CN102727213B - Method for manifesting latent fingerprints on basis of electrochemical luminescence marker - Google Patents
Method for manifesting latent fingerprints on basis of electrochemical luminescence marker Download PDFInfo
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- 239000010452 phosphate Substances 0.000 claims description 10
- IWSZDQRGNFLMJS-UHFFFAOYSA-N 2-(dibutylamino)ethanol Chemical compound CCCCN(CCO)CCCC IWSZDQRGNFLMJS-UHFFFAOYSA-N 0.000 claims description 8
- 238000002372 labelling Methods 0.000 claims description 8
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Abstract
The invention discloses a method for manifesting latent fingerprints on the basis of an electrochemical luminescence marker. According to the method, an activated terpyridine ruthenium composite is used as the electrochemical luminescence marker; the activated terpyridine ruthenium composite can be subjected to covalent binding with an amino group in fingerprint amino acid through N-hydroxysuccinimide eater on a molecule, so that the terpyridine ruthenium composite is marked and fixed on the fingerprints; then the terpyridine ruthenium composite and a coreactant (namely dinormal-butyl ethanolamine) in a solution are subjected to electrochemical luminescence reaction under certain potential, so that lines of the fingerprints comprising the integral morphology (namely a primary structure) and detailed features (namely a secondary structure) are manifested; according to the adopted electrochemical luminescence technology, an excitation light source is not required to be added, back light is eliminated, a self-quenching phenomenon of a radiant agent is greatly avoided, and the method is obviously superior to the traditional fluorescence imaging method; and an image can be quickly acquired by an imaging technology, and the speed of acquiring the image by the imaging technology is far higher than the speed of acquiring the image by a scanning electrochemical microscopy; and the used electrochemical luminescence coreactant is dinormal-butyl ethanolamine, and has the characteristics of high luminous intensity and environment-friendliness.
Description
Technical field
The invention belongs to latent fingerprint appearing technique field, particularly a kind of latent fingerprint process for show based on electrochemiluminescence label.
Background technology
Fingerprint is made up of a kind of ridge projections series that is called friction ridge, has very special physiological structure and feature architecture.Fingerprint is being served as important function aspect forensic identification and personal identification, is widely used in the fields such as safety verification in daily life, access control, personal authentication simultaneously.So-called latent fingerprint, when the finger, palm that refers to people touches object, due to the sweat mixed with dirt of secretion and the interaction of oils and fats and object plane, on object plane, leave the impression (being divided into the ridge line region of sweat mixed with dirt and composition and the line region, valley of depression) of reflection fingers and palms surface skin papillary ridges.This impression, can not directly be examined and see by eyesight or instrument as a rule, forms latent image through overexposure as photo sensitive film, needs could show original image by development treatment, so be called latent fingerprint.According to the difference that manifests principle, latent fingerprint process for show mainly contains three classes: optics appearance method, chemical appearance method and physisorphtion, its ultimate principle is exactly to use a kind of light or material to act on the perspiration material of finger mark, makes the sweat fingerprint that can not see become visible.
Constantly there is in recent years researcher to utilize various new techniques to carry out the detection of fingerprint manifestation and fingerprint composition, as mass spectrum imaging, infrared/Raman image, immune labeled imaging, scan-type electrochemical micro-imaging and local current imaging etc.The technology that wherein manifests latent fingerprint based on electrochemical principle is subject to people and more and more pays close attention to.The local current that Shan etc. utilize surface plasma resonance optical signal to cause changes fingerprint is manifested, and detects for TNT, and achievement is published in Sicence upper (Science, 2010,327).Qin etc. for the fingerprint manifestation on multiple object, react scan-type electrochemical microscope (SECM) technology to the topological structure (Electroanalysis, 2012,24,1-6) of fingerprint according to the variation of faradic currents.Although fingerprint manifestation method is various, in Appearing Techniques of Human Fingerprints, still there is many difficulties at present.For example, successfully latent fingerprint manifests the chemical composition that depends on very much fingerprint residues thing, in practice because the phenomenon of having selected inappropriate appearing technique to destroy fingerprint material evidence happens occasionally.For another example,, although Scanning electrochemical microscopy is a kind of very sensitive non-wound detection technique, its testing process is time-consuming, need to expend for ten a few to tens of hours if obtain Centimeter Level image.Therefore at present still need a kind of technology method simple, quick, applied widely to manifest latent fingerprint.
Electrochemiluminescence is the product that electrochemical reaction and chemiluminescence combine, and realizes by converting electric energy to radiant energy.Because electrochemiluminescence produces at electrode surface, therefore can reflect electrode reaction activity, and there is the advantages such as background is low, space-time is controlled.Therefore, electrochemiluminescence is widely used in imaging research, for example, observe functional area, the inspection electro-chemical activity site etc. of electrode.Simultaneous electrochemical luminescence imaging is also successful for the preparation of various micro-electrochemistry and microfluid system, screening metabolite toxicity and detection tumor marker protein etc.During electrochemiluminescence detects, the most widely used luminous marker is the tris (bipyridine) ruthenium of N-hydroxy-succinamide ester activation.In the time of its labelled protein, antibody or nucleic acid, ester chain interruption, the amino in biomolecule is combined.At present, the tris (bipyridine) ruthenium complex of activation is used for to Finger-print labelling method and carries out electrochemiluminescence imaging do not have report.
Summary of the invention
The object of the invention is for the deficiencies in the prior art, a kind of method that manifests latent fingerprint based on electrochemiluminescence label is provided; The method is simple, quick, luminous intensity is high.
The object of the invention is to be achieved through the following technical solutions: a kind of method that manifests latent fingerprint based on electrochemiluminescence label, the method realizes in electrochemiluminescence imaging system; Electrochemiluminescence imaging system comprises electrochemical reaction cell, constant potential control instrument and CCD photographing unit, electrochemical reaction cell comprises base and cell body, has groove on base, cell body hollow, be fixed on groove by O RunddichtringO and screw, cell body one side has an aperture; Constant potential control instrument comprises working electrode, to electrode and reference electrode, reference electrode is placed in aperture, wherein, working electrode is ITO(indium tin oxide electro-conductive glass), be platinum loop to electrode, reference electrode is Ag/AgCl electrode or Ag electrode; The method comprises the following steps:
(1) electrode pretreatment: by working electrode successively each ultrasonic cleaning 10-20min in acetone, ethanol and deionized water, then use deionized water cleaning down clean, dry up with argon.
(2) finger mark sample preparation: the finger mark on different objects is extracted with adhesive tape, then transfer on working electrode, form finger mark sample;
(3) with the tris (bipyridine) ruthenium complex labelling finger mark activating: by 50
the tris (bipyridine) ruthenium composite coated of activation, on finger mark sample, covers surface plate and prevents solution evaporation, more than at room temperature reacting 30min,, dries up with argon to remove unreacted complex with deionized water lavage specimens;
(4) electrochemiluminescence imaging: by the working electrode of above-mentioned processing, electrode and reference electrode are placed in to electrochemical reaction cell, then the reaction solution containing coreagent is added in electrochemical reaction cell, constant potential control instrument energising, CCD photographing unit gathers fingerprint image; Described reaction solution by adding 50mmol di-n-butyl ethanolamine and 0.15mol sodium chloride to form in every liter of phosphate buffered solution, and the pH of phosphate buffered solution is 7.4, and the current potential of constant potential control instrument is 1.3V.
Further, in described step (2), described object includes but not limited to computer screen, CD, coin, desktop and stainless steel ware.
Further, in described step (3), the tris (bipyridine) ruthenium complex of described activation is the tris (bipyridine) ruthenium of N-hydroxy-succinamide activation.
The invention has the beneficial effects as follows,
1, the method detects rapidly, only needs the several seconds can obtain Centimeter Level image, far away faster than Scanning electrochemical microscopy (tens to tens hours).
2, do not need expensive instrument; Do not need external excitation light source, therefore do not exist bias light to disturb, be better than fluorescence method.
3, because electrochemiluminescence reaction is to be produced with the coreagent being dissolved in reaction solution by the luminous body being fixed on finger mark, therefore the self-quenching effect of luminous body is low, manifests successful and is better than fluorescence method.
4, the method is highly sensitive, both can, for manifesting oily latent, also can be used for manifesting the less antiperspirant latent of active substance.
5,, compared with traditional coreagent Tri-n-Propylamine, the coreagent di-n-butyl ethanolamine that the method is used has high, the eco-friendly advantage of luminous intensity.
Brief description of the drawings
Fig. 1 is electrochemiluminescence imaging system schematic diagram;
Fig. 2 is the structural representation of electrochemical reaction cell;
Fig. 3 is the electrochemiluminescence figure that processes the oily latent of 3.5h with the tris (bipyridine) ruthenium complex of activation;
Fig. 4 is the electrochemiluminescence figure that processes the oily latent of 6 h with the tris (bipyridine) ruthenium complex of activation;
Fig. 5 is the electrochemiluminescence figure that processes the oily latent of 3.5h with the tris (bipyridine) ruthenium complex of the activation of dilution twice;
Fig. 6 is the electrochemiluminescence figure that processes the antiperspirant latent of 3.5h with the tris (bipyridine) ruthenium complex of activation;
In figure, electrochemical reaction cell 1, constant potential control instrument 2, CCD photographing unit 3, base 4, cell body 5, groove 6, O RunddichtringO 7, screw 8, aperture 9, working electrode 10, to electrode 11, reference electrode 12.
Detailed description of the invention
Principle of the present invention is: human finger's surface skin is covered with sweat gland, touches thing trace.In general the fingerprint material of staying object surface is less, is generally 0.11mg, and wherein 99% is moisture, can evaporate rapidly; Solid matter only accounts for 1%, and wherein 2/3 is organic substance, as: aminoacid, protein, fatty acid, carbamide etc.; Residue 1/3 is inorganic substances.The present invention, taking the aminoacid in finger mark as detecting thing, has prepared the tris (bipyridine) ruthenium complex of activation.It can be by the amino generation covalent bond in N-hydroxy-succinamide ester and finger mark aminoacid on molecule, thus labelling being fixed on fingerprint.Then the good sample of labelling is arranged in electrochemical reaction cell, add the reaction solution containing coreagent, apply certain potentials, on fingerprint, the tris (bipyridine) ruthenium complex of labelling can react with the coreagent generation electrochemiluminescence in solution, thereby shows the lines of fingerprint.
The present invention is based on the method that electrochemiluminescence label manifests latent fingerprint realizes in electrochemiluminescence imaging system.
As illustrated in fig. 1 and 2, electrochemiluminescence imaging system comprises electrochemical reaction cell 1, constant potential control instrument 2 and CCD photographing unit 3, electrochemical reaction cell 1 comprises base 4 and cell body 5, on base 4, there is groove 6, cell body 5 hollows, be fixed on groove 6 by O RunddichtringO 7 and screw 8, cell body 5 one sides have an aperture 9.Constant potential control instrument 2 comprises working electrode 10, to electrode 11 and reference electrode 12, reference electrode 12 is placed in aperture 9, wherein, working electrode is ITO(indium tin oxide electro-conductive glass), be platinum loop to electrode, reference electrode is Ag/AgCl electrode or Ag electrode.The material of electrochemical reaction cell 1 can be politef; But be not limited to this.
Method of the present invention comprises the following steps:
1, electrode pretreatment: by working electrode 10 successively each ultrasonic cleaning 10-20min in acetone, ethanol and deionized water, then use deionized water cleaning down clean, dry up with argon.
2, finger mark sample preparation: the finger mark on different objects is extracted with adhesive tape, then transfer on working electrode 10 formation finger mark sample with moderate dynamics; Object includes but not limited to computer screen, CD, coin, desktop and stainless steel ware.
3, with the tris (bipyridine) ruthenium complex labelling finger mark activating: by 50
the tris (bipyridine) ruthenium composite coated of activation, on finger mark sample, covers surface plate and prevents solution evaporation, more than at room temperature reacting 30min,, dries up with argon to remove unreacted complex with deionized water lavage specimens.
The tris (bipyridine) ruthenium complex of activation is the tris (bipyridine) ruthenium of N-hydroxy-succinamide activation, can be according to document (Biophysical Journal, 1995,68,342-350) synthetic, the end-product obtaining is the dimethyl formamide solution of this complex, in this step, is coated on finger mark sample.
4, electrochemiluminescence imaging: by the working electrode of above-mentioned processing 10, electrode 11 and reference electrode 12 are placed in to electrochemical reaction cell 1, then the reaction solution containing coreagent is added in electrochemical reaction cell 1, constant potential control instrument 2 is switched on, and CCD photographing unit 3 gathers fingerprint image.
Reaction solution by adding 50mmol di-n-butyl ethanolamine and 0.15mol sodium chloride to form in every liter of phosphate buffered solution, and the pH of phosphate buffered solution is 7.4.The current potential of constant potential control instrument 2 is 1.3V.
Below in conjunction with drawings and Examples, the present invention is described in more detail.
The present invention manifests latent fingerprint based on electrochemiluminescence label, after tris (bipyridine) ruthenium complex labelling by one piece of finger mark with activation, be arranged in electrochemical reaction cell as shown in Figure 2, be assembled into three-electrode system according to shown in Fig. 1, by applying certain current potential, the electrochemiluminescence that electrode surface produces can be caught by the highly sensitive CCD photographing unit of top, obtains thus finger mark image.
(1) on ITO, press one piece of oily latent;
(2) with activation tris (bipyridine) ruthenium complex hatch 4h, with deionized water rinsing to remove unreacted complex;
(3) sample is arranged in electrochemical reaction cell, adds the phosphate buffered solution of 50mM di-n-butyl ethanolamine, apply 1.3V current potential by three-electrode system, with highly sensitive CCD photographing unit, image is caught, obtain the electrochemiluminescence image shown in Fig. 3.
(1) on ITO, press one piece of oily latent;
(2) with activation tris (bipyridine) ruthenium complex hatch 6h, with deionized water rinsing to remove unreacted complex;
(3) sample is arranged in electrochemical reaction cell, adds the phosphate buffered solution of 50mM di-n-butyl ethanolamine, apply 1.3V current potential by three-electrode system, with highly sensitive CCD photographing unit, image is caught, obtain the electrochemiluminescence image shown in Fig. 4.
(1) on ITO, press one piece of oily latent;
(2) then hatch 3.5h with the tris (bipyridine) ruthenium complex of activation of dilution twice, with deionized water rinsing to remove unreacted complex;
(3) sample is arranged in electrochemical reaction cell, adds the phosphate buffered solution of 50mM di-n-butyl ethanolamine, apply 1.3V current potential by three-electrode system, with highly sensitive CCD photographing unit, image is caught, obtain the electrochemiluminescence image shown in Fig. 5.
(1) on ITO, press one piece of antiperspirant latent;
(2) with activation tris (bipyridine) ruthenium complex hatch 3.5h, with deionized water rinsing to remove unreacted complex;
(3) sample is arranged in electrochemical reaction cell, adds the phosphate buffered solution of 50mM di-n-butyl ethanolamine, apply 1.3V current potential by three-electrode system, with highly sensitive CCD photographing unit, image is caught, obtain the electrochemiluminescence image shown in Fig. 6.
Above-described embodiment is used for the present invention that explains, instead of limits the invention, and in the protection domain of spirit of the present invention and claim, any amendment and change that the present invention is made, all fall into protection scope of the present invention.
Claims (1)
1. a method that manifests latent fingerprint based on electrochemiluminescence label, the method realizes in electrochemiluminescence imaging system; Electrochemiluminescence imaging system comprises electrochemical reaction cell, constant potential control instrument and CCD photographing unit, electrochemical reaction cell comprises base and cell body, has groove on base, cell body hollow, be fixed on groove by O RunddichtringO and screw, cell body one side has an aperture; Constant potential control instrument comprises working electrode, to electrode and reference electrode, reference electrode is placed in aperture, wherein, working electrode is ITO, is platinum loop to electrode, reference electrode is Ag/AgCl electrode or Ag electrode; It is characterized in that, the method comprises the following steps:
(1) electrode pretreatment: by working electrode successively each ultrasonic cleaning 10-20min in acetone, ethanol and deionized water, then use deionized water cleaning down clean, dry up with argon;
(2) finger mark sample preparation: the finger mark on different objects is extracted with adhesive tape, then transfer on working electrode, form finger mark sample;
(3) the tris (bipyridine) ruthenium complex labelling finger mark activating with N-hydroxy-succinamide ester: by 50
the tris (bipyridine) ruthenium composite coated of N-hydroxy-succinamide ester activation, on finger mark sample, covers surface plate and prevents solution evaporation, more than at room temperature reacting 30min,, dries up with argon to remove unreacted complex with deionized water lavage specimens;
(4) electrochemiluminescence imaging: by the working electrode of above-mentioned processing, electrode and reference electrode are placed in to electrochemical reaction cell, then the reaction solution containing coreagent is added in electrochemical reaction cell, constant potential control instrument energising, CCD photographing unit gathers fingerprint image; Described reaction solution by adding 50mmol di-n-butyl ethanolamine and 0.15mol sodium chloride to form in every liter of phosphate buffered solution, and the pH of phosphate buffered solution is 7.4, and the current potential of constant potential control instrument is 1.3V.
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| CN103374132B (en) * | 2013-07-12 | 2015-04-08 | 中科院广州化学有限公司 | Preparation and application of metal ion directly induced fluorescent supramolecular gel |
| CN103543145B (en) * | 2013-10-18 | 2015-05-20 | 浙江大学 | Potential fingerprint imaging method based on chemiluminescence enzyme-linked immunoassay |
| CN103536297B (en) * | 2013-10-18 | 2015-06-17 | 浙江大学 | Immune colloidal gold based latent fingerprint imaging method |
| CN103536295B (en) * | 2013-10-18 | 2015-02-25 | 浙江大学 | Potential fingerprint imaging method based on electrochemiluminescence immunoassay |
| CN103536296B (en) * | 2013-10-18 | 2015-06-17 | 浙江大学 | Method of detecting human sweat secretion |
| CN103919558B (en) * | 2014-04-13 | 2016-03-16 | 中南民族大学 | Fluorescent quenching system is used for the method that latent fingerprint manifests |
| RU2604747C1 (en) * | 2015-06-04 | 2016-12-10 | Александр Сергеевич Козлов | Device and method for detection of traces of ridge pattern, device for application of tracer substance on surface if observing papillary pattern |
| CN109425597A (en) * | 2017-09-04 | 2019-03-05 | 中国科学院上海光学精密机械研究所 | The device and method of Sweat latent fingerprint detection on a kind of large format sample |
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