CN102698400B - Method for degrading amantadine organism by photoelectrocatalysis - Google Patents
Method for degrading amantadine organism by photoelectrocatalysis Download PDFInfo
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- CN102698400B CN102698400B CN201210162445.0A CN201210162445A CN102698400B CN 102698400 B CN102698400 B CN 102698400B CN 201210162445 A CN201210162445 A CN 201210162445A CN 102698400 B CN102698400 B CN 102698400B
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Abstract
The invention discloses a method for degrading an amantadine organism by photoelectrocatalysis, which comprises the following steps: adding a glucose solution into a solution containing the amantadine organism for photoelectrocatalytic degradation, wherein the working electrode for the photoelectrocatalytic degradation is a TiO2 nanotube array film, the reference electrode is Ag/AgCl, the counter electrode is Pt, the electrolyte is sodium nitrate, the COD concentration of the amantadine organic solution is 50 to 350 mg/L, and the COD concentration ratio of the glucose solution to the amantadine organic solution is 2 to 3; applying bias voltage and turning on a light source, the ultraviolet light wavelength of the light source is 365 nm, and the light intensity is 7.9 mW/cm<2>. The method for degrading the amantadine organism by the photoelectrocatalysis can greatly improve the photoelectrocatalytic degradation efficiency of the amantadine organism which is very difficult to degrade, and can implement the entire mineralization of amantadine.
Description
Technical field
The present invention relates to organic biodegrading process, be specifically related to a kind of organic method of collaborative photoelectric catalysis degrading amantadine, belong to environmental technology field.
Background technology
Amantadine is the aminoderivative of adamantane.Adamantane is symmetrical, the highly stable cage shape hydrocarbon of a kind of height, because the structure of the similar diamond carbon of its molecular structure is therefore named.Although amantadine is the aminoderivative of adamantane, but still there is high chemical stability.Amantadine is due to its special chemical stability, can suppress microbial growth simultaneously, because of but be typically difficult to biodegradable organic matter.The undressed waste water that contains amantadine will retain in environment for a long time, to human health, cause great hidden danger.
For the organic processing of hard degradation, generally adopt the advanced technology row pretreatment of advanced oxidation, make organic matter change into the product of easy degraded, and then carry out a biological disposal upon.Photoelectrocatalysis is a kind of effective treating method to persistent organic pollutants, thereby has caused increasing concern.The factor that affects photoelectrocatalysis reaction comprises the performance of electrode, the performance of reactor etc.The research of at present relevant electrode catalyst performance has obtained significant progress, as the people such as U.S. Grimes utilize the anodised method of Titanium successfully to prepare TiO in hydrofluoric acid aqueous solution medium
2nano-pipe array thin film high-efficient electrode (Gong D W et al J.Mater.Res. (2001) 16:3331-3334), at this titanium base TiO
2in nanometer pipe array electrode, photochemical catalyst TiO
2nanotube is arranged in metallic titanium matrix vertical, in good orderly, is conducive to separation and the transmission of photogenerated charge, shows the performance of high catalyzing oxidation of organic compounds.After this, people are to this titanium base TiO
2the preparation method of nano-pipe array thin film material has carried out a lot of research and application.Aspect the transformation of reactor, adopt thin layer reaction device can obviously promote the photoelectric catalysis degrading efficiency (Applied Catalysis B:Environmental 98 (2010) 154-160) of organic pollution.The people's such as Zhou Baoxue research also shows, utilize the photoelectrocatalysis of organic matter in thin layer reaction device to exhaust oxidation reaction, can study organic photoelectrocatalysis response characteristic, and can determine complexity (Acta PhySico-Chimica Sinica .2011,27 (9): 2153-2159) of organic matter degradation.Even yet aspect electrode and reactor, taking above-mentioned measure, for the organic matter of the extremely stable similar amantadine of chemical property, be also difficult to realize its complete oxidation.Therefore, how to realize rapidly and efficiently the processing of utmost point hardly degraded organic substance that chemical constitution is extremely stable is that photoelectrocatalysis field needs the problem of further exploring always.
Summary of the invention
The object of the invention is to for the deficiencies in the prior art, provide a kind of collaborative photoelectric catalysis degrading amantadine organic method, by adding glucose solution and controlling it and the COD concentration ratio of amantadine organic solution, realize the rapidly and efficiently oxidation of amantadine.
The present invention by following technical proposals to realize above object:
The organic method of collaborative photoelectric catalysis degrading amantadine, it adds glucose solution to containing in the organic solution of amantadine, carries out photoelectric catalysis degrading processing, and wherein, the working electrode of processing for photoelectric catalysis degrading is TiO
2nano-pipe array thin film, reference electrode is Ag/AgCl, to electrode, be Pt, electrolyte is sodium nitrate, and the COD concentration of amantadine organic solution is 50～350mg/L, and the COD concentration ratio of glucose solution and amantadine organic solution is 2～3, apply bias-voltage, open light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2.
TiO of the present invention
2nano-pipe array thin film adopts known anodizing technology preparation and obtains through known sintering process.
Compared with prior art, collaborative photoelectric catalysis degrading amantadine method of the present invention can increase substantially the organic degradation efficiency of amantadine of utmost point difficult degradation, and can realize the permineralization of amantadine.This is because add the glucose of a certain amount of easy degraded in amantadine solution after, glucose has produced a large amount of hydroxy radicals in degraded, the existence of a large amount of hydroxy radicals has promoted the oxidation of amantadine, thereby has produced the collaborative photoelectrocatalysis effect of the two.
Accompanying drawing explanation
Fig. 1 be variable concentrations amantadine solution at thin layer reaction device photoelectric catalysis degrading at the end, the relation between amantadine initial concentration and its final handling rate α.
Fig. 2 is the amantadine of initial COD concentration 100mg/L, under existing, processes at the end the relation between amantadine initial concentration and its final handling rate α at thin layer reaction device photoelectrocatalysis from different COD concentration glucose is common
Fig. 3 is the COD concentration ratio A of amantadine (A) and glucose (G): G is 1 and 2, when the two coexists, processes at the end the relation between amantadine initial concentration and its final handling rate α at thin layer reaction device photoelectrocatalysis
The specific embodiment
Below in conjunction with drawings and Examples, technical scheme of the present invention is described further.Following examples do not form limitation of the invention.
Embodiment 1:
With TiO
2nano-pipe array thin film is working electrode, Ag/AgCl is reference electrode, Pt is to electrode, in thin layer reaction device, injecting COD concentration is the amantadine organic solution of 100mg/L, and sodium nitrate is made electrolyte, adds the glucose solution that COD concentration is 200mg/L, apply bias-voltage, open light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2, carry out the reaction of catalyzing oxidation of organic compounds, in electrochemical workstation monitoring photoelectrocatalysis course of reaction, photoelectric current, with the variation of reaction time (I-t), found that when the reaction time be 90 seconds, photoelectric catalysis degrading reaches end of a period.By I-t curvilinear integral, obtain the transfer amount of electronics in this course of reaction, by known method, calculate the organic matter that reacts and the ratio of total organic matter, this ratio is that organic matter reacts final handling rate α at the end in thin layer reaction device.By calculating, find that its handling rate α is 99.8%, see Fig. 2.
In contrast, with TiO
2nano-pipe array thin film is working electrode, Ag/AgCl is reference electrode, Pt is to electrode, in thin layer reaction device, only injecting COD concentration is the amantadine organic solution of 100mg/L, sodium nitrate is made electrolyte, applies bias-voltage, opens light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2carry out the reaction of catalyzing oxidation of organic compounds, in electrochemical workstation monitoring photoelectrocatalysis course of reaction, photoelectric current is with the variation of reaction time (I-t), found that in the reaction time be 32 seconds, it is only 22.0% that photoelectric catalysis degrading reaches at the end its final handling rate α, see Fig. 1, illustrate and do not having the amantadine under glucose existence condition can not be completely oxidized.
In contrast, with TiO
2nano-pipe array thin film is working electrode, Ag/AgCl is reference electrode, Pt is to electrode, in thin layer reaction device, inject respectively COD concentration and be 50,200,300, the amantadine organic solution of 400mg/L, sodium nitrate is made electrolyte, applies bias-voltage, opens light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2carry out the reaction of catalyzing oxidation of organic compounds, in electrochemical workstation monitoring photoelectrocatalysis course of reaction, photoelectric current is with the variation of reaction time (I-t), found that at photoelectric catalysis degrading, reaching at the end its final handling rate α is respectively 28.0%, 20.0%, 16.8% and 16.5%, see Fig. 1, no matter explanation is the amantadine of low concentration or the amantadine of high concentration not having under glucose existence condition, all can not be completely oxidized.
Embodiment 2:
With TiO
2nano-pipe array thin film is working electrode, Ag/AgCl is reference electrode, Pt is to electrode, in thin layer reaction device, injecting COD concentration is the amantadine organic solution of 50mg/L, and sodium nitrate is made electrolyte, adds the glucose solution that COD concentration is 150mg/L, apply bias-voltage, open light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2, carry out the reaction of catalyzing oxidation of organic compounds, in electrochemical workstation monitoring photoelectrocatalysis course of reaction, photoelectric current, with the variation of reaction time (I-t), found that working as photoelectric catalysis degrading reaches at the end, organic handling rate α is 99.7%.
In contrast, with TiO
2nano-pipe array thin film is working electrode, Ag/AgCl is reference electrode, Pt is to electrode, in thin layer reaction device, injecting COD concentration is the amantadine solution of 50mg/L, and sodium nitrate is made electrolyte, adds the glucose solution that COD concentration is 50mg/L, apply bias-voltage, open light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2carry out the reaction of catalyzing oxidation of organic compounds, in electrochemical workstation monitoring photoelectrocatalysis course of reaction, photoelectric current is with the variation of reaction time (I-t), found that at photoelectric catalysis degrading, reaching at the end its final handling rate α is respectively 78.0%, see Fig. 3, when glucose and amantadine COD concentration ratio < 2 are described, amantadine can not be completely oxidized.
Embodiment 3:
With TiO
2nano-pipe array thin film is working electrode, Ag/AgCl is reference electrode, Pt is to electrode, in thin layer reaction device, injecting COD concentration is the amantadine organic solution of 100mg/L, and sodium nitrate is made electrolyte, adds the glucose solution that COD concentration is 250mg/L, apply bias-voltage, open light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2carry out the reaction of catalyzing oxidation of organic compounds, in electrochemical workstation monitoring photoelectrocatalysis course of reaction, photoelectric current, with the variation of reaction time (I-t), found that working as photoelectric catalysis degrading reaches at the end, organic handling rate α is 99.5%, sees Fig. 2.
Embodiment 4:
With TiO
2nano-pipe array thin film is working electrode, Ag/AgCl is reference electrode, Pt is to electrode, in thin layer reaction device, injecting COD concentration is the amantadine organic solution of 350mg/L, and sodium nitrate is made electrolyte, adds the glucose solution that COD concentration is 700mg/L, apply bias-voltage, open light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2, carry out the reaction of catalyzing oxidation of organic compounds, in electrochemical workstation monitoring photoelectrocatalysis course of reaction, photoelectric current, with the variation of reaction time (I-t), found that working as photoelectric catalysis degrading reaches at the end, organic handling rate α is 100.5%.
In contrast, with TiO
2nano-pipe array thin film is working electrode, Ag/AgCl is reference electrode, Pt is to electrode, in thin layer reaction device, injecting COD concentration is the amantadine organic solution of 350mg/L, and sodium nitrate is made electrolyte, adds the glucose solution that COD concentration is 350mg/L, apply bias-voltage, open light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2carry out the reaction of catalyzing oxidation of organic compounds, in electrochemical workstation monitoring photoelectrocatalysis course of reaction, photoelectric current is with the variation of reaction time (I-t), found that at photoelectric catalysis degrading, reaching at the end its final handling rate α is respectively 50.2%, see Fig. 3, illustrate that glucose and amantadine COD concentration ratio are at 1 o'clock, amantadine can not be completely oxidized.
Claims (2)
1. the organic method of collaborative photoelectric catalysis degrading amantadine, is characterized in that: to containing in the organic solution of amantadine, add glucose solution, carry out photoelectric catalysis degrading processing, wherein, the working electrode of processing for photoelectric catalysis degrading is TiO
2nano-pipe array thin film, reference electrode is Ag/AgCl, to electrode, be Pt, electrolyte is sodium nitrate, and the COD concentration of amantadine organic solution is 50～350mg/L, and the COD concentration ratio of glucose solution and amantadine organic solution is 2～3, apply bias-voltage, open light source, light source ultraviolet wavelength is 365nm, and light intensity is 7.9mW/cm
2.
2. the organic method of collaborative photoelectric catalysis degrading amantadine according to claim 1, is characterized in that: described TiO
2nano-pipe array thin film adopts known anodizing technology preparation and obtains through known sintering process.
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| CN101285789A (en) * | 2008-04-25 | 2008-10-15 | 中国科学院长春应用化学研究所 | Titanic oxide nanometer tube modified electrode applications |
| US7786339B2 (en) * | 2006-12-28 | 2010-08-31 | Industrial Technology Research Institute | Method of removing organic contaminants from surfaces of solid wastes |
| CN102442712A (en) * | 2011-10-24 | 2012-05-09 | 沈阳建筑大学 | Method for treating amantadine hydrochloride-containing wastewater by using titanium-containing blast furnace slag as photocatalyst |
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| US7786339B2 (en) * | 2006-12-28 | 2010-08-31 | Industrial Technology Research Institute | Method of removing organic contaminants from surfaces of solid wastes |
| CN101285789A (en) * | 2008-04-25 | 2008-10-15 | 中国科学院长春应用化学研究所 | Titanic oxide nanometer tube modified electrode applications |
| CN102442712A (en) * | 2011-10-24 | 2012-05-09 | 沈阳建筑大学 | Method for treating amantadine hydrochloride-containing wastewater by using titanium-containing blast furnace slag as photocatalyst |
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| ESR and photoluminescence evidence for the photocatalytic formation of hydroxyl radical on small TiO2 particles;Shima T,et al;《CHEMISTRY LETTERS》;19851231;第85卷(第12期);全文 * |
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