CN111063399A - Method, medium and equipment for applying stable isotope mixture model to contribution rate of Pb source - Google Patents
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Abstract
The invention belongs to the technical field of pollution source identification and analysis, and discloses a method, a medium and equipment for applying a stable isotope mixing model to the contribution rate of Pb sources. The method provided by the invention utilizes the stable isotope composition of the lead in the near-shore water body sediment, can distinguish and analyze the pollution source of the lead, has important scientific significance for knowing the behavior characteristics, the source and the lodging of the lead in the environment, is also beneficial to environmental management, and scientifically guides the emission reduction of the lead.
Description
Technical Field
The invention belongs to the technical field of pollution source identification, and particularly relates to an application method of a stable isotope mixture model in quantification of Pb source contribution rate, a storage medium and equipment.
Background
Lead is a common heavy metal pollutant in the environment, and is generally generated by human activities such as ore mining and smelting, lead storage batteries, ammunition, pesticides, pigments, electronic wastes and the like and discharged into the environment such as soil, water and the like. Lead has obvious harm to human body, and can damage the brain and nervous system of human body, influence the intelligence development of children, and cause abnormal behaviors. Lead has a long residence time in the environment and is difficult to decompose, and lead and its compounds are listed as priority control chemicals. The source of lead in the environment and the migration and transformation path thereof are identified, which is important for understanding the behavior characteristics of lead in the environment and environmental management.
The ratio of the stable isotope of lead is only relevant to the source mining area of lead, but is not relevant to the biogeochemical process in which the stable isotope of lead participates, so that the stable isotope of lead is a reliable index for distinguishing the pollution source of lead in the environment. When the lead pollution source is identified by using the lead stable isotope, the contribution rate of each source to the lead in the environment can be calculated by using a binary or ternary linear mixed model of the isotope in the past research. However, the linear model can only calculate the contribution rate of at most three end members. However, in practical situations, lead often has multiple complex sources, such as various sources of coal combustion, gasoline combustion emission, mining and metal smelting, building dust and the like, and the traditional linear model cannot meet the requirements for the calculation of the contribution rate of the various sources.
In summary, the problems of the prior art are as follows: the contribution rates of at most three end members can only be calculated when the lead stable isotope is used for pollution source identification at present, and the traditional linear model can not meet the requirements.
The difficulty of solving the technical problems is as follows: the ratio of two nonlinearly related Pb-stable isotopes (B) is commonly used in the environmental field207Pb/206Pb and208Pb/206pb) to calculate the contribution rate of Pb pollution sources, and according to the mass conservation law, the contribution rate of at most three end members can be quantified according to a linear mixed model. If the contribution ratios of more than three end-members are calculated, an iterative and bayesian probabilistic statistics based calculation model needs to be applied to calculate the estimate of the contribution ratio. A stable isotope mixture model simmer can implement this calculation process.
The significance of solving the technical problems is as follows: the method has the advantages that Pb in the water body environment has various pollution sources and natural sources, contribution rates of lead from various sources in the environment can be quantitatively estimated, the method has important significance for scientifically recognizing the source and destination of the Pb in the environment, the process and flux of pollution emission and the like, and meanwhile, the method is beneficial to environmental management, scientifically formulating the emission capacity of the lead and guiding the emission reduction work of the lead.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides an application method of a stable isotope mixture model in the quantification of the contribution rate of a Pb source.
In order to achieve the purpose, the invention adopts the technical scheme that: an application method of stable isotope mixture model in quantifying Pb source contribution rate, which is used for measuring the ratio of Pb stable isotope in water area sediment (A)207Pb/206Pb,208Pb/206Pb and206Pb/204pb), determining the Pb isotope ratio of natural lithogenetic sources according to the Pb isotope ratio in deep sediments, and applying a stable isotope mixing model simmer to estimate the contribution rate of various Pb sources in a water area according to the Pb stable isotope ratio in the sediments, the Pb isotope value of the natural source and the Pb isotope ratio data of artificial sources.
Further, the method further comprises:
step one, measuring the ratio of Pb stable isotope in the sediment of the water area by using stable isotope mass spectrum (207Pb/206Pb,208Pb/206Pb and206Pb/204pb); determining the Pb stable isotope ratio in the sediment before the deep layer is not influenced by human activities (usually before 1900 s) as the Pb isotope background value of natural sources; analyzing and determining isotope ratios of Pb samples of mining and metallurgical smoke and waste, gasoline combustion and tail gas emission smoke, cement manufacturing and building dust, northern coal combustion smoke, southern coal combustion smoke and the like which are close to a sampling area; loading a simmer (version 0.4.1) installation package in the R studio platform, and inputting Pb stable isotope ratio data in the sediment as mix parameters into a stable isotope mixing model 'simmer'; step five, taking the average value and the standard deviation of the stable isotope ratios of the five artificial sources Pb as s _ means and s _ sds to be respectively input into a model simmer; step six, inputting the names of the five artificial sources into a model semmer as s _ names, and setting grouping parameters grp as default (1 group) or other selected numbers; step seven, loading the parameters into the simmer _ in and transportingThe line Markov chain Monte Carlo method simmr _ mcmc is calculated, and the iteration number in the calculation is set to be 1 multiplied by 104-1×107Burn-in is set to 1X 103-1×105Obtaining the simmer _ out result when thining is 10-40 and Chains is 4-6; step eight, performing convergence diagnosis (Geoman-Rubin diagnostics) on the obtained result simmer _ out, and performing the next step when the obtained result is lower than 1.1, otherwise, increasing iteration times, burn-in, thining and chassis parameters and re-operating mcmc; and step nine, analyzing the obtained result simmer-out, operating statistics and qualites to obtain the average value, deviation and quantile data of the contribution ratios of different sources Pb, operating density to obtain the density distribution diagram of the contribution ratios of different sources Pb, operating matrix to obtain the matrix diagram of the contribution ratios of different sources Pb, and operating match _ source to obtain the sequencing and box diagram of the contribution ratios of different sources Pb.
Further, the ratio of Pb-stable isotope in the surface layer and columnar sediment of the water area was measured (207Pb/206Pb,208Pb/206Pb and206Pb/204pb), determining the Pb isotope ratio of natural lithogenetic sources according to the Pb isotope ratio in deep columnar sediments before 1900 years, and estimating the contribution rate and density distribution of various Pb sources in a water area by applying a stable isotope mixing model simmer based on a Markov chain Monte Carlo method and a Behcs probability statistical method based on the Pb stable isotope ratio in surface layer/columnar sediments, the Pb isotope value of natural sources and Pb isotope ratio data of several artificial sources of southern coal, northern coal, mining and metallurgy, gasoline combustion, cement manufacture and building dust.
Further, the isotopic ratio of Pb in the deposit is determined207Pb/206Pb,208Pb/206Pb and206Pb/204pb is input into the simmer model as the mixture, and the possible sources of Pb are: the average value and standard deviation of corresponding Pb isotope ratios of natural rock weathering sources, coal combustion, mining and metallurgy, gasoline combustion, cement manufacture, building dust and other sources are respectively used as s _ sources and s _ sdsEnter the simmer model.
Further, the correction coefficients c-means and c-sds in the simmer model and the concentration effect coefficient cons are set to 0. Chans was set to 4-6, and the number of iterations was set to 1 × 104-1×107Burn-in is set to 1X 103-1×105The thinning is set to the Markov chain Monte Carlo method (mcmc) of lines 10-40. And after Gelman-Rubin result verification is carried out, the results of the average value, the quantile, the density distribution and the like of the contribution rate of each source are output.
In summary, the advantages and positive effects of the invention are:
the environmental lead stable isotope ratio is independent of the lead production process and other biogeochemical processes, and is only related to the characteristic values of the lead source mine area. Thus, lead stable isotopes are an indicator of reliable tracking of the source of Pb input. The method has the advantages that the Pb pollution sources in the environment are distinguished by applying the lead stable isotope, the contribution ratio of Pb from each source is estimated, the method has important scientific significance for knowing the behavior characteristics, the sources and the destination of the lead pollutants in the environment, and meanwhile, the method is beneficial to environmental management and scientifically guides the control of lead pollution.
The stable isotope mixture model in the invention is a calculation model established based on iteration and Bayesian statistics, and can be used for estimating the contribution proportion of various end members. The stable isotope mixing model is applied to lead stable isotopes in the environment for the first time, calculation and analysis are carried out on the basis of the ratio of Pb stable isotopes in the sediment and isotope ratio data of possible sources, and the contribution ratio of different sources to lead in the water area is obtained. The calculation result shows that coal combustion becomes the most main lead pollution source in the offshore area in China, and the contribution rate of gasoline combustion, mining, metallurgy, building dust and the like is equivalent. By utilizing an isotope mixture model, estimation of the contribution ratio of lead from various sources in a complex environment is realized.
Drawings
Fig. 1 is a density profile of the results of a stable isotope mixture model simmer quantitatively estimating the contribution rate of Pb input sources in a deposit of a certain area.
Fig. 2 is a box-type distribution diagram of the results of the stable isotope mixture model simmer in quantitatively estimating the contribution rate of the Pb input source in the deposit of a certain region.
FIG. 3 is an interface for stable isotope mixture model simmer application.
FIG. 4 is a summary and contents of a stable isotope mixture model simmer (version 0.4.1) installation package.
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 with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
Aiming at the problems in the prior art, the invention provides an application method of a stable isotope mixture model in the quantification of the contribution rate of a Pb source, and the invention is described in detail below with reference to the accompanying drawings.
The application method of the stable isotope mixing model in the quantification of the contribution rate of the Pb source provided by the embodiment of the invention is used for measuring the ratio of the Pb stable isotope in the sediment of a water area (207Pb/206Pb,208Pb/206Pb and206Pb/204pb), determining the Pb isotope ratio of natural lithogenetic sources according to the Pb isotope ratio in deep sediments, and applying a stable isotope mixing model simmer to estimate the contribution rate of various Pb sources in a water area according to the Pb stable isotope ratio in the sediments, the Pb isotope value of the natural source and the Pb isotope ratio data of artificial sources.
In the embodiment of the invention, the ratio of Pb stable isotope in the surface layer and columnar sediment of the water area is determined by multi-receiving plasma mass spectrometry (207Pb/206Pb,208Pb/206Pb and206Pb/204pb), determining the Pb isotope ratio of natural lithogenous sources according to the Pb isotope ratio in deep columnar sediments before 1900 years, and applying a method based on Pb stable isotope ratio in surface layer/columnar sediments, natural source Pb isotope value and Pb isotope ratio data of several artificial sources including southern coal, northern coal, mining and metallurgy, gasoline combustion, cement manufacture and building dustA stable isotope mixture model simmer based on a Markov chain Monte Carlo method and a Behcs probability statistical method estimates the contribution rate and density distribution of various Pb sources in a water area.
In the examples of the present invention, the isotopic ratio of Pb in the deposit was determined207Pb/206Pb,208Pb/206Pb and206Pb/204pb is input into the simmer model as the mixture, and the possible sources of Pb are: the average value and standard deviation of corresponding Pb isotope ratios of natural rock weathering sources, coal combustion, mining and metallurgy, gasoline combustion, cement manufacturing, building dust and other sources are respectively input into the simmer model as s _ sources and s _ sds.
In the embodiment of the present invention, the correction coefficients c-means and c-sds and the concentration effect coefficient cons in the simmer model are set to 0. Chans was set to 4-6, and the number of iterations was set to 1 × 104-1×107Burn-in is set to 1X 103-1×105The thining is set to 10-40, line Markov chain Monte Carlo method (mcmc). And after Gelman-Rubin result verification is carried out, the results of the average value, the quantile, the density distribution and the like of the contribution rate of each source are output.
The application method of the stable isotope mixing model in the quantification of the Pb source contribution rate, provided by the embodiment of the invention, comprises the following steps:
s101: in the deposit207Pb/206Pb,208Pb/206Pb and206Pb/204pb in the range of 0.837-0.845, 2.081-2.097and 18.53-18.71; in the deposition of the column,207Pb/206Pb and208Pb/206the Pb is gradually increased from more than 30cm, and the increase of artificially input Pb in the near-shore area since 1980s is recorded;
s102: in the planar distribution of the Pb isotope,207Pb/206Pb and208Pb/206pb gradually rises from the shore to the sea, and the atmospheric input is the main pollution source of Pb in the east sea area; a mixture model of stable isotopes, simmer, was used to estimate the contribution of each source of Pb in the deposit.
The technical solution of the present invention is further described with reference to the following specific examples.
Example 1
Calculating to obtain the Pb isotope ratio of the artificial pollution input end member in the columnar sediment in the east China sea207Pb/206Pb,208Pb/206Pb and206Pb/204pb 0.859,2.114, and 18.180, respectively, as the texture input model. Northern coal, southern coal, gasoline combustion, mining and metallurgy and cement manufacture207Pb/206The average value +/-sd of Pb is respectively 0.869 +/-0.010, 0.855 +/-0.010, 0.8855 +/-0.080, 0.8608 +/-0.011, 0.8577 +/-0.015,208Pb/206the average value + -sd of Pb is 2.126 + -0.018, 2.102 + -0.021, 2.1442 + -0.006, 2.1501 + -0.032, 2, 1167 + -0.036 respectively,206Pb/204the mean values of Pb, +/-sd, are 17.914 + -0.185, 18.308 + -0.257, 17.716 + -0.261, 18.435 + -0.145 and 18.034 + -0.397, respectively, which are input as s _ sources and s _ sds input models, the number of sets is set to 1, and c-means, c-sds and cons in the simmer model are set to 0. Chans is set to 4, and the number of iterations is set to 1 × 104Burn-in is set to 1X 103Then, thining is set to 10 and the mcmc calculation is run. FIG. 1 is a density distribution diagram of the calculated output contribution rate of each source. It can be seen that coal (the sum of northern coal and southern coal) is the most important source of Pb pollution, the contribution rate is 45 +/-18%, and the contribution rates of gasoline combustion, mining, metallurgy and cement manufacturing are 19.8 +/-14%, 16.5 +/-12% and 18.3 +/-13%, respectively.
Example 2
Determining to obtain the isotope ratio of lead in the surface sediment of the east China sea207Pb/206Pb,208Pb/206Pb and206Pb/204pb is respectively 0.838-0.844, 2.081-2.097and 18.549-18.705, and the Pb is used as a texture input model. The natural source characteristic value of the lead is obtained according to the lead isotope value in the deep columnar sediment and is respectively 0.838, 2.081 and 18.705. Sources of lead pollution include northern coal, southern coal, gasoline combustion, mining and metallurgy and cement manufacturing207Pb/206The average value +/-sd of Pb is respectively 0.869 +/-0.010, 0.855 +/-0.010, 0.8855 +/-0.080, 0.8608 +/-0.011, 0.8577 +/-0.015,208Pb/206the average value + -sd of Pb is 2.126 + -0.018, 2.102 + -0.021, 2.1442 + -0.006, 2.1501 + -0.032, 2, 1167 + -0.036 respectively,206Pb/204the mean values of Pb, +/-sd, are 17.914 + -0.185, 18.308 + -0.257, 17.716 + -0.261, 18.435 + -0.145 and 18.034 + -0.397, respectively, which are input as s _ sources and s _ sds input models, the number of sets is set to 1, and c-means, c-sds and cons in the simmer model are set to 0. Chans is set to 4, and the number of iterations is set to 1 × 105Burn-in is set to 1X 104Then, thining is set to 20 and the mcmc calculation is run. The contribution ratio distribution of each source is obtained as shown in fig. 2. FIG. 1 is a density distribution diagram of the calculated output contribution rate of each source. The results show that 12-21% of the lead in the sediment was the pollutant input, 40% of which was from coal combustion, and the average contributions of cement, metallurgy and gasoline combustion were 27, 22, 12%, respectively.
The invention is further described below in connection with the positive effects.
The invention uses stable isotope of lead in surface layer and columnar sediment to distinguish Pb pollution source of Yangtze river mouth and adjacent sea area. In the deposit207Pb/206Pb,208Pb/206Pb and206Pb/204pb ranges from 0.837 to 0.845, 2.081 to 2.097and 18.53 to 18.71. In the deposition of the column,207Pb/206Pb and208Pb/206the increase in Pb from 30cm or more was recorded since 1980s in the near-shore region. In the planar distribution of the Pb isotope,207Pb/206Pb and208Pb/206pb gradually rises from the shore to the sea, reflecting that atmospheric input is a main pollution source of Pb in the east sea area. A mixture model of stable isotopes, simmer, was used to estimate the contribution of each source of Pb in the deposit. The results show that after 1990s the source of lithogenesis (mainly the sediment input in Yangtze river) was 78-88% of Pb in the sediment, while the source of man-made pollution was 12-22%. Coal is the most significant source of pollution and accounts for 46% of the pollution input, while cement, metallurgical dust and automobile exhaust emissions account for 19%, 17%, 20% of the pollution input, respectively.
The invention discloses that the atmospheric input is a main input source of Pb pollution in the east China sea area, and the stable isotope mixing model has good application prospect in quantitative research of the source contribution rate of Pb.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (7)
1. A method for applying a stable isotope mixture model to quantification of Pb source contribution rate is characterized by comprising the following steps:
the method comprises the steps of measuring the ratio of Pb stable isotopes in sediments in a water area, determining the ratio of Pb isotopes from natural lithogenetic sources according to the ratio of Pb isotopes in deep sediments, and estimating the contribution rate of various Pb sources in the water area by applying a stable isotope mixing model simmer according to the ratio of Pb stable isotopes in sediments, the value of Pb isotopes from natural sources and the ratio data of Pb isotopes from artificial sources.
2. The method for applying the stable isotope mixture model in quantifying the Pb-source contribution rate according to claim 1, wherein the method specifically comprises:
step one, measuring the ratio of Pb stable isotope in water area sediment by using stable isotope mass spectrum207Pb/206Pb,208Pb/206Pb and206Pb/204Pb；
determining the ratio of the Pb stable isotope in the sediment before the deep layer is not influenced by human activities as the background value of the Pb isotope of the natural source;
analyzing and determining isotope ratios of Pb samples of mining and metallurgical smoke and waste, gasoline combustion and tail gas emission smoke, cement manufacturing and building dust, northern coal combustion smoke, southern coal combustion smoke and the like which are close to a sampling area;
loading a simmer (version 0.4.1) installation package in the R studio platform, and inputting Pb stable isotope ratio data in the sediment as mix parameters into a stable isotope mixing model 'simmer';
step five, taking the average value and the standard deviation of the stable isotope ratios of the five artificial sources Pb as s _ means and s _ sds to be respectively input into a model simmer;
step six, inputting the names of the five artificial sources into a model semmer as s _ names, and setting grouping parameters grp as default (1 group) or other selected numbers;
step seven, loading the parameters into the simmer _ in, operating the Markov chain Monte Carlo method simmer _ mcmc for calculation, and setting the iteration number to be 1 multiplied by 10 in the calculation4-1×107Burn-in is set to 1X 103-1×105Obtaining the simmer _ out result when thining is 10-40 and Chains is 4-6;
step eight, performing convergence diagnosis (Geoman-Rubin diagnostics) on the obtained result simmer _ out, and performing the next step when the obtained result is lower than 1.1, otherwise, increasing iteration times, burn-in, thining and chassis parameters and re-operating mcmc;
and step nine, analyzing the obtained result simmer-out, operating statistics and qualites to obtain the average value, deviation and quantile data of the contribution ratios of different sources Pb, operating density to obtain the density distribution diagram of the contribution ratios of different sources Pb, operating matrix to obtain the matrix diagram of the contribution ratios of different sources Pb, and operating match _ source to obtain the sequencing and box diagram of the contribution ratios of different sources Pb.
3. The method of applying the stable isotope mixture model in quantifying the Pb-source contribution rate according to claim 1, wherein the contribution rate and the density distribution of each Pb source in the water area are estimated by applying the stable isotope mixture model simmer based on the markov chain monte carlo method and the bekes probability statistical method.
4. The method of using the stable isotope mixture model in quantifying Pb-source contribution rate according to claim 1, wherein the deposit is depositedIsotopic ratio of Pb in207Pb/206Pb,208Pb/206Pb and206Pb/204pb is input into the simmer model as the mixture, and the possible sources of Pb are: the mean and standard deviation of the corresponding Pb isotope ratios for natural rock weathering sources, coal combustion, mining and metallurgy, gasoline combustion, cement manufacture and construction dust sources were input to the simmer model as s _ sources and s _ sds, respectively.
5. The method for applying the stable isotope mixture model to the quantification of the Pb-source contribution ratio according to claim 1, wherein correction coefficients c-means and c-sds and a concentration effect coefficient cons in the simmer model are set to 0; chans was set to 4-6, and the number of iterations was set to 1 × 105-1×107Burn-in is set to 1X 104-1×106Thinning is set to the 20-40 line markov chain monte carlo method; and after Gelman-Rubin result verification is carried out, the average value, quantile and density distribution results of the contribution rates of all sources are output.
6. A program storage medium storing a program for a method of applying a stable isotope mixture model to quantify a Pb source contribution rate, the stored computer program causing an electronic device to execute the steps comprising: the method comprises the steps of measuring the ratio of Pb stable isotopes in sediments in a water area, determining the ratio of Pb isotopes from natural lithogenetic sources according to the ratio of Pb isotopes in deep sediments, and estimating the contribution rate of various Pb sources in the water area by applying a stable isotope mixing model simmer according to the ratio of Pb stable isotopes in sediments, the value of Pb isotopes from natural sources and the ratio data of Pb isotopes from artificial sources.
7. An apparatus for performing the method of estimating the contribution of various sources of Pb in water as claimed in any one of claims 1 to 5.
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| CN104391031A (en) * | 2014-11-17 | 2015-03-04 | 中国环境科学研究院 | Qualitative source analyzing method for lead exposure source in human urine |
| CN109920492A (en) * | 2019-03-26 | 2019-06-21 | 中国水利水电科学研究院 | A kind of method of plumbic harm parsing in water body deposit |
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| CN112698005A (en) * | 2020-12-30 | 2021-04-23 | 中国有色桂林矿产地质研究院有限公司 | Quantitative analysis method for heavy metal Pb source of farmland soil |
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