CN1460542A - Photo-magnetic concerted catalysis technology and application thereof in degrading organic pollutants - Google Patents
Photo-magnetic concerted catalysis technology and application thereof in degrading organic pollutants Download PDFInfo
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- CN1460542A CN1460542A CN 03137060 CN03137060A CN1460542A CN 1460542 A CN1460542 A CN 1460542A CN 03137060 CN03137060 CN 03137060 CN 03137060 A CN03137060 A CN 03137060A CN 1460542 A CN1460542 A CN 1460542A
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- 238000005516 engineering process Methods 0.000 title claims abstract description 12
- 238000006555 catalytic reaction Methods 0.000 title claims abstract description 8
- 239000002957 persistent organic pollutant Substances 0.000 title claims abstract description 8
- 230000002153 concerted effect Effects 0.000 title claims abstract description 7
- 230000000593 degrading effect Effects 0.000 title abstract 3
- 230000001699 photocatalysis Effects 0.000 claims abstract description 24
- 238000006243 chemical reaction Methods 0.000 claims abstract description 22
- 239000003054 catalyst Substances 0.000 claims abstract description 16
- 238000005859 coupling reaction Methods 0.000 claims abstract description 8
- 238000007146 photocatalysis Methods 0.000 claims description 23
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 10
- 239000004408 titanium dioxide Substances 0.000 claims description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- 239000008187 granular material Substances 0.000 claims description 4
- 230000005672 electromagnetic field Effects 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- 238000010574 gas phase reaction Methods 0.000 claims description 2
- 229910052742 iron Inorganic materials 0.000 claims description 2
- 239000007791 liquid phase Substances 0.000 claims description 2
- 229910052759 nickel Inorganic materials 0.000 claims description 2
- 229910052763 palladium Inorganic materials 0.000 claims description 2
- 229910052697 platinum Inorganic materials 0.000 claims description 2
- 229910052703 rhodium Inorganic materials 0.000 claims description 2
- 229910052707 ruthenium Inorganic materials 0.000 claims description 2
- 239000007787 solid Substances 0.000 claims description 2
- 229910052723 transition metal Inorganic materials 0.000 claims description 2
- 150000003624 transition metals Chemical class 0.000 claims description 2
- 238000005286 illumination Methods 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 13
- 230000008569 process Effects 0.000 abstract description 11
- 230000033558 biomineral tissue development Effects 0.000 abstract description 5
- 239000002912 waste gas Substances 0.000 abstract description 2
- 239000002351 wastewater Substances 0.000 abstract description 2
- 230000002195 synergetic effect Effects 0.000 abstract 1
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 15
- 150000003254 radicals Chemical class 0.000 description 12
- 230000000694 effects Effects 0.000 description 9
- 150000001875 compounds Chemical class 0.000 description 6
- 239000007789 gas Substances 0.000 description 5
- 229910010413 TiO 2 Inorganic materials 0.000 description 4
- 238000002474 experimental method Methods 0.000 description 4
- 238000011160 research Methods 0.000 description 4
- 230000005284 excitation Effects 0.000 description 3
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Substances [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 230000005364 hyperfine coupling Effects 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000003287 optical effect Effects 0.000 description 2
- 150000005837 radical ions Chemical class 0.000 description 2
- 239000000376 reactant Substances 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 230000005526 G1 to G0 transition Effects 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 239000012159 carrier gas Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
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- 238000010586 diagram Methods 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 239000000839 emulsion Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 230000005283 ground state Effects 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 230000000977 initiatory effect Effects 0.000 description 1
- 230000005426 magnetic field effect Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 239000005416 organic matter Substances 0.000 description 1
- MUMZUERVLWJKNR-UHFFFAOYSA-N oxoplatinum Chemical compound [Pt]=O MUMZUERVLWJKNR-UHFFFAOYSA-N 0.000 description 1
- 229910003446 platinum oxide Inorganic materials 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000007348 radical reaction Methods 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 239000000126 substance Chemical group 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 238000002604 ultrasonography Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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Abstract
The invention discloses a photo-magnetic concerted catalysis technology and application thereof in degrading organic pollutants. The structure of the device is that a photocatalytic reactor irradiated by sunlight or ultraviolet rays is placed in an external magnetic field to form the magnetic field-photocatalytic coupling reaction device. The invention adds a magnetic field on the basis of the original photocatalytic reactor, and generates a photocatalysis-magnetic field synergistic effect by the influence of the magnetic field on the catalyst and the intermediate in the photocatalytic process, thereby greatly improving the photocatalytic conversion efficiency and the mineralization rate of organic pollutants and achieving the purpose of efficiently degrading the organic pollutants in waste water and waste gas.
Description
Technical field
The present invention relates to catalysis technique and the application in environmental pollution improvement thereof, a kind of specifically light-magnetic concerted catalysis technology and the application on degradable organic pollutant thereof.
Background technology
With TiO
2Conductor oxidate is photocatalysis technology be widely used at aspects such as clear energy sources, environmental protection and the new materials background and the important meaning on basis.Yet, TiO
2The photochemical catalyst quantum efficiency is too low, and is not high to solar energy utilization rate, seriously restricting the extensive extensive use of photocatalysis technology.For improving the efficient of photochemical catalyst and photocatalytic process, carried out a large amount of exploratory developments both at home and abroad.To TiO
2Photochemical catalyst has carried out comprising mix various metals and nonmetalloid, compound second kind of semiconductor even the third semiconductor, the loadization on carrier and change acidity and manufacturing lattice defect or the like modification widely or modification research; Photocatalytic process has been carried out additional various outfields, as electric field, microwave field, ultrasound field, plasma etc. with fortifying catalytic agent absorptivity, photo-generated carrier separative efficiency with prolong the exploration that its life-span is a purpose.These methods all in various degree make TiO
2Photocatalysis performance improve, but still unsatisfactory.
Magnetic field as with above-mentioned outfield equally to the influential physical factor of electric charge, photon and phonon, it is used in photocatalysis and is not but seen report always.People once did considerable research with regard to magnetic field to the influence of chemical reaction before last century the seventies and since do not find tangible effect once quiet get off.Recently, Bhaswust is at one piece of comment (Chem.Soc.Rev., 2002, summed up achievement in research in recent decades 31:301), point out that magnetic field really can be not influential to the reaction of most ground state molecule, yet, the reaction that takes place between free radical or radical ion is had very important influence.It is admitted facts that thereby influence of magnetic field atomic nucleus and electronic spin state influence the multiple degree of excitation state free radical.Usually radical pair is with singlet (S attitude) and triplet state (T
+, T
0, T) form exists, but the compound of radical pair can only occur between the singlet, therefore, the carrying out of reaction can be controlled by the rate of selecting that influences severe in magnetic field.During no magnetic field, singlet and triplet state are degeneracy on energy, can transform mutually; Under the effect in magnetic field, singlet is not owing to there is Net magnetic moment, and energy remains unchanged, and triplet state is then passed through the division of Zeeman effect generation energy.If the effect of Zeeman effect is less than hyperfine coupling effect, still can transform mutually between singlet and the triplet state, magnetic field is then very little to the reaction influence, but when the Zeeman effect surpasses hyperfine coupling, have only between the To attitude in singlet and the triplet state and can exchange, reaction will be subjected to the influence of magnetic field effect.People such as Turro are about the research (J.Am.Chem.Soc.1980 of magnetic field to the styrene emulsion polymerisation, 102:7391) from experimentally having confirmed the influence of magnetic field to free radical reaction course, magnetic field energy is controlled the productive rate of reaction, the molecular weight of polymer and the regularity of chain effectively.
Photocatalytic process is one and forms the chain processes that secondary process, free radical electric charge and energy transmit mutually and series of steps such as compound and chemical bond rupture subsequent process are formed that electronics-holoe carrier primary process, these carrier initiation reaction thing molecules produce charged free radical by the optical excitation catalyst.When these processes are carried out continuously can with the final non-selectivity of organic matter be oxidized to nontoxic carbon dioxide and water.But a plurality of processes wherein are reversible, promptly by elementary e-that optical excitation produced and h+ to life-span very short (ns level), if can not separate effectively, e-will get back to valence band by conduction band and compound again with the hole soon, make transition invalid; Pass through O
2, though life-span of surface hydroxyl or formed secondary free radical of other molecule trapping electronics or hole or radical ion is a little longer, do not have enough stationary phases also can be compound fast, and reaction is interrupted.Obviously, apply external magnetic field, can increase the ratio of triplet state free radical by the zeeman effect, this will prolong the life-span of free radical, reduce the compound of free radical, thereby improve light-catalysed efficient.
Summary of the invention
In order to overcome the existing inefficient problem of photocatalysis technology, the invention provides a kind of magnetic-light concerted catalysis technology that can improve the photocatalysis quantum efficiency, promptly act on the photocatalysis system simultaneously, can reach organic pollution in efficient decomposition waste water and the waste gas by magnetic field and sunshine or ultraviolet.
The technical solution adopted in the present invention is: the photo catalysis reactor of sunshine or ultraviolet ray irradiation is placed externally-applied magnetic field, constitute a magnetic field-photocatalysis coupled reaction unit, it is characterized in that: the artificial light source that the catalyst in the photo catalysis reactor is applied sunshine or wavelength 200～800nm, add simultaneously the electromagnetic field of intensity a 10～2000mT again, constituted magnetic field of the present invention-photocatalysis coupled reaction unit.Photochemical catalyst in the described photo catalysis reactor is the titanium dioxide solid that titanium dioxide, particularly transition metal (as Fe, Co, Ni, Pt, Pd, Ru, Rh etc.) mix and modifies; To gas-phase reaction, catalyst granules places in the quartz glass tubular type reactor, and magnetic field means and light source place around the reactor; To liquid phase reactor, catalyst granules is suspended in the interior solution of quartz glass reaction container, and the placement of reactor outer wall is close in magnetic field, and the set-up mode of light source has two kinds: the one, place the reaction vessel center; The 2nd, around magnetic field places reaction vessel.When reacting gas or flow of solution were crossed light of the present invention-magnetic catalytic reactor, under the synergy of catalyst and light, magnetic, the organic pollution that it contained then was decomposed, and what flow out from reactor outlet then is cleaned gas or solution.
Effect of the present invention is: because photo catalysis reactor has been added a magnetic field, it is by influencing photochemical catalyst level structure and photocatalysis intermediate free radical species electron spin state, photocatalytic process is played auxiliary or collaborative facilitation, thereby improved organic photocatalytic conversion efficient and mineralization rate greatly.Therefore, the present invention can reach the purpose to the organic pollution efficient degradation.
Description of drawings
The invention will be further described below in conjunction with drawings and Examples.
Fig. 1 is the block diagram of the technology of the present invention.Photo catalysis reactor is applied light source (comprise sunshine and artificial ultraviolet source) and magnetic field simultaneously, after contaminated air or flow of solution are crossed reactor, then be cleaned.
The specific embodiment
Embodiment 1
Platinum oxide/titanium dioxide (Pt/TiO with the sol-gel process preparation
2, contain Pt 0.5wt%) and be that catalyst is a reactant with containing benzene air (500ppm, carrier gas employing standard purifies air).Adopt the reaction unit of Fig. 1, first experiment only adds light source (four 8W wavelength 254nm uviol lamps), and second experiment adds the electromagnet magnetic field sources of above-mentioned light source and 70mT field intensity simultaneously.When reactant gas with the flow velocity of 30ml/min during continuously by this reactor, the concentration and the CO of residue benzene in the reactor outlet gas when using the reaction of U.S. HP6890 type gas chromatograph on-line determination to reach stable state
2Concentration, and calculate the conversion ratio and the mineralization rate of benzene.Experimental result is: by first experiment condition, when promptly having light source not have magnetic field, the stable state conversion ratio and the mineralization rate of benzene are respectively 15.5% and 19.0%; And by second experiment condition, when promptly applying light source and magnetic field simultaneously, the stable state conversion ratio and the mineralization rate of benzene are respectively 22.0% and 52%.
Claims (6)
1, the photo catalysis reactor with sunshine or ultraviolet ray irradiation places externally-applied magnetic field, constitute a magnetic field-photocatalysis coupled reaction unit, it is characterized in that: the catalyst in the photo catalysis reactor is applied sunshine or artificial light source, add simultaneously one electromagnetic field again, constituted magnetic field of the present invention-photocatalysis coupled reaction unit.
2, magnetic field according to claim 1-photocatalysis coupled reaction unit, it is characterized in that: the photochemical catalyst in the described photo catalysis reactor is: the titanium dioxide solid that titanium dioxide, transition-metal Fe, Co, Ni, Pt, Pd, Ru, Rh mix and modify.
3, magnetic field according to claim 1-photocatalysis coupled reaction unit is characterized in that: described illumination wavelength is the artificial light source of 200～800nm.
4, magnetic field according to claim 1-photocatalysis coupled reaction unit is characterized in that: its intensity of described electromagnetic field is 10～2000mT.
5, a kind of light-magnetic concerted catalysis technology and the application on degradable organic pollutant thereof is characterized in that: for gas-phase reaction, catalyst granules places in the quartz glass tubular type reactor, and magnetic field means and light source place around the reactor.
6, a kind of light-magnetic concerted catalysis technology and the application on degradable organic pollutant thereof, it is characterized in that: for liquid phase reactor, catalyst granules is suspended in the interior solution of quartz glass reaction container, the placement of reactor outer wall is close in magnetic field, and the set-up mode of light source has two kinds: the one, place the reaction vessel center; The 2nd, around magnetic field places reaction vessel.
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| Application Number | Priority Date | Filing Date | Title |
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| CN 03137060 CN1257766C (en) | 2003-05-31 | 2003-05-31 | Photo-magnetic concerted catalysis technology and application thereof in degrading organic pollutants |
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| CN 03137060 CN1257766C (en) | 2003-05-31 | 2003-05-31 | Photo-magnetic concerted catalysis technology and application thereof in degrading organic pollutants |
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| CN1460542A true CN1460542A (en) | 2003-12-10 |
| CN1257766C CN1257766C (en) | 2006-05-31 |
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Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1312061C (en) * | 2003-12-31 | 2007-04-25 | 彭云龙 | Waste water purifying method and its magnetic puddler integrated device |
| CN1331586C (en) * | 2005-03-30 | 2007-08-15 | 福州大学 | Composite photocatalytic reaction system for eliminating environmental pollutants in air or water efficiently |
| CN101244375B (en) * | 2008-03-14 | 2010-06-09 | 陕西师范大学 | Magnetically reinforced photocatalysis wind wheel and air purification method |
| CN101941773A (en) * | 2010-09-03 | 2011-01-12 | 武汉慧邦环境工程技术有限公司 | Cyclic photocatalyzed waste water purifying system |
| CN104368240A (en) * | 2014-11-18 | 2015-02-25 | 昆明理工大学 | Method and device for magnetizing and purifying flue gas in gas-solid reaction |
| WO2020011123A1 (en) * | 2018-07-11 | 2020-01-16 | 深圳汇盛环保科技有限公司 | Purification factor generator and environment purification device |
| CN112058082A (en) * | 2020-09-13 | 2020-12-11 | 昆明理工大学 | Method for removing zero-valent mercury and arsenic hydride by magnetic field in cooperation with photocatalytic oxidation |
| CN113351132A (en) * | 2021-05-13 | 2021-09-07 | 西北矿冶研究院 | Device for correspondingly degrading ziram through photo-magnetic cooperation and use method |
| CN113856460A (en) * | 2021-11-02 | 2021-12-31 | 昆明理工大学 | Method for purifying reductive tail gas by magnetic field-photocatalysis multi-effect coupling |
| CN115289740A (en) * | 2022-05-12 | 2022-11-04 | 广州吉祥行量子科技有限公司 | Micro-energy bionic ice-control fresh-keeping environment-friendly refrigerator |
| CN115745239A (en) * | 2022-11-08 | 2023-03-07 | 河北工业大学 | Method for degrading antibiotic wastewater by magnetic field enhanced photocatalysis-biological direct coupling system |
-
2003
- 2003-05-31 CN CN 03137060 patent/CN1257766C/en not_active Expired - Fee Related
Cited By (13)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1312061C (en) * | 2003-12-31 | 2007-04-25 | 彭云龙 | Waste water purifying method and its magnetic puddler integrated device |
| CN1331586C (en) * | 2005-03-30 | 2007-08-15 | 福州大学 | Composite photocatalytic reaction system for eliminating environmental pollutants in air or water efficiently |
| CN101244375B (en) * | 2008-03-14 | 2010-06-09 | 陕西师范大学 | Magnetically reinforced photocatalysis wind wheel and air purification method |
| CN101941773A (en) * | 2010-09-03 | 2011-01-12 | 武汉慧邦环境工程技术有限公司 | Cyclic photocatalyzed waste water purifying system |
| CN104368240A (en) * | 2014-11-18 | 2015-02-25 | 昆明理工大学 | Method and device for magnetizing and purifying flue gas in gas-solid reaction |
| WO2020011123A1 (en) * | 2018-07-11 | 2020-01-16 | 深圳汇盛环保科技有限公司 | Purification factor generator and environment purification device |
| CN112058082A (en) * | 2020-09-13 | 2020-12-11 | 昆明理工大学 | Method for removing zero-valent mercury and arsenic hydride by magnetic field in cooperation with photocatalytic oxidation |
| CN113351132A (en) * | 2021-05-13 | 2021-09-07 | 西北矿冶研究院 | Device for correspondingly degrading ziram through photo-magnetic cooperation and use method |
| CN113856460A (en) * | 2021-11-02 | 2021-12-31 | 昆明理工大学 | Method for purifying reductive tail gas by magnetic field-photocatalysis multi-effect coupling |
| CN113856460B (en) * | 2021-11-02 | 2023-12-22 | 昆明理工大学 | Method for purifying reductive tail gas by magnetic field-photocatalysis multi-effect coupling |
| CN115289740A (en) * | 2022-05-12 | 2022-11-04 | 广州吉祥行量子科技有限公司 | Micro-energy bionic ice-control fresh-keeping environment-friendly refrigerator |
| CN115745239A (en) * | 2022-11-08 | 2023-03-07 | 河北工业大学 | Method for degrading antibiotic wastewater by magnetic field enhanced photocatalysis-biological direct coupling system |
| CN115745239B (en) * | 2022-11-08 | 2023-05-16 | 河北工业大学 | Method for degrading antibiotic wastewater by using magnetic field enhanced photocatalysis-biological direct coupling system |
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| CN1257766C (en) | 2006-05-31 |
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