CN101940875B - Method for decomposing high-concentration methane mixed gas by fast photocatalysis by using low pressure mercury lamp - Google Patents
Method for decomposing high-concentration methane mixed gas by fast photocatalysis by using low pressure mercury lamp Download PDFInfo
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- CN101940875B CN101940875B CN201010516920A CN201010516920A CN101940875B CN 101940875 B CN101940875 B CN 101940875B CN 201010516920 A CN201010516920 A CN 201010516920A CN 201010516920 A CN201010516920 A CN 201010516920A CN 101940875 B CN101940875 B CN 101940875B
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Abstract
The invention discloses a method for decomposing high-concentration methane mixed gas by fast photocatalysis by using low pressure mercury lamp. According to the invention, photocatalysis decomposing of methane is implemented by using a low pressure mercury lamp (dominant wavelength is 253.7nm) as light source and TiO2 as catalyst in a manner of intermittent illumination, i.e. the lamp is turned on for a certain time, then turned off for a period of time and turned off once again. The method for decomposing high-concentration methane mixed gas by fast photocatalysis by using low pressure mercury lamp realizes 78-92% of the conversion rate and 10.15-884mg/ of the conversion speed, and has the advantages of fast conversion speed, high conversion rate, low conversion cost, etc.
Description
Technical field
The present invention relates to the method that high concentration methane blended gas is decomposed in a kind of normal temperature and pressure photocatalysis fast.
Background technology
Methane is a kind of greenhouse gases, its CH
3-H bond dissociation energy is 435 kJ/mol, is difficult for transforming.TiO
2Be that a kind of activity is very high, non-secondary pollution and cheap and maneuverable catalysis material.Mainly be to utilize vacuum-ultraviolet light (dominant wavelength is 185nm) in the light-catalysed research of methane at present as light source, TiO
2Be catalyst; And the mode that adopts is that continuous photodissociation is promptly opened vacuum UV lamp in entire reaction course continuously; The method of this vacuum UV lamp illumination can not realize in the application of reality: the one since the aerial transmission capacity of vacuum-ultraviolet light very a little less than, and price is more expensive; The 2nd, because gas has very big influence in adsorbing in advance of catalyst surface to catalytic efficiency, the transformation efficiency of methane is lower.Zhang Pengyi is (being that gas flow rate is that 8L/min, humidity are 26%-30%RH) under optimum experimental condition, and (can handle the methane concentration scope is about 0.01%, and the methane initial concentration is 60mg/m to adopt vacuum-ultraviolet light continuous illumination degraded to contain the low-concentration methane air
3), the conversion rate of methane is merely 7mg/
(China Environmental Science,, the 26th volume first phase: 653-656) in 2006.
Summary of the invention
Of the present invention in order to solve the above problems, provide a kind of normal temperature and pressure to utilize low pressure mercury lamp to be aided with TiO
2The method of photochemical catalyst quick optical catalytic decomposition high concentration methane blended gas.
Technical scheme of the present invention
Utilize low pressure mercury lamp (dominant wavelength is 253.7nm) and TiO
2The application of organic pollution aspects such as photocatalysis to degrade organic matter such as formaldehyde, chloroform, Polychlorinated biphenyls, organic phosphorus compound, polycyclic aromatic hydrocarbon is a lot, and photolytic process all is continuous illumination.But because methane is very stable, present this method is not but also being appeared in the newspapers aspect the methane photocatalytic degradation.
The present invention utilizes the mechanism of low pressure mercury lamp photocatalytic degradation methane to be: TiO
2Be a kind of N-type semiconductor, have photosensitive conducting property, generally be full of the low energy valence band (VB) of electronics and high energy conduction band (CB) formation of a sky, separate by the forbidden band between valence band and the conduction band by one.Can band and conduction band between band-gap energy be 3.2eV, its energy is equivalent to the ultraviolet light that wavelength is 387.5nm, when semiconductor is penetrated in the illumination that is equal to or greater than energy gap (Eg) when used energy, the electronics (e on the valence band
-) being excited transits to conduction band, on valence band, produces photohole (h
+):
, and under electric field action, separate and move to particle surface.Photohole has the extremely strong electronic capability that gets, and can capture the electronics in semiconductor grain surface organic matter or the solvent, makes the not light absorbing material of script all be activated oxidation, therefore has very strong oxidability, with the OH of its surface adsorption
-And H
2The O molecular oxygen changes into free radical OH, and the hydroxyl radical free radical attack methane molecule of generation makes it oxidation and decomposition, finally makes the methane degraded.
Method of the present invention is earlier to the ventilation of reaction vessel the inside; And adjustments of gas humidity, when conditions such as gas content, humidity all reach stable after, open low pressure mercury lamp and react; Close low pressure mercury lamp after reaching certain hour when turning on light; Turn off the light and turn on light again after reaching certain hour, repeat this process, in whole process, write down the content and the humidity of methane in the container simultaneously respectively with gas-chromatography and hygrometer.
Principle schematic such as Fig. 1 of the device that a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition high concentration methane blended gas of the present invention is used.Comprise among Fig. 1 that reactor 2, column type are coated with TiO
2Titanium mesh plate 3, low pressure mercury lamp 4, voltage-stablizer 5,220V power supply 6, Hygrothermograph inductor 8, Hygrothermograph data logger 9 have air inlet 1 and air hatch 7, the cylindrical TiO that is coated with on the reactor
2Titanium mesh plate 3 covers the luminous component of low pressure mercury lamp, and voltage-stablizer 5 is pressed for low pressure mercury lamp 4 provides galvanic current, and Hygrothermograph inductor 8 and Hygrothermograph data logger 9 detect and write down the temperature and the humidity of gaseous mixture in the reactor in real time.
A kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition high concentration methane blended gas specifically comprises the steps:
(1), reaction vessel is installed catalyst and be coated with TiO
2The titanium half tone feeds the gaseous mixture of being made up of methane and carbon dioxide inside, adjustments of gas content and humidity;
CH wherein
4Content accounts for 10% ~ 90% (volume ratio), CO
2Account for 90% ~ 10% (volume ratio), and adjustments of gas relative humidity is 15%;
Described catalyst is coated with TiO
2The titanium half tone is the column type cover, and diameter is 5cm, highly is 12.5cm, and wherein said catalyst is for being coated with TiO
2The TiO that is coated with in the titanium half tone
2The ratio of the mist volume (being the dischargeable capacity of reaction vessel) formed by itself and methane and carbon dioxide of amount be 0.06g/L;
(2), behind methane content and the moisture stable, sealed reactor, ON/OFF low pressure mercury lamp alternately, the open and close time of low pressure mercury lamp is 5～30min in each switch periods, and can be unequal, and writes down methane content and the humidity in each process;
Described low pressure mercury lamp dominant wavelength is 253.4nm, power 20W;
(3), when accumulative total after lighting time reaches certain hour, reaction finishes, and record methane content and humidity, calculates methane degradation rate and efficient.
Utilize in the method for the high methane concentration gaseous mixture of low pressure mercury lamp quick optical catalytic decomposition at this, catalyst is coated with TiO
2The titanium half tone is reusable, and can loss of activity.
Beneficial effect of the present invention
A kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition methane of the present invention compared with prior art because it utilizes low pressure mercury lamp (dominant wavelength is 253.7nm) as light source, to be coated with TiO
2The titanium half tone is a catalyst; Adopt intermittent illumination mode (promptly turn on light the regular hour, a period of time of turning off the light then turns on light again again) to carry out the photocatalysis of methane, be applicable to the conversion of methane in the high concentration methane blended gas; Conversion ratio is 78～92%, and conversion rate is 10.15～884mg/
, promptly having the conversion ratio height, conversion rate is fast, and transforms advantage with low cost etc.
Description of drawings
The principle schematic of the device that Fig. 1, a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition high concentration methane blended gas of the present invention are used.
The specific embodiment
Through embodiment the present invention is further set forth below, but do not limit the present invention.
The assay method of methane degradation rate and degradation rate: adopt the gas chromatography determination methane concentration, splitter is a stainless steel, and detector is the thermal conductance type;
Methane primary quantity * 100% before reacting in methane reduction/reactor before and after the reaction in degradation rate (%)=reactor;
Degradation rate (%)=degradation rate (%)/(reactor effective volume * total reaction time).Wherein total reaction time comprises light application time and illumination intermittent time.
Embodiment 1
This mist utilization be the high-pressure cylinder gaseous mixture, CH in the gas
4Content accounts for 90%, CO
2Account for 10%;
Adopt the glass reaction device, the effective volume of device is 2.2L; The low pressure mercury lamp dominant wavelength of utilizing is 253.4nm, power 20W; The employing radius is 5cm, highly covers the luminous component of low pressure mercury lamp for the cylindrical titanium mesh plate of 12.5cm; Adopt the humiture recorder of the big instrument plant in pool, Hangzhou to write down the temperature and humidity situation of change in the entire reaction course in addition.
The first step: connect experimental provision, and install catalyst and be coated with TiO
2Behind the titanium half tone, mist is fed in the reaction vessel, the content of adjustments of gas and humidity are measured the gas of gas port, treat that the methane content in the container reaches 0.6542g/L, and relative humidity reaches 15% simultaneously, stop air inlet and air inlet and gas outlet are sealed.
Second step: open low pressure mercury lamp and carry out light-catalyzed reaction, when continuous lighting time reached 10min, the gas that takes out gas port utilized gas chromatograph to measure, and after noting humidity and having got gas, closed low pressure mercury lamp.
The 3rd step: when the time of turning off the light reaches 10min, take out the gas of gas port again and measure, note gas humidity simultaneously, open low pressure mercury lamp then.
The 4th step: repeat third and fourth step, after the accumulative total lighting time reaches 150min, stop reaction, this moment, the content of methane was 0.0706g/L.
Calculating methane conversion is 89.21%, and conversion rate is 884mg/
.Conversion ratio is higher and conversion rate is very fast.Methane conversion speed 884mg/ wherein
Be higher than China Environmental Science far away, 2006, the 26th volume first phase: the employing vacuum-ultraviolet light continuous illumination degraded that 653-656 reported contains the low-concentration methane air, and (the methane initial concentration was 60mg/m
3, volume ratio is less than 0.01%) in the conversion rate 7mg/ of methane
, explanation thus, a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition methane of the present invention compared with prior art because it utilizes low pressure mercury lamp (dominant wavelength is 253.7nm) as light source, to be coated with TiO
2The titanium half tone is a catalyst; Adopt intermittent illumination mode (promptly turn on light the regular hour, a period of time of turning off the light then turns on light again again) to carry out the photocatalysis of methane, be applicable to the conversion of methane in the high concentration methane blended gas; It is fast to have conversion rate, transforms the advantage of grade with low cost.
Embodiment 2
This mist utilization be the high-pressure cylinder gaseous mixture, CH in the gas
4Content accounts for 50%, CO
2Account for 50%;
Adopt the glass reaction device, the effective volume of device is 2.2L; The low pressure mercury lamp dominant wavelength of utilizing is 253.4nm, power 20W; The employing radius is 5cm, highly covers the luminous component of low pressure mercury lamp for the cylindrical titanium mesh plate of 12.5cm; Adopt the humiture recorder of the big instrument plant in pool, Hangzhou to write down the temperature and humidity situation of change in the entire reaction course in addition.
The first step: connect experimental provision, and install catalyst and be coated with TiO
2Behind the titanium half tone, mist is fed in the reaction vessel, the content of adjustments of gas and humidity are measured the gas of gas port, treat that the methane content in the container reaches 0.3820g/L, and relative humidity reaches 15% simultaneously, stop air inlet and air inlet and gas outlet are sealed.
Second step: open low pressure mercury lamp and carry out light-catalyzed reaction, when continuous lighting time reached 10min, the gas that takes out gas port utilized gas chromatograph to measure, and after noting humidity and having got gas, closed low pressure mercury lamp.
The 3rd step: when the time of turning off the light reaches 10min, take out the gas of gas port again and measure, note gas humidity simultaneously, open low pressure mercury lamp then.
The 4th step: repeat third and fourth step, after the accumulative total lighting time reaches 150min, stop reaction, this moment, the content of methane was 0.0825g/L.
Calculating methane conversion is 78.40%, and conversion rate is 454mg/
.Conversion ratio is higher and conversion rate is very fast.Methane conversion speed 454mg/ wherein
Be higher than China Environmental Science far away, 2006, the 26th volume first phase: the employing VUV light degradation that 653-656 reported contains the low-concentration methane air, and (the methane initial concentration was 60mg/m
3, volume ratio is less than 0.01%) in the conversion rate 7mg/ of methane
, explanation thus, a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition methane of the present invention compared with prior art because it utilizes low pressure mercury lamp (dominant wavelength is 253.7nm) as light source, to be coated with TiO
2The titanium half tone is a catalyst; Adopt intermittent illumination mode (promptly turn on light the regular hour, a period of time of turning off the light then turns on light again again) to carry out the photocatalysis of methane, be applicable to the conversion of methane in the high concentration methane blended gas; It is fast to have conversion rate, transforms the advantage of grade with low cost.
Embodiment 3
This mist utilization be the high-pressure cylinder gaseous mixture, CH in the gas
4Content accounts for 10%, CO
2Account for 90%;
Adopt the glass reaction device, the effective volume of device is 2.2L; The low pressure mercury lamp dominant wavelength of utilizing is 253.4nm, power 20W; The employing radius is 5cm, highly covers the luminous component of low pressure mercury lamp for the cylindrical titanium mesh plate of 12.5cm; Adopt the humiture recorder of the big instrument plant in pool, Hangzhou to write down the temperature and humidity situation of change in the entire reaction course in addition.
The first step: connect experimental provision, and install catalyst and be coated with TiO
2Behind the titanium half tone, mist is fed in the reaction vessel, the content of adjustments of gas and humidity are measured the gas of gas port, treat that the methane content in the container reaches 0.0073g/L, and relative humidity reaches 15% simultaneously, stop air inlet and air inlet and gas outlet are sealed.
Second step: open low pressure mercury lamp and carry out light-catalyzed reaction, when continuous lighting time reached 10min, the gas that takes out gas port utilized gas chromatograph to measure, and after noting humidity and having got gas, closed low pressure mercury lamp.
The 3rd step: when the time of turning off the light reaches 10min, take out the gas of gas port again and measure, note gas humidity simultaneously, open low pressure mercury lamp then.
The 4th step: repeat third and fourth step, after the accumulative total lighting time reaches 150min, stop reaction, this moment, the content of methane was 0.0006g/L.
Calculating methane conversion is 91.78%, and conversion rate is 10.15mg/
.Conversion ratio is higher and conversion rate is very fast.Methane conversion speed 10.15mg/ wherein
Be higher than China Environmental Science, 2006, the 26th volume first phase: the employing VUV light degradation that 653-656 reported contained the conversion rate 7mg/ of the airborne methane of low-concentration methane
, explanation thus, a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition methane of the present invention compared with prior art because it utilizes low pressure mercury lamp (dominant wavelength is 253.7nm) as light source, to be coated with TiO
2The titanium half tone is a catalyst; Adopt intermittent illumination mode (promptly turn on light the regular hour, a period of time of turning off the light then turns on light again again) to carry out the photocatalysis of methane, be applicable to the conversion of methane in the high concentration methane blended gas; It is fast to have conversion rate, transforms the advantage of grade with low cost.
The above content is merely the basic explanation of the present invention under conceiving, and according to any equivalent transformation that technical scheme of the present invention is done, all should belong to protection scope of the present invention.
Claims (5)
1. a method of utilizing low pressure mercury lamp quick optical catalytic decomposition high concentration methane blended gas is characterized in that comprising the steps:
(1), place catalyst in the reaction vessel after, feed the mist of methane and carbon dioxide composition again in the reactor, adjustments of gas relative humidity is 15%;
The gaseous mixture that described methane and carbon dioxide are formed, CH wherein by volume
4Content accounts for 10% ~ 90%, CO
2Account for 90% ~ 10%;
Described catalyst is for being coated with TiO
2Titanium mesh plate
(2), behind methane content and the moisture stable, sealed reactor, alternately the ON/OFF low pressure mercury lamp is promptly turned on light a period of time earlier; Turn off the light a period of time again, turn on light a period of time again, turn off the light a period of time again; Carry out this process repeatedly, after the accumulative total lighting time reached certain hour, reaction finished;
Wherein said low pressure mercury lamp dominant wavelength is 253.4nm, and power is 20W.
2. a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition high concentration methane blended gas as claimed in claim 1 is characterized in that the described TiO of being coated with of step (1)
2The TiO that is coated with in the titanium mesh plate
2The ratio of the mist volume formed of quality and methane and carbon dioxide be 0.06g/L.
3. a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition high concentration methane blended gas as claimed in claim 1 is characterized in that step (1) is described
Be coated withTiO
2Titanium mesh plate is the column type cover, to cover the luminous component of low pressure mercury lamp.
4. a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition high concentration methane blended gas as claimed in claim 1 is characterized in that the described reaction vessel of step (1) is a column type.
5. a kind of method of utilizing low pressure mercury lamp quick optical catalytic decomposition high concentration methane blended gas as claimed in claim 1; It is characterized in that the alternately ON/OFF low pressure mercury lamp described in the step (2), the open and close time of low pressure mercury lamp is 5～30min in each switch periods.
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| US20130239469A1 (en) * | 2012-03-14 | 2013-09-19 | Board Of Regents, The University Of Texas System | Photochemical Processes and Compositions for Methane Reforming Using Transition Metal Chalcogenide Photocatalysts |
| CN103285799B (en) * | 2013-06-18 | 2015-03-18 | 上海电力学院 | Photocatalytic reactor for increasing photocatalytic degradation rate of methane and application of photocatalytic reactor |
| CN104710279A (en) * | 2013-12-16 | 2015-06-17 | 裴振昭 | Method for preparing methanol through photocatalytic oxidation of methane |
| CN104324673B (en) * | 2014-10-20 | 2016-07-06 | 内蒙古师范大学 | A kind of Revolving-drum photocatalytic reaction device |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN1657142A (en) * | 2004-12-10 | 2005-08-24 | 清华大学 | Air purifying technology |
| CN1695784A (en) * | 2005-03-30 | 2005-11-16 | 福州大学 | Composite photocatalytic reaction system for eliminating environmental pollutants in air or water efficiently |
| CN101613137A (en) * | 2008-06-25 | 2009-12-30 | 中国科学院大连化学物理研究所 | Reductive pollutants is produced the method for hydrogen simultaneously in the Photocatalytic Activity for Degradation water |
| CN201402227Y (en) * | 2009-03-16 | 2010-02-10 | 西安理工大学 | Photo-catalysis gas purifier |
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| US6241856B1 (en) * | 1997-11-11 | 2001-06-05 | The Board Of Regents Of The University Of Oklahoma | Enhanced oxidation of air contaminants on an ultra-low density UV-accessible aerogel photocatalyst |
| US7691342B2 (en) * | 2006-04-28 | 2010-04-06 | The United States Of America As Represented By The U.S. Environmental Protection Agency | Process using compact embedded electron induced ozonation and activation of nanostructured titanium dioxide photocatalyst for photocatalytic oxidation |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1657142A (en) * | 2004-12-10 | 2005-08-24 | 清华大学 | Air purifying technology |
| CN1695784A (en) * | 2005-03-30 | 2005-11-16 | 福州大学 | Composite photocatalytic reaction system for eliminating environmental pollutants in air or water efficiently |
| CN101613137A (en) * | 2008-06-25 | 2009-12-30 | 中国科学院大连化学物理研究所 | Reductive pollutants is produced the method for hydrogen simultaneously in the Photocatalytic Activity for Degradation water |
| CN201402227Y (en) * | 2009-03-16 | 2010-02-10 | 西安理工大学 | Photo-catalysis gas purifier |
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