CN107389645B - The method that the Fisher model that wavelet transform parses oil product fluorescent characteristic identifies marine oil overflow - Google Patents
The method that the Fisher model that wavelet transform parses oil product fluorescent characteristic identifies marine oil overflow Download PDFInfo
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
- G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
- G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
- G01N21/64—Fluorescence; Phosphorescence
- G01N21/6402—Atomic fluorescence; Laser induced fluorescence
Abstract
The present invention relates to the methods that the Fisher model of wavelet transform parsing oil product fluorescent characteristic identifies marine oil overflow, belong to marine environmental pollution monitoring and improvement field.The present invention carries out 6 layers of decomposition to oil sample fluorescence spectra by db7 wavelet basis function, extracts d3 detail coefficients feature, the quantitative formula for identifying marine oil overflow is established in conjunction with Fisher diagnostic method, and verified by actual sample.The result of this method quantization is higher for oil sample identification accuracy, overcomes the defect of current Qualitive test marine oil overflow, and provide a foundation to research and develop real-time, the quick portable instrument for identifying marine oil overflow.
Description
Technical field
The present invention relates to wavelet transform parsing oil product fluorescent characteristic Fisher model identify marine oil overflow method,
Oil sample fluorogram is decomposed using wavelet transform more particularly to a kind of, quickly identifies sea in conjunction with Fisher diagnostic method
The fuel oil and crude oil of upper oil spilling and the method for further discriminating between middle-eastern crude belong to marine environmental pollution monitoring and administer neck
Domain.
Background technique
With the development of marine transportation industry, oil spill accident happens occasionally, and not only threatens marine ecosystems, also strong to the mankind
Kang Zaocheng is seriously endangered.So promptly and accurately identifying oil spilling source, taking urgent measure to protect the marine environment seems especially heavy
It wants[1]。
The complex mixture that petroleum is made of different compounds, domestic and foreign scholars by n-alkane in oil sample,
100 multiple compounds such as polycyclic aromatic hydrocarbon and biomarker carry out discriminatory analysis to oil sample[2-5].Wang Xin equality[6]Pass through gas phase color
Internal standard method establishes n-alkane in crude oil to spectrum, the analysis method of biomarker (steroid, terpane class) identifies crude oil sample；
In view of compound fragrant hydrocarbon rich in petroleum[7]And fluorescence spectrophotometry have high-resolution, high sensitivity,
The features such as sample pre-treatments are simple[8], the research of oil product fluorescent characteristic has received widespread attention.Wang etc.[9]With based on difference
Synchronous fluorimetric method under concentration, using principal component analysis, Partial Least Squares Method, Gobar transformation respectively to oil sample into
Row feature extraction, compares the spectral signature between oil spilling sample and doubtful oil spilling source, total accuracy is respectively 77%, 79%,
92%, but Gobar transformation can not extract some abrupt informations and unstable information, information extraction is imperfect.And it is discrete small
Wave (DWT) is by specific flexible and shift factor and suitable wavelet basis function is selected to handle original signal, can produce
The approximation coefficient of raw reflection original signal large scale information and the detail coefficients of smaller scale information[10]。
Bibliography:
[1] Zhao Yunying, the progress marine environment science of development in oil spills identification by fluorescence spectroscopy, 1997,2 (16)
29-35
[2]Merv Fingas The basics of spill cleanup 2nd[M].New York:Lewis
Publishers,2001
[3]Wang Zhendi,Fingas M,Page D S.Oil spill identification.Journal of
Chromatography A,1999,843(1/2):369-411
[4]Ebrahimi D,Lia J,Hibbert D B.Classification of weathered petroleum
oils by multi-way of gas chromatography-mass spectrometry data using PARAFAC2
parallel factor analysis,Journal of Chromatography A,2007,1166(1/2):163-170
[5] Liu Xiaoxing, Sun Huiqing, Wang Yahui accord with high Yao distribution of normal alkanes characteristic differentiation sea mixed crude [J] ring
Border chemistry, 2016,35 (2): 305-310.
[6] Wang Xinping, Sun Peiyan, Zhou Qing, Li Mei, Cao Lixin, Zhao Yuhui, the internal standard method analysis of crude oil saturated hydrocarbons fingerprint
[J] analytical chemistry 2007,35 (8): 1121-1126.
[7]Weng N,Wan S,Wang H,et al.Journal of Chromatography A,2015,1398:94
~107.
[8]Greene L V,Elzey B,Franklin M,et al.Spectrochimica Acta Part A:
Molecular and Biomolecular Spectroscopy, 2017,174:316~325.
[9]Wang C,Shi X,Li W,et al.Marine Pollution Bulletin,2016,104(1-2):
322~328.
[10]Ha D,Park D,Koo J,et al.Computers&Chemical Engineering,2016,94:
362~369.
Summary of the invention
The present invention establishes one kind using wavelet transform combination Fisher diagnostic method and quickly identifies fuel oil and crude oil simultaneously
The method for further discriminating between middle-eastern crude carries out 6 layers of decomposition to oil sample fluorescence spectra by db7 wavelet basis function, extracts d3
Detail coefficients feature is established the quantitative formula for identifying marine oil overflow in conjunction with Fisher diagnostic method, and is tested by actual sample
Card.The result of this method quantization is higher for oil sample identification accuracy, overcomes the defect of current Qualitive test marine oil overflow, and
To research and develop, in real time, quickly the portable instrument of identification marine oil overflow provides a foundation.
The method that the Fisher model that wavelet transform parses oil product fluorescent characteristic identifies marine oil overflow, including following steps
It is rapid:
1. carrying out 6 layers of decomposition to oil sample fluorescence spectra using db7 wavelet basis function, d3 detail coefficients feature is extracted, is obtained
Sample to be tested 255 ± 2nm, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354 ± 2nm, five characteristic wave strong points small echo
Coefficient X1~X5；
2. bringing the wavelet coefficient of 1. five characteristic wave strong points that step obtains into following Fisher discrimination formula Y1And Y2
In,
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5
Wherein, X1~X5D3 is respectively indicated at 255 ± 2nm, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354 ± 2nm
Wavelet coefficient.
3. calculating 2. sample (Y that step obtains1, Y2) Euclidean distance between value and each group mass center judges to belong to, judge to advise
Then are as follows: smaller with certain group centroid distance, sample then belongs to this group of classification,
Wherein, the group mass center of fuel oil is O1(Y1=3.293, Y2=0.211)；The group mass center of middle-eastern crude is O2(Y1=-
2.114 Y2=0.769)；The group mass center of non-middle-eastern crude is O3(Y1=-0.825, Y2=-0.505).
" d3 detail coefficients " of the present invention are to carry out 6 layers of decomposition to oil sample fluorogram by db7 wavelet basis function, will
Original spectrogram resolves into 6 layers of approximation coefficient and 6 layers of detail coefficients, and the present invention chooses the 3rd layer of 6 layers of detail coefficients, due to details
It is " d " that coefficient, which is write a Chinese character in simplified form, and the 3rd layer of detail coefficients herein write d3.
Preferred steps of the present invention 1. in, the fluorescence spectra of the sample is measured using permanent wavelength method.
Preferred steps of the present invention 1. in, the fluorescence spectra of the sample is measured by molecular fluorescence spectrophotometer.
Step of the present invention 2. described in discrimination formula utilize Fisher diagnostic method obtain.Fisher diagnostic method is by variance
The method that the thought of analysis constructs a linear discriminant function, this method to distinguish maximum between all kinds of groupings, and makes to be grouped
Internal deviation is minimum, achievees the purpose that classification with this.Oil sample is divided into three classes by the present invention: fuel oil, middle-eastern crude, the non-Middle East
Crude oil.
The invention has the benefit that the present invention carries out details using fluorescence spectrum information of the wavelet transform to oil sample
Coefficient extracts, and the Fisher discrimination model for identifying oil product is established with this, which, can while distinguishing fuel oil and crude oil
Middle-eastern crude is further discriminated between.The model established identification accuracy with higher, such as just to the identification of non-modeling oil sample
True rate is 95.7%, it is also applied for the identification of weathering oil product.Identification formula of the invention can quickly, quantitatively identify sea
The fuel oil and crude oil of oil spilling simultaneously further discriminate between middle-eastern crude, to realize that online, identification marine oil overflow is portable in real time from now on
The research and development of formula instrument provide a theoretical basis.
Detailed description of the invention
Fig. 1 is that embodiment 1 addresses No. 16 floor exploded view of non-weathering light-weight fuel oil；
Fig. 2 is that embodiment 1 addresses No. 16 floor exploded view of light-weight fuel oil after weathering；
Fig. 3 is that embodiment 2 addresses 6 layers of exploded view of non-weathering United Arab Emirates crude oil；
Fig. 4 is that embodiment 2 addresses 6 layers of exploded view of United Arab Emirates' crude oil after weathering；
Fig. 5 is that embodiment 3 addresses 6 layers of exploded view of non-weathering Daqing crude oil；
Fig. 6 is that embodiment 3 addresses 6 layers of exploded view of Daqing crude oil after weathering.
Specific embodiment
Following non-limiting embodiments can with a person of ordinary skill in the art will more fully understand the present invention, but not with
Any mode limits the present invention.
Test method described in following embodiments is unless otherwise specified conventional method；The reagent and material, such as
Without specified otherwise, commercially obtain.
Discrimination formula of the present invention is established according to the wavelet coefficient of oil sample, specific as follows:
1, modeling parameters are extracted in optimization
6 layers of decomposition are carried out to oil sample fluorescence spectra using db7 wavelet basis function, d3 detail coefficients feature is extracted, extracts
255 ± 2nm, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, the wavelet coefficient at 354 ± 2nm are modeled；
2, fluorescence spectra measures
Using molecular fluorescence spectrometry, using the above-mentioned required so-called fluorescence spectra of decomposition of permanent wavelength method measurement.
3, the foundation of discrimination model
Using 8 kinds of fuel oil, 14 kinds of non-middle-eastern crudes and 7 kinds of middle-eastern crudes as analysis object, all analysis objects are measured
Fluorescence spectra, carry out wavelet transform to it, obtain 255 ± 2nm, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354
Wavelet coefficient combination Fisher diagnostic method at ± 2nm establishes model.
Following is the implementation example an of model foundation:
Using 8 kinds of fuel oil, 14 kinds of non-middle-eastern crudes and 7 kinds of middle-eastern crudes as analysis object, all analysis objects are measured
Fluorescence spectra.The fluorescence intensity of oil sample fluorescence spectra is imported into Matlab R2012b, in Matlab R2012b
Command Window input " wavemenu " recall wavelet toolbox, select " Wavelet 1-D " to enter window, in the window
Selection File → Load → Signal recalls the fluorescence intensity imported, and Wavelet selects db7, and Level selects 6 layers, to spectrum
Figure carries out wavelet decomposition.Extract the wavelet systems of 255 ± 2nm of d3 layer, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354 ± 2nm
Number is used as modeling parameters, carries out Fisher discriminant analysis.Utilize (the Statistical Analysis System of SAS 9.1
(SAS) application software) Fisher differentiation is carried out, the group of fuel oil is set as 0, and middle-eastern crude group is set as 1, non-middle-eastern crude group
It is not set as 2.
Program is as follows:
Data dataset name
The wavelet coefficient grouping of 255 ± 2nm of Input, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354 ± 2nm；
Datalines；
Input data ...
；
The above-mentioned dataset name out=of Proc Candisc data=exports canonical variable data name (present invention Y
It indicates)；
Class grouping；
The wavelet coefficient of 255 ± 2nm of Var, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354 ± 2nm；
Run；
The equation coefficients obtained by Candisc process；
Y1Factor alpha1For (- 0.396 0.384-0.142-0.167 0.151)
Y2Factor alpha2For (0.114 0.207-0.103 of 0.803-0.314)；
Participate in d3 layers of 29 kinds of oil samples of 255 ± 2nm, the 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354 ± 2nm of modeling
Wavelet coefficient average value β be (11.882 28.426 8.060 9.707 7.929).Its formula constant term C=- αi*βT, i
=1,2；It is computed two formula are as follows:
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5
Wherein Y1、Y2For Fisher discrimination formula, X1~X5Indicate d3 layers 255 ± 2nm, 280 ± 2nm, 302 ± 2nm,
Wavelet coefficient at 332 ± 2nm, 354 ± 2nm.
4, the accuracy of model is verified
Identify model to the fuel oil of marine oil overflow, middle-eastern crude and non-Middle East original to verify the oil sample that the present invention establishes
The accuracy that oil identifies, is verified with 29 kinds of modeling oil samples after short-term weathering 30 days, and total accuracy is 96.6%.In addition,
It is also verified with 23 kinds of non-modeling oil samples, up to 95.7%, the accuracy rate differentiated is higher than is returned total accuracy using binary linearity
Return the model of establishing equation.
Oil sample fluorescence spectra is measured using molecular fluorescence spectrometry in following embodiments, and selected instrument and method are such as
Under:
Instrument and reagent: analysis instrument is Cary Eclipse type Fluorescence spectrophotometer (Varian company, the U.S.)；
Solvent: n-hexane (chromatographically pure, German Merck)；
Sample pre-treatments: with beaker weigh (0.05 ± 0.0002) g sample oil, by acquired oil sample be dissolved in 10mL just oneself
Alkane, concussion is to being completely dissolved, then static 5min, pipettes 40uL supernatant in test tube, and 10mL n-hexane is added, continues to employ to be measured.
Embodiment 1: with light-weight fuel oil 1 verifying before and after weathering
Table 1: wavelet coefficient at No. 1 d3 floor five of non-weathering light-weight fuel oil
| λ/nm | 255±2 | 280±2 | 302±2 | 332±2 | 354±2 |
| Wavelet coefficient | 19.485 | 42.393 | 8.420 | 4.086 | 3.221 |
Wavelet systems numerical tape in table 1 is entered into following calculation formula:
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5=2.531
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5=1.087
(Y1, Y2) with the group mass center O of fuel oil1(Y1=3.293, Y2=0.211), the group mass center O of middle-eastern crude2(Y1=-
2.114 Y2=0.769), the group mass center O of non-middle-eastern crude3(Y1=-0.825, Y2=-0.505) Euclidean distance is respectively
1.161,4.656,3.715.It can thus be appreciated that and O1Recently, this oil sample is fuel oil to distance, is met with known case.
Table 2: wavelet coefficient at No. 1 d3 floor five of light-weight fuel oil after weathering
| λ/nm | 255±2 | 280±2 | 302±2 | 332±2 | 354±2 |
| Wavelet coefficient | 16.789 | 35.860 | 8.120 | 6.602 | 5.040 |
Wavelet systems numerical tape in table 2 is entered into following calculation formula:
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5=0.987
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5=1.272
(Y1, Y2) with the group mass center O of fuel oil1(Y1=3.293, Y2=0.211), the group mass center O of middle-eastern crude2(Y1=-
2.114 Y2=0.769), the group mass center O of non-middle-eastern crude3(Y1=-0.825, Y2=-0.505) Euclidean distance is respectively
2.538,3.142,2.982.It can thus be appreciated that and O1Recently, this oil sample is fuel oil to distance, is met with known case.
Embodiment 2: it is verified with United Arab Emirates' crude oil before and after weathering
Table 3: wavelet coefficient at non-weathering United Arab Emirates crude oil d3 layer five
| λ/nm | 255±2 | 280±2 | 302±2 | 332±2 | 354±2 |
| Wavelet coefficient | 12.628 | 24.524 | 8.163 | 10.717 | 7.379 |
Wavelet systems numerical tape in table 3 is entered into following calculation formula:
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5=-2.058
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5=2.107
(Y1, Y2) with the group mass center O of fuel oil1(Y1=3.293, Y2=0.211), the group mass center O of middle-eastern crude2(Y1=-
2.114 Y2=0.769), the group mass center O of non-middle-eastern crude3(Y1=-0.825, Y2=-0.505) Euclidean distance is respectively
5.677,1.340,2.890.It can thus be appreciated that and O2Recently, this oil sample is middle-eastern crude to distance, is met with known case.
Table 4: wavelet coefficient at non-weathering United Arab Emirates crude oil d3 layer five
| λ/nm | 255±2 | 280±2 | 302±2 | 332±2 | 354±2 |
| Wavelet coefficient | 11.498 | 21.365 | 5.063 | 7.466 | 5.488 |
Wavelet systems numerical tape in table 4 is entered into following calculation formula:
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5=-2.126
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5=1.360
(Y1, Y2) with the group mass center O of fuel oil1(Y1=3.293, Y2=0.211), the group mass center O of middle-eastern crude2(Y1=-
2.114 Y2=0.769), the group mass center O of non-middle-eastern crude3(Y1=-0.825, Y2=-0.505) Euclidean distance is respectively
5.540,0.591,2.273.It can thus be appreciated that and O2Recently, this oil sample is middle-eastern crude to distance, is met with known case.
Embodiment 3: it is verified with the Daqing crude oil before and after weathering
Table 5: wavelet coefficient at non-weathering Daqing crude oil d3 layer five
| λ/nm | 255±2 | 280±2 | 302±2 | 332±2 | 354±2 |
| Wavelet coefficient | 7.551 | 16.640 | 4.820 | 6.090 | 6.393 |
Wavelet systems numerical tape in table 5 is entered into following calculation formula:
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5=-1.977
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5=-0.732
(Y1, Y2) with the group mass center O of fuel oil1(Y1=3.293, Y2=0.211), the group mass center O of middle-eastern crude2(Y1=-
2.114 Y2=0.769), the group mass center O of non-middle-eastern crude3(Y1=-0.825, Y2=-0.505) Euclidean distance is respectively
5.353,1.501,1.174.It can thus be appreciated that and O3Recently, this oil sample is non-middle-eastern crude to distance, is met with known case.
Table 6: wavelet coefficient at Daqing crude oil d3 layer five after weathering
| λ/nm | 255±2 | 280±2 | 302±2 | 332±2 | 354±2 |
| Wavelet coefficient | 7.379 | 16.669 | 4.756 | 5.031 | 5.618 |
Wavelet systems numerical tape in table 6 is entered into following calculation formula:
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5=-1.828
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5=-1.026
(Y1, Y2) with the group mass center O of fuel oil1(Y1=3.293, Y2=0.211), the group mass center O of middle-eastern crude2(Y1=-
2.114 Y2=0.769), the group mass center O of non-middle-eastern crude3(Y1=-0.825, Y2=-0.505) Euclidean distance is respectively
5.268,1.817,1.131.It can thus be appreciated that and O3Recently, this oil sample is non-middle-eastern crude to distance, is met with known case.
Claims (3)
1. the method that the Fisher model that wavelet transform parses oil product fluorescent characteristic identifies marine oil overflow, it is characterised in that:
Include the following steps:
1. using db7 wavelet basis function to oil product fluorescence spectra carry out 6 layers decomposition, extract d3 detail coefficients feature, obtain to
Survey oil product 255 ± 2nm, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354 ± 2nm, five characteristic wave strong points wavelet coefficient
X1~X5；
2. bringing the wavelet coefficient of 1. five characteristic wave strong points that step obtains into following Fisher discrimination formula Y1And Y2In,
Y1=-4.642-0.396*X1+0.384*X2-0.142*X3-0.167*X4+0.151*X5
Y2=-2.727+0.803*X1-0.314*X2+0.114*X3+0.207*X4-0.103*X5
Wherein, X1~X5It is small at 255 ± 2nm, 280 ± 2nm, 302 ± 2nm, 332 ± 2nm, 354 ± 2nm to respectively indicate d3
Wave system number；
3. calculating 2. oil product (Y that step obtains1, Y2) Euclidean distance between value and each group mass center judges to belong to, judgment rule
Are as follows: smaller with certain group centroid distance, oil product then belongs to this group of classification,
Wherein, the group mass center of fuel oil is O1(Y1=3.293, Y2=0.211)；The group mass center of middle-eastern crude is O2(Y1=-
2.114 Y2=0.769)；The group mass center of non-middle-eastern crude is O3(Y1=-0.825, Y2=-0.505),
The d3 detail coefficients are to carry out 6 layers of decomposition to oil product fluorogram by db7 wavelet basis function, by original pattern decomposition
At 6 layers of approximation coefficient and 6 layers of detail coefficients, the 3rd layer for choosing 6 layers of detail coefficients is used as the 3rd layer of detail coefficients.
2. according to the method described in claim 1, it is characterized by: step 1. in, the fluorescence spectra of the sample is using permanent
The measurement of wavelength method.
3. according to the method described in claim 1, it is characterized by: step 1. in, the fluorescence spectra of the sample is to pass through
Molecular fluorescence spectrophotometer measures.
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