CN111001295A - Device and method for degrading VOCs (volatile organic compounds) by ultraviolet illumination and monatomic catalyst - Google Patents
Device and method for degrading VOCs (volatile organic compounds) by ultraviolet illumination and monatomic catalyst Download PDFInfo
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- B01D53/34—Chemical or biological purification of waste gases
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Abstract
The invention relates to a device and a method for degrading VOCs (volatile organic compounds) by ultraviolet illumination in cooperation with a monatomic catalyst. Comprises a gas distribution system, an ultraviolet photolysis-monoatomic catalysis system and a detection system which are connected in sequence. The temperature of the catalytic oxidation reactor is controlled to be 20-40 ℃, the pressure is controlled to be 0.1-0.15 MPa, and the humidity is controlled to be 10-50%; dividing gas discharged from the lower part of the reactor and having complete reaction into three paths, wherein one part of the gas is directly introduced into a gas chromatograph for online detection of VOCs conversion rate, the other part of the gas is introduced into a methane converter for detection of the mineralization rate of VOCs, and the last part of the gas is discharged after being processed to reach the standard. Effectively reducing the loading of noble metal (b)<1 wt%), improves the utilization rate of atoms, and promotes O by ultraviolet irradiation2Activating at the interface site of the monatomic catalyst to generate high-activity oxygen species, and efficiently catalyzing and oxidizing VOCs (volatile organic compounds) to degrade into CO2And H2And O, further improving the reaction activity.
Description
Technical Field
The invention relates to the field of industrial waste gas purification, in particular to a device and a method for degrading VOCs (volatile organic compounds) by ultraviolet irradiation in cooperation with a monatomic catalyst.
Background
VOCs are used as a large category of air pollutants, so that the air pollutants are seriously harmful to human bodies and have serious carcinogenic, teratogenic and mutagenic effects; but also can cause great harm to the environment, and the VOCs can take place atmosphere photochemical reaction and lead to the production of photochemistry smog, and the VOCs is the precursor matter of haze simultaneously. The great harm of VOCs to human bodies and environment arouses the attention of relevant national departments, and relevant laws and regulations are made to limit the discharge of VOCs. By 2020, VOCs emission reduction in key areas and key industries is more than 10%.
At present, a catalytic combustion method is common in VOCs treatment methods. The method utilizes the catalytic action of the catalyst to realize the catalytic oxidative degradation of the toluene at higher temperature (>100 ℃). Therefore, the preparation of a high activity catalyst is the key to the process. The catalytic oxidation catalysts for VOCs are mainly divided into two main types, one is a supported noble metal catalyst (such as Pt-series and Pd-series catalysts), and the other is a transition metal catalyst (such as oxides of Mn, Ce, Cu, Co and the like). Although both of these catalysts have a certain effect on the degradation of VOCs, the high loading (even up to 30 wt%) of noble metals causes the catalyst to have a high cost, which is not favorable for the large-scale application of the supported noble metal nano-catalyst; the transition metal oxide catalyst needs higher reaction temperature (>200 ℃) to obtain higher reaction activity, and the energy consumption is higher. The monatomic noble metal catalyst can greatly reduce the loading of noble metals and improve the utilization efficiency of noble metal atoms, and simultaneously adopts transition metal oxides with the same catalytic activity as a carrier to jointly catalyze and oxidize the degradation of VOCs by utilizing the synergistic effect between the noble metal monatomic and the transition metal oxides. However, at present, ozone is often used as an oxidant for catalytic degradation of VOCs at normal temperature, and incomplete reaction of ozone in the reaction process is likely to cause secondary pollution, so that it is necessary to use oxygen as the oxidant for catalytic degradation of VOCs.
With the introduction of energy-saving and environmental protection concepts, the drawback of non-sustainable development exposed by the traditional catalytic combustion method and the catalytic ozonation method has become increasingly unacceptable.
Disclosure of Invention
Photochemistry, an emerging science, has been rapidly developed. Compared with the traditional catalytic combustion, the photochemical catalyst is cleaner and more energy-saving. Therefore, a new method for catalyzing and degrading aromatic VOCs enhanced by ultraviolet light is needed to be solved.
The object of the present invention is to provide a device for purifying waste gas containing VOCs, which solves the problems mentioned in the background art.
The invention relates to a method for efficiently catalyzing and oxidizing VOCs (volatile organic compounds) to decompose at normal temperature by adopting oxygen with the same oxidizing property to replace polluting ozone and activating the oxygen by utilizing ultraviolet light to generate oxidizing species (such as hydroxyl radicals, superoxide ions and the like) with higher oxidizing activity. The principle of the invention is as follows: under the irradiation of 2 ultraviolet lamp tubes, the interface active site of the monatomic catalyst greatly promotes oxygen (O)2) To an active state (e.g. superoxide ion O)2-Peroxo ion O2 2-Etc.), a large number of active oxygen species collide with the reaction substrate adsorbed on the active site to transfer energy to the reaction substrate molecules, so that the substrate molecules reach a high-energy excited state, thereby catalyzing the substrate molecules VOCs to be oxidized into CO2And H2O。
In order to achieve the above purpose, the technical scheme adopted by the invention is as follows:
a device for degrading VOCs (volatile organic compounds) by ultraviolet light and monatomic catalysis comprises a gas distribution system, an ultraviolet photolysis-monatomic catalysis system and a detection system which are sequentially connected.
The gas distribution system consists of an air generator 1, a nitrogen steel cylinder 2, a mass flow meter 3, a VOCs (volatile organic chemicals) purging bottle 4, a water vapor bubbling bottle 5 and a mixer 6; the air generator 1 is sequentially connected with a mass flow meter 3 and a mixer 6 through pipelines; the outlet of the nitrogen steel cylinder 2 is divided into two paths, and the first path of nitrogen pipeline is sequentially connected with a VOCs (volatile organic compounds) purging cylinder 4 filled with VOCs and a mixer 6; the second path of nitrogen pipeline is connected with a steam bubbling bottle 5 for generating steam and a mixer 6 in sequence; the outlet of the mixer 6 is connected to the upper inlet of the reaction tube of the reactor 8 via a mixer line.
The ultraviolet photolysis-monoatomic catalysis system consists of two ultraviolet lamp tubes 7, a reactor 8 and an outer layer of light shield; the bottom outlet of the reaction tube 8 is provided with three pipelines; the first outlet gas branch pipeline is connected with the methane reformer 9 so that a part of gas passes through the methane reformer to detect the mineralization rate of VOCs; the second outlet gas branch pipeline is connected with the gas chromatograph 10 so as to lead a part of gas to carry out on-line detection on the conversion rate of VOCs through the gas chromatograph; the third outlet gas line is connected to a treatment unit to process a portion of the gas to a standard and then vent it.
The detection system consists of a gas chromatograph 10 and a methane converter 9.
The device is used for degrading VOCs by ultraviolet irradiation in cooperation with the monatomic catalyst; VOCs is introduced into the reaction system in a nitrogen purging mode, VOCs, air and water vapor are mixed in a mixing bottle and then enter the reaction device, reacted gas respectively enters the gas chromatography detector, the ozone detection device and the methane conversion furnace, and finally the conversion rate and the mineralization rate of VOCs are calculated.
The device is used for degrading VOCs by ultraviolet irradiation in cooperation with the monatomic catalyst; the method comprises the following operation steps:
(1) gas distribution: the method specifically comprises the following steps: mixing air with the flow rate of 100-;
(2) catalytic oxidation reaction: under the irradiation of ultraviolet lamp light, the gas in the mixer is completely mixed and then enters a reaction tube filled with catalyst in the reactor from the upper part of the reactor, and then is discharged from the lower part of the reaction tube; the temperature of the reactor is controlled to be 20-40 ℃, the pressure is controlled to be 0.1-0.15 MPa, and the humidity is controlled to be 10-50%;
(3) dividing gas discharged from the lower part of the reactor and having complete reaction into three paths, wherein one part of the gas is directly introduced into a gas chromatograph for online detection of VOCs conversion rate, the other part of the gas is introduced into a methane converter for detection of the mineralization rate of VOCs, and the last part of the gas is discharged after being processed to reach the standard.
The photocatalyst is preferably 0.2 to 1 weight percent of Pt/CeO2Single atom catalyst or 0.2 wt% -1 wt% Au/CeO2A single atom catalyst or 0.2 to 1 weight percent of Pd/TiO2Isomonatomic catalyst, herein dividedOther than CeO2And TiO2The percentage content of the noble metal is calculated on the basis of the mass of (A).
The oxygen source in the device is from an air generator.
The ultraviolet light source comprises 2 ultraviolet light sources with effective wavelength of 254nm and effective ultraviolet radiation intensity of 78 μ W/cm2The ultraviolet lamp tube.
The dosage of the monatomic photocatalyst is such that the ratio of the height of a catalyst bed layer to the diameter of the reactor is 8-10, and the particle size of the monatomic photocatalyst is such that the ratio of the diameter of the reactor to the diameter of the catalyst particles is 6-12.
Compared with the prior art, the device and the method for degrading VOCs by ultraviolet light and monatomic catalyst have the remarkable advantages that:
firstly, the noble metal single-atom catalyst loaded by active metal oxide is adopted instead of the metal oxide catalyst or the loaded noble metal nano-catalyst, so that the loading amount of the noble metal is effectively reduced<1 wt%), improves the utilization rate of atoms, and promotes O by ultraviolet irradiation2Activating at the interface site of the monatomic catalyst to generate high-activity oxygen species, and efficiently catalyzing and oxidizing VOCs (volatile organic compounds) to degrade into CO2And H2And O, further improving the reaction activity.
And secondly, the higher reaction activity promotes the catalytic degradation reaction of the VOCs to be carried out at room temperature, and compared with the traditional catalytic combustion process (100-300 ℃), the energy consumption is greatly reduced.
Thirdly, the invention adopts oxygen as oxidant instead of ozone, is clean and environment-friendly, utilizes ultraviolet lamp light irradiation to make up activity reduction caused by adopting oxygen, and can efficiently and environmentally degrade VOCs at normal temperature.
Drawings
FIG. 1 is a flow chart of UV light in cooperation with a monatomic catalyst to degrade VOCs. Wherein 1-an air generator; 2-nitrogen cylinder; 3-mass flow meter; 4-VOCs purging bottle; 5-steam bubbling bottle; 6-a mixer; 7-ultraviolet lamp tube; 8-a reactor; 9-a methane reformer; 10-gas chromatograph.
Detailed Description
The technical solution of the present patent will be described in further detail with reference to the following embodiments.
Referring to fig. 1, an apparatus for catalyzing degradation of VOCs by ultraviolet light in cooperation with monatomic light includes a gas distribution system, an ultraviolet photolysis-monatomic catalysis system, and a detection system. The gas distribution system consists of an air generator 1, a nitrogen steel cylinder 2, a mass flow meter 3, a VOCs (volatile organic chemicals) purging bottle 4, a water vapor bubbling bottle 5 and a mixer 6; the air generator 1 is sequentially connected with a mass flow meter 3 and a mixer 6 through pipelines; the outlet of the nitrogen steel cylinder 2 is divided into two paths, and the first path of nitrogen pipeline is sequentially connected with a VOCs (volatile organic compounds) purging cylinder 4 filled with VOCs and a mixer 6; the second nitrogen pipeline is connected with a water vapor bubbling bottle 5 for generating water vapor and a mixer 6 in sequence; the outlet of the mixer 6 is connected to the upper inlet of the reaction tube of the reactor 8 via a mixer line. The ultraviolet photolysis-monoatomic catalysis system consists of two ultraviolet lamp tubes 7, a reactor 8 and an outer layer of light shield; the bottom outlet of the reaction tube 8 is provided with three pipelines; the first outlet gas branch pipeline is connected with the methane reformer 9 so that a part of gas passes through the methane reformer to detect the mineralization rate of VOCs; the second outlet gas branch pipeline is connected with the gas chromatograph 10 so as to lead a part of gas to carry out on-line detection on the conversion rate of VOCs through the gas chromatograph; the third outlet gas line is connected to a treatment unit to process a portion of the gas to a standard and then vent it. The detection system consists of a gas chromatograph 10 and a methane converter 9.
The air generator 1 is sequentially connected with a mass flow meter 3 and a mixer 6 through pipelines, the outlet of the nitrogen steel cylinder 2 is divided into two paths, the first path of nitrogen pipeline is sequentially connected with a VOCs blowing bottle 4 and the mixer 6 which are provided with VOCs, the second path of nitrogen pipeline is sequentially connected with a steam bubbling bottle 5 and the mixer 6 which generate steam, the outlet of the mixer 6 is connected with the upper inlet of the reaction tube of the reactor 8 through a mixer pipeline, the bottom outlet of the reaction tube is divided into three paths by a main pipe, the first outlet gas branch pipeline is connected with a methane reformer 9 so as to lead a part of gas to pass through the methane reformer to detect the mineralization rate of VOCs, the second outlet gas branch pipeline is connected with the gas chromatograph 10 so as to lead a part of gas to carry out on-line detection on the conversion rate of VOCs by the gas chromatograph, the third outlet gas pipeline is connected with a processing device so as to lead a part of gas to be processed and discharged after reaching the standard.
In a preferred embodiment of the present invention, quartz wool is placed in the upper and lower ends of a reaction tube filled with a monatomic catalyst to prevent blowing out of the catalyst.
Example 1
Adopting oxygen generated by an air generator, adopting 2 branches of oxygen with the effective wavelength of 254nm and the effective radiation intensity of ultraviolet light of 78 mu W/cm2The ultraviolet lamp tube is used as an ultraviolet light source.
Selecting 0.2 wt% Pt/CeO2Monoatomic catalyst, 0.2 wt% Pt/CeO2The ratio of the height of the monatomic catalyst bed to the reactor diameter was 8, 0.2 wt% Pt/CeO2The ratio of the particle size of the monatomic photocatalyst to the diameter of the catalyst particles was 6.
The invention discloses a device and a method for degrading VOCs (volatile organic compounds) by ultraviolet illumination and a monatomic catalyst, which comprises the following operation steps:
(1) the gas distribution specifically comprises the following steps: mixing air with the flow rate of 100mL/min and nitrogen buffer gas with the flow rate of 100mL/min, and then feeding the mixture, nitrogen containing VOCs with the flow rate of 1mL/min and nitrogen containing water vapor with the flow rate of 1mL/min into a mixer for mixing, wherein the concentration of VOCs in the mixer is 100 ppm;
(2) the catalytic oxidation reaction specifically comprises the following steps: under the irradiation of ultraviolet lamp light, the gas in the mixer is completely mixed and then enters a reaction tube filled with catalyst in the reactor from the upper part of the reactor, and then is discharged from the lower part of the reaction tube; the temperature of the reactor is controlled to be 20 ℃, the pressure is controlled to be 0.1MPa, and the humidity is controlled to be 10 percent;
(3) dividing gas discharged from the lower part of the reactor and having complete reaction into three paths, wherein one part of the gas is directly introduced into a gas chromatograph for online detection of VOCs conversion rate, the other part of the gas is introduced into a methane converter for detection of the mineralization rate of VOCs, and the last part of the gas is discharged after being processed to reach the standard.
Example 2:
adopting oxygen generated by an air generator, adopting 2 branches of oxygen with the effective wavelength of 254nm and the effective radiation intensity of ultraviolet light of 78 mu W/cm2The ultraviolet lamp tube is used as an ultraviolet light source.
0.6 wt% of Au/CeO was selected2Monoatomic catalyst, 0.6 wt% Au/CeO2The ratio of the height of the monatomic catalyst bed to the reactor diameter was 9, 0.6 wt% Au/CeO2The ratio of the particle size of the monatomic photocatalyst to the diameter of the catalyst particles was 9.
The invention discloses a device and a method for degrading VOCs (volatile organic compounds) by ultraviolet illumination and a monatomic catalyst, which comprises the following operation steps:
(1) the gas distribution specifically comprises the following steps: mixing air with the flow rate of 1300mL/min and nitrogen buffer gas with the flow rate of 550mL/min, and then feeding the mixture, VOCs-containing nitrogen with the flow rate of 15.5mL/min and water vapor-containing nitrogen with the flow rate of 25.5mL/min into a mixer for mixing, wherein the concentration of VOCs in the mixer is 550 ppm;
(2) the catalytic oxidation reaction specifically comprises the following steps: under the irradiation of ultraviolet lamp light, the gas in the mixer is completely mixed and then enters a reaction tube filled with catalyst in the reactor from the upper part of the reactor, and then is discharged from the lower part of the reaction tube; the temperature of the reactor is controlled to be 30 ℃, the pressure is controlled to be 0.125MPa, and the humidity is controlled to be 30 percent;
(3) and dividing the gas which is completely reacted and discharged from the lower part of the reactor into three paths, and directly introducing one part of the gas into a gas chromatograph for online detection of VOC.
Example 3:
adopting oxygen generated by an air generator, adopting 2 branches of oxygen with the effective wavelength of 254nm and the effective radiation intensity of ultraviolet light of 78 mu W/cm2The ultraviolet lamp tube is used as an ultraviolet light source.
Selecting 1 wt% Pd/TiO2Monatomic catalyst, 1 wt% Pd/TiO2The ratio of the height of the monatomic catalyst bed to the reactor diameter was 10, 1 wt% Pd/TiO2The ratio of the particle size of the monatomic photocatalyst to the diameter of the catalyst particles was 12.
The invention discloses a device and a method for degrading VOCs (volatile organic compounds) by ultraviolet illumination and a monatomic catalyst, which comprises the following operation steps:
(1) the gas distribution specifically comprises the following steps: mixing air with the flow rate of 2500mL/min and nitrogen buffer gas with the flow rate of 1000mL/min, and then feeding the mixture, nitrogen containing VOCs with the flow rate of 30mL/min and nitrogen containing water vapor with the flow rate of 50mL/min into a mixer for mixing, wherein the concentration of VOCs in the mixer is 1000 ppm;
(2) the catalytic oxidation reaction specifically comprises the following steps: under the irradiation of ultraviolet lamp light, the gas in the mixer is completely mixed and then enters a reaction tube filled with catalyst in the reactor from the upper part of the reactor, and then is discharged from the lower part of the reaction tube; the temperature of the reactor is controlled to be 40 ℃, the pressure is controlled to be 0.15MPa, and the humidity is controlled to be 50 percent;
(3) and dividing the gas which is completely reacted and discharged from the lower part of the reactor into three paths, and directly introducing one part of the gas into a gas chromatograph for online detection of VOC.
While the methods and techniques of the present invention have been described in terms of preferred embodiments, it will be apparent to those of ordinary skill in the art that variations and/or modifications of the methods and techniques described herein may be made without departing from the spirit and scope of the invention. It is expressly intended that all such similar substitutes and modifications apparent to those skilled in the art are deemed to be within the spirit, scope and content of the invention.
Claims (9)
1. A device for degrading VOCs (volatile organic compounds) by ultraviolet light and monatomic catalysis is characterized by comprising a gas distribution system, an ultraviolet photolysis-monatomic catalysis system and a detection system which are sequentially connected.
2. The device of claim 1, wherein the gas distribution system comprises an air generator 1, a nitrogen gas steel cylinder 2, a mass flow meter 3, a VOCs purging bottle 4, a water vapor bubbling bottle 5 and a mixer 6; the air generator 1 is sequentially connected with a mass flow meter 3 and a mixer 6 through pipelines; the outlet of the nitrogen steel cylinder 2 is divided into two paths, and the first path of nitrogen pipeline is sequentially connected with a VOCs (volatile organic compounds) purging cylinder 4 filled with VOCs and a mixer 6; the second path of nitrogen pipeline is connected with a steam bubbling bottle 5 for generating steam and a mixer 6 in sequence; the outlet of the mixer 6 is connected to the upper inlet of the reaction tube of the reactor 8 via a mixer line.
3. The apparatus according to claim 1, wherein said uv photolysis-monatomic catalytic system comprises two uv lamps 7, a reactor 8 and an outer light shield; the bottom outlet of the reaction tube 8 is provided with three pipelines; the first outlet gas branch pipeline is connected with the methane reformer 9 so that a part of gas passes through the methane reformer to detect the mineralization rate of VOCs; the second outlet gas branch pipeline is connected with the gas chromatograph 10 so as to lead a part of gas to carry out on-line detection on the conversion rate of VOCs through the gas chromatograph; the third outlet gas line is connected to a treatment unit to process a portion of the gas to a standard and then vent it.
4. The apparatus of claim 1, wherein said detection system is comprised of a gas chromatograph 10 and a methane reformer 9.
5. A method for degrading VOCs using ultraviolet light in conjunction with a monatomic catalyst using the apparatus of claim 1; the method is characterized by comprising the following operation steps:
(1) gas distribution: the method specifically comprises the following steps: mixing air with the flow rate of 100-;
(2) catalytic oxidation reaction: under the irradiation of ultraviolet lamp light, the gas in the mixer is completely mixed and then enters a reaction tube filled with catalyst in the reactor from the upper part of the reactor, and then is discharged from the lower part of the reaction tube; the temperature of the reactor is controlled to be 20-40 ℃, the pressure is controlled to be 0.1-0.15 MPa, and the humidity is controlled to be 10-50%;
(3) dividing gas discharged from the lower part of the reactor and having complete reaction into three paths, wherein one part of the gas is directly introduced into a gas chromatograph for online detection of VOCs conversion rate, the other part of the gas is introduced into a methane converter for detection of the mineralization rate of VOCs, and the last part of the gas is discharged after being processed to reach the standard.
6. The method of claim 5, wherein the photocatalyst is 0.2 wt% to 1 wt% of Pt/CeO2Monoatomic catalyst, 0.2 wt% -1 wt% Au/CeO2A single atom catalyst or 0.2 to 1 weight percent of Pd/TiO2A monatomic catalyst.
7. The method as set forth in claim 5, wherein the source of oxygen in the device is from an air generator.
8. The method of claim 5, wherein the ultraviolet light source comprises 2 ultraviolet light beams having an effective wavelength of 254nm and an effective ultraviolet radiation intensity of 78 μ W/cm2The ultraviolet lamp tube.
9. The method according to claim 5, wherein the monatomic photocatalyst is used in such an amount that the ratio of the height of the catalyst bed to the diameter of the reactor is 8 to 10, and the particle diameter of the monatomic photocatalyst is such that the ratio of the diameter of the reactor to the diameter of the catalyst particles is 6 to 12.
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| CN111603929A (en) * | 2020-05-30 | 2020-09-01 | 西安交通大学 | System and method for treating VOCs by excimer light coupling catalysis means |
| CN111760452A (en) * | 2020-06-29 | 2020-10-13 | 盐城工学院 | Experimental device for testing performance of photocatalytic ozone synergistic catalytic degradation of volatile organic gas and operation process thereof |
| CN112156773A (en) * | 2020-10-29 | 2021-01-01 | 苏州圣典企业管理咨询有限公司 | High-efficiency VOC photolysis catalyst |
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