CN103435132B - Activated carbon fiber for treating oily wastewater as well as regeneration method and device of activated carbon fiber - Google Patents
Activated carbon fiber for treating oily wastewater as well as regeneration method and device of activated carbon fiber Download PDFInfo
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Abstract
The invention discloses an activated carbon fiber for treating oily wastewater as well as a regeneration method and device of the activated carbon fiber. Specifically, the method provided by the invention integrates adsorption, electrolysis and desorption of oil in the oily wastewater and regeneration of the activated carbon fiber through an electrochemical reaction device taking an activated carbon fiber felt as anodes and net-shaped titanium as cathodes; the electrochemical reaction device is composed of a reactor, an electric mixer and a voltage-stabilizing direct-current power source connected to the exterior of the electrochemical reaction device, wherein the reactor is internally provided with multiple groups of dismountable anodes and cathodes; the anodes are jointly formed by the activated carbon fiber felt serving as a main body and a titanium base metal oxide serving as a supporting body, and the net-shaped pure titanium is utilized as the cathode electrodes, the anode and cathode groups are alternately connected with the power source through wires, and the number of the electrode groups can be increased or reduced by assembling or disassembly, and can be regulated according to the treatment requirement. Compared with the prior art, the method provided by the invention integrates the electrochemical treatment for the oily wastewater by the activated carbon fiber and an in-situ regeneration technology of the activated carbon fiber, the regeneration period is prolonged, the technological process and secondary pollution are reduced, the operating control is easy, and the industrialized application is easy.
Description
Technical field
The present invention relates to technical field of sewage, specifically a kind of activated carbon fiber process oily(waste)water and renovation process thereof, and the corollary apparatus of foundation the method.
Background technology
Oily(waste)water is from the processing of petroleum industry PetroChina Company Limited. and oil product, refinement, storage and transport; The cooling-lubricant produced in the machinofacture course of processing, steel rolling water etc.; Transport industry in locomotive waste water, railway locomotive depot oil-washing tank waste water etc., also all contain a large amount of oil in foodstuffs industry, textile industry and other manufacturing waste water, to environment protection and the eubiosis very harmful.At present Physical, chemical method, physico-chemical processes and microbial method etc. are mainly contained to the technology of oiliness sewage treatment.Although as the Physical non-secondary pollution of comparatively welcome membrane sepn, efficiency is high, easy to operate, costly, the cleaning of film also comparatively bothers film device; There is secondary pollution in chemical method, the troublesome shortcoming of post-processed; Biological rule length consuming time, not easy to operate; Absorption is as method comparatively main in physico-chemical processes, and wherein activated carbon fiber is comparatively conventional, although treatment effect is better, but expensive, regeneration difficulty, and also hot recycling is the regeneration techniques commonly used the most at present, but it exists costly, the shortcoming that charcoal loss is larger.
In recent years, electrochemical catalytic oxidation method with its catalytic oxidation system using electronics as reactant, the extremely strong hydroxyl radical free radical of oxidisability, as catalyzer, can carry out under the condition of normal temperature, normal pressure, and the effective, easy and simple to handle of process easily realizes the obviously advantage such as automatization, environmental friendliness.The organism of people to electrochemical oxidation technology process difficult degradation has carried out studying widely, and compared with chemical oxidation or photochemical oxidation method, the competitive capacity of electrochemical oxidation method depends primarily on the structure of electrode materials and electrolyzer.According to the study, investigation of titanium anode coated with metal oxide good conductivity, catalytic performance is excellent, but when independent metal or metal oxide use as electrode, current density and the electrolyte concentration of these class methods are high, and cause water treatment somewhat expensive, practical application is very restricted.
Activated carbon fiber (Activated carbon fiber, ACF), a kind ofly just grows up in recent years
Novel absorption material, the conduction property possessed because it is special, its effect in Environmental electrochemistry has started the attention causing people.Current Activated Carbon Fiber Electrodes applies among wastewater treatment as a kind of novel oxidizing electrode, because activated carbon fiber has conduction, absorption property, it has very strong concentration effect as electrode pair organism, electrolytic speed can be significantly improved, so not only cause the extensive concern of people in wastewater treatment, in the regeneration of absorbent charcoal material, provide new thinking simultaneously.But absorbent charcoal material regeneration most is at present all take out to be positioned in reclaim equiment to regenerate, and is unfavorable for actually operating.And there is number of drawbacks when processing oily(waste)water by single method: Chinese invention patent (ZL 01259205.6) discloses " a kind for the treatment of unit of oily(waste)water ".This device uses multiple lipophilicity absorption filtering material to combine process oily(waste)water, although the clearance of oil reaches 99%, but adsorption filtration material used is oil loving, the blocking in aperture is very easily caused after process for some time, need constantly to change absorption filtering material, technique is comparatively loaded down with trivial details, and post-processed comparatively bothers; Xu Zhida etc. (" activated carbon fiber Refinery Wastewater prospect ", Treatment of Industrial Water, 1998,18 (2)) activated carbon treatment refinery water is used, the overheated steam of 200 DEG C-500 DEG C is used to carry out desorption and regeneration after saturated again, although the effect of process and regeneration is all good, process and regeneration process respectively in different devices, and technique is loaded down with trivial details and energy consumption is larger; Chinese invention patent (ZL 03151224.0) discloses " a kind of electrolytic oxidation treatment process of wastewater containing phenol ".This technique uses Ti base PbO
2for anode, stainless steel are cathode treatment wastewater containing phenol, although the clearance of volatile phenol and COD reaches 93% and 90% respectively, during its independent utilization metal electrode, the easy loss of electrode, and current density is comparatively large, consumes energy higher; Huang Yaohui etc. (" Case study on the bioeffluent of petrochemical wastewater by electro-Fenton method ", Water Science and Technology, 1999,39 (10-11)) produce Fe with anode
2+and H
2o
2electric Fenton method process petrochemical wastewater, although achieve good effect, the requirement of whole process to pH value is higher, but also along with electricity flocculation reaction, produce a large amount of mud, had a strong impact on the process in later stage.Occur above-mentioned variety of problems, key reason is to lack the combination namely realizing various wastewater treatment technology in same device kind in existing technology, can reach again the Apparatus and method for of absorbent charcoal material regeneration.
Summary of the invention
The object of the invention is to lack for prior art the combination simultaneously realizing various wastewater treatment technology, the technological deficiency of activated carbon fiber regeneration can be reached again, a kind of process is provided and regenerates the integrated activated carbon fiber process oily(waste)water that runs and renovation process thereof and device.
The present invention is realized by following technical proposal:
A kind of activated carbon fiber electrochemical treatment oily(waste)water and renovation process thereof, is characterized in that the method in the electrochemical reaction appts of negative electrode, completes the efficient process of oily(waste)water and the regenerative process of activated carbon fiber using the active carbon fiber felt be wrapped on titanium-based metal oxide compound as anode, pure titanium metal.This electrochemical appliance Anodic is alternately connected power supply with cathode sets by wire, and the group number of electrode can regulate according to the requirement of process, thus achieves the integration of activated carbon fiber electrochemical treatment oily(waste)water and in-situ regeneration thereof.
Its concrete performing step is as follows:
(1) by the importing reactor of oily(waste)water interval, open direct supply and agitator, carry out absorption electrolysis wastewater, pass into air with air compressor to reactor simultaneously.
(2) when water outlet oleaginousness is too high, waste water is discharged, import regenerated liquid, open direct supply and agitator, carry out activated carbon fiber regeneration.
(3), after having regenerated, discharge regenerated liquid, then import oily(waste)water and carry out absorption electrolysis treatment, iterative cycles carries out.
The described titanium-based metal oxide compound as anode active carbon fiber felt supporter is netted.
Described negative electrode is netted pure titanium metal.
Described absorption electrolysis and the current density of regeneration are 10 ~ 50mA/m
2, voltage is 10 ~ 20V
The pH value of described waste water is 3 ~ 10.
During described absorption electrolysis oily(waste)water, the time of absorption electrolysis is 30 ~ 120min.
During described regeneration activity Carbon fibe, the recovery time is 30 ~ 120min.
Described regenerated liquid is one or both of the KCl solution of 5 ~ 15g/L or NaCl solution.
Described regenerated liquid pH value is 3 ~ 10.
Technical scheme of the present invention also comprises according to activated carbon fiber process oily(waste)water and renovation process custom-designed activated carbon fiber process oily(waste)water thereof and regenerating unit thereof, comprise reactor and be arranged on the mouth of pipe, the electric blender on reactor, in reactor, be provided with the many groups of anodes and cathode sets be alternately arranged, anode and negative electrode introduce reactor external direct current power supply respectively by wire or pole plate.
Described anode is the active carbon fiber felt be wrapped on titanium-based metal oxide compound is anode, and described negative electrode is pure titanium metal is negative electrode.
Described titanium-based metal oxide compound and pure titanium metal are reticulated structure.
The mouth of pipe be arranged on reactor comprises: be positioned at the assisted Regeneration liquid water-in of reactor head, venting port, wastewater effluent mouth and be positioned at assisted Regeneration liquid water outlet and the water intake of reactor bottom.
Innovation Mechanism of the present invention is as follows:
Method of the present invention contains organic Electrocatalytic Oxidation and indirect electrooxidation in degrading waste water; Wherein, Electrocatalytic Oxidation is that in waste water, first an organic part is adsorbed onto Activated Carbon Fiber Electrodes surface, afterwards with Activated Carbon Fiber Electrodes generation electron transmission and being degraded, a small amount of part directly and the anode that serves as of titanium-based metal oxide compound directly oxidized; And indirect electrooxidation is short life intermediate (solvated electron and OH, O of utilizing electrochemistry to produce
2, HO
2deng free radical and Cl
2, ClO
-with the strong oxidizing property muriate of HClO) destroy and oxidize contaminants, roughly click step and carry out:
(1) mass transfer in liquid phase---pollutent moves from solution to electrode surface (the adsorption and enrichment effect of ACF);
(2) electrode adsorption---pollutent is adsorbed on electrode surface (the adsorption and enrichment effect of ACF);
(3) electrode reaction---pollutent electric discharge (obtain or lose electronics) generates small molecules intermediate product, CO
2and H
2o (Electrocatalytic Oxidation effect);
(4) electrode desorption---intermediate product is by electrode surface desorb (regeneration of ACF);
(5) mass transfer in liquid phase---intermediate product is moved (regeneration of ACF) to solution bulk mutually by electrode surface liquid layer;
(6) near electrode surface, there is chemical reaction (indirect electrooxidation effect) in chemical reaction---pollutent or intermediate product;
(7) cenotype generates---and pollutant oxidation becomes CO
2and H
2o and reach the object of final removing.
The principal reaction comprised has:
The first, active carbon fiber felt wraps up in the hydroxyl radical free radical (OH) due to electric discharge generation physical adsorption state on netted or tabular titanium-based metal oxide compound composition anode:
H
2O - e
-→ ·OH + H
+
The second, on Ti cathode because oxygen diffusion is in solution, obtain electronics and be reduced into hydrogen peroxide (H
2o
2):
O
2(g) + 2 e
-+ H
+→ H
2O
2
Three, Cl in ionogen
-cl can be produced in electrocatalysis process
2, Cl
-with the material synergistic oxidation organism such as HClO:
2Cl
-→ Cl
2+ 2e
-
Cl
2+ H
2O → HClO + Cl
-+ H
+
6HClO + 3H
2O → 2ClO
3 -+ 4Cl
-+ 12H
++ 1/2O
2↑+ 6e
-
Four, the removal (ultimate aim) of organism R:
R+OH (comprises H
2o
2, O
2, HO
2, Cl
2, ClO
-and HClO) → CO
2↑+H
2o
The calculating of regeneration rate:
In formula: Q is the adsorptive capacity (mg/g) that activated carbon fiber reaches when adsorbing state of saturation for the first time
Q` is the adsorptive capacity (mg/g) that the activated carbon fiber after regeneration reaches when adsorbing state of saturation
The Advantageous Effects that the present invention possesses is:
(1) the group number of adjustable electrode, electrode is installed and is exchanged conveniently;
(2) fix active carbon fiber felt as anode using netted titanium-based metal oxide compound, not only reach the effect that absorption-electrochemistry combines process oily(waste)water, realize the in-situ regeneration of activated carbon fiber simultaneously;
(3) device adopted not only realizes the regeneration of activated carbon fiber, also extends the regeneration period of activated carbon fiber simultaneously, greatly reduces cost, and operation controls easily, to be convenient to industrial applications;
(4) the anti-load change ability of device is strong, can process the oily(waste)water of different concns and regenerate the activated carbon fiber of different degree of saturation, generates, decrease technical process and secondary pollution without precipitation.
Accompanying drawing explanation
Fig. 1 is activated carbon fiber process oily(waste)water of the present invention and regenerating unit structural representation thereof.
In figure: 1 reactor, 2 regenerated liquid water-ins, 3 venting ports, 4 electric blender, 5 wastewater effluent mouths, 6 anodes, 7 negative electrodes, 8 regenerated liquid water outlets, 9 water intakes.
Embodiment
First by reference to the accompanying drawings 1 the embodiment relating to device is provided in the present invention
Device embodiment 1
A kind of activated carbon fiber process oily(waste)water and regenerating unit thereof, comprise reactor 1 and be positioned at reactor bottom with the mouth of pipe be arranged on reactor 1, electric blender 4(agitator, do not mark in figure), in reactor 1, be provided with the many groups of anodes be alternately arranged 6 and 7 groups, negative electrode, anode 6 and negative electrode 7 introduce reactor external direct current power supply respectively by wire or pole plate.
Device embodiment 2
On the basis of above-described embodiment 1, described anode is the active carbon fiber felt be wrapped on titanium-based metal oxide compound is anode, and described negative electrode is pure titanium metal is negative electrode.And titanium-based metal oxide compound and pure titanium metal are reticulated structure.
Device embodiment 3
On the basis of above-described embodiment 1 or embodiment 2, the mouth of pipe be arranged on reactor comprises: be positioned at the assisted Regeneration liquid water-in 2 at reactor 1 top, venting port 3, wastewater effluent mouth 5 and the assisted Regeneration liquid water outlet 8 be positioned at bottom reactor 1 and water intake 9.By the setting of specific nozzle position, make that wastewater treatment process takes low level to enter, a high position goes out, be more conducive to it and fully degrade; An assisted Regeneration liquid employing high position is entered, low level goes out, and operation of being more convenient for, improves work efficiency.
Secondly just method part of the present invention is described further by the following example
The impact that embodiment of the method 4. treatment time regenerates oil removing rate and activated carbon fiber
Get oily(waste)water that 1000ml concentration is 100mg/L (be 0.3mol/L containing NaCl concentration) in reactor, adjust ph is 6, netted titanium-based metal oxide compound is anode (2 groups) to adopt active carbon fiber felt to wrap up in, titanium net is as negative electrode (4 groups), under agitation, constant output current density is 40 mA/m
2carry out electrolysis 120 minutes.The clearance of oil 30,60,90,120 minutes time as shown in table 1 below, shows under the inventive method process, and after 120 minutes, the clearance of oil reaches 95%.Simultaneously also to carry out at identical conditions in the present embodiment, netted titanium-based metal oxide compound is wrapped up in for anode (2 groups) with the active carbon fiber felt that the absorption of the identical weight of identical type is saturated, titanium net is as negative electrode (4 groups), the NaCl concentration that regenerated liquid contains 0.15 mol/L carries out manipulation of regeneration, and after 120 minutes, regeneration reaches 97%.
The effect of table 1 different treatment time Electrochemistry process oily(waste)water oil removing rate and activated carbon fiber regeneration
| Time | 30min | 60min | 90min | 120min |
| Oil removing rate (%) | 57.5 | 75.8 | 87.6 | 95 |
| Regeneration rate (%) | 56.9 | 79.2 | 88.3 | 97 |
Embodiment of the method 5. initial pH value is on the impact of oil removing rate and regeneration rate
In electrolyzer, adjust ph is 3 ~ 10 to get oily(waste)water that 1000ml concentration is 200mg/L (be 0.35mol/L containing NaCl concentration), and netted titanium-based metal oxide compound is anode (4 to adopt active carbon fiber felt to wrap up in
Group), titanium net is as negative electrode (6 groups), and under agitation, constant output voltage is that 14V carries out electrolysis 120 minutes.Simultaneously also to carry out at identical conditions in the present embodiment, netted titanium-based metal oxide compound is wrapped up in for anode (4 groups) with the active carbon fiber felt that the absorption of the identical weight of identical type is saturated, titanium net is as negative electrode (6 groups), regenerated liquid contains the NaCl solution of 0.10 mol/L, carries out manipulation of regeneration.The clearance of the oil when pH value is respectively 3,5,7,10 as shown in table 2 below and regeneration rate, from result, under the condition of neutrality, the clearance of (pH=7) oil also can reach 93.2%, and regeneration rate is 95%.
Table 2 initial pH value is on the impact of oil removing rate and regeneration rate
| PH value | 3 | 5 | 7 | 10 |
| Oil removing rate (%) | 94.5 | 94.1 | 93.2 | 90.2 |
| Regeneration rate (%) | 96.5 | 96.3 | 95 | 95.1 |
Embodiment of the method 6. voltage is on the impact of oil removing rate and regeneration rate
Get oily(waste)water that 1000ml concentration is 100mg/L (be 0.3mol/L containing NaCl concentration) in electrolyzer, adjust ph is 7, netted titanium-based metal oxide compound is anode (2 groups) to adopt active carbon fiber felt to wrap up in, titanium net is as negative electrode (4 groups), under agitation, constant output voltage is that 10V, 14V, 18V, 20V carry out electrolysis 120 minutes; Simultaneously also to carry out at identical conditions in the present embodiment, netted titanium-based metal oxide compound is wrapped up in for anode (2 groups) with the active carbon fiber felt that the absorption of the identical weight of identical type is saturated, titanium net is as negative electrode (4 groups), regenerated liquid contains the KCl solution of 0.15 mol/L, carries out manipulation of regeneration.Effect is as shown in table 3.
Table 3 voltage is on the impact of oil removing rate
| Voltage (V) | 10 | 14 | 18 | 20 |
| Oil removing rate (%) | 89.5 | 93.2 | 95.5 | 96.2 |
| Regeneration rate (%) | 91.2 | 95.3 | 96.7 | 97.5 |
The circular treatment of embodiment of the method 7. activated carbon fiber electrochemical treatment oily(waste)water and regeneration thereof
get oily(waste)water that concentration is 100mg/L (be 0.3mol/L containing NaCl concentration) in electrolyzer, adjust ph is 7, netted titanium-based metal oxide compound is anode (2 groups) to adopt active carbon fiber felt to wrap up in, titanium net is as negative electrode (4 groups), under agitation, constant output voltage is that 14V carries out electrolysis, each importing new waste water absorption electrolysis 120 minutes, repeatedly carry out 30 times, in its process, when water outlet oleaginousness reaches less than when requiring, manipulation of regeneration need be carried out, regenerative voltage is 14V, regenerated liquid is the NaCl concentration of 0.15 mol/L, regenerate 120 minutes.Result is as shown in table 4.
The effect of the circular treatment of table 4 activated carbon fiber electrochemical treatment oily(waste)water and regeneration thereof
| For the first time | For the second time | For the third time | 4th time | 5th time | |
| Oil removing rate (%) | 94.1 | 92.2 | 90.2 | 88.5 | 87.5 |
| Regeneration rate (%) | 96 | 93.1 | 91.2 | 87 | 84.3 |
The circular treatment of embodiment of the method 8. non-mesh Electrode treatment oily(waste)water and regeneration thereof
get oily(waste)water that concentration is 100mg/L (be 0.3mol/L containing NaCl concentration) in electrolyzer, adjust ph is 7, tabular titanium-based metal oxide compound is anode (2 groups) to adopt active carbon fiber felt to wrap up in, titanium plate is as negative electrode (4 groups), under agitation, constant output voltage is that 20V carries out electrolysis, each importing new waste water absorption electrolysis 120 minutes, repeatedly carry out 30 times, in its process, when water outlet oleaginousness reaches less than when requiring, manipulation of regeneration need be carried out, regenerative voltage is 20V, regenerated liquid is the KCl concentration of 0.15 mol/L, regenerate 120 minutes.Result is as shown in table 4.
The effect of the circular treatment of table 5 non-mesh Electrode treatment oily(waste)water and regeneration thereof
| For the first time | For the second time | For the third time | 4th time | 5th time | |
| Oil removing rate (%) | 92.3 | 90.4 | 88.2 | 86.5 | 84.3 |
| Regeneration rate (%) | 94.2 | 91.7 | 89.3 | 85.6 | 81.7 |
above about the preferred device of the present invention of the device in embodiment of the method, but be not limited to device of the present invention, that is, utilize existing electrolyzer (or tank) to increase and stir and aerator, the object that technical solution of the present invention will realize can be completed equally.
Claims (5)
1. an activated carbon fiber process oily(waste)water and renovation process thereof, it is characterized in that, in the reactor that the active carbon fiber felt be wrapped on titanium-based metal oxide compound is anode, pure titanium metal is negative electrode, carrying out by means of assisted Regeneration liquid the integration that activated carbon fiber electrochemistry efficiently processes oily(waste)water and in-situ regeneration thereof; Its concrete performing step is as follows:
Step one, by oily(waste)water interval importing reactor in, open direct supply and agitator, carry out absorption electrolysis wastewater, while pass into air to reactor;
When step 2, detection reaction device water outlet oleaginousness are too high, reactor waste water is discharged, import assisted Regeneration liquid, open direct supply and agitator, carry out activated carbon fiber regeneration;
After step 3, activated carbon fiber have regenerated, discharge reactor assisted Regeneration liquid, again import oily(waste)water and enter reactor and carry out absorption electrolysis treatment;
Iterative cycles carries out;
Wherein: the pH value of described oily(waste)water is 3 ~ 10, the current density of adsorbing electrolysis and regeneration is 10 ~ 50mA/m
2, voltage is 10 ~ 20V; Described assisted Regeneration liquid is one or both of the KCl solution of 5 ~ 15g/L or NaCl solution; Assisted Regeneration liquid pH value is 3 ~ 10.
2. activated carbon fiber process oily(waste)water according to claim 1 and renovation process thereof, is characterized in that the described titanium-based metal oxide compound as anode active carbon fiber felt supporter is netted; Negative electrode is netted pure titanium metal.
3. activated carbon fiber process oily(waste)water according to claim 1 and 2 and renovation process thereof, is characterized in that: during described absorption electrolysis oily(waste)water, and the time of absorption electrolysis is 30 ~ 120min; The described regenerated carbon regeneration time is 30 ~ 120min.
4. according to activated carbon fiber process oily(waste)water and the regenerating unit thereof of activated carbon fiber process oily(waste)water described in above-mentioned arbitrary claim and renovation process thereof, comprise reactor and be arranged on the mouth of pipe, electric blender on reactor, it is characterized in that: the mouth of pipe be arranged on reactor comprises: be positioned at the assisted Regeneration liquid water-in of reactor head, venting port, wastewater effluent mouth and be positioned at assisted Regeneration liquid water outlet and the water intake of reactor bottom; In reactor, be provided with the many groups of anodes and cathode sets be alternately arranged, anode and negative electrode introduce reactor external direct current power supply respectively by wire or pole plate; Described anode is the active carbon fiber felt be wrapped on titanium-based metal oxide compound is anode, and described negative electrode is pure titanium metal is negative electrode.
5. activated carbon fiber process oily(waste)water and regenerating unit thereof according to claim 4, is characterized in that: described titanium-based metal oxide compound and pure titanium metal are reticulated structure.
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