Aerosol growth mechanism decoupling monitoring system and secondary aerosol heterogeneous nucleation and agglomeration contribution share quantification method

Abstract

The invention relates to an aerosol growth mechanism decoupling monitoring system and a secondary aerosol heterogeneous nucleation and agglomeration contribution share quantification method. The monitoring system comprises a condensation nucleus control module, an isotope CO2 regulation and control module, a multi-measuring-point absorption tower and a particle monitoring analysis module, and the condensation nucleus control module is used for generating carbon-free monodisperse SiO2 aerosol condensation nucleuses; the isotope CO2 regulation and control module is used for providing 13CO2 mixed gas with target regulation and control concentration for the premixing tank; a tower body of the multi-measuring-point absorption tower is axially provided with a plurality of particle sampling points for capturing dynamic changes in the aerosol growth process; the particle monitoring and analyzing module is used for collecting and analyzing the silicon content difference and the carbon isotope content difference of particles at adjacent measuring points. Compared with the prior art, the method provided by the invention can be used for quasi-decoupling heterogeneous nucleation and agglomeration, quantifies the contribution of the heterogeneous nucleation and agglomeration to aerosol mass transfer growth, and provides a scientific basis for optimizing parameters of an amine method carbon capture process and reducing the escape rate of an absorbent.

Description

Technical Field

[0001] The present invention relates to the field of carbon capture and storage technology, and in particular to an aerosol growth mechanism decoupling monitoring system and a method for quantifying heterogeneous nucleation and agglomeration contribution shares. Background Art

[0002] With the growing need for global carbon emission reduction, carbon capture, utilization, and storage (CCUS) technology has become a key path to achieving carbon neutrality. Organic amine-based carbon capture processes, due to their high absorption efficiency and advanced technology, are widely used in coal-fired power plants, chemical plants, and other locations. However, this process suffers from absorbent escape during operation, primarily due to the abnormal growth of secondary aerosols within the absorption tower.

[0003] This type of aerosol is formed by the reaction of amines with CO₂, generating volatile substances (such as carbamates) that combine with heterogeneous condensation nuclei. Its growth mechanism involves complex physical and chemical processes, including reaction-induced heterogeneous nucleation and interparticle collision and agglomeration. The continued growth of the aerosol not only leads to absorbent loss and increased operating costs, but also exacerbates equipment corrosion and subsequent energy consumption for capture fluid regeneration, severely restricting the economic viability and scalability of amine-based processes.

[0004] Reference patents CN117782702A and CN106226842A, respectively, address radioactivity monitoring methods for nuclear detection and testing the impact of urban surface aerosols on lightning processes. These technologies focus on monitoring and analyzing aerosols under specific conditions, providing important technical support for the field of environmental science. However, these methods and technologies have limitations in analyzing aerosol growth mechanisms, particularly the contribution of heterogeneous nucleation and agglomeration processes, making it difficult to achieve decoupled monitoring and precise quantification of aerosol growth mechanisms.

[0005] Although the reference patent CN117782702A provides a method for monitoring trace uranium and plutonium radioactivity, the method mainly focuses on the monitoring of radioactive nuclides and fails to deeply explore the growth mechanism of aerosols.

[0006] Although reference patent CN106226842A involves the impact of aerosols on lightning processes, its focus is on the relationship between the observation of lightning activity and aerosol distribution. It also fails to conduct in-depth research on the aerosol growth mechanism, especially the contribution analysis of heterogeneous nucleation and agglomeration processes.

[0007] At present, research on secondary aerosol growth mostly focuses on the heterogeneous nucleation mechanism. For example, the mainstream theory holds that: amine-CO2-condensation nuclei generate stable salt particles through chemical reactions, and the concentration gradient between the aerosol surface and the gas phase drives the mass transfer of amine and CO2 to the interior of the particles, while water migration further promotes particle growth. However, in actual working conditions, aerosol growth is also significantly affected by the physical agglomeration between particles, such as van der Waals forces or particle mergers caused by turbulent collisions. Since heterogeneous nucleation and agglomeration are highly coupled in time and space, traditional experimental methods (such as particle size distribution monitoring and total particle mass balance) are difficult to distinguish the contribution of the two, resulting in large errors in aerosol dynamics models and a lack of targeted control strategies in engineering.

[0008] The limitations of existing technologies are mainly reflected in:

[0009] Insufficient labeling methods: If the condensation nuclei themselves contain carbon (such as carbon black particles), the background carbon element will interfere with the detection of the carbon increment generated by the reaction, leading to an overestimation of the contribution of heterogeneous nucleation;

[0010] Lack of dynamic monitoring: Single-point sampling or overall mass balance methods cannot capture the dynamic evolution of aerosols along the height of the absorption tower, making it difficult to establish the correlation between growth mechanism and spatial location;

[0011] Gaps in decoupling algorithms: There is a lack of quantitative separation methods based on characteristic markers, and existing models rely on hypothetical parameters, lacking universality and accuracy.

[0012] To this end, it is urgent to develop a method that can accurately decouple heterogeneous nucleation and agglomeration and quantify the contribution of the two to aerosol mass transfer growth, so as to provide a scientific basis for optimizing amine carbon capture process parameters and reducing absorbent escape rate. Summary of the Invention

[0013] The purpose of the present invention is to overcome the defects of the above-mentioned prior art and to provide an aerosol growth mechanism decoupling monitoring system and a method for quantifying the contribution of secondary aerosol heterogeneous nucleation and agglomeration. It can be used to quasi-decouple heterogeneous nucleation and agglomeration, quantify the contribution of the two to aerosol mass transfer growth, and provide a scientific basis for optimizing amine carbon capture process parameters and reducing absorbent escape rate.

[0014] The purpose of the present invention can be achieved by the following technical solutions:

[0015] The first aspect of the present invention provides an aerosol growth mechanism decoupling monitoring system, comprising a condensation nucleus control module, an isotope CO2 control module, a multi-point absorption tower, and a particle monitoring and analysis module, wherein specifically:

[0016] The condensation nucleus control module is used to generate carbon-free monodisperse SiO2 aerosol condensation nuclei;

[0017] The isotope CO2 control module is connected to the condensation nucleus control module to provide the target control concentration to the premix tank. 13 CO2 mixed gas;

[0018] The multi-point absorption tower is connected to the isotope CO2 control module and is used to carry out the aerosol growth process and the gas-liquid mass transfer process. The multi-point absorption tower is provided with a plurality of particle sampling points along the axial direction for capturing the dynamic changes of the aerosol growth process.

[0019] The particle monitoring and analysis module is connected to each particle sampling point through a pipeline. The particle monitoring and analysis module is used to collect and analyze the silicon content differences and carbon isotope content differences of particles at adjacent measuring points. The silicon content differences and carbon isotope content differences are used to generate a decoupling report on the contribution share of the heterogeneous nucleation and agglomeration mechanism.

[0020] Furthermore, the condensation nucleus control module includes a monodisperse SiO2 particle generator, a magnetic stirring device, an ultrasonic atomizer, a silica gel drying tube, and a premixing tank, which are sequentially connected through pipelines;

[0021] The monodisperse SiO2 particle generator is used to generate a carbon-free monodisperse SiO2 particle suspension with a particle size range of 50-500 nm and a controllable concentration;

[0022] The magnetic stirring device is used to stir and disperse the SiO2 particle suspension to prevent the particles from agglomerating;

[0023] The silica gel drying tube is used to dehydrate the atomized wet particles to generate dry SiO2 aerosol condensation nuclei;

[0024] The output end of the premixing tank is connected to the bottom air inlet of the multi-point absorption tower, and is used to mix the dry SiO2 aerosol condensation nuclei with the isotope 13 The CO2 mixed gas is evenly mixed to form a simulated flue gas aerosol environment.

[0025] Furthermore, the isotope CO2 control module includes a gas cylinder group, which is connected to the premixing tank through a gas delivery pipeline, and the gas delivery pipeline is matched with a mass flow meter group.

[0026] Furthermore, the gas cylinder group includes 13 CO2 gas cylinder, N2 gas cylinder, O2 gas cylinder, and 13 The CO2 gas cylinder, N2 gas cylinder, and O2 gas cylinder are respectively connected to the premixing tank through gas delivery pipelines, and each of the gas delivery pipelines is provided with a mass flow meter;

[0027] The isotope CO2 control module also includes a heating belt, which is wound on the pipeline between the silica gel drying tube and the premixing tank, and on the pipeline between the premixing tank and the multi-measuring point absorption tower.

[0028] Furthermore, the particle sampling points in the multi-point absorption tower are evenly spaced along the axial direction of the tower body, with a spacing of 10%-15% of the tower height;

[0029] The top of the multi-measurement point absorption tower is provided with an organic amine absorbent liquid input port and a purified gas discharge port;

[0030] A simulated flue gas injection port and a rich amine liquid discharge port are provided at the bottom of the multi-measuring point absorption tower.

[0031] Furthermore, the particle monitoring and analysis module includes a micro HEPA filter array and a solid phase component analysis unit;

[0032] The micro HEPA filter array includes a plurality of micro HEPA filters (high efficiency air filters), each micro HEPA filter is connected to a particle sampling point via a pipeline, and each micro HEPA filter is connected to a solid phase component analysis unit;

[0033] The solid phase component analysis unit includes one or more of an inductively coupled plasma emission spectrometer, an isotope ratio mass spectrometer, and a scanning electron microscope-energy dispersive spectrometer. The solid phase component analysis unit is used to simultaneously measure the silicon content, carbon isotope abundance, particle size distribution, and surface morphology of the particles.

[0034] A second aspect of the present invention provides a method for quantifying the contribution of heterogeneous nucleation and agglomeration of secondary aerosols, comprising the following steps:

[0035] S1. Condensation nuclei mixed with isotope-labeled gas:

[0036] The carbon-free monodisperse SiO2 aerosol condensation nuclei are generated by atomization drying through the condensation nucleus control module, and the carbon-free monodisperse SiO2 aerosol condensation nuclei are mixed with the isotope CO2 control module. 13 The CO2 mixed gas is evenly mixed in the premixing tank to generate simulated smoke aerosol;

[0037] S2. Dynamic aerosol collection at multiple measurement points:

[0038] The aerosol obtained in S1 is passed into a multi-point absorption tower for gas-liquid mass transfer, and aerosol particle information at different heights is synchronously collected through multiple particle sampling points arranged at equal intervals along the axial direction of the multi-point absorption tower;

[0039] S3. Decoupling calculation of agglomeration and nucleation contributions:

[0040] Based on the differences in silicon content and carbon isotope content between adjacent particle sampling points, the contributions of agglomeration and heterogeneous nucleation to aerosol mass transfer growth were calculated respectively.

[0041] Furthermore, in S1, the specific steps of generating carbon-free monodisperse SiO2 aerosol condensation nuclei include:

[0042] The SiO2 particle suspension is stirred and dispersed by a magnetic stirring device, then atomized and dehydrated through a silica gel drying tube to form a dry aerosol;

[0043] will contain 13 CO2 mixed gas 13 The volume concentration of CO2 is regulated by a mass flow meter and mixed with the dehydrated SiO2 aerosol in a premixing tank. The gas mixing temperature is controlled by a heating tape wrapped around the pipeline.

[0044] Furthermore, in S2, the particle sampling points of the multi-point absorption tower are evenly spaced along the axial direction of the tower body, and the spacing is 10%-15% of the tower body height;

[0045] During collection, aerosol particles are captured by a micro HEPA filter, and the particle mass concentration and sampling time of each measuring point are recorded.

[0046] Furthermore, in S3, the specific steps for calculating the contribution share include:

[0047] Solid phase composition analysis was used to determine the differences in silicon content and carbon isotope content of particles at adjacent measurement points. The silicon content difference was used to characterize the mass transfer increment caused by agglomeration, while the carbon isotope content difference was used to characterize the mass transfer increment caused by heterogeneous nucleation.

[0048] The sum of the differences in mass transfer increments caused by agglomeration and heterogeneous nucleation was taken as the total mass transfer growth. The agglomeration contribution was calculated by the ratio of the silicon content difference to the total mass transfer growth, and the heterogeneous nucleation contribution was calculated by the ratio of the carbon isotope content difference to the total mass transfer growth.

[0049] Compared with the prior art, the present invention has the following beneficial effects:

[0050] 1) Monodisperse SiO2 particles are used as condensation nuclei. Their carbon-free nature avoids the interference of traditional carbon black and other carbon-containing condensation nuclei on the carbon increment detection in the heterogeneous nucleation process, ensuring the carbon isotope ( 13 C) The uniqueness and accuracy of the marking data provide a reliable benchmark for contribution share calculation.

[0051] 2) Pass 13CO2-directed labeling of carbon sources, combined with solid-phase component analysis technology (such as IRMS), can specifically distinguish the source of carbon elements in aerosols (reaction generation vs. environmental background), directly correlate the quantitative relationship between heterogeneous nucleation and carbon increment, and break through the limitation of traditional total carbon detection methods that cannot eliminate background interference.

[0052] 3) Carbon content and particle size distribution data, combined with time-space evolution laws, dynamically analyze the competitive / synergistic relationship between heterogeneous nucleation and agglomeration, providing data support for the establishment of a refined kinetic model.

[0053] 4) Based on the difference in silicon content (ΔSi%) between adjacent measuring points, the contribution of pure physical agglomeration is characterized, and the difference in carbon isotope content (Δ 13 The nucleation contribution driven by chemical reactions is characterized by the difference ratio (C%), which directly quantifies the proportion of the two. The algorithm has clear logic and does not require complex assumptions. The decoupling accuracy is improved by more than 60% compared with the traditional single-parameter method.

[0054] 5) By clarifying the contribution weights of heterogeneous nucleation and agglomeration, absorber operating parameters (such as temperature, amine concentration, and gas flow rate) can be optimized to prioritize the suppression of the dominant growth mechanism. For example, if agglomeration contributes more than 70%, particle collisions can be suppressed by enhancing turbulence. If nucleation is the primary contribution, CO2 partial pressure can be adjusted or inhibitors can be added to block the reaction pathway, thereby reducing the absorbent escape rate by 30%-50% and extending the equipment maintenance cycle. BRIEF DESCRIPTION OF THE DRAWINGS

[0055] Figure 1 Schematic diagram of the overall structure of the aerosol growth mechanism decoupling monitoring system of the present invention;

[0056] Figure 2 Schematic diagram of the structure of the isotope CO2 control module in the present invention;

[0057] Figure 3 It is a structural schematic diagram of the multi-measuring point absorption tower of the present invention;

[0058] Figure 4 Schematic diagram of the packed absorption tower 3 module with multiple measuring points in the present invention

[0059] Figure 5 It is a structural diagram of the particle monitoring and analysis module of the present invention.

[0060] In the picture:

[0061] 1.1. Monodisperse silica particles; 1.2. Magnetic stirring device; 1.3. Atomizer device; 1.4. Silica gel drying tube device; 1.5. Premix tank;

[0062] 2.1. Gas cylinder assembly; 2.2. Mass flow meter assembly; 2.3. Heating tape;

[0063] 3.1, particle sampling point;

[0064] 4.1. Micro HEPA filter; 4.2. Solid phase product detection. DETAILED DESCRIPTION

[0065] The present invention is described in detail below with reference to the accompanying drawings and specific embodiments. Component models, material names, connection structures, circuit structures, control methods, algorithms, and other features not explicitly described in this technical solution are considered common technical features disclosed in the prior art.

[0066] Example 1

[0067] The aerosol growth mechanism decoupling monitoring system in this embodiment includes a condensation nucleus control module 1, an isotope CO2 control module 2, a multi-point absorption tower 3, and a particle monitoring and analysis module 4. Figures 1 to 5 .

[0068] The condensation nucleus control module 1 is used to generate carbon-free monodisperse SiO2 aerosol condensation nuclei; the isotope CO2 control module 2 is connected to the condensation nucleus control module 1 and is used to provide the target control concentration to the premixing tank 1.5. 13 CO2 mixed gas; a multi-measuring point absorption tower 3 is connected to the isotope CO2 control module 2, and is used to carry out the aerosol growth process and the gas-liquid mass transfer process. The tower body of the multi-measuring point absorption tower 3 is axially provided with multiple particle sampling points 3.1 for capturing the dynamic changes of the aerosol growth process; a particle monitoring and analysis module 4 is connected to each particle sampling point 3.1 through a pipeline. The particle monitoring and analysis module 4 is used to collect and analyze the silicon content difference and carbon isotope content difference of particles at adjacent measuring points. The silicon content difference and carbon isotope content difference are used to generate a decoupling report on the contribution share of the heterogeneous nucleation and agglomeration mechanism.

[0069] During specific implementation, the condensation nucleus control module 1 includes a monodisperse SiO2 particle generator 1.1, a magnetic stirring device 1.2, an ultrasonic atomizer 1.3, a silica gel drying tube 1.4, and a premixing tank 1.5, which are connected in sequence through pipelines; the monodisperse SiO2 particle generator 1.1 is used to generate a carbon-free monodisperse SiO2 particle suspension with a particle size range of 50-500nm and a controllable concentration; the magnetic stirring device 1.2 is used to stir and disperse the SiO2 particle suspension to prevent particle agglomeration; the silica gel drying tube 1.4 is used to dehydrate the atomized wet particles to generate dry SiO2 aerosol condensation nuclei; the premixing tank 1.5, whose output end is connected to the bottom air inlet of the multi-measuring point absorption tower 3, is used to mix the dry SiO2 aerosol condensation nuclei with the isotope 13 The CO2 mixed gas is evenly mixed to form a simulated flue gas aerosol environment.

[0070] During specific implementation, the multi-measuring point absorption tower 3 is a packed tower.

[0071] In a specific implementation, the premixing tank 1.5 is connected via a gas delivery pipeline, and the gas delivery pipeline is matched with a mass flow meter group 2.2.

[0072] In specific implementation, the gas cylinder group 2.1 includes 13 CO2 gas cylinder, N2 gas cylinder, O2 gas cylinder, and 13 The CO2 gas cylinder, N2 gas cylinder, and O2 gas cylinder are respectively connected to the premixing tank 1.5 through gas delivery pipelines, and each of the gas delivery pipelines is provided with a mass flow meter.

[0073] In specific implementation, the isotope CO2 control module 2 further includes a heating belt 2.3, which is wound on the pipeline between the silica gel drying tube 1.4 and the premixing tank 1.5, and on the pipeline between the premixing tank 1.5 and the multi-measuring point absorption tower 3.

[0074] In specific implementation, the particle sampling points 3.1 in the multi-point absorption tower 3 are evenly spaced along the axial direction of the tower body, with the spacing being 10%-15% of the tower height.

[0075] The top of the multi-measuring point absorption tower 3 is provided with an organic amine absorbent liquid inlet and a purified gas outlet; the bottom of the multi-measuring point absorption tower 3 is provided with a simulated flue gas injection port and a rich amine liquid outlet.

[0076] The particle monitoring and analysis module 4 includes a micro HEPA filter array 4.1 and a solid phase component analysis unit 4.2.

[0077] In specific implementation, the micro HEPA filter array 4.1 includes multiple micro HEPA filters (high efficiency air filters), each micro HEPA filter is connected to a particle sampling point 3.1 through a pipeline, and each micro HEPA filter is connected to the solid phase component analysis unit 4.2.

[0078] In specific implementation, the solid phase component analysis unit 4.2 includes one or more of an inductively coupled plasma emission spectrometer, an isotope ratio mass spectrometer, and a scanning electron microscope-energy spectrometer. The solid phase component analysis unit 4.2 is used to simultaneously measure the silicon content, carbon isotope abundance, particle size distribution, and surface morphology of the particles.

[0079] The operating mechanism of the aerosol growth mechanism decoupling monitoring system in this embodiment is as follows (combined with Figure 1-5): The condensation nucleus control module 1 generates carbon-free condensation nuclei through the monodisperse SiO2 particle generator 1.1, disperses them through the magnetic stirring device 1.2, atomizes them by the ultrasonic atomizer 1.3, and dehydrates them through the silica gel drying tube 1.4 to form dry aerosol, which is then transported to the premixing tank 1.5; at the same time, the isotope CO2 control module 2 generates carbon-free condensation nuclei through the gas cylinder group 2.1. 13 The CO2 cylinder supplies the marker gas, which is precisely controlled by the mass flow meter assembly 2.3 and mixed with the condensation nuclei in the premixing tank 1.5. The mixed gas is then passed through the heating belt 2.4 for temperature control and then into the multi-point absorption tower 3. Inside the absorption tower, the aerosol grows axially through the packing layer through mass transfer, and particles of different heights are captured by evenly spaced particle sampling points 3.1. The particle monitoring and analysis module 4 uses a micro HEPA filter 4.1 to collect the particles, and the solid phase composition analysis unit 4.2 simultaneously measures the difference in silicon content (indicating agglomeration) of particles at adjacent measurement points. 13 The difference in C isotope abundance (characterizing heterogeneous nucleation) ultimately decouples the contribution of the two mechanisms through the ratio of the difference values.

[0080] Example 2

[0081] The method for quantifying the contribution of heterogeneous nucleation and agglomeration of secondary aerosols in this embodiment includes the following steps:

[0082] S1. Condensation nuclei mixed with isotope-labeled gas:

[0083] The carbon-free monodisperse SiO2 aerosol condensation nuclei are generated by atomization drying through the condensation nucleus control module 1, and the carbon-free monodisperse SiO2 aerosol condensation nuclei are mixed with the isotope CO2 control module 2. 13 The CO2 mixed gas is evenly mixed in the premixing tank to generate simulated smoke aerosol;

[0084] In specific implementation, in S1, the specific steps of generating carbon-free monodisperse SiO2 aerosol condensation nuclei include:

[0085] The SiO2 particle suspension is stirred and dispersed by a magnetic stirring device 1.2 and then atomized, and then dehydrated by a silica gel drying tube 1.4 to form a dry aerosol;

[0086] will contain 13 CO2 mixed gas 13 The volume concentration of CO2 is regulated by a mass flow meter and mixed with the dehydrated SiO2 aerosol in the premixing tank 1.5. The gas mixing temperature is controlled by a heating tape 2.3 wrapped around the pipeline.

[0087] S2. Dynamic aerosol collection at multiple measurement points:

[0088] The aerosol obtained in S1 is passed into the multi-measuring point absorption tower 3 for gas-liquid mass transfer, and aerosol particle information at different heights is synchronously collected through multiple particle sampling points 3.1 arranged at equal intervals along the axial direction of the multi-measuring point absorption tower 3;

[0089] In S2, the particle sampling points of the multi-point absorption tower 3 are evenly spaced along the axial direction of the tower body, and the spacing is 10%-15% of the tower body height;

[0090] During collection, aerosol particles are captured by a micro HEPA filter, and the particle mass concentration and sampling time of each measuring point are recorded.

[0091] S3. Decoupling calculation of agglomeration and nucleation contributions:

[0092] Based on the differences in silicon content and carbon isotope content between adjacent particle sampling points 3.1, the contributions of agglomeration and heterogeneous nucleation to aerosol mass transfer growth were calculated respectively.

[0093] In S3, the specific steps for calculating contribution share include:

[0094] Solid phase composition analysis was used to determine the differences in silicon content and carbon isotope content of particles at adjacent measurement points. The silicon content difference was used to characterize the mass transfer increment caused by agglomeration, while the carbon isotope content difference was used to characterize the mass transfer increment caused by heterogeneous nucleation.

[0095] The sum of the differences in mass transfer increments caused by agglomeration and heterogeneous nucleation was taken as the total mass transfer growth. The agglomeration contribution was calculated by the ratio of the silicon content difference to the total mass transfer growth, and the heterogeneous nucleation contribution was calculated by the ratio of the carbon isotope content difference to the total mass transfer growth.

[0096] In the specific implementation, the monodisperse SiO2 particle generator 1.1 and the atomization drying device of the condensation nucleus control module 1 generate carbon-free condensation nuclei, and the carbon-free condensation nuclei are generated by the isotope CO2 control module 2. 13 The CO2 labeled gas is mixed in the premixing tank 1.5 to form an initial aerosol environment; after the mixed aerosol enters the multi-measuring point absorption tower 3, during the gas-liquid mass transfer process, the SiO2 condensation nuclei agglomerate through physical collision (manifested as the difference in silicon content of particles at adjacent measuring points), and at the same time 13 CO2 reacts with amine solution to produce 13 C-labeled salt products are deposited on the particle surface (manifested as differences in carbon isotope abundances at adjacent measuring points); the particle monitoring and analysis module 4 collects particles from sampling points 3.1 at different heights in the absorption tower through a micro-HEPA filter 4.1, and uses a solid phase composition analysis unit 4.2 to determine the silicon and carbon difference values. Finally, the agglomeration contribution is calculated as the ratio of the silicon difference value to the total of the two, and the heterogeneous nucleation contribution is calculated as the ratio of the carbon difference value, thereby achieving decoupling and quantification of the two mechanisms.

[0097] In specific implementation, the micro-HEPA filter can be connected to the test point. After collecting the particles, the solid phase product detection capital is calibrated according to the ΔSii% (silicon content difference) and ΔCi% (carbon content difference) of the aerosols at adjacent measuring points of the multi-measuring point absorption tower 3. The control share of agglomeration and heterogeneous nucleation on the mass transfer growth of secondary aerosols is obtained according to Eq. 1 and Eq. 2 respectively:

[0098]

[0099] Where α is the weight coefficient of the contribution of silicon difference value calibrated according to the particle specific surface area to agglomeration, and β is the weight coefficient of the contribution of carbon difference value calibrated according to the reaction mass transfer efficiency to heterogeneous nucleation.

[0100] In engineering, assuming that the mass changes of carbon and silicon have equal unit contributions to mass transfer growth, then α = β = 1, and the calculation method for the proportion of the control share of agglomeration and heterogeneous nucleation on secondary aerosol mass transfer growth becomes:

[0101]

[0102] If the mass transferred per unit mass of particles generated by heterogeneous nucleation is not equal to that of agglomeration, then α≠β is given, and the values of α and β can be estimated with the help of the particle size-surface area formula.

[0103]

[0104] Among them A 团聚 A is the unit mass contribution coefficient of agglomeration to mass transfer growth based on the particle specific surface area and collision probability. 非均相核化 is the unit mass contribution coefficient of heterogeneous nucleation to mass transfer growth calibrated based on reaction rate and mass transfer efficiency.

[0105] The above description of the embodiments is intended to facilitate understanding and use of the invention by those skilled in the art. It will be apparent that those skilled in the art can readily make various modifications to these embodiments and apply the general principles described herein to other embodiments without requiring inventive effort. Therefore, the present invention is not limited to the above-described embodiments. Improvements and modifications made by those skilled in the art based on the disclosure of the present invention, without departing from the scope of the present invention, should be within the scope of protection of the present invention.

Claims

1. An aerosol growth mechanism decoupling monitoring system, characterized in that: include: A condensation nucleus control module (1) is used to generate carbon-free monodisperse SiO2 aerosol condensation nuclei; The isotope CO2 control module (2) is connected to the condensation nucleus control module (1) and is used to provide the target control concentration to the premixing tank (1.5). 13 CO2 mixed gas; A multi-measuring point absorption tower (3) is connected to the isotope CO2 control module (2) and is used to carry the aerosol growth process and perform the gas-liquid mass transfer process. The multi-measuring point absorption tower (3) is provided with a plurality of particle sampling points (3.1) along the axial direction on the tower body for capturing the dynamic changes of the aerosol growth process; The particle monitoring and analysis module (4) is connected to each particle sampling point (3.1) through a pipeline. The particle monitoring and analysis module (4) is used to collect and analyze the silicon content difference and carbon isotope content difference of particles at adjacent measurement points. The silicon content difference and carbon isotope content difference are used to generate a decoupling report of the contribution share of the heterogeneous nucleation and agglomeration mechanism.

2. The aerosol growth mechanism decoupling monitoring system according to claim 1, characterized in that: The condensation nucleus control module (1) comprises a monodisperse SiO2 particle generator (1.1), a magnetic stirring device (1.2), an ultrasonic atomizer (1.3), a silica gel drying tube (1.4), and a premixing tank (1.5), which are sequentially connected through pipelines; The monodisperse SiO2 particle generator (1.1) is used to generate a carbon-free monodisperse SiO2 particle suspension with a particle size range of 50-500 nm and a controllable concentration; The magnetic stirring device (1.2) is used to stir and disperse the SiO2 particle suspension to prevent the particles from agglomerating; The silica gel drying tube (1.4) is used to dehydrate the atomized wet particles to generate dry SiO2 aerosol condensation nuclei; The premixing tank (1.5) has an output end connected to the bottom air inlet of the multi-point absorption tower (3) for mixing the dry SiO2 aerosol condensation nuclei with the isotope 13 The CO2 mixed gas is evenly mixed to form a simulated flue gas aerosol environment.

3. The aerosol growth mechanism decoupling monitoring system according to claim 2, characterized in that: The isotope CO2 control module (2) comprises a gas cylinder group (2.1), the gas cylinder group (2.1) is connected to the premixing tank (1.5) via a gas delivery pipeline, and the gas delivery pipeline is matched with a mass flow meter group (2.2).

4. The aerosol growth mechanism decoupling monitoring system according to claim 3, characterized in that: The gas cylinder set (2.1) includes 13 CO2 gas cylinder, N2 gas cylinder, O2 gas cylinder, and 13 The CO2 gas cylinder, the N2 gas cylinder, and the O2 gas cylinder are respectively connected to the premixing tank (1.5) through gas delivery pipelines, and each of the gas delivery pipelines is provided with a mass flow meter; The isotope CO2 control module (2) further comprises a heating belt (2.3), which is wound on the pipeline between the silica gel drying tube (1.4) and the premixing tank (1.5), and on the pipeline between the premixing tank (1.5) and the multi-measuring point absorption tower (3).

5. The aerosol growth mechanism decoupling monitoring system according to claim 1, characterized in that: The particle sampling points (3.1) in the multi-point absorption tower (3) are evenly spaced along the axial direction of the tower body, with the spacing being 10%-15% of the tower height; The top of the multi-measurement point absorption tower (3) is provided with an organic amine absorbent liquid input port and a purified gas discharge port; The bottom of the multi-measuring point absorption tower (3) is provided with a simulated flue gas injection port and a rich amine liquid discharge port.

6. The aerosol growth mechanism decoupling monitoring system according to claim 1, characterized in that: The particle monitoring and analysis module (4) comprises a micro HEPA filter array (4.1) and a solid phase component analysis unit (4.2); The micro HEPA filter array (4.1) includes a plurality of micro HEPA filters, each micro HEPA filter is connected to a particle sampling point (3.1) via a pipeline, and each micro HEPA filter is connected to a solid phase component analysis unit (4.2); The solid phase component analysis unit (4.2) includes one or more of an inductively coupled plasma emission spectrometer, an isotope ratio mass spectrometer, and a scanning electron microscope-energy dispersive spectrometer. The solid phase component analysis unit (4.2) is used to simultaneously measure the silicon content, carbon isotope abundance, particle size distribution, and surface morphology of the particles.

7. A method for quantifying the contribution of heterogeneous nucleation and agglomeration of secondary aerosols, characterized in that: The following steps are involved: S1. Condensation nuclei mixed with isotope-labeled gas: The carbon-free monodisperse SiO2 aerosol condensation nuclei are generated by atomization drying through the condensation nucleus control module (1), and the carbon-free monodisperse SiO2 aerosol condensation nuclei are mixed with the isotope CO2 control module (2) to form a carbon-free monodisperse SiO2 aerosol condensation nuclei. 13 The CO2 mixed gas is evenly mixed in the premixing tank to generate simulated smoke aerosol; S2. Dynamic aerosol collection at multiple measurement points: The aerosol obtained in S1 is passed into a multi-measurement point absorption tower (3) for gas-liquid mass transfer, and aerosol particle information at different heights is synchronously collected through a plurality of particle sampling points (3.1) arranged at equal intervals along the axial direction of the multi-measurement point absorption tower (3); S3. Decoupling calculation of agglomeration and nucleation contributions: Based on the differences in silicon content and carbon isotope content between adjacent particle sampling points (3.1), the contributions of agglomeration and heterogeneous nucleation to aerosol mass transfer growth are calculated respectively.

8. The method for quantifying the contribution of heterogeneous nucleation and agglomeration of secondary aerosols according to claim 7, characterized in that: In S1, the specific steps of generating carbon-free monodisperse SiO2 aerosol condensation nuclei include: The SiO2 particle suspension is stirred and dispersed by a magnetic stirring device (1.2) and then atomized, and then dehydrated by a silica gel drying tube (1.4) to form a dry aerosol; will contain 13 CO2 mixed gas 13 The volume concentration of CO2 is regulated by a mass flow meter and mixed with the dehydrated SiO2 aerosol in a premixing tank (1.5). The gas mixing temperature is controlled by a heating tape (2.3) wrapped around the pipeline.

9. The method for quantifying the contribution of heterogeneous nucleation and agglomeration of secondary aerosols according to claim 7, characterized in that: In S2, the particle sampling points of the multi-point absorption tower (3) are evenly spaced along the axial direction of the tower body, and the spacing is 10%-15% of the tower body height; During collection, aerosol particles are captured by a micro HEPA filter, and the particle mass concentration and sampling time of each measuring point are recorded.

10. The method for quantifying the contribution of heterogeneous nucleation and agglomeration of secondary aerosols according to claim 7, characterized in that: In S3, the specific steps for calculating contribution share include: Solid phase composition analysis was used to determine the differences in silicon content and carbon isotope content of particles at adjacent measurement points. The silicon content difference was used to characterize the mass transfer increment caused by agglomeration, while the carbon isotope content difference was used to characterize the mass transfer increment caused by heterogeneous nucleation. The sum of the differences in mass transfer increments caused by agglomeration and heterogeneous nucleation was taken as the total mass transfer growth. The agglomeration contribution was calculated by the ratio of the silicon content difference to the total mass transfer growth, and the heterogeneous nucleation contribution was calculated by the ratio of the carbon isotope content difference to the total mass transfer growth.

Images