthropogenic emission of [VOCs].

[0142] Furthermore, the full-spectrum tracer refers to the target tracer of the i-th full-spectrum [VOCs] selected according to the target machine learning algorithm. The fitted reaction rate value of the i-th [VOCs] refers to the fitted value of the reaction rate constant of the i-th [VOCs] with OH radicals. The theoretical reaction rate constant refers to the reaction rate constant of the i-th [VOCs] with OH radicals measured in the laboratory. The initial concentration of the i-th primary anthropogenic emission of [VOCs] refers to the initial concentration of the i-th [VOCs] emitted from the emission source.

[0143] S5. According to the pre-constructed PMF receptor model, use the initial concentration of the primary anthropogenic emission of [VOCs] to analyze the sources of VOCs, and complete the source analysis of the primary anthropogenic emission of VOCs based on the receptor model.

[0144] It can be understood that the PMF receptor model refers to the Positive Matrix Factorization (PMF) model. Since the source analysis of VOCs based on the initial concentration of the primary anthropogenic emission of [VOCs] and the PMF receptor model is a prior art, it will not be elaborated here.

[0145] To solve the problems described in the background art, the present invention first needs to construct a photochemical age parameterization model, and then calculate the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model. Since the photochemical age parameterization model includes known parameters, multiple unknown variables, multiple sets of measurable parameters, and multiple sets of computable parameters. Among them, the known parameters are: tracer reaction rate constants; multiple sets of unknown variables include: the emission ratio variable of [OVOCs] relative to the tracer, the emission ratio variable of [OVOCs] precursors relative to the tracer, the reaction rate variable of [OVOCs] precursors with OH radicals, the emission ratio variable of [OVOCs] relative to the initial emission concentration of isoprene, and the background concentration of [OVOCs]; multiple sets of measurable parameters include: the observed concentration of [OVOCs], the observed concentration of the tracer; multiple sets of computable parameters include: OH exposure, the reference reaction rate constant of [OVOCs], and the initial emission concentration of isoprene. Therefore, the observed concentration of [OVOCs], the observed concentration of the tracer, and the tracer reaction rate constant can be obtained first, and then the OH exposure, the initial emission concentration of isoprene, and the actual reaction rate constant of [OVOCs] can be calculated. At this time, the photochemical age parameterization model can be constructed based on the above-obtained and calculated parameters and multiple sets of unknown variables, and then the theoretical concentration of primary anthropogenic emissions of [OVOCs] can be calculated according to the photochemical age parameterization model. The anthropogenic emission observed concentration of [NMHCs] is observed by using a pre-constructed observation instrument to obtain the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs]. Among them, the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] refers to: the theoretical concentration of primary anthropogenic emissions of [OVOCs] and the anthropogenic emission observed concentration of [NMHCs]. Due to atmospheric photochemical loss and atmospheric diffusion, the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] needs to be corrected for photochemical loss and corrected for atmospheric diffusion to obtain the initial concentration of primary anthropogenic emissions of [VOCs]. Finally, based on the pre-constructed PMF receptor model, the source analysis of VOCs from primary anthropogenic emissions is completed by using the initial concentration of primary anthropogenic emissions of [VOCs]. Therefore, the present invention can improve the analysis accuracy of the PMF receptor model for the sources of VOCs in the actual atmosphere.

[0146] As Figure 2 shown, it is a functional module diagram of a source analysis system for primary anthropogenic emissions of VOCs based on a receptor model provided by an embodiment of the present invention.

[0147] The source analysis system 100 for primary anthropogenic VOC emissions based on the receptor model according to the present invention can be installed in an electronic device. According to the functions achieved, the source analysis system 100 for primary anthropogenic VOC emissions based on the receptor model can include a photochemical age parameterization model construction module 101, a calculation module 102 for the observed concentration of primary anthropogenic [OVOCs] emissions, a calculation module 103 for the initial concentration of primary anthropogenic [VOCs] emissions, and a source apportionment module 104 for [VOCs]. The modules in the present invention can also be referred to as units, which refer to a series of computer program segments that can be executed by the processor of an electronic device and can complete fixed functions, and are stored in the memory of the electronic device.

[0148] The photochemical age parameterization model construction module 101 is used to obtain the observed concentration of [OVOCs], the observed concentration of tracers, and the tracer reaction rate constant, calculate the OH exposure, the initial isoprene emission concentration, and the actual [OVOCs] reaction rate constant; and construct a photochemical age parameterization model using the OH exposure, the initial isoprene emission concentration, the observed concentration of [OVOCs], the observed concentration of tracers, the actual [OVOCs] reaction rate constant, and the tracer reaction rate constant.

[0149] The calculation module 102 for the observed concentration of primary anthropogenic [OVOCs] emissions is used to calculate the theoretical concentration of primary anthropogenic [OVOCs] emissions according to the photochemical age parameterization model, and use a pre-built observation instrument to observe the observed concentration of anthropogenic [NMHCs] emissions to obtain the observed concentration of primary anthropogenic full-spectrum [VOCs] emissions, where the observed concentration of primary anthropogenic full-spectrum [VOCs] emissions refers to the theoretical concentration of primary anthropogenic [OVOCs] emissions and the observed concentration of anthropogenic [NMHCs] emissions.

[0150] The calculation module 103 for the initial concentration of primary anthropogenic [VOCs] emissions is used to perform photochemical loss correction and atmospheric diffusion correction on the observed concentration of primary anthropogenic full-spectrum [VOCs] emissions to obtain the initial concentration of primary anthropogenic [VOCs] emissions.

[0151] The source apportionment module 104 for [VOCs] is used to perform VOCs source apportionment according to a pre-built PMF receptor model using the initial concentration of primary anthropogenic [VOCs] emissions.

[0152] Specifically, each of the modules in the source analysis system 100 for primary anthropogenic VOC emissions based on the receptor model in the embodiments of the present invention adopts the same technical means as those in the Figure 1 source analysis method for primary anthropogenic VOC emissions based on the receptor model described above, and can produce the same technical effects, which will not be elaborated here.

[0153] As shown Figure 3 in the figure, it is a schematic structural diagram of an electronic device for implementing a source analysis method of primary anthropogenic emission VOCs based on a receptor model provided by an embodiment of the present invention.

[0154] The electronic device 1 may include a processor 10, a memory 11, and a bus 12, and may further include a computer program stored in the memory 11 and executable on the processor 10, such as a source analysis method program of primary anthropogenic emission VOCs based on a receptor model.

[0155] Among them, the memory 11 includes at least one type of readable storage medium, and the readable storage medium includes flash memory, mobile hard disk, multimedia card, card-type memory (such as SD or DX memory, etc.), magnetic memory, magnetic disk, optical disc, etc. The memory 11 may be an internal storage unit of the electronic device 1 in some embodiments, such as the mobile hard disk of the electronic device 1. The memory 11 may also be an external storage device of the electronic device 1 in other embodiments, such as a plug-in mobile hard disk, a Smart Media Card (SMC), a Secure Digital (SD) card, a Flash Card, etc. equipped on the electronic device 1. Further, the memory 11 further includes an internal storage unit of the electronic device 1 and also includes an external storage device. The memory 11 can be used not only to store application software installed in the electronic device 1 and various types of data, such as the code of the source analysis method program of primary anthropogenic emission VOCs based on a receptor model, etc., but also to temporarily store data that has been output or will be output.

[0156] The processor 10 may be composed of integrated circuits in some embodiments. For example, it may be composed of a single packaged integrated circuit, or may be composed of multiple integrated circuits with the same or different functions, including a combination of one or more Central Processing Units (CPUs), microprocessors, digital processing chips, graphics processors, and various control chips. The processor 10 is the control core (Control Unit) of the electronic device, connecting various components of the entire electronic device through various interfaces and lines, and by running or executing programs or modules stored in the memory 11 (such as the source analysis method program of primary anthropogenic emission VOCs based on a receptor model, etc.), and calling data stored in the memory 11, to execute various functions of the electronic device 1 and process data.

[0157] The bus 12 can be a Peripheral Component Interconnect (PCI) bus, an Extended Industry Standard Architecture (EISA) bus, or the like. The bus 12 can be divided into an address bus, a data bus, a control bus, etc. The bus 12 is configured to enable connection and communication between the memory 11 and at least one processor 10, etc.

[0158] Figure 3 Only an electronic device with components is shown. Those skilled in the art can understand that Figure 3 The shown structure does not constitute a limitation on the electronic device 1, and it may include fewer or more components than shown, or combine certain components, or have a different component arrangement.

[0159] For example, although not shown, the electronic device 1 may further include a power source (such as a battery) for powering each component. Preferably, the power source can be logically connected to the at least one processor 10 through a power management device, so as to implement functions such as charge management, discharge management, and power consumption management through the power management device. The power source may also include any components such as one or more DC or AC power sources, a recharge device, a power failure detection circuit, a power converter or inverter, a power status indicator, etc. The electronic device 1 may also include various sensors, a Bluetooth module, a Wi-Fi module, etc., which will not be elaborated here.

[0160] Furthermore, the electronic device 1 may further include a network interface. Optionally, the network interface may include a wired interface and / or a wireless interface (such as a WI-FI interface, a Bluetooth interface, etc.), which is generally used to establish a communication connection between the electronic device 1 and other electronic devices.

[0161] Optionally, the electronic device 1 may further include a user interface. The user interface may be a display, an input unit (such as a keyboard), and optionally, the user interface may also be a standard wired interface or a wireless interface. Optionally, in some embodiments, the display may be an LED display, a liquid crystal display, a touch liquid crystal display, and an OLED (Organic Light-Emitting Diode) toucher, etc. Among them, the display may also be appropriately referred to as a display screen or a display unit, which is used to display the information processed in the electronic device 1 and to display a visual user interface.

[0162] The program of the source analysis method of primary anthropogenic emission VOCs based on the receptor model stored in the memory 11 in the electronic device 1 is a combination of multiple instructions. When running in the processor 10, it can achieve:

[0163] Obtain the observed concentration of [OVOCs], the observed concentration of tracers, and the tracer reaction rate constant, and calculate the OH exposure, the initial emission concentration of isoprene, and the actual reaction rate constant of [OVOCs];

[0164] Use the OH exposure, the initial emission concentration of isoprene, the observed concentration of [OVOCs], the observed concentration of tracers, the actual reaction rate constant of [OVOCs], and the tracer reaction rate constant to construct a photochemical age parameterization model;

[0165] Calculate the theoretical concentration of primary anthropogenic emission of [OVOCs] according to the photochemical age parameterization model, and use the pre-built observation instrument to observe the observed concentration of anthropogenic emission of [NMHCs] to obtain the observed concentration of primary anthropogenic emission of full-spectrum [VOCs]. Among them, the observed concentration of primary anthropogenic emission of full-spectrum [VOCs] refers to: the theoretical concentration of primary anthropogenic emission of [OVOCs] and the observed concentration of anthropogenic emission of [NMHCs];

[0166] Perform photochemical loss correction and atmospheric diffusion correction on the observed concentration of primary anthropogenic emission of full-spectrum [VOCs] to obtain the initial concentration of primary anthropogenic emission of [VOCs];

[0167] According to the pre-built PMF receptor model, use the initial concentration of primary anthropogenic emission of [VOCs] to perform source analysis of VOCs, and complete the source analysis of primary anthropogenic emission VOCs based on the receptor model.

[0168] Specifically, the specific implementation method of the above instructions by the processor 10 can refer to Figures 1 to 3 The description of the relevant steps in the corresponding embodiments will not be repeated here.

[0169] Furthermore, if the module / unit integrated in the electronic device 1 is implemented in the form of a software functional unit and sold or used as an independent product, it can be stored in a computer-readable storage medium. The computer-readable storage medium can be volatile or non-volatile. For example, the computer-readable medium can include: any entity or device capable of carrying the computer program code, a recording medium, a USB flash drive, a mobile hard disk, a magnetic disk, an optical disc, a computer memory, a read-only memory (ROM, Read-Only Memory).

[0170] The present invention also provides a computer-readable storage medium storing a computer program, which when executed by a processor of an electronic device, can implement:

[0171] Obtain the observed concentrations of [OVOCs], the observed concentrations of tracers, and the tracer reaction rate constants, and calculate the OH exposure, the initial isoprene emission concentration, and the actual [OVOCs] reaction rate constants;

[0172] Construct a photochemical age parameterization model using the OH exposure, the initial isoprene emission concentration, the [OVOCs] observed concentration, the tracer observed concentration, the actual [OVOCs] reaction rate constants, and the tracer reaction rate constants;

[0173] Calculate the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model, and use a pre-constructed observation instrument to observe the anthropogenic emission observed concentration of [NMHCs] to obtain the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs], where the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] refers to: the theoretical concentration of primary anthropogenic emissions of [OVOCs] and the anthropogenic emission observed concentration of [NMHCs];

[0174] Perform photochemical loss correction and atmospheric diffusion correction on the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] to obtain the initial concentration of primary anthropogenic emissions of [VOCs];

[0175] According to the pre-constructed PMF receptor model, perform source analysis of VOCs using the initial concentration of primary anthropogenic emissions of [VOCs] to complete the source analysis of primary anthropogenic emissions of VOCs based on the receptor model.

[0176] In several embodiments provided by the present invention, it should be understood that the disclosed devices, systems, and methods can be implemented in other ways. For example, the system embodiments described above are only illustrative, and there can be other division methods in actual implementation.

[0177] The modules described as separate components may or may not be physically separated, and the components shown as modules may or may not be physical units, that is, they can be located in one place, or they can be distributed to multiple network units. Some or all of the modules can be selected according to actual needs to achieve the purpose of the solution of this embodiment.

[0178] In addition, in each embodiment of the present invention, the functional modules can be integrated into one processing unit, or each unit can exist physically alone, or two or more units can be integrated into one unit. The above integrated units can be implemented in the form of hardware, or in the form of a combination of hardware and software functional modules.

[0179] It is obvious to those skilled in the art that the present invention is not limited to the details of the above-described exemplary embodiments, and that the present invention can be implemented in other specific forms without departing from the spirit or essential characteristics of the present invention.

[0180] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and not to limit them. Although the present invention has been described in detail with reference to the preferred embodiments, those of ordinary skill in the art should understand that the technical solutions of the present invention can be modified or equivalently replaced without departing from the spirit and scope of the technical solutions of the present invention.

Claims

1. A method for analyzing the sources of primary anthropogenic VOC emissions based on a receptor model, characterized in that, The method includes: Obtaining the observed concentrations of [OVOCs], the observed concentrations of tracers, and the reaction rate constants of tracers, and calculating the OH exposure, the initial emission concentration of isoprene, and the actual reaction rate constant of [OVOCs]; Constructing a photochemical age parameterization model using the OH exposure, the initial emission concentration of isoprene, the observed concentration of [OVOCs], the observed concentration of tracers, the actual reaction rate constant of [OVOCs], and the reaction rate constant of tracers; Calculating the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model, and using a pre-constructed observation instrument to observe the anthropogenic emission observed concentration of [NMHCs] to obtain the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs], where the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] refers to: the theoretical concentration of primary anthropogenic emissions of [OVOCs] and the anthropogenic emission observed concentration of [NMHCs]; Performing photochemical loss correction and atmospheric diffusion correction on the observed concentration of primary anthropogenic emissions of full-spectrum [VOCs] to obtain the initial concentration of primary anthropogenic emissions of [VOCs]; According to a pre-constructed PMF receptor model, using the initial concentration of primary anthropogenic emissions of [VOCs] to conduct source analysis of VOCs, and completing the source analysis of primary anthropogenic emissions of VOCs based on the receptor model; After calculating the theoretical concentration of primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model, the method further includes: Successively extracting atmospheric volatile organic compounds in a pre-constructed set of atmospheric volatile organic compounds to obtain multiple sets of tracer-[OVOCs] training sets and multiple sets of tracer-[OVOCs] validation sets of the atmospheric volatile organic compounds, where the tracer training concentration in the tracer-[OVOCs] training set is the independent variable, and the [OVOCs] observed training concentration is the dependent variable, each set of tracer-[OVOCs] training set and each set of tracer-[OVOCs] validation set correspond to the tracer category, the multiple sets of tracer-[OVOCs] validation sets are calculated according to the photochemical age parameterization model, and the atmospheric volatile organic compounds belong to non-methane hydrocarbons or oxygenated volatile organic compounds; Successively extracting initial machine learning algorithms in a pre-constructed set of machine learning algorithms, where the initial machine learning algorithms include: decision tree algorithm, random forest algorithm, extremely randomized tree algorithm, gradient boosting decision tree algorithm, Adaboost algorithm, Catboost algorithm, Xgboost algorithm, LightGBM algorithm; Successively extracting the tracer-[OVOCs] training set in the multiple sets of tracer-[OVOCs] training sets; Training the initial machine learning algorithm using the tracer-[OVOCs] training set to obtain a target machine learning algorithm; Verify the target machine learning algorithm using the tracer-[OVOCs] verification set to obtain a prediction accuracy set, and calculate the average prediction accuracy of the prediction accuracy set. The average prediction accuracy in the average prediction accuracy set represents the voting score value of the target machine learning algorithm for the tracer category; Summarize the average prediction accuracies corresponding to each group of tracer-[OVOCs] training sets to obtain an average prediction accuracy set; Summarize the average prediction accuracy sets corresponding to each target machine learning algorithm to obtain multiple groups of average prediction accuracy sets; Use the following formula to calculate the tracer score value based on the multiple groups of average prediction accuracy sets to obtain a tracer score value set: Among them, represents the tracer score value of the p-th tracer, Q represents the number of target machine learning algorithms, represents the average prediction accuracy of the q-th target machine learning algorithm for the p-th tracer; Extract the maximum tracer score in the tracer score value set and identify the tracer category corresponding to the maximum tracer score; Use the tracer category corresponding to the maximum tracer score as the target tracer for the atmospheric volatile organic compounds.

2. The source analysis method of primary anthropogenic VOC emissions based on the receptor model according to claim 1, wherein, The calculation of the OH exposure, isoprene initial emission concentration, and actual [OVOCs] reaction rate constant includes: Obtain the emission concentration ratio and observed concentration ratio of the benzene series species pair, where the two benzene series species in the benzene series species pair have the same source and different chemical activities; Calculate the OH exposure using the emission concentration ratio and observed concentration ratio according to the pre-constructed OH exposure formula; Obtain the observed concentration of isoprene, and calculate the isoprene initial emission concentration using the following formula based on the OH exposure and the observed concentration of isoprene: Among them, represents the initial emission concentration of isoprene, represents the observed concentration of isoprene at time represents the reaction rate constant of isoprene, represents the OH exposure; Calculate the photolysis rate of [OVOCs] using the pre-constructed photolysis rate formula; Calculate the actual [OVOCs] reaction rate constant according to the OVOCs photolysis rate using the pre-constructed OVOCs reaction rate formula.

3. The method for analyzing the sources of anthropogenic VOC emissions based on the receptor model according to claim 2, wherein The OH exposure formula is as follows: Among them, represents the OH exposure amount, represents the reaction rate constant of species C and OH radicals in the benzene series species pair, represents the reaction rate constant of species B and OH radicals in the benzene series species pair, represents the natural logarithm symbol, represents the emission concentration ratio of species C and species B at time, represents the observed concentration ratio of species C and species B at time.

4. The method for analyzing the source of anthropogenic VOC emissions based on the receptor model according to claim 3, characterized in that The photolysis rate formula is as follows: Among them, represents the photolysis rate of [OVOCs], represents the photolysis rate of [OVOCs] under clear sky conditions, represents the photolysis rate under clear sky conditions, represents the measured photolysis rate.

5. The source analysis method of primary anthropogenic VOC emissions based on the receptor model according to claim 4, characterized in that, The OVOCs reaction rate formula is as follows: Among them, represents the actual [OVOCs] reaction rate constant, represents the reference [OVOCs] reaction rate constant, represents the [OVOCs] photolysis rate, represents the OH radical concentration.

6. The receptor model-based source analysis method for primary anthropogenic VOC emissions as claimed in claim 5, wherein, The photochemical age parameterization model is as follows: Among them, represents the observed concentration of [OVOCs], represents the observed concentration of the tracer, represents the emission ratio variable of [OVOCs] relative to the tracer, represents the reaction rate constant of the tracer, represents the observed concentration of the tracer, represents the emission ratio variable of the [OVOCs] precursor relative to the tracer, represents the reaction rate variable of the [OVOCs] precursor with the OH radical, represents the emission ratio variable of [OVOCs] relative to the initial emission concentration of isoprene, represents the background concentration of [OVOCs].

7. The method for analyzing the sources of VOCs emitted by a single anthropogenic emission based on the receptor model according to claim 6, characterized in that The calculation of the theoretical concentration of the primary anthropogenic emissions of [OVOCs] according to the photochemical age parameterization model includes: Perform non-linear fitting on the actual [OVOCs] reaction rate constant, [OVOCs] observed concentration, tracer observed concentration, OH exposure, and isoprene initial emission concentration using the photochemical age parameterization model, and calculate the emission ratio of [OVOCs] relative to the tracer, the emission ratio of [OVOCs] precursors relative to the tracer, the reaction rate constant of [OVOCs] precursors with OH radicals, the emission ratio of [OVOCs] relative to the isoprene initial emission concentration, and the [OVOCs] background concentration according to the preset least squares method; Substitute the emission ratio of [OVOCs] relative to the tracer, the emission ratio of [OVOCs] precursors relative to the tracer, the reaction rate constant of [OVOCs] precursors with OH radicals, the emission ratio of [OVOCs] relative to the isoprene initial emission concentration, and the [OVOCs] background concentration into the photochemical age parameterization model for calculation to obtain the theoretical concentration of the primary anthropogenic emissions of [OVOCs].

8. The source analysis method of primary anthropogenic emission VOCs based on the receptor model according to claim 7, wherein Performing photochemical loss correction and atmospheric diffusion correction on the observed concentration of the primary anthropogenic emissions of the full-spectrum [VOCs] to obtain the initial concentration of the primary anthropogenic emissions of [VOCs], including: According to the observed concentration of the first anthropogenic emissions of the full-spectrum [VOCs], calculate using the following formula Fitted reaction rate: Among them, represents the observed concentration of the i-th [VOCs] from anthropogenic emissions at time t, represents the emission ratio of the i-th [VOCs] relative to a preset full-spectrum tracer, represents the fitted value of the reaction rate of the i-th [VOCs]; Obtain the theoretical reaction rate constant, according to the theoretical reaction rate constant, the fitted reaction rate value, calculate the empirical coefficient using the following formula: Among them, represents the empirical coefficient, represents the theoretical constant of the reaction rate of the i-th [VOCs]; Calculating the initial concentration of the primary anthropogenic emissions of [VOCs] using the following formula according to the empirical coefficient: Among them, represents the initial concentration of the i-th primary anthropogenic emission of [VOCs].

9. A source analysis system for primary anthropogenic VOC emissions based on a receptor model, characterized in that, The system includes: A photochemical age parameterization model construction module, configured to obtain the observed concentration of [OVOCs], the observed concentration of the tracer, and the reaction rate constant of the tracer, calculate the OH exposure, the initial emission concentration of isoprene, and the actual reaction rate constant of [OVOCs]; constructing a photochemical age parameterization model using the OH exposure, the initial emission concentration of isoprene, the observed concentration of [OVOCs], the observed concentration of the tracer, the actual reaction rate constant of [OVOCs], and the reaction rate constant of the tracer; [OVOCs] Primary anthropogenic emission observed concentration calculation module, which is used to calculate the theoretical concentration of [OVOCs] primary anthropogenic emissions according to the photochemical age parameterization model, and use pre-built observation instruments to observe the anthropogenic emission observed concentration of [NMHCs] to obtain the observed concentration of [VOCs] primary anthropogenic emissions in the full spectrum, where the observed concentration of [VOCs] primary anthropogenic emissions in the full spectrum refers to: the theoretical concentration of [OVOCs] primary anthropogenic emissions and the observed concentration of [NMHCs] anthropogenic emissions; after calculating the theoretical concentration of [OVOCs] primary anthropogenic emissions according to the photochemical age parameterization model, successively extract atmospheric volatile organic compounds in the pre-built atmospheric volatile organic compounds to obtain multiple groups of tracers - [OVOCs] training sets and multiple groups of tracers - [OVOCs] validation sets, where the tracer training concentration in the tracer - [OVOCs] training set is the independent variable, and the observed training concentration of [OVOCs] is the dependent variable. Each group of tracers - [OVOCs] training set and each group of tracers - [OVOCs] validation set correspond to the tracer category. The multiple groups of tracers - [OVOCs] validation sets are calculated and obtained according to the photochemical age parameterization model. The atmospheric volatile organic compounds belong to non-methane hydrocarbons or oxygenated volatile organic compounds; successively extract initial machine learning algorithms in the pre-built machine learning algorithm set, where the initial machine learning algorithms include: decision tree algorithm, random forest algorithm, extremely randomized tree algorithm, gradient boosting decision tree algorithm, Adaboost algorithm, Catboost algorithm, Xgboost algorithm, LightGBM algorithm; successively extract the tracer - [OVOCs] training set in the multiple groups of tracers - [OVOCs] training sets; use the tracer - [OVOCs] training set to train the initial machine learning algorithm to obtain the target machine learning algorithm; use the tracer - [OVOCs] validation set to verify the target machine learning algorithm to obtain the prediction accuracy set, and calculate the average prediction accuracy of the prediction accuracy set, where the average prediction accuracy in the average prediction accuracy set represents the voting score value of the target machine learning algorithm for the tracer category; summarize the average prediction accuracy corresponding to each group of tracers - [OVOCs] training sets to obtain the average prediction accuracy set; summarize the average prediction accuracy sets corresponding to each target machine learning algorithm to obtain multiple groups of average prediction accuracy sets; use the following formula to calculate the tracer score value according to the multiple groups of average prediction accuracy sets to obtain the tracer score value set: Among them, represents the tracer score value of the p-th tracer, Q represents the number of target machine learning algorithms, represents the average prediction accuracy of the q-th target machine learning algorithm for the p-th tracer; extract the maximum tracer score from the set of tracer score values, and identify the tracer category corresponding to the maximum tracer score; use the tracer category corresponding to the maximum tracer score as the target tracer of the atmospheric volatile organic compounds; [VOCs] Primary anthropogenic emission initial concentration calculation module, which is used to correct the photochemical loss and correct the atmospheric diffusion of the observed concentration of [VOCs] primary anthropogenic emissions in the full spectrum to obtain the initial concentration of [VOCs] primary anthropogenic emissions; [VOCs] Source apportionment module, which is used to perform VOCs source apportionment according to the pre-built PMF receptor model by using the initial concentration of [VOCs] primary anthropogenic emissions.

Images