CN110501265B - Method and system for measuring wet clearance coefficient of atmospheric particulate matter under cloud - Google Patents

Method and system for measuring wet clearance coefficient of atmospheric particulate matter under cloud Download PDF

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CN110501265B
CN110501265B CN201910911481.4A CN201910911481A CN110501265B CN 110501265 B CN110501265 B CN 110501265B CN 201910911481 A CN201910911481 A CN 201910911481A CN 110501265 B CN110501265 B CN 110501265B
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atmosphere
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CN110501265A (en
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葛宝珠
徐丹卉
刘冉冉
王自发
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Institute of Atmospheric Physics of CAS
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    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N1/00Sampling; Preparing specimens for investigation
    • G01N1/28Preparing specimens for investigation including physical details of (bio-)chemical methods covered elsewhere, e.g. G01N33/50, C12Q
    • G01N1/34Purifying; Cleaning
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N15/00Investigating characteristics of particles; Investigating permeability, pore-volume, or surface-area of porous materials
    • G01N15/02Investigating particle size or size distribution
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N15/00Investigating characteristics of particles; Investigating permeability, pore-volume, or surface-area of porous materials
    • G01N15/06Investigating concentration of particle suspensions
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N15/00Investigating characteristics of particles; Investigating permeability, pore-volume, or surface-area of porous materials
    • G01N15/10Investigating individual particles
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N30/00Investigating or analysing materials by separation into components using adsorption, absorption or similar phenomena or using ion-exchange, e.g. chromatography or field flow fractionation
    • G01N30/02Column chromatography

Abstract

The invention discloses a method and a system for measuring an atmospheric particulate matter under-cloud wet removal coefficient, which comprises the following steps of sampling rainwater in a segmented manner to obtain a rainwater sample; pretreating a rainwater sample, filtering insoluble components in the rainwater sample, and refrigerating and storing the filtered rainwater sample; detecting aerosol components in the filtered rainwater sample and the quality of black carbon in single aerosol particles; collecting an atmospheric sample in the same period as each rainwater sample, and detecting aerosol components and number concentration in the collected atmospheric sample and the quality of black carbon in single aerosol particles; and acquiring the rainfall intensity and the average cloud bottom height of the rainwater sample in the same period, and calculating the wet removal coefficient by combining the detected data in the rainwater sample and the atmospheric sample in the same period. The advantages are that: the invention realizes the synchronous measurement of the precipitation and the content of the aerosol in the atmosphere, obtains the direct measurement of the wet clearance coefficient of the particles under the cloud, and realizes the innovation of the measurement of the wet clearance coefficient of the single-field precipitation in different time periods.

Description

Method and system for measuring wet clearance coefficient of atmospheric particulate matter under cloud
Technical Field
The invention relates to the technical field of environmental science, in particular to a method and a system for measuring a wet clearance coefficient of atmospheric particulates under cloud.
Background
With the rapid development of economy, the accelerated urbanization process and the remarkable increase of the motor vehicle keeping amount in China, the emission of SO2 and NOx in a large number of industrial processes is the most fundamental cause of regional atmospheric fine particulate matter (PM2.5) pollution in China at present. A great deal of research shows that the enhancement of atmospheric pollutants caused by human emission increasingly affects the production and life of human beings, which not only affects the global land and marine ecosystems, changes the soil and water chemical circulation, but also increases the human health risk and reduces the biodiversity. Wet settling of atmospheric particulates is one of the important pathways by which aerosols are removed from the atmosphere. From the results of a number of global chemical transport models, sulfur and nitrogen (the important inorganic aerosol components of particulate matter) predominate in most areas of china by wet sedimentation. The wet clearance coefficient of the aerosol is a key parameter for accurately simulating the wet settlement flux of the aerosol in a numerical mode.
In the theoretical calculation of wet clearance coefficients, the estimation method is only applicable to small particles with a size less than 100 nm particle size fraction (dominated by brownian motion) and large particles with a size fraction greater than 20 μm (dominated by directional interception and collision cleaning), and the wet clearance coefficient for PM2.5 aerosol particles with a size fraction of 2.5 μm remains to be studied (presence of "Greenfield gap"). In the mode estimation, the estimation of the wet clearance coefficient by the current mode mostly comes from the basis of the existing theoretical research and is simplified into the relation between the merging coefficient and the precipitation intensity. The model therefore has a significant underestimation of the wet clearance coefficient estimate, which also results in some underestimation of the amount of wet settling. In external field observation, no mature detection device is available on the market at present. Previous studies have estimated the wet clearance coefficient by combining the monthly average scale aerosol constituent concentrations with precipitation constituent concentrations. However, the estimation method cannot achieve high time precision resolution and cannot be used for single-field precipitation cases.
Precipitation sample analysis is usually composed of two parts, namely field collection and laboratory analysis. The rainwater sample collected by the outfield is manually pretreated and stored in an environment of about zero degrees, so that a time difference exists when the outdoor field collects laboratory analysis, the change of the acidity of the rainwater enables chemical components of the rainwater to change in the time difference, and how to realize the automatic separation technology of the rainwater sample, and the separation pretreatment at the first time after sampling is the key for accurately measuring the content of aerosol in the rainwater.
Disclosure of Invention
The invention aims to provide a method and a system for measuring the wet clearance coefficient of atmospheric particulates under cloud, so as to solve the problems in the prior art.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a method for measuring the wet clearance coefficient under atmospheric particulate cloud comprises the following steps,
s1, performing sectional sampling on the rainwater to obtain a rainwater sample;
s2, preprocessing the rainwater sample, filtering insoluble components in the rainwater sample, and refrigerating and storing the filtered rainwater sample;
s3, detecting aerosol components in the filtered rainwater sample and the quality of black carbon in single aerosol particles;
s4, collecting atmospheric samples in the same period as each rainwater sample, and detecting aerosol components and number concentration in the collected atmospheric samples and the quality of black carbon in single aerosol particles;
and S5, acquiring the rainfall intensity and the average cloud bottom height of the rainwater sample in the same period, and calculating the wet removal coefficient by combining the detected data in the rainwater sample and the atmospheric sample in the same period.
Preferably, the rainwater sample and the atmosphere sample are collected synchronously, and the rainwater sample and the atmosphere sample are detected synchronously.
Preferably, the wet clearance coefficient calculation in step S4 specifically includes two methods, i.e. an off-line calculation method and an on-line calculation method, where the off-line calculation method includes the following steps,
Figure BDA0002214867030000021
Figure BDA0002214867030000022
wherein K is the wet clearance coefficient under certain aerosol cloud, CprecipitationConcentration of aerosol in rain water sample, CaerosolThe concentration of aerosol in an atmospheric sample, P is the precipitation intensity, and h is the average cloud bottom height; (z) is a weight coefficient function of the aerosol concentration vertical distribution under the cloud base height; c'aerosol(Z) is the aerosol concentration in Z height, C'aerosol(0) For aerosol concentration on the ground, h' (z) is the thickness layer of the aerosol vertical distribution.
Preferably, the on-line calculation process is as follows,
Figure BDA0002214867030000031
wherein, K (d)p) Is a particle diameter of dpCoefficient of wet removal under cloud, N, of aerosol particles0(dp) And N1(dp) Respectively before precipitation0Time and after precipitation t1When the particle diameter is dpThe number concentration of aerosol particles of (a).
The invention also aims to provide a system for measuring the wet clearance coefficient under the atmospheric particulate cloud, which is used for realizing any one of the measuring methods, comprising,
the rainwater sectional sampling device is used for realizing sectional sampling of rainwater and acquiring rainwater samples under the conditions of the same rainfall intensity in different rainfall periods, different rainfall intensities in different rainfall periods and different rainfall intensities in the same rainfall period;
the rainwater separation pretreatment device is used for pretreating a rainwater sample, filtering insoluble components in the rainwater sample, and refrigerating and storing the filtered rainwater sample;
the atmosphere collection device is used for collecting the atmosphere sample in the same period as the rainwater sample;
the basic data acquisition device is used for acquiring the rainfall intensity and the average cloud bottom height of the rainwater sample in the same period;
the rainwater detection device is used for detecting aerosol components in the pretreated rainwater sample and the quality of black carbon in single aerosol particles;
the atmosphere detection device is used for detecting aerosol components and number concentration in an atmosphere sample and the quality of black carbon in single aerosol particles;
the synchronous measurement control module is used for controlling the synchronous operation of the rainwater subsection sampling device, the atmosphere acquisition device and the basic data acquisition device and also controlling the synchronous operation of the rainwater detection device and the atmosphere detection device;
and the wet clearance coefficient estimation module is used for calculating the wet clearance coefficient according to the data detected by the atmosphere detection device and the synchronous measurement control module.
Preferably, the measuring system further comprises an atmosphere drying device, and the atmosphere drying device is used for drying the atmosphere sample in the humid environment to obtain the atmosphere sample which can be directly used by the atmosphere detecting device.
Preferably, the rainwater detection device comprises a liquid chromatograph and a first single-particle black carbon instrument; the atmosphere detection device comprises an aerosol particle size spectrometer, a second single-particle black carbon instrument and an aerosol mass spectrometer.
Preferably, the rainwater separation pretreatment device comprises an injector, a first connecting pipe, a second connecting pipe, a filter membrane, a rainwater collector and a collecting bottle, wherein two ends of the first connecting pipe are respectively connected with the injector and the collecting bottle, two ends of the second connecting pipe are respectively connected with the first connecting pipe and the rainwater collector, the filter membrane is arranged on the first connecting pipe, and a connecting point of the second connecting pipe and the first connecting pipe is positioned at the upstream of the filter membrane in the direction from the injector to the collecting bottle; the rainwater collector is connected with the rainwater sectional sampling device.
Preferably, a first one-way valve and a second one-way valve are respectively arranged on the first connecting pipe and the second connecting pipe, and the first one-way valve is located between the connecting point of the second connecting pipe and the first connecting pipe and the filter membrane.
Preferably, the rainwater collector is hollow, the upper end and the lower end of the rainwater collector are arranged in an open mode, a flow channel with gradually narrowed width is formed from the upper end to the lower end of the rainwater collector, the upper end of the rainwater collector is connected with the rainwater section sampling device, and the lower end of the rainwater collector is connected with one end of the second connecting pipe; the other end of the second connecting pipe is connected to the first connecting pipe.
The invention has the beneficial effects that: 1. the invention realizes the synchronous measurement of precipitation and the content of aerosol in the atmosphere, and obtains the direct measurement of the wet clearance coefficient of the particles under the cloud. 2. The method can ensure the simultaneity of the collection and detection of the rainwater sample and the atmospheric sample, and greatly reduce the estimation error of the wet clearance coefficient caused by the non-simultaneous collection and detection. 3. The rainwater separation pretreatment device can be used for pretreating the collected rainwater sample, so that the change of the content of soluble components caused by the influence of rainwater acidity on the rainwater sample is avoided. 4. The atmosphere drying device can dry the atmosphere sample in a humid environment, and avoids component content change in the atmosphere sample caused by overlarge humidity. 5. The invention realizes the synchronous measurement of the contents of rainwater and aerosol in the atmosphere by the development of a whole set of equipment for the first time, and makes the calculation of wet clearance coefficient estimation of single-field rainfall in different time periods possible. 6. Compared with the traditional method for obtaining a single coefficient by the whole precipitation, the method realizes the innovation of supporting the measurement of the wet clearance coefficient of the single precipitation in different time periods.
Drawings
FIG. 1 is a schematic flow chart of a measurement method in an embodiment of the present invention;
FIG. 2 is a schematic diagram of a measurement system according to an embodiment of the present invention;
FIG. 3 is a schematic structural diagram of a rainwater separation pretreatment device in an embodiment of the invention.
In the figure: 1. an injector; 11. an injection pump; 2. a first connecting pipe; 3. a second connecting pipe; 4. a first check valve; 5. a second one-way valve; 6. filtering the membrane; 7. a rainwater collector; 8. and (6) collecting the bottle.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail below with reference to the accompanying drawings. It should be understood that the detailed description and specific examples, while indicating the invention, are intended for purposes of illustration only and are not intended to limit the scope of the invention.
Example one
As shown in fig. 1, the present embodiment provides a method for measuring a wet clearance coefficient under an atmospheric particulate cloud, comprising the following steps,
s1, performing sectional sampling on the rainwater to obtain a rainwater sample;
s2, preprocessing the rainwater sample, filtering insoluble components in the rainwater sample, and refrigerating and storing the filtered rainwater sample;
s3, detecting aerosol components in the filtered rainwater sample and the quality of black carbon in single aerosol particles;
s4, collecting atmospheric samples in the same period as each rainwater sample, and detecting aerosol components and number concentration in the collected atmospheric samples and the quality of black carbon in single aerosol particles;
and S5, acquiring the rainfall intensity and the average cloud bottom height of the rainwater sample in the same period, and calculating the wet removal coefficient by combining the detected data in the rainwater sample and the atmospheric sample in the same period.
In this embodiment, the rainwater sample and the atmospheric sample are collected synchronously, and the detection of the rainwater sample and the atmospheric sample is performed synchronously.
In this embodiment, the wet clearance coefficient calculation in step S4 specifically includes two methods, i.e., an off-line calculation method and an on-line calculation method, where the off-line calculation method includes the following steps,
Figure BDA0002214867030000051
Figure BDA0002214867030000052
wherein K is the wet clearance coefficient under certain aerosol cloud, CprecipitationConcentration of aerosol in rain water sample, CaerosolThe concentration of aerosol in an atmospheric sample, P is the precipitation intensity, and h is the average cloud bottom height; (z) is a weight coefficient function of the aerosol concentration vertical distribution under the cloud base height; c'aerosol(Z) is the aerosol concentration in Z height, C'aerosol(0) For aerosol concentration on the ground, h' (z) is the thickness layer of the aerosol vertical distribution.
Preferably, the on-line calculation process is as follows,
Figure BDA0002214867030000061
in this example, K (d)p) Is a particle diameter of dpCoefficient of wet removal under cloud, N, of aerosol particles0(dp) And N1(dp) Respectively before precipitation0Time and after precipitation t1When the particle diameter is dpThe number concentration of aerosol particles of (a).
Example two
As shown in fig. 2 to 3, the present embodiment provides an atmospheric particulate matter cloud wet clearance coefficient measuring system, which is used for implementing the above measuring method, including,
the rainwater sectional sampling device is used for realizing sectional sampling of rainwater and acquiring rainwater samples under the conditions of the same rainfall intensity in different rainfall periods, different rainfall intensities in different rainfall periods and different rainfall intensities in the same rainfall period;
the rainwater separation pretreatment device is used for pretreating a rainwater sample, filtering insoluble components in the rainwater sample, and refrigerating and storing the filtered rainwater sample;
the atmosphere collection device is used for collecting the atmosphere sample in the same period as the rainwater sample;
the basic data acquisition device is used for acquiring the rainfall intensity and the average cloud bottom height of the rainwater sample in the same period;
the rainwater detection device is used for detecting aerosol components in the pretreated rainwater sample and the quality of black carbon in single aerosol particles;
the atmosphere detection device is used for detecting aerosol components and number concentration in an atmosphere sample and the quality of black carbon in single aerosol particles;
the synchronous measurement control module is used for controlling the synchronous operation of the rainwater subsection sampling device, the atmosphere acquisition device and the basic data acquisition device and also controlling the synchronous operation of the rainwater detection device and the atmosphere detection device;
and the wet clearance coefficient estimation module is used for calculating the wet clearance coefficient according to the data detected by the atmosphere detection device and the synchronous measurement control module.
In this embodiment, but rainwater segmentation sampling device automatically regulated sampling volume size mainly adopts telescopic 2 grades of rainwater to accept the tray, accept the tray and pass through the automatic sampling area that enlarges or dwindles of the size of rainwater collection volume, and then adjust sampling volume size and sampling frequency. The mode that adopts the spiral formula to switch rainwater collection pipeline realizes the segmentation sampling of rainwater to obtain the rainwater sample of precipitation different periods (preceding, middle, later stage), distinguish in the cloud and clear away the process under the cloud, still possess the ability of collecting and analyzing the rainwater sample of single-field precipitation different periods, different rain strong conditions. Aiming at different periods of single-field precipitation, the technology of automatically adjusting the size of the bearing tray is adopted, fine grading sampling is realized, and comprehensive knowledge of the precipitation process is improved.
In this embodiment, the rainwater separation pretreatment device includes a syringe 1, a first connection pipe 2, a second connection pipe 3, a filter membrane 6, a rainwater collector 7 and a collection bottle 8, two ends of the first connection pipe 2 are respectively connected with the syringe 1 and the collection bottle 8, two ends of the second connection pipe 3 are respectively connected with the first connection pipe 2 and the rainwater collector, the filter membrane 6 is disposed on the first connection pipe 2, and a connection point of the second connection pipe 3 and the first connection pipe 2 is located at an upstream of the filter membrane 6 in a direction from the syringe 1 to the collection bottle 8; the rainwater collector 7 is connected with the rainwater subsection sampling device.
In this embodiment, the first connecting pipe 2 and the second connecting pipe 3 are respectively provided with a first check valve 4 and a second check valve 5, and the first check valve 4 is located between a connection point of the second connecting pipe 3 and the first connecting pipe 2 and the filter membrane 6.
In this embodiment, the rainwater collector 7 is hollow and has openings at the upper and lower ends, and the rainwater collector 7 forms a flow channel with gradually narrowed width from the upper end to the lower end thereof, the upper end of the rainwater collector 7 is connected with the rainwater section sampling device, and the lower end of the rainwater collector 7 is connected with one end of the second connecting pipe 3; the other end of the second connection pipe 3 is connected to the first connection pipe 2.
In this embodiment, the use process of the rainwater pretreatment device is as follows: rainwater collected by the rainwater sectional sampling device enters the rainwater collector 7 through the upper end of the rainwater collector 7, when the rainwater collector 7 collects rainwater, the injector 1 is pushed by the injection pump 11 to suck a rainwater sample into the injector 1 through the second one-way valve 5, the suction speed is consistent with the rainwater collection speed or is slightly slow so as to avoid air suction, and the first one-way valve 4 is not conducted at the moment. When the sample in the syringe 1 reaches a specific volume, the syringe pump 11 is pushed reversely, the sample is pushed to the filter membrane 6 through the first one-way valve 4, the solid insoluble substances are blocked and stored by the filter membrane 6, meanwhile, the liquid sample enters the collection bottle 8, and at the moment, the second one-way valve 5 is not conducted. After the samples in the injector 1 are completely filtered, the mechanical arm is used for disconnecting the group of filter membranes 6 and the collection bottles 8 from the outlet of the first one-way valve 4, the automatic converter moves the filter membranes away, the next group of clean filter membranes 6 and the empty collection bottles 8 are moved to the position, the mechanical arm is used for connecting the filter membranes with the first one-way valve 4, and the next section of rainwater sample is continuously filtered.
In the embodiment, after rainfall or sampling is finished, the filter membrane 6 is collected, dried and weighed, and the mass difference before and after sampling is the mass of insoluble substances in the rainwater; the filtered rainwater sample is collected into a 100ml Teflon collecting bottle 8 to be stored in a refrigerating way, the rainwater sample is stored as far as possible without being influenced by off-line analysis and collection time difference, and then the water sample in the collecting bottle 8 is analyzed by ion chromatography and the like, so that the quality of total soluble substances and main components in rainwater, such as sulfate, nitrate and the like, can be obtained.
In this embodiment, synchronous measurement control module discerns the precipitation signal when taking place the precipitation, reads rainwater segmentation sampling device and atmosphere collection system's time rapidly to the record is rainwater collection start time, realizes the synchronization of rainwater collection and the time of atmospheric sample collection. When precipitation occurs, precipitation signals are identified, the gas circuit measured by the concentration or mass concentration instrument is rapidly switched, and the original normal atmosphere is switched into the gas circuit pretreated by the system. The atmosphere collection device of the system is synchronous with the rainwater sectional sampling device, collects the atmosphere samples in the same time period and transmits the atmosphere samples to the atmosphere detection device for analyzing the components, the number concentration and other elements of the particulate matters.
In this embodiment, the measurement system further includes an atmospheric drying device, and the atmospheric drying device is used for drying an atmospheric sample in a humid environment to obtain the atmospheric sample that can be directly used by the atmospheric detection device. The atmospheric drying device carries out drying process to atmospheric sample under the humid environment, avoids causing number concentration or mass concentration instrument detection error or data to lack because of humidity is too big, considers to receive the great influence of steam. The atmospheric drying module is connected with the atmospheric detection device, so that the atmospheric detection device can obtain an atmospheric sample which can be directly measured, and meanwhile, the working efficiency of the drying device in different precipitation periods is calculated, and the optimal physical control parameters are obtained. The drying device is adjusted to an optimum drying state.
In this embodiment, the measuring system collects rainwater in different periods of time in a single field of precipitation and stores the rainwater in the filter membrane 6 or the collecting bottle 8 according to the solubility of the rainwater. Meanwhile, the synchronous control module and the atmosphere drying module are utilized to realize the consistency of time and frequency with the rainwater detection device and the atmosphere detection device, and finally, the wet clearance coefficient is calculated in an online mode and an offline mode, so that the measurement of the wet clearance coefficient of the particles in different periods of single-field rainfall is obtained.
In this embodiment, the calculation of the aerosol wet removal coefficient requires that the aerosol content in rainwater and atmosphere be measured simultaneously, so the simultaneous measurement of the rainwater sample and the atmosphere sample is crucial, and the realization of the synchronous control of sampling and measurement of the rainwater sample and the atmosphere sample mainly depends on the synchronous measurement control module to control the rainwater sectional sampling device and the atmosphere collection device. The atmosphere acquisition device comprises three air acquisition bags, three air extraction pumps and an electromagnetic valve. When the rainwater subsection sampling device starts to collect a 1 st section rainwater sample, namely the injector 1 in the rainwater automatic separation preassembly starts to suck rainwater, the air suction pump A receives the same signal and starts to operate, and the atmospheric sample is sucked into the air suction bag A until the injector 1 stops sucking. At the moment, the electromagnetic valve switches the sample injection gas circuit of the atmosphere detection device to the outlet end of the gas production bag A, and the 1 st section of air sample is analyzed. Meanwhile, the air extracting bag B is inflated by the air extracting pump B, and the 2 nd section air sample is acquired. When the 2 nd section of sample collection stops, the solenoid valve switches the appearance gas circuit of atmosphere detection device to the exit end of gas production bag B, carries out the analysis of 2 nd section of air sample. Meanwhile, the air pump A pumps the residual air sample in the air collecting bag A away for next sampling, the air pump C starts to inflate the air collecting bag C, the 3 rd section of air sample is collected, and the process is repeated. At the same time, one sampling bag is collecting the sample, one is providing the sample to an atmosphere detection device or the like, and one is preparing for evacuation for the next sampling.
In the embodiment, the rainwater detection device comprises a liquid chromatograph and a first single-particle black carbon instrument SP 2; the atmospheric detection device comprises an aerosol particle size spectrometer SMPS, a second single-particle blackcarbon instrument SP2 and an aerosol mass spectrometer AMS. The liquid chromatograph and the first single-particle black carbon instrument SP2 are used for detecting aerosol components in a rainwater sample and the mass of black carbon in single aerosol particles, and the aerosol particle size spectrometer SMPS, the second single-particle black carbon instrument SP2 and the aerosol mass spectrometer AMS are used for detecting aerosol components, number concentration and the mass of black carbon in single aerosol particles in an atmospheric sample.
By adopting the technical scheme disclosed by the invention, the following beneficial effects are obtained:
the invention provides a method and a system for measuring the wet clearance coefficient of atmospheric particulates, which realize the synchronous measurement of precipitation and aerosol content in the atmosphere and obtain the direct measurement of the wet clearance coefficient of the particulates under cloud; the method can ensure the simultaneity of the collection and detection of the rainwater sample and the atmospheric sample, and greatly reduce the estimation error of the wet clearance coefficient caused by the non-simultaneous collection and detection; the rainwater separation pretreatment device can be used for pretreating the collected rainwater sample, so that the change of the content of soluble components caused by the influence of rainwater acidity on the rainwater sample is avoided; the atmosphere drying device can dry the atmosphere sample in a humid environment, so that the component content change in the atmosphere sample caused by overlarge humidity is avoided; the invention realizes the synchronous measurement of the contents of rainwater and aerosol in the atmosphere by the development of a whole set of equipment for the first time, and makes the calculation of wet clearance coefficient estimation of single-field rainfall in different time periods possible; compared with the traditional method for obtaining a single coefficient by the whole precipitation, the method realizes the innovation of supporting the measurement of the wet clearance coefficient of the single precipitation in different time periods.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and improvements can be made without departing from the principle of the present invention, and such modifications and improvements should also be considered within the scope of the present invention.

Claims (8)

1. A method for measuring the wet clearance coefficient of atmospheric particulates under cloud is characterized by comprising the following steps: comprises the following steps of (a) carrying out,
s1, performing sectional sampling on the rainwater to obtain a rainwater sample;
s2, preprocessing the rainwater sample, filtering insoluble components in the rainwater sample, and refrigerating and storing the filtered rainwater sample;
s3, detecting aerosol components in the filtered rainwater sample and the quality of black carbon in single aerosol particles;
s4, collecting atmospheric samples in the same period as each rainwater sample, and detecting aerosol components and number concentration in the collected atmospheric samples and the quality of black carbon in single aerosol particles;
s5, acquiring rainfall intensity and average cloud bottom height of the rainwater sample in the same period, and calculating a wet clearance coefficient by combining the detected data in the rainwater sample and the atmospheric sample in the same period;
the wet clearance coefficient calculation in step S5 specifically includes two methods, i.e., an off-line calculation method and an on-line calculation method, where the off-line calculation method includes the following steps,
Figure FDA0002404102220000011
Figure FDA0002404102220000012
wherein K is the wet clearance coefficient under certain aerosol cloud, CprecipitationConcentration of aerosol in rain water sample, CaerosolThe concentration of aerosol in an atmospheric sample, P is the precipitation intensity, and h is the average cloud bottom height; (z) is a weight coefficient function of the aerosol concentration vertical distribution under the cloud base height; c'aerosol(Z) is the aerosol concentration in Z height, C'aerosol(0) Is the aerosol concentration on the ground, h' (z) is the thickness layer of the aerosol vertical distribution;
the on-line calculation process is as follows,
Figure FDA0002404102220000013
wherein, K (d)p) Is a particle diameter of dpCoefficient of wet removal under cloud, N, of aerosol particles0(dp) And N1(dp) Respectively before precipitation0Time and after precipitation t1When the particle diameter is dpThe number concentration of aerosol particles of (a).
2. The method of measuring the atmospheric particulate matter cloud wet clearance coefficient of claim 1, wherein: the rainwater sample and the atmospheric sample are collected synchronously, and the rainwater sample and the atmospheric sample are detected synchronously.
3. An atmospheric particulate matter cloud wet clearance coefficient measurement system for implementing the measurement method of claim 1 or 2, characterized in that: comprises the steps of (a) preparing a mixture of a plurality of raw materials,
the rainwater sectional sampling device is used for realizing sectional sampling of rainwater and acquiring rainwater samples under the conditions of the same rainfall intensity in different rainfall periods, different rainfall intensities in different rainfall periods and different rainfall intensities in the same rainfall period;
the rainwater separation pretreatment device is used for pretreating a rainwater sample, filtering insoluble components in the rainwater sample, and refrigerating and storing the filtered rainwater sample;
the atmosphere collection device is used for collecting the atmosphere sample in the same period as the rainwater sample;
the basic data acquisition device is used for acquiring the rainfall intensity and the average cloud bottom height of the rainwater sample in the same period;
the rainwater detection device is used for detecting aerosol components in the pretreated rainwater sample and the quality of black carbon in single aerosol particles;
the atmosphere detection device is used for detecting aerosol components and number concentration in an atmosphere sample and the quality of black carbon in single aerosol particles;
the synchronous measurement control module is used for controlling the synchronous operation of the rainwater subsection sampling device, the atmosphere acquisition device and the basic data acquisition device and also controlling the synchronous operation of the rainwater detection device and the atmosphere detection device;
and the wet clearance coefficient estimation module is used for calculating the wet clearance coefficient according to the data acquired or detected by the atmosphere detection device, the rainwater detection device and the basic data acquisition device.
4. The atmospheric particulate matter cloud wet clearance coefficient measurement system of claim 3, wherein: the measuring system further comprises an atmosphere drying device, and the atmosphere drying device is used for drying the atmosphere sample in the humid environment so as to obtain the atmosphere sample which can be directly used by the atmosphere detecting device.
5. The atmospheric particulate matter cloud wet clearance coefficient measurement system of claim 3, wherein: the rainwater detection device comprises a liquid chromatograph and a first single-particle black carbon instrument; the atmosphere detection device comprises an aerosol particle size spectrometer, a second single-particle black carbon instrument and an aerosol mass spectrometer.
6. The atmospheric particulate matter cloud wet clearance coefficient measurement system of claim 3, wherein: the rainwater separation pretreatment device comprises an injector, a first connecting pipe, a second connecting pipe, a filter membrane, a rainwater collector and a collecting bottle, wherein two ends of the first connecting pipe are respectively connected with the injector and the collecting bottle, two ends of the second connecting pipe are respectively connected with the first connecting pipe and the rainwater collector, the filter membrane is arranged on the first connecting pipe, and a connecting point of the second connecting pipe and the first connecting pipe is positioned at the upstream of the filter membrane in the direction from the injector to the collecting bottle; the rainwater collector is connected with the rainwater sectional sampling device.
7. The atmospheric particulate matter cloud wet clearance coefficient measurement system of claim 6, wherein: and the first connecting pipe and the second connecting pipe are respectively provided with a first one-way valve and a second one-way valve, and the first one-way valve is positioned between the connecting point of the second connecting pipe and the first connecting pipe and the filter membrane.
8. The atmospheric particulate matter cloud wet clearance coefficient measurement system of claim 6, wherein: the rainwater collector is hollow, the upper end and the lower end of the rainwater collector are arranged in an open mode, a flow channel with the width gradually narrowed is formed from the upper end to the lower end of the rainwater collector, the upper end of the rainwater collector is connected with the rainwater section sampling device, and the lower end of the rainwater collector is connected with one end of the second connecting pipe; the other end of the second connecting pipe is connected to the first connecting pipe.
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