CN101327970A - Low mass transfer resistance infiltration flow type electrochemical method and reaction apparatus thereof - Google Patents
Low mass transfer resistance infiltration flow type electrochemical method and reaction apparatus thereof Download PDFInfo
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- CN101327970A CN101327970A CNA2008100412078A CN200810041207A CN101327970A CN 101327970 A CN101327970 A CN 101327970A CN A2008100412078 A CNA2008100412078 A CN A2008100412078A CN 200810041207 A CN200810041207 A CN 200810041207A CN 101327970 A CN101327970 A CN 101327970A
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Abstract
The invention relates to a low mass transfer resistance seepage type electrochemical method and a reaction device belonging to the electrochemical technology field. The method comprises: respectively connecting the anode and cathode of a reaction vessel with the positive and negative poles of a direct power supply, pumping the waste water into the reaction vessel by a peristaltic pump, keeping the two electrodes apart by an insulation, discharging the waste water which passes through the anode and cathode of the reaction vessel from the reaction vessel, or circularly processing the waste water in the reaction vessel through the peristaltic pump. The device comprises the reaction vessel with the anode and cathode in it or surrounding it, the insulation is arranged between the anode and the cathode, the positive and negative poles of the direct power supply are respectively connected with the anode and cathode, and the peristaltic pump is connected with the reaction vessel. The method of the invention reduces the mass transfer resistance on the electrode surface by the interaction between the waste water across the electrode and the electrode, improves the mass transfer coefficient, then improves the current efficiency and reduces the energy consumption.
Description
Technical field
The present invention relates to a kind of method and device thereof of technical field of electrochemistry, specifically, what relate to is a kind of low mass transfer resistance infiltration flow type electrochemical method and reaction unit thereof.
Background technology
In recent years, electrochemical method as a kind of eco-friendly Pollutant Treatment method development rapidly.A kind of treatment process of the electronics that electrochemical techniques are based on efficiently, clean need not to add other reagent, does not produce pollution in treating processes substantially.Because the good environment compatibility of electrochemical method, it plays an important role in pollutent control field.In addition, electric current in the electrochemical process and voltage are more easily measured, and realize control automatically easily.Though electrochemical method has good treatment effect, is not also used on a large scale in practice, main application bottleneck is that efficient is on the low side, the energy consumption height, and running cost is higher.Cause the lower major cause mass-transfer efficiency of electrochemical efficiency lower.According to the literature, the electrochemical method oxidation of organic compounds can be in electrode surface and solution (O, OH and O
3) take place simultaneously, principal reaction occurs in electrode surface.When reactant concn was low, the reaction efficiency of electrode surface mainly was subjected to the restriction of organism from solution to the electrode surface rate of mass transfer.Because reactant can only transmit in the mode of diffusion in the electrostatic double layer of electrode surface, limited the transfer rate of reactant.
Find through literature search prior art, " the Removal ofcolour and COD from wastewater containing acid blue 22 by electrochemicaloxidation " that Marco Panizza etc. delivered on the phase 83-88 page or leaf at " Journal of HazardousMaterials " (dangerous substances magazine) in 2008 153 (electrochemical oxidation method is removed colourity and the COD that contains acid blue 22 waste water), propose in this article, electrochemical reaction efficiency mainly is subjected to the restriction of rate of mass transfer, method by the increased water flow speed of circulation in the literary composition improves mass transfer coefficient, though this method has improved mass transfer effect to a certain extent, its deficiency is that fundamentally not changing organism transmits drawback slowly at electrode surface, and effect is limited.
Summary of the invention
The objective of the invention is at the existing slower problem of electrochemical method mass transfer, a kind of low mass transfer resistance infiltration flow type electrochemical method and reaction unit thereof have been proposed, by making organic waste water reduce resistance to mass transfer from wearing the out of date interaction between electrode, improve mass transfer coefficient, then improve current efficiency, reduce energy expenditure.
The present invention is achieved by the following technical solutions:
Low mass transfer resistance infiltration flow type electrochemical method involved in the present invention, be specially: the positive and negative electrode that the anode and the negative electrode of reaction vessel is connected respectively to direct supply, adopt peristaltic pump that waste water is pumped in the reaction vessel, waste water from reaction vessel anode and negative electrode in pass, there is insulation layer to separate between two electrodes, the waste water that passes behind the electrode is discharged from reaction vessel, perhaps makes waste water carry out circular treatment in reaction vessel by peristaltic pump.Among the present invention, waste water is passed from electrode, when utilizing waste water to penetrate and the interaction of electrode reduce the resistance that reactant transmits to electrode surface, the exchange of having accelerated electrode surface and main body solution material that circulates of waste water is simultaneously upgraded, thereby improve mass transfer coefficient and current efficiency, reduce the energy consumption of electrochemical method.
In order to improve current efficiency, can in waste water, add ionogen, by regulating conditions such as electric current, reaction times and electrolyte concentration organism is fully degraded.Electric current, reaction times and electrolyte concentration are determined according to the size of what and reactor of the character of process object and concentration, treatment capacity.In the present invention, electric current should be controlled at below the 1A, and the reaction times, electrolyte concentration should be not more than 3g/L as far as possible in 3h.
Described ionogen is vitriol or hydrochloride.
Described anode adopts the activated carbon fiber carbon nanotube electrode, and it is long-pending to have increased electrode reaction surfaces, utilizes the peculiar property intensified response activity of carbon nanotube simultaneously; Negative electrode can adopt activated carbon fiber carbon nanotube electrode or wire mesh electrode; Insulation layer adopts insulating material.
Described negative electrode and anodic area can increase along with the increase of treatment capacity, and can be multi-layered electrode.
Low mass transfer resistance infiltration flow type electrochemical reaction unit involved in the present invention, comprise reaction vessel, be provided with anode and negative electrode in the described reaction vessel, perhaps anode and negative electrode are wrapped up in the outside of reaction vessel, be provided with insulation layer between anode and negative electrode, anode links to each other with the positive and negative electrode of direct supply respectively with negative electrode, and reaction vessel is connected with peristaltic pump.Open peristaltic pump, reaction soln is circulated between reaction container bottom and top, solution sees through the electrode sluggish flow in the process, fully contacts the oxidized degraded of organism in this process with electrode.
Described anode adopts the activated carbon fiber carbon nanotube electrode; Negative electrode can adopt activated carbon fiber carbon nanotube electrode or wire mesh electrode.
Described anode and negative electrode are wrapped in the reaction vessel outside, and the impellent by pump makes solution successively by the aperture of reaction vessel sidewall and the electrode of outside, reaches the effect that reduces resistance to mass transfer in this process, improves electrochemical efficiency.The aperture of sidewall is the hole of directly opening on the sidewall of reaction vessel, and effect is exactly that current are passed through, and its big I is determined according to the reaction vessel size, should not make the aperture excessive in principle.For current can be passed through from the reaction vessel all directions uniformly, should make the aperture distribution rule even, and guarantee certain quantity, in principle with the flow velocity of outside current match well the most suitable.
Described anode and negative electrode can be single right, also can adopt the form of many antianodes and negative electrode parallel connection, to increase the processing power of reflection container.
The present invention has significant advantage: when the present invention utilizes the waste water through electrode and the interaction between the electrode reduced the resistance that pollutent transmits to electrode surface greatly, the exchange of having accelerated electrode surface and main body solution material that circulates of waste water is simultaneously upgraded, improved mass transfer coefficient, and finally improved electrochemical efficiency, reduced energy consumption.Adopt activated carbon fiber combined carbon nanotube electrode, improved the reaction table area and the activity of electrode.Simple to operate, equipment takes up an area of less, and various parameters are easy to control, can regulate according to practical situation.
Description of drawings
Fig. 1 is apparatus of the present invention structural representation one;
Fig. 2 is apparatus of the present invention structural representation two;
Among the figure, 1 is anode, and 2 is negative electrode, and 3 is insulation layer, and 4 is peristaltic pump, and 5 is D.C. regulated power supply, and 6 is reaction vessel, and 7 is water-in, and 8 is water outlet.
Embodiment
Below in conjunction with accompanying drawing embodiments of the invention are elaborated: present embodiment is being to implement under the prerequisite with the technical solution of the present invention, provided detailed embodiment and concrete operating process, but protection scope of the present invention is not limited to following embodiment.
As shown in Figure 1, the reaction unit that present embodiment adopts comprises reaction vessel 6, reaction vessel 6 is divided into two portions up and down, the centre is separated by anode 1, negative electrode 2 and insulation layer 3, solution is constantly circulated between reaction vessel 6 top and the bottom by peristaltic pump 4, in the solution circulated process, constantly see through anode 1 and negative electrode 2, in this process by with interelectrode interaction, reduced resistance to mass transfer.D.C. regulated power supply 5 is applied to voltage on anode 1 and the negative electrode 2, and can regulate according to reaction conditions.
During enforcement, anode 1, negative electrode 2 and insulation layer 3 are separately fixed on the reaction vessel 6, with lead anode 1 is connected with D.C. regulated power supply 5 with negative electrode 2, in pending solution, add ionogen, then solution is injected reaction vessel 6, start peristaltic pump 4 and circulate, connect D.C. regulated power supply 5, regulate current density, make reactant obtain good removal.
Implementation condition and result that present embodiment is concrete are as follows:
Reaction target solution volume: 300mL
Reaction target solution concentration: reactive brilliant red x-3b 100mg/L
Envrionment temperature: 25 ℃
Initial pH value: 7
Electrolyte concentration: 3g/L
Electrode area: 28cm
2
Voltage: 10V
Anode: activated carbon fiber carbon nanotube electrode
Negative electrode: activated carbon fiber carbon nanotube electrode
Volumetric flow rate: 80.2mL/min.
Percent of decolourization and the COD clearance of handling the back dyestuff are as shown in table 1.
Table 1 embodiment 1 handles the percent of decolourization and the COD clearance of back dyestuff
| Time (min) | 15 | 30 | 45 | 60 | 75 | 90 |
| Percent of decolourization (%) | 39.7 | 66.0 | 79.9 | 88.8 | 93.6 | 96.4 |
| COD clearance (%) | 6.2 | 16.3 | 35.0 | 46.7 | 51.4 | 57.5 |
The reaction unit that present embodiment adopts is identical with embodiment 1 with implementation process.
Implementation condition and result that present embodiment is concrete are as follows:
Reaction target solution volume: 300mL
Reaction target solution concentration: reactive brilliant red x-3b 50mg/L
Envrionment temperature: 25 ℃
Initial pH value: 7
Electrolyte concentration: 2g/L
Electrode area: 28cm
2
Anode: activated carbon fiber carbon nanotube electrode
Negative electrode: activated carbon fiber carbon nanotube electrode
Volumetric flow rate: 80.2mL/min.
The percent of decolourization that different voltages are handled is as shown in table 2.
The dye decolored rate (%) that table 2 embodiment 2 different voltages are handled
The reaction unit that present embodiment adopts is identical with embodiment 1 with implementation process.
Implementation condition and result that present embodiment is concrete are as follows:
Reaction target solution volume: 300mL
Reaction target solution concentration: Reactive Brilliant Blue X-BR 100mg/L
Envrionment temperature: 25 ℃
Initial pH value: 2
Electrolyte concentration: 1g/L
Electrode area: 28cm
2
Voltage: 8V
Anode: activated carbon fiber carbon nanotube electrode
Negative electrode: copper mesh
Volumetric flow rate: 122.5mL/min.
Percent of decolourization and the COD clearance of handling the back dyestuff are as shown in table 3.
Table 3 embodiment 3 handles the percent of decolourization and the COD clearance of back dyestuff
| Time (min) | 15 | 30 | 45 | 60 | 75 | 90 |
| Percent of decolourization (%) | 25.5 | 51.9 | 67.5 | 78.3 | 83.9 | 87.4 |
| COD clearance (%) | 13.4 | 23.3 | 33.7 | 38.8 | 44.2 | 50.6 |
The reaction unit that present embodiment adopts is identical with embodiment 1 with implementation process.
Implementation condition and result that present embodiment is concrete are as follows:
Reaction target solution volume: 300mL
Reaction target solution concentration: Reactive Brilliant Blue X-BR 100mg/L
Envrionment temperature: 25 ℃
Electrode area: 28cm
2
Voltage: 8V
Electrolyte concentration: 1g/L
Anode: activated carbon fiber carbon nanotube electrode
Negative electrode: copper mesh
Volumetric flow rate: 122.5mL/min.
The percent of decolourization of handling the back dyestuff is as shown in table 4.
The dye decolored rate (%) of table 4 embodiment 4 different initial pH value
The reaction unit that present embodiment adopts is identical with embodiment 1 with implementation process.
Implementation condition and result that present embodiment is concrete are as follows:
Reaction target solution volume: 300mL
Reaction target solution concentration: Reactive Brilliant Blue X-BR 100mg/L
Envrionment temperature: 25 ℃
Electrode area: 28cm
2
Voltage: 8V
Initial pH value: 7
Anode: activated carbon fiber carbon nanotube electrode
Negative electrode: copper mesh
Volumetric flow rate: 122.5mL/min.
The percent of decolourization of handling the back dyestuff is as shown in table 5.
The dye decolored rate (%) of table 5 embodiment 5 different electrolyte concentrations
The above embodiment of the present invention also can adopt reaction unit as shown in Figure 2, this reaction unit comprises reaction vessel 6, reaction vessel 6 is cylindrical, sidewall is covered with aperture, anode 1, negative electrode 2 and insulation layer 3 are wrapped in the outside of reaction vessel 6 successively, and solution is constantly circulated between inside and outside the reaction vessel 6 by peristaltic pump 4.The principle of work of its enforcement is identical with above-mentioned device shown in Figure 1.
Claims (9)
1, a kind of low mass transfer resistance infiltration flow type electrochemical method, it is characterized in that: the positive and negative electrode that the anode and the negative electrode of reaction vessel is connected respectively to direct supply, adopt peristaltic pump that waste water is pumped in the reaction vessel, waste water from reaction vessel anode and negative electrode in pass, there is insulation layer to separate between two electrodes, the waste water that passes behind the electrode is discharged from reaction vessel, perhaps makes waste water carry out circular treatment in reaction vessel by peristaltic pump.
2, low mass transfer resistance infiltration flow type electrochemical method according to claim 1 is characterized in that, described anode adopts the activated carbon fiber carbon nanotube electrode, and negative electrode adopts activated carbon fiber carbon nanotube electrode or wire mesh electrode.
3, low mass transfer resistance infiltration flow type electrochemical method according to claim 1 and 2 is characterized in that, described negative electrode and anodic area increase along with the increase of treatment capacity, and negative electrode and anode are single-layer electrodes or multi-layered electrode.
4, low mass transfer resistance infiltration flow type electrochemical method according to claim 1, it is characterized in that, add ionogen in the described waste water, make organism obtain degraded by regulating electric current, reaction times and electrolyte concentration, wherein: current control is below 1A, reaction times, electrolyte concentration was less than or equal to 3g/L in 3h.
5, low mass transfer resistance infiltration flow type electrochemical method according to claim 4 is characterized in that, described described ionogen is vitriol or hydrochloride.
6, a kind of low mass transfer resistance infiltration flow type electrochemical reaction unit, comprise reaction vessel, it is characterized in that, be provided with anode and negative electrode in the described reaction vessel, perhaps anode and negative electrode are wrapped up in the outside of reaction vessel, be provided with insulation layer between anode and negative electrode, anode links to each other with the positive and negative electrode of direct supply respectively with negative electrode, and reaction vessel is connected with peristaltic pump.
7, low mass transfer resistance infiltration flow type electrochemical reaction unit according to claim 6 is characterized in that, described anode and negative electrode, anode are the activated carbon fiber carbon nanotube electrode, and negative electrode is activated carbon fiber carbon nanotube electrode or wire mesh electrode.
8, low mass transfer resistance infiltration flow type electrochemical reaction unit according to claim 6 is characterized in that, described anode and negative electrode are wrapped in the reaction vessel outside, and the reaction vessel sidewall is provided with distribution rule, uniform aperture.
According to claim 6 or 7 or 8 described low mass transfer resistance infiltration flow type electrochemical reaction units, it is characterized in that 9, described anode and negative electrode are single right, or many antianodes and negative electrode parallel connection.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109399812A (en) * | 2018-12-20 | 2019-03-01 | 大连理工大学 | A kind of electrochemical descaling device |
| CN115849522A (en) * | 2023-03-01 | 2023-03-28 | 广东工业大学 | Flow anode electrochemical sewage treatment device and process based on screening type current collector |
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2008
- 2008-07-31 CN CN2008100412078A patent/CN101327970B/en not_active Expired - Fee Related
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109399812A (en) * | 2018-12-20 | 2019-03-01 | 大连理工大学 | A kind of electrochemical descaling device |
| CN115849522A (en) * | 2023-03-01 | 2023-03-28 | 广东工业大学 | Flow anode electrochemical sewage treatment device and process based on screening type current collector |
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