CN107983342A - A kind of method of decomposing ethylene, its application in air purification and vegetables and fruits are fresh-keeping - Google Patents
A kind of method of decomposing ethylene, its application in air purification and vegetables and fruits are fresh-keeping Download PDFInfo
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- CN107983342A CN107983342A CN201610960614.3A CN201610960614A CN107983342A CN 107983342 A CN107983342 A CN 107983342A CN 201610960614 A CN201610960614 A CN 201610960614A CN 107983342 A CN107983342 A CN 107983342A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/42—Platinum
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/46—Ruthenium, rhodium, osmium or iridium
- B01J23/462—Ruthenium
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- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/48—Silver or gold
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/48—Silver or gold
- B01J23/52—Gold
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/06—Polluted air
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Abstract
A kind of method of decomposing ethylene, it is characterised in that the gas containing ethene and oxygen supports noble metal catalyst with carbon nanotubes and contacts, and is carbon dioxide and water by all or part of ethylene decomposition in gas.The above method can be used in air purification removing ethene, and during vegetables and fruits storage/transportation it is fresh-keeping.
Description
Technical field
This application involves carbon nanotubes to support catalytic degradation ethene skill under noble metal catalyst normal pressure and often/low-temperature atmosphere-pressure
Art, belongs to inorganic nano catalysis material field.
Background technology
With the continuous development of human civilization, the propulsion of process of industrialization, the life band of the use of fossil fuel to the mankind
While carrying out huge intellectual treasure, since the burn incompletely of fossil fuel causes atmosphere pollution, the also health care belt to the mankind
Great harm is carried out.The burn incompletely of fossil fuel cause ethylene gas discharge and nature in plant growing
Releasing ethylene gas in journey, causes the content of ethylene gas in air constantly to raise.According to the literature, atmosphere is discharged into every year
In ethene reach 18-45 × 106Ton.Micro ethene passes through a series of differentiation in air, may eventually form photochemical fog, leads
Serious atmosphere pollution is caused, health and the existence to the mankind bring great harm.At home, according to China Environmental Monitoring General Station
Statistics, 2013 to 2014 Pekinese's air qualities have reached " serious pollution ".National Middle East most area is also deep by mist
Haze perplexs, and Beijing whole city generally reaches pole heavily contaminated degree for a long time.In the world, what nineteen fifty-five Los Angeles,U.S occurred is photochemical
Learn smog episode and cause the dead people more than 400 of over-65s old man, ten hundreds of people by blood-shot eye illness, laryngalgia, brain be vexed etc. roll over by symptom
Mill, at the same time forest, vegetation, crops sparetime university area are aggrieved;The photochemical fog event that Tokyo in 1970 occurs causes entirely
6000 people of city is aggrieved.Meanwhile fruit and vegetable can discharge microscale ethylene in storage process, cause rotting for fruit and vegetable, give
The life of the mankind causes great economic loss.Development can be in efficient degradation air and fruit and vegetable is in storage process
The technology of microscale ethylene gas has extremely important scientific research, economy and realistic meaning.
Ethylene gas in air has the characteristics that low concentration, difficult absorption and sufficiently stable, causes its extremely difficult to be degraded.Mesh
The main method of microscale ethylene gas has physisorphtion, strong oxidizer oxidizing process, photocatalytic method and heat to urge in preceding elimination air
Change method.Physisorphtion is that ethene is adsorbed using activated carbon and molecular sieve etc., but adsorbance is limited, and in temperature
Easily it is desorbed in the case of elevated.Strong oxdiative method uses strong oxidizer oxidative degradation ethene, but easily environment is caused secondary
Pollution.Although photocatalytic method is a kind of environmentally protective effective way using sunlight photocatalysis degradation ethene, it is restricted
Influence in weather conditions and round the clock can not carry out practicality.Simultaneously as needed extremely in the storage process of fruit and vegetable
Exacting terms, such as:It is low temperature, humidity, closed lucifuge, environmentally protective.These exacting terms cause physisorphtion, Strong oxdiative
Agent oxidizing process and photocatalytic method can not use.Heat catalytic oxidation degrading ethylene is a kind of method of highly effective, at present both at home and abroad
More using some metal oxides (such as:Co3O4、MnO2Deng) or mesoporous silicon oxide as supported carrier noble metal thermocatalytic
Ethylene oxide, but general thermocatalyst catalytic degradation ethene need to be in 250 DEG C of progress, although there is few a part of catalyst to exist
At room temperature can thermocatalytic degrading ethylene, but under moist cryogenic conditions, the water generated during ethylene catalytic oxidation causes
These thermocatalysts can inactivate quickly and can not be practical.
Carbon nanotubes has broad application prospects as a kind of one-dimensional carbon nano material of new industrialized production,
Its higher specific surface area, excellent electric conductivity and many abnormal mechanics, electricity and chemical properties cause vast science
The concern of researcher, or even the application in real life, but utilize the super-hydrophobicity of carbon nanotubes and larger ratio table
Area, as supported carrier noble metal heat catalytic oxidation degrading ethylene, so far there is not yet any type of report.
The content of the invention
According to the one side of the application, there is provided your gold is carbon nanotubes is supported by a kind of method of decomposing ethylene, this method
Metal catalyst is used for catalytic degradation ethylene gas under normal pressure and low (normal) normal temperature and pressure.The carbon nanotubes supports noble metal catalyst
With excellent hydrophobicity;When the carbon nanotubes supports noble metal catalyst and contains platinum, to big under room temperature (25 DEG C) normal pressure
Ethene in gas has efficient catalytic performance and stability, to second under low temperature (0 DEG C) normal pressure of simulation fruit and vegetable storage
Alkene has efficient catalytic performance and stability.
The method of the decomposing ethylene, it is characterised in that the gas containing ethene and oxygen is received with carbon nanotubes and/or carbon
Mitron supports noble metal catalyst contact, is carbon dioxide and water by all or part of ethylene decomposition in gas.
The carbon nanotubes and carbon nanotubes, which support noble metal catalyst, has super-hydrophobicity.
Preferably, the noble metal that the carbon nanotubes is supported in noble metal catalyst contains in Au Ag Pt Pd, ruthenium extremely
Few one kind.It is further preferred that the noble metal that the carbon nanotubes is supported in noble metal catalyst contains in silver, platinum, palladium, ruthenium
It is at least one.
Preferably, the noble metal that the carbon nanotubes is supported in noble metal catalyst includes platinum.
It is further preferred that the noble metal that the carbon nanotubes supports in noble metal catalyst is platinum;Or the carbon is received
The noble metal that mitron is supported in noble metal catalyst includes platinum and selected from least one of gold, silver, palladium, ruthenium metal.
Preferably, the carbon nanotubes is supported in noble metal catalyst, the mass percentage of noble metal for 0.1%~
10%.It is further preferred that the carbon nanotubes is supported in noble metal catalyst, the mass percentage of noble metal for 1~
5%.As a kind of embodiment, the carbon nanotubes is supported in noble metal catalyst, the mass percentage of noble metal for 1~
3%.As another embodiment, the carbon nanotubes is supported in noble metal catalyst, and the mass percentage of noble metal is 3
~5%.
Preferably, the molar ratio m of ethene and oxygen in the gasEthene:mOxygen≤1。
As a kind of embodiment, the oxygen sources in the gas are in air.
As a kind of specific embodiment, the gas is the air containing ethene.
Preferably, in the gas, the molar content of ethene is no more than 1000ppm.It is further preferred that the gas
In, the molar content of ethene is no more than 500ppm.It is further preferred that in the gas, the molar content of ethene is 1ppm
~500ppm.
Carbon nanotubes supports noble metal catalyst and is used for ethylene decomposition, (such as 250 DEG C) can both carry out, and also might be used at high temperature
To be carried out under low temperature or room temperature;Both can also be reacted under normal pressure with compressive reaction.
As a preferred embodiment, the carbon nanotubes support noble metal in noble metal catalyst include platinum,
During at least one of silver, palladium, ruthenium metal, the gas containing ethene and oxygen supports noble metal catalyst with carbon nanotubes
The temperature of contact is 0 DEG C~50 DEG C.It is further preferred that the noble metal that the carbon nanotubes is supported in noble metal catalyst includes
During at least one of platinum, silver, palladium, ruthenium metal, the gas containing ethene and oxygen supports noble metal with carbon nanotubes and urges
The temperature of agent contact is 0 DEG C~40 DEG C.
As a preferred embodiment, the noble metal that the carbon nanotubes is supported in noble metal catalyst includes platinum
When, it is 0 DEG C~50 DEG C that the gas containing ethene and oxygen and carbon nanotubes, which support the temperature that noble metal catalyst contacts,.Into
One step is preferably, described to contain ethene and oxygen when the noble metal that the carbon nanotubes supports in noble metal catalyst includes platinum
Gas and carbon nanotubes to support the temperature that noble metal catalyst contacts be 0 DEG C~40 DEG C.
According to the another aspect of the application, there is provided the method is used for the application for removing ethene in air purification.
Preferably, the noble metal that the carbon nanotubes is supported in noble metal catalyst contains in platinum, silver, palladium, ruthenium at least
It is a kind of.
It is further preferred that the noble metal that the carbon nanotubes is supported in noble metal catalyst contains platinum.
It is further preferred that the noble metal that the carbon nanotubes supports in noble metal catalyst is platinum;Or the carbon
Noble metal in nanotube supported noble metal catalyst includes platinum and selected from least one of gold, silver, palladium, ruthenium metal.
According to the another aspect of the application, there is provided carbon nanotubes supports noble metal catalyst in vegetables and fruits storage/transportation process
Application in fresh-keeping, the noble metal that the carbon nanotubes is supported in noble metal catalyst contain at least one in platinum, silver, palladium, ruthenium
Kind.
Preferably, the noble metal that the carbon nanotubes is supported in noble metal catalyst contains platinum.
It is further preferred that the noble metal that the carbon nanotubes supports in noble metal catalyst is platinum;Or the carbon is received
The noble metal that mitron is supported in noble metal catalyst includes platinum and selected from least one of gold, silver, palladium, ruthenium metal.
The beneficial effect of the application includes but not limited to:
(1) method provided herein, supports noble metal catalyst by carbon nanotubes first and is reacted for ethylene decomposition,
New reaction method is provided for ethylene degradative.
(2) method provided herein, available for air contaminant treatment, removes a small amount of existing ethene in air, and
There is efficient catalytic performance and stability to the ethene in air under room temperature (25 DEG C) normal pressure.
(3) method provided herein, it is fresh-keeping available for vegetables and fruits, it is normal in the low temperature (0 DEG C) of simulation fruit and vegetable storage
Pressure has efficient catalytic performance and stability to ethene.
Brief description of the drawings
Fig. 1 is the different noble metal catalyst thermocatalytics degraded second that carbon nanotubes supports that mass fraction is 3% in embodiment 2
Alkene figure.
Fig. 2 is the Pt catalyst thermo-catalytic degrading ethylene figures that carbon nanotubes supports different quality containing in embodiment 2.
Fig. 3 is that to support Pt catalyst that mass fraction is 3% long under room temperature (25 DEG C) normal pressure for carbon nanotubes in embodiment 3
The stability diagram of time catalytic degradation ethene.
Fig. 4 is that to support Pt catalyst that mass fraction is 3% long under low temperature (0 DEG C) normal pressure for carbon nanotubes in embodiment 4
The stability diagram of time catalytic degradation ethene.
Fig. 5 is different hydrophilic and hydrophobic supported carrier mass fractions are 3% in embodiment 5 Pt catalyst at room temperature (25 DEG C)
The stability diagram of long-time catalytic degradation ethene under normal pressure.
Embodiment
The application is described in detail with reference to embodiment, but the application is not limited to these embodiments.
In embodiment, ethene and carbon dioxide use the GC9720 type gas phases of Zhejiang Fu Li analytical instrument limited company
Chromatograph detects.
Hydrophilic and hydrophobic is detected using the JC2000D3 type contact angle instruments of Shanghai Zhongchen digital technology equipment Co., Ltd.
The carbon nanotubes is purchased from Sinopharm Chemical Reagent Co., Ltd..
The preparation of 1 sample of embodiment
Carbon nanotubes supports the preparation of noble metal catalyst sample
Concretely comprise the following steps:1 gram of the carbon nanotubes of 40-60 mesh is added in 100 milliliters of ethanol and with stirring, then
Adding noble metal source, (addition of noble metal source supports precious metal element in noble metal catalyst sample according to gained carbon nanotubes
Mass content is calculated), continue to stir half an hour.The solution is dry in 80 DEG C of constant temperature stirring evaporations, and then 200 DEG C of air move back
When fire 2 is small, finally when hydrogen annealing 2 is small, that is, obtains carbon nanotubes and support noble metal catalyst sample.
Gained sample number into spectrum, gained carbon nanotubes support precious metal element mass content in noble metal catalyst sample, tool
The species and quality for the precious metal salt that body uses are as shown in table 1.
Table 1
The preparation of other supported carrier noble metal catalyst samples
Specific steps are sameCarbon nanotubes supports the preparation of noble metal catalyst sample, difference is, by carbon nanotubes
The carbon black (CB) and graphene phase carbon nitride (g-C of 40-60 mesh are replaced with respectively3N4), gained sample number into spectrum, used carrier,
Precious metal element mass content, the species of the precious metal salt specifically used and quality are as shown in table 2 in gained sample.
Table 2
2 thermopnore thermocatalytic degrading ethylene gas of embodiment
Test respectively gained sample Au-3%, Ag-3% in carbon nanotubes MCNTs, embodiment 1, Pd-3%, Ru-3%,
The catalytic performance of Pt-3%, Pt-2% and Pt-1% thermocatalytic degrading ethylene gas in thermopnore.Detailed process is as follows:
The sample 0.2g of 40-60 mesh is weighed respectively, is encased in the U-shaped quartz ampoule that internal diameter is 4 millimeters, reaction temperature uses
Temperature programming, programming rate are 1 DEG C/min, are raised to 250 DEG C for 25 DEG C from room temperature, reacting gas is the sky containing 200ppm ethene
Gas, gas flow rate 10mL/min, every 5 minutes sampling once, use gas chromatograph detection reactor in ethylene gas with
And the concentration change of reaction product carbon dioxide.
Test result is as shown in Figure 1, MCNTs represents that the test result of sample carbon nanotubes, Au represent sample Au- in figure
3% test result, Ag represent that the test result of sample Ag-3%, Pd represent that the test result of sample P d-3%, Ru represent sample
The test result of product Ru-3%, Pt represent the test result of sample P t-3%;As seen from the figure, noble metal loadings are identical
In the case of 3wt%, during 0~130 DEG C of reaction temperature, catalyst reaction activity is Pt-3%>Ru-3%>Pd-3%>Ag-
3%>Au-3%~MCNTs;When reaction temperature is more than 130 DEG C, catalyst reaction activity is Pt-3%~Ru-3%~Pd-3%>
Au-3%>Ag-3%>MCNTs.At room temperature, gas flow rate is the Pt catalyst that the mass fraction that carbon nanotubes supports is 3%
Being capable of degradable ethene during 10mL/min.
As shown in Fig. 2, with the increase of Pt mass fractions, the performance that carbon nanotubes supports Pt catalyst gradually steps up, when
When the mass fraction of Pt reaches 3%, which can at room temperature, the complete catalytic degradation second when flow velocity is 10mL/min
Alkene.
It is extremely excellent to support noble metal catalyst catalytic performance for carbon nanotubes as can be seen here, and it is normal which is used for room temperature
Degrading ethylene is depressed, control atmosphere pollution has very big actual application value.
Microscale ethylene gas in degraded air under the conditions of 3 thermopnore analog room temperature of embodiment
In testing example 1 gained sample P t-3% in thermopnore under the conditions of analog room temperature degrade air in microscale ethylene
The catalytic performance of gas, carries out under room temperature (25 DEG C) normal pressure.Detailed process is as follows:
Weigh 0.2g sample P t-3%, being encased in internal diameter is in 4 millimeters of U-shaped quartz ampoule, temperature control in 25 DEG C of room temperature,
Reacting gas is the air containing 200ppm ethene, and gas flow rate 10mL/min, sampled once every 5 minutes, using gas phase
The concentration of ethylene gas and reaction product carbon dioxide changes in chromatograph detection reactor.
Test result as shown in figure 3, sample P t-3% shows excellent ethylene catalyst degradation property and stability,
120 interior catalyst when small can keep degradable ethene.The catalyst is entirely capable of being practically applicable to administering under normal temperature and pressure as can be seen here
Atmosphere pollution.
Microscale ethylene gas in degraded refrigerating chamber under 4 thermopnore of embodiment simulation cryogenic conditions
Gained sample P t-3% simulates micro second in refrigerating chamber of degrading under cryogenic conditions in thermopnore in testing example 1
The catalytic performance of alkene gas, carries out under low temperature (0 DEG C) normal pressure.Detailed process is as follows:
Weigh 0.2g sample P t-3%, being encased in internal diameter is in 4 millimeters of U-shaped quartz ampoule, temperature control in 25 DEG C of room temperature,
Reacting gas is the air containing 200ppm ethene, and gas flow rate 10mL/min, sampled once every 5 minutes, using gas phase
The concentration of ethylene gas and reaction product carbon dioxide changes in chromatograph detection reactor.
Test result is as shown in figure 4, sample P t-3% remains able to degradable ethene, Er Qie under low temperature (0 DEG C)
Property retention is highly stable in two hours, and degradation rate drops to 70% or so after four hours.
Its superior catalytic performance of the catalyst and its stability make it in the ultralow temperature of fruit and vegetable storage as can be seen here
Have a good application prospect under degree, while also bring along huge economic benefit.
5 sample P t-3% of embodiment, sample P t-3%-CB, sample P t-3%-g-C3N4Thermopnore mould at ambient temperature
Intend the contrast of microscale ethylene gas in degraded air
Gained sample P t-3%, sample P t-3%-CB and sample P t-3%-g-C in testing example 13N4In thermopnore
Under the conditions of analog room temperature degrade air in microscale ethylene gas catalytic performance, carried out under room temperature (25 DEG C) normal pressure.Specific mistake
Journey is as follows:
Sample P t-3%, sample P t-3%-CB and sample P t-3%-g-C are weighed respectively3N4Each 0.2g, being encased in internal diameter is
In 4 millimeters of U-shaped quartz ampoule, temperature control is in 25 DEG C of room temperature, and reacting gas is the air containing 200ppm ethene, gas flow rate
For 10mL/min, every sampling in 5 minutes once, ethylene gas and reaction product two in reactor are detected using gas chromatograph
The concentration change of carbonoxide.The hydrophilic and hydrophobic of catalyst is characterized using contact angle instrument test contact angle.
Test result as shown in figure 5, sample P t-3% has a maximum contact angle, its catalytic stability be also it is best,
Sample P t-3%-g-C3N4Contact angle is minimum, its catalytic stability is worst, it is seen that the hydrophilic and hydrophobic and catalyst of catalyst
The stability of performance has direct relation, and catalyst hydrophobicity is better, and its catalytic performance is more stable.Therefore selection has hydrophobic
Property material can have good catalytic performance and stability as supported carrier precious metal catalyst ethene.
The above, is only several embodiments of the application, any type of limitation is not done to the application, although this Shen
Please with preferred embodiment disclose as above, but and be not used to limitation the application, any person skilled in the art, is not taking off
In the range of technical scheme, make a little variation using the technology contents of the disclosure above or modification is equal to
Case study on implementation is imitated, is belonged in the range of technical solution.
Claims (10)
- A kind of 1. method of decomposing ethylene, it is characterised in that the gas containing ethene and oxygen and carbon nanotubes and/or carbon nanometer Pipe supports noble metal catalyst contact, is carbon dioxide and water by all or part of ethylene decomposition in gas.
- 2. according to the method described in claim 1, it is characterized in that, the carbon nanotubes supports your gold in noble metal catalyst Belong to selected from least one of Au Ag Pt Pd, ruthenium.
- 3. according to the method described in claim 1, it is characterized in that, the carbon nanotubes supports your gold in noble metal catalyst Category includes at least one of silver, platinum, palladium, ruthenium.
- 4. according to the method described in claim 1, it is characterized in that, the carbon nanotubes supports your gold in noble metal catalyst Category includes platinum;Preferably, the noble metal that the carbon nanotubes supports in noble metal catalyst is platinum;Or the carbon nanotubes support it is expensive Noble metal in metallic catalyst includes platinum and selected from least one of gold, silver, palladium, ruthenium metal.
- 5. according to the method described in claim 1, it is characterized in that, the carbon nanotubes is supported in noble metal catalyst, your gold The mass percentage of category is 0.1%~10%;Preferably, the carbon nanotubes is supported in noble metal catalyst, and the mass percentage of noble metal is 1~5%.
- 6. according to the method described in claim 1, it is characterized in that, the oxygen sources in the gas are in air.
- 7. the method according to claim 1 or 6, it is characterised in that in the gas, the molar content of ethene is no more than 1000ppm;It is further preferred that in the gas, the molar content of ethene is no more than 500ppm;It is further preferred that in the gas, the molar content of ethene is 1ppm~500ppm.
- 8. according to the method described in claim 1 or 3 or 4, it is characterised in that the gas containing ethene and oxygen is received with carbon The temperature that mitron supports noble metal catalyst contact is 0 DEG C~50 DEG C;Preferably, the temperature that the gas containing ethene and oxygen and carbon nanotubes support that noble metal catalyst contacts is 0 DEG C ~40 DEG C.
- 9. any the method for claim 1 to 8 is used for the application for removing ethene in air purification.
- 10. carbon nanotubes supports application of the noble metal catalyst in vegetables and fruits storage/transportation process is fresh-keeping, the carbon nanotubes load Noble metal in supported noble metal catalyst contains at least one of platinum, silver, palladium, ruthenium.
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