CN108663416B - Gas sensor for formaldehyde detection and manufacturing method thereof - Google Patents
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Abstract
The invention relates to a gas sensor and a preparation method thereof, wherein the surface of the gas sensor is In modified by graphene oxide2O3/Au/MnO2The composite metal oxide gas-sensitive material is prepared by firstly forming in (OH)3Colloid, how to add chloroauric acid and manganese chlorideReacting with sodium borohydride and the like, and calcining under the protection of inert gas to obtain In2O3/Au/MnO2And (2) attaching graphene oxide to the surface of the composite metal oxide particles, preparing the particles modified by the graphene oxide into slurry, coating the slurry on a substrate, calcining and aging to obtain the final gas sensor. The preparation method of the gas sensor has simple process and mild reaction conditions, and is suitable for large-scale industrial production. The gas sensor is arranged In2O3In-situ doping of Au and MnO2Meanwhile, the graphene oxide material is attached to the surface of the gas sensitive material, so that the detection sensitivity of the gas sensitive material to flammable gases, particularly formaldehyde, is effectively improved, and the response speed is higher.
Description
Technical Field
The invention relates to a gas sensor and a manufacturing method thereof, In particular to a gas sensor for detecting formaldehyde and a manufacturing method thereof, wherein the surface of the gas sensor is In modified by graphene oxide2O3/Au/MnO2Preparing the composite metal oxide gas-sensitive material. The gas-sensitive material has excellent gas-sensitive performance to various flammable gases, particularly formaldehyde gas.
Background
Gas sensors are an important branch of sensor technology. The matrix material of the core gas sensor of the gas sensor is mainly inorganic metal oxide semiconductor material such as SnO2、Fe2O3、WO3、In2O3And the like. These gas-sensitive materials play an important role in the detection of flammable, explosive, toxic and harmful gases.
In the past, the research was conducted on SnO2、Fe2O3、WO3The metal oxide semiconductor materials have more researches on gas sensitivity, but the traditional gas sensitive materials have the defect of poor selectivity. Therefore, the development of a new material is of great significance. And In2O3As a new gas sensitive material, its research was active after 1993. The earliest research on relevant aspects in China appeared in 1995. At present, the research depth in the aspect of domestic is far from abroad. Development of In2O3The new function of the gas sensitive material is significant for improving the application value of the gas sensor.
Pure In2O3Although the gas-sensitive material has good performance in gas sensitivity to gases such as ethanol and ammonia gas, the gas-sensitive performance still needs to be further improved. Compounding and modification are common methods for improving material properties. Graphene, as a novel carbon nanomaterial with a single carbon atom layer, has an ultra-large specific surface area and high electron mobility, and can adsorb gas molecules when encountering the gas molecules, and the adsorbed gas molecules serve as acceptors or donors to accept or provide electrons, so that the conductivity of the graphene is changed. The special properties make it have great prospect in the field of gas sensitive material application. Meanwhile, Au is adopted to carry out surface modification on the material, so that the Au has a catalytic effect on the oxidation of reducing gas, the reaction temperature is reduced, and the property of the material can be improved greatly.
Disclosure of Invention
In view of the problems of the prior art, according to one aspect of the present invention, there is provided a gas sensor using In whose surface is modified with graphene oxide2O3/Au/MnO2Preparing the composite metal oxide gas-sensitive material.
According to another aspect of the present invention, there is provided a method for producing the gas sensor, the method including the steps of:
1) adding indium salt into a reactor, adding deionized water, controlling the concentration of the indium salt to be in the range of 0.05-0.5 mol/L, stirring at constant temperature of room temperature to 35 ℃, introducing ammonia gas, adjusting the pH to about 10, and reacting for 3-5 hours to obtain in (OH)3After the colloid is formed, the introduction of ammonia gas is stopped, and then the prepared colloidal solution is washed with distilled water.
2) Adding chloroauric acid solution with the concentration of 0.01-0.2 mol/L into the precipitate, mixing, stirring at normal temperature to uniformly disperse, and then adjusting the pH value to about 10 by using ammonia water to form colloidal solution.
3) Dropwise adding manganese metallocenes (Mn (C) to the colloidal solution of the step 2) at 10 to 20 DEG C5H5)2) Then adding sodium borohydride, heating the reaction system to 40-50 ℃, and stirring for 6-10 hours to obtain a precipitate.
4) Centrifugally separating the precipitate obtained in the step 3), washing the precipitate with deionized water, then placing the precipitate into a reaction kettle for reaction at 120-140 ℃ for 2-6 hours, taking out the precipitate, washing and drying the precipitate.
5) Then calcining the product obtained In the step 4) for 3-6 hours at the temperature of 200-400 ℃ under the protection of inert gas to obtain In2O3/Au/MnO2Composite metal oxide particles, and then grinding the particles.
6) Dispersing graphene oxide In deionized water, performing ultrasonic dispersion to obtain a graphene oxide colloidal solution, adding the composite metal oxide particles obtained In the step 5) into the graphene oxide colloidal solution, and calcining for 3-6 hours at 200-400 ℃ under the protection of inert gas to obtain In with the surface modified by the graphene oxide2O3/Au/MnO2Composite metal oxide particles.
7) Modifying the surface of the In prepared In the step 6) with graphene oxide2O3/Au/MnO2Dry grinding the composite metal oxide particles in a mortar for a period of time to make the particles uniform and fine, adding a small amount of deionized water and a proper amount of adhesive, fully grinding to form slurry, coating the obtained slurry on the surface of a substrate, and then strip-grinding the substrate coated with the slurry at 300-550 DEG CKeeping the temperature for 2 to 6 hours under the condition, then electrifying direct current on an aging table, and aging for 5 to 7 days at the temperature of 400 ℃.
Preferably, the indium salt in step 1) is indium nitrate or indium chloride.
Preferably, in (OH) in step 2)3The molar ratio of the gold chloride to the gold chloride is controlled to be between 1:0.02 and 1:0.4, preferably between 1:0.05 and 1:0.2, and more preferably between 1:0.07 and 1: 0.1.
Preferably, the molar ratio of In to Mn In step 3) is from 1:0.1 to 1:0.6, preferably from 1:0.2 to 1:0.5, more preferably from 1:0.3 to 1: 0.4.
Preferably, the molar ratio of sodium borohydride to chloroauric acid in step 3) is controlled to be about 1:0.8 to 1: 1.
Preferably, the inert gas during the calcination in steps 5) and 6) is selected from nitrogen or argon.
Preferably, the graphene oxide and In step 6)2O3/Au/MnO2The weight ratio of the composite metal oxide particles is 0.04:1 to 0.08:1, preferably 0.04:1 to 0.06:1, more preferably 0.05: 1.
Preferably, the substrate in step 7) is Al2O3Ceramic tube substrate or glass substrate, preferably Al2O3A ceramic tube; the coating operation can be any one of brushing, spraying, screen printing and the like.
Preferably, the binder in step 7) is selected from terpineol and the like.
According to another aspect of the invention, the use of the gas sensor for detecting the flammable gas formaldehyde is provided.
Advantageous effects
The preparation method of the gas sensor disclosed by the invention is simple in process, mild in reaction conditions and suitable for large-scale industrial production. The gas sensor prepared by the method of the invention is prepared by In2O3In-situ doping of Au and MnO2Meanwhile, the graphene oxide material is attached to the surface of the gas sensitive material, so that the detection sensitivity of the gas sensitive material to flammable gases, particularly formaldehyde, is effectively improved, and the response speed is higher.
Drawings
FIG. 1 shows In prepared In example 1 and surface-modified with graphene oxide2O3/Au/MnO2Scanning electron micrographs of the composite metal oxide particles.
FIG. 2 shows In prepared In example 1 and surface-modified with graphene oxide2O3/Au/MnO2Transmission electron micrographs of the composite metal oxide particles.
FIG. 3 shows In prepared In example 1 and surface-modified with graphene oxide2O3/Au/MnO2Gas sensitivity curve of composite metal oxide particles to 10ppm formaldehyde.
Detailed Description
Hereinafter, the present invention will be described in detail. Before the description is made, it should be understood that the terms used in the present specification and the appended claims should not be construed as limited to general and dictionary meanings, but interpreted based on the meanings and concepts corresponding to technical aspects of the present invention on the basis of the principle that the inventor is allowed to define terms appropriately for the best explanation. Accordingly, the description proposed herein is just a preferable example for the purpose of illustrations only, not intended to limit the scope of the invention, so it should be understood that other equivalents and modifications could be made thereto without departing from the spirit and scope of the invention.
The preparation method according to the invention is carried out by adding In2O3Middle doped Au and MnO2And simultaneously, the composite material obtained by modifying the graphene oxide on the outer surface has particularly high sensitivity to formaldehyde. The detection limit of formaldehyde in the air can be greatly improved, and the response time is fast.
In (OH) in step 2) of the production method according to the present invention3The molar ratio of the gold chloride to the gold chloride is controlled to be between 1:0.02 and 1:0.4, preferably between 1:0.05 and 1:0.2, and more preferably between 1:0.07 and 1: 0.1. When in (OH)3When the molar ratio of the gold chloride to the chloroauric acid is less than 1:0.4, namely the content of gold is excessive, phase separation is easy to occur, the accurate control of the proportion of the composite oxide is not facilitated, and meanwhile, the gas sensitivity is reduced; when in (OH)3The molar ratio of the gold chloride to the gold chloride acid is more than 1:0.0When 2, i.e., the gold content is insufficient, the response time is not good.
Also preferably, the molar ratio of In to Mn In step 3) is from 1:0.1 to 1:0.6, preferably from 1:0.2 to 1:0.5, more preferably from 1:0.3 to 1: 0.4. When the molar ratio of In to Mn is less than 1:0.6, that is, Mn is excessive, the gas sensitivity is poor; when the molar ratio of In to Mn is more than 1:0.4, that is, Mn is insufficient, the gas sensitivity is also poor.
Preferably, the molar ratio of sodium borohydride to chloroauric acid in step 3) is about 1:0.8 to 1:1, and the present invention needs to ensure that all chloroauric acid is reduced, so the molar ratio of sodium borohydride to chloroauric acid needs to be controlled within a range of about 1:0.8 to 1:1, i.e. sodium borohydride is slightly excessive to ensure that the reduction reaction of chloroauric acid is smoothly performed. Surprisingly, the inventors of the present invention found that manganese dioleyl (Mn (C) in step 3)5H5)2) And the order of addition of sodium borohydride has a significant influence on the product, and manganese (Mn (C) is added firstly5H5)2) And (3) adding sodium borohydride after the tetrahydrofuran solution is uniformly mixed with the colloidal solution In the step 2), so that Au can be quickly and effectively reduced into Au atoms, and good combination of In/Au/Mn can be realized. If sodium borohydride is added to reduce chloroauric acid, manganese metallocene (Mn (C) is added5H5)2) The three metal elements are not easy to be compounded. This is probably because the premature reduction of the Au atoms makes the Au atoms likely to phase separate and precipitate during the later calcination. Further manganese Dicyclopentadiene (Mn (C)5H5)2) May act like a catalyst to facilitate the reduction of chloroauric acid.
Further, preferably, the graphene oxide and In step 6)2O3/Au/MnO2The weight ratio of the composite metal oxide particles is 0.04:1 to 0.08:1, preferably 0.04:1 to 0.06:1, more preferably 0.05: 1. If graphene oxide is mixed with In2O3/Au/MnO2If the weight ratio of the composite metal oxide particles is out of the above range, the response time of the composite material is not good.
The following examples are given by way of illustration of embodiments of the invention and are not to be construed as limiting the invention, and it will be understood by those skilled in the art that modifications may be made without departing from the spirit and scope of the invention. Unless otherwise specified, reagents and equipment used in the following examples are commercially available products.
Example 1
1) Adding indium nitrate into a reactor, adding deionized water, controlling the concentration of indium salt to be 0.02mol/L, controlling the temperature to be between room temperature and 35 ℃, stirring at constant temperature, introducing ammonia gas, adjusting the pH value to be about 10, and reacting for 3 hours to obtain in (OH)3After the colloid is formed, the introduction of ammonia gas is stopped, and then the prepared colloidal solution is washed with distilled water.
2) Adding chloroauric acid solution with concentration of 0.002mol/L into the precipitate, stirring at room temperature to disperse uniformly, and adjusting pH to about 10 with ammonia water to obtain colloidal solution in (OH)3The molar ratio to chloroauric acid was 1: 0.1.
3) Dropwise adding manganese metallocenes (Mn (C) to the colloidal solution of the step 2) at 10 to 20 DEG C5H5)2) Then adding sodium borohydride into the tetrahydrofuran solution, heating the reaction system to 40-50 ℃, and stirring for 6-10 hours to obtain a precipitate, wherein the molar ratio of the sodium borohydride to the manganese dicyclopentadienyl is about 1:0.8, and the atomic ratio of In to Mn is 1: 0.3.
4) Centrifugally separating the precipitate obtained in the step 3), washing the precipitate with deionized water, then placing the precipitate in a reaction kettle for reaction at 120 ℃ for 4 hours, taking out the precipitate, washing and drying the precipitate.
5) Then calcining the product obtained In the step 4) for 5 hours at 200 ℃ under the protection of nitrogen atmosphere to obtain In2O3/Au/MnO2Composite metal oxide particles, and then grinding the particles.
6) Dispersing graphene oxide In deionized water, performing ultrasonic dispersion to obtain a graphene oxide colloidal solution, adding the composite metal oxide particles obtained In the step 5) into the graphene oxide colloidal solution, and calcining for 4 hours at 300 ℃ under the protection of nitrogen atmosphere to obtain In with the surface modified by the graphene oxide2O3/Au/MnO2Composite metal oxide particlesWherein graphene oxide is reacted with In2O3/Au/MnO2The weight ratio of the composite metal oxide particles was 0.05: 1.
FIG. 1 shows In prepared by modifying graphene oxide on the surface2O3/Au/MnO2Scanning electron micrographs of the composite metal oxide particles. FIG. 2 shows In prepared by modifying graphene oxide on the surface2O3/Au/MnO2Transmission electron micrographs of the composite metal oxide particles. As can be seen from fig. 1 and 2, the prepared composite metal oxide particles are approximately square particles with uniform particle size, and have uniform and complete morphology. FIG. 3 shows In prepared by modifying graphene oxide on the surface2O3/Au/MnO2Gas sensitivity curve of composite metal oxide particles to 10ppm formaldehyde.
Example 2
In whose surface was modified with graphene oxide was prepared In the same manner as In example 1, except that the molar ratio of In to Au was controlled to 1:0.42O3/Au/MnO2A composite metal oxide gas-sensitive material.
Example 3
In whose surface was modified with graphene oxide was prepared In the same manner as In example 1, except that the molar ratio of In to Au was controlled to 1:0.22O3/Au/MnO2A composite metal oxide gas-sensitive material.
Example 4
In whose surface was modified with graphene oxide was prepared In the same manner as In example 1, except that the molar ratio of In to Mn was controlled to 1:0.12O3/Au/MnO2A composite metal oxide gas-sensitive material.
Example 5
In whose surface was modified with graphene oxide was prepared In the same manner as In example 1, except that the molar ratio of In to Mn was controlled to 1:0.62O3/Au/MnO2A composite metal oxide gas-sensitive material.
Example 6
Except that In step 6) is oxidized with graphene2O3/Au/MnO2Composite metal oxygenIn whose surface was modified with graphene oxide was prepared In the same manner as In example 1, except that the weight ratio of the compound particles was 0.08:12O3/Au/MnO2A composite metal oxide gas-sensitive material.
Comparative example 1
Except using MnCl2Instead of manganese (Mn (C) in step 3)5H5)2) In whose surface was modified with graphene oxide, In the same manner as In example 1, was prepared2O3/Au/MnO2A composite metal oxide gas-sensitive material.
Comparative example 2
In whose surface was modified with graphene oxide was prepared In the same manner as In example 1, except that step 2) was omitted, and Au was not doped2O3/MnO2A composite metal oxide gas-sensitive material.
Comparative example 3
Except for omitting step 3), without doping MnO2Except that In, the surface of which was modified with graphene oxide, was prepared In the same manner as In example 12O3the/Au composite metal oxide gas-sensitive material.
Comparative example 4
Except using Fe (NO)3)3Instead of manganese (Mn (C) in step 3)5H5)2) In prepared In the same manner as In example 1, except that sodium borohydride was not added, In of which surface was modified with graphene oxide2O3/Au/Fe2O3A composite metal oxide gas-sensitive material.
Comparative example 5
Except using SnCl2Instead of manganese (Mn (C) in step 3)5H5)2) In whose surface was modified with graphene oxide, In the same manner as In example 1, was prepared2O3/Au/SnO2A composite metal oxide gas-sensitive material.
Comparative example 6
Except for not carrying out step 6), i.e. not attachingIn was prepared In the same manner as In example 1, except that graphene oxide was used2O3/Au/SnO2A composite metal oxide gas-sensitive material.
Test example 1
The products prepared in examples 1 to 6 and comparative examples 1 to 6, respectively, were dry-milled in a mortar, and then an appropriate amount of deionized water and a small amount of terpineol were added, and wet-milled sufficiently to form a slurry. Dipping a small amount of slurry by a fine brush pen and uniformly coating the slurry on Al2O3And naturally drying the surface of the ceramic tube for 1h, calcining the surface of the ceramic tube for 2h at 450 ℃ in a muffle furnace under the nitrogen atmosphere, and then electrifying direct current on an aging table to age the surface of the ceramic tube for 7 days at 400 ℃ to obtain the gas sensor.
Gas sensitivity of the gas sensors prepared from the products prepared in examples 1 to 6 and comparative examples 1 to 6 to air containing 10ppm of formaldehyde was measured by measuring the gas sensing performance of the gas sensor using a WS-30B gas sensor tester, setting the heating voltage to 4.5V, and the results are shown in table 1. Sensitivity is defined as the ratio of the resistance of the gas sensor in air to its resistance in a reducing gas, i.e., Ra/Rg(ii) a The response time is defined as the time required for the resistance of the sensor to drop to 90% of the final resistance value; the recovery time is defined as the time required for the resistance of the sensor to recover 90% of the initial stable value.
TABLE 1
| Response time(s) | Recovery time(s) | Sensitivity (R)a/Rg) | |
| Example 1 | 8 | 12 | 34.7 |
| Example 2 | 17 | 27 | 24.1 |
| Example 3 | 14 | 22 | 24.2 |
| Example 4 | 15 | 20 | 27.3 |
| Example 5 | 17 | 26 | 26.8 |
| Example 6 | 19 | 23 | 20.3 |
| Comparative example 1 | 21 | 32 | 15.6 |
| Comparative example 2 | 45 | 75 | 7.3 |
| Comparative example 3 | 31 | 64 | 9.5 |
| Comparative example 4 | 29 | 58 | 10.3 |
| Comparative example 5 | 32 | 59 | 10.1 |
| Comparative example 6 | 36 | 60 | 8.9 |
Test example 2
The gas sensitivity of the gas sensor prepared from the product prepared in example 1 to air with different contents of formaldehyde was measured by using a WS-30B gas sensor tester to measure the gas sensitivity of the gas sensor, setting the heating voltage to 3.5V, and the results are shown in table 2:
TABLE 2
Test example 3
The gas-sensitive properties of the gas sensor were measured using a WS-30B gas sensor tester, setting the heating voltage to 3.5V, and measuring the sensitivity of the gas sensor made from the product prepared in example 1 to different flammable gases (10ppm), the results of which are shown in table 3.
TABLE 3
As seen from the data of test examples 1 to 3, In of surface-attached graphene oxide obtained according to the preparation method of the present invention2O3/Au/MnO2The gas sensitive element prepared from the metal oxide particle composite material has excellent sensitivity to combustible gases, particularly formaldehyde gas, high response speed, short recovery time and good application prospect.
Claims (16)
1. A gas sensor, which uses In with a graphene oxide-modified surface2O3/Au/MnO2The composite metal oxide gas-sensitive material is prepared,
the preparation method of the gas sensor comprises the following steps:
1) adding indium salt into a reactor, adding deionized water, controlling the concentration of the indium salt to be in the range of 0.05-0.5 mol/L, stirring at constant temperature of room temperature to 35 ℃, introducing ammonia gas, adjusting the pH to about 10, and reacting for 3-5 hours to obtain in (OH)3Stopping introducing ammonia gas after colloid formation, and washing the prepared colloidal solution with distilled water;
2) adding a chloroauric acid solution with the concentration of 0.01-0.2 mol/L into the precipitate, mixing, stirring at normal temperature to uniformly disperse the chloroauric acid solution, and then adjusting the pH value to about 10 by using ammonia water to form a colloidal solution;
3) dropwise adding manganese metallocenes (Mn (C) to the colloidal solution of the step 2) at 10 to 20 DEG C5H5)2) Then adding sodium borohydride into the tetrahydrofuran solution, heating the reaction system to 40-50 ℃, and stirring for 6-10 hours to obtain a precipitate;
4) centrifugally separating the precipitate obtained in the step 3), washing the precipitate with deionized water, then placing the precipitate into a reaction kettle for reaction at 120-140 ℃ for 2-6 hours, taking out the precipitate, washing and drying the precipitate;
5) then step 4)Calcining the product obtained In (1) for 3-6 hours at 200-400 ℃ under the protection of inert gas to obtain In2O3/Au/MnO2Compounding metal oxide particles, and then grinding and pulverizing the particles;
6) dispersing graphene oxide In deionized water, performing ultrasonic dispersion to obtain a graphene oxide colloidal solution, adding the composite metal oxide particles obtained In the step 5) into the graphene oxide colloidal solution, and calcining for 3-6 hours at 200-400 ℃ under the protection of inert gas to obtain In with graphene oxide attached to the surface2O3/Au/MnO2Composite metal oxide particles;
7) modifying the surface of the In prepared In the step 6) with graphene oxide2O3/Au/MnO2The composite metal oxide particles are dry-ground in a mortar for a period of time to make the particles uniform and fine, then a small amount of deionized water and a proper amount of adhesive are added, the mixture is fully ground to form slurry, the obtained slurry is coated on the surface of a substrate, then the substrate coated with the slurry is kept for 2 to 6 hours at the temperature of 300 to 550 ℃, then direct current is supplied on an aging table, and the aging is carried out for 5 to 7 days at the temperature of 400 ℃.
2. The gas sensor according to claim 1, wherein in the method for producing the gas sensor, the indium salt in step 1) is indium nitrate or indium chloride.
3. The gas sensor according to claim 1, wherein in (OH) in step 2) in the method for producing the gas sensor3The molar ratio of the gold chloride to the gold chloride acid is controlled between 1:0.02 and 1: 0.4.
4. The gas sensor according to claim 3, wherein in (OH) in step 2) in the method for producing the gas sensor3The molar ratio of the gold chloride to the gold chloride acid is controlled between 1:0.05 and 1: 0.2.
5. The gas sensor of claim 3, wherein the gas sensor is preparedIn the method, in (OH) in step 2)3The molar ratio of the gold chloride to the gold chloride acid is controlled between 1:0.07 and 1: 0.1.
6. The gas sensor according to claim 1, wherein In the method for producing a gas sensor, the molar ratio of In to Mn In step 3) is 1:0.1 to 1: 0.6.
7. The gas sensor according to claim 6, wherein In the method for producing a gas sensor, the molar ratio of In to Mn In step 3) is 1:0.2 to 1: 0.5.
8. The gas sensor according to claim 6, wherein In the method for producing a gas sensor, the molar ratio of In to Mn In step 3) is 1:0.3 to 1: 0.4.
9. The gas sensor according to claim 1, wherein in the method for producing a gas sensor, the molar ratio of sodium borohydride to chloroauric acid in step 3) is controlled to be 1:0.8 to 1: 1.
10. The gas sensor according to claim 1, wherein in the method for producing a gas sensor, the inert gas during calcination in steps 5) and 6) is selected from nitrogen or argon.
11. The gas sensor according to claim 1, wherein In the method for producing a gas sensor, graphene oxide and In step 6)2O3/Au/MnO2The weight ratio of the composite metal oxide particles is 0.04:1 to 0.08: 1.
12. The gas sensor according to claim 1, wherein In the method for producing a gas sensor, graphene oxide and In step 6)2O3/Au/MnO2The weight ratio of the composite metal oxide particles is 0.04:1 to 0.06: 1.
13. The gas sensor according to claim 1, wherein In the method for producing a gas sensor, graphene oxide and In step 6)2O3/Au/MnO2The weight ratio of the composite metal oxide particles was 0.05: 1.
14. The gas sensor according to claim 1, wherein in the method for producing a gas sensor, the substrate in step 7) is Al2O3A ceramic tube substrate or a glass substrate; the coating operation is any one of brushing, spraying and screen printing; the adhesive is terpineol.
15. The gas sensor according to claim 1, wherein in the method for producing a gas sensor, the substrate in step 7) is Al2O3A ceramic tube.
16. Use of the gas sensor of claim 1 for detecting the flammable gas formaldehyde.
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