CN104043439B - The aeration electrochemical regeneration method of NACF - Google Patents
The aeration electrochemical regeneration method of NACF Download PDFInfo
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- CN104043439B CN104043439B CN201410332704.9A CN201410332704A CN104043439B CN 104043439 B CN104043439 B CN 104043439B CN 201410332704 A CN201410332704 A CN 201410332704A CN 104043439 B CN104043439 B CN 104043439B
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- regeneration
- nacf
- aeration
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Abstract
The aeration electrochemical regeneration method of NACF, relate to the electrochemical regeneration technology of active carbon adsorption material, significantly reduce the air film diffusional resistance because adsorbent gaseous product causes by aeration tube and distributor, improve regeneration effect and COD clearance.In regenerative process, first NACF saturated for adsorbing phenol be placed in anode region or be scattered in electrolyte, after process, taking out adsorbent, washing, oven dry, subsequent adsorbtion-regeneration cycle operation can be carried out.Compare other regeneration technologies, present device is simple, mild condition and easy to operate, and the comparatively lossy that can effectively avoid NACF to cause in regenerative process; By setting up aerator, specific aim can solve the larger problem of external diffusion resistance to mass tranfer, improving regeneration efficiency.
Description
Technical field
The present invention relates to regenerating unit and the method for porous adsorbent, be specially for the three-phase electrochemical regeneration reactor to the saturated NACF of adsorbing phenol, feature for adopting intermittent operation, and with aeration mode strengthening mass transfer.
Technical background
Phenol wastewater (phenol and its derivatives) wide material sources, and its composition and concentration have larger difference according to source from the different of technique.Conventional bioanalysis is larger for the wastewater treatment difficulty of this type of instability.Absorption method has the feature of wide spectrum in wastewater treatment, can be effective to the process of all kinds of phenol wastewater, especially to the process of low concentration phenol wastewater, possesses skills and feasibility economically.
Active carbon is that wide material sources are easy to get, effective adsorbent reliable for effect, this has benefited from its huge specific area, and suitable activity Carbon Materials can be selected as adsorbent according to the difference of adsorbate kind, which further improves the applicability of active carbon absorption technology.According to the difference of preparation technology and pattern, common porous active Carbon Materials has dust active carbon (PAC), particle charcoal (GAC), Carbon fibe (ACF) etc., wherein, activated carbon fiber material compares the active carbon of other patterns, has the superiority of more huge specific area and mass transfer aspect.Huge specific surface provides more adsorption activity position, and mass transport process can be then one dimension mass transfer by Simplified Three-dimensional by filamentary structure, will greatly reduce inside and outside diffusional resistance.
The active carbon that adsorbing phenol is saturated needs to carry out regeneration process to it, to recover its second adsorption ability, improves the service efficiency of active carbon, reduces process cost.Conventional renovation process mainly contains hot recycling method, chemical regeneration method and bio-regeneration method.Said method has its respective feature and limitation.Hot recycling commercial Application is comparatively wide, but the loss of regenerative process to active carbon is larger; Chemical regeneration is simply effective, but in subsequent treatment, have larger difficulty; The technique of bio-regeneration and device are comparatively loaded down with trivial details, and running cost is higher.Electrochemical regeneration method is a kind of comparatively novel adsorbent regeneration method, its principle is for produce oxidant (as OH) by electrode reaction, these oxidants are had an effect to adsorbent surface mass transfer and to it thus are reached the object of the regeneration to adsorbent, meanwhile, original adsorbate is oxidized to less the molecule even inorganic molecules of oxidation state (as CO
2, H
2o etc.), thus realize the harmless treatment to environment.
Therefore, take NACF as sorbent treatment phenol wastewater, and electrochemical regeneration is carried out, the advance on possessing skills and feasibility economically to the NACF inhaling phenol saturated.In electrochemical regeneration process, electrode reaction can produce bubble, and the bubble being dispersed in solution system can be adsorbed in its surface by porous adsorbent and cause extra resistance to mass tranfer.Therefore, in the electrochemical regeneration of porous material absorption agent, how effectively eliminating the inside and outside diffusional resistance owing to penetrating bubble (or air film) and the existence of duct inner transmission matter process, is the whether effective key factor of electrochemical regenerating device and renovation process.
Summary of the invention
The NACF that the object of the invention is for adsorbing phenol is saturated provides a kind of renovation process, to solve the large problem of the external diffusion resistance to mass tranfer that produces in electrochemical regeneration process.
Technical solution of the present invention is: under aeration condition, NACF saturated for adsorbing phenol is placed in the anode region of three-phase electrochemical reactor or is scattered in electrolyte, is 12mAcm in operating current
-2condition under electrochemical regeneration process is carried out to NACF, then take out NACF, through washing, dry, obtain the NACF of regeneration.
The electrode reaction occurred in regenerative process of the present invention mainly contains:
Anode reaction: H
2o → OH+H
++ e
-; 2H
2o → O
2+ 4H
++ 4e
-
Cathode reaction: 2H
2o+4e
-→ 2OH
-+ H
2
Wherein, OH and O
2the oxidant that regenerative process is possible, gaseous state O simultaneously
2and H
2dispersion is in systems in which and by can form new external diffusion resistance to mass tranfer at outer wall after adsorbent.
The present invention adopts electrochemical regeneration reactor, and equipment is simple, easy to operate.Compare other renovation process, electrochemical regeneration process of the present invention is gentle, thus the comparatively lossy that can effectively avoid NACF to cause in regenerative process.The aeration system that the present invention adopts, can solve the problem that electrochemical regeneration process China and foreign countries diffusion mass transfer resistance is larger pointedly, the conspicuousness reaching regenerative process efficiency improves.First regeneration rate after process of the present invention can reach more than 60%, COD clearance and reach more than 20%.
In addition, described three-phase electrochemical reactor of the present invention is with β-PbO
2for anode, Cu plate is negative electrode; With NaNO
3the aqueous solution is electrolyte.The present invention adopts β-PbO
2for anode, this electrode can produce hydroxyl radical free radical in the course of the work.The oxidisability of hydroxyl radical free radical is only second to fluorine, and therefore regeneration effect improves greatly.Experiment shows: adopt β-PbO
2for anode regeneration rate can reach more than 65%, improve more than 40% than employing ordinary electrode (as graphite, stainless steel electrode).In addition, by adding aerator, can reduce the external diffusion resistance in regenerative process, regeneration rate improves about 15% than during not aeration.Employing NaCl is electrolyte, and anode can produce hypochlorous acid.Hypochlorous acid and phenol reactant easily produce the chlorinated organics of difficult degradation.Experiment shows: with NaNO
3for electrolytical COD clearance is 29.3%, high by about 10% when being electrolyte than NaCl.So the present invention adopts NaNO
3for electrolyte.
When the present invention regenerates process, the temperature of electrolyte is 20 ~ 50 DEG C.In regenerative process, electrolyte temperature is higher, and the clearance of regeneration rate and COD is larger.Experiment shows: improve about 15% when regeneration rate when electrolyte temperature is 50 DEG C and COD clearance are than 20 DEG C.
The pH value of described electrolyte is 3.In regenerative process, as the pH=3 of electrolyte, regeneration rate is 62.3%, improves more than 10% than when pH=10.
Described electrochemical regeneration is treated to 1 ~ 2h.Under the effect of aeration, external diffusion resistance reduces greatly, and effect of mass transmitting is strengthened, and desorption, the degradation rate of phenol are accelerated.Experiment shows, after process 2h, the regeneration rate of NACF reaches about 65%, COD clearance and reaches 26.3%.
Described aeration gas is nitrogen or oxygen or air.The clearance adopting the regeneration rate of oxygen when being aeration atmosphere and improve about 5%, COD than regeneration rate when adopting air or nitrogen to do aeration atmosphere improves about 8% when also doing aeration atmosphere than employing air or nitrogen.The factors such as comprehensive regeneration rate, COD clearance and economy, adopt air to do aeration atmosphere for best.
The flow of described aeration is 200mL/min.Adopt the regeneration rate of aeration rate when being 200mL/min to be 63.6%, the clearance that regeneration rate when being 20mL/min than aeration rate improves about 10%, COD is 26.7% improves about 15% when being 20mL/min than aeration rate.
Detailed description of the invention
Embodiment 1: feature: not aeration.
Take 0.3g NACF put into initial concentration be the phenol solution of 1500ppm be adsorbed to saturated after, be placed on the regeneration of three-phase electrochemical regeneration reactor middle-jiao yang, function of the spleen and stomach polar region.
Regeneration reactor is with β-PbO
2for anode, Cu plate is negative electrode; 5gL
-1naNO
3the aqueous solution is electrolyte, regulates pH to be 3; Operating current is 12mAcm
-2; 2h is regenerated under the temperature of electrolyte is 20 DEG C of conditions.
Take out adsorbent after washing, drying operation, test for subsequent adsorbtion.After first regeneration, regeneration rate is 48.3%, COD clearance is 19.2%.
(regeneration rate is calculated by the ratio of double adsorbance and obtains.COD clearance is the ratio calculating acquisition of difference with theoretical COD of theoretical COD and actual measurement COD after electrochemical regeneration, represents the removal degree causing COD due to the oxidative degradation of regenerative process generation.）
Embodiment 2: feature: N
2aeration.
Take 0.3g NACF put into initial concentration be the phenol solution of 1500ppm be adsorbed to saturated after, be placed on the regeneration of three-phase electrochemical regeneration reactor middle-jiao yang, function of the spleen and stomach polar region.
Regeneration reactor is with β-PbO
2for anode, Cu plate is negative electrode; 5gL
-1naNO
3the aqueous solution is electrolyte, regulates pH to be 3; Operating current is 12mAcm
-2; Adopt N
2atmosphere concentrates aeration, and flow is 200mL/min; 2h is regenerated under the temperature of electrolyte is the condition of 20 DEG C.
Take out adsorbent after washing, drying operation, test for subsequent adsorbtion.After first regeneration, regeneration rate is 62.3%, COD clearance is 22.4%.
Embodiment 3: feature: O
2aeration.
Take 0.3g NACF put into initial concentration be the phenol solution of 1500ppm be adsorbed to saturated after, regenerate in the anode region being distributed in three-phase electrochemical regeneration reactor.
Regeneration reactor is with β-PbO
2for anode, Cu plate is negative electrode; 5gL
-1naNO
3the aqueous solution is electrolyte, regulates pH to be 3; Operating current is 12mAcm
-2; Adopt O
2atmosphere concentrates aeration, and flow is 200mL/min; 2h is regenerated under the temperature of electrolyte is the condition of 20 DEG C.
Take out adsorbent after washing, drying operation, test for subsequent adsorbtion.After first regeneration, regeneration rate is 66.6%, COD clearance is 28.5%.
Embodiment 4: feature: air concentrates aeration.
0.3g NACF is put into initial concentration be the phenol solution of 1500ppm be adsorbed to saturated after, be placed on the regeneration of three-phase electrochemical regeneration reactor middle-jiao yang, function of the spleen and stomach polar region.
Regeneration reactor is with β-PbO
2for anode, Cu plate is negative electrode; 5gL
-1naNO
3the aqueous solution is electrolyte, regulates pH to be 3; Operating current is 12mAcm
-2; Adopt air atmosphere to concentrate aeration, flow is 200mL/min; 2h is regenerated under the temperature of electrolyte is the condition of 20 DEG C.
Take out adsorbent after washing, drying operation, test for subsequent adsorbtion.After first regeneration, regeneration rate is 63.6%, COD clearance is 26.7%.
Embodiment 5:
0.3g NACF is put into initial concentration be the phenol solution of 1500ppm be adsorbed to saturated after, just regeneration in its anode region being distributed in three-phase electrochemical regeneration reactor.
Regeneration reactor is with β-PbO
2for anode, Cu plate is negative electrode; 5gL
-1naNO
3the aqueous solution is electrolyte, regulates pH to be 3; Operating current is 12mAcm
-2; Adopt the distributed aeration of air atmosphere, flow is 200mL/min; 2h is regenerated under the temperature of electrolyte is the condition of 20 DEG C.
Take out adsorbent after washing, drying operation, test for subsequent adsorbtion.After first regeneration, regeneration rate is 60.6%, COD clearance is 37.2%.
Embodiment 6:
0.3g NACF is put into initial concentration be the phenol solution of 1500ppm be adsorbed to saturated after, be placed on the regeneration of three-phase electrochemical regeneration reactor middle-jiao yang, function of the spleen and stomach polar region.
Regeneration reactor is with β-PbO
2for anode, Cu plate is negative electrode; 5gL
-1naNO
3the aqueous solution is electrolyte, regulates pH to be 3; Operating current is 12mAcm
-2; Adopt air atmosphere to concentrate aeration, flow is 200mL/min; 1h is regenerated under the temperature of electrolyte is the condition of 50 DEG C.
Take out adsorbent after washing, drying operation, test for subsequent adsorbtion.After first regeneration, regeneration rate is 68.7%, COD clearance is 37.6%.
Embodiment 7: feature: cathodic region regenerates.
0.3g NACF is put into initial concentration be the phenol solution of 1500ppm be adsorbed to saturated after, be placed on cathodic region regeneration in three-phase electrochemical regeneration reactor.
Regeneration reactor is with β-PbO
2for anode, Cu plate is negative electrode; 5gL
-1naNO
3the aqueous solution is electrolyte, regulates pH to be 3; Operating current is 12mAcm
-2; Adopt air atmosphere to concentrate aeration, flow is 200mL/min; 1.5h is regenerated under the temperature of electrolyte is the condition of 50 DEG C.
Take out adsorbent after washing, drying operation, test for subsequent adsorbtion.After first regeneration, regeneration rate is 57.7%, COD clearance is 19.2%.
Embodiment 8:
0.3g NACF is put into initial concentration be the phenol solution of 1500ppm be adsorbed to saturated after, just regeneration in its anode region being distributed in three-phase electrochemical regeneration reactor.
Regeneration reactor is with β-PbO
2for anode, Cu plate is negative electrode; 5gL
-1naNO
3the aqueous solution is electrolyte, regulates pH to be 3; Operating current is 12mAcm
-2; Adopt air atmosphere to concentrate aeration, flow is 200mL/min; 2h is regenerated under the temperature of electrolyte is the condition of 50 DEG C.
Take out adsorbent after washing, drying operation, test for subsequent adsorbtion.After first regeneration, regeneration rate is 65.1%, COD clearance is 20.7%.
Contrast above embodiment visible: carry out in electrochemical treatment process, adopting aeration effectively can improve regeneration rate and COD clearance at regeneration reactor.Anode region NACF being placed in three-phase electrochemical regeneration reactor or the regeneration rate being distributed in anode region, COD clearance are all higher than being placed in cathodic region.
Claims (6)
1. the aeration electrochemical regeneration method of NACF, under aeration condition, is placed in the anode region of three-phase electrochemical reactor by NACF saturated for adsorbing phenol or is scattered in electrolyte, is 12mAcm in operating current
-2condition under electrochemical regeneration process is carried out to NACF, then take out NACF, through washing, dry, obtain the NACF of regeneration; It is characterized in that: described three-phase electrochemical reactor is with β-PbO
2for anode, Cu plate is negative electrode; With NaNO
3the aqueous solution is electrolyte; The concentration of described electrolyte is 5g/L.
2. renovation process according to claim 1, when it is characterized in that regenerating process, the temperature of electrolyte is 20 ~ 50 DEG C.
3. renovation process according to claim 1, is characterized in that the pH value of described electrolyte is 3.
4. renovation process according to claim 1, is characterized in that described electrochemical regeneration is treated to 1 ~ 2h.
5. renovation process according to claim 1, is characterized in that described aeration gas is nitrogen or oxygen or air.
6. renovation process according to claim 5, is characterized in that the flow of described aeration is 200mL/min.
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| CN105771893B (en) * | 2015-12-17 | 2018-08-17 | 北京赛诺水务科技有限公司 | A kind of device for regenerating Powdered Activated Carbon |
| CN108793346A (en) * | 2018-08-06 | 2018-11-13 | 兰州交通大学 | A kind of Electro Sorb coupling extension activated carbon handles the apparatus and method of micro- pollution bitter |
| CN111495347B (en) * | 2020-06-04 | 2024-02-09 | 江西康乾环保科技有限公司 | Activated carbon regeneration system and regeneration process thereof |
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| CN1263539C (en) * | 2004-03-11 | 2006-07-12 | 上海交通大学 | Electrochemical regeneration method of flue gas demercury adsorbing material |
| CN1263683C (en) * | 2004-09-29 | 2006-07-12 | 浙江大学 | Equipment and method for treating organic waste water through electrocatalysis of cathode in combination with anode |
| CN101962240A (en) * | 2010-10-12 | 2011-02-02 | 昆明理工大学 | Method for processing waste water containing heavy metals by utilizing internal electrolysis-electrolysis method |
| CN102652916B (en) * | 2012-03-31 | 2014-04-09 | 南京工业大学 | Activated carbon regeneration device and process |
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Effective date of registration: 20190116 Address after: 225000 West Development Road 217, Hangjiang High-tech Industrial Development Zone, Yangzhou City, Jiangsu Province Patentee after: Yangzhou Xingyide Photoelectric Technology Co., Ltd. Address before: No. 88, South Road, University of Yangzhou, Jiangsu, Jiangsu Patentee before: Yangzhou University |
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Granted publication date: 20151209 Termination date: 20190714 |