CN101531411A - Method for electrochemically disinfecting gas diffusion electrode system - Google Patents
Method for electrochemically disinfecting gas diffusion electrode system Download PDFInfo
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- CN101531411A CN101531411A CN200910049125A CN200910049125A CN101531411A CN 101531411 A CN101531411 A CN 101531411A CN 200910049125 A CN200910049125 A CN 200910049125A CN 200910049125 A CN200910049125 A CN 200910049125A CN 101531411 A CN101531411 A CN 101531411A
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Abstract
The invention provides a method for electrically disinfecting a gas diffusion electrode system. The method adopts a nondiaphragm electrolysis system, uses active carbon with membrane structure/PTFE gas diffusion electrode as a cathode, a metal dimensionally stable electrode or a graphite polar plate as an anode, adopts aeration which is simple and practical in environmental engineering close to the cathode, controls the density of electrolytic current below 15mA/cm<2> and flow rate of oxygen in a range between 15 and 75L/h, uses reducing capacity of the cathode and electrocatalysis to generate H2O2, and decomposes the H2O2 to generate hydroxyl radical to sterilize, thereby achieving the aims of sterilization with safety and non-toxicity, equipment investment reduction and treatment effect improvement. The system has wider application range of pH value and is expected to be used in disinfection treatment of tap water or effluent of a secondary sedimentation tank of a sewage treatment plant.
Description
Technical field
The invention belongs to the environmental protection and energy saving field, relate to a kind of electro-chemical water and handle sterilization method, especially adopt the electro-chemical water of gas diffusion electrode system to handle sterilization method.
Background technology
At present, Chang Yong sterilization process has traditional chlorination, disinfection by ultraviolet light and ozonization.The chlorination technology is occupied dominant position in water treatment field, but its major defect is to prepare the raw material of chlorhexidine-containing disinfectant---chlorine, and severe toxicity is not only arranged, and initiation fire, blast easily in storage and transport process, even the accident of loss of life and personal injury.Simultaneously, after it is found that the chlorine disinfectant meeting produces more carcinogenic substance, also more and more careful to the use of chlorine.Ozonization, disinfection by ultraviolet light exist then that technical difficulty is big, investment is big and continue shortcoming such as sterilization effect, and practical application has certain limitation.And on-site preparation sterilizing agent technology has solved the high risk problem that chlorine exists in storage and transport process, thereby is the focus that people pay close attention to always.And the electrochemical disinfection method is one of important method of on-site preparation sterilizing agent.So-called electrochemical disinfection method allows exactly and is sterilized object by electrochemical appliance, thereby reaches sterilization, disinfectant purpose.Adopt the advantage of electrochemical disinfection method to be: at first, electrochemical process can be killed multiple harmful microorganism; Secondly, can utilize anodizing or reduction characteristic to remove different kinds of ions impurity in the water; The 3rd, the electrochemical disinfection system has lasting sterilizing ability, and electric field still can sterilization algae removal after disappearing.And the electrochemical process operational management is simple, safety, reliable, and through the overtesting confirmation, sterilization speed is fast.Current consumption is lower.The amount of the trichloromethane that the employing electrochemical process generates is lower than the amount that chlorination generates, even contain the more water of precursor substance of THMs (haloform), through the electrochemical content of handling haloform in the water of back still be lower than defined in the national standard numerical value (Chang Yu etc. the electrochemical disinfection method is handled the feasibility study of reuse water, Techniques and Equipment for Environmental Pollution Control, 2002, Vol.3:46-50).
Existing much about germ-resistant research report of electricity consumption and actual case, but up to now, this technology fails to obtain large-scale widespread use.Various dissimilar electrochemical reactors also just are used for producing sterilizing agent chlorine or ozone, and the research of electrochemical method sterilization organic waste water and tap water is also just concentrated on the anode aspect.The existing steady electrode of multiple shape (DSA) is as anode, as Ti/IrO
2, Ti/RuO
2In being applied to water treatment morely and being sterilized.But only in the higher aqueous solution of Cl-concentration, just can obtain than higher sterilizing rate; Do not containing Cl
-Water in, mainly rely on the active group that produces on the electrode to realize germicidal action.
Electric current passes through Cl by pending water on the anode
-The HClO that oxidation produces is main disinfecting substance.Meanwhile, there are a large amount of oxygen to overflow on the anode, useless evolving hydrogen reaction takes place on the negative electrode.The oxygen mix that these hydrogen and anode produce may form the mixture of explosive hydrogen and oxygen.And the accumulation of a large amount of hydrogen can destroy normal water movement in the pipeline.Hydrogen can permeate many metals, causes hydrogen-type corrosion, thereby metal is become fragile.In addition, running cost also because useless liberation of hydrogen becomes the comparison costliness (with liquid chlorine sterilization relatively).
H
2O
2Be successfully used to handle and disinfectant soup water and all kinds of sewage, its oxidizing reaction can not stay any byproduct of reaction in water, and reaction itself is not with danger, carries out under the condition of gentleness.Peroxidation on the electrode would not produce carcinogenic substance, does not need to add any chemical agent, and running cost reduces.Turbidity and colourity are basic all to be removed, and the removal of turbidity is main because organism and bacterium are oxidized.The H that cathode surface produces
2O
2Can permeates cell membranes through nucleus, and it also is proved to be has lasting disinfection (Drogui, et al., Wat.Res., 2001, Vol.35:3235～3241).Booch and Stocklin (German Patent: DE19631842) once the oxygen consumption negative electrode was used for the on-the-spot H of generation
2O
2The disinfectant soup water.On the oxygen consumption negative electrode, oxygen is reduced into H
2O
2And OH
-Compare H with other disinfecting substance
2O
2Redox potential lower, but germ-killing efficiency do not have to improve substantially, this is because the H that forms on the oxygen consumption negative electrode
2O
2React with the free chlorine residue that generates on the anode and to generate HCl.Another shortcoming of oxygen consumption negative electrode is: H can take place in the oxygen that only is dissolved in the water
2O
2The solubleness of oxygen in water is very low, when the P=1 normal atmosphere, has only 8～10mg/L.If use the pure oxygen oxygenation, the concentration＜25mg/L of dissolved oxygen in the water.So, H
2O
2Output very low, negative electrode generates H
2O
2Efficient very low, be difficult to practical application in waste water and drinking water disinfection field, therefore the oxygen consumption electrode is not widely used yet.
Summary of the invention
The objective of the invention is at the deficiencies in the prior art, adopt gas diffusion electrode system to carry out electro-chemical water and handle sterilization, a kind of water treatment sterilization method of efficient and safety non-toxic is provided.
For reaching above purpose, solution of the present invention is: adopt the compound gas diffusion electrode system to carry out electro-chemical water and handle sterilization, its essence is to produce H in electrochemical process
2O
2And highly active hydroxyl radical free radical kill bacteria.
The present invention has following feature:
Compound gas diffusion electrode as electrolytic process negative electrode of the present invention is made up of conducting matrix grain and diffusing catalyst layer two portions.Wherein any material of employing C, Fe, elements such as Ni, Cu or its alloy are as conduction and support skeleton, adopt the big carbon of specific surface area, comprise the base material of wherein any materials such as Powdered Activated Carbon, Graphite Powder 99, acetylene black, carbon black, carbon fiber as the diffusing catalyst layer, wherein any material of elements such as employing Pt, Au, Ag, Cu, Fe, Ni, Mn or its alloy are as the catalyzer in the diffusion layer, and the mass ratio of catalyzer and diffusing catalyst layer base material is 0～5 ‰.Also contain a certain amount of low temperature pore-forming material NH in the diffusing catalyst layer
4HCO
3Perhaps (NH
4)
2CO
3, the mass ratio of pore-forming material and diffusing catalyst layer base material is 0～70%.
Electrolytic process carries out under applying direct current, and current density is controlled at 15mA/cm
2Below.The excessive reduction current efficiency of current density, the too small generating rate that influences free radical of current density.
It is to carry out in having the reactor of gas diffusion electrode that electro-chemical water is handled sterilizing process, and anode adopts graphite pole plate or the steady electrode of shape.Reduction reaction takes place in the oxygen that electrolysis produces or the oxygen of feeding on diffusion electrode, the oxygen gas flow rate of feeding is controlled in 15～75L/h scope.By gas diffusion electrode, can reduce voltage pressure reduction between battery lead plate, reduce the generation of analysing side reactions such as oxygen or liberation of hydrogen, improve current efficiency.
Former water is after 10～30min reaction, and total plate count greatly reduces.The present invention is expected to be used for the electrochemical disinfection water treatment.
Owing to adopted such scheme, the present invention has the following advantages:
1. this operation is carried out at normal temperatures and pressures, and easy and simple to handle, equipment is simple.
2. adopt this technology to carry out electro-chemical water and handle sterilization, it is low to have an investment, and treatment effect is good, and is stable, the advantage of safety non-toxic.
3. this system pH scope of application is wider.
4. this equipment is particularly useful for the sterilization and disinfection of the few tap water of bacteria content, and its current residence time is short, and occupation area of equipment is few.
Description of drawings
Fig. 1 is the equipment configuration synoptic diagram of the embodiment of the invention.
Embodiment
Below in conjunction with specific embodiment technical scheme of the present invention is described further.
Electrolysis reaction device mainly is made up of oxygen bottle 1 and under meter 2, electrolyzer 3 and dc current regulator power supply 7 three parts as shown in Figure 1.Adopt above-mentioned homemade gac/PTFE gas diffusion electrode 4 as negative electrode, anode adopts common graphite pole plate 5 or the steady electrode of metal shape, electrolytic reduction O
2H takes place
2O
21 rectangle anode and 1 rectangular cathode are positioned at the centre of electrolyzer, and spacing is 10mm, the thick 5mm of pole plate.
Sterilizing mechanisms:
Negative electrode: oxygen obtains two electron reductions and generates H
2O
2:
O
2+2H
++2e
-→H
2O
2 (1)
When negative electrode uses when having the absorbent charcoal material of strong adsorptivity, bacterium is adsorbed onto the surface of electrode, carry out sterilization and disinfection at electrode surface then.
The compound gas diffusion electrode that embodiment 1 usefulness does not contain pore-forming material and catalyzer carries out electrochemical disinfection as negative electrode
The present invention is to containing total plate count 10
6The water distribution of CFU/mL under the composite gas dispenser cathode effect that does not contain pore-forming material and catalyzer, is carried out electrolysis, control current density 6.6mA/cm
2, oxygen gas flow rate reacts at 30L/h, takes a sample in different time respectively, with bacterial detection sum behind the standard Plating cultivation 24h.Germ-killing efficiency only was 63.27% when from following table as can be seen, energy consumption equaled 0.62Wh/L.
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 7.14 |
| 10 | 0.21 | 19.39 |
| 15 | 0.31 | 28.57 |
| 20 | 0.41 | 37.76 |
| 25 | 0.52 | 50.00 |
| 30 | 0.62 | 63.27 |
Embodiment 2 usefulness contain pore-forming material NH
4HCO
3Compound gas diffusion electrode carry out electrochemical disinfection as negative electrode
The present invention is to containing total plate count 10
6The water distribution of CFU/mL is under 30% the compound gas diffusion electrode effect, to carry out electrolysis at pore-forming material content.Other conditions are with application example 1.Germ-killing efficiency reached more than 77% when from following table as can be seen, energy consumption equaled 0.63Wh/L.
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 25.00 |
| 10 | 0.21 | 39.58 |
| 15 | 0.31 | 50.00 |
| 20 | 0.42 | 58.33 |
| 25 | 0.52 | 66.67 |
| 30 | 0.63 | 77.92 |
Be that other reaction conditionss are the same, carry out electrolysis, obtain following result under 40% the compound diffusion electrode effect at pore-forming material content:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 25.53 |
| 10 | 0.22 | 42.55 |
| 15 | 0.32 | 57.45 |
| 20 | 0.42 | 72.09 |
| 25 | 0.53 | 85.93 |
| 30 | 0.64 | 93.62 |
Be that germ-killing efficiency reached more than 93% when energy consumption equaled 0.64Wh/L under 40% the compound diffusion electrode effect at pore-forming material content.
Be that other reaction conditionss are the same, carry out electrolysis, obtain following result under 70% the compound diffusion electrode effect at pore-forming material content:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.11 | 31.11 |
| 10 | 0.22 | 45.19 |
| 15 | 0.33 | 62.96 |
| 20 | 0.44 | 79.26 |
| 25 | 0.55 | 90.03 |
| 30 | 0.66 | 97.04 |
Be that germ-killing efficiency reached more than 97% when energy consumption equaled 0.66Wh/L under 70% the compound diffusion electrode effect at pore-forming material content.The increase of pore-forming material has obviously improved sterilization effect.
The compound gas diffusion electrode that embodiment 3 usefulness contain catalyst Pt carries out electrochemical disinfection as negative electrode
The present invention is to containing the water distribution of total plate count 106CFU/mL, at catalyst Pt content is under 2 ‰ the compound gas diffusion electrode effect, to carry out electrolysis.Other conditions are with application example 1.Germ-killing efficiency reached more than 79% when from following table as can be seen, energy consumption equaled 0.58Wh/L.
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 14.63 |
| 10 | 0.20 | 32.93 |
| 15 | 0.29 | 48.78 |
| 20 | 0.39 | 58.54 |
| 25 | 049 | 67.07 |
| 30 | 0.58 | 79.27 |
Be that other reaction conditionss are the same, carry out electrolysis, obtain following result under 3 ‰ the compound diffusion electrode effect at catalyst Pt content:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 15.92 |
| 10 | 0.20 | 41.78 |
| 15 | 0.30 | 57.21 |
| 20 | 0.40 | 65.67 |
| 25 | 0.50 | 75.64 |
| 30 | 0.60 | 89.05 |
Be that germ-killing efficiency reached more than 89% when energy consumption equaled 0.60Wh/L under 3 ‰ the compound diffusion electrode effect at catalyst Pt content.Catalyst Pt can improve H
2O
2The current efficiency of producing, its carrying capacity is high more, and the quantity that is in activity site Pt is many more, and sterilization effect is good more.
The present invention is to containing the water distribution of total plate count 106CFU/mL, at catalyst content is under 3 ‰ the compound gas diffusion electrode effect, to carry out electrolysis.The control oxygen gas flow rate is at 15L/h, and other conditions are with application example 1.When from following table as can be seen, energy consumption equals 0.60Wh/L germ-killing efficiency reach～80%.
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 10.47 |
| 10 | 0.20 | 34.88 |
| 15 | 0.30 | 48.26 |
| 20 | 0.40 | 58.14 |
| 25 | 0.50 | 68.02 |
| 30 | 0.60 | 79.65 |
Be that the control oxygen gas flow rate is at 30L/h under 3 ‰ the compound diffusion electrode effect at catalyst content, other reaction conditionss are the same, obtain following result:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 22.17 |
| 10 | 0.20 | 47.78 |
| 15 | 0.30 | 61.58 |
| 20 | 0.40 | 76.35 |
| 25 | 0.50 | 84.24 |
| 30 | 0.60 | 91.13 |
Be that oxygen gas flow rate is 30L/h under 3 ‰ the compound gas diffusion electrode effect at catalyst content, when energy consumption equals 0.60Wh/L germ-killing efficiency reach～more than 91%.
Be that the control oxygen gas flow rate is at 75L/h under 3 ‰ the compound diffusion electrode effect at catalyst content, other reaction conditionss are the same, obtain following result:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.11 | 45.00 |
| 10 | 0.22 | 71.11 |
| 15 | 0.33 | 89.17 |
| 20 | 0.44 | 92.78 |
| 25 | 0.55 | 94.44 |
| 30 | 0.66 | 97.83 |
Be that oxygen gas flow rate is 75L/h under 3 ‰ the compound gas diffusion electrode effect at catalyst content, germ-killing efficiency reached 97.83% when energy consumption equaled 0.66Wh/L.On the one hand, the raising of oxygen gas flow rate has improved sterilization effect to a certain extent, has shortened the treatment time, thereby facility investment is reduced; On the other hand, the raising of oxygen gas flow rate has increased the sterilization energy consumption, thereby the germ-resistant running cost of this system is improved.
The present invention is to containing the water distribution of total plate count 106CFU/mL, at catalyst content is under 3 ‰ the compound gas diffusion electrode effect, to carry out electrolysis.Former water pH=5.Other conditions are with application example 1.Result such as following table:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 41.68 |
| 10 | 0.22 | 58.46 |
| 15 | 0.32 | 76.35 |
| 20 | 0.42 | 85.54 |
| 25 | 0.53 | 89.90 |
| 30 | 0.64 | 92.31 |
Be that former water pH is 6 under 3 ‰ the compound diffusion electrode effect at catalyst content, other reaction conditionss are the same, obtain following result:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 37.34 |
| 10 | 0.22 | 45.43 |
| 15 | 0.32 | 53.55 |
| 20 | 0.42 | 58.80 |
| 25 | 0.53 | 67.60 |
| 30 | 0.64 | 88.30 |
Be that former water pH is 8 under 3 ‰ the compound diffusion electrode effect at catalyst content, other reaction conditionss are the same, obtain following result:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.10 | 30.87 |
| 10 | 0.22 | 38.70 |
| 15 | 0.32 | 46.43 |
| 20 | 0.42 | 52.39 |
| 25 | 0.53 | 58.91 |
| 30 | 0.64 | 85.81 |
Germ-killing efficiency reduces along with the rising of pH, but the amplitude that changes is little.When pH=5～8, electrolysis after 30 minutes germ-killing efficiency all can reach more than 85%.Generally the total plate count of Sewage Plant second pond water outlet is～104CFU/mL, is far smaller than the total plate count in the experimental water, utilizes body series to carry out the electrochemical disinfection water treatment and be expected to obtain effect preferably in the shorter treatment time.So this system is expected to be used for the sterilization and disinfection of water outlet of Sewage Plant second pond and tap water.
Embodiment 6 usefulness catalyst Pt content are that 3 ‰ compound gas diffusion electrode carries out electrochemical disinfection as negative electrode under different current densities
The present invention is to containing the water distribution of total plate count 106CFU/mL, is under 3 ‰ the compound gas diffusion electrode effect at catalyst content, control current density 3.3mA/cm
2, carry out electrolysis.Other conditions are with application example 1.Result such as following table:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.04 | 14.75 |
| 10 | 0.08 | 33.33 |
| 15 | 0.12 | 43.72 |
| 20 | 0.15 | 57.92 |
| 25 | 0.19 | 71.04 |
| 30 | 0.23 | 82.51 |
Be under 3 ‰ the compound diffusion electrode effect at catalyst content, control current density 10mA/cm
2, other reaction conditionss are the same, obtain following result:
| Time (min) | Energy consumption (Wh/L) | Germ-killing efficiency (%) |
| 5 | 0.16 | 35.30 |
| 10 | 0.33 | 52.42 |
| 15 | 0.49 | 69.39 |
| 20 | 0.65 | 83.94 |
| 25 | 0.81 | 91.45 |
| 30 | 0.98 | 95.85 |
The above-mentioned description to embodiment is can understand and apply the invention for ease of those skilled in the art.The person skilled in the art obviously can easily make various modifications to these embodiment, and needn't pass through performing creative labour being applied in the General Principle of this explanation among other embodiment.Therefore, the invention is not restricted to the embodiment here, those skilled in the art should be within protection scope of the present invention for improvement and modification that the present invention makes according to announcement of the present invention.
Claims (5)
1, a kind of water treatment sterilization method is characterized in that: adopt the compound gas diffusion electrode system to carry out electro-chemical water and handle sterilization, produce H in electrochemical process
2O
2And highly active hydroxyl radical free radical kill bacteria.
2, water treatment sterilization method according to claim 1, it is characterized in that: adopt the diaphragm-free electrolysis system, adopt membrane structure gac/PTFE gas diffusion electrode as negative electrode, adopt steady electrode of metal shape or graphite pole plate as anode, and at the next door of negative electrode aeration.
3, water treatment sterilization method according to claim 1, it is characterized in that: described compound gas diffusion electrode is made up of conducting matrix grain and diffusing catalyst layer two portions, adopt C, Fe, Ni, any one material in the Cu element or its alloy are as conduction and support skeleton, adopt Powdered Activated Carbon, Graphite Powder 99, acetylene black, carbon black, any one material in the carbon fiber is as the base material of diffusing catalyst layer, adopt Pt, Au, Ag, Cu, Fe, Ni, any one material in the Mn element or its alloy are as the catalyzer in the diffusion layer, the mass ratio of catalyzer and diffusing catalyst layer base material is in 5 ‰, also contains low temperature pore-forming material NH in the diffusing catalyst layer
4HCO
3Perhaps (NH
4)
2CO
3, the mass ratio of pore-forming material and diffusing catalyst layer base material is less than 70%.
4, water treatment sterilization method according to claim 1, it is characterized in that: electrolytic process carries out under applying direct current, and current density is controlled at 15mA/cm
2Below.
5, water treatment sterilization method according to claim 1 is characterized in that: the oxygen that electrolysis produces or the oxygen of feeding, reduction reaction takes place on diffusion electrode, and the oxygen gas flow rate of feeding is controlled in 15～75L/h scope.
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| CN112795941A (en) * | 2020-12-22 | 2021-05-14 | 哈尔滨工业大学 | Method for electrosynthesis of hydrogen peroxide by utilizing columnar active coke |
| CN113718280A (en) * | 2021-08-31 | 2021-11-30 | 苏州清缘环保科技有限公司 | Gas diffusion electrode and method for producing same |
| CN113718280B (en) * | 2021-08-31 | 2024-04-26 | 苏州清氧环境科技有限公司 | Gas diffusion electrode and method for producing same |
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