CN109283167B - Sensor array based on monolayer fluorescence sensing film and mode recognition of toxic gas by sensor array - Google Patents
Sensor array based on monolayer fluorescence sensing film and mode recognition of toxic gas by sensor array Download PDFInfo
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- CN109283167B CN109283167B CN201811300927.1A CN201811300927A CN109283167B CN 109283167 B CN109283167 B CN 109283167B CN 201811300927 A CN201811300927 A CN 201811300927A CN 109283167 B CN109283167 B CN 109283167B
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Abstract
The invention discloses a sensor array based on a monolayer fluorescence sensing film and mode identification of toxic gas, wherein the sensor array consists of 6 kinds of microarray monolayer fluorescence sensing films, each sensing film is formed by adsorbing ionic liquid or PEG 200 solution of different amphiphilic BODIPY derivatives at a hydrophilic micro area of a gold substrate with a hydrophilic and hydrophobic micro area, and the amphiphilic BODIPY derivatives are formed by self-assembling at a gas-liquid interface. According to the invention, the fluorescent response signals of each sensing film in the sensor array to the toxic gas are respectively collected, and the obtained multidimensional fluorescent signals are processed, so that the mode recognition of the toxic gases such as volatile organic compounds, nerve gases, explosives and the like is realized. The sensor array is low in cost, the micro-arrayed monolayer fluorescent sensing film is good in stability, long in service life and high in detection sensitivity, and the detection method is simple and easy to operate and wide in application range.
Description
Technical Field
The invention belongs to the technical field of chemical analysis and detection, and particularly relates to a sensor array based on a monolayer fluorescent sensing film and a method for detecting and identifying various toxic gases by adopting the array.
Background
In recent years, terrorism and environmental pollution seriously threaten life and production safety of people. Nerve gas, one of the organophosphorous compounds, was first synthesized in 1854 and developed into a widely used chemical warfare weapon in the past eighty years. Short-term skin absorption can lead to muscle paralysis, and in severe cases, suffocation of the human body can occur. In addition, with the general improvement of the production and living standards of human beings, environmental pollution becomes a factor which harms human health more and more, volatile organic compounds are common chemical substances widely existing in the air and mainly come from building materials, interior decoration materials and living and office supplies. For example: organic solvents, paints and aqueous coatings; incomplete combustion of household fuel and tobacco leaves, human body wastes, outdoor industrial waste gas, automobile exhaust, photochemical smog and the like. When the concentration of volatile organic compounds in indoor air is too high, acute poisoning is easily caused, and a light person can have headache, dizziness, cough, nausea, vomiting or a drunk shape; serious patients can have hepatotoxicity and even coma, and some of them can be life-threatening. Therefore, it is necessary to find a method for detecting different toxic gases with low cost, high efficiency and high sensitivity.
At present, methods for detecting different toxic gases at home and abroad mainly comprise semiconductor electronic sensors, gas chromatography, resistance sensors, surface acoustic wave sensors and the like, and the methods can realize detection of different toxic gases, but have some defects, such as complex operation, long time and high cost. Meanwhile, the single sensor has higher requirement on the selectivity of the sensor, and the application range of the sensor is greatly limited.
Disclosure of Invention
The invention aims to overcome the defects in the prior art, construct a sensor array based on a monolayer fluorescence sensing film, provide a new application for the sensor array and realize the mode identification of various toxic gases.
In view of the above, the sensor array based on the monolayer fluorescence sensing film provided by the invention comprises microarray monolayer fluorescence sensing films S1, S2, S3, S4, S5 and S6, wherein S1, S3 and S5 are microarray monolayer fluorescence sensing films formed by adsorption of an ionic liquid solution of a probe 1, an ionic liquid solution of a probe 2 and an ionic liquid solution of a probe 3 on a hydrophilic micro region of a gold substrate with hydrophilic and hydrophobic micro regions in sequence; s2, S4 and S6 are microarray monolayer fluorescence sensing films formed by adsorption of PEG 200 solution of probe 1, PEG 200 solution of probe 2 and PEG 200 solution of probe 3 on hydrophilic microdomains of a gold substrate with hydrophilic and hydrophobic microdomains in sequence;
the structural formula of the probe 1 is as follows:
the structural formula of the probe 2 is as follows:
the structural formula of the probe 3 is as follows:
the probe 1 of the invention is synthesized according to the method with the publication number of CN 107118228A; probe 2 was synthesized according to the method disclosed in publication No. CN 105524611 a; probe 3 is synthesized by the method of reference probe 2; gold substrates with hydrophilic and hydrophobic domains were prepared according to the method in publication No. CN 105524611 a.
In the microarray monolayer fluorescent sensing film S1, the concentration of the ionic liquid solution of the probe 1 is 5-25 mu mol/L; in the microarray monomolecular layer fluorescent sensing film S2, the concentration of PEG 200 solution of the probe 1 is 30-70 mu mol/L; in the microarray monomolecular layer fluorescent sensing film S3, the concentration of the ionic liquid solution of the probe 2 is 40-85 mu mol/L; in the microarray monomolecular layer fluorescent sensing film S4, the concentration of PEG 200 solution of the probe 2 is 35-75 mu mol/L; in the microarray monomolecular layer fluorescent sensing film S5, the concentration of the ionic liquid solution of the probe 3 is 5-25 mu mol/L; in the microarray monolayer fluorescent sensing film S6, the concentration of the PEG 200 solution of the probe 3 is 30 to 70 [ mu ] mol/L.
The ionic liquid is any one of 1-butyl-3-methylimidazole tetrafluoroborate, 1-butyl-3-methylimidazole hexafluoroborate and 1-octyl-3-methylimidazole chloride.
In the sensor array, the diameter of a liquid drop of a microarray formed by adsorption on the hydrophilic micro-area of the gold substrate is 25-100 mu m.
The invention discloses application of a sensor array based on a monomolecular layer fluorescence sensing film in distinguishing and detecting volatile organic matters, nerve poison gas and explosives, wherein the volatile organic matters are at least one of benzene, toluene, xylene, aniline, formaldehyde and acetaldehyde, the nerve poison gas is at least one of diethyl chlorophosphate, dimethyl methylphosphonate, diethyl methylphosphonate and triethyl phosphate, and the explosives are picric acid. The specific detection method comprises the following steps: and (3) carrying out fluorescence detection by using a fluorescence spectrometer, respectively collecting fluorescence response signals of the micro-arrayed monolayer fluorescence sensing film to toxic gases with different concentrations, and processing the obtained multidimensional fluorescence signals to obtain a standard model so as to carry out qualitative and quantitative analysis on the target object to be detected.
The invention has the following beneficial effects:
according to the invention, the fluorescent response signals of different micro-arrayed monomolecular layer fluorescent sensing films in the sensor array to toxic gases are respectively collected, and the obtained multidimensional fluorescent signals are processed, so that the mode recognition of toxic gases such as volatile organic compounds, nerve toxic gases, explosives and the like is realized. The sensor array is low in cost, the micro-arrayed monolayer fluorescent sensing film is good in stability and long in service life, high-sensitivity differential detection on various toxic gases can be realized, and the detection method is simple and easy to operate and wide in application range.
Drawings
FIG. 1 is a bar graph of the fluorescence signals of the sensor array of example 1 versus 11 toxic gases at immediate life-threatening and healthy concentrations.
FIG. 2 is a graph of principal component analysis of fluorescence signals of the sensor array of example 1 against 11 toxic gases at immediately life-threatening and healthy concentrations.
FIG. 3 is a graph of the principal components of the fluorescence signals of the sensor array of example 1 for picric acid, diethyl chlorophosphate, toluene, formaldehyde toxic gases at immediately life-threatening and healthy concentrations.
FIG. 4 is a graph of the principal components of the fluorescence signals of the sensor array of example 1 for picric acid, diethyl chlorophosphate, toluene, formaldehyde, and toxic gases at the highest allowable concentrations.
Detailed Description
The invention will be further described in detail with reference to the following figures and examples, but the scope of the invention is not limited to these examples.
Example 1
Dissolving the probe 1 in 1-butyl-3-methylimidazole tetrafluoroborate to prepare an ionic liquid solution of the probe 1 with the concentration of 20 mu mol/L; contacting an ionic liquid solution of the probe 1 with a gold substrate with a hydrophilic and hydrophobic micro-region to form an ordered pattern with the droplet diameter of 50 mu m in a hydrophilic mercaptoundecanoic acid monomolecular layer region, and preparing a microarray monomolecular layer fluorescence sensing film S1; dissolving the probe 2 in PEG 200 to prepare PEG 200 solution of the probe 2 at 65 mu mol/L; and (3) contacting the PEG 200 solution of the probe 2 with a gold substrate with a hydrophilic and hydrophobic micro-region to form an ordered pattern with the droplet diameter of 50 mu m in the hydrophilic mercaptoundecanoic acid monomolecular layer region, so as to prepare the microarray monomolecular layer fluorescence sensing film S2. Preparing an ionic liquid solution of 80 mu mol/L of probe 2 according to the method, and preparing a microarray monomolecular layer fluorescent sensing film S3; preparing 70 mu mol/L of PEG 200 solution of the probe 2, and preparing a microarray monomolecular layer fluorescent sensing film S4; preparing 20 mu mol/L of ionic liquid solution of the probe 3, and preparing a microarray monomolecular layer fluorescent sensing film S5; a PEG 200 solution of 65 mu mol/L of the probe 3 is prepared, and a microarray monomolecular layer fluorescence sensing film S6 is prepared. The 6 micro-arrayed monomolecular layer fluorescence sensing films form a sensor array.
Example 2
Detection of 11 toxic gases at immediate life-threatening and healthy concentrations using the sensor array of example 1
11 groups of micro-arrayed monomolecular layer fluorescence sensing films S1 (each group has 3 repetitions) were taken and placed in the air first, and the fluorescence emission intensity I of S1 was measured by FLS980 type single photon counting time-resolved fluorescence spectrometer0Then, the 11 groups of S1 were respectively placed in picric acid (1), diethyl chlorophosphate (2), dimethyl methylphosphonate (3), diethyl methylphosphonate (4), triethyl phosphate (5), benzene (6), toluene (7), xylene (8), formaldehyde (9), acetaldehyde (10) and aniline (11) vapors at concentrations immediately threatening life and health, the fluorescence emission intensity I corresponding to the lower system at a wavelength of 509nm was measured by a fluorescence spectrometer, and I-I was calculated0The value is obtained. Push buttonAccording to the method, S2, S3, S4, S5 and S6 are respectively adopted to carry out fluorescence detection on picric acid, diethyl chlorophosphate, dimethyl methylphosphonate, diethyl methylphosphonate, triethyl phosphate, benzene, toluene, xylene, formaldehyde, acetaldehyde and aniline steam which are in immediate threat to life and health.
Subjecting the thus-obtained I-I0The values were plotted as a histogram and subjected to principal component analysis by SPSS software, the results are shown in fig. 1 and 2, the points in fig. 2 represent the results obtained by principal component analysis of the difference in fluorescence signals before and after addition of toxic gas to the sensor array, each point on the graph represents one toxic gas, and the points of different shapes represent different toxic gases. As can be seen from fig. 2, the different shaped dots can be well distinguished, which means that the sensor array can well distinguish 11 toxic gases with concentration immediately threatening life and health, and can well distinguish the same series of diethyl chlorophosphate, dimethyl methylphosphonate, diethyl methylphosphonate and triethyl phosphate; the method has good distinction for benzene, toluene and xylene in the same series; the method can be used for distinguishing formaldehyde and acetaldehyde in the same series.
8 groups of micro-arrayed monomolecular layer fluorescence sensing films S1 (each group has 3 repetitions) were taken and placed in the air first, and the fluorescence emission intensity I of S1 was measured by FLS980 type single photon counting time-resolved fluorescence spectrometer0Then, the 8 groups of S1 were placed in picric acid (1), diethyl chlorophosphate (2), toluene (7) and formaldehyde (9) vapor with immediate life and health threatening concentration and highest allowable concentration, respectively, fluorescence emission intensity I corresponding to the lower system at 509nm was measured by fluorescence spectrometer, and I-I was calculated0The value is obtained. According to the method, picric acid, diethyl chlorophosphate, toluene and formaldehyde steam with the highest allowable concentration are subjected to fluorescence detection by respectively adopting S2, S3, S4, S5 and S6.
Subjecting the thus-obtained I-I0The values were analyzed for principal components by SPSS software, and the results are shown in FIGS. 3 and 4. As can be seen from FIGS. 3 and 4, the different shaped dots are well distinguishable, indicating that the sensor array is well able to distinguish picric acid, diethyl chlorophosphate, at the highest permissible concentration, between immediate life-threatening and healthy concentrationsToluene, formaldehyde toxic gases.
Claims (7)
1. A sensor array based on monolayer fluorescence sensing film is characterized in that: the sensor array consists of microarray monolayer fluorescence sensing films S1, S2, S3, S4, S5 and S6, wherein S1, S3 and S5 are microarray monolayer fluorescence sensing films formed by adsorption of an ionic liquid solution of a probe 1, an ionic liquid solution of a probe 2 and an ionic liquid solution of a probe 3 on a hydrophilic micro area of a gold substrate with a hydrophilic and hydrophobic micro area in sequence; s2, S4 and S6 are microarray monolayer fluorescence sensing films formed by adsorption of PEG 200 solution of probe 1, PEG 200 solution of probe 2 and PEG 200 solution of probe 3 on hydrophilic microdomains of a gold substrate with hydrophilic and hydrophobic microdomains in sequence;
the structural formula of the probe 1 is as follows:
；
the structural formula of the probe 2 is as follows:
；
the structural formula of the probe 3 is as follows:
；
the ionic liquid is any one of 1-butyl-3-methylimidazole tetrafluoroborate, 1-butyl-3-methylimidazole hexafluoroborate and 1-octyl-3-methylimidazole chloride.
2. The monolayer fluorescent sensing film-based sensor array of claim 1, wherein: in the microarray monolayer fluorescent sensing film S1, the concentration of the ionic liquid solution of the probe 1 is 5-25 mu mol/L; in the microarray monolayer fluorescent sensing film S2, the concentration of a PEG 200 solution of a probe 1 is 30-70 mu mol/L; in the microarray monolayer fluorescent sensing film S3, the concentration of the ionic liquid solution of the probe 2 is 40-85 mu mol/L; in the microarray monolayer fluorescent sensing film S4, the concentration of PEG 200 solution of the probe 2 is 35-75 mu mol/L; in the microarray monolayer fluorescent sensing film S5, the concentration of the ionic liquid solution of the probe 3 is 5-25 mu mol/L; in the microarray monolayer fluorescent sensing film S6, the concentration of the PEG 200 solution of the probe 3 is 30-70 mu mol/L.
3. The monolayer fluorescent sensing film-based sensor array of claim 1 or 2, wherein: the diameter of the liquid drop of the microarray formed by adsorption on the hydrophilic micro-area of the gold substrate is 25-100 mu m.
4. The use of the monolayer fluorescent sensing film-based sensor array of claim 1 for the differential detection of volatile organic compounds, nerve gases, explosives.
5. The application of the sensor array based on the monolayer fluorescence sensing film in the detection of volatile organic compounds, nerve gases and explosives in the differentiation of the volatile organic compounds, nerve gases and explosives is characterized in that: the volatile organic compound is at least one of benzene, toluene, xylene, aniline, formaldehyde and acetaldehyde.
6. The application of the sensor array based on the monolayer fluorescence sensing film in the distinguishing detection of volatile organic compounds, nerve gases and explosives, which is characterized in that: the nerve gas is at least one of diethyl chlorophosphate, dimethyl methylphosphonate, diethyl methylphosphonate and triethyl phosphate.
7. The application of the sensor array based on the monolayer fluorescence sensing film in the distinguishing detection of volatile organic compounds, nerve gases and explosives, which is characterized in that: the explosive is picric acid.
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