CN104614437A - Electrode spacing optimization method for carbon nanotube three-electrode gas sensor - Google Patents
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- CN104614437A CN104614437A CN201510081873.4A CN201510081873A CN104614437A CN 104614437 A CN104614437 A CN 104614437A CN 201510081873 A CN201510081873 A CN 201510081873A CN 104614437 A CN104614437 A CN 104614437A
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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, be specifically related to a kind of die opening optimization method of carbon nano-tube three electrode gas sensor.
Background technology
In recent years, along with the development of carbon nanometer technology, be that air-sensitive, the temperature sensitive and moisture sensor that sensitive material is formed continues to bring out with carbon nano-tube.CN102081073A discloses a kind of micro-nano carbon nano-tube film three electrode sensor, adopts three electrodes (substrate of the first electrode inside surface distribution carbon nano-tube film) by insulation column is mutually isolated to constitute the sensor detecting gas, temperature and humidity; CN102095791B proposes carbon nano-tube film three electrode sensor disclosed in CN102081073A and forms the method that sensor array realizes the detection of polycomponent mixed gas concentration.
Because carbon nano tube sensor has the unique advantages such as operating voltage is low, overall dimensions is little, it is had broad application prospects at the numerous areas such as biology, chemistry, machinery, aviation.But current carbon nano-tube three electrode sensor all works under specific several die opening, does not still have specific aim support structure for different detection gas, is difficult to obtain higher detection sensitivity; In addition, detect mixed gas for the sensor array be made up of multiple sensor, which kind of die opening multiple sensor respectively adopts carry out combining the Detection results that can obtain the best and need clearly.Therefore, urgently needing a kind of method can be optimized the die opening of carbon nano-tube three electrode sensor, to improve detection sensitivity, accelerates the popularization of sensor application.
Summary of the invention
The present invention is directed to the problems referred to above and the deficiency of the existence of existing carbon nano-tube three electrode sensor, a kind of die opening optimization method that can be used for respectively forming when Single Carbon Nanotubes three electrode sensor and multiple carbon nano-tube three electrode sensor are combined to form sensor array sensor is provided, effectively can obtain the best die opening detecting single-sensor corresponding to gas for difference, with the best die opening of composition sensor each in sensor array corresponding to mixed gas, thus obtain higher detection sensitivity.
To achieve these goals, technical scheme of the present invention is:
The die opening optimization method of carbon nano-tube three electrode gas sensor, first electrode of carbon nano-tube three electrode gas sensor and the second electrode, the second electrode and three electrode die opening are optimized, first electrode inside surface distribution carbon nano-tube film substrate of described carbon nano-tube three electrode gas sensor, second electrode is the extraction pole pole plate being provided with fairlead, 3rd electrode is collector, three electrodes are mutually isolated by insulation column, in three electrodes, the die opening scope of adjacent two electrodes is 50 μm ~ 250 μm, it is characterized in that adopting following Optimization Steps:
1) die opening is designed
In the sensor array be made up of n carbon nano-tube three electrode gas sensor, the first electrode of i-th sensor and the die opening of the second electrode are d
i1, the second electrode and three electrode die opening are d
i2, wherein, i=1,2 ..., n, when n is 1, then refers to Single Carbon Nanotubes three electrode gas sensor, the d of each sensor
i1and d
i2there are equidistant and unequal-interval two kinds of situations:
Equidistant: d
i1with d
i2equal, d
i1or d
i2increase progressively with step-length S from 50 μm, until d
i1or d
i2be more than or equal to 250 μm, S is the arbitrary integer between 0 μm-200 μm;
Unequal-interval: d
i1with d
i2unequal, d
i1with step-length S from 50 μm
1increase progressively, until d
i1be more than or equal to 250 μm, d
i2with step-length S from 50 μm
2increase progressively, until d
i2be more than or equal to 250 μm, S
1and S
2be the arbitrary integer between 0 μm-200 μm, work as d
i1when getting a value in aforementioned value, d
i2get and d
i1different values;
2) sensor array be made up of different die opening sensor is built
For the tested gas of single component or the mixed gas that is made up of R kind component, selected number of probes n, n>=R, adopt step 1) the middle die opening designed, build the carbon nano-tube three electrode gas sensor of m group n individual not equal pitch and unequal-interval respectively, form the carbon nano-tube three electrode gas sensor array of the different die opening of m group, the d of all the sensors in m group sensor array
i1and d
i2step 1) in all possible exhaustive or selection empirically of design die opening;
3) with building sensor array, Concentration Testing is carried out to concentration known gas
Calibrating gas is adopted to prepare single-component gas or the polycomponent mixed gas sample of multiple variable concentrations, adopting by step 2) the m group carbon nano-tube three electrode gas sensor array column split of different die openings that builds detects, and obtains the gas discharge ion flow valuve of each tested gas sample;
4) die opening of sensor array and corresponding gas detect result database thereof is set up
With the d of composition sensor each in all m group carbon nano-tube three electrode gas sensor arraies
i1and d
i2, detect gas discharge ion flow valuve that gas sample obtains and the concentration of tested gas sets up die opening and corresponding gas detect result database thereof;
5) tested gas concentration quantitative model is set up
Adopting support vector machine method, with step 4) tested gas discharge ion flow valuve is input in institute's building database, with its corresponding gas concentration for exporting, sets up tested gas concentration quantitative model;
6) die opening of each composition sensor in sensor array is optimized
Adopting by step 5) gas concentration of tested gas concentration quantitative model to all tested gas samples set up analyze, and obtains the detectable concentration of tested gas; Actual concentrations corresponding with it for the detectable concentration of tested gas is asked difference, then divided by the actual concentrations of tested gas, obtains the relative error detecting this gas; Adopt particle swarm optimization algorithm, minimum for target with the relative error of tested gas detect, to by step 2) each d forming sensor in the m group carbon nano-tube three electrode gas sensor array that builds
i1and d
i2be in optimized selection, the final best die opening obtaining each sensor in the carbon nano-tube three electrode gas sensor array detecting this gas.
Carbon nano-tube three electrode gas sensor can be replaced carbon nano-tube three electrode temperature sensors or carbon nano-tube three electrode humidity sensor, for detected temperatures or humidity.
The present invention has following beneficial effect:
1) extensibility is strong: the method can be optimized the die opening of each sensor in the carbon nano-tube three electrode gas sensor array detecting single-component gas and multicomponent gas, also extends to the temperature and moisture sensors be made up of it simultaneously.
2) associativity is good: for certain specific gas, and the gas sample of certain concentration can be selected to be optimized, and also the gas sample of choosing multiple variable concentrations is optimized, and gas sample is simple, and can analyze multiple gases, associativity is good.
3) dirigibility is strong: can adopt other multiple quantitative analysis method except support vector machine when setting up tested gas concentration quantitative model, by obtaining the best Quantitative Analysis Model of the method to its parameter optimization, has very strong dirigibility.
Accompanying drawing explanation
Fig. 1 is optimization method process flow diagram of the present invention;
Fig. 2 detects NO and SO in the embodiment of the present invention
2the relative error of mixed gas.
Embodiment
Detailed technology scheme of the present invention is introduced below in conjunction with accompanying drawing:
The die opening optimization method of carbon nano-tube three electrode gas sensor, the first electrode and the second electrode, the second electrode and three electrode die opening that respectively form sensor in carbon nano-tube three electrode gas sensor array are optimized, first electrode inside surface distribution carbon nano-tube film substrate of described carbon nano-tube three electrode gas sensor, second electrode is the extraction pole pole plate being provided with fairlead, 3rd electrode is collector, three electrodes are mutually isolated by insulation column, and in three electrodes, the die opening scope of adjacent two electrodes is 50 μm ~ 250 μm.It adopts following Optimization Steps:
1) die opening is designed
In the sensor array be made up of n carbon nano-tube three electrode gas sensor, the first electrode of i-th sensor and the die opening of the second electrode are d
i1, the second electrode and three electrode die opening are d
i2, wherein, i=1,2 ..., n, when n is 1, then refers to Single Carbon Nanotubes three electrode gas sensor, the d of each sensor
i1and d
i2there are equidistant and unequal-interval two kinds of situations:
Equidistant: d
i1with d
i2equal, d
i1or d
i2increase progressively with step-length S from 50 μm, until d
i1or d
i2be more than or equal to 250 μm, S is the arbitrary integer between 0 μm-200 μm;
Unequal-interval: d
i1with d
i2unequal, d
i1with step-length S from 50 μm
1increase progressively, until d
i1be more than or equal to 250 μm, d
i2with step-length S from 50 μm
2increase progressively, until d
i2be more than or equal to 250 μm, S
1and S
2be the arbitrary integer between 0 μm-200 μm, work as d
i1when getting a value in aforementioned value, d
i2get and d
i1different values;
2) sensor array be made up of different die opening sensor is built
For the tested gas of single component or the mixed gas that is made up of R kind component, selected number of probes n, n>=R, adopt step 1) the middle die opening designed, build the carbon nano-tube three electrode gas sensor of m group n individual not equal pitch and unequal-interval respectively, form the carbon nano-tube three electrode gas sensor array of the different die opening of m group, the d of all the sensors in m group sensor array
i1and d
i2step 1) in all possible exhaustive or selection empirically of design die opening;
3) with building sensor array, Concentration Testing is carried out to concentration known gas
Calibrating gas is adopted to prepare single-component gas or the polycomponent mixed gas sample of multiple variable concentrations, adopting by step 2) the m group carbon nano-tube three electrode gas sensor array column split of different die openings that builds detects, and obtains the gas discharge ion flow valuve of each tested gas sample;
4) die opening of sensor array and corresponding gas detect result database thereof is set up
With the d of composition sensor each in all m group carbon nano-tube three electrode gas sensor arraies
i1and d
i2, detect gas discharge ion flow valuve that gas sample obtains and the concentration of tested gas sets up die opening and corresponding gas detect result database thereof;
5) tested gas concentration quantitative model is set up
Adopting support vector machine method, with step 4) tested gas discharge ion flow valuve is input in institute's building database, with its corresponding gas concentration for exporting, sets up tested gas concentration quantitative model;
6) die opening of each composition sensor in sensor array is optimized
Adopting by step 5) gas concentration of tested gas concentration quantitative model to all tested gas samples set up analyze, and obtains the detectable concentration of tested gas; Actual concentrations corresponding with it for the detectable concentration of tested gas is asked difference, then divided by the actual concentrations of tested gas, obtains the relative error detecting this gas; Adopt particle swarm optimization algorithm, minimum for target with the relative error of tested gas detect, to by step 2) each d forming sensor in the m group carbon nano-tube three electrode gas sensor array that builds
i1and d
i2be in optimized selection, the final best die opening obtaining each sensor in the carbon nano-tube three electrode gas sensor array detecting this gas.
For the tested gas of single component, this kind gas sample of Single Carbon Nanotubes three electrode gas sensor to multiple variable concentrations of multiple different die opening can be selected to detect, and the die opening that the minimum carbon nano-tube three electrode gas sensor of metrical error is corresponding is the die opening of this gas detect the most applicable; Also multiple carbon nano-tube three electrode gas sensor can be adopted to form sensor array, grouping detects this kind of gas sample of multiple variable concentrations, and the die opening that the minimum carbon nano-tube three electrode gas sensor of metrical error is corresponding is the die opening of this gas detect the most applicable.
To polycomponent mixed gas, needing to build sensor array and detect, generally, have several component to form mixed gas, just needing the carbon nano-tube three electrode gas sensor with being more than or equal to mixing gas component quantity to form sensor array.Embodiment is only with nitrogen monoxide (NO) and sulphuric dioxide (SO
2) mixed gas be that example is described, the component quantity of mixed gas can be expanded.
As shown in Figure 1, the die opening optimization method of carbon nano-tube three electrode gas sensor array adopts following steps:
1) die opening is designed
In the sensor array be made up of 2 sensors, if wherein the die opening of the 1st sensor first electrode and the second electrode is d
11, the second electrode and three electrode die opening be d
12; The die opening of the 2nd sensor first electrode and the second electrode is d
21, the second electrode and three electrode die opening be d
22, have equidistantly and unequal-interval two kinds of situations two die openings of each sensor:
Equidistant: two die openings namely forming the single-sensor of sensor array are equal, d
11, d
12, d
21and d
22increase progressively with step-length 30 μm from 50 μm, form 50 μm, 80 μm, 110 μm, 140 μm, 170 μm, 200 μm, 230 μm, 250 μm and amount to 8 die openings.
Unequal-interval: two die openings namely forming the single-sensor of sensor array are unequal, as d
11increase progressively with step-length 30 μm from 50 μm, form 50 μm, 80 μm, 110 μm, 140 μm, 170 μm, 200 μm, 230 μm, 250 μm and amount to 8 d
11value; d
12also increase progressively with step-length 30 μm from 50 μm, same formation 50 μm, 80 μm, 110 μm, 140 μm, 170 μm, 200 μm, 230 μm, 250 μm amounts to 8 d
12value; In theory, d is worked as
i1, d
i2get above-mentioned different value when combining, possible combination has 56 kinds, wherein, and i=1,2.
Concerning single-sensor, above-mentioned equidistantly and unequal-interval can form totally 64 kinds of different die openings and combine.
2) sensor array be made up of different die opening sensor is built
For NO and SO
2mixed gas, selected number of probes is 2, according to existing experiment experience, from step 1) the die opening that designs, choose 6 to different d
i1and d
i2combination, build the 6 groups of carbon nano-tube be made up of 2 sensors three electrode gas sensor arraies, wherein, d
i1with d
i2combination in table 1:
The combination of the different die opening of table 16 group sensor array
| Group | d 11/μm | d 12/μm | d 21/μm | d 22/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) with building sensor array, Concentration Testing is carried out to concentration known gas
Calibrating gas is adopted to prepare NO and SO of five kinds of variable concentrations
2mixed gas sample, its proportioning refers to table 2.Adopt the 6 groups of carbon nano-tube three electrode gas sensor arraies built in table 1 respectively to NO and SO of 5 kinds of variable concentrations
2mixed gas sample detects, and obtains the gas discharge ion flow valuve of 30 groups of 60 tested gas samples altogether.
NO and SO of table 25 kind of variable concentrations
2mixed gas
| Sequence number | NO/ppm | SO 2/ppm |
| 1 | 500 | 500 |
| 2 | 500 | 800 |
| 3 | 500 | 1000 |
| 4 | 800 | 800 |
| 5 | 800 | 1100 |
4) die opening of sensor array and corresponding gas detect result database thereof is set up
To often organize the d of each sensor in carbon nano-tube three electrode gas sensor array
i1and d
i2, detect gas discharge ion flow valuve that gas sample obtains and the concentration of tested gas sets up die opening and corresponding gas detect result database thereof;
5) tested gas concentration quantitative model is set up
Ignore the impact of temperature and humidity on gas detect, adopt support vector machine method, select gaussian kernel function, with step 4) in the database set up, detect NO and SO
2the discharge ion flow valuve that mixed gas sample each carbon nano-tube three electrode gas sensor obtains is input, with its corresponding tested gas concentration for exporting, sets up tested gas concentration quantitative model;
Step 6 optimizes the die opening of each composition sensor in sensor array
Adopting by step 5) the tested gas concentration quantitative model set up is to NO and SO in 30 groups of tested gas samples
2the concentration of gas is analyzed, and obtains NO and SO
2detectable concentration; Ask for NO and SO
2the relative error of gas detect, as shown in Figure 2; Adopt particle swarm optimization algorithm, minimum for target with tested gas detect error, to by step 2) each d in 6 groups of carbon nano-tube three electrode gas sensor arraies building
i1and d
i2be in optimized selection, find that the 5th group of sensor array that die opening is combined to form detects NO and SO
2the relative error of mixed gas is minimum, and therefore, final acquisition detects NO and SO
2mixed gas adopts in carbon nano-tube three electrode gas sensor array, the best die opening d of two sensors
i1and d
i2be respectively: 150 μm, 180 μm and 180 μm, 180 μm.
The die opening optimization method of the carbon nano-tube three electrode gas sensor that this patent proposes, be equally applicable to the optimization of carbon nano-tube three electrode temperature and humidity sensor die opening, as long as substitute carbon nano-tube three electrode gas sensor with carbon nano-tube three electrode temperature or humidity sensor to form sensor array, step 4 is included in by detecting the temperature and humidity data obtained) in the database set up, then perform step 5) and step 6).
Step 5) in support vector machine method can also be other homing methods such as neural network, least square regression, kernel method; Step 6) in particle swarm optimization algorithm can also be other optimized algorithm such as ant colony optimization algorithm, genetic algorithm.
Claims (2)
1. the die opening optimization method of carbon nano-tube three electrode gas sensor, to the first electrode and second electrode of carbon nano-tube three electrode gas sensor, second electrode and three electrode die opening are optimized, first electrode inside surface distribution carbon nano-tube film substrate of described carbon nano-tube three electrode gas sensor, second electrode is the extraction pole pole plate being provided with fairlead, 3rd electrode is collector, three electrodes are mutually isolated by insulation column, in three electrodes, the die opening scope of adjacent two electrodes is 50 μm ~ 250 μm, it is characterized in that adopting following Optimization Steps:
1) die opening is designed
In the sensor array be made up of n carbon nano-tube three electrode gas sensor, the first electrode of i-th sensor and the die opening of the second electrode are d
i1, the second electrode and three electrode die opening are d
i2, wherein, i=1,2 ..., n, when n is 1, then refers to Single Carbon Nanotubes three electrode gas sensor, the d of each sensor
i1and d
i2there are equidistant and unequal-interval two kinds of situations:
Equidistant: d
i1with d
i2equal, d
i1or d
i2increase progressively with step-length S from 50 μm, until d
i1or d
i2be more than or equal to 250 μm, S is the arbitrary integer between 0 μm-200 μm;
Unequal-interval: d
i1with d
i2unequal, d
i1with step-length S from 50 μm
1increase progressively, until d
i1be more than or equal to 250 μm, d
i2with step-length S from 50 μm
2increase progressively, until d
i2be more than or equal to 250 μm, S
1and S
2be the arbitrary integer between 0 μm-200 μm, work as d
i1when getting a value in aforementioned value, d
i2get and d
i1different values;
2) sensor array be made up of different die opening sensor is built
For the tested gas of single component or the mixed gas that is made up of R kind component, selected number of probes n, n>=R, adopt step 1) the middle die opening designed, build the carbon nano-tube three electrode gas sensor of m group n individual not equal pitch and unequal-interval respectively, form the carbon nano-tube three electrode gas sensor array of the different die opening of m group, the d of all the sensors in m group sensor array
i1and d
i2step 1) in all possible exhaustive or selection empirically of design die opening;
3) with building sensor array, Concentration Testing is carried out to concentration known gas
Calibrating gas is adopted to prepare single-component gas or the polycomponent mixed gas sample of multiple variable concentrations, adopting by step 2) the m group carbon nano-tube three electrode gas sensor array column split of different die openings that builds detects, and obtains the gas discharge ion flow valuve of each tested gas sample;
4) die opening of sensor array and corresponding gas detect result database thereof is set up
With the d of composition sensor each in all m group carbon nano-tube three electrode gas sensor arraies
i1and d
i2, detect gas discharge ion flow valuve that gas sample obtains and the concentration of tested gas sets up die opening and corresponding gas detect result database thereof;
5) tested gas concentration quantitative model is set up
Adopting support vector machine method, with step 4) tested gas discharge ion flow valuve is input in institute's building database, with its corresponding gas concentration for exporting, sets up tested gas concentration quantitative model;
6) die opening of each composition sensor in sensor array is optimized
Adopting by step 5) gas concentration of tested gas concentration quantitative model to all tested gas samples set up analyze, and obtains the detectable concentration of tested gas; Actual concentrations corresponding with it for the detectable concentration of tested gas is asked difference, then divided by the actual concentrations of tested gas, obtains the relative error detecting this gas; Adopt particle swarm optimization algorithm, minimum for target with the relative error of tested gas detect, to by step 2) each d forming sensor in the m group carbon nano-tube three electrode gas sensor array that builds
i1and d
i2be in optimized selection, the final best die opening obtaining each sensor in the carbon nano-tube three electrode gas sensor array detecting this gas.
2. the die opening optimization method of carbon nano-tube three electrode gas sensor according to claim 1, it is characterized in that: carbon nano-tube three electrode gas sensor can be replaced carbon nano-tube three electrode temperature sensors or carbon nano-tube three electrode humidity sensor, for detected temperatures or humidity.
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| CN114018326A (en) * | 2021-11-03 | 2022-02-08 | 国网湖南省电力有限公司 | Low-voltage transformer area environment multi-parameter detection method based on micro-system sensor array |
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| CN104614437B (en) | 2017-03-22 |
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