CN105628856B - A kind of catalytic luminescence sensitive material of benzene and sulfur dioxide - Google Patents
A kind of catalytic luminescence sensitive material of benzene and sulfur dioxide Download PDFInfo
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- CN105628856B CN105628856B CN201511031120.9A CN201511031120A CN105628856B CN 105628856 B CN105628856 B CN 105628856B CN 201511031120 A CN201511031120 A CN 201511031120A CN 105628856 B CN105628856 B CN 105628856B
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- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N31/00—Investigating or analysing non-biological materials by the use of the chemical methods specified in the subgroup; Apparatus specially adapted for such methods
- G01N31/10—Investigating or analysing non-biological materials by the use of the chemical methods specified in the subgroup; Apparatus specially adapted for such methods using catalysis
Abstract
A kind of catalytic luminescence sensitive material of benzene and sulfur dioxide, it is characterized in that graphene-supported by Bi2O3, PbO and In2O3The composite of composition.Its preparation method is：By oxidation processes of the native graphite respectively through oleum, potassium permanganate concentrated sulfuric acid solution and hydrogen peroxide, graphene oxide is made；Solution is made in bismuth oxalate, lead acetate and indium nitrate, agar powder formation gel is added, the drying of this gel, roasting and cooling is obtained by Bi2O3, PbO and In2O3The metal composite oxide of composition；This metal composite oxide and foregoing graphene oxide are added in hydrazine hydrate aqueous solution, irradiated with xenon lamp, filter and drying to graphene-supported by Bi2O3, PbO and In2O3The composite of composition.Make gas sensor using sensitive material provided by the present invention, can at the scene the quick, micro-benzene in Accurate Determining air and sulfur dioxide without being disturbed by common concurrent.
Description
Technical field
The present invention relates to the catalytic luminescence sensitive material of a kind of benzene and sulfur dioxide, particularly by graphene-supported
Bi2O3, PbO and In2O3The composite of composition, belongs to new catalytic material technical field.
Background technology
Benzene be a kind of benzene in industrial chemicals with aromatic odor, air be mainly derived from building coating, paint for decoration,
Adhesive solvent and vehicle exhaust etc..Chronic Benzene Poisoning mainly has stimulation to skin, eyes and the upper respiratory tract；Often connect
Touch benzene, skin can because of degreasing desiccation furfur, some appearance allergic eczemas；Long-term suction benzene can cause aplastic poor
Blood.Benzene confirms as carcinogen by IARC (IARC), is the major pollutants of room air.
Sulfur dioxide is one of major pollutants in air, and sulfur dioxide has acidity, can be with the material of other in air
Reaction, generates small sulphite and sulphate particle.When these particles are inhaled into, they will be gathered in lung, be to exhale
The one of the main reasons of desorption system symptom and disease.During with eye contact, red and swollen and pain can be caused.Sulfur dioxide enters breathing
Behind road, because its is soluble in water, therefore major part is arrested in the upper respiratory tract, and generation has corrosive sulfurous on the mucous membrane of moistening
Acid, sulfuric acid and sulfate, strengthen stimulation.When sulfur dioxide concentration is 10~15ppm, respiratory tract ciliary movement and mucous membrane
Secreting function can be suppressed.When concentration reaches 20ppm, cause cough and stimulate eyes.If daily inhaled concentration is
100ppm was up to 8 hours, and obvious irritation occur in bronchus and lung, make damaged lung tissue.Concentration can make when reaching 400ppm
People produces expiratory dyspnea.Sulfur dioxide is inhaled into together with floating dust, and sulfur dioxide can be taken to lung by floating dust aerosol particles to be made
Toxicity increases by 3~4 times.If floating dust adsorption metal particle, under its catalytic action, it is sulfuric acid mist to make oxidizing sulfur dioxide,
Its stimulation is more stronger than sulfur dioxide.Live in for a long time in the environment of atmosphere pollution, due to the joint of sulfur dioxide and floating dust
Effect, can promote alveolar fibroplasia.If hyperplasia scope involves extensively, fibrous lesions are formed, development goes down that fiber can be made
Break to form pulmonary emphysema.Sulfur dioxide can strengthen the carcinogenesis of carcinogenic substance BaP.According to animal experiment, in sulfur dioxide and
Under the synergy of BaP, the incidence of disease of animal lung cancer is higher than the incidence of disease of the single factor, and lung can be induced in a short time
Squamous cell carcinoma.
Benzene in air and the detection method of sulfur dioxide mainly have：AAS, fluorimetry, flow injection chemistry
Luminescence method, gas chromatography, liquid chromatography and electrochemical process etc..These method sensitivity are all higher, but complex operation, must
It must be completed in laboratory, it is impossible to realize at scene.
The content of the invention
The purpose of the present invention is to overcome the shortcomings of that conventional art has compared with high selectivity there is provided a kind of to benzene and sulfur dioxide
Catalytic luminescence sensitive material.The monitoring benzene and the gas sensor of sulfur dioxide made of this sensitive material, can be existing
Field is quick, the micro-benzene in Accurate Determining air and sulfur dioxide by common concurrent without being disturbed.
The catalytic luminescence sensitive material of a kind of benzene and sulfur dioxide of the present invention is graphene-supported by Bi2O3、
PbO and In2O3The composite of composition, can be prepared by native graphite, bismuth salt, lead salt and indium salts.Wherein, with bismuth oxalate, vinegar
Lead plumbate and indium nitrate are for the preparation method of primary raw material：
(1) native graphite is slowly added in 40 DEG C of oleum with continuous stirring, constant temperature is slow after stirring 2 hours
The phosphoric acid of the weight such as addition and native graphite, continues constant temperature and stirs 3 hours, much filtrate is simultaneously washed to neutrality by suction filtration；By filter cake
Mass fraction is added in 15% potassium permanganate concentrated sulfuric acid solution, to be warming up to 45-55 DEG C and continuously stirring 2 hours, it is slow to add
Enter aqueous hydrogen peroxide solution that mass fraction is 25% untill bubble-free, continue constant temperature and stir 1 hour, suction filtration and by much filtrate
Neutrality is washed to, graphene oxide is obtained；
(2) bismuth oxalate is dissolved in the aqueous hydrochloric acid solution that mass fraction is 10-20% and forms solution A, lead acetate is dissolved in
Indium nitrate is dissolved in the isobutyl that mass fraction is 30-40% by mass fraction to form solution B in 20-30% aqueous citric acid solutions
Solution C is formed in alcohol solution；With continuous stirring, solution A and solution B are slowly added in solution C successively, stirred 2 hours
Afterwards, add a small amount of agar powder continuation stirring and form gel；After this gel is dried, it is no more than in chamber type electric resistance furnace with per minute
3 DEG C of speed is warming up to 200-250 DEG C, keeps this temperature 4 hours, and continuation is warming up to the speed per minute for being no more than 3 DEG C
450-500 DEG C, keep this temperature 3 hours, naturally cool to room temperature and obtain by Bi2O3, PbO and In2O3The composition metal oxygen of composition
Compound；With continuous stirring, this metal composite oxide is added mass fraction in 20% hydrazine hydrate aqueous solution, then will
Foregoing graphene oxide is also added thereto, and is warming up to 40 DEG C, constant temperature is stirred 4 hours, is irradiated 3 hours with 300 watts of xenon lamps, mistake
It is washed with deionized after filter 3 times, is subsequently placed in 60 DEG C of vacuum drying oven drying, that is, obtains graphene-supported by Bi2O3, PbO and
In2O3The composite powder material of composition.
Wherein, bismuth salt is anhydride or the hydration of bismuth acetate, bismuth oxalate, bismuth nitrate, bismuth sulfate, bismuth phosphate and bismuth trichloride
One or more of mixtures of thing, lead salt be the anhydride of plumbi nitras, lead acetate and plumbous rhodanate or one kind of hydrate or
Several mixtures, indium salts are the anhydride of inidum chloride, indium nitrate, indium sulfate, indium acetate and indium phosphate or one kind of hydrate
Or two kinds of mixture.
When obtained composite each component mass fraction meets Bi2O3(10-20%), PbO (15-25%), In2O3
It is very high for having as the catalytic luminescence sensitive material for determining benzene and sulfur dioxide when (14-24%) and C (45-60%)
Sensitivity and selectivity.
Embodiment
Embodiment 1
[1] native graphite is slowly added in 40 DEG C of oleum with continuous stirring, constant temperature is slow after stirring 2 hours
The phosphoric acid of the weight such as addition and native graphite, continues constant temperature and stirs 3 hours, much filtrate is simultaneously washed to neutrality by suction filtration；By filter cake
Mass fraction is added in 15% potassium permanganate concentrated sulfuric acid solution, to be warming up to 50 DEG C and continuously stir 2 hours, be slowly added to matter
The aqueous hydrogen peroxide solution that amount fraction is 25% continues constant temperature and stirred 1 hour, suction filtration simultaneously washes much filtrate untill bubble-free
To neutral, graphene oxide is obtained；
[2] seven water bismuth oxalates are dissolved in the aqueous hydrochloric acid solution that mass fraction is 15% and form solution A, by acetate trihydrate lead
Be dissolved in mass fraction to form solution B in 25% aqueous citric acid solution, by nitrate trihydrate indium be dissolved in mass fraction for 35% it is different
Solution C is formed in the butanol aqueous solution；With continuous stirring, solution A and solution B are slowly added in solution C successively, stirring 2 is small
Shi Hou, adds a small amount of agar powder continuation stirring and forms gel；After this gel is dried, do not surpassed with per minute in chamber type electric resistance furnace
The speed for crossing 3 DEG C is warming up to 220 DEG C, keeps this temperature 4 hours, and continuation is warming up to 480 with the speed per minute for being no more than 3 DEG C
DEG C, keep this temperature 3 hours, naturally cool to room temperature and obtain by Bi2O3, PbO and In2O3The metal composite oxide of composition；
Continuously stir down, this metal composite oxide is added in the hydrazine hydrate aqueous solution that mass fraction is 20%, then will be foregoing
Graphene oxide is also added thereto, and is warming up to 40 DEG C, constant temperature is stirred 4 hours, is irradiated 3 hours, used after filtering with 300 watts of xenon lamps
Deionized water is washed 3 times, is subsequently placed in 60 DEG C of vacuum drying oven drying, that is, is obtained graphene-supported by Bi2O3, PbO and In2O3
The composite powder material of composition.
Analysis：Constituent analysis is carried out to composite powder material, the mass percent for measuring each component is respectively 12.1%
Bi2O3, 23.5%PbO, 19.2%In2O3And 45.2%C.
Using：The catalytic luminescence sensitive material for determining benzene and sulfur dioxide, the range of linearity are used as using this composite powder material
For benzene 0.2-156mg/m3With sulfur dioxide 0.15-79mg/m3, detect and be limited to benzene 0.1mg/m3With sulfur dioxide 0.08mg/m3,
Other common concurrents are not interfered with.
Embodiment 2
[1] native graphite is slowly added in 40 DEG C of oleum with continuous stirring, constant temperature is slow after stirring 2 hours
The phosphoric acid of the weight such as addition and native graphite, continues constant temperature and stirs 3 hours, much filtrate is simultaneously washed to neutrality by suction filtration；By filter cake
Mass fraction is added in 15% potassium permanganate concentrated sulfuric acid solution, to be warming up to 46 DEG C and continuously stir 2 hours, be slowly added to matter
The aqueous hydrogen peroxide solution that amount fraction is 25% continues constant temperature and stirred 1 hour, suction filtration simultaneously washes much filtrate untill bubble-free
To neutral, graphene oxide is obtained；
[2] bismuth acetate is dissolved in the aqueous hydrochloric acid solution that mass fraction is 11% and forms solution A, plumbi nitras is dissolved in quality
It is water-soluble that fraction is dissolved in the isobutanol that mass fraction is 39% to form solution B in 21% aqueous citric acid solution, by nitrate trihydrate indium
Solution C is formed in liquid；With continuous stirring, solution A and solution B are slowly added in solution C successively, after stirring 2 hours, added
A small amount of agar powder continues stirring and forms gel；After this gel is dried, with the speed per minute for being no more than 3 DEG C in chamber type electric resistance furnace
Degree is warming up to 210 DEG C, keeps this temperature 4 hours, and continuation is warming up to 460 DEG C with the speed per minute for being no more than 3 DEG C, keeps this temperature
Degree 3 hours, naturally cools to room temperature and obtains by Bi2O3, PbO and In2O3The metal composite oxide of composition；With continuous stirring,
This metal composite oxide is added in the hydrazine hydrate aqueous solution that mass fraction is 20%, then by foregoing graphene oxide
It is added thereto, is warming up to 40 DEG C, constant temperature is stirred 4 hours, is irradiated 3 hours, be washed with deionized after filtering with 300 watts of xenon lamps
3 times, 60 DEG C of vacuum drying oven drying are subsequently placed in, that is, obtain graphene-supported by Bi2O3, PbO and In2O3The composite powder of composition
Body material.
Analysis：Constituent analysis is carried out to composite powder material, the mass percent for measuring each component is respectively 18.8%
Bi2O3, 16.1%PbO, 14.3%In2O3And 50.8%C.
Using：The catalytic luminescence sensitive material for determining benzene and sulfur dioxide, the range of linearity are used as using this composite powder material
For benzene 0.15-125mg/m3With sulfur dioxide 0.2-87mg/m3, detect and be limited to benzene 0.08mg/m3With sulfur dioxide 0.1mg/m3,
Other common concurrents are not interfered with.
Embodiment 3
[1] native graphite is slowly added in 40 DEG C of oleum with continuous stirring, constant temperature is slow after stirring 2 hours
The phosphoric acid of the weight such as addition and native graphite, continues constant temperature and stirs 3 hours, much filtrate is simultaneously washed to neutrality by suction filtration；By filter cake
Mass fraction is added in 15% potassium permanganate concentrated sulfuric acid solution, to be warming up to 54 DEG C and continuously stir 2 hours, be slowly added to matter
The aqueous hydrogen peroxide solution that amount fraction is 25% continues constant temperature and stirred 1 hour, suction filtration simultaneously washes much filtrate untill bubble-free
To neutral, graphene oxide is obtained；
[2] five water bismuth nitrates are dissolved in the aqueous hydrochloric acid solution that mass fraction is 19% and form solution A, plumbous rhodanate is molten
Solution B is formed in mass fraction is 24% aqueous citric acid solution, five water indium sulfates are dissolved in the isobutyl that mass fraction is 31%
Solution C is formed in alcohol solution；With continuous stirring, solution A and solution B are slowly added in solution C successively, stirred 2 hours
Afterwards, add a small amount of agar powder continuation stirring and form gel；After this gel is dried, it is no more than in chamber type electric resistance furnace with per minute
3 DEG C of speed is warming up to 230 DEG C, keeps this temperature 4 hours, and continuation is warming up to 470 DEG C with the speed per minute for being no more than 3 DEG C,
Keep this temperature 3 hours, naturally cool to room temperature and obtain by Bi2O3, PbO and In2O3The metal composite oxide of composition；Even
Under continuous stirring, this metal composite oxide is added in the hydrazine hydrate aqueous solution that mass fraction is 20%, then by foregoing oxygen
Graphite alkene is also added thereto, and is warming up to 40 DEG C, constant temperature is stirred 4 hours, is irradiated 3 hours, spent after filtering with 300 watts of xenon lamps
Ion water washing 3 times, is subsequently placed in 60 DEG C of vacuum drying oven drying, that is, obtains graphene-supported by Bi2O3, PbO and In2O3Group
Into composite powder material.
Analysis：Constituent analysis is carried out to composite powder material, the mass percent for measuring each component is respectively 11.5%
Bi2O3, 16.2%PbO, 15.1%In2O3And 57.2%C.
Using：The catalytic luminescence sensitive material for determining benzene and sulfur dioxide, the range of linearity are used as using this composite powder material
For benzene 0.25-142mg/m3With sulfur dioxide 0.2-88mg/m3, detect and be limited to benzene 0.15mg/m3With sulfur dioxide 0.1mg/m3,
Other common concurrents are not interfered with.
Embodiment 4
[1] native graphite is slowly added in 40 DEG C of oleum with continuous stirring, constant temperature is slow after stirring 2 hours
The phosphoric acid of the weight such as addition and native graphite, continues constant temperature and stirs 3 hours, much filtrate is simultaneously washed to neutrality by suction filtration；By filter cake
Mass fraction is added in 15% potassium permanganate concentrated sulfuric acid solution, to be warming up to 52 DEG C and continuously stir 2 hours, be slowly added to matter
The aqueous hydrogen peroxide solution that amount fraction is 25% continues constant temperature and stirred 1 hour, suction filtration simultaneously washes much filtrate untill bubble-free
To neutral, graphene oxide is obtained；
[2] bismuth sulfate is dissolved in the aqueous hydrochloric acid solution that mass fraction is 14% and forms solution A, plumbi nitras is dissolved in quality
Indium acetate is dissolved in the isobutyl alcohol solution that mass fraction is 36% by fraction to form solution B in 29% aqueous citric acid solution
Form solution C；With continuous stirring, solution A and solution B are slowly added in solution C successively, after stirring 2 hours, added a small amount of
Agar powder continues stirring and forms gel；After this gel is dried, with the speed liter per minute for being no more than 3 DEG C in chamber type electric resistance furnace
Temperature keeps this temperature 4 hours to 240 DEG C, and continuation is warming up to 470 DEG C with the speed per minute for being no more than 3 DEG C, keeps this temperature 3
Hour, naturally cool to room temperature and obtain by Bi2O3, PbO and In2O3The metal composite oxide of composition；With continuous stirring, will
This metal composite oxide adds mass fraction in 20% hydrazine hydrate aqueous solution, then also to add foregoing graphene oxide
Enter wherein, be warming up to 40 DEG C, constant temperature is stirred 4 hours, irradiated 3 hours with 300 watts of xenon lamps, 3 are washed with deionized after filtering
It is secondary, 60 DEG C of vacuum drying oven drying are subsequently placed in, that is, obtain graphene-supported by Bi2O3, PbO and In2O3The composite granule of composition
Material.
Analysis：Constituent analysis is carried out to composite powder material, the mass percent for measuring each component is respectively 13.2%
Bi2O3, 15.3%PbO, 23.1%In2O3And 48.4%C.
Using：The catalytic luminescence sensitive material for determining benzene and sulfur dioxide, the range of linearity are used as using this composite powder material
For benzene 0.1-85mg/m3With sulfur dioxide 0.2-84mg/m3, detect and be limited to benzene 0.05mg/m3With sulfur dioxide 0.1mg/m3, its
Its common concurrent is not interfered with.
Embodiment 5
[1] native graphite is slowly added in 40 DEG C of oleum with continuous stirring, constant temperature is slow after stirring 2 hours
The phosphoric acid of the weight such as addition and native graphite, continues constant temperature and stirs 3 hours, much filtrate is simultaneously washed to neutrality by suction filtration；By filter cake
Mass fraction is added in 15% potassium permanganate concentrated sulfuric acid solution, to be warming up to 48 DEG C and continuously stir 2 hours, be slowly added to matter
The aqueous hydrogen peroxide solution that amount fraction is 25% continues constant temperature and stirred 1 hour, suction filtration simultaneously washes much filtrate untill bubble-free
To neutral, graphene oxide is obtained；
[2] bismuth phosphate is dissolved in the aqueous hydrochloric acid solution that mass fraction is 17% and forms solution A, by plumbi nitras and lead acetate
Mass fraction is dissolved in form solution B in 25% aqueous citric acid solution, and nitrate trihydrate indium and indium phosphate are dissolved in into mass fraction is
Solution C is formed in 32% isobutyl alcohol solution；With continuous stirring, solution A and solution B are slowly added in solution C successively,
After stirring 2 hours, add a small amount of agar powder continuation stirring and form gel；After this gel is dried, with every in chamber type electric resistance furnace
Speed of the minute no more than 3 DEG C is warming up to 205 DEG C, keeps this temperature 4 hours, continues with the speed liter per minute for being no more than 3 DEG C
Temperature keeps this temperature 3 hours, naturally cools to room temperature and obtain by Bi to 490 DEG C2O3, PbO and In2O3The composition metal oxygen of composition
Compound；With continuous stirring, this metal composite oxide is added mass fraction in 20% hydrazine hydrate aqueous solution, then will
Foregoing graphene oxide is also added thereto, and is warming up to 40 DEG C, constant temperature is stirred 4 hours, is irradiated 3 hours with 300 watts of xenon lamps, mistake
It is washed with deionized after filter 3 times, is subsequently placed in 60 DEG C of vacuum drying oven drying, that is, obtains graphene-supported by Bi2O3, PbO and
In2O3The composite powder material of composition.
Analysis：Constituent analysis is carried out to composite powder material, the mass percent for measuring each component is respectively 12.6%
Bi2O3, 24.7%PbO, 16.4%In2O3And 46.3%C.
Using：The catalytic luminescence sensitive material for determining benzene and sulfur dioxide, the range of linearity are used as using this composite powder material
For benzene 0.18-132mg/m3With sulfur dioxide 0.25-118mg/m3, detect and be limited to benzene 0.1mg/m3With sulfur dioxide 0.15mg/
m3, other common concurrents do not interfere with.
Claims (1)
1. the catalytic luminescence sensitive material of a kind of benzene and sulfur dioxide, it is characterized in that graphene-supported by Bi2O3, PbO and In2O3
The composite of composition, each component mass fraction is 10-20%Bi2O3, 15-25%PbO, 14-24%In2O3And 45-60%C,
Its preparation method is：
(1) native graphite is slowly added in 40 DEG C of oleum with continuous stirring, constant temperature is slowly added to after stirring 2 hours
With the phosphoric acid of the weight such as native graphite, continue constant temperature and stir 3 hours, much filtrate is simultaneously washed to neutrality by suction filtration；Filter cake is added
Mass fraction for 15% potassium permanganate concentrated sulfuric acid solution in, be warming up to 45-55 DEG C and continuously stir 2 hours, be slowly added to matter
The aqueous hydrogen peroxide solution that amount fraction is 25% continues constant temperature and stirred 1 hour, suction filtration simultaneously washes much filtrate untill bubble-free
To neutral, graphene oxide is obtained；
(2) bismuth oxalate is dissolved in the aqueous hydrochloric acid solution that mass fraction is 10-20% and forms solution A, lead acetate is dissolved in quality
Indium nitrate is dissolved in the isobutanol water that mass fraction is 30-40% by fraction to form solution B in 20-30% aqueous citric acid solutions
Solution C is formed in solution；With continuous stirring, solution A and solution B are slowly added in solution C successively, after stirring 2 hours, plus
Enter a small amount of agar powder continuation stirring and form gel；After this gel is dried, 3 DEG C are no more than with per minute in chamber type electric resistance furnace
Speed is warming up to 200-250 DEG C, keeps this temperature 4 hours, and continuation is warming up to 450-500 with the speed per minute for being no more than 3 DEG C
DEG C, keep this temperature 3 hours, naturally cool to room temperature and obtain by Bi2O3, PbO and In2O3The metal composite oxide of composition；
Continuously stir down, this metal composite oxide is added in the hydrazine hydrate aqueous solution that mass fraction is 20%, then will be foregoing
Graphene oxide is also added thereto, and is warming up to 40 DEG C, constant temperature is stirred 4 hours, is irradiated 3 hours, used after filtering with 300 watts of xenon lamps
Deionized water is washed 3 times, is subsequently placed in 60 DEG C of vacuum drying oven drying, that is, is obtained graphene-supported by Bi2O3, PbO and In2O3
The composite of composition.
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| CN108314030B (en) * | 2018-03-29 | 2020-11-17 | 北京联合大学 | Mercury ion polluted water body repairing material |
| CN108802016B (en) * | 2018-08-08 | 2019-10-08 | 北京联合大学 | A kind of high selection measures the sensitive material of trace formaldehyde in air |
| CN109490372B (en) * | 2018-11-30 | 2020-11-17 | 北京联合大学 | Catalytic luminous sensitive material of ethanol |
| CN109490374B (en) * | 2018-11-30 | 2020-11-13 | 北京联合大学 | Cross sensitive material for formaldehyde, benzene, ammonia and carbon monoxide in air |
| CN109775668A (en) * | 2019-04-01 | 2019-05-21 | 四川中科贝特纳米科技有限公司 | A kind of sulfur dioxide catalytic reduction device and method |
| CN110095559B (en) * | 2019-04-03 | 2021-09-14 | 北京联合大学 | Catalytic luminous sensitive material of low-temperature formaldehyde, benzene and ammonia |
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| JP3950812B2 (en) * | 2003-04-28 | 2007-08-01 | 日本特殊陶業株式会社 | Gas sensor and manufacturing method thereof |
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| JP3950812B2 (en) * | 2003-04-28 | 2007-08-01 | 日本特殊陶業株式会社 | Gas sensor and manufacturing method thereof |
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