CN104614437B - Electrode spacing optimization method for carbon nanotube three-electrode gas sensor - Google Patents
Electrode spacing optimization method for carbon nanotube three-electrode gas sensor Download PDFInfo
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- CN104614437B CN104614437B CN201510081873.4A CN201510081873A CN104614437B CN 104614437 B CN104614437 B CN 104614437B CN 201510081873 A CN201510081873 A CN 201510081873A CN 104614437 B CN104614437 B CN 104614437B
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Abstract
The invention discloses an electrode spacing optimization method for a carbon nanotube three-electrode gas sensor. The method is used for optimizing the electrode spacing between the first electrode and the second electrode and between the second electrode and the third electrode of the carbon nanotube three-electrode gas sensor. The method comprises the following steps: designing the electrode spacing, constructing a sensor array consisting of different electrode spacing sensors, performing concentration detection on gas of known concentration by using the constructed sensor array, constructing a database for the electrode spacing of the sensor array and the corresponding gas detection result, constructing a quantitative analysis model for the detected gas concentration, and optimizing the electrode spacing of each composition sensor in the sensor array, so that the optimal electrode spacing aiming at a single sensor which corresponds to different detection gases and the optimal electrode spacing aiming at each composition sensor in the sensor array which corresponds to the mixed gas can be effectively obtained. Therefore, high detection sensitivity can be obtained.
Description
Technical field
The invention belongs to gas sensing field, and in particular to a kind of die opening of three electrode gas sensor of CNT is excellent
Change method.
Background technology
In recent years, with the continuous development of carbon nanotechnology, the air-sensitive constituted as sensitive material with CNT, it is temperature sensitive and
Moisture sensor is continued to bring out.CN102081073A discloses a kind of three electrode sensor of micro-nano carbon nano-tube film, adopts
Detection is constituted by three mutually isolated electrodes of insulation column (first electrode inner surface is distributed the substrate of carbon nano-tube film)
The sensor of gas, temperature and humidity；CN102095791B proposes carbon nano-tube film three by disclosed in CN102081073A
The method that electrode sensor composition sensor array realizes the detection of multicomponent mixed gas concentration.
As carbon nano tube sensor has the unique advantages such as running voltage is low, overall dimensions are little so which is in biological, change
The numerous areas such as, machinery, aviation have broad application prospects.But, current three electrode sensor of CNT exists
Work under specific several die openings, for the still no specific aim structural support of different detected gas, it is difficult to obtain higher
Detection sensitivity；Additionally, for the sensor array being made up of multiple sensors is detected to mixed gas, multiple sensors
Respectively it is combined using which kind of die opening and can obtains optimal Detection results and need clearly.Therefore, urgently need a kind of method
The die opening of three electrode sensor of CNT can be optimized, to improve detection sensitivity, accelerate sensor application
Promote.
The content of the invention
The problems referred to above and deficiency that the present invention is present for three electrode sensor of existing CNT, there is provided one kind can be used for
Three electrode sensor of Single Carbon Nanotubes and three electrode sensor of multiple CNTs are respectively constituted when combining to form sensor array
The die opening optimization method of sensor, can effectively obtain the optimal interpolar for single sensor corresponding to different detected gas
Away from, and for the optimal die opening of each composition sensor in sensor array corresponding to mixed gas, so as to obtain higher inspection
Survey sensitivity.
To achieve these goals, the technical scheme is that：
The die opening optimization method of three electrode gas sensor of CNT, to three electrode gas sensor of CNT
First electrode is optimized with second electrode, second electrode and the die opening of the 3rd electrode, three electrode gas of the CNT
The first electrode inner surface distribution carbon nano-tube film substrate of sensor, second electrode is the extraction pole pole plate for being provided with fairlead,
3rd electrode is collector, and three electrodes are mutually isolated by insulation column, the die opening scope of adjacent two electrode in three electrodes
For 50 μm～250 μm, it is characterised in that using following optimization step：
1) design die opening
In the sensor array be made up of three electrode gas sensor of n CNT, the first electrode of i-th sensor
Die opening with second electrode is di1, second electrode is d with the die opening of the 3rd electrodei2, wherein, i=1,2 ... ..., n work as n
For 1 when, then refer to three electrode gas sensor of Single Carbon Nanotubes, the d of each sensori1And di2Between not having equidistantly and not etc.
Away from two kinds of situations：
Equidistantly：di1With di2It is equal, di1Or di2Start to be incremented by with step-length S from 50 μm, until di1Or di2More than or equal to 250
μm, S is the arbitrary integer between 0 μm -200 μm；
Unequal-interval：di1With di2It is unequal, di1Start from 50 μm with step-length S1It is incremented by, until di1More than or equal to 250 μm,
di2Start from 50 μm with step-length S2It is incremented by, until di2More than or equal to 250 μm, S1And S2It is any whole between 0 μm -200 μm
Number, works as di1When taking a value in aforementioned value, di2Take and di1Different values；
2) build by different die opening sensor groups into sensor array
The mixed gas constituted for the tested gas of one pack system or by R kind components, select number of probes n, n >=R, adopt
Step 1) the middle die opening for designing, three electrode gas of the CNT biography of m groups n individual not equal pitch and unequal-interval is built respectively
Sensor, forms the three electrode gas sensor array of CNT of m groups difference die opening, all sensings in m group sensor arrays
The d of devicei1And di2Step 1) in design die opening is all possible exhaustive or selection empirically；
3) Concentration Testing is carried out to concentration known gas with building sensor array
The single-component gas or multicomponent mixed gas sample of various variable concentrations are prepared using calibrating gas, using by step
The three electrode gas sensor array column split of m groups CNT of the rapid different die openings for 2) building is detected, is obtained each tested
The gas discharge ion flow valuve of gas sample；
4) die opening and its correspondence gas detecting result database of sensor array are set up
With the d of each composition sensor in all three electrode gas sensor arrays of m groups CNTi1And di2, detected gas
The gas discharge ion flow valuve and the concentration of tested gas that sample is obtained sets up die opening and its correspondence gas detecting number of results
According to storehouse；
5) set up tested gas concentration quantitative model
Using support vector machine method, with step 4) in set up data base tested gas discharge ion flow valuve as input, with
Its correspondence gas concentration is output, sets up tested gas concentration quantitative model；
6) optimize the die opening of each composition sensor in sensor array
Using by step 5) the tested gas concentration quantitative model set up is dense to the gas of all tested gas samples
Degree is analyzed, and obtains the detectable concentration of tested gas；The detectable concentration of tested gas corresponding actual concentrations are asked into poor
Value, then divided by the actual concentrations of tested gas, obtain the relative error for detecting the gas；Using particle swarm optimization algorithm, with quilt
The minimum target of relative error of gas detecting is surveyed, to by step 2) the three electrode gas sensor array of m groups CNT that builds
The d of each composition sensor in rowi1And di2It is in optimized selection, it is final to obtain three electrode gas of CNT for detecting the gas
The optimal die opening of each sensor in sensor array.
Three electrode gas sensor of CNT can be replaced three electrode temperature sensors of CNT or CNT three
Electrode humidity sensor, for detection temperature or humidity.
The invention has the advantages that：
1) extensibility is strong：The method can be to detection single-component gas and three electrode gas of CNT of multicomponent gases
In sensor array, the die opening of each sensor is optimized, while also extending to the temperature and humidity sensing being made up of which
Device.
2) associativity is good：For certain specific gas, the gas sample that certain concentration may be selected is optimized, also optional
The gas sample for selecting various variable concentrations is optimized, and gas sample is simple, and multiple gases can be analyzed, and associativity is good.
3) motility is strong：Can be using in addition to support vector machine, other be various when setting up tested gas concentration quantitative model
Quantitative analysis method, by obtaining the optimal Quantitative Analysis Model of the method to its parameter optimization, with very strong motility.
Description of the drawings
Fig. 1 is optimization method flow chart of the present invention；
Fig. 2 is detection NO and SO in the embodiment of the present invention2The relative error of mixed gas.
Specific embodiment
Detailed technology scheme of the present invention is introduced below in conjunction with accompanying drawing：
The die opening optimization method of three electrode gas sensor of CNT, to three electrode gas sensor array of CNT
In row, the first electrode of each composition sensor is optimized with second electrode, second electrode and the die opening of the 3rd electrode, described
The first electrode inner surface distribution carbon nano-tube film substrate of three electrode gas sensor of CNT, second electrode are drawn for being provided with
The extraction pole pole plate for portalling, the 3rd electrode are collector, and three electrodes are mutually isolated by insulation column, adjacent two in three electrodes
The die opening scope of electrode is 50 μm～250 μm.Which adopts following optimization step：
1) design die opening
In the sensor array be made up of three electrode gas sensor of n CNT, the first electrode of i-th sensor
Die opening with second electrode is di1, second electrode is d with the die opening of the 3rd electrodei2, wherein, i=1,2 ... ..., n work as n
For 1 when, then refer to three electrode gas sensor of Single Carbon Nanotubes, the d of each sensori1And di2Between not having equidistantly and not etc.
Away from two kinds of situations：
Equidistantly：di1With di2It is equal, di1Or di2Start to be incremented by with step-length S from 50 μm, until di1Or di2More than or equal to 250
μm, S is the arbitrary integer between 0 μm -200 μm；
Unequal-interval：di1With di2It is unequal, di1Start from 50 μm with step-length S1It is incremented by, until di1More than or equal to 250 μm,
di2Start from 50 μm with step-length S2It is incremented by, until di2More than or equal to 250 μm, S1And S2It is any whole between 0 μm -200 μm
Number, works as di1When taking a value in aforementioned value, di2Take and di1Different values；
2) build by different die opening sensor groups into sensor array
The mixed gas constituted for the tested gas of one pack system or by R kind components, select number of probes n, n >=R, adopt
Step 1) the middle die opening for designing, three electrode gas of the CNT biography of m groups n individual not equal pitch and unequal-interval is built respectively
Sensor, forms the three electrode gas sensor array of CNT of m groups difference die opening, all sensings in m group sensor arrays
The d of devicei1And di2Step 1) in design die opening is all possible exhaustive or selection empirically；
3) Concentration Testing is carried out to concentration known gas with building sensor array
The single-component gas or multicomponent mixed gas sample of various variable concentrations are prepared using calibrating gas, using by step
The three electrode gas sensor array column split of m groups CNT of the rapid different die openings for 2) building is detected, is obtained each tested
The gas discharge ion flow valuve of gas sample；
4) die opening and its correspondence gas detecting result database of sensor array are set up
With the d of each composition sensor in all three electrode gas sensor arrays of m groups CNTi1And di2, detected gas
The gas discharge ion flow valuve and the concentration of tested gas that sample is obtained sets up die opening and its correspondence gas detecting number of results
According to storehouse；
5) set up tested gas concentration quantitative model
Using support vector machine method, with step 4) in set up data base tested gas discharge ion flow valuve as input, with
Its correspondence gas concentration is output, sets up tested gas concentration quantitative model；
6) optimize the die opening of each composition sensor in sensor array
Using by step 5) the tested gas concentration quantitative model set up is dense to the gas of all tested gas samples
Degree is analyzed, and obtains the detectable concentration of tested gas；The detectable concentration of tested gas corresponding actual concentrations are asked into poor
Value, then divided by the actual concentrations of tested gas, obtain the relative error for detecting the gas；Using particle swarm optimization algorithm, with quilt
The minimum target of relative error of gas detecting is surveyed, to by step 2) the three electrode gas sensor array of m groups CNT that builds
The d of each composition sensor in rowi1And di2It is in optimized selection, it is final to obtain three electrode gas of CNT for detecting the gas
The optimal die opening of each sensor in sensor array.
For the tested gas of one pack system, can be sensed from three electrode gas of Single Carbon Nanotubes of multiple different die openings
Device detected to this kind of gas sample of various variable concentrations, the minimum three electrode gas sensor of CNT of detection error
Corresponding die opening is the die opening for being best suitable for the gas detecting；Three electrode gas sensor of multiple CNTs can also be adopted
Sensor array is constituted, this kind of gas sample to various variable concentrations is grouped and is detected, the minimum carbon nanometer of detection error
The corresponding die opening of three electrode gas sensor of pipe is the die opening for being best suitable for the gas detecting.
To multicomponent mixed gas, need structure sensor array to be detected, generally, there are several components to constitute
Mixed gas, it is necessary to constitute sensor with the three electrode gas sensor of CNT more than or equal to mixing gas component quantity
Array.Embodiment is only with nitric oxide (NO) and sulfur dioxide (SO2) mixed gas as a example by illustrate, the group of mixed gas
Dosis refracta can extend.
As shown in figure 1, the die opening optimization method of three electrode gas sensor array of CNT adopts following steps：
1) design die opening
In the sensor array be made up of 2 sensors, if the pole of wherein the 1st sensor first electrode and second electrode
Spacing is d11, second electrode and the 3rd electrode die opening be d12；The interpolar of the 2nd sensor first electrode and second electrode
Away from for d21, second electrode and the 3rd electrode die opening be d22, two die openings of each sensor are had equidistantly and
Two kinds of situations of spacing：
Equidistantly：Two die openings for constituting the single sensor of sensor array are equal, d11、d12、d21And d22From 50
μm start to be incremented by with 30 μm of step-length, form 50 μm, 80 μm, 110 μm, 140 μm, 170 μm, 200 μm, 230 μm, 250 μm and amount to 8
Die opening.
Unequal-interval：Two die openings for constituting the single sensor of sensor array are unequal, such as d11Open from 50 μm
Begin incremental with 30 μm of step-length, form 50 μm, 80 μm, 110 μm, 140 μm, 170 μm, 200 μm, 230 μm, 250 μm and amount to 8 d11
Value；d12Also start to be incremented by with 30 μm of step-length from 50 μm, be similarly formed 50 μm, 80 μm, 110 μm, 140 μm, 170 μm, 200 μm, 230
μm, 250 μm amount to 8 d12Value；In theory, work as di1、di2When taking above-mentioned different value and being combined, possible combination has 56
Kind, wherein, i=1,2.
It is for single sensor, above-mentioned equidistantly to form totally 64 kinds of different die opening combinations with unequal-interval.
2) build by different die opening sensor groups into sensor array
For NO and SO2Mixed gas, select number of probes be 2, according to existing experiment experience, from step 1) design
Die opening in, choose 6 couples of different di1And di2Combination, build 6 groups by 2 sensor groups into three electrode of CNT
Gas sensor array, wherein, di1With di2Combination be shown in Table 1：
The combination of 16 groups of sensor array difference die openings of table
| Group | d11/μm | d12/μm | d21/μm | d22/μm |
| First group | 50 | 150 | 150 | 150 |
| Second group | 50 | 180 | 180 | 180 |
| 3rd group | 100 | 180 | 100 | 150 |
| 4th group | 100 | 200 | 180 | 200 |
| 5th group | 150 | 180 | 180 | 180 |
| 6th group | 150 | 200 | 200 | 200 |
3) Concentration Testing is carried out to concentration known gas with building sensor array
The NO and SO of five kinds of variable concentrations are prepared using calibrating gas2Mixed gas sample, its proportioning refer to table 2.Using
6 groups of CNTs, the three electrode gas sensor array built in table 1 NO and SO respectively to 5 kinds of variable concentrations2Mixed gas
Sample detected, obtains the gas discharge ion flow valuve of 30 groups of 60 tested gas samples altogether.
The NO and SO of 25 kinds of variable concentrations of table2Mixed gas
| Sequence number | NO/ppm | SO2/ppm |
| 1 | 500 | 500 |
| 2 | 500 | 800 |
| 3 | 500 | 1000 |
| 4 | 800 | 800 |
| 5 | 800 | 1100 |
4) die opening and its correspondence gas detecting result database of sensor array are set up
By the d of each sensor in three electrode gas sensor array of every group of CNTi1And di2, detected gas sample obtains
The gas discharge ion flow valuve for obtaining and the concentration of tested gas set up die opening and its correspondence gas detecting result database；
5) set up tested gas concentration quantitative model
Ignore impact of the temperature and humidity to gas detecting, using support vector machine method, from gaussian kernel function, with step
4), in the data base for setting up, detect NO and SO2The electric discharge that each three electrode gas sensor of CNT of mixed gas sample is obtained
Ion flow valuve is input, with its tested gas concentration of correspondence as output, sets up tested gas concentration quantitative model；
The die opening of each composition sensor in step 6 optimization sensor array
Using by step 5) the tested gas concentration quantitative model set up is to NO and SO in 30 groups of tested gas samples2
The concentration of gas is analyzed, and obtains NO and SO2Detectable concentration；Ask for NO and SO2The relative error of gas detecting, such as Fig. 2 institutes
Show；Using particle swarm optimization algorithm, with the minimum target of tested gas detecting error, to by step 2) 6 groups of carbon nanometers building
Each d in three electrode gas sensor array of pipei1And di2It is in optimized selection, it is found that the 5th group of die opening combines the sensing to be formed
Device array detection NO and SO2The relative error of mixed gas is minimum, therefore, it is final to obtain detection NO and SO2Mixed gas adopt carbon
In three electrode gas sensor array of nanotube, optimal die opening d of two sensorsi1And di2Respectively：150μm、180μm
With 180 μm, 180 μm.
The die opening optimization method of the three electrode gas sensor of CNT that this patent is proposed, is equally applicable to carbon nanometer
The optimization of three electrode temperature of pipe and humidity sensor die opening, as long as substituted with three electrode temperature of CNT or humidity sensor
Three electrode gas sensor of CNT constitutes sensor array, and the temperature and humidity data that detection is obtained are included step 4) build
In vertical data base, then execution step 5) and step 6).
Step 5) in support vector machine method can also be neutral net, least square regression, kernel method etc. other recurrence
Method；Step 6) in particle swarm optimization algorithm can also be other optimized algorithms such as ant colony optimization algorithm, genetic algorithm.
Claims (2)
1. the die opening optimization method of three electrode gas sensor of CNT, to three electrode gas sensor of CNT
One electrode is optimized with second electrode, second electrode and the die opening of the 3rd electrode, and three electrode gas of the CNT are passed
The first electrode inner surface distribution carbon nano-tube film substrate of sensor, second electrode is the extraction pole pole plate for being provided with fairlead, the
Three electrodes are collector, and three electrodes are mutually isolated by insulation column, and in three electrodes, the die opening scope of adjacent two electrode is
50 μm～250 μm, it is characterised in that using following optimization step：
1) design die opening
In the sensor array be made up of three electrode gas sensor of n CNT, the first electrode of i-th sensor and the
The die opening of two electrodes is di1, second electrode is d with the die opening of the 3rd electrodei2, wherein, i=1,2 ... ..., n, when n is 1
When, then refer to three electrode gas sensor of Single Carbon Nanotubes, the d of each sensori1And di2There is equidistant and unequal-interval two
The situation of kind：
Equidistantly：di1With di2It is equal, di1Or di2Start to be incremented by with step-length S from 50 μm, until di1Or di2Equal to 250 μm, S is 0 μ
Arbitrary integer between m-200 μm；
Unequal-interval：di1With di2It is unequal, di1Start from 50 μm with step-length S1It is incremented by, until di1Equal to 250 μm, di2From 50 μm
Start with step-length S2It is incremented by, until di2Equal to 250 μm, S1And S2The arbitrary integer being between 0 μm -200 μm, works as di1Take aforementioned
When one in numerical value is worth, di2Take and di1Different values；
2) build by different die opening sensor groups into sensor array
The mixed gas constituted for the tested gas of one pack system or by R kind components, select number of probes n, n >=R, using step
1) die opening of design in, builds three electrode gas of the CNT sensing of m groups n individual not equal pitch and unequal-interval respectively
Device, forms the three electrode gas sensor array of CNT of m groups difference die opening, all the sensors in m group sensor arrays
Di1And di2Step 1) in design die opening is all possible exhaustive or selection empirically；
3) Concentration Testing is carried out to concentration known gas with building sensor array
The single-component gas or multicomponent mixed gas sample of various variable concentrations are prepared using calibrating gas, using by step 2)
The three electrode gas sensor array column split of m groups CNT of the different die openings of structure detected, obtains each tested gas
The gas discharge ion flow valuve of sample；
4) die opening and its correspondence gas detecting result database of sensor array are set up
With the d of each composition sensor in all three electrode gas sensor arrays of m groups CNTi1And di2, detected gas sample
The concentration of the gas discharge ion flow valuve of acquisition and tested gas sets up die opening and its correspondence gas detecting result database；
5) set up tested gas concentration quantitative model
Using support vector machine method, with step 4) tested gas discharge ion flow valuve is as input, right with which in set up data base
Gas concentration is answered for exporting, tested gas concentration quantitative model is set up；
6) optimize the die opening of each composition sensor in sensor array
Using by step 5) the tested gas concentration quantitative model set up enters to the gas concentration of all tested gas samples
Row analysis, obtains the detectable concentration of tested gas；The detectable concentration of tested gas corresponding actual concentrations are sought into difference, then
Divided by the actual concentrations of tested gas, the relative error for detecting the gas is obtained；Using particle swarm optimization algorithm, with tested gas
The minimum target of relative error of detection, to by step 2) it is each in the three electrode gas sensor array of m groups CNT that builds
The d of composition sensori1And di2It is in optimized selection, it is final to obtain the three electrode gas sensor of CNT for detecting the gas
The optimal die opening of each sensor in array.
2. the die opening optimization method of three electrode gas sensor of CNT according to claim 1, it is characterised in that：
Three electrode gas sensor of CNT can be replaced three electrode humidity of three electrode temperature sensors of CNT or CNT
Sensor, for detection temperature or humidity.
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| CN106250632B (en) * | 2016-08-03 | 2019-05-24 | 西安交通大学 | A kind of structural optimization method of three electrodes ionization type carbon nanotube gas sensor |
| CN114018326B (en) * | 2021-11-03 | 2024-04-16 | 国网湖南省电力有限公司 | Low-voltage transformer area environment multi-parameter detection method based on microsystem sensor array |
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