CN101508423A - Method for producing reducing pollutant in water with ultraviolet light photocatalysis degradation - Google Patents
Method for producing reducing pollutant in water with ultraviolet light photocatalysis degradation Download PDFInfo
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- CN101508423A CN101508423A CNA2007100648118A CN200710064811A CN101508423A CN 101508423 A CN101508423 A CN 101508423A CN A2007100648118 A CNA2007100648118 A CN A2007100648118A CN 200710064811 A CN200710064811 A CN 200710064811A CN 101508423 A CN101508423 A CN 101508423A
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 23
- 239000003344 environmental pollutant Substances 0.000 title claims abstract description 12
- 231100000719 pollutant Toxicity 0.000 title claims abstract description 12
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 11
- 238000004519 manufacturing process Methods 0.000 title claims description 15
- 238000007146 photocatalysis Methods 0.000 title claims description 10
- 230000015556 catabolic process Effects 0.000 title claims description 8
- 238000006731 degradation reaction Methods 0.000 title claims description 8
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 30
- 238000000034 method Methods 0.000 claims abstract description 21
- 238000006243 chemical reaction Methods 0.000 claims abstract description 16
- 239000001301 oxygen Substances 0.000 claims abstract description 12
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 12
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 11
- 239000011941 photocatalyst Substances 0.000 claims abstract description 10
- 239000012298 atmosphere Substances 0.000 claims abstract description 4
- 150000001491 aromatic compounds Chemical class 0.000 claims description 4
- 230000008030 elimination Effects 0.000 claims description 4
- 238000003379 elimination reaction Methods 0.000 claims description 4
- 239000000463 material Substances 0.000 claims description 4
- 239000000356 contaminant Substances 0.000 claims description 2
- 238000007789 sealing Methods 0.000 claims description 2
- 239000001257 hydrogen Substances 0.000 abstract description 29
- 229910052739 hydrogen Inorganic materials 0.000 abstract description 29
- 230000002829 reductive effect Effects 0.000 abstract description 10
- 150000002431 hydrogen Chemical class 0.000 abstract description 4
- 238000013033 photocatalytic degradation reaction Methods 0.000 abstract description 4
- 239000000126 substance Substances 0.000 abstract description 3
- 238000005265 energy consumption Methods 0.000 abstract description 2
- 125000003118 aryl group Chemical group 0.000 abstract 1
- 238000000354 decomposition reaction Methods 0.000 abstract 1
- 125000000524 functional group Chemical group 0.000 abstract 1
- 230000017525 heat dissipation Effects 0.000 abstract 1
- 239000002957 persistent organic pollutant Substances 0.000 abstract 1
- MXWJVTOOROXGIU-UHFFFAOYSA-N atrazine Chemical compound CCNC1=NC(Cl)=NC(NC(C)C)=N1 MXWJVTOOROXGIU-UHFFFAOYSA-N 0.000 description 12
- 238000005516 engineering process Methods 0.000 description 7
- 238000006555 catalytic reaction Methods 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 238000006303 photolysis reaction Methods 0.000 description 5
- 239000003403 water pollutant Substances 0.000 description 5
- 239000003905 agrochemical Substances 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 3
- 238000013019 agitation Methods 0.000 description 3
- 230000006837 decompression Effects 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 239000004009 herbicide Substances 0.000 description 3
- 238000007254 oxidation reaction Methods 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- VGVRPFIJEJYOFN-UHFFFAOYSA-N 2,3,4,6-tetrachlorophenol Chemical class OC1=C(Cl)C=C(Cl)C(Cl)=C1Cl VGVRPFIJEJYOFN-UHFFFAOYSA-N 0.000 description 2
- 239000005631 2,4-Dichlorophenoxyacetic acid Substances 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 102000014150 Interferons Human genes 0.000 description 2
- 108010050904 Interferons Proteins 0.000 description 2
- 241000283973 Oryctolagus cuniculus Species 0.000 description 2
- 229910010413 TiO 2 Inorganic materials 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 238000004817 gas chromatography Methods 0.000 description 2
- 230000002363 herbicidal effect Effects 0.000 description 2
- 238000005286 illumination Methods 0.000 description 2
- 229940079322 interferon Drugs 0.000 description 2
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 2
- 229910052753 mercury Inorganic materials 0.000 description 2
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 230000005855 radiation Effects 0.000 description 2
- 230000028327 secretion Effects 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 1
- 239000002028 Biomass Substances 0.000 description 1
- QOFJYAIAWNGTOH-UHFFFAOYSA-N C(C)OCC(=O)O.ClC1=CC=CC(=C1)Cl Chemical compound C(C)OCC(=O)O.ClC1=CC=CC(=C1)Cl QOFJYAIAWNGTOH-UHFFFAOYSA-N 0.000 description 1
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 1
- 241000196324 Embryophyta Species 0.000 description 1
- 208000031320 Teratogenesis Diseases 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000007059 acute toxicity Effects 0.000 description 1
- 231100000403 acute toxicity Toxicity 0.000 description 1
- 239000005030 aluminium foil Substances 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- 235000011089 carbon dioxide Nutrition 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000004587 chromatography analysis Methods 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000000706 filtrate Substances 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 235000019253 formic acid Nutrition 0.000 description 1
- 238000010413 gardening Methods 0.000 description 1
- 230000002070 germicidal effect Effects 0.000 description 1
- 230000036571 hydration Effects 0.000 description 1
- 238000006703 hydration reaction Methods 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 238000004811 liquid chromatography Methods 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 238000005374 membrane filtration Methods 0.000 description 1
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 235000006408 oxalic acid Nutrition 0.000 description 1
- 238000010525 oxidative degradation reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000012797 qualification Methods 0.000 description 1
- 238000005070 sampling Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000000967 suction filtration Methods 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- 238000009281 ultraviolet germicidal irradiation Methods 0.000 description 1
- 238000001291 vacuum drying Methods 0.000 description 1
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Abstract
The invention relates to a method for realizing photocatalytic degradation of reductive pollutants in water through feeble ultraviolet light and simultaneously producing hydrogen, which is to realize the removal of the reductive pollutants in water body and simultaneously produce the hydrogen in a closed system with an atmosphere which is oxygen-free or has the oxygen content of less than 5 mmol.dm<-3>, in the presence of photocatalyst and under the irradiation of light with the wavelength of between 200 and 400 nanometers, wherein the reaction temperature is between 0 and 95 DEGC; the reaction pressure is between 0 and 3 atmospheric pressure; and the light intensity of a single ultraviolet light source is less than 100 mW.cm<-2>. Compared with the prior photocatalytic decomposition water, the method has the advantages that the hydrogen yield is obviously increased; reductive water body pollutants, particularly organic pollutants provided with a plurality of aromatic functional groups can be effectively removed; light energy and energy of the reductive pollutants can be converted into chemical energy of the hydrogen-the future energy carrier; and the energy consumption is low, heat dissipation is not required, and industrialization is easy.
Description
Technical field
The present invention relates to a kind of utilize faint ultraviolet light photocatalysis to eliminate to be extensive use of and environment in pollutents such as the agricultural chemicals that exists and the intermediate method of producing hydrogen simultaneously, relate in particular to the method that the especially fragrant pollutent of water pollutant that a kind of elimination has reductibility is significantly produced hydrogen simultaneously.
Background technology
Photochemical catalyzing is because it directly utilizes sunlight to produce the prospect of reproducible energy carrier hydrogen and obtains extensive concern.Ultimate principle is that photocatalyst is produced light induced electron and the photohole with reactive behavior under the effect of illumination.The light induced electron reductive water generates hydrogen, and the photohole oxidizing water is produced oxygen.The improvement of still needing that comes with some shortcomings of present photodissociation water technology:
1, the hydrogen of reaction production and oxygen mixed gas are easy to blast;
2, productive rate is lower.
Comprise that at 1 improvement of weak point compartmentation produces more complex technology such as hydrogen and oxygen, duplicature, perforation duplicature respectively.These technology realize hydrogen-oxygens separate be with the utilization ratio that reduces luminous energy and (or) to increase the complicacy of technology and cost be cost.
Comprise the photocatalyst of developing highlight catalytic active more and add electron donor(ED) at 2 improvement of weak point.Reported and added electron donor(ED) formaldehyde, formic acid, oxalic acid, methyl alcohol and biomass etc. can promote photochemical catalysis hydrogen under strong UV-light (as high voltage mercury lamp) irradiation production.And Weak ultraviolet power is low, and heat radiation is few, does not have harm, and therefore the value of application arranged very much.Other reductibility water pollutants such as faint ultraviolet light photocatalysis degradation agricultural chemicals, intermediate and can significantly promote the production of hydrogen that report is not also arranged.
Summary of the invention
The purpose of this invention is to provide a kind of method that realizes that reductive pollutants is produced hydrogen simultaneously in the faint water with ultraviolet light photocatalysis degradation.
Method provided by the invention particularly can significantly be produced hydrogen during aromatic compound such as agricultural chemicals, intermediate at photocatalytic degradation reductibility water pollutant.
For achieving the above object, the method for producing reducing pollutant in the water with ultraviolet light photocatalysis degradation provided by the invention in the sealing system less than 5mmol/l, adopts photocatalyst Pt/TiO in anaerobic or oxygen level
2, in wavelength be under the rayed of 200-400nm with the photocatalyst reaction, realize the elimination and the hydrogen gas production of pollutent in the water body.
Described method, wherein, temperature of reaction is 0-95 ℃.
Described method, wherein, reaction pressure is 0-3 normal atmosphere.
Described method, wherein, pollutent is the material with reductibility.
Described method, wherein, the material with reductibility is an aromatic compound.
Described method, wherein, the UV-light light intensity of single source is less than 100mWcm
-2
Described method wherein, adopts a plurality of ultraviolet sources to realize the regulation and control to light-catalysed contaminant degradation and hydrogen gas production efficient during rayed.
Compare with known technology, the present invention has the following advantages:
1, significantly increased the production of photochemical catalysis hydrogen;
2, pollutent has been eliminated in the simultaneous oxidation of photochemical catalysis production hydrogen;
3, the problem of having avoided hydrogen and oxygen reversed reaction and mixing to be easy to explode;
4, the chemical energy in luminous energy and the pollutent is converted into the chemical energy of future source of energy carrier hydrogen gas.
5, energy consumption is low, need not heat radiation, is easy to industrialization.
Description of drawings
The device synoptic diagram that Fig. 1 adopts for the present invention.
Fig. 2 is faint ultraviolet light photocatalysis reaction hydrogen output (a) and G-30027 concentration (b) synoptic diagram over time in the embodiment of the invention 1.
Fig. 3 is a faint ultraviolet light photocatalysis reaction hydrogen output (a) and 2 in the embodiment of the invention 2, and 4-D concentration is (b) synoptic diagram over time.
Embodiment
For further specifying the present invention, enumerate following examples, but be not to be used for limiting the defined invention scope of claim.
Significantly the principle of the principle of production hydrogen and photodissociation water is similar simultaneously for photocatalytic degradation reductibility water pollutant under anaerobic or the trace oxygen atmosphere.The prerequisite of producing hydrogen all is that the valence band current potential of semiconductor light-catalyst is lower than 0V (Vs NHE).And the absorption of ultraviolet and visible light requires semi-conductive energy gap between 1.6-6.3eV.Different is, and what photocatalysis oxidation reaction to take place is reductive pollutants.Because it is oxidized that reductive pollutants generally is easier to than water, and the thermodynamic(al)equilibrium that oxygen caused that photodissociation water oxidation produces and the generation of hydrogen-oxygen reversed reaction have been avoided, again because the singularity of structure such as some agricultural chemicals, intermediate and character, so significantly promoted the production of hydrogen.In order better to obtain target product hydrogen, logical rare gas element of needs or decompression remove the oxygen in the reaction system.
The method according to this invention, following embodiment reacts in the enclosed system and carries out.Enclosed system (referring to Fig. 1) is made up of insert reactor, vacuum unit part and Varian gas-chromatography.Magnetic agitation mixes reaction solution, and the gas in the whole enclosed system mixes (because this device is a known technology, and be not the emphasis that the present invention discusses, therefore be not described in detail) by Electromagnetic Recirculation Pump in the vacuum unit.
Embodiment 1
Photocatalyst Pt/TiO
2The light deposition preparation method: six hydration chloroplatinic acid aqueous solutions are added DegussaP25 TiO
2In the suspension of powder and water (add-on of catalyzer there is no strict the qualification among the present invention), under nitrogen atmosphere and magnetic agitation, 250W high voltage mercury lamp top irradiation 10h, 25 ± 3 ℃ of reactor constant temperature, reaction finishes the back with No. 5 sand core funnels and vacuum decompression filtration, use the deionized water wash photocatalyst again, the filtrate specific conductivity to the suction filtration is less than 10 μ scm
-1Behind 120 ℃ of vacuum-drying 10h, ground 300 mesh sieve.
Be that example describes with reduced form water pollutant G-30027 (atrazine) in the present embodiment.G-30027 is a large amount of selective herbicides that use, cause residual serious, the polluted underground water source.G-30027 is again a kind of internal secretion Interferon, rabbit, and biology is had teratogenesis, carcinogenic and cause female harm.Therefore the G-30027 of eliminating in the water body has important Significance for Environment.
With the 160ml G-30027 aqueous solution (concentration is 50umol/l) and the above-mentioned Pt1wt%/TiO that makes of 0.160g
2Photocatalyst places reactor, and the connection vacuum unit is an enclosed system.Decompression removes the oxygen in the system, and puts into high-purity argon gas as spirit.Magnetic agitation is opened light source 8W germicidal lamp (last 2/3rds parts of fluorescent tube are covered by aluminium foil) after 1 hour, the beginning light-catalyzed reaction.Gas composition directly detects by gas-chromatography, and the concentration decay of G-30027 is passed through from the thief hatch water sampling, and behind 0.22 μ m membrane filtration, the feed liquor analysis of hplc obtains again.Shown in Fig. 2 a, b, in faint UV-irradiation after 9 hours, the hydrogen of 72.5 μ mol produces, and is 7 times of photodissociation aquatic products hydrogen under the similarity condition; There is simultaneously the carbonic acid gas of 30.6 μ mol to generate again, because the carbon atom that has only G-30027 to contain in the solution, and the detected result of liquid chromatography shows that also the G-30027 of this moment existing 95.8% is degraded, so this process has significantly promoted the generation of hydrogen when having realized the photocatalytic degradation G-30027 really.
With the difference of embodiment 1 be reductive pollutants adopt the 2,4 dichloro benzene ethoxyacetic acid (2,4-D) (concentration is 1.0mmol/l).2,4-D is first weedicide in the world, also is second largest in the world selective herbicide, but also is the big broadleaf weed herbicide of the first in the world.Its by agricultural and gardening uses the same with G-30027 pollutes water body.2, though the 4-D acute toxicity is lower, it is a kind of potential internal secretion Interferon, rabbit, and its main biodegradable product is 2,4-two chlorophenols, and 2 of skin contact molten state, 4-two chlorophenols can cause death fast. therefore, and 2, the elimination of 4-D also has important Significance for Environment.
With the operation of embodiment 1, the result is shown in Fig. 3 a, b.The liquid-phase chromatographic analysis 2 of illumination after 2 hours, existing 84% degraded of 4-D.Produce hydrogen 38.4 μ mol hydrogen this moment.The aquatic hydrogen producing 0.925 μ mol of photodissociation under the similarity condition.Therefore, 2, the production of the promotion photochemical catalysis hydrogen that this aromatic compound of 4-D also can highly significant self has obtained oxidative degradation simultaneously.
Claims (7)
1, the method for producing reducing pollutant in a kind of water with ultraviolet light photocatalysis degradation in the sealing system less than 5mmol/l, adopts photocatalyst Pt/TiO in anaerobic or oxygen level
2, in wavelength be under the rayed of 200-400nm with the photocatalyst reaction, realize the elimination and the hydrogen gas production of pollutent in the water body.
2, the method for claim 1, wherein temperature of reaction is 0-95 ℃.
3, the method for claim 1, wherein reaction pressure is 0-3 normal atmosphere.
4, the method for claim 1, wherein pollutent is the material with reductibility.
5, method as claimed in claim 4, wherein, the material with reductibility is an aromatic compound.
6, the method for claim 1, wherein the UV-light light intensity of single source less than 100mWcm
-2
7,, wherein, adopt a plurality of ultraviolet sources during rayed to realize regulation and control to light-catalysed contaminant degradation and hydrogen gas production efficient as claim 1 or 6 described methods.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNA2007100648118A CN101508423A (en) | 2007-03-27 | 2007-03-27 | Method for producing reducing pollutant in water with ultraviolet light photocatalysis degradation |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNA2007100648118A CN101508423A (en) | 2007-03-27 | 2007-03-27 | Method for producing reducing pollutant in water with ultraviolet light photocatalysis degradation |
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| Publication Number | Publication Date |
|---|---|
| CN101508423A true CN101508423A (en) | 2009-08-19 |
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| CNA2007100648118A Pending CN101508423A (en) | 2007-03-27 | 2007-03-27 | Method for producing reducing pollutant in water with ultraviolet light photocatalysis degradation |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2011106864A1 (en) * | 2010-03-02 | 2011-09-09 | Trojan Technologies | Photocatalyst composition of matter |
| CN102747106A (en) * | 2012-07-02 | 2012-10-24 | 同济大学 | Method for increasing protein bio-hydrogen production |
| CN104760932A (en) * | 2015-03-25 | 2015-07-08 | 水沐清源（天津）能源环境技术有限公司 | Photocatalytic water decomposition hydrogen production plant |
| CN104843915A (en) * | 2014-10-30 | 2015-08-19 | 林志勋 | Portable sewage purification and electricity generation apparatus |
| CN106631671A (en) * | 2016-09-20 | 2017-05-10 | 郑州轻工业学院 | Method for preparing alkane and hydrogen by utilizing short-chain fatty acids in aqueous solution |
-
2007
- 2007-03-27 CN CNA2007100648118A patent/CN101508423A/en active Pending
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2011106864A1 (en) * | 2010-03-02 | 2011-09-09 | Trojan Technologies | Photocatalyst composition of matter |
| CN102947247A (en) * | 2010-03-02 | 2013-02-27 | 特洁安科技有限公司 | Photocatalyst composition of matter |
| US20130082009A1 (en) * | 2010-03-02 | 2013-04-04 | Trojan Technologies | Photocatalyst composition of matter |
| CN102747106A (en) * | 2012-07-02 | 2012-10-24 | 同济大学 | Method for increasing protein bio-hydrogen production |
| CN104843915A (en) * | 2014-10-30 | 2015-08-19 | 林志勋 | Portable sewage purification and electricity generation apparatus |
| CN104843915B (en) * | 2014-10-30 | 2017-06-13 | 林志勋 | A kind of Portable sewage purification and power generating device |
| CN104760932A (en) * | 2015-03-25 | 2015-07-08 | 水沐清源（天津）能源环境技术有限公司 | Photocatalytic water decomposition hydrogen production plant |
| CN106631671A (en) * | 2016-09-20 | 2017-05-10 | 郑州轻工业学院 | Method for preparing alkane and hydrogen by utilizing short-chain fatty acids in aqueous solution |
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Application publication date: 20090819 |