CN1151084C - Three-dimension electrode reactor and use for treating organic waste water - Google Patents
Three-dimension electrode reactor and use for treating organic waste water Download PDFInfo
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- CN1151084C CN1151084C CNB02114740XA CN02114740A CN1151084C CN 1151084 C CN1151084 C CN 1151084C CN B02114740X A CNB02114740X A CN B02114740XA CN 02114740 A CN02114740 A CN 02114740A CN 1151084 C CN1151084 C CN 1151084C
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 34
- 239000010815 organic waste Substances 0.000 title abstract description 10
- 238000005273 aeration Methods 0.000 claims abstract description 13
- 239000008187 granular material Substances 0.000 claims description 25
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 18
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 18
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 16
- 239000003999 initiator Substances 0.000 claims description 15
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 14
- 150000001875 compounds Chemical class 0.000 claims description 14
- 239000011230 binding agent Substances 0.000 claims description 13
- 230000004888 barrier function Effects 0.000 claims description 10
- 229910002804 graphite Inorganic materials 0.000 claims description 9
- 239000010439 graphite Substances 0.000 claims description 9
- 229910052763 palladium Inorganic materials 0.000 claims description 9
- 229910052697 platinum Inorganic materials 0.000 claims description 9
- 229920000728 polyester Polymers 0.000 claims description 9
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 8
- 239000004745 nonwoven fabric Substances 0.000 claims description 8
- 229910052725 zinc Inorganic materials 0.000 claims description 8
- 239000011701 zinc Substances 0.000 claims description 8
- 229910052799 carbon Inorganic materials 0.000 claims description 7
- 229910052742 iron Inorganic materials 0.000 claims description 7
- 238000000034 method Methods 0.000 claims description 5
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 2
- 230000004913 activation Effects 0.000 claims description 2
- 229910017052 cobalt Inorganic materials 0.000 claims description 2
- 239000010941 cobalt Substances 0.000 claims description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 2
- 229910052802 copper Inorganic materials 0.000 claims description 2
- 239000010949 copper Substances 0.000 claims description 2
- 229910052759 nickel Inorganic materials 0.000 claims description 2
- 238000010792 warming Methods 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims 1
- 239000002351 wastewater Substances 0.000 abstract description 18
- 239000002245 particle Substances 0.000 abstract description 9
- 239000002957 persistent organic pollutant Substances 0.000 abstract description 8
- 238000005516 engineering process Methods 0.000 abstract description 5
- 230000005284 excitation Effects 0.000 abstract description 4
- 239000003795 chemical substances by application Substances 0.000 abstract description 2
- 239000007800 oxidant agent Substances 0.000 abstract description 2
- 239000002994 raw material Substances 0.000 abstract description 2
- 238000000354 decomposition reaction Methods 0.000 abstract 1
- 230000000977 initiatory effect Effects 0.000 abstract 1
- 229910010272 inorganic material Inorganic materials 0.000 abstract 1
- 239000011147 inorganic material Substances 0.000 abstract 1
- 239000011368 organic material Substances 0.000 abstract 1
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 description 12
- -1 hydroxyl radical free radical Chemical class 0.000 description 11
- 229910000428 cobalt oxide Inorganic materials 0.000 description 6
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 description 6
- 229960004643 cupric oxide Drugs 0.000 description 6
- 239000011159 matrix material Substances 0.000 description 6
- 229910000480 nickel oxide Inorganic materials 0.000 description 6
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 4
- 230000000694 effects Effects 0.000 description 3
- 230000005611 electricity Effects 0.000 description 3
- 238000012545 processing Methods 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 238000004042 decolorization Methods 0.000 description 2
- 238000004043 dyeing Methods 0.000 description 2
- 238000003487 electrochemical reaction Methods 0.000 description 2
- 239000010842 industrial wastewater Substances 0.000 description 2
- 239000013067 intermediate product Substances 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 230000035484 reaction time Effects 0.000 description 2
- 238000004065 wastewater treatment Methods 0.000 description 2
- VCUVETGKTILCLC-UHFFFAOYSA-N 5,5-dimethyl-1-pyrroline N-oxide Chemical compound CC1(C)CCC=[N+]1[O-] VCUVETGKTILCLC-UHFFFAOYSA-N 0.000 description 1
- FBPFZTCFMRRESA-KVTDHHQDSA-N D-Mannitol Chemical compound OC[C@@H](O)[C@@H](O)[C@H](O)[C@H](O)CO FBPFZTCFMRRESA-KVTDHHQDSA-N 0.000 description 1
- 229930195725 Mannitol Natural products 0.000 description 1
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
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- 238000001362 electron spin resonance spectrum Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 239000011152 fibreglass Substances 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 239000003112 inhibitor Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 235000010355 mannitol Nutrition 0.000 description 1
- 239000000594 mannitol Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
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- 229910052751 metal Inorganic materials 0.000 description 1
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- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 230000002906 microbiologic effect Effects 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Substances N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 1
- 238000010525 oxidative degradation reaction Methods 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
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- 239000010802 sludge Substances 0.000 description 1
- MNWBNISUBARLIT-UHFFFAOYSA-N sodium cyanide Chemical compound [Na+].N#[C-] MNWBNISUBARLIT-UHFFFAOYSA-N 0.000 description 1
- 238000013319 spin trapping Methods 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
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Abstract
The present invention relates to a three-dimension electrode reactor and an application thereof in treating organic waste water. The three-dimension electrode reactor comprises a bed body 5, a feed negative electrode 1, a feed positive electrode 6, a particle electrode 2, a water-distributing plate 9, an aeration plate and a DC power supply 8. The three-dimension electrode reactor uses electric energy as excitation energy, uses cheap air as a raw material and uses the particle electrode containing an initiating agent as a working electrode. The three-dimension electrode reactor can produce strong oxidizing agents of H2O2 and OH in site, and thus, can effectively make oxidation-decomposition. The three-dimension electrode reactor can even completely mineralize organic pollutants into inorganic materials of CO2, water, etc. The three-dimension electrode reactor can be used for pre-treating organic waste water with high concentration and low biodegradability, and the organic waste water are decomposed into organic materials with small molecular weight and high biodegradability, so the biodegradability of waste water is greatly improved. The three-dimension electrode reactor can also be used for the post treatment of a waste water biodegradability technology so as to ensure the standard discharge of the waste water.
Description
Technical field
The present invention relates to a kind of three-diemsnional electrode electrochemical reaction appts that can produce hydroxyl radical free radical.
Background technology
The processing of organic pollutant, especially high concentration organic contaminant is the difficult point and the focus of our times Industrial Wastewater Treatment.The deep oxidation technology (AOTs) that people such as Glaze propose provides an important approach (W.H.Glaze for administering organic pollutant, F.Beltranand T.Tuhkanen, Water Pollution Res.J.Canada, 1992,27:23), become a water treatment new technology among developing rapidly.Its principal character is to make full use of free radical, the extremely strong oxidisability of the OH of hydroxyl radical free radical particularly, meeting is the oxidative degradation organic pollutant up hill and dale, and novel method and the relevant device of therefore researching and developing effective and cheap hydroxyl radical free radical (OH) generation are very significant.
3 D electrode reactor has bigger dignity ratio, mass transfer effect and high current efficient preferably, be a kind of have higher practicality and theoretical electrochemical reactor that is worth, it has obtained many application in wastewater treatment, but all concentrate on the processing of heavy metal ion-containing waste water at present mostly, and at the research in organic waste water field actually rare (Simonsson, D.Chem.Soc.Rev.1997,26 (3), 181-189).
Summary of the invention
The purpose of this invention is to provide a kind of three-diemsnional electrode electrochemical reaction appts, this device can produce the extremely strong hydroxyl radical free radical of oxidisability, can decompose organic pollutant in the waste water rapidly up hill and dale.
3 D electrode reactor of the present invention is made of bed body, electrode cathode, electrode anode, granule electrode, water distributor or plate, aeration tube or plate and direct supply; Electrode cathode and electrode anode are composited by graphite and polyester non-woven fabric barrier film, place a body both sides respectively, and are connected with anodal with the negative pole of direct supply respectively; Granule electrode is filled in the body; Water distribution board and aeration board lay respectively at a body upper and lower part, and there is water inlet the water distribution board top, and there is inlet mouth the aeration board below; Bed body bottom also has water outlet.
The one-tenth of the granule electrode in the aforesaid 3 D electrode reactor is grouped into by weight and is generally: as the carbon of matrix or/and iron filings 85-96%, initiator 3-10%, binding agent 1-5%.Initiator wherein is made up of platinum, palladium and multiple metal oxide, usually form by the oxide compound of the copper of the zinc of the cobalt of the nickel of the Manganse Dioxide that accounts for granule electrode total weight percent 1-4%, 0.01% platinum, 0.02% palladium and 0.77-2%, 0.2-0.3%, 0.5-2%, 0.5-1.67%; Binding agent is Suo Jia base Xian Wei Su Na.
Said granule electrode can be prepared from by following method: by required proportioning with initiator, carbon or/and iron filings and binding agent to add the water mechanically mixing even, extruder grain, then under 200 ± 20 ℃ and anaerobic condition, heat and the binding agent in the granule electrode carried out charing in 2-3 hour, be warming up to 350 ± 20 ℃ of activation 2-3 hour again.
The granular size of the granule electrode of 3 D electrode reactor of the present invention is generally 4-6mm.
3 D electrode reactor of the present invention can be used for efficiently handling organic waste water.
Utilize hydroxyl radical free radical to handle organic waste water three essential conditions are arranged: the one, excitation energy, the 2nd, initiator, the 3rd, appropriate reaction conditions.Reactor of the present invention is as excitation energy with cheap electric energy.Two electron reductions take place in purity oxygen that feeds in this reactor or air on granule electrode under the exciting of pulse direct current, produce the status nascendi H with certain oxidisability
2O
2Its reaction is as follows:
These status nascendis H
2O
2The Fenton-like reaction takes place under the catalysis of the initiator in granule electrode then, produces the extremely strong hydroxyl radical free radical of oxidisability:
(M is a metal in the formula)
Employed granule electrode has organic effect in the enrichment solution, so that the high reactivity OH on granule electrode surface had an opportunity fully to contact with organic pollutant before by the water molecules cancellation, therefore can be rapidly mineralising organic pollutant effectively and up hill and dale:
(R is an organism in the formula)
The efficient of this reactor depends primarily on two kinds of active intermediate products, H from the above analysis
2O
2And OH.We measure and have confirmed two kinds of active intermediate products of key, H with diverse ways
2O
2With OH existing in this reactor (seeing Fig. 1 and 2).The life-span of hydroxyl radical free radical is very short, can not directly measure its ESR signal, needs to adopt spin trapping ESR method.The present invention adopts trapping agent commonly used 5, and 5-dimethyl-1-pyrroles-nitrogen oxidation DMPO detects the hydroxyl radical free radical that this 3 D electrode reactor produced.Its detected result is seen Fig. 3.Can obviously see the feature quartet of DMPO-OH ESR spectrum on scheme, g-factor is 2.007, matches with the theoretical value of hydroxyl free.After adding hydroxyl radical free radical inhibitor N.F,USP MANNITOL, above-mentioned feature quartet disappears.These test-results can regard that the on-the-spot electricity of this 3 D electrode reactor energy causes the admissible evidence of hydroxyl radical free radical as.
The above explanation, 3 D electrode reactor of the present invention, be with electric energy as excitation energy, be raw material with the air of cheapness, be the 3 D electrode reactor of working electrode with the granule electrode that contains initiator.This reactor can on-the-spotly produce strong oxidizer H
2O
2And OH, thereby oxygenolysis effectively, even the permineralization organic pollutant is CO
2With inorganicss such as water.It both can be used for the pre-treatment of the organic waste water of high density and bio-refractory, made it to be decomposed into the less organism that is easy to microbiological deterioration of molecular weight, thereby improved the biodegradability of waste water greatly; Also can be used for the aftertreatment of wastewater biochemical technology, to guarantee standard wastewater discharge.
Description of drawings
Fig. 1 is the structural representation of the embodiment of 3 D electrode reactor of the present invention.
Fig. 2 be 3 D electrode reactor of the present invention under different air pressures, electricity causes H
2O
2Concentration with the variation in reaction times.Test shows that in air pressure electricity causes H not too under the situation of highland
2O
2Concentration increase with the increase of reaction times and air pressure.But when air pressure was too high, because stirring is too violent, oxygen was too short in the residence time on granule electrode surface, so that H
2O
2Concentration reduce on the contrary.The suitable air pressure of this explanation control is to produce higher concentration H
2O
2Essential condition.
Fig. 3 is the DMPO-OHESR spectrogram.
Embodiment
The invention will be further described below in conjunction with accompanying drawing.
With reference to Fig. 1, the bed body 5 of 3 D electrode reactor of the present invention can be made rectangle, makes with glass-reinforced plastic material.Electrode cathode 1 and electrode anode 6 place a body both sides respectively, and are connected with anodal with the negative pole of direct supply 8 respectively; Electrode is composited with graphite and polyester tNonwovens barrier film, and barrier film mainly works to the variation buffering of actual industrial waste water ionic strength; Water distribution board 9 and aeration tube or aeration board 10 lay respectively at a body upper and lower part; Granule electrode 2 is filled in wherein.The size of bed body, two distance between electrodes can be regulated according to the water yield of the waste water of handling and the character of waste water.Waste water enters the reactor by water distribution board from water inlet 7; Pressurized air from the inlet mouth 3 of reactor bottom by micropore aeration pipe or micro-pore aeration plate 10 to reactor aeration and and the mixing of waste water adverse current; Waste water after reaction treatment is discharged from water outlet 4.
When 3 D electrode reactor of the present invention is used to handle organic waste water, start air compressor aeration in reactor earlier, open water intaking valve then and advance waste water, connect direct supply, regulate suitable voltage and air flow quantity, waste water is discharged from water outlet after treatment.
Below by specific embodiment application and the effect thereof of 3 D electrode reactor of the present invention in handling organic waste water is described further:
Example 1
Iron filings with 91.0% (particle diameter is 2-4mm) are matrix, with 2% Manganse Dioxide, 0.01% platinum, 0.02% palladium, 0.5% cupric oxide, 1.5% nickel oxide, 0.27% cobalt oxide and 0.7% oxide compound zinc are initiator, the Suo Jia base Xian Wei Na with 4% is that the particle diameter that binding agent is made is that the 4-6mm granule electrode is a working electrode; Compound with graphite and polyester non-woven fabric barrier film is the 3 D electrode reactor of electrode.At 0.3m
3Under the air flow quantity of/h, the phenol solution to 100mg/l under 20 volts the voltage was handled 60 minutes, and its clearance reaches 92%.To 500mg/l trichoro-aldehyde solution-treated 30 minutes, its clearance reached 95%.
Example 2
Carbon with 90% is matrix, with 2.0% Manganse Dioxide, and 1.0% cupric oxide, 1.25% nickel oxide, 0.22% cobalt oxide, 1.5% oxide compound zinc, 0.01% platinum and 0.02% palladium are initiator, are that particle diameter that binding agent is made is that the granule electrode of 4-6mm is a working electrode with 4% Suo Jia base Xian Wei Na; Compound with graphite and polyester non-woven fabric barrier film is the 3 D electrode reactor of electrode.At 0.16m
3Under the air flow quantity of/h, under 20 volts the voltage to the NaCN solution-treated of 100mg/l 30 minutes, its CN
-Clearance reaches 97%.To trichoro-aldehyde solution-treated 30 minutes, its clearance reached 95%.
Example 3
Iron filings with 90% are matrix, with 3.0% Manganse Dioxide, and 0.77% cupric oxide, 2.1% nickel oxide, 0.3% cobalt oxide, 0.8% oxide compound zinc, 0.01% platinum and 0.02% palladium are initiator, and the Suo Jia base Xian Wei Na with 3% is that the particle diameter that binding agent is made is that the 4-6mm granule electrode is a working electrode; Compound with graphite and polyester non-woven fabric barrier film is the 3 D electrode reactor of electrode.At 0.6m
3Under the air flow quantity of/h, under 28 volts the voltage to the COD of Taiwan printing and dyeing mill
CrConcentration is up to the treatment of dyeing wastewater of 10608mg/l 15 minutes, COD
CrDensity loss is 3672mg/l, its COD
CrClearance is 65.3%, and percent of decolourization is 95%.
Example 4
Guangdong Huizhou Taiwan investment computer enterprise is by different production line discharging D class and E class waste water, its COD
CrConcentration is respectively 986.3 and 340.8mg/l.They are at 30 volts voltage and 0.2m
3Under/h the air flow quantity, through the carbon with 89% is matrix, with 3.5% Manganse Dioxide, 0.375% cupric oxide, 1.8% nickel oxide, 0.3% cobalt oxide, 1.0% oxide compound zinc, 0.01% platinum and 0.015% palladium are initiator, are that particle diameter that binding agent is made is that the granule electrode of 4-6mm is a working electrode with 4% Suo Jia base Xian Wei Na, compound with graphite and polyester non-woven fabric barrier film is that the 3 D electrode reactor of electrode was handled COD 40 minutes
CrConcentration drops to 312.8 and 68.6mg/l respectively, its COD
CrClearance is respectively 68.4% and 79.9%, and percent of decolourization is 100%.
Example 5
Percolate from garbage filling field Pollutant levels height, complicated component, its effective, harmless processing are the difficult problems of world's water treatment field always.The COD of Guangzhou Li Keng percolate from garbage filling field
CrConcentration is up to 4000-6000mg/l and NH
3The concentration of-N is up to 1600-1800mg/l.Through the iron with 89.5% is matrix, with 2.5% Manganse Dioxide, 0.5% cupric oxide, 1.2% nickel oxide, 0.3% cobalt oxide, 1.975% oxide compound zinc, 0.01% platinum and 0.015% palladium are initiator, with 4% Suo Jia base Xian Wei Na is that particle diameter that binding agent is made is that the granule electrode of 4-6mm is a working electrode, and compound with graphite and polyester non-woven fabric barrier film is that the 3 D electrode reactor of electrode was handled 15 minutes; Be substrate through carbon again with 87%, with 4.0% Manganse Dioxide, 1.0% cupric oxide, 1.775% nickel oxide, 0.2% cobalt oxide, 2.0% oxide compound zinc, 0.01% platinum and 0.015% palladium are initiator, with 4% Suo Jia base Xian Wei Na is that particle diameter that binding agent is made is that the granule electrode of 4-6 is a working electrode, compound with graphite and polyester non-woven fabric barrier film is to handle in second step of carrying out 15 minutes of the 3 D electrode reactor of electrode, they reduce to 1040-1579mg/l and 585-810mg/l respectively, and have improved the biodegradability of percolate widely.The percolates of handling through above two steps are again through common Wastewater Treated by Activated Sludge Process, but qualified discharge.
Claims (3)
1. a 3 D electrode reactor is characterized in that this reactor is made of bed body (5), electrode cathode (1), electrode anode (6), granule electrode (2), water distributor or plate (9), aeration tube or plate (10) and direct supply (8); Electrode cathode and electrode anode are composited by graphite and polyester non-woven fabric barrier film, place a body both sides respectively, and are connected with anodal with the negative pole of direct supply respectively; Granule electrode is filled in the body; Water distribution board and aeration board lay respectively at a body upper and lower part, and there is water inlet (7) the water distribution board top, and there is inlet mouth (3) the aeration board below; Bed body bottom also has water outlet (4); The one-tenth of said granule electrode (2) is grouped into by weight and is: carbon is or/and iron filings 85-96%, initiator 3-10%, binding agent 1-5%; Initiator wherein is by weight being made up of the oxide compound of 1-4% Manganse Dioxide and 0.01% platinum, 0.02% palladium, 0.77-2% nickel, 0.2-0.3% cobalt, 0.5-2% zinc, 0.5-1.67% copper; Binding agent is Suo Jia base Xian Wei Su Na.
2. according to the described 3 D electrode reactor of claim 1, it is characterized in that said granule electrode (2) is prepared from by following method: by required proportioning with initiator, carbon or/and iron filings and binding agent add water mixes, extruder grain, then under 200 ± 20 ℃ and anaerobic condition, heating charing 2-3 hour is warming up to 350 ± 20 ℃ of activation 2-3 hour again.
3. according to claim 1 or 2 described 3 D electrode reactors, the granular size that it is characterized in that said granule electrode (2) is 4-6mm.
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-
2002
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN101844822A (en) * | 2010-05-11 | 2010-09-29 | 沈阳建筑大学 | Three-dimensional electrode/ electro-Fenton reactor |
CN101844822B (en) * | 2010-05-11 | 2012-09-26 | 沈阳建筑大学 | Three-dimensional electrode/ electro-Fenton reactor |
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